femtosecond pump-probe photoionization: Topics by Science.gov

Sample records for femtosecond pump-probe photoionization

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

2009-10-07

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.
Analysis of femtosecond pump-probe photoelectron-photoion coincidence measurements applying Bayesian probability theory

NASA Astrophysics Data System (ADS)

Rumetshofer, M.; Heim, P.; Thaler, B.; Ernst, W. E.; Koch, M.; von der Linden, W.

2018-06-01

Ultrafast dynamical processes in photoexcited molecules can be observed with pump-probe measurements, in which information about the dynamics is obtained from the transient signal associated with the excited state. Background signals provoked by pump and/or probe pulses alone often obscure these excited-state signals. Simple subtraction of pump-only and/or probe-only measurements from the pump-probe measurement, as commonly applied, results in a degradation of the signal-to-noise ratio and, in the case of coincidence detection, the danger of overrated background subtraction. Coincidence measurements additionally suffer from false coincidences, requiring long data-acquisition times to keep erroneous signals at an acceptable level. Here we present a probabilistic approach based on Bayesian probability theory that overcomes these problems. For a pump-probe experiment with photoelectron-photoion coincidence detection, we reconstruct the interesting excited-state spectrum from pump-probe and pump-only measurements. This approach allows us to treat background and false coincidences consistently and on the same footing. We demonstrate that the Bayesian formalism has the following advantages over simple signal subtraction: (i) the signal-to-noise ratio is significantly increased, (ii) the pump-only contribution is not overestimated, (iii) false coincidences are excluded, (iv) prior knowledge, such as positivity, is consistently incorporated, (v) confidence intervals are provided for the reconstructed spectrum, and (vi) it is applicable to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, the Bayesian approach allows us to run experiments at higher ionization rates, resulting in a significant reduction of data acquisition times. The probabilistic approach is thoroughly scrutinized by challenging mock data. The application to pump-probe coincidence measurements on acetone molecules enables quantitative interpretations
Femtosecond Pump-Push-Probe and Pump-Dump-Probe Spectroscopy of Conjugated Polymers: New Insight and Opportunities.

PubMed

Kee, Tak W

2014-09-18

Conjugated polymers are an important class of soft materials that exhibit a wide range of applications. The excited states of conjugated polymers, often referred to as excitons, can either deactivate to yield the ground state or dissociate in the presence of an electron acceptor to form charge carriers. These interesting properties give rise to their luminescence and the photovoltaic effect. Femtosecond spectroscopy is a crucial tool for studying conjugated polymers. Recently, more elaborate experimental configurations utilizing three optical pulses, namely, pump-push-probe and pump-dump-probe, have been employed to investigate the properties of excitons and charge-transfer states of conjugated polymers. These studies have revealed new insight into femtosecond torsional relaxation and detrapping of bound charge pairs of conjugated polymers. This Perspective highlights (1) the recent achievements by several research groups in using pump-push-probe and pump-dump-probe spectroscopy to study conjugated polymers and (2) future opportunities and potential challenges of these techniques.
High-speed femtosecond pump-probe spectroscopy with a smart pixel detector array.

PubMed

Bourquin, S; Prasankumar, R P; Kärtner, F X; Fujimoto, J G; Lasser, T; Salathé, R P

2003-09-01

A new femtosecond pump-probe spectroscopy technique is demonstrated that permits the high-speed, parallel acquisition of pump-probe measurements at multiple wavelengths. This is made possible by use of a novel, two-dimensional smart pixel detector array that performs amplitude demodulation in real time on each pixel. This detector array can not only achieve sensitivities comparable with lock-in amplification but also simultaneously performs demodulation of probe transmission signals at multiple wavelengths, thus permitting rapid time- and wavelength-resolved femtosecond pump-probe spectroscopy. Measurements on a thin sample of bulk GaAs are performed across 58 simultaneous wavelengths. Differential probe transmission changes as small as approximately 2 x 10(-4) can be measured over a 5-ps delay scan in only approximately 3 min. This technology can be applied to a wide range of pump-probe measurements in condensed matter, chemistry, and biology.
Photoionization of NaK molecule with a double-well potential in femtosecond pump probe pulse laser fields

NASA Astrophysics Data System (ADS)

Yu, Jie; Wang, Sen-Ming; Yuan, Kai-Jun; Cong, Shu-Lin

2006-09-01

The method of time-dependent quantum wave packet dynamics is used to calculate the femtosecond pump-probe photoelectron spectra and study the wave packet dynamic processes of the double-minimum potential state 61Σ+ of NaK in intense laser fields. The evolutions of the wave packet and the photoelectron energy spectra with time and internuclear distance are described in detail. The wave packet dynamic information of the 61Σ+ state can be extracted from the photoelectron energy spectra.
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
Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

DOE PAGES

Picón, A.; Lehmann, C. S.; Bostedt, C.; ...

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 XeF 2 molecules following X-ray absorption at the Xe site.« less
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

2016-05-23

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

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

van Thor, Jasper J.; Madsen, Anders

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

DOE PAGES

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
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.
Two-tint pump-probe measurements using a femtosecond laser oscillator and sharp-edged optical filters.

PubMed

Kang, Kwangu; Koh, Yee Kan; Chiritescu, Catalin; Zheng, Xuan; Cahill, David G

2008-11-01

We describe a simple approach for rejecting unwanted scattered light in two types of time-resolved pump-probe measurements, time-domain thermoreflectance (TDTR) and time-resolved incoherent anti-Stokes Raman scattering (TRIARS). Sharp edged optical filters are used to create spectrally distinct pump and probe beams from the broad spectral output of a femtosecond Ti:sapphire laser oscillator. For TDTR, the diffusely scattered pump light is then blocked by a third optical filter. For TRIARS, depolarized scattering created by the pump is shifted in frequency by approximately 250 cm(-1) relative to the polarized scattering created by the probe; therefore, spectral features created by the pump and probe scattering can be easily distinguished.
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
Focal overlap gating in velocity map imaging to achieve high signal-to-noise ratio in photo-ion pump-probe experiments

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

Shivaram, Niranjan; Champenois, Elio G.; Cryan, James P.

We demonstrate a technique in velocity map imaging (VMI) that allows spatial gating of the laser focal overlap region in time resolved pump-probe experiments. This significantly enhances signal-to-noise ratio by eliminating background signal arising outside the region of spatial overlap of pump and probe beams. This enhancement is achieved by tilting the laser beams with respect to the surface of the VMI electrodes which creates a gradient in flight time for particles born at different points along the beam. By suitably pulsing our microchannel plate detector, we can select particles born only where the laser beams overlap. Furthermore, this spatialmore » gating in velocity map imaging can benefit nearly all photo-ion pump-probe VMI experiments especially when extreme-ultraviolet light or X-rays are involved which produce large background signals on their own.« less
Focal overlap gating in velocity map imaging to achieve high signal-to-noise ratio in photo-ion pump-probe experiments

DOE PAGES

Shivaram, Niranjan; Champenois, Elio G.; Cryan, James P.; ...

2016-12-19

We demonstrate a technique in velocity map imaging (VMI) that allows spatial gating of the laser focal overlap region in time resolved pump-probe experiments. This significantly enhances signal-to-noise ratio by eliminating background signal arising outside the region of spatial overlap of pump and probe beams. This enhancement is achieved by tilting the laser beams with respect to the surface of the VMI electrodes which creates a gradient in flight time for particles born at different points along the beam. By suitably pulsing our microchannel plate detector, we can select particles born only where the laser beams overlap. Furthermore, this spatialmore » gating in velocity map imaging can benefit nearly all photo-ion pump-probe VMI experiments especially when extreme-ultraviolet light or X-rays are involved which produce large background signals on their own.« less
Control of nitromethane photoionization efficiency with shaped femtosecond pulses.

PubMed

Roslund, Jonathan; Shir, Ofer M; Dogariu, Arthur; Miles, Richard; Rabitz, Herschel

2011-04-21

The applicability of adaptive femtosecond pulse shaping is studied for achieving selectivity in the photoionization of low-density polyatomic targets. In particular, optimal dynamic discrimination (ODD) techniques exploit intermediate molecular electronic resonances that allow a significant increase in the photoionization efficiency of nitromethane with shaped near-infrared femtosecond pulses. The intensity bias typical of high-photon number, nonresonant ionization is accounted for by reference to a strictly intensity-dependent process. Closed-loop adaptive learning is then able to discover a pulse form that increases the ionization efficiency of nitromethane by ∼150%. The optimally induced molecular dynamics result from entry into a region of parameter space inaccessible with intensity-only control. Finally, the discovered pulse shape is demonstrated to interact with the molecular system in a coherent fashion as assessed from the asymmetry between the response to the optimal field and its time-reversed counterpart.
Ultrafast hopping dynamics of 5f electrons in the Mott insulator UO₂ studied by femtosecond pump-probe spectroscopy.

PubMed

An, Yong Q; Taylor, Antoinette J; Conradson, Steven D; Trugman, Stuart A; Durakiewicz, Tomasz; Rodriguez, George

2011-05-20

We describe a femtosecond pump-probe study of ultrafast hopping dynamics of 5f electrons in the Mott insulator UO₂ following Mott-gap excitation at temperatures of 5-300 K. Hopping-induced response of the lattice and electrons is probed by transient reflectivity at mid- and above-gap photon energies, respectively. These measurements show an instantaneous hop, subsequent picosecond lattice deformation, followed by acoustic phonon emission and microsecond relaxation. Temperature-dependent studies indicate that the slow relaxation results from Hubbard excitons formed by U³⁺-U⁵⁺ pairs.
Temporal-spatial measurement of electron relaxation time in femtosecond laser induced plasma using two-color pump-probe imaging technique

NASA Astrophysics Data System (ADS)

Pan, Changji; Jiang, Lan; Wang, Qingsong; Sun, Jingya; Wang, Guoyan; Lu, Yongfeng

2018-05-01

The femtosecond (fs) laser is a powerful tool to study ultrafast plasma dynamics, especially electron relaxation in strong ionization of dielectrics. Herein, temporal-spatial evolution of femtosecond laser induced plasma in fused silica was investigated using a two-color pump-probe technique (i.e., 400 nm and 800 nm, respectively). We demonstrated that when ionized electron density is lower than the critical density, free electron relaxation time is inversely proportional to electron density, which can be explained by the electron-ion scattering regime. In addition, electron density evolution within plasma was analyzed in an early stage (first 800 fs) of the laser-material interaction.
Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering at flame temperatures using a second-harmonic bandwidth-compressed probe.

PubMed

Kearney, Sean P; Scoglietti, Daniel J

2013-03-15

We demonstrate an approach for picosecond probe-beam generation that enables hybrid femtosecond/picosecond pure-rotational coherent anti-Stokes Raman scattering (CARS) measurements in flames. Sum-frequency generation of bandwidth-compressed picosecond radiation from femtosecond pumps with phase-conjugate chirps provides probe pulses with energies in excess of 1 mJ that are temporally locked to the femtosecond pump/Stokes preparation. This method overcomes previous limitations on hybrid femtosecond/picosecond rotational CARS techniques, which have relied upon less efficient bandwidth-reduction processes that have generally resulted in prohibitively low probe energy for flame measurements. We provide the details of the second-harmonic approach and demonstrate the technique in near-adiabatic hydrogen/air flames.

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.
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.
Time-resolved multi-mass ion imaging: Femtosecond UV-VUV pump-probe spectroscopy with the PImMS camera.

PubMed

Forbes, Ruaridh; Makhija, Varun; Veyrinas, Kévin; Stolow, Albert; Lee, Jason W L; Burt, Michael; Brouard, Mark; Vallance, Claire; Wilkinson, Iain; Lausten, Rune; Hockett, Paul

2017-07-07

The Pixel-Imaging Mass Spectrometry (PImMS) camera allows for 3D charged particle imaging measurements, in which the particle time-of-flight is recorded along with (x, y) position. Coupling the PImMS camera to an ultrafast pump-probe velocity-map imaging spectroscopy apparatus therefore provides a route to time-resolved multi-mass ion imaging, with both high count rates and large dynamic range, thus allowing for rapid measurements of complex photofragmentation dynamics. Furthermore, the use of vacuum ultraviolet wavelengths for the probe pulse allows for an enhanced observation window for the study of excited state molecular dynamics in small polyatomic molecules having relatively high ionization potentials. Herein, preliminary time-resolved multi-mass imaging results from C 2 F 3 I photolysis are presented. The experiments utilized femtosecond VUV and UV (160.8 nm and 267 nm) pump and probe laser pulses in order to demonstrate and explore this new time-resolved experimental ion imaging configuration. The data indicate the depth and power of this measurement modality, with a range of photofragments readily observed, and many indications of complex underlying wavepacket dynamics on the excited state(s) prepared.
Investigation of the S1/ICT equilibrium in fucoxanthin by ultrafast pump-dump-probe and femtosecond stimulated Raman scattering spectroscopy.

PubMed

Redeckas, Kipras; Voiciuk, Vladislava; Vengris, Mikas

2016-05-01

Time-resolved multi-pulse spectroscopic methods-pump-dump-probe (PDP) and femtosecond stimulated Raman spectroscopy-were used to investigate the excited state photodynamics of the carbonyl group containing carotenoid fucoxanthin (FX). PDP experiments show that S1 and ICT states in FX are strongly coupled and that the interstate equilibrium is rapidly (<5 ps) reestablished after one of the interacting states is deliberately depopulated. Femtosecond stimulated Raman scattering experiments indicate that S1 and ICT are vibrationally distinct species. Identification of the FSRS modes on the S1 and ICT potential energy surfaces allows us to predict a possible coupling channel for the state interaction.
Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation.

PubMed

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho, Jr-Wei; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-28

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH 3 ) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH 3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S 1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH 3 ] + cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.
Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation

NASA Astrophysics Data System (ADS)

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho-Wei, Jr.; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-01

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH3) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH3]+ cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ˜70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.
All-optical switching in GaAs microdisk resonators by a femtosecond pump-probe technique through tapered-fiber coupling.

PubMed

Lin, Yen-Chih; Mao, Ming-Hua; Lin, You-Ru; Lin, Hao-Hsiung; Lin, Che-An; Wang, Lon A

2014-09-01

We demonstrate ultrafast all-optical switching in GaAs microdisk resonators using a femtosecond pump-probe technique through tapered-fiber coupling. The temporal tuning of the resonant modes resulted from the refractive index change due to photoexcited carrier density variation inside the GaAs microdisk resonator. Transmission through the GaAs microdisk resonator can be modulated by more than 10 dB with a switching time window of 8 ps in the switch-off operation using pumping pulses with energies as low as 17.5 pJ. The carrier lifetime was fitted to be 42 ps, much shorter than that of the bulk GaAs, typically of the order of nanoseconds. The above observation indicates that the surface recombination plays an important role in increasing the switching speed.
Tabletop Femtosecond VUV Photoionization and PEPICO Detection of Microreactor Pyrolysis Products.

PubMed

Couch, David E; Buckingham, Grant T; Baraban, Joshua H; Porterfield, Jessica P; Wooldridge, Laura A; Ellison, G Barney; Kapteyn, Henry C; Murnane, Margaret M; Peters, William K

2017-07-20

We report the combination of tabletop vacuum ultraviolet photoionization with photoion-photoelectron coincidence spectroscopy for sensitive, isomer-specific detection of nascent products from a pyrolysis microreactor. Results on several molecules demonstrate two essential capabilities that are very straightforward to implement: the ability to differentiate isomers and the ability to distinguish thermal products from dissociative ionization. Here, vacuum ultraviolet light is derived from a commercial tabletop femtosecond laser system, allowing data to be collected at 10 kHz; this high repetition rate is critical for coincidence techniques. The photoion-photoelectron coincidence spectrometer uses the momentum of the ion to identify dissociative ionization events and coincidence techniques to provide a photoelectron spectrum specific to each mass, which is used to distinguish different isomers. We have used this spectrometer to detect the pyrolysis products that result from the thermal cracking of acetaldehyde, cyclohexene, and 2-butanol. The photoion-photoelectron spectrometer can detect and identify organic radicals and reactive intermediates that result from pyrolysis. Direct comparison of laboratory and synchrotron data illustrates the advantages and potential of this approach.
Pump-probe micro-spectroscopy by means of an ultra-fast acousto-optics delay line.

PubMed

Audier, Xavier; Balla, Naveen; Rigneault, Hervé

2017-01-15

We demonstrate femtosecond pump-probe transient absorption spectroscopy using a programmable dispersive filter as an ultra-fast delay line. Combined with fast synchronous detection, this delay line allows for recording of 6 ps decay traces at 34 kHz. With such acquisition speed, we perform single point pump-probe spectroscopy on bulk samples in 80 μs and hyperspectral pump-probe imaging over a field of view of 100 μm in less than a second. The usability of the method is illustrated in a showcase experiment to image and discriminate between two pigments in a mixture.
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

2015-12-18

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.
Photochemical Kinetics of a Phosphine Oxide Free Radical Initiator from Femtosecond UV-Pump/Mid-IR-Probe Spectroscopy.

PubMed

Straub, Steffen; Lindner, Jörg; Vöhringer, Peter

2017-07-06

Femtosecond UV-pump/mid-infrared-probe spectroscopy was used to explore in detail the primary photochemical events of the free radical initiator, (2,4,6-trimethylbenzoyl)diphenylphosphine oxide, in liquid dichloromethane solution at room temperature. Following electronic excitation of its lowest excited singlet state, S 1 , the radical initiator undergoes an intersystem crossing to the triplet ground state, T 1 , with a time constant of 135 ps. A subsequent α-cleavage occurs from the triplet state with a time constant of 15 ps and yields a trimethylbenzoyl radical together with a diphenylphosphinoyl radical. Transient absorptions from the S 1 and T 1 states are observed that can be assigned to the P═O stretching mode and the symmetric in-plane deformation mode of the trimethylphenyl moiety of the radical initiator.
Characterization of the intramolecular transfer state of marine carotenoid fucoxanthin by femtosecond pump-probe spectroscopy.

PubMed

Kosumi, Daisuke; Fujii, Ritsuko; Sugisaki, Mitsuru; Oka, Naohiro; Iha, Masahiko; Hashimoto, Hideki

2014-07-01

Fucoxanthin, containing a carbonyl group in conjugation with its polyene backbone, is a naturally occurring pigment in marine organisms and is essential to the photosynthetic light-harvesting function in brown alga and diatom. Fucoxanthin exhibits optical characteristics attributed to an intramolecular charge transfer (ICT) state that arises in polar environments due to the presence of the carbonyl group. In this study, we report the spectroscopic properties of fucoxanthin in methanol (polar and protic solvent) observed by femtosecond pump-probe measurements in the near-infrared region, where transient absorption associated with the optically allowed S2 (1(1)B u (+) ) state and stimulated emission from the strongly coupled S1/ICT state were observed following one-photon excitation to the S2 state. The results showed that the amplitude of the stimulated emission of the S1/ICT state increased with decreasing excitation energy, demonstrating that the fucoxanthin form associated with the lower energy of the steady-state absorption exhibits stronger ICT character.
Femtosecond imaging of nonlinear acoustics in gold.

PubMed

Pezeril, Thomas; Klieber, Christoph; Shalagatskyi, Viktor; Vaudel, Gwenaelle; Temnov, Vasily; Schmidt, Oliver G; Makarov, Denys

2014-02-24

We have developed a high-sensitivity, low-noise femtosecond imaging technique based on pump-probe time-resolved measurements with a standard CCD camera. The approach used in the experiment is based on lock-in acquisitions of images generated by a femtosecond laser probe synchronized to modulation of a femtosecond laser pump at the same rate. This technique allows time-resolved imaging of laser-excited phenomena with femtosecond time resolution. We illustrate the technique by time-resolved imaging of the nonlinear reshaping of a laser-excited picosecond acoustic pulse after propagation through a thin gold layer. Image analysis reveals the direct 2D visualization of the nonlinear acoustic propagation of the picosecond acoustic pulse. Many ultrafast pump-probe investigations can profit from this technique because of the wealth of information it provides over a typical single diode and lock-in amplifier setup, for example it can be used to image ultrasonic echoes in biological samples.
Pump-probe experiments at the TEMPO beamline using the low-α operation mode of Synchrotron SOLEIL.

PubMed

Silly, Mathieu G; Ferté, Tom; Tordeux, Marie Agnes; Pierucci, Debora; Beaulieu, Nathan; Chauvet, Christian; Pressacco, Federico; Sirotti, Fausto; Popescu, Horia; Lopez-Flores, Victor; Tortarolo, Marina; Sacchi, Maurizio; Jaouen, Nicolas; Hollander, Philippe; Ricaud, Jean Paul; Bergeard, Nicolas; Boeglin, Christine; Tudu, Bharati; Delaunay, Renaud; Luning, Jan; Malinowski, Gregory; Hehn, Michel; Baumier, Cédric; Fortuna, Franck; Krizmancic, Damjan; Stebel, Luigi; Sergo, Rudi; Cautero, Giuseppe

2017-07-01

The SOLEIL synchrotron radiation source is regularly operated in special filling modes dedicated to pump-probe experiments. Among others, the low-α mode operation is characterized by shorter pulse duration and represents the natural bridge between 50 ps synchrotron pulses and femtosecond experiments. Here, the capabilities in low-α mode of the experimental set-ups developed at the TEMPO beamline to perform pump-probe experiments with soft X-rays based on photoelectron or photon detection are presented. A 282 kHz repetition-rate femtosecond laser is synchronized with the synchrotron radiation time structure to induce fast electronic and/or magnetic excitations. Detection is performed using a two-dimensional space resolution plus time resolution detector based on microchannel plates equipped with a delay line. Results of time-resolved photoelectron spectroscopy, circular dichroism and magnetic scattering experiments are reported, and their respective advantages and limitations in the framework of high-time-resolution pump-probe experiments compared and discussed.
Investigation of electronically excited indole relaxation dynamics via photoionization and fragmentation pump-probe spectroscopy.

PubMed

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

2014-07-28

The studies herein investigate the involvement of the low-lying (1)La and (1)Lb states with (1)ππ(*) character and the (1)πσ(*) 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 (1)πσ(*) state, is afforded. Through an extensive analysis of the TR-PES data presented here, it is deduced that the initial excitation of the (1)Bb state decays to the (1)La state on a timescale beyond the resolution of the current experimental setup. Relaxation proceeds on the (1)La state with an ultrafast decay constant (<100 femtoseconds (fs)) to the lower-lying (1)Lb 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 (1)πσ(*) state. TR-KER and TR-IY experiments, both specifically probing (1)πσ(*) dynamics, exhibit similar decay constants, further validating these observations.
Effect of nuclear motion on molecular high order harmonic pump probe spectroscopy.

PubMed

Bredtmann, Timm; Chelkowski, Szczepan; Bandrauk, André D

2012-11-26

We study pump-probe schemes for the real time observation of electronic motion on attosecond time scale in the molecular ion H(2)(+) and its heavier isotope T(2)(+) while these molecules dissociate on femtosecond time scale by solving numerically the non-Born-Oppenheimer time-dependent Schrödinger equation. The UV pump laser pulse prepares a coherent superposition of the three lowest lying quantum states and the time-delayed mid-infrared, intense few-femtosecond probe pulse subsequently generates molecular high-order harmonics (MHOHG) from this coherent electron-nuclear wavepacket (CENWP). Varying the pump-probe time delay by a few hundreds of attoseconds, the MHOHG signal intensity is shown to vary by orders of magnitude. Due to nuclear movement, the coherence of these two upper states and the ground state is lost after a few femtoseconds and the MHOHG intensity variations as function of pump-probe delay time are shown to be equal to the period of electron oscillation in the coherent superposition of the two upper dissociative quantum states. Although this electron oscillation period and hence the periodicity of the harmonic spectra are quite constant over a wide range of internuclear distances, a strong signature of nuclear motion is seen in the actual shapes and ways in which these spectra change as a function of pump-probe delay time, which is illustrated by comparison of the MHOHG spectra generated by the two isotopes H(2)(+) and T(2)(+). Two different regimes corresponding roughly to internuclear distances R < 4a(0) and R > 4a(0) are identified: For R < 4a(0), the intensity of a whole range of frequencies in the plateau region is decreased by orders of magnitude when the delay time is changed by a few hundred attoseconds whereas in the cutoff region the peaks in the MHOHG spectra are red-shifted with increasing pump-probe time delay. For R > 4a(0), on the other hand, the peaks both in the cutoff and plateau region are red-shifted with increasing delay times
Broadband sensitive pump-probe setup for ultrafast optical switching of photonic nanostructures and semiconductors.

PubMed

Euser, Tijmen G; Harding, Philip J; Vos, Willem L

2009-07-01

We describe an ultrafast time resolved pump-probe spectroscopy setup aimed at studying the switching of nanophotonic structures. Both femtosecond pump and probe pulses can be independently tuned over broad frequency range between 3850 and 21,050 cm(-1). A broad pump scan range allows a large optical penetration depth, while a broad probe scan range is crucial to study strongly photonic crystals. A new data acquisition method allows for sensitive pump-probe measurements, and corrects for fluctuations in probe intensity and pump stray light. We observe a tenfold improvement of the precision of the setup compared to laser fluctuations, allowing a measurement accuracy of better than DeltaR=0.07% in a 1 s measurement time. Demonstrations of the improved technique are presented for a bulk Si wafer, a three-dimensional Si inverse opal photonic bandgap crystal, and z-scan measurements of the two-photon absorption coefficient of Si, GaAs, and the three-photon absorption coefficient of GaP in the infrared wavelength range.
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.
Femtosecond-laser-induced nonadiabatic alignment in photoexcited pyrimidine

NASA Astrophysics Data System (ADS)

Li, Shuai; Ling, Fengzi; Wang, Yanmei; Long, Jinyou; Deng, Xulan; Jin, Bing; Zhang, Bing

2017-09-01

The rotational wave-packet dynamics in electronically excited pyrimidine induced by a femtosecond laser pulse at 321.5 nm has been studied by time-resolved mass spectroscopy and photoelectron velocity-map imaging. The rotational revival features at 81.3 ps, which are the direct manifestation of field-free nonadiabatic alignment, are clearly observed in both the time-dependent ion yields and photoelectron angular distributions. In particular, the out-of-phase recurrences in the parent-ion and fragment-ions transients indicate the different directions of the ionization transition-dipole moments for the generation of the parent ion and fragment ions. By tuning the polarization of the probe light parallel or perpendicular to that of the pump light, we demonstrate the potential application of nonadiabatic alignment to manipulate the branching ratio of photoionization products.
Ultrafast spatiotemporal relaxation dynamics of excited electrons in a metal nanostructure detected by femtosecond-SNOM.

PubMed

Li, Zhi; Yue, Song; Chen, Jianjun; Gong, Qihuang

2010-06-21

Ultrahigh spatiotemporal resolved pump-probe signal near a gold nano-slit is detected by femtosecond-SNOM. By employing two-color pump-probe configuration and probing at the interband transition wavelength of the gold, signal contributed by surface plasmon polariton is avoided and spatiotemporal evolvement of excited electrons is successfully observed. From the contrast decaying of the periodical distribution of the pump-probe signal, ultrafast diffusion of excited electrons with a time scale of a few hundred femtoseconds is clearly identified. For comparison, such phenomenon cannot be observed by the one-color pump-probe configuration.

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

2016-03-03

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.
Femtosecond optical switches by squarylium dye J-aggregates films

NASA Astrophysics Data System (ADS)

Pu, Lyong Sun

2003-01-01

Formation of Langmuir and spincoated films containing squarylium dye (SQ) J-aggregates and their femtosecond optical response are described. Pump-probe measurements show that saturable absorption of SQJ-films reveal ultrafast decay with time constants of 100-300 fs. We have applied SQJ-film to new femtosecond time-to-space conversion. A pump (gate) pulse and a train of four probe (signal) pulses were illuminated on the same area of the film in the direction of oblique and normal to the film-plane respectively. Demultiplexing operation for T bps optical signals was demonstrated with femtosecond nonlinear optical response of the SQJ-film.
Quantum Nuclear Dynamics Pumped and Probed by Ultrafast Polarization Controlled Steering of a Coherent Electronic State in LiH.

PubMed

Nikodem, Astrid; Levine, R D; Remacle, F

2016-05-19

The quantum wave packet dynamics following a coherent electronic excitation of LiH by an ultrashort, polarized, strong one-cycle infrared optical pulse is computed on several electronic states using a grid method. The coupling to the strong field of the pump and the probe pulses is included in the Hamiltonian used to solve the time-dependent Schrodinger equation. The polarization of the pump pulse allows us to control the localization in time and in space of the nonequilibrium coherent electronic motion and the subsequent nuclear dynamics. We show that transient absorption, resulting from the interaction of the total molecular dipole with the electric fields of the pump and the probe, is a very versatile probe of the different time scales of the vibronic dynamics. It allows probing both the ultrashort, femtosecond time scale of the electronic coherences as well as the longer dozens of femtoseconds time scales of the nuclear motion on the excited electronic states. The ultrafast beatings of the electronic coherences in space and in time are shown to be modulated by the different periods of the nuclear motion.
Tabletop Femtosecond VUV Photoionization and PEPICO Detection of Microreactor Pyrolysis Products

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

Couch, David E.; Buckingham, Grant T.; Baraban, Joshua H.

Here, we report the combination of tabletop vacuum ultraviolet photoionization with photoion--photoelectron coincidence spectroscopy for sensitive, isomer-specific detection of nascent products from a pyrolysis microreactor. Results on several molecules demonstrate two essential capabilities that are very straightforward to implement: the ability to differentiate isomers, and to distinguish thermal products from dissociative ionization. We derive vacuum ultraviolet light is from a commercial tabletop femtosecond laser system, allowing data to be collected at 10 kHz; this high repetition rate is critical for coincidence techniques. The photoion—photoelectron coincidence spectrometer uses the momentum of the ion to identify dissociative ionization events, and coincidence techniquesmore » to provide a photoelectron spectrum specific to each mass, which is used to distinguish different isomers. We also have used this spectrometer to detect the pyrolysis products that result from the thermal cracking of acetaldehyde, cyclohexene, and 2-butanol. The photoion—photoelectron spectrometer can detect and identify organic radicals and reactive intermediates that result from pyrolysis. Direct comparison of laboratory and synchrotron data illustrate the advantages and potential of this approach.« less
Tabletop Femtosecond VUV Photoionization and PEPICO Detection of Microreactor Pyrolysis Products

DOE PAGES

Couch, David E.; Buckingham, Grant T.; Baraban, Joshua H.; ...

2017-06-29

Here, we report the combination of tabletop vacuum ultraviolet photoionization with photoion--photoelectron coincidence spectroscopy for sensitive, isomer-specific detection of nascent products from a pyrolysis microreactor. Results on several molecules demonstrate two essential capabilities that are very straightforward to implement: the ability to differentiate isomers, and to distinguish thermal products from dissociative ionization. We derive vacuum ultraviolet light is from a commercial tabletop femtosecond laser system, allowing data to be collected at 10 kHz; this high repetition rate is critical for coincidence techniques. The photoion—photoelectron coincidence spectrometer uses the momentum of the ion to identify dissociative ionization events, and coincidence techniquesmore » to provide a photoelectron spectrum specific to each mass, which is used to distinguish different isomers. We also have used this spectrometer to detect the pyrolysis products that result from the thermal cracking of acetaldehyde, cyclohexene, and 2-butanol. The photoion—photoelectron spectrometer can detect and identify organic radicals and reactive intermediates that result from pyrolysis. Direct comparison of laboratory and synchrotron data illustrate the advantages and potential of this approach.« less
Femtosecond Beam Sources and Applications

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

Uesaka, Mitsuru

2004-12-07

Short particle beam science has been promoted by electron linac and radiation chemistry up to picoseconds. Recently, table-top TW laser enables several kinds of short particle beams and pump-and-probe analyses. 4th generation SR sources aim to generation and application of about 100 fs X-ray. Thus, femtosecond beam science has become one of the important field in advanced accelerator concepts. By using electron linac with photoinjector, about 200 fs single bunch and 3 fs multi-bunches are available. Tens femtoseconds monoenergetic electron bunch is expected by laser plasma cathode. Concerning the electron bunch diagnosis, we have seen remarkable progress in streak camera,more » coherent radiation spectroscopy, fluctuation method and E/O crystal method. Picosecond time-resolved pump-and-probe analysis by synchronizing electron linac and laser is now possible, but the timing jitter and drift due to several fluctuations in electronic devices and environment are still in picoseconds. On the other hand, the synchronization between laser and secondary beam is done passively by an optical beam-splitter in the system based on one TW laser. Therefore, the timing jitter and drift do not intrinsically exist there. The author believes that the femtosecond time-resolved pump-and-probe analysis must be initiated by the laser plasma beam sources. As to the applications, picosecond time-resolved system by electron photoinjector/linac and femtosecond laser are operating in more than 5 facilities for radiation chemistry in the world. Ti:Sapphire-laser-based repetitive pump-and-probe analysis started by time-resolved X-ray diffraction to visualize the atomic motion. Nd:Glass-laser-based single-shot analysis was performed to visualize the laser ablation via the single-shot ion imaging. The author expects that protein dynamics and ultrafast nuclear physics would be the next interesting targets. Monograph titled 'Femtosecond Beam Science' is published by Imperial College Press
Observation of femtosecond X-ray interactions with matter using an X-ray–X-ray pump–probe scheme

PubMed Central

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

2016-01-01

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 (∼1019 W/cm2) 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
A novel setup for femtosecond pump-repump-probe IR spectroscopy with few cycle CEP stable pulses.

PubMed

Bradler, Maximilian; Werhahn, Jasper C; Hutzler, Daniel; Fuhrmann, Simon; Heider, Rupert; Riedle, Eberhard; Iglev, Hristo; Kienberger, Reinhard

2013-08-26

We present a three-color mid-IR setup for vibrational pump-repump-probe experiments with a temporal resolution well below 100 fs and a freely selectable spectral resolution of 20 to 360 cm(-1) for the pump and repump. The usable probe range without optical realignment is 900 cm(-1). The experimental design employed is greatly simplified compared to the widely used setups, highly robust and includes a novel means for generation of tunable few-cycle pulses with stable carrier-envelope phase. A Ti:sapphire pump system operating with 1 kHz and a modest 150 fs pulse duration supplies the total pump energy of just 0.6 mJ. The good signal-to-noise ratio of the setup allows the determination of spectrally resolved transient probe changes smaller than 6·10(-5) OD at 130 time delays in just 45 minutes. The performance of the spectrometer is demonstrated with transient IR spectra and decay curves of HDO molecules in lithium nitrate trihydrate and ice and a first all MIR pump-repump-probe measurement.
Controlling nanoscale acoustic strains in silicon using chirped femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Tzianaki, E.; Bakarezos, M.; Tsibidis, G. D.; Petrakis, S.; Loukakos, P. A.; Kosmidis, C.; Tatarakis, M.; Papadogiannis, N. A.

2016-06-01

The influence of femtosecond laser pulse chirp on laser-generated longitudinal acoustic strains in Si (100) monocrystal substrates is studied. Degenerate femtosecond pump-probe transient reflectivity measurements are performed using a layered structure of thin Ti transducer film on an Si substrate. Experimental results show that acoustic strains, manifested as strong Brillouin oscillations, are more effectively induced when negatively chirped femtosecond laser pulses pump the transducer. These results are theoretically supported by a modified thermo-mechanical model based on the combination of a revised two-temperature model and elasticity theory that takes into account the instantaneous frequency of the chirped femtosecond laser pump pulses.
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

2016-03-15

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.
Low frequency dynamics of the nitrogenase MoFe protein via femtosecond pump probe spectroscopy - Observation of a candidate promoting vibration.

PubMed

Maiuri, Margherita; Delfino, Ines; Cerullo, Giulio; Manzoni, Cristian; Pelmenschikov, Vladimir; Guo, Yisong; Wang, Hongxin; Gee, Leland B; Dapper, Christie H; Newton, William E; Cramer, Stephen P

2015-12-01

We have used femtosecond pump-probe spectroscopy (FPPS) to study the FeMo-cofactor within the nitrogenase (N2ase) MoFe protein from Azotobacter vinelandii. A sub-20-fs visible laser pulse was used to pump the sample to an excited electronic state, and a second sub-10-fs pulse was used to probe changes in transmission as a function of probe wavelength and delay time. The excited protein relaxes to the ground state with a ~1.2ps time constant. With the short laser pulse we coherently excited the vibrational modes associated with the FeMo-cofactor active site, which are then observed in the time domain. Superimposed on the relaxation dynamics, we distinguished a variety of oscillation frequencies with the strongest band peaks at ~84, 116, 189, and 226cm(-1). Comparison with data from nuclear resonance vibrational spectroscopy (NRVS) shows that the latter pair of signals comes predominantly from the FeMo-cofactor. The frequencies obtained from the FPPS experiment were interpreted with normal mode calculations using both an empirical force field (EFF) and density functional theory (DFT). The FPPS data were also compared with the first reported resonance Raman (RR) spectrum of the N2ase MoFe protein. This approach allows us to outline and assign vibrational modes having relevance to the catalytic activity of N2ase. In particular, the 226cm(-1) band is assigned as a potential 'promoting vibration' in the H-atom transfer (or proton-coupled electron transfer) processes that are an essential feature of N2ase catalysis. The results demonstrate that high-quality room-temperature solution data can be obtained on the MoFe protein by the FPPS technique and that these data provide added insight to the motions and possible operation of this protein and its catalytic prosthetic group. Copyright © 2015 Elsevier Inc. All rights reserved.
Broadly tunable ultrafast pump-probe system operating at multi-kHz repetition rate

NASA Astrophysics Data System (ADS)

Grupp, Alexander; Budweg, Arne; Fischer, Marco P.; Allerbeck, Jonas; Soavi, Giancarlo; Leitenstorfer, Alfred; Brida, Daniele

2018-01-01

Femtosecond systems based on ytterbium as active medium are ideal for driving ultrafast optical parametric amplifiers in a broad frequency range. The excellent stability of the source and the repetition rate tunable to up to hundreds of kHz allow for the implementation of an advanced two-color pump probe setup with the capability to achieve excellent signal-to-noise performances with sub-10 fs temporal resolution.
Effect of Osmolytes on the Conformational Behavior of a Macromolecule in a Cytoplasm-like Crowded Environment: A Femtosecond Mid-IR Pump-Probe Spectroscopy Study.

PubMed

Kundu, Achintya; Verma, Pramod Kumar; Cho, Minhaeng

2018-02-15

Osmolytes found endogenously in almost all living beings play an important role in regulating cell volume under harsh environment. Here, to address the longstanding questions about the underlying mechanism of osmolyte effects, we use femtosecond mid-IR pump-probe spectroscopy with two different IR probes that are the OD stretching mode of HDO and the azido stretching mode of azido-derivatized poly(ethylene glycol) dimethyl ether (PEGDME). Our experimental results show that protecting osmolytes bind strongly with water molecules and dehydrate polymer surface, which results in promoting intramolecular interactions of the polymer. By contrast, urea behaves like water molecules without significantly disrupting water H-bonding network and favors extended and random-coil segments of the polymer chain by directly participating in solvation of the polymer. Our findings highlight the importance of direct interaction between urea and macromolecule, while protecting osmolytes indirectly affect the macromolecule through enhancing the water-osmolyte interaction in a crowded environment, which is the case that is often encountered in real biological systems.
Femtosecond laser pulse induced phase transition of Cr-doped Sb2Te1 films studied with a pump-probe system

NASA Astrophysics Data System (ADS)

Jiang, Minghui; Wang, Qing; Lei, Kai; Wang, Yang; Liu, Bo; Song, Zhitang

2016-10-01

The Femtosecond laser pulse induced phase transition dynamics of Cr-doped Sb2Te1 films was studied by real-time reflectivity measurements with a pump-probe system. It was found that crystallization of the as-deposited CrxSb2Te1 phase-change thin films exhibits a multi-stage process lasting for about 40ns.The time required for the multi-stage process seems to be not related to the contents of Cr element. The durations of the crystallization and amorphization processes are approximately the same. Doping Cr into Sb2Te1 thin film can improve its photo-thermal stability without obvious change in the crystallization rate. Optical images and image intensity cross sections are used to visualize the transformed regions. This work may provide further insight into the phase-change mechanism of CrxSb2Te1 under extra-non-equilibrium conditions and aid to develop new ultrafast phase-change memory materials.
Femtosecond pump-supercontinuum probe and transient lens spectroscopy of adonixanthin.

PubMed

Lenzer, Thomas; Schubert, Steffen; Ehlers, Florian; Lohse, Peter W; Scholz, Mirko; Oum, Kawon

2009-03-15

The ultrafast internal conversion (IC) dynamics of adonixanthin in organic solvents were studied by pump-supercontinuum probe (PSCP) and transient lens (TL) spectroscopy after photoexcitation to the S(2) state. Transient PSCP spectra in the range 344-768 nm provided the spectral evolution of the S(0)-->S(2) ground state bleach and S(1)-->S(n) excited state absorption. Time constants were tau(2) =115 and 111 fs for the S(2)-->S(1) IC and tau(1)=6.4 and 5.8 ps for the S(1)-->S(0) IC in acetone and methanol, respectively. There was only an insignificant polarity dependence of tau(1), underlining the negligible importance of intramolecular charge transfer (ICT) in the lowest-lying excited state of C(40) carotenoids with carbonyl substitution on the beta-ionone ring. A blueshift and a spectral narrowing of the S(1)-->S(n) ESA band, likely due to solvation dynamics, and formation of the adonixanthin radial cation at high pump energies via resonant two-photon ionization were found.
Excitons in Cuprous Oxide: Photoionization and Other Multiphoton Processes

NASA Astrophysics Data System (ADS)

Frazer, Nicholas Laszlo

In cuprous oxide (Cu2O), momentum from the absorption of two infrared photons to make an orthoexciton is conserved and detected through the photon component of a resulting mixed exciton/photon (quadrupole exciton polariton) state. I demonstrated that this process, which actually makes the photon momentum more precisely defined, is disrupted by photoionization of excitons. Some processes are known to affect exciton propagation in both the pump and exciton stages, such as phonon emission, exciton-exciton (Auger) scattering, and third harmonic generation. These processes alone were not able to explain all observed losses of excitons or all detected scattering products, which lead me to design an optical pump-probe experiment to measure the exciton photoionization cross section, which is (3.9+/-0.2) x 10-22 m2. This dissertation describes the synthesis of cuprous oxide crystals using oxidation of copper, crystallization from melt with the optical floating zone method, and annealing. The cuprous oxide crystals were characterized using time and space resolved luminescence, leading to the discovery of new defect properties. Selection rules and overall efficiency of third harmonic generation in these crystals were characterized. Exciton photoionization was demonstrated through the depletion of polariton luminescence by an optical probe, the production of phonon linked luminescence as a scattering product, temporal delay of the probe, and time resolved luminescence. The results are integrated with the traditional dynamical model of exciton densities. An additional investigation of copper/cuprous oxide/gold photovoltaic devices is appended.
Simultaneous generation of sub-5-femtosecond 400 nm and 800 nm pulses for attosecond extreme ultraviolet pump-probe spectroscopy.

PubMed

Chang, Hung-Tzu; Zürch, Michael; Kraus, Peter M; Borja, Lauren J; Neumark, Daniel M; Leone, Stephen R

2016-11-15

Few-cycle laser pulses with wavelengths centered at 400 nm and 800 nm are simultaneously obtained through wavelength separation of ultrashort, spectrally broadened Vis-NIR laser pulses spanning 350-1100 nm wavelengths. The 400 nm and 800 nm pulses are separately compressed, yielding pulses with 4.4 fs and 3.8 fs duration, respectively. The pulse energy exceeds 5 μJ for the 400 nm pulses and 750 μJ for the 800 nm pulses. Intense 400 nm few-cycle pulses have a broad range of applications in nonlinear optical spectroscopy, which include the study of photochemical dynamics, semiconductors, and photovoltaic materials on few-femtosecond to attosecond time scales. The ultrashort 400 nm few-cycle pulses generated here not only extend the spectral range of the optical pulse for NIR-XUV attosecond pump-probe spectroscopy but also pave the way for two-color, three-pulse, multidimensional optical-XUV spectroscopy experiments.
Femtosecond to picosecond transient effects in WSe 2 observed by pump-probe angle-resolved photoemission spectroscopy.

PubMed

Liu, Ro-Ya; Ogawa, Yu; Chen, Peng; Ozawa, Kenichi; Suzuki, Takeshi; Okada, Masaru; Someya, Takashi; Ishida, Yukiaki; Okazaki, Kozo; Shin, Shik; Chiang, Tai-Chang; Matsuda, Iwao

2017-11-22

Time-dependent responses of materials to an ultrashort optical pulse carry valuable information about the electronic and lattice dynamics; this research area has been widely studied on novel two-dimensional materials such as graphene, transition metal dichalcogenides (TMDs) and topological insulators (TIs). We report herein a time-resolved and angle-resolved photoemission spectroscopy (TRARPES) study of WSe 2 , a layered semiconductor of interest for valley electronics. The results for below-gap optical pumping reveal energy-gain and -loss Floquet replica valence bands that appear instantaneously in concert with the pump pulse. Energy shift, broadening, and complex intensity variation and oscillation at twice the phonon frequency for the valence bands are observed at time scales ranging from the femtosecond to the picosecond and beyond. The underlying physics is rich, including ponderomotive interaction, dressing of the electronic states, creation of coherent phonon pairs, and diffusion of charge carriers - effects operating at vastly different time domains.
Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

DOE PAGES

Savelyev, Evgeny; Boll, Rebecca; Bomme, Cedric; ...

2017-04-10

In pump-probe experiments employing a free-electron laser (FEL) in combination with a synchronized optical femtosecond laser, the arrival-time jitter between the FEL pulse and the optical laser pulse often severely limits the temporal resolution that can be achieved. Here, we present a pump-probe experiment on the UV-induced dissociation of 2,6-difluoroiodobenzene C 6H 3F 2I) molecules performed at the FLASH FEL that takes advantage of recent upgrades of the FLASH timing and synchronization system to obtain high-quality data that are not limited by the FEL arrival-time jitter. Here, we discuss in detail the necessary data analysis steps and describe the originmore » of the time-dependent effects in the yields and kinetic energies of the fragment ions that we observe in the experiment.« less
Note: Deep UV-pump THz-probe spectroscopy of the excess electron in water.

PubMed

Berger, Arian; Savolainen, Janne; Shalit, Andrey; Hamm, Peter

2017-06-28

In the work of Savolainen et al. [Nat. Chem. 6, 697 (2014)], we studied the excess (hydrated) electron in water with the help of transient THz spectroscopy, which is a sensitive probe of its delocalization length. In that work, we used laser pulses at 800 nm, 400 nm, and 267 nm for photoionization. While the detachment mechanism for 400 nm and 267 nm is complicated and requires a concerted nuclear rearrangement, we provided evidence that 800 nm pumping excites the excess electron directly and vertically into the conduction band, despite a highly nonlinear field-ionization process. In the present note, we extend that work to 200 nm pumping, which provides a much cleaner way to reach the conduction band. We show that the detachment pathways upon 200 nm and 800 nm pumping are in essence the same, as indicated by the same initial size of the electron wavefunction and the same time scales for the collapse of the wavefunction and geminate recombination.

Vibrational energy flow in photoactive yellow protein revealed by infrared pump-visible probe spectroscopy.

PubMed

Nakamura, Ryosuke; Hamada, Norio

2015-05-14

Vibrational energy flow in the electronic ground state of photoactive yellow protein (PYP) is studied by ultrafast infrared (IR) pump-visible probe spectroscopy. Vibrational modes of the chromophore and the surrounding protein are excited with a femtosecond IR pump pulse, and the subsequent vibrational dynamics in the chromophore are selectively probed with a visible probe pulse through changes in the absorption spectrum of the chromophore. We thus obtain the vibrational energy flow with four characteristic time constants. The vibrational excitation with an IR pulse at 1340, 1420, 1500, or 1670 cm(-1) results in ultrafast intramolecular vibrational redistribution (IVR) with a time constant of 0.2 ps. The vibrational modes excited through the IVR process relax to the initial ground state with a time constant of 6-8 ps in parallel with vibrational cooling with a time constant of 14 ps. In addition, upon excitation with an IR pulse at 1670 cm(-1), we observe the energy flow from the protein backbone to the chromophore that occurs with a time constant of 4.2 ps.
Diode-pumped Kerr-lens mode-locked femtosecond Yb:YAG ceramic laser

NASA Astrophysics Data System (ADS)

Zi-Ye, Gao; Jiang-Feng, Zhu; Ke, Wang; Jun-Li, Wang; Zhao-Hua, Wang; Zhi-Yi, Wei

2016-02-01

We experimentally demonstrated a diode-pumped Kerr-lens mode-locked femtosecond laser based on an Yb:YAG ceramic. Stable laser pulses with 97-fs duration, 2.8-nJ pulse energy, and 320-mW average power were obtained. The femtosecond oscillator operated at a central wavelength of 1049 nm and a repetition rate of 115 MHz. To the best of our knowledge, this is the first demonstration of a Kerr-lens mode-locked operation in a diode-pumped Yb:YAG ceramic laser with sub-100 fs pulse duration. Project supported by the National Major Scientific Instrument Development Project of China (Grant No. 2012YQ120047), the National Natural Science Foundation of China (Grant No. 61205130), and the Fundamental Research Funds for the Central Universities, China (Grant No. JB140502).
Effects of surface nanostructuring and impurity doping on ultrafast carrier dynamics of silicon photovoltaic cells: a pump-probe study

NASA Astrophysics Data System (ADS)

Chen, Tianyu; Nam, Yoon-Ho; Wang, Xinke; Han, Peng; Sun, Wenfeng; Feng, Shengfei; Ye, Jiasheng; Song, Jae-Won; Lee, Jung-Ho; Zhang, Chao; Zhang, Yan

2018-01-01

We present femtosecond optical pump-terahertz probe studies on the ultrafast dynamical processes of photo-generated charge carriers in silicon photovoltaic cells with various nanostructured surfaces and doping densities. The pump-probe measurements provide direct insight on the lifetime of photo-generated carriers, frequency-dependent complex dielectric response along with photoconductivity of silicon photovoltaic cells excited by optical pump pulses. A lifetime of photo-generated carriers of tens of nanosecond is identified from the time-dependent pump-induced attenuation of the terahertz transmission. In addition, we find a large value of the imaginary part of the dielectric function and of the real part of the photoconductivity in silicon photovoltaic cells with micron length nanowires. We attribute these findings to the result of defect-enhanced electron-photon interactions. Moreover, doping densities of phosphorous impurities in silicon photovoltaic cells are also quantified using the Drude-Smith model with our measured frequency-dependent complex photoconductivities.
Pump-probe nonlinear phase dispersion spectroscopy.

PubMed

Robles, Francisco E; Samineni, Prathyush; Wilson, Jesse W; Warren, Warren S

2013-04-22

Pump-probe microscopy is an imaging technique that delivers molecular contrast of pigmented samples. Here, we introduce pump-probe nonlinear phase dispersion spectroscopy (PP-NLDS), a method that leverages pump-probe microscopy and spectral-domain interferometry to ascertain information from dispersive and resonant nonlinear effects. PP-NLDS extends the information content to four dimensions (phase, amplitude, wavelength, and pump-probe time-delay) that yield unique insight into a wider range of nonlinear interactions compared to conventional methods. This results in the ability to provide highly specific molecular contrast of pigmented and non-pigmented samples. A theoretical framework is described, and experimental results and simulations illustrate the potential of this method. Implications for biomedical imaging are discussed.
Pump-probe nonlinear phase dispersion spectroscopy

PubMed Central

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

2013-01-01

Pump-probe microscopy is an imaging technique that delivers molecular contrast of pigmented samples. Here, we introduce pump-probe nonlinear phase dispersion spectroscopy (PP-NLDS), a method that leverages pump-probe microscopy and spectral-domain interferometry to ascertain information from dispersive and resonant nonlinear effects. PP-NLDS extends the information content to four dimensions (phase, amplitude, wavelength, and pump-probe time-delay) that yield unique insight into a wider range of nonlinear interactions compared to conventional methods. This results in the ability to provide highly specific molecular contrast of pigmented and non-pigmented samples. A theoretical framework is described, and experimental results and simulations illustrate the potential of this method. Implications for biomedical imaging are discussed. PMID:23609646
Femtosecond Laser--Pumped Source of Entangled Photons for Quantum Cryptography Applications

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

Pan, D.; Donaldson, W.; Sobolewski, R.

2007-07-31

We present an experimental setup for generation of entangled-photon pairs via spontaneous parametric down-conversion, based on the femtosecond-pulsed laser. Our entangled-photon source utilizes a 76-MHz-repetition-rate, 100-fs-pulse-width, mode-locked, ultrafast femtosecond laser, which can produce, on average, more photon pairs than a cw laser of an equal pump power. The resulting entangled pairs are counted by a pair of high-quantum-efficiency, single-photon, silicon avalanche photodiodes. Our apparatus is intended as an efficient source/receiver system for the quantum communications and quantum cryptography applications.
Femtosecond OPO based on MgO:PPLN synchronously pumped by a 532 nm fiber laser

NASA Astrophysics Data System (ADS)

Cao, Jianjun; Shen, Dongyi; Zheng, Yuanlin; Feng, Yaming; Kong, Yan; Wan, Wenjie

2017-05-01

With the rapid progress in fiber technologies, femtosecond fiber lasers, which are compact, cost-effective and stable, have been developed and are commercially available. Studies of optical parametric oscillators (OPOs) pumped by this type of laser are demanding. Here we report a femtosecond optical parametric oscillator (OPO) at 79.6 MHz repetition rate based on MgO-doped periodically poled LiNbO3 (MgO:PPLN), synchronously pumped by the integrated second harmonic radiation of a femtosecond fiber laser at 532 nm. The signal delivered by the single resonant OPO is continuously tunable from 757 to 797 nm by tuning the crystal temperature in a poling period of 7.7 μ \\text{m} . The output signal shows good beam quality in TEM00 mode profile with pulse duration of 206 fs at 771 nm. Maximum output signal power of 71 mW is obtained for a pump power of 763 mW and a low pumping threshold of 210 mW is measured. Moreover, grating tuning and cavity length tuning of the signal wavelength are also investigated.
Traveling-wave laser-produced-plasma energy source for photoionization laser pumping and lasers incorporating said

DOEpatents

Sher, Mark H.; Macklin, John J.; Harris, Stephen E.

1989-09-26

A traveling-wave, laser-produced-plasma, energy source used to obtain single-pass gain saturation of a photoionization pumped laser. A cylindrical lens is used to focus a pump laser beam to a long line on a target. Grooves are cut in the target to present a surface near normal to the incident beam and to reduce the area, and hence increase the intensity and efficiency, of plasma formation.
Dynamics of spallation during femtosecond laser ablation studied by time-resolved reflectivity with double pump pulses

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

Kumada, Takayuki, E-mail: kumada.takayuki@jaea.go.jp; Otobe, Tomohito; Nishikino, Masaharu

2016-01-04

The dynamics of photomechanical spallation during femtosecond laser ablation of fused silica was studied by time-resolved reflectivity with double pump pulses. Oscillation of reflectivity was caused by interference between the probe pulses reflected at the sample surface and the spallation layer, and was enhanced when the surface was irradiated with the second pump pulse within a time interval, Δτ, of several picoseconds after the first pump pulse. However, as Δτ was increased, the oscillation amplitude decreased with an exponential decay time of 10 ps. The oscillation disappeared when Δτ exceeded 20 ps. This result suggests that the formation time of the spallationmore » layer is approximately 10 ps. A second pump pulse with Δτ shorter than 10 ps excites the bulk sample. The spallation layer that is photo-excited by the first and second pump pulses is separated afterward. In contrast, a pulse with Δτ longer than the formation time excites and breaks up the spallation layer that has already been separated from the bulk. The formation time of the spallation layer, as determined in this experiment, is attributed to the characteristic time of the mechanical equilibration corresponding to the thickness divided by the sound velocity of the photo-excited layer.« less
Diode-pumped mode-locked femtosecond Tm:CLNGG disordered crystal laser.

PubMed

Ma, J; Xie, G Q; Gao, W L; Yuan, P; Qian, L J; Yu, H H; Zhang, H J; Wang, J Y

2012-04-15

A diode-end-pumped passively mode-locked femtosecond Tm-doped calcium lithium niobium gallium garnet (Tm:CLNGG) disordered crystal laser was demonstrated for the first time to our knowledge. With a 790 nm laser diode pumping, stable CW mode-locking operation was obtained by using a semiconductor saturable absorber mirror. The disordered crystal laser generated mode-locked pulses as short as 479 fs, with an average output power of 288 mW, and repetition rate of 99 MHz in 2 μm spectral region. © 2012 Optical Society of America
Analysis of a measurement scheme for ultrafast hole dynamics by few femtosecond resolution X-ray pump-probe Auger spectroscopy.

PubMed

Cooper, Bridgette; Kolorenč, Přemysl; Frasinski, Leszek J; Averbukh, Vitali; Marangos, Jon P

2014-01-01

Ultrafast hole dynamics created in molecular systems as a result of sudden ionisation is the focus of much attention in the field of attosecond science. Using the molecule glycine we show through ab initio simulations that the dynamics of a hole, arising from ionisation in the inner valence region, evolves with a timescale appropriate to be measured using X-ray pulses from the current generation of SASE free electron lasers. The examined pump-probe scheme uses X-rays with photon energy below the K edge of carbon (275-280 eV) that will ionise from the inner valence region. A second probe X-ray at the same energy can excite an electron from the core to fill the vacancy in the inner-valence region. The dynamics of the inner valence hole can be tracked by measuring the Auger electrons produced by the subsequent refilling of the core hole as a function of pump-probe delay. We consider the feasibility of the experiment and include numerical simulation to support this analysis. We discuss the potential for all X-ray pump-X-ray probe Auger spectroscopy measurements for tracking hole migration.
Investigating radiation induced damage processes with femtosecond x-ray pulses (Conference Presentation)

NASA Astrophysics Data System (ADS)

Song, Changyong

2017-05-01

Interest in high-resolution structure investigation has been zealous, especially with the advent of X-ray free electron lasers (XFELs). The intense and ultra-short X-ray laser pulses ( 10 GW) pave new routes to explore structures and dynamics of single macromolecules, functional nanomaterials and complex electronic materials. In the last several years, we have developed XFEL single-shot diffraction imaging by probing ultrafast phase changes directly. Pump-probe single-shot imaging was realized by synchronizing femtosecond (<10 fs in FWHM) X-ray laser (probe) with femtosecond (50 fs) IR laser (pump) at better than 1 ps resolution. Nanoparticles under intense fs-laser pulses were investigated with fs XFEL pulses to provide insight into the irreversible particle damage processes with nanoscale resolution. Research effort, introduced, aims to extend the current spatio-temporal resolution beyond the present limit. We expect this single-shot dynamic imaging to open new science opportunity with XFELs.
Femtosecond pulses generated from a synchronously pumped chromium-doped forsterite laser

NASA Technical Reports Server (NTRS)

Seas, A.; Petricevic, V.; Alfano, R. R.

1993-01-01

Kerr lens mode-locking (KLM) has become a standard method to produce femtosecond pulses from tunable solid state lasers. High power inside the laser resonator propagating through the laser-medium with nonlinear index of refraction, coupled with the stability conditions of the laser modes in the resonator, result in a passive amplitude modulation which explains the mechanism for pulse shortening. Recently, chromium doped forsterite was shown to exhibit similar pulse behavior. A successful attempt to generate femtosecond pulses from a synchronously pumped chromium-doped forsterite laser with intracavity dispersion compensation is reported. Stable, transform limited pulses with duration of 105 fs were routinely generated, tunable between 1240 to 1270 nm.
Pump-probe Kelvin-probe force microscopy: Principle of operation and resolution limits

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

Murawski, J.; Graupner, T.; Milde, P., E-mail: peter.milde@tu-dresden.de

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.
Dual echelon femtosecond single-shot spectroscopy

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

Shin, Taeho; Wolfson, Johanna W.; Teitelbaum, Samuel W.

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-noisemore » 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.« less
Femtosecond pump/supercontinuum-probe spectroscopy: optimized setup and signal analysis for single-shot spectral referencing.

PubMed

Dobryakov, A L; Kovalenko, S A; Weigel, A; Pérez-Lustres, J L; Lange, J; Müller, A; Ernsting, N P

2010-11-01

A setup for pump/supercontinuum-probe spectroscopy is described which (i) is optimized to cancel fluctuations of the probe light by single-shot referencing, and (ii) extends the probe range into the near-uv (1000-270 nm). Reflective optics allow 50 μm spot size in the sample and upon entry into two separate spectrographs. The correlation γ(same) between sample and reference readings of probe light level at every pixel exceeds 0.99, compared to γ(consec)<0.92 reported for consecutive referencing. Statistical analysis provides the confidence interval of the induced optical density, ΔOD. For demonstration we first examine a dye (Hoechst 33258) bound in the minor groove of double-stranded DNA. A weak 1.1 ps spectral oscillation in the fluorescence region, assigned to DNA breathing, is shown to be significant. A second example concerns the weak vibrational structure around t=0 which reflects stimulated Raman processes. With 1% fluctuations of probe power, baseline noise for a transient absorption spectrum becomes 25 μOD rms in 1 s at 1 kHz, allowing to record resonance Raman spectra of flavine adenine dinucleotide in the S(0) and S(1) state.
Highly efficient and high-power diode-pumped femtosecond Yb:LYSO laser

NASA Astrophysics Data System (ADS)

Tian, Wenlong; Wang, Zhaohua; Zhu, Jiangfeng; Zheng, Lihe; Xu, Jun; Wei, Zhiyi

2017-04-01

A diode-pumped high-power femtosecond Yb:LYSO laser with high efficiency is demonstrated. With a semiconductor saturable absorber mirror for passive mode-locking and a Gires-Tournois interferometer mirror for intracavity dispersion compensation, stable mode-locking pulses of 297 fs duration at 1042 nm were obtained. The maximum average power of 3.07 W was realized under 5.17 W absorbed pump power, corresponding to as high as 59.4% opt-opt efficiency. The single pulse energy and peak power are about 35.5 nJ and 119.5 kW, respectively.
Femtosecond Lasers with Diode Pumping for Using in Precision Metrology and Optical Fiber Communication

DTIC Science & Technology

2008-11-24

folding angle of 32° to compensate astigmatism of the Brewster -cut Cr:F crystal. The gain crystal was 17 mm long and introduced positive group-delay...accomplished. For complete stabilization of the femtosecond comb one needs to control its absolute frequency. To realize this we use either angle - tilted...Kerr- lens mode-locking. To the best of our knowledge there is no published works on KLM ytterbium femtosecond lasers with multimode pumping. Stable
X-ray Pump–Probe Investigation of Charge and Dissociation Dynamics in Methyl Iodine Molecule

DOE PAGES

Fang, Li; Xiong, Hui; Kukk, Edwin; ...

2017-05-19

Molecular dynamics is of fundamental interest in natural science research. The capability of investigating molecular dynamics is one of the various motivations for ultrafast optics. Here, we present our investigation of photoionization and nuclear dynamics in methyl iodine (CH 3I) molecule with an X-ray pump X-ray probe scheme. The pump–probe experiment was realized with a two-mirror X-ray split and delay apparatus. Time-of-flight mass spectra at various pump–probe delay times were recorded to obtain the time profile for the creation of high charge states via sequential ionization and for molecular dissociation. We observed high charge states of atomic iodine up tomore » 29+, and visualized the evolution of creating these high atomic ion charge states, including their population suppression and enhancement as the arrival time of the second X-ray pulse was varied. We also show the evolution of the kinetics of the high charge states upon the timing of their creation during the ionization-dissociation coupled dynamics. We demonstrate the implementation of X-ray pump–probe methodology for investigating X-ray induced molecular dynamics with femtosecond temporal resolution. The results indicate the footprints of ionization that lead to high charge states, probing the long-range potential curves of the high charge states.« less
Broad-Band Pump-Probe Spectroscopy Quantifies Ultrafast Solvation Dynamics of Proteins and Molecules.

PubMed

Jumper, Chanelle C; Arpin, Paul C; Turner, Daniel B; McClure, Scott D; Rafiq, Shahnawaz; Dean, Jacob C; Cina, Jeffrey A; Kovac, Philip A; Mirkovic, Tihana; Scholes, Gregory D

2016-11-17

In this work, we demonstrate the use of broad-band pump-probe spectroscopy to measure femtosecond solvation dynamics. We report studies of a rhodamine dye in methanol and cryptophyte algae light-harvesting proteins in aqueous suspension. Broad-band impulsive excitation generates a vibrational wavepacket that oscillates on the excited-state potential energy surface, destructively interfering with itself at the minimum of the surface. This destructive interference gives rise to a node at a certain probe wavelength that varies with time. This reveals the Gibbs free-energy changes of the excited-state potential energy surface, which equates to the solvation time correlation function. This method captures the inertial solvent response of water (∼40 fs) and the bimodal inertial response of methanol (∼40 and ∼150 fs) and reveals how protein-buried chromophores are sensitive to the solvent dynamics inside and outside of the protein environment.

Effective temperature of an ultracold electron source based on near-threshold photoionization.

PubMed

Engelen, W J; Smakman, E P; Bakker, D J; Luiten, O J; Vredenbregt, E J D

2014-01-01

We present a detailed description of measurements of the effective temperature of a pulsed electron source, based on near-threshold photoionization of laser-cooled atoms. The temperature is determined by electron beam waist scans, source size measurements with ion beams, and analysis with an accurate beam line model. Experimental data is presented for the source temperature as a function of the wavelength of the photoionization laser, for both nanosecond and femtosecond ionization pulses. For the nanosecond laser, temperatures as low as 14 ± 3 K were found; for femtosecond photoionization, 30 ± 5 K is possible. With a typical source size of 25 μm, this results in electron bunches with a relative transverse coherence length in the 10⁻⁴ range and an emittance of a few nm rad. © 2013 Elsevier B.V. All rights reserved.
Weak-field few-femtosecond VUV photodissociation dynamics of water isotopologues

NASA Astrophysics Data System (ADS)

Baumann, Arne; Bazzi, Sophia; Rompotis, Dimitrios; Schepp, Oliver; Azima, Armin; Wieland, Marek; Popova-Gorelova, Daria; Vendrell, Oriol; Santra, Robin; Drescher, Markus

2017-07-01

We present a joint experimental and theoretical study of the VUV-induced dynamics of H2O and its deuterated isotopologues in the first excited state (A ˜1B1 ) utilizing a VUV-pump VUV-probe scheme combined with a b initio classical trajectory calculations. 16-fs VUV pulses centered at 161 nm created by fifth-order harmonic generation are employed for single-shot pump-probe measurements. Combined with a precise determination of the VUV pulses' temporal profile, they provide the necessary temporal resolution to elucidate sub-10-fs dissociation dynamics in the 1+1 photon ionization time window. Ionization with a single VUV photon complements established strong-field ionization schemes by disclosing the molecular dynamics under perturbative conditions. Kinetic isotope effects derived from the pump-probe experiment are found to be in agreement with our by ab initio classical trajectory calculations, taking into account photoionization cross sections for the ground and first excited state of the water cation.
Sub-100 fs pump-probe spectroscopy of Single Wall Carbon Nanotubes with a 100 MHz Er-fiber laser system.

PubMed

Gambetta, A; Galzerano, G; Rozhin, A G; Ferrari, A C; Ramponi, R; Laporta, P; Marangoni, M

2008-08-04

An extremely compact and versatile near-infrared two-color femtosecond pump-probe spectroscopy apparatus based on an amplified Erfiber laser system is presented and applied to the characterization of the relaxation dynamics of single-wall carbon nanotubes with fundamental absorption in the 2 microm spectral region. By implementing a fast-scan technique, dynamics as long as 3 ps are acquired in 5 s with a relative sensitivity of 10(-4) and a temporal resolution below 100 fs at 2 microm.
Pump-Probe Noise Spectroscopy of Molecular Junctions.

PubMed

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

2015-02-05

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.
Femtosecond transient absorption, Raman, and electrochemistry studies of tetrasulfonated copper phthalocyanine in water solutions.

PubMed

Abramczyk, H; Brozek-Płuska, B; Kurczewski, K; Kurczewska, M; Szymczyk, I; Krzyczmonik, P; Błaszczyk, T; Scholl, H; Czajkowski, W

2006-07-20

Ultrafast time-resolved electronic spectra of the primary events induced in the copper tetrasulfonated phthalocyanine Cu(tsPc)4-) in aqueous solution has been measured by femtosecond pump-probe transient absorption spectroscopy. The primary events initiated by the absorption of a photon occurring within the femtosecond time scale are discussed on the basis of the electron transfer mechanism between the adjacent phthalocyanine rings proposed recently in our laboratory. The femtosecond transient absorption results are compared with the low temperature emission spectra obtained with Raman spectroscopy and the voltammetric curves.
Split-probe hybrid femtosecond/picosecond rotational CARS for time-domain measurement of S-branch Raman linewidths within a single laser shot.

PubMed

Patterson, Brian D; Gao, Yi; Seeger, Thomas; Kliewer, Christopher J

2013-11-15

We introduce a multiplex technique for the single-laser-shot determination of S-branch Raman linewidths with high accuracy and precision by implementing hybrid femtosecond (fs)/picosecond (ps) rotational coherent anti-Stokes Raman spectroscopy (CARS) with multiple spatially and temporally separated probe beams derived from a single laser pulse. The probe beams scatter from the rotational coherence driven by the fs pump and Stokes pulses at four different probe pulse delay times spanning 360 ps, thereby mapping collisional coherence dephasing in time for the populated rotational levels. The probe beams scatter at different folded BOXCARS angles, yielding spatially separated CARS signals which are collected simultaneously on the charge coupled device camera. The technique yields a single-shot standard deviation (1σ) of less than 3.5% in the determination of Raman linewidths and the average linewidth values obtained for N(2) are within 1% of those previously reported. The presented technique opens the possibility for correcting CARS spectra for time-varying collisional environments in operando.
Time-gated real-time pump-probe imaging spectroscopy

NASA Astrophysics Data System (ADS)

Ferrari, Raffaele; D'Andrea, Cosimo; Bassi, Andrea; Valentini, Gianluca; Cubeddu, Rinaldo

2007-07-01

An experimental technique which allows one to perform pump-probe transient absorption spectroscopy in real-time is an important tool to study irreversible processes. This is particularly interesting in the case of biological samples which easily deteriorate upon exposure to light pulses, with the formation of permanent photoproducts and structural changes. In particular pump-probe spectroscopy can provide fundamental information for the design of optical chromophores. In this work a real-time pump-probe imaging spectroscopy system has been realized and we have explored the possibility to further reduce the number of laser pulses by using a time-gated camera. We believe that the use of a time-gated camera can provide an important step towards the final goal of pump-probe single shot spectroscopy.
Three-dimensional wide-field pump-probe structured illumination microscopy

PubMed Central

Kim, Yang-Hyo; So, Peter T.C.

2017-01-01

We propose a new structured illumination scheme for achieving depth resolved wide-field pump-probe microscopy with sub-diffraction limit resolution. By acquiring coherent pump-probe images using a set of 3D structured light illumination patterns, a 3D super-resolution pump-probe image can be reconstructed. We derive the theoretical framework to describe the coherent image formation and reconstruction scheme for this structured illumination pump-probe imaging system and carry out numerical simulations to investigate its imaging performance. The results demonstrate a lateral resolution improvement by a factor of three and providing 0.5 µm level axial optical sectioning. PMID:28380860
Irreversible transformation of ferromagnetic ordered stripe domains in single-shot infrared-pump/resonant-x-ray-scattering-probe experiments

NASA Astrophysics Data System (ADS)

Bergeard, Nicolas; Schaffert, Stefan; López-Flores, Víctor; Jaouen, Nicolas; Geilhufe, Jan; Günther, Christian M.; Schneider, Michael; Graves, Catherine; Wang, Tianhan; Wu, Benny; Scherz, Andreas; Baumier, Cédric; Delaunay, Renaud; Fortuna, Franck; Tortarolo, Marina; Tudu, Bharati; Krupin, Oleg; Minitti, Michael P.; Robinson, Joe; Schlotter, William F.; Turner, Joshua J.; Lüning, Jan; Eisebitt, Stefan; Boeglin, Christine

2015-02-01

The evolution of a magnetic domain structure upon excitation by an intense, femtosecond infrared (IR) laser pulse has been investigated using single-shot based time-resolved resonant x-ray scattering at the x-ray free electron laser LCLS. A well-ordered stripe domain pattern as present in a thin CoPd alloy film has been used as a prototype magnetic domain structure for this study. The fluence of the IR laser pump pulse was sufficient to lead to an almost complete quenching of the magnetization within the ultrafast demagnetization process taking place within the first few hundreds of femtoseconds following the IR laser pump pulse excitation. On longer time scales this excitation gave rise to subsequent irreversible transformations of the magnetic domain structure. Under our specific experimental conditions, it took about 2 ns before the magnetization started to recover. After about 5 ns the previously ordered stripe domain structure had evolved into a disordered labyrinth domain structure. Surprisingly, we observe after about 7 ns the occurrence of a partially ordered stripe domain structure reoriented into a novel direction. It is this domain structure in which the sample's magnetization stabilizes as revealed by scattering patterns recorded long after the initial pump-probe cycle. Using micromagnetic simulations we can explain this observation based on changes of the magnetic anisotropy going along with heat dissipation in the film.
Strong and Long Makes Short: Strong-Pump Strong-Probe Spectroscopy.

PubMed

Gelin, Maxim F; Egorova, Dassia; Domcke, Wolfgang

2011-01-20

We propose a new time-domain spectroscopic technique that is based on strong pump and probe pulses. The strong-pump strong-probe (SPSP) technique provides temporal resolution that is not limited by the durations of the pump and probe pulses. By numerically exact simulations of SPSP signals for a multilevel vibronic model, we show that the SPSP signals exhibit electronic and vibrational beatings on time scales which are significantly shorter than the pulse durations. This suggests the possible application of SPSP spectroscopy for the real-time investigation of molecular processes that cannot be temporally resolved by pump-probe spectroscopy with weak pump and probe pulses.
Photoisomerization and photoionization of the photoactive yellow protein chromophore in solution.

PubMed

Larsen, Delmar S; Vengris, Mikas; van Stokkum, Ivo H M; van der Horst, Michael A; de Weerd, Frank L; Hellingwerf, Klaas J; van Grondelle, Rienk

2004-04-01

Dispersed pump-dump-probe spectroscopy has the ability to characterize and identify the underlying ultrafast dynamical processes in complicated chemical and biological systems. This technique builds on traditional pump-probe techniques by exploring both ground- and excited-state dynamics and characterizing the connectivity between constituent transient states. We have used the dispersed pump-dump-probe technique to investigate the ground-state dynamics and competing excited-state processes in the excitation-induced ultrafast dynamics of thiomethyl p-coumaric acid, a model chromophore for the photoreceptor photoactive yellow protein. Our results demonstrate the parallel formation of two relaxation pathways (with multiple transient states) that jointly lead to two different types of photochemistry: cis-trans isomerization and detachment of a hydrated electron. The relative transition rates and quantum yields of both pathways have been determined. We find that the relaxation of the photoexcited chromophores involves multiple, transient ground-state intermediates and the chromophore in solution does not generate persistent photoisomerized products, but instead undergoes photoionization resulting in the generation of detached electrons and radicals. These results are of great value in interpreting the more complex dynamical changes in the optical properties of the photoactive yellow protein.
Photoisomerization and Photoionization of the Photoactive Yellow Protein Chromophore in Solution

PubMed Central

Larsen, Delmar S.; Vengris, Mikas; van Stokkum, Ivo H. M.; van der Horst, Michael A.; de Weerd, Frank L.; Hellingwerf, Klaas J.; van Grondelle, Rienk

2004-01-01

Dispersed pump-dump-probe spectroscopy has the ability to characterize and identify the underlying ultrafast dynamical processes in complicated chemical and biological systems. This technique builds on traditional pump-probe techniques by exploring both ground- and excited-state dynamics and characterizing the connectivity between constituent transient states. We have used the dispersed pump-dump-probe technique to investigate the ground-state dynamics and competing excited-state processes in the excitation-induced ultrafast dynamics of thiomethyl p-coumaric acid, a model chromophore for the photoreceptor photoactive yellow protein. Our results demonstrate the parallel formation of two relaxation pathways (with multiple transient states) that jointly lead to two different types of photochemistry: cis-trans isomerization and detachment of a hydrated electron. The relative transition rates and quantum yields of both pathways have been determined. We find that the relaxation of the photoexcited chromophores involves multiple, transient ground-state intermediates and the chromophore in solution does not generate persistent photoisomerized products, but instead undergoes photoionization resulting in the generation of detached electrons and radicals. These results are of great value in interpreting the more complex dynamical changes in the optical properties of the photoactive yellow protein. PMID:15041690
Pump-Probe Fragmentation Action Spectroscopy: A Powerful Tool to Unravel Light-Induced Processes in Molecular Photocatalysts.

PubMed

Imanbaew, Dimitri; Lang, Johannes; Gelin, Maxim F; Kaufhold, Simon; Pfeffer, Michael G; Rau, Sven; Riehn, Christoph

2017-05-08

We present a proof of concept that ultrafast dynamics combined with photochemical stability information of molecular photocatalysts can be acquired by electrospray ionization mass spectrometry combined with time-resolved femtosecond laser spectroscopy in an ion trap. This pump-probe "fragmentation action spectroscopy" gives straightforward access to information that usually requires high purity compounds and great experimental efforts. Results of gas-phase studies on the electronic dynamics of two supramolecular photocatalysts compare well to previous findings in solution and give further evidence for a directed electron transfer, a key process for photocatalytic hydrogen generation. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Dual-wavelength pump-probe microscopy analysis of melanin composition

NASA Astrophysics Data System (ADS)

Thompson, Andrew; Robles, Francisco E.; Wilson, Jesse W.; Deb, Sanghamitra; Calderbank, Robert; Warren, Warren S.

2016-11-01

Pump-probe microscopy is an emerging technique that provides detailed chemical information of absorbers with sub-micrometer spatial resolution. Recent work has shown that the pump-probe signals from melanin in human skin cancers correlate well with clinical concern, but it has been difficult to infer the molecular origins of these differences. Here we develop a mathematical framework to describe the pump-probe dynamics of melanin in human pigmented tissue samples, which treats the ensemble of individual chromophores that make up melanin as Gaussian absorbers with bandwidth related via Frenkel excitons. Thus, observed signals result from an interplay between the spectral bandwidths of the individual underlying chromophores and spectral proximity of the pump and probe wavelengths. The model is tested using a dual-wavelength pump-probe approach and a novel signal processing method based on gnomonic projections. Results show signals can be described by a single linear transition path with different rates of progress for different individual pump-probe wavelength pairs. Moreover, the combined dual-wavelength data shows a nonlinear transition that supports our mathematical framework and the excitonic model to describe the optical properties of melanin. The novel gnomonic projection analysis can also be an attractive generic tool for analyzing mixing paths in biomolecular and analytical chemistry.
Dual-wavelength pump-probe microscopy analysis of melanin composition

PubMed Central

Thompson, Andrew; Robles, Francisco E.; Wilson, Jesse W.; Deb, Sanghamitra; Calderbank, Robert; Warren, Warren S.

2016-01-01

Pump-probe microscopy is an emerging technique that provides detailed chemical information of absorbers with sub-micrometer spatial resolution. Recent work has shown that the pump-probe signals from melanin in human skin cancers correlate well with clinical concern, but it has been difficult to infer the molecular origins of these differences. Here we develop a mathematical framework to describe the pump-probe dynamics of melanin in human pigmented tissue samples, which treats the ensemble of individual chromophores that make up melanin as Gaussian absorbers with bandwidth related via Frenkel excitons. Thus, observed signals result from an interplay between the spectral bandwidths of the individual underlying chromophores and spectral proximity of the pump and probe wavelengths. The model is tested using a dual-wavelength pump-probe approach and a novel signal processing method based on gnomonic projections. Results show signals can be described by a single linear transition path with different rates of progress for different individual pump-probe wavelength pairs. Moreover, the combined dual-wavelength data shows a nonlinear transition that supports our mathematical framework and the excitonic model to describe the optical properties of melanin. The novel gnomonic projection analysis can also be an attractive generic tool for analyzing mixing paths in biomolecular and analytical chemistry. PMID:27833147
High-repetition-rate setup for pump-probe time-resolved XUV-IR experiments employing ion and electron momentum imaging

NASA Astrophysics Data System (ADS)

Pathak, Shashank; Robatjazi, Seyyed Javad; Wright Lee, Pearson; Raju Pandiri, Kanaka; Rolles, Daniel; Rudenko, Artem

2017-04-01

J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan KS, USA We report on the development of a versatile experimental setup for XUV-IR pump-probe experiments using a 10 kHz high-harmonic generation (HHG) source and two different charged-particle momentum imaging spectrometers. The HHG source, based on a commercial KM Labs eXtreme Ultraviolet Ultrafast Source, is capable of delivering XUV radiation of less than 30 fs pulse duration in the photon energy range of 17 eV to 100 eV. It can be coupled either to a conventional velocity map imaging (VMI) setup with an atomic, molecular, or nanoparticle target; or to a novel double-sided VMI spectrometer equipped with two delay-line detectors for coincidence studies. An overview of the setup and results of first pump-probe experiments including studies of two-color double ionization of Xe and time-resolved dynamics of photoionized CO2 molecule will be presented. This project is supported in part by National Science Foundation (NSF-EPSCOR) Award No. IIA-1430493 and in part by the Chemical science, Geosciences, and Bio-Science division, Office of Basic Energy Science, Office of science, U.S. Department of Energy. K.
Tracking reaction dynamics in solution by pump-probe X-ray absorption spectroscopy and X-ray liquidography (solution scattering).

PubMed

Kim, Jeongho; Kim, Kyung Hwan; Oang, Key Young; Lee, Jae Hyuk; Hong, Kiryong; Cho, Hana; Huse, Nils; Schoenlein, Robert W; Kim, Tae Kyu; Ihee, Hyotcherl

2016-03-07

Characterization of transient molecular structures formed during chemical and biological processes is essential for understanding their mechanisms and functions. Over the last decade, time-resolved X-ray liquidography (TRXL) and time-resolved X-ray absorption spectroscopy (TRXAS) have emerged as powerful techniques for molecular and electronic structural analysis of photoinduced reactions in the solution phase. Both techniques make use of a pump-probe scheme that consists of (1) an optical pump pulse to initiate a photoinduced process and (2) an X-ray probe pulse to monitor changes in the molecular structure as a function of time delay between pump and probe pulses. TRXL is sensitive to changes in the global molecular structure and therefore can be used to elucidate structural changes of reacting solute molecules as well as the collective response of solvent molecules. On the other hand, TRXAS can be used to probe changes in both local geometrical and electronic structures of specific X-ray-absorbing atoms due to the element-specific nature of core-level transitions. These techniques are complementary to each other and a combination of the two methods will enhance the capability of accurately obtaining structural changes induced by photoexcitation. Here we review the principles of TRXL and TRXAS and present recent application examples of the two methods for studying chemical and biological processes in solution. Furthermore, we briefly discuss the prospect of using X-ray free electron lasers for the two techniques, which will allow us to keep track of structural dynamics on femtosecond time scales in various solution-phase molecular reactions.
Pump-Probe Spectroscopy Using the Hadamard Transform.

PubMed

Beddard, Godfrey S; Yorke, Briony A

2016-08-01

A new method of performing pump-probe experiments is proposed and experimentally demonstrated by a proof of concept on the millisecond scale. The idea behind this method is to measure the total probe intensity arising from several time points as a group, instead of measuring each time separately. These measurements are multiplexes that are then transformed into the true signal via multiplication with a binary Hadamard S matrix. Each group of probe pulses is determined by using the pattern of a row of the Hadamard S matrix and the experiment is completed by rotating this pattern by one step for each sample excitation until the original pattern is again produced. Thus to measure n time points, n excitation events are needed and n probe patterns each taken from the n × n S matrix. The time resolution is determined by the shortest time between the probe pulses. In principle, this method could be used over all timescales, instead of the conventional pump-probe method which uses delay lines for picosecond and faster time resolution, or fast detectors and oscilloscopes on longer timescales. This new method is particularly suitable for situations where the probe intensity is weak and/or the detector is noisy. When the detector is noisy, there is in principle a signal to noise advantage over conventional pump-probe methods. © The Author(s) 2016.
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.
Reaction pathways of photoexcited retinal in proteorhodopsin studied by pump-dump-probe spectroscopy.

PubMed

Rupenyan, Alisa; van Stokkum, Ivo H M; Arents, Jos C; van Grondelle, Rienk; Hellingwerf, Klaas J; Groot, Marie Louise

2009-12-17

Proteorhodopsin (pR) is a membrane-embedded proton pump from the microbial rhodopsin family. Light absorption by its retinal chromophore initiates a photocycle, driven by trans/cis isomerization on the femtosecond to picosecond time scales. Here, we report a study on the photoisomerization dynamics of the retinal chromophore of pR, using dispersed ultrafast pump-dump-probe spectroscopy. The application of a pump pulse initiates the photocycle, and with an appropriately tuned dump pulse applied at a time delay after the dump, the molecules in the initial stages of the photochemical process can be de-excited and driven back to the ground state. In this way, we were able to resolve an intermediate on the electronic ground state that represents chromophores that are unsuccessful in isomerization. In particular, the fractions of molecules that undergo slow isomerization (20 ps) have a high probability to enter this state rather than the isomerized K-state. On the ground state reaction surface, return to the stable ground state conformation via a structural or vibrational relaxation occurs in 2-3 ps. Inclusion of this intermediate in the kinetic scheme led to more consistent spectra of the retinal-excited state, and to a more accurate estimation of the quantum yield of isomerization (Phi = 0.4 at pH 6).

Real-time detection of S(1D2) photofragments produced from the 1B2(1Σu+) state of CS2 by vacuum ultraviolet photoelectron imaging using 133 nm probe pulses

NASA Astrophysics Data System (ADS)

Horio, Takuya; Spesyvtsev, Roman; Furumido, Yu; Suzuki, Toshinori

2017-07-01

Ultrafast photodissociation dynamics from the 1B2(1Σu+) state of CS2 are studied by time-resolved photoelectron imaging using the fourth (4ω, 198 nm) and sixth (6ω, 133 nm) harmonics of a femtosecond Ti:sapphire laser. The 1B2 state of CS2 was prepared with the 4ω pulses, and subsequent dynamics were probed using the 6ω vacuum ultraviolet (VUV) pulses. The VUV pulses enabled real-time detection of S(1D2) photofragments, produced via CS2*(1B2(1Σu+)) → CS(X 1Σ+) + S(1D2). The photoionization signal of dissociating CS2*(1B2(1Σu+)) molecules starts to decrease at about 100 fs, while the S(1D2) fragments appear with a finite (ca. 400 fs) delay time after the pump pulse. Also discussed is the configuration interaction of the 1B2(1Σu+) state based on relative photoionization cross-sections to different cationic states.
Theory of attosecond delays in molecular photoionization.

PubMed

Baykusheva, Denitsa; Wörner, Hans Jakob

2017-03-28

We present a theoretical formalism for the calculation of attosecond delays in molecular photoionization. It is shown how delays relevant to one-photon-ionization, also known as Eisenbud-Wigner-Smith delays, can be obtained from the complex dipole matrix elements provided by molecular quantum scattering theory. These results are used to derive formulae for the delays measured by two-photon attosecond interferometry based on an attosecond pulse train and a dressing femtosecond infrared pulse. These effective delays are first expressed in the molecular frame where maximal information about the molecular photoionization dynamics is available. The effects of averaging over the emission direction of the electron and the molecular orientation are introduced analytically. We illustrate this general formalism for the case of two polyatomic molecules. N 2 O serves as an example of a polar linear molecule characterized by complex photoionization dynamics resulting from the presence of molecular shape resonances. H 2 O illustrates the case of a non-linear molecule with comparably simple photoionization dynamics resulting from a flat continuum. Our theory establishes the foundation for interpreting measurements of the photoionization dynamics of all molecules by attosecond metrology.
Femtosecond measurements of near-infrared pulse induced mid-infrared transmission modulation of quantum cascade lasers

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

Cai, Hong; Liu, Sheng; Center for Advanced Studied in Photonics Research

2014-05-26

We temporally resolved the ultrafast mid-infrared transmission modulation of quantum cascade lasers (QCLs) using a near-infrared pump/mid-infrared probe technique at room temperature. Two different femtosecond wavelength pumps were used with photon energy above and below the quantum well (QW) bandgap. The shorter wavelength pump modulates the mid-infrared probe transmission through interband transition assisted mechanisms, resulting in a high transmission modulation depth and several nanoseconds recovery lifetime. In contrast, pumping with a photon energy below the QW bandgap induces a smaller transmission modulation depth but much faster (several picoseconds) recovery lifetime, attributed to intersubband transition assisted mechanisms. The latter ultrafast modulationmore » (>60 GHz) could provide a potential way to realize fast QCL based free space optical communication.« less
Time zero determination for FEL pump-probe studies based on ultrafast melting of bismuth.

PubMed

Epp, S W; Hada, M; Zhong, Y; Kumagai, Y; Motomura, K; Mizote, S; Ono, T; Owada, S; Axford, D; Bakhtiarzadeh, S; Fukuzawa, H; Hayashi, Y; Katayama, T; Marx, A; Müller-Werkmeister, H M; Owen, R L; Sherrell, D A; Tono, K; Ueda, K; Westermeier, F; Miller, R J D

2017-09-01

A common challenge for pump-probe studies of structural dynamics at X-ray free-electron lasers (XFELs) is the determination of time zero (T 0 )-the time an optical pulse (e.g., an optical laser) arrives coincidently with the probe pulse (e.g., a XFEL pulse) at the sample position. In some cases, T 0 might be extracted from the structural dynamics of the sample's observed response itself, but generally, an independent robust method is required or would be superior to the inferred determination of T 0 . In this paper, we present how the structural dynamics in ultrafast melting of bismuth can be exploited for a quickly performed, reliable and accurate determination of T 0 with a precision below 20 fs and an overall experimental accuracy of 50 fs to 150 fs (estimated). Our approach is potentially useful and applicable for fixed-target XFEL experiments, such as serial femtosecond crystallography, utilizing an optical pump pulse in the ultraviolet to near infrared spectral range and a pixelated 2D photon detector for recording crystallographic diffraction patterns in transmission geometry. In comparison to many other suitable approaches, our method is fairly independent of the pumping wavelength (UV-IR) as well as of the X-ray energy and offers a favorable signal contrast. The technique is exploitable not only for the determination of temporal characteristics of the experiment at the interaction point but also for investigating important conditions affecting experimental control such as spatial overlap and beam spot sizes.
Tunable femtosecond lasers with low pump thresholds

NASA Astrophysics Data System (ADS)

Oppo, Karen

The work in this thesis is concerned with the development of tunable, femtosecond laser systems, exhibiting low pump threshold powers. The main motive for this work was the development of a low threshold, self-modelocked Ti:Al2O3 laser in order to replace the conventional large-frame argon-ion pump laser with a more compact and efficient all-solid-state alternative. Results are also presented for an all-solid-state, self-modelocked Cr:LiSAF laser, however most of this work is concerned with self-modelocked Ti:Al2O3 laser systems. In chapter 2, the operation of a regeneratively-initiated, and a hard-aperture self- modelocked Ti:Al2O3 laser, pumped by an argon-ion laser, is discussed. Continuous- wave oscillation thresholds as low as 160mW have been demonstrated, along with self-modelocked threshold powers as low as 500mW. The measurement and suppression of phase noise on modelocked lasers is discussed in chapter 3. This is followed by a comparison of the phase noise characteristics of the regeneratively-initiated, and hard-aperture self-modelocked Ti:Al2O3 lasers. The use of a synchronously-operating, high resolution electron-optical streak camera in the evaluation of timing jitter is also presented. In chapter 4, the construction and self-modelocked operation of an all-solid-state Ti:Al2O3 laser is described. The all-solid-state alternative to the conventional argon-ion pump laser was a continuous-wave, intracavity-frequency doubled, diode-laser pumped Nd:YLF ring laser. At a total diode-laser pump power of 10W, this minilaser was capable of producing a single frequency output of 1W, at 523.5nm in a TEM00 beam. The remainder of this thesis looks at the operation of a self-modelocked Ti:Al2O3 laser generating ultrashort pulses at wavelengths as long as 1053nm. The motive for this work was the development of an all-solid-state, self- modelocked Ti:Al2O3 laser operating at 1053nm, for use as a master oscillator in a Nd:glass power chain.
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 Î¸ 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 Î¸. 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.
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.
100-kHz shot-to-shot broadband data acquisition for high-repetition-rate pump-probe spectroscopy.

PubMed

Kanal, Florian; Keiber, Sabine; Eck, Reiner; Brixner, Tobias

2014-07-14

Shot-to-shot broadband detection is common in ultrafast pump-probe spectroscopy. Taking advantage of the intensity correlation of subsequent laser pulses improves the signal-to-noise ratio. Finite data readout times of CCD chips in the employed spectrometer and the maximum available speed of mechanical pump-beam choppers typically limit this approach to lasers with repetition rates of a few kHz. For high-repetition (≥ 100 kHz) systems, one typically averages over a larger number of laser shots leading to inferior signal-to-noise ratios or longer measurement times. Here we demonstrate broadband shot-to-shot detection in transient absorption spectroscopy with a 100-kHz femtosecond laser system. This is made possible using a home-built high-speed chopper with external laser synchronization and a fast CCD line camera. Shot-to-shot detection can reduce the data acquisition time by two orders of magnitude compared to few-kHz lasers while keeping the same signal-to-noise ratio.
Photodissociation dynamics of nitromethane at 226 and 271 nm at both nanosecond and femtosecond time scales.

PubMed

Guo, Y Q; Bhattacharya, A; Bernstein, E R

2009-01-08

Photodissociation of nitromethane has been investigated for decades both theoretically and experimentally; however, as a whole picture, the dissociation dynamics for nitromethane are still not clear, although many different mechanisms have been proposed. To make a complete interpretation of these different mechanisms, photolysis of nitromethane at 226 and 271 nm under both collisional and collisionless conditions is investigated at nanosecond and femtosecond time scales. These two laser wavelengths correspond to the pi* <-- pi and pi* <-- n excitations of nitromethane, respectively. In nanosecond 226 nm (pi* <-- pi) photolysis experiments, CH(3) and NO radicals are observed as major products employing resonance enhanced multiphoton ionization techniques and time-of-flight mass spectrometry. Additionally, OH and CH(3)O radicals are weakly observed as dissociation products employing laser induced fluorescence spectroscopy; the CH(3)O product is only observed under collisional conditions. In femtosecond 226 nm experiments, CH(3), NO(2), and NO products are observed. These results confirm that rupture of C-N bond should be the main primary process for the photolysis of nitromethane after the pi* <-- pi excitation at 226 nm, and the NO(2) molecule should be the precursor of the observed NO product. Formation of the CH(3)O radical after the recombination of CH(3) and NO(2) species under collisional conditions rules out a nitro-nitrite isomerization mechanism for the generation of CH(3)O and NO from pi pi* CH(3)NO(2). The OH radical formation for pi pi* CH(3)NO(2) should be a minor dissociation channel because of the weak OH signal in both nanosecond and femtosecond (nonobservable) experiments. Single color femtosecond pump-probe experiments at 226 nm are also employed to monitor the dynamics of the dissociation of nitromethane after the pi* <-- pi excitation. Because of the ultrafast dynamics of product formation at 226 nm, the pump-probe transients for the three
Ultrafast amorphization in Ge(10)Sb(2)Te(13) thin film induced by single femtosecond laser pulse.

PubMed

Konishi, Mitsutaka; Santo, Hisashi; Hongo, Yuki; Tajima, Kazuyuki; Hosoi, Masaharu; Saiki, Toshiharu

2010-06-20

We demonstrate amorphization in a Ge(10)Sb(2)Te(13) (GST) thin film through a nonthermal process by femtosecond electronic excitation. Amorphous recording marks were formed by irradiation with a single femtosecond pulse, and were confirmed to be recrystallized by laser thermal annealing. Scanning electron microscope observations revealed that amorphization occurred below the melting temperature. We performed femtosecond pump-probe measurements to investigate the amorphization dynamics of a GST thin film. We found that the reflectivity dropped abruptly within 500fs after excitation by a single pulse and that a small change in the reflectivity occurred within 5ps of this drop.
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.
Pump-probe optical microscopy for imaging nonfluorescent chromophores.

PubMed

Wei, Lu; Min, Wei

2012-06-01

Many chromophores absorb light intensely but have undetectable fluorescence. Hence microscopy techniques other than fluorescence are highly desirable for imaging these chromophores inside live cells, tissues, and organisms. The recently developed pump-probe optical microscopy techniques provide fluorescence-free contrast mechanisms by employing several fundamental light-molecule interactions including excited state absorption, stimulated emission, ground state depletion, and the photothermal effect. By using the pump pulse to excite molecules and the subsequent probe pulse to interrogate the created transient states on a laser scanning microscope, pump-probe microscopy offers imaging capability with high sensitivity and specificity toward nonfluorescent chromophores. Single-molecule sensitivity has even been demonstrated. Here we review and summarize the underlying principles of this emerging class of molecular imaging techniques.
Femtosecond study of A1g phonons in the strong 3D topological insulators: From pump-probe to coherent control

NASA Astrophysics Data System (ADS)

Hu, Jianbo; Igarashi, Kyushiro; Sasagawa, Takao; Nakamura, Kazutaka G.; Misochko, Oleg V.

2018-01-01

Fully symmetric A1g phonons are expected to play a dominant role in electron scattering in strong topological insulators (TIs), thus limiting the ballistic transport of future electronic devices. Here, we report on femtosecond time-resolved observation of a pair of A1g coherent phonons and their optical control in two strong 3D TIs, Bi2Te3 and Bi2Se3, by using a second pump pulse in ultrafast spectroscopy measurements. Along with well-defined phonon properties such as frequency and lifetime, an obvious phonon chirp has been observed, implying a strong coupling between photo-carriers and lattices. The coherent phonon manipulation, on the other hand, allows us to change the phonon amplitude selectively but does not affect either the frequency or coherence lifetime of the chosen mode.
Strong-field Photoionization of Sputtered Neutral Molecules for Molecular Depth Profiling

PubMed Central

Willingham, D; Brenes, D. A.; Wucher, A

2009-01-01

Molecular depth profiles of an organic thin film of guanine vapor deposited onto a Ag substrate are obtained using a 40 keV C60 cluster ion beam in conjunction with time-of-flight secondary ion mass spectrometric (ToF-SIMS) detection. Strong-field, femtosecond photoionization of intact guanine molecules is used to probe the neutral component of the profile for direct comparison with the secondary ion component. The ability to simultaneously acquire secondary ions and photoionized neutral molecules reveals new fundamental information about the factors that influence the properties of the depth profile. Results show that there is an increased ionization probability for protonated molecular ions within the first 10 nm due to the generation of free protons within the sample. Moreover, there is a 50% increase in fragment ion signal relative to steady state values 25 nm before reaching the guanine/Ag interface as a result of interfacial chemical damage accumulation. An altered layer thickness of 20 nm is observed as a consequence of ion beam induced chemical mixing. In general, we show that the neutral component of a molecular depth profile using the strong-field photoionization technique can be used to elucidate the effects of variations in ionization probability on the yield of molecular ions as well as to aid in obtaining accurate information about depth dependent chemical composition that cannot be extracted from TOF-SIMS data alone. PMID:20495665
Ultra-broadband infrared pump-probe spectroscopy using synchrotron radiation and a tuneable pump.

PubMed

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

2011-06-01

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 μm) 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 μm 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 pump
Diode-pumped femtosecond mode-locked Nd, Y-codoped CaF2 laser

NASA Astrophysics Data System (ADS)

Zhu, Jiangfeng; Zhang, Lijuan; Gao, Ziye; Wang, Junli; Wang, Zhaohua; Su, Liangbi; Zheng, Lihe; Wang, Jingya; Xu, Jun; Wei, Zhiyi

2015-03-01

A passively mode-locked femtosecond laser based on an Nd, Y-codoped CaF2 disordered crystal was demonstrated. The Y3+-codoping in Nd : CaF2 markedly suppressed the quenching effect and improved the fluorescence quantum efficiency and emission spectra. With a fiber-coupled laser diode as the pump source, the continuous wave tuning range covering from 1042 to 1076 nm was realized, while the mode-locked operation generated 264 fs pulses with an average output power of 180 mW at a repetition rate of 85 MHz. The experimental results show that the Nd, Y-codoped CaF2 disordered crystal has potential in a new generation diode-pumped high repetition rate chirped pulse amplifier.
Mid-infrared picosecond pump-dump-probe and pump-repump-probe experiments to resolve a ground-state intermediate in cyanobacterial phytochrome Cph1.

PubMed

van Wilderen, Luuk J G W; Clark, Ian P; Towrie, Michael; van Thor, Jasper J

2009-12-24

Multipulse picosecond mid-infrared spectroscopy has been used to study photochemical reactions of the cyanobacterial phytochrome photoreceptor Cph1. Different photophysical schemes have been discussed in the literature to describe the pathways after photoexcitation, particularly, to identify reaction phases that are linked to photoisomerisation and electronic decay in the 1566-1772 cm(-1) region that probes C=C and C=O stretching modes of the tetrapyrrole chromophore. Here, multipulse spectroscopy is employed, where, compared to conventional visible pump-mid-infrared probe spectroscopy, an additional visible pulse is incorporated that interacts with populations that are evolving on the excited- and ground-state potential energy surfaces. The time delays between the pump and the dump pulse are chosen such that the dump pulse interacts with different phases in the reaction process. The pump and dump pulses are at the same wavelength, 640 nm, and are resonant with the Pr ground state as well as with the excited state and intermediates. Because the dump pulse additionally pumps the remaining, partially recovered, and partially oriented ground-state population, theory is developed for estimating the fraction of excited-state molecules. The calculations take into account the model-dependent ground-state recovery fraction, the angular dependence of the population transfer resulting from the finite bleach that occurs with linearly polarized intense femtosecond optical excitation, and the partially oriented population for the dump field. Distinct differences between the results from the experiments that use a 1 or a 14 ps dump time favor a branching evolution from S1 to an excited state or reconfigured chromophore and to a newly identified ground-state intermediate (GSI). Optical dumping at 1 ps shows the instantaneous induced absorption of a delocalized C=C stretching mode at 1608 cm(-1), where the increased cross section is associated with the electronic ground
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.
Pump-dump-probe and pump-repump-probe ultrafast spectroscopy resolves cross section of an early ground state intermediate and stimulated emission in the photoreactions of the Pr ground state of the cyanobacterial phytochrome Cph1.

PubMed

Fitzpatrick, Ann E; Lincoln, Craig N; van Wilderen, Luuk J G W; van Thor, Jasper J

2012-01-26

The primary photoreactions of the red absorbing ground state (Pr) of the cyanobacterial phytochrome Cph1 from Synechocystis PCC 6803 involve C15═C16 Z-E photoisomerization of its phycocyanobilin chromophore. The first observable product intermediate in pump-probe measurements of the photocycle, "Lumi-R", is formed with picosecond kinetics and involves excited state decay reactions that have 3 and 14 ps time constants. Here, we have studied the photochemical formation of the Lumi-R intermediate using multipulse picosecond visible spectroscopy. Pump-dump-probe (PDP) and pump-repump-probe (PRP) experiments were carried out by employing two femtosecond visible pulses with 1, 14, and 160 ps delays, together with a broadband dispersive visible probe. The time delays between the two excitation pulses have been selected to allow interaction with the dominant (3 and 14 ps) kinetic phases of Lumi-R formation. The frequency dependence of the PDP and PRP amplitudes was investigated at 620, 640, 660, and 680 nm, covering excited state absorption (λ(max) = 620 nm), ground state absorption (λ(max) = 660 nm), and stimulated emission (λ(max) = 680 nm) cross sections. Experimental double difference transient absorbance signals (ΔΔOD), from the PDP and PRP measurements, required corrections to remove contributions from ground state repumping. The sensitivity of the resulting ΔΔOD signals was systematically investigated for possible connectivity schemes and photochemical parameters. When applying a homogeneous (sequentially decaying) connectivity scheme in both the 3 and 14 ps kinetic phases, evidence for repumping of an intermediate that has an electronic ground state configuration (GSI) is taken from the dump-induced S1 formation with 620, 640, and 660 nm wavelengths and 1 and 14 ps repump delays. Evidence for repumping a GSI is also seen, for the same excitation wavelengths, when imposing a target connectivity scheme proposed in the literature for the 1 ps repump delay. In
A novel femtosecond-gated, high-resolution, frequency-shifted shearing interferometry technique for probing pre-plasma expansion in ultra-intense laser experiments

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

Feister, S., E-mail: feister.7@osu.edu; Orban, C.; Innovative Scientific Solutions, Inc., Dayton, Ohio 45459

Ultra-intense laser-matter interaction experiments (>10{sup 18} W/cm{sup 2}) with dense targets are highly sensitive to the effect of laser “noise” (in the form of pre-pulses) preceding the main ultra-intense pulse. These system-dependent pre-pulses in the nanosecond and/or picosecond regimes are often intense enough to modify the target significantly by ionizing and forming a plasma layer in front of the target before the arrival of the main pulse. Time resolved interferometry offers a robust way to characterize the expanding plasma during this period. We have developed a novel pump-probe interferometry system for an ultra-intense laser experiment that uses two short-pulse amplifiersmore » synchronized by one ultra-fast seed oscillator to achieve 40-fs time resolution over hundreds of nanoseconds, using a variable delay line and other techniques. The first of these amplifiers acts as the pump and delivers maximal energy to the interaction region. The second amplifier is frequency shifted and then frequency doubled to generate the femtosecond probe pulse. After passing through the laser-target interaction region, the probe pulse is split and recombined in a laterally sheared Michelson interferometer. Importantly, the frequency shift in the probe allows strong plasma self-emission at the second harmonic of the pump to be filtered out, allowing plasma expansion near the critical surface and elsewhere to be clearly visible in the interferograms. To aid in the reconstruction of phase dependent imagery from fringe shifts, three separate 120° phase-shifted (temporally sheared) interferograms are acquired for each probe delay. Three-phase reconstructions of the electron densities are then inferred by Abel inversion. This interferometric system delivers precise measurements of pre-plasma expansion that can identify the condition of the target at the moment that the ultra-intense pulse arrives. Such measurements are indispensable for correlating laser pre

Pump and probe spectroscopy with continuous wave quantum cascade lasers.

PubMed

Kirkbride, James M R; Causier, Sarah K; Dalton, Andrew R; Weidmann, Damien; Ritchie, Grant A D

2014-02-07

This paper details infra-red pump and probe studies on nitric oxide conducted with two continuous wave quantum cascade lasers both operating around 5 μm. The pump laser prepares a velocity selected population in a chosen rotational quantum state of the v = 1 level which is subsequently probed using a second laser tuned to a rotational transition within the v = 2 ← v = 1 hot band. The rapid frequency scan of the probe (with respect to the molecular collision rate) in combination with the velocity selective pumping allows observation of marked rapid passage signatures in the transient absorption profiles from the polarized vibrationally excited sample. These coherent transient signals are influenced by the underlying hyperfine structure of the pump and probe transitions, the sample pressure, and the coherent properties of the lasers. Pulsed pump and probe studies show that the transient absorption signals decay within 1 μs at 50 mTorr total pressure, reflecting both the polarization and population dephasing times of the vibrationally excited sample. The experimental observations are supported by simulation based upon solving the optical Bloch equations for a two level system.
Multi-gigahertz, femtosecond Airy beam optical parametric oscillator pumped at 78 MHz

PubMed Central

Aadhi, A.; Sharma, Varun; Chaitanya, N. Apurv; Samanta, G. K.

2017-01-01

We report a high power ultrafast Airy beam source producing femtosecond pulses at multi-gigahertz (GHz) repetition rate (RR). Based on intra-cavity cubic phase modulation of an optical parametric oscillator (OPO) designed in high harmonic cavity configuration synchronous to a femtosecond Yb-fiber laser operating at 78 MHz, we have produced ultrafast 2D Airy beam at multi-GHz repetition rate through the fractional increment in the cavity length. While small (<1 mm) crystals are used in femtosecond OPOs to take the advantage of broad phase-matching bandwidth, here, we have exploited the extended phase-matching bandwidth of a 50-mm long Magnesium-oxide doped periodically poled LiNbO3 (MgO:PPLN) crystal for efficient generation of ultrafast Airy beam and broadband mid-IR radiation. Pumping the MgO:PPLN crystal of grating period, Λ = 30 μm and crystal temperature, T = 100 °C using a 5-W femtosecond laser centred at 1064 nm, we have produced Airy beam radiation of 684 mW in ~639 fs (transform limited) pulses at 1525 nm at a RR of ~2.5 GHz. Additionally, the source produces broadband idler radiation with maximum power of 510 mW and 94 nm bandwidth at 3548 nm in Gaussian beam profile. Using an indirect method (change in cavity length) we estimate maximum RR of the Airy beam source to be ~100 GHz. PMID:28262823
Use of ultrafast dispersed pump-dump-probe and pump-repump-probe spectroscopies to explore the light-induced dynamics of peridinin in solution.

PubMed

Papagiannakis, Emmanouil; Vengris, Mikas; Larsen, Delmar S; van Stokkum, Ivo H M; Hiller, Roger G; van Grondelle, Rienk

2006-01-12

Optical pump-induced dynamics of the highly asymmetric carotenoid peridinin in methanol was studied by dispersed pump-probe, pump-dump-probe, and pump-repump-probe transient absorption spectroscopy in the visible region. Dispersed pump-probe measurements show that the decay of the initially excited S2 state populates two excited states, the S1 and the intramolecular charge-transfer (ICT) state, at a ratio determined by the excitation wavelength. The ensuing spectral evolution occurs on the time scale of a few picoseconds and suggests the equilibration of these states. Dumping the stimulated emission of the ICT state with an additional 800-nm pulse after 400- and 530-nm excitation preferentially removes the ICT state contribution from the broad excited-state absorption, allowing for its spectral characterization. At the same time, an unrelaxed ground-state species, which has a subpicosecond lifetime, is populated. The application of the 800-nm pulse at early times, when the S2 state is still populated, led to direct generation of the peridinin cation, observed for the first time in a transient absorption experiment. The excited and ground electronic states manifold of peridinin has been reconstructed using target analysis; this approach combined with the measured multipulse spectroscopic data allows us to estimate the spectra and time scales of the corresponding transient states.
Highly Resolved Studies of Vacuum Ultraviolet Photoionization Dynamics

NASA Astrophysics Data System (ADS)

Kakar, Sandeep

We use measurements of dispersed fluorescence from electronically excited photoions to study fundamental aspects of intramolecular dynamics. Our experimental innovations make it possible to obtain highly resolved photoionization data that offer qualitative insights into molecular scattering. In particular, we obtain vibrationally resolved data to probe coupling between the electronic and nuclear degrees of freedom by studying the distribution of vibrational energy among photoions. Vibrationally resolved branching ratios are measured over a broad spectral range of excitation energy and their non-Franck-Condon behavior is used as a tool to investigate two diverse aspects of shape resonant photoionization. First, vibrational branching ratios are obtained for the SiF_4 5a _1^{-1} and CS_2 5sigma_{rm u} ^{-1} photoionization channels to help elucidate the microscopic aspects of shape resonant wavefunction for polyatomic molecules. It is shown that in such molecules the shape resonant wavefunction is not necessarily attributable to a specific bond in the molecule. Second, the multichannel aspect of shape resonant photoionization dynamics, reflected in continuum channel coupling, is investigated by obtaining vibrational branching ratios for the 2 sigma_{rm u}^{ -1} and 4sigma^{ -1} photoionization of the isoelectronic molecules N_2 and CO, respectively. These data indicate that effects of continuum coupling may be widespread. We also present the first set of rotationally resolved data over a wide energy range for the 2 sigma_{rm u}^{ -1} photoionization of N_2. These data probe the partitioning of the angular momentum between the photoelectron and photoion, and highlight the multicenter nature of the molecular potential. These case studies illustrate the utility of dispersed fluorescence measurements as a complement to photoelectron spectroscopy for obtaining highly resolved data for molecular photoionization. These measurements makes it possible to probe intrinsically
Ultra-Broadband Two-Dimensional Electronic Spectroscopy and Pump-Probe Microscopy of Molecular Systems

NASA Astrophysics Data System (ADS)

Spokoyny, Boris M.

Ultrafast spectroscopy offers an unprecedented view on the dynamic nature of chemical reactions. From charge transfer in semiconductors to folding and isomerization of proteins, these all important processes can now be monitored and in some instances even controlled on real, physical timescales. One of the biggest challenges of ultrafast science is the incredible energetic complexity of most systems. It is not uncommon to encounter macromolecules or materials with absorption spectra spanning significant portions of the visible spectrum. Monitoring a multitude of electronic and vibrational transitions, all dynamically interacting with each other on femtosecond timescales poses a truly daunting experimental task. The first part of this thesis deals with the development of a novel Two-Dimensional Electronic Spectroscopy (2DES) and its associated, advanced detection methodologies. Owing to its ultra-broadband implementation, this technique enables us to monitor femtosecond chemical dynamics that span the energetic landscape of the entire visible spectrum. In order to demonstrate the utility of our method, we apply it to two laser dye molecules, IR-144 and Cresyl Violet. Variation of photophysical properties on a microscopic scale in either man-made or naturally occurring systems can have profound implications on how we understand their macroscopic properties. Recently, inorganic hybrid perovskites have been tapped as the next generation solar energy harvesting materials. Their remarkable properties include low exciton binding energy, low exciton recombination rates and long carrier diffusion lengths. Nevertheless, considerable variability in device properties made with nearly identical preparation methods has puzzled the community. In the second part of this thesis we use non-linear pump probe microscopy to study the heterogeneous nature of femtosecond carrier dynamics in thin film perovskites. We show that the local morphology of the perovskite thin films has a
Dynamics of solvation and desolvation of rubidium attached to He nanodroplets

NASA Astrophysics Data System (ADS)

von Vangerow, J.; John, O.; Stienkemeier, F.; Mudrich, M.

2015-07-01

The real-time dynamics of photoexcited and photoionized rubidium (Rb) atoms attached to helium (He) nanodroplets is studied by femtosecond pump-probe mass spectrometry. While excited Rb atoms in the perturbed 6p-state (Rb*) desorb off the He droplets, Rb+ photoions tend to sink into the droplet interior when created near the droplet surface. The transition from Rb+ solvation to full Rb* desorption is found to occur at a delay time τ ˜ 600 fs for Rb* in the 6pΣ-state and τ ˜ 1200 fs for the 6pΠ-state. Rb+He ions are found to be created by directly exciting bound Rb*He exciplex states as well as by populating bound Rb+He-states in a photoassociative ionization process.
Sequential picosecond isomerizations in a photochromic ruthenium sulfoxide complex triggered by pump-repump-probe spectroscopy.

PubMed

King, Albert W; Jin, Yuhuan; Engle, James T; Ziegler, Christopher J; Rack, Jeffrey J

2013-02-18

The complex [Ru(bpy)(2)(bpSO)](PF(6))(2), where bpy is 2,2'-bipydine and bpSO is 1,2-bis(phenylsulfinyl)ethane, exhibits three distinct isomers which are accessible upon metal-to-ligand charge-transfer (MLCT) irradiation. This complex and its parent, [Ru(bpy)(2)(bpte)](PF(6))(2), where bpte is 1,2-bis(phenylthio)ethane, have been synthesized and characterized by UV-visible spectroscopy, NMR, X-ray crystallography, and femtosecond transient absorption spectroscopy. A novel method of 2-color Pump-Repump-Probe spectroscopy has been employed to investigate all three isomers of the bis-sulfoxide complex. This method allows for observation of the isomerization dynamics of sequential isomerizations of each sulfoxide from MLCT irradiation of the S,S-bonded complex to ultimately form the O,O-bonded metastable complex. One-dimensional (1-D) and two-dimensional (2-D) (COSY, NOESY, and TOCSY) (1)H NMR data show the thioether and ground state S,S-bonded sulfoxide complexes to be rigorously C(2) symmetric and are consistent with the crystal structures. Transient absorption spectroscopy reveals that the S,S to S,O isomerization occurs with an observed time constant of 56.8 (±7.4) ps. The S,O to O,O isomerization time constant was found to be 59 (±4) ps by pump-repump-probe spectroscopy. The composite S,S- to O,O-isomer quantum yield is 0.42.
Observation of coherent optical phonons excited by femtosecond laser radiation in Sb films by ultrafast electron diffraction method

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

Mironov, B. N.; Kompanets, V. O.; Aseev, S. A., E-mail: isanfemto@yandex.ru

2017-03-15

The generation of coherent optical phonons in a polycrystalline antimony film sample has been investigated using femtosecond electron diffraction method. Phonon vibrations have been induced in the Sb sample by the main harmonic of a femtosecond Ti:Sa laser (λ = 800 nm) and probed by a pulsed ultrashort photoelectron beam synchronized with the pump laser. The diffraction patterns recorded at different times relative to the pump laser pulse display oscillations of electron diffraction intensity corresponding to the frequencies of vibrations of optical phonons: totally symmetric (A{sub 1g}) and twofold degenerate (E{sub g}) phonon modes. The frequencies that correspond to combinationsmore » of these phonon modes in the Sb sample have also been experimentally observed.« less
Femtosecond pulsed laser processing of electronic materials: Fundamentals and micro/nano-scale applications

NASA Astrophysics Data System (ADS)

Choi, Tae-Youl

Ultra-short pulsed laser radiation has been shown to be effective for precision materials processing and surface micro-modification. One of advantages is the substantial reduction of the heat penetration depth, which leads to minimal lateral damage. Other advantages include non-thermal nature of ablation process, controlled ablation and ideal characteristics for precision micro-structuring. Yet, fundamental questions remain unsolved regarding the nature of melting and ablation mechanisms in femtosecond laser processing of materials. In addition to micro engineering problems, nano-structuring and nano-fabrication are emerging fields that are of particular interest in conjunction with femtosecond laser processing. A comprehensive experimental study as well as theoretical development is presented to address these issues. Ultra-short pulsed laser irradiation was used to crystallize 100 nm amorphous silicon (a-Si) films. The crystallization process was observed by time-resolved pump-and-probe reflection imaging in the range of 0.2 ps to 100 ns. The in-situ images in conjunction with post-processed SEM and AFM mapping of the crystallized structure provide evidence for non-thermal ultra-fast phase transition and subsequent surface-initiated crystallization. Mechanisms of ultra-fast laser-induced ablation on crystalline silicon and copper are investigated by time-resolved pump-and-probe microscopy in normal imaging and shadowgraph arrangements. A one-dimensional model of the energy transport is utilized to predict the carrier temperature and lattice temperature as well as the electron and vapor flux emitted from the surface. The temporal delay between the pump and probe pulses was set by a precision translation stage up to about 500 ps and then extended to the nanosecond regime by an optical fiber assembly. The ejection of material was observed at several picoseconds to tens of nanoseconds after the main (pump) pulse by high-resolution, ultra-fast shadowgraphs. The
Properties of the anion-binding site of pharaonis Halorhodopsin studied by ultrafast pump-probe spectroscopy and low-temperature FTIR spectroscopy.

PubMed

Nakashima, Keisuke; Nakamura, Takumi; Takeuchi, Satoshi; Shibata, Mikihiro; Demura, Makoto; Tahara, Tahei; Kandori, Hideki

2009-06-18

Halorhodopsin (HR) is a light-driven chloride pump. Cl(-) is bound in the Schiff base region of the retinal chromophore, and unidirectional Cl(-) transport is probably enforced by the specific hydrogen-bonding interaction with the protonated Schiff base and internal water molecules. It is known that HR from Natronobacterium pharaonis (pHR) also pumps NO(3)(-) with similar efficiency, suggesting that NO(3)(-) binds to the Cl(-)-binding site. In the present study, we investigated the properties of the anion-binding site by means of ultrafast pump-probe spectroscopy and low-temperature FTIR spectroscopy. The obtained data were surprisingly similar between pHR-NO(3)(-) and pHR-Cl(-), even though the shapes and sizes of the two anions are quite different. Femtosecond pump-probe spectroscopy showed very similar excited-state dynamics between pHR-NO(3)(-) and pHR-Cl(-). Low-temperature FTIR spectroscopy of unlabeled and [zeta-(15)N]Lys-labeled pHR revealed almost identical hydrogen-bonding strengths of the protonated retinal Schiff base between pHR-NO(3)(-) and pHR-Cl(-), which is similarly strengthened after retinal isomerization. There were spectral variations for water stretching vibrations between pHR-NO(3)(-) and pHR-Cl(-), suggesting that the water molecules hydrate each anion. Nevertheless, the overall spectral features were similar for the two species. These observations strongly suggest that the anion-binding site has a flexible structure and that the interaction between retinal and the anions is weak, despite the presence of an electrostatic interaction. Such a flexible hydrogen-bonding network in the Schiff base region in HR appears to be in remarkable contrast to that in light-driven proton-pumping proteins.
A versatile and reconfigurable setup for all-terahertz time-resolved pump-probe spectroscopy.

PubMed

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.
Pump-probe spectroscopy in organic semiconductors: monitoring fundamental processes of relevance in optoelectronics.

PubMed

Cabanillas-Gonzalez, Juan; Grancini, Giulia; Lanzani, Guglielmo

2011-12-08

In this review we highlight the contribution of pump-probe spectroscopy to understand elementary processes taking place in organic based optoelectronic devices. The techniques described in this article span from conventional pump-probe spectroscopy to electromodulated pump-probe and the state-of-the-art confocal pump-probe microscopy. The article is structured according to three fundamental processes (optical gain, charge photogeneration and charge transport) and the contribution of these techniques on them. The combination of these tools opens up new perspectives for assessing the role of short-lived excited states on processes lying underneath organic device operation. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Effect of attochirp on attosecond streaking time delay in photoionization of atoms

NASA Astrophysics Data System (ADS)

Goldsmith, C.; Jaroń-Becker, A.; Becker, A.

2018-01-01

We present a theoretical analysis of the effect of the attochirp on the streaking time delay, intrinsic to photoionization of an atom by an attosecond laser pulse at extreme ultraviolet wavelengths superposed by a femtosecond streaking pulse. To this end, we determine the expectation value of the delay in a chirped pulse using a recently developed model formula. Results of our calculations show that the attochirp can be relevant for photoemission from the 3p shell in argon atom at frequencies near the Cooper minimum, while it is negligible if the photoionization cross section as a function of frequency varies smoothly.
Cross-phase modulation spectral shifting: nonlinear phase contrast in a pump-probe microscope

PubMed Central

Wilson, Jesse W.; Samineni, Prathyush; Warren, Warren S.; Fischer, Martin C.

2012-01-01

Microscopy with nonlinear phase contrast is achieved by a simple modification to a nonlinear pump-probe microscope. The technique measures cross-phase modulation by detecting a pump-induced spectral shift in the probe pulse. Images with nonlinear phase contrast are acquired both in transparent and absorptive media. In paraffin-embedded biopsy sections, cross-phase modulation complements the chemically-specific pump-probe images with structural context. PMID:22567580
Tunable near- to mid-infrared pump terahertz probe spectroscopy in reflection geometry

NASA Astrophysics Data System (ADS)

Zhang, S. J.; Wang, Z. X.; Dong, T.; Wang, N. L.

2017-10-01

Strong-field mid-infrared pump-terahertz (THz) probe spectroscopy has been proven as a powerful tool for light control of different orders in strongly correlated materials. We report the construction of an ultrafast broadband infrared pump-THz probe system in reflection geometry. A two-output optical parametric amplifier is used for generating mid-infrared pulses with GaSe as the nonlinear crystal. The setup is capable of pumping bulk materials at wavelengths ranging from 1.2 μm to 15 μm and beyond, and detecting the subtle, transient photoinduced changes in the reflected electric field of the THz probe at different temperatures. As a demonstration, we present 15 μm pump-THz probe measurements of a bulk EuSbTe3 single crystal. A 0:5% transient change in the reflected THz electric field can be clearly resolved. The widely tuned pumping energy could be used in mode-selective excitation experiments and applied to many strongly correlated electron systems.
Enhancement of 800 nm upconversion emission in a thulium doped tellurite microstructured fiber pumped by a 1560 nm femtosecond fiber laser

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

Jia, Zhixu; Zheng, Kezhi; State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, Changchun 130012

We report enhanced upconversion (UC) fluorescence in Tm{sup 3+} doped tellurite microstructured fibers (TDTMFs) fabricated by using a rod-in-tube method. Under the pumping of a 1560 nm femtosecond fiber laser, ultrabroadband supercontinuum light expanding from ∼1050 to ∼2700 nm was generated in a 4 cm long TDTMF. Simultaneously, intense 800 nm UC emission from the {sup 3}H{sub 4} → {sup 3}H{sub 6} transition of Tm{sup 3+} was observed in the same TDTMF. Compared to that pumped by a 1560 nm continuous wave fiber laser, the UC emission intensity was enhanced by ∼4.1 times. The enhancement was due to the spectral broadening in the TDTMF under themore » pumping of the 1560 nm femtosecond fiber laser.« less
Femtosecond MeV Electron Energy-Loss Spectroscopy

DOE PAGES

Li, R. K.; Wang, X. J.

2017-11-09

Pump-probe electron energy-loss spectroscopy (EELS) with femtosecond temporal resolution will be a transformative research tool for studying nonequilibrium chemistry and electronic dynamics of matter. Here in this article, we propose a concept of femtosecond EELS utilizing mega-electron-volt electron beams from a radio-frequency (rf) photocathode source. The high acceleration gradient and high beam energy of the rf gun are critical to the generation of 10-fs electron beams, which enables an improvement of the temporal resolution by more than 1 order of magnitude beyond the state of the art. In our proposal, the “referencebeam technique” relaxes the energy stability requirement of themore » rf power source by roughly 2 orders of magnitude. The requirements for the electron-beam quality, photocathode, spectrometer, and detector are also discussed. Supported by particle-tracking simulations, we demonstrate the feasibility of achieving subelectron- volt energy resolution and approximately 10-fs temporal resolution with existing or near-future hardware performance.« less
Femtosecond MeV Electron Energy-Loss Spectroscopy

NASA Astrophysics Data System (ADS)

Li, R. K.; Wang, X. J.

2017-11-01

Pump-probe electron energy-loss spectroscopy (EELS) with femtosecond temporal resolution will be a transformative research tool for studying nonequilibrium chemistry and electronic dynamics of matter. In this paper, we propose a concept of femtosecond EELS utilizing mega-electron-volt electron beams from a radio-frequency (rf) photocathode source. The high acceleration gradient and high beam energy of the rf gun are critical to the generation of 10-fs electron beams, which enables an improvement of the temporal resolution by more than 1 order of magnitude beyond the state of the art. In our proposal, the "reference-beam technique" relaxes the energy stability requirement of the rf power source by roughly 2 orders of magnitude. The requirements for the electron-beam quality, photocathode, spectrometer, and detector are also discussed. Supported by particle-tracking simulations, we demonstrate the feasibility of achieving sub-electron-volt energy resolution and approximately 10-fs temporal resolution with existing or near-future hardware performance.
Femtosecond MeV Electron Energy-Loss Spectroscopy

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

Li, R. K.; Wang, X. J.

Pump-probe electron energy-loss spectroscopy (EELS) with femtosecond temporal resolution will be a transformative research tool for studying nonequilibrium chemistry and electronic dynamics of matter. Here in this article, we propose a concept of femtosecond EELS utilizing mega-electron-volt electron beams from a radio-frequency (rf) photocathode source. The high acceleration gradient and high beam energy of the rf gun are critical to the generation of 10-fs electron beams, which enables an improvement of the temporal resolution by more than 1 order of magnitude beyond the state of the art. In our proposal, the “referencebeam technique” relaxes the energy stability requirement of themore » rf power source by roughly 2 orders of magnitude. The requirements for the electron-beam quality, photocathode, spectrometer, and detector are also discussed. Supported by particle-tracking simulations, we demonstrate the feasibility of achieving subelectron- volt energy resolution and approximately 10-fs temporal resolution with existing or near-future hardware performance.« less
Prompt and delayed Coulomb explosion of doubly ionized hydrogen chloride molecules in intense femtosecond laser fields

NASA Astrophysics Data System (ADS)

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

2018-06-01

We experimentally investigate the dissociative double ionization of hydrogen chloride (HCl) molecules in intense femtosecond laser pulses. In addition to the prompt dissociation channels which occur on femtosecond timescales, long-lived hydrogen chloride dications which Coulomb-explode in flight towards the detector are clearly identified in the photoion-photoion coincidence spectrum. Different pathways leading to these prompt and delayed dissociation channels involving various bound and repulsive states of the HCl dication are discussed based on the observed kinetic energy release and momentum distributions. Our results indicate that the specific features of the HCl dication potential energy curves are responsible for the generation of the delayed fragmentation channels, which are expected to be general processes for the hydrogen halides.

Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.

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

Kearney, Sean Patrick

A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti-Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited, or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximum Raman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparationmore » bandwidth. Shifts of 100 cm -1 or more are attainable and allow for enhanced detection of high-energy (150-300 cm -1) rotational Raman transitions at near transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H 2/air flat flame.« less
Bandwidth optimization of femtosecond pure-rotational coherent anti-Stokes Raman scattering by pump/Stokes spectral focusing.

DOE PAGES

Kearney, Sean Patrick

2014-07-01

A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti-Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited, or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximum Raman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparationmore » bandwidth. Shifts of 100 cm -1 or more are attainable and allow for enhanced detection of high-energy (150-300 cm -1) rotational Raman transitions at near transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H 2/air flat flame.« less
Study of the relaxation rate of photoexcited indole molecules by the interferometric pump-and-probe method at picosecond resolution

NASA Astrophysics Data System (ADS)

Glazov, A. L.; Il'ina, A. D.; Sukharev, A. A.; Vasyutinskii, O. S.

2017-09-01

We present a new interferometric method that can be used for studying the dynamics of photoinduced processes in biologically important molecules at ultrahigh temporal resolution. The method is based upon the detection of changes in the refractive index of a substance excited by pulsed radiation of a femtosecond laser, which are measured by the pump-and-probe technique using time-delayed pulses of the same laser. The high sensitivity and stability of the interferometer allow this method to be used for monitoring variation of the concentration of short-lived excited states of biomolecules in solution. The proposed method has been verified by application to indole solutions in propylene glycol. The upper estimate of the lifetime of photoexcited indole molecules in solution amounted to about 40 ps.
Comparison of femtosecond laser ablation of aluminum in water and in air by time-resolved optical diagnosis.

PubMed

Hu, Haofeng; Liu, Tiegen; Zhai, Hongchen

2015-01-26

The dynamic process of material ejection and shock wave evolution during one single femtosecond laser pulse ablation of aluminum target in water and air is experimentally investigated by employing pump-probe technique. Shadowgraphs and digital holograms with high temporal resolution are recorded, which intuitively reveal the characteristics of femtosecond laser ablation in the water-confined environment. The experimental result indicates that the liquid significantly restrict the diffusion of the ejected material, and it has a considerable effect on the attenuation of the shock wave. In addition, the expansion Mach wave generated by the ultrasonic expansion of the shock wave is observed.
Mid-infrared supercontinuum generation up to 4.6 µm using step-index indium fluoride fiber pumped by a femtosecond fiber laser near 2 µm

NASA Astrophysics Data System (ADS)

Salem, Reza; Jiang, Zack; Liu, Dongfeng; Pafchek, Robert; Foy, Paul; Saad, Mohammed; Jenkins, Doug; Cable, Alex; Fendel, Peter

2016-03-01

We report mid-infrared supercontinuum (SC) generation in a dispersion-engineered step-index indium fluoride fiber pumped by a femtosecond fiber laser near 2 μm. The SC spans 1.8 octaves from 1.25 μm to 4.6 μm with an average output power of 270 mW. The pump source is an all-fiber femtosecond laser that generates sub-100 fs pulses at 50 MHz repetition rate with 570 mW average power. The indium fluoride fiber used for SC generation is designed to have a zerodispersion wavelength close to 1.9 μm. Two fiber lengths of 30 cm and 55 cm are selected for the SC generation experiments based on the numerical modelling results. The measured spectra and the numerical modelling results are presented showing good agreement for both lengths. The femtosecond pumping regime is a key requirement for generating a coherent SC. We show by modelling that the SC is coherent for a pump with the same pulse width and energy as our fiber laser and added quantum-limited noise. The results are promising for the realization of coherent and high-repetition-rate SC sources, two conditions that are critical for spectroscopy applications using FTIR spectrometers. Additionally, the entire SC system is built using optical fibers with similar core diameters, which enables integration into a compact platform.
Mapping and controlling ultrafast dynamics of highly excited H 2 molecules by VUV-IR pump-probe schemes

DOE PAGES

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

2017-01-09

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

NASA Astrophysics Data System (ADS)

Cadatal-Raduban, Marilou; Pham, Minh Hong; Gabayno, Jacque Lynn; Yamanoi, Kohei; Empizo, Melvin John F.; Shimizu, Toshihiko; Sarukura, Nobuhiko; Nguyen, Hung Dai; Yoshikawa, Akira; Fukuda, Tsuguo

2018-02-01

Two side-pumping schemes suitable for the development of an ultraviolet femtosecond amplifier system using a Ce3+:LiCaAlF6 crystal are reported. Firstly, a Bethune-type prismatic cell configuration that uniformly illuminates the four sides of a micro-pulling down method-grown crystal is used to amplify 290 nm, femtosecond pulses with no significant increase in pulse duration and B-integral. The second pumping scheme uses a two-side-pumped large crystal. These two side-pumping schemes can pave new possibilities for achieving high-energy ultraviolet femtosecond pulses.
Femtosecond Nonlinearities in Indium Gallium Arsenic Phosphide Diode Lasers

NASA Astrophysics Data System (ADS)

Hall, Katherine Lavin

Semiconductor optical amplifiers are receiving increasing attention for possible applications to broadband optical communication and switching systems. In this thesis we report the results of an extensive experimental study of the ultrafast gain and refractive index nonlinearities in 1.5 μm InGaAsP laser diode amplifiers. The temporal resolution afforded by the femtosecond optical pulses used in these experiments allows us to study carrier interactions with other carriers as well as carrier interactions with the lattice. The 100-200 fs optical pulses used in the pump -probe experiments are generated by an Additive Pulse Modelocked color center laser. The measured group velocity dispersion in the diodes ranged from -0.6 to -0.95 mu m^{-1 }. Differences in the group velocity for TE - and TM-polarized pulses suggested that cross-polarized pump-probe pulses walk off from each other in the diode. This walk-off can diminish the time resolution of some experiments. A novel heterodyne pump-probe technique was developed to distinguish collinear, copolarized, pump and probe pulses that were nominally at the same wavelength. Comparing cross-polarized and copolarized pump-probe results yielded new information about the physical mechanisms responsible for nonlinear gain in the diodes. We observed a gain compression across the entire bandwidth of the diode, associated with carrier heating. The hot carrier distribution cooled back to the lattice temperature with a 0.6 to 1.0 ps time constant, depending on the device structure. In addition, we observed a 0.1 to 0.25 ps delay in onset of carrier heating. Large gain compression due to two photon absorption was also observed. A small portion of the nonlinear gain is attributed to spectral hole burning. Pulsewidth-dependent output saturation energies were explained by a rate equation model that included the effect of carrier heating. Measurements of pump-induced probe phase changes revealed index nonlinearities due to delayed carrier
Optical synchronization system for femtosecond X-ray sources

DOEpatents

Wilcox, Russell B [El Cerrito, CA; Holzwarth, Ronald [Munich, DE

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.
Femtosecond laser lithotripsy: feasibility and ablation mechanism.

PubMed

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

2010-01-01

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 (lambda=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 microm, 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 microm, 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.
Multiphoton microscopy system with a compact fiber-based femtosecond-pulse laser and handheld probe

PubMed Central

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

2012-01-01

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

PubMed

Andersen, T V; Schmidt, O; Bruchmann, C; Limpert, J; Aguergaray, C; Cormier, E; Tünnermann, A

2006-05-29

We report on the generation of high energy femtosecond pulses at 1 MHz repetition rate from a fiber laser pumped optical parametric amplifier (OPA). Nonlinear bandwidth enhancement in fibers provides the intrinsically synchronized signal for the parametric amplifier. We demonstrate large tunability extending from 700 nm to 1500 nm of femtosecond pulses with pulse energies as high as 1.2 muJ when the OPA is seeded by a supercontinuum generated in a photonic crystal fiber. Broadband amplification over more than 85 nm is achieved at a fixed wavelength. Subsequent compression in a prism sequence resulted in 46 fs pulses. With an average power of 0.5 W these pulses have a peak-power above 10 MW. In particular, the average power and pulse energy scalability of both involved concepts, the fiber laser and the parametric amplifier, will enable easy up-scaling to higher powers.
Evolution of energy deposition during glass cutting with pulsed femtosecond laser radiation

NASA Astrophysics Data System (ADS)

Kalupka, C.; Großmann, D.; Reininghaus, M.

2017-05-01

We report on investigations of the energy deposition in the volume of thin glass during an ablation cutting process with pulsed femtosecond laser radiation by time-resolved pump-probe shadowgraphy. For a single laser pulse, the temporal evolution of the transient electronic excitation of the glass volume is imaged up to 10 ps after initial excitation. For an increasing number of laser pulses, the spatial excitation of the glass volume significantly changes compared to single pulse irradiation. Sharp spikes are observed, which reduce the transmission of the illuminating probe pulse. This indicates local maxima of the absorption and, therefore, energy deposition of the pump pulse energy in the glass volume. Furthermore, for an increasing number of pulses, different shapes of the surface ablation crater are observed. To study the correlation between the shape of the surface ablation crater and the energy deposition in the glass volume, simulations of the spatial intensity distribution of the pump pulse are executed by means of linear beam propagation method. We show that the transient excitation spikes observed by pump-probe shadowgraphy can be explained by refraction and diffraction of the laser radiation at the surface ablation crater. Our results provide an experimental validation for the physical reason of an ablation stop for an ablation cutting process. Moreover, the simulations allow for the prediction of damage inside the glass volume.
A Femtosecond Visible/Visible and Visible/Mid-Infrared Transient Absorption Study of the Light Harvesting Complex II

PubMed Central

Stahl, Andreas D.; Di Donato, Mariangela; van Stokkum, Ivo; van Grondelle, Rienk; Groot, Marie Louise

2009-01-01

Abstract Light harvesting complex II (LHCII) is the most abundant protein in the thylakoid membrane of higher plants and green algae. LHCII acts to collect solar radiation, transferring this energy mainly toward photosystem II, with a smaller amount going to photosystem I; it is then converted into a chemical, storable form. We performed time-resolved femtosecond visible pump/mid-infrared probe and visible pump/visible probe absorption difference spectroscopy on purified LHCII to gain insight into the energy transfer in this complex occurring in the femto-picosecond time regime. We find that information derived from mid-infrared spectra, together with structural and modeling information, provides a unique visualization of the flow of energy via the bottleneck pigment chlorophyll a604. PMID:20006959
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
Dynamics of femtosecond laser-induced periodic surface structures on silicon by high spatial and temporal resolution imaging

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

Jia, X., E-mail: jiaxin@sdju.edu.cn; Department of Mathematics and Physics, Shanghai Dianji University, Shanghai 201306; Jia, T. Q., E-mail: tqjia@phy.ecnu.edu.cn

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. Themore » 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.« less
Deciphering excited state evolution in halorhodopsin with stimulated emission pumping.

PubMed

Bismuth, Oshrat; Komm, Pavel; Friedman, Noga; Eliash, Tamar; Sheves, Mordechai; Ruhman, Sanford

2010-03-04

The primary photochemical dynamics of Hb. pharaonis Halorhodopsin (pHR) are investigated by femtosecond visible pump-near IR dump-hyperspectral probe spectroscopy. The efficiency of excited state depletion is deduced from transient changes in absorption, recorded with and without stimulated emission pumping (SEP), as a function of the dump delay. The concomitant reduction of photocycle population is assessed by probing the "K" intermediate difference spectrum. Results show that the cross section for stimulating emission is nearly constant throughout the fluorescent state lifetime. Probing "K" demonstrates that dumping produces a proportionate reduction in photocycle yields. We conclude that, despite its nonexponential internal conversion (IC) kinetics, the fluorescent state in pHR constitutes a single intermediate in the photocycle. This contrasts with conclusions drawn from the study of primary events in the related chloride pump from Hb. salinarum (sHR), believed to produce the "K" intermediate from a distinct short-lived subpopulation in the excited state. Our discoveries concerning internal conversion dynamics in pHR are discussed in light of recent expectations for similar excited state dynamics in both proteins.
High average power, widely tunable femtosecond laser source from red to mid-infrared based on an Yb-fiber-laser-pumped optical parametric oscillator.

PubMed

Gu, Chenglin; Hu, Minglie; Zhang, Limeng; Fan, Jintao; Song, Youjian; Wang, Chingyue; Reid, Derryck T

2013-06-01

We report on the highly efficient generation of widely tunable femtosecond pulses based on intracavity second harmonic generation (SHG) and sum frequency generation (SFG) in a MgO-doped periodically poled LiNbO(3) optical parametric oscillator (OPO), which is pumped by a Yb-doped large-mode-area photonics crystal fiber femtosecond laser. Red and near infrared from intracavity SHG and SFG and infrared signals were directly obtained from the OPO. A 2 mm β-BaB(2)O(4) is applied for Type I (oo → e) intracavity SHG and SFG, and then femtosecond laser pulses over 610 nm ~ 668 nm from SFG and 716 nm ~ 970 nm from SHG are obtained with high efficiency. In addition, the oscillator simultaneously generates signal and idler femtosecond pulses over 1450 nm ~ 2200 nm and 2250 nm ~ 4000 nm, respectively.
Pressure measurements using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering.

PubMed

Kearney, Sean P; Danehy, Paul M

2015-09-01

We investigate the feasibility of gas-phase pressure measurements using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is probed by a high-energy 5-ps pulse introduced at a time delay from the Raman preparation. These ultrafast laser pulses are shorter than collisional-dephasing time scales, enabling a new hybrid time- and frequency-domain detection scheme for pressure. Single-laser-shot rotational CARS spectra were recorded from N2 contained in a room-temperature gas cell for pressures from 0.4 to 3 atm and probe delays ranging from 16 to 298 ps. Sensitivity of the accuracy and precision of the pressure data to probe delay was investigated. The technique exhibits superior precision and comparable accuracy to previous laser-diagnostic pressure measurements.
Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime.

PubMed

Palacino-González, Elisa; Gelin, Maxim F; Domcke, Wolfgang

2017-12-13

We present a theoretical description of double-pump femtosecond single-molecule signals with fluorescence detection. We simulate these signals in the weak-field regime for a model mimicking a chromophore with a Franck-Condon-active vibrational mode. We establish several signatures of these signals which are characteristic for the weak-field regime. The signatures include the quenching of vibrational beatings by electronic dephasing and a pronounced tilt of the phase-time profiles in the two-dimensional (2D) maps. We study how environment-induced slow modulations of the electronic dephasing and relevant chromophore parameters (electronic energy, orientation, vibrational frequency and relative shift of the potential energy surfaces) affect the signals.

Stimulated emission and spontaneous loss pump-probe microscopy for background removal

NASA Astrophysics Data System (ADS)

Das, Subir; Ho, Bo-Wei; Kao, Fu-Jen

2018-02-01

In this work, we have established a double modulation lock-in detection technique using two semiconductor laser diodes in stimulated emission based pump-probe microscopy. By modulating the pump and probe beams at two different frequencies, f1 and f2, the signal is then recovered with the sum frequency, (f1+ f2), so as to minimize the leak-through noise due to the spontaneous emission caused by the pump beam. In this way, the DC background that is often attributed to the stimulated emission is effectively removed. Our technique has implemented in ATTO647N fluorescent dye which is applicable for many biological applications.
Laser emission from diode-pumped Nd:YAG ceramic waveguide lasers realized by direct femtosecond-laser writing technique.

PubMed

Salamu, Gabriela; Jipa, Florin; Zamfirescu, Marian; Pavel, Nicolaie

2014-03-10

We report on realization of buried waveguides in Nd:YAG ceramic media by direct femtosecond-laser writing technique and investigate the waveguides laser emission characteristics under the pump with fiber-coupled diode lasers. Laser pulses at 1.06 μm with energy of 2.8 mJ for the pump with pulses of 13.1-mJ energy and continuous-wave output power of 0.49 W with overall optical efficiency of 0.13 were obtained from a 100-μm diameter circular cladding waveguide realized in a 0.7-at.% Nd:YAG ceramic. A circular waveguide of 50-μm diameter yielded laser pulses at 1.3 μm with 1.2-mJ energy.
Following the dynamics of matter with femtosecond precision using the X-ray streaking method

DOE PAGES

David, C.; Karvinen, P.; Sikorski, M.; ...

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
5-nJ Femtosecond Ti3+:sapphire laser pumped with a single 1 W green diode

NASA Astrophysics Data System (ADS)

Muti, Abdullah; Kocabas, Askin; Sennaroglu, Alphan

2018-05-01

We report a Kerr-lens mode-locked, extended-cavity femtosecond Ti3+:sapphire laser directly pumped at 520 nm with a 1 W AlInGaN green diode. To obtain energy scaling, the short x-cavity was extended with a q-preserving multi-pass cavity to reduce the pulse repetition rate to 5.78 MHz. With 880 mW of incident pump power, we obtained as high as 90 mW of continuous-wave output power from the short cavity by using a 3% output coupler. In the Kerr-lens mode-locked regime, the extended cavity produced nearly transform-limited 95 fs pulses at 776 nm. The resulting energy and peak power of the pulses were 5.1 nJ and 53 kW, respectively. To our knowledge, this represents the highest pulse energy directly obtained to date from a mode-locked, single-diode-pumped Ti3+:sapphire laser.
Dynamics of photoprocesses induced by femtosecond infrared radiation in free molecules and clusters of iron pentacarbonyl

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

Kompanets, V. O.; Lokhman, V. N.; Poydashev, D. G., E-mail: poydashev@isan.troitsk.ru

2016-04-15

The dynamics of photoprocesses induced by femtosecond infrared radiation in free Fe(CO){sub 5} molecules and their clusters owing to the resonant excitation of vibrations of CO bonds in the 5-μm range has been studied. The technique of infrared excitation and photoionization probing (λ = 400 nm) by femtosecond pulses has been used in combination with time-of-flight mass spectrometry. It has been found that an infrared pulse selectively excites vibrations of CO bonds in free molecules, which results in a decrease in the yield of the Fe(CO){sub 5}{sup +} molecular ion. Subsequent relaxation processes have been analyzed and the results havemore » been interpreted. The time of the energy transfer from excited vibrations to other vibrations of the molecule owing to intramolecular relaxation has been measured. The dynamics of dissociation of [Fe(CO){sub 5}]{sub n} clusters irradiated by femtosecond infrared radiation has been studied. The time dependence of the yield of free molecules has been measured under different infrared laser excitation conditions. We have proposed a model that well describes the results of the experiment and makes it possible, in particular, to calculate the profile of variation of the temperature of clusters within the “evaporation ensemble” concept. The intramolecular and intracluster vibrational relaxation rates in [Fe(CO){sub 5}]{sub n} clusters have been estimated.« less
Towards attosecond measurement in molecules and at surfaces

NASA Astrophysics Data System (ADS)

Marangos, Jonathan

2015-05-01

1) We will present a number of experimental approaches that are being developed at Imperial College to make attosecond timescale measurements of electronic dynamics in suddenly photoionized molecules and at surfaces. A brief overview will be given of some of the unanswered questions in ultrafast electron and hole dynamics in molecules and solids. These questions include the existence of electronic charge migration in molecules and how this process might couple to nuclear motion even on the few femtosecond timescale. How the timescale of photoemission from a surface may differ from that of an isolated atom, e.g. due to electron transport phenomena associated with the distance from the surface of the emitting atom and the electron dispersion relation, is also an open question. 2) The measurement techniques we are currently developing to answer these questions are HHG spectroscopy, attosecond pump-probe photoelectron/photoion studies, and attosecond pump-probe transient absorption as well as attosecond streaking for measuring surface emission. We will present recent advances in generating two synchronized isolated attosecond pulses at different colours for pump-probe measurements (at 20 eV and 90 eV respectively). Results on generation of isolated attosecond pulses at 300 eV and higher photon energy using a few-cycle 1800 nm OPG source will be presented. The use of these resources for making pump-probe measurements will be discussed. Finally we will present the results of streaking measurement of photoemission wavepackets from two types of surface (WO3 and a evaporated Au film) that show a temporal broadening of ~ 100 as compared to atomic streaks that is consistent with the electron mean free path in these materials. Work supported by ERC and EPSRC.
Pump-probe spectroscopy and imaging of heme proteins: temperature effects and data analysis

NASA Astrophysics Data System (ADS)

Wang, Erkang; Domingue, Scott R.; Bartels, Randy A.; Wilson, Jesse W.

2017-08-01

Ultrafast pump-probe microscopy enables visualization of non-fluorescent materials in biological tissue, such as melanin and hemoglobin. Whereas transient absorption has been primarily a physical chemistry technique, used to gain insight into molecular and electronic structure, pump-probe microscopy represents a paradigm shift in translating transient absorption into an analytical technique, which can clearly resolve pigments with nearly indistinguishable linear absorption spectra. Extending this technique to other important targets, such as mitochondrial respiratory chain hemes, will require new laser sources and new data processing techniques to estimate heme content from the pump-probe response. We will present recent developments on both of these fronts. The laser system we have developed to elicit a pump probe response of respiratory chain hemes is based on an amplified Yb:fiber ultrafast laser that uses modest spectral broadening followed by sum frequency generation to produce a tunable pulse pair in the visible region. Wavelength tuning is accomplished by changing quasi-phase matching conditions. We will present preliminary imaging data in addition to discussing management of sample heating problems that arise from performing transient absorption measurements at the high repetition rates needed for imaging microscopy. In the second part of the talk, we will present the use of regularized and non-negative least squares fitting, along with feature-preserving noise removal to estimate composition of a pixel from its pump-probe response.
Femtosecond time-resolved vibrational SFG spectroscopy of CO/Ru( 0 0 1 )

NASA Astrophysics Data System (ADS)

Hess, Ch.; Wolf, M.; Roke, S.; Bonn, M.

2002-04-01

Vibrational sum-frequency generation (SFG) employing femtosecond infrared (IR) laser pulses is used to study the dynamics of the C-O stretch vibration on Ru(0 0 1). Time-resolved measurements of the free induction decay (FID) of the IR-polarization for 0.33 ML CO/Ru(0 0 1) exhibit single exponential decays over three decades corresponding to dephasing times of T2=1.94 ps at 95 K and T2=1.16 ps at 340 K. This is consistent with pure homogeneous broadening due to anharmonic coupling with the thermally activated low-frequency dephasing mode together with a contribution from saturation of the IR transition. In pump-probe SFG experiments using a strong visible (VIS) pump pulse the perturbation of the FID leads to transient line shifts even at negative delay times, i.e. when the IR-VIS SFG probe pair precedes the pump pulse. Based on an analysis of the time-dependent polarization we discuss the influence of the perturbed FID on time-resolved SFG spectra. We investigate how coherent effects affect the SFG spectra and we examine the time resolution in these experiments, in particular in dependence of the dephasing time.
Femtosecond deep-infrared optical parametric oscillator pumped directly by a Ti:sapphire laser

NASA Astrophysics Data System (ADS)

O'Donnell, Callum; Chaitanya Kumar, S.; Zawilski, Kevin T.; Schunemann, Peter G.; Ebrahim-Zadeh, Majid

2018-02-01

We report a high-repetition-rate femtosecond optical parametric oscillator (OPO) for the deep-infrared (deep-IR) based on the nonlinear optical crystal, CdSiP2 (CSP), pumped directly by a Ti:sapphire laser, for the first time. By pumping CSP at <1 μm, we have achieved practical output powers at the longest wavelengths generated by any Ti:sapphire-pumped OPO. Using a combination of pump wavelength tuning, type-I critical phase-matching, and cavity delay tuning, we have generated continuously tunable radiation across 6654-8373 nm (1194-1503 cm-1) at 80.5 MHz repetition rate, providing up to 20 mW of average power at 7314 nm and <7 mW beyond 8000 nm, with idler spectra exhibiting bandwidths of 140-180 nm across the tuning range. Moreover, the near-IR signal is tunable across 1127-1192 nm, providing up to 37 mW of average power at 1150 nm. Signal pulses, characterised using intensity autocorrelation, have durations of 260-320 fs, with corresponding time-bandwidth product of ΔυΔτ 1. The idler and signal output exhibit a TEM00 spatial profile with single-peak Gaussian distribution. With an equivalent spectral brightness of 6.68×1020 photons s-1 mm-2 sr-1 0.1% BW-1, this OPO represents a viable table-top alternative to synchrotron and supercontinuum sources for deep-IR applications in spectroscopy, metrology and medical diagnostics.
The effect of the Gouy phase in optical-pump-THz-probe spectroscopy.

PubMed

Ahmed, Saima; Savolainen, Janne; Hamm, Peter

2014-02-24

We show theoretically as well as experimentally that the Gouy-phase shift, which depends on the exact positioning of a sample in relation to the focus of a probe beam in a pump-probe experiment, may have a pronounced effect on the shape of the pump-probe signal. The effect occurs only when single-cycle probe pulses are used, i.e. when the slowly varying envelope approximation breaks down, while it disappears for multi-cycle pulses. The effect is thus most relevant in THz time-resolved spectroscopy, where such single cycle pulses are most commonly used, but it should not be overlooked also in other spectral regimes when correspondingly short pulses are involved.
Time-resolved coherent Raman spectroscopy by high-speed pump-probe delay scanning.

PubMed

Domingue, S R; Winters, D G; Bartels, R A

2014-07-15

Using a spinning window pump-probe delay scanner, we demonstrate a means of acquiring time-resolved vibrational spectra at rates up to 700 Hz. The time-dependent phase shift accumulated by the probe pulse in the presence of a coherently vibrating sample gives rise to a Raman-induced frequency shifting readily detectable in a balanced detector. This rapid delay scanning system represents a 23-fold increase in averaging speed and is >10× faster than state-of-the-art voice coil delay lines. These advancements make pump-probe spectroscopy a more practical means of imaging complex media.
Laser-Induced Damage with Femtosecond Pulses

NASA Astrophysics Data System (ADS)

Kafka, Kyle R. P.

The strong electric fields of focused femtosecond laser pulses lead to non-equilibrium dynamics in materials, which, beyond a threshold intensity, causes laser-induced damage (LID). Such a strongly non-linear and non-perturbative process renders important LID observables like fluence and intensity thresholds and damage morphology (crater) extremely difficult to predict quantitatively. However, femtosecond LID carries a high degree of precision, which has been exploited in various micro/nano-machining and surface engineering applications, such as human eye surgery and super-hydrophobic surfaces. This dissertation presents an array of experimental studies which have measured the damage behavior of various materials under femtosecond irradiation. Precision experiments were performed to produce extreme spatio-temporal confinement of the femtosecond laser-solid damage interaction on monocrystalline Cu, which made possible the first successful direct-benchmarking of LID simulation with realistic damage craters. A technique was developed to produce laser-induced periodic surface structures (LIPSS) in a single pulse (typically a multi-pulse phenomenon), and was used to perform a pump-probe study which revealed asynchronous LIPSS formation on copper. Combined with 1-D calculations, this new experimental result suggests more drastic electron heating than expected. Few-cycle pulses were used to study the LID performance and morphology of commercial ultra-broadband optics, which had not been systematically studied before. With extensive surface analysis, various morphologies were observed, including LIPSS, swelling (blisters), simple craters, and even ring-shaped structures, which varied depending on the coating design, number of pulses, and air/vacuum test environment. Mechanisms leading to these morphologies are discussed, many of which are ultrafast in nature. The applied damage behavior of multi-layer dielectric mirrors was measured and compared between long pulse (150 ps
Mapping Rotational Wavepacket Dynamics with Chirped Probe Pulses

NASA Astrophysics Data System (ADS)

Romanov, Dmitri; Odhner, Johanan; Levis, Robert

2014-05-01

We develop an analytical model description of the strong-field pump-probe polarization spectroscopy of rotational transients in molecular gases in a situation when the probe pulse is considerably chirped: the frequency modulation over the pulse duration is comparable with the carrier frequency. In this scenario, a femtosecond pump laser pulse prepares a rotational wavepacket in a gas-phase sample at room temperature. The rotational revivals of the wavepacket are then mapped onto a chirped broadband probe pulse derived from a laser filament. The slow-varying envelope approximation being inapplicable, an alternative approach is proposed which is capable of incorporating the substantial chirp and the related temporal dispersion of refractive indices. Analytical expressions are obtained for the probe signal modulation over the interaction region and for the resulting heterodyned transient birefringence spectra. Dependencies of the outputs on the probe pulse parameters reveal the trade-offs and the ways to optimize the temporal-spectral imaging. The results are in good agreement with the experiments on snapshot imaging of rotational revival patterns in nitrogen gas. We gratefully acknowledge financial support through AFOSR MURI Grant No. FA9550-10-1-0561.
Probing dynamics in colloidal crystals with pump-probe experiments at LCLS: Methodology and analysis

DOE PAGES

Mukharamova, Nastasia; Lazarev, Sergey; Meijer, Janne -Mieke; ...

2017-05-19

We present results of the studies of dynamics in colloidal crystals performed by pump-probe experiments using an X-ray free-electron laser (XFEL). Colloidal crystals were pumped with an infrared laser at a wavelength of 800 nm with varying power and probed by XFEL pulses at an energy of 8 keV with a time delay up to 1000 ps. The positions of the Bragg peaks, and their radial and azimuthal widths were analyzed as a function of the time delay. The spectral analysis of the data did not reveal significant enhancement of frequencies expected in this experiment. As a result, this allowedmore » us to conclude that the amplitude of vibrational modes excited in colloidal crystals was less than the systematic error caused by the noise level.« less
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.
Invited Review Article: Pump-probe microscopy

PubMed Central

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

2016-01-01

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
Femtosecond Cr:LiSAF and Cr:LiCAF lasers pumped by tapered diode lasers.

PubMed

Demirbas, Umit; Schmalz, Michael; Sumpf, Bernd; Erbert, Götz; Petrich, Gale S; Kolodziejski, Leslie A; Fujimoto, James G; Kärtner, Franz X; Leitenstorfer, Alfred

2011-10-10

We report compact, low-cost and efficient Cr:Colquiriite lasers that are pumped by high brightness tapered laser diodes. The tapered laser diodes provided 1 to 1.2 W of output power around 675 nm, at an electrical-to-optical conversion efficiency of about 30%. Using a single tapered diode laser as the pump source, we have demonstrated output powers of 500 mW and 410 mW together with slope efficiencies of 47% and 41% from continuous wave (cw) Cr:LiSAF and Cr:LiCAF lasers, respectively. In cw mode-locked operation, sub-100-fs pulse trains with average power between 200 mW and 250 mW were obtained at repetition rates around 100 MHz. Upon pumping the Cr:Colquiriite lasers with two tapered laser diodes (one from each side of the crystal), we have observed scaling of cw powers to 850 mW in Cr:LiSAF and to 650 mW in Cr:LiCAF. From the double side pumped Cr:LiCAF laser, we have also obtained ~220 fs long pulses with 5.4 nJ of pulse energy at 77 MHz repetition rate. These are the highest energy levels reported from Cr:Colquiriite so far at these repetition rates. Our findings indicate that tapered diodes in the red spectral region are likely to become the standard pump source for Cr:Colquiriite lasers in the near future. Moreover, the simplified pumping scheme might facilitate efficient commercialization of Cr:Colquiriite systems, bearing the potential to significantly boost applications of cw and femtosecond lasers in this spectral region (750-1000 nm).
In situ magnetic compensation for potassium spin-exchange relaxation-free magnetometer considering probe beam pumping effect.

PubMed

Fang, Jiancheng; Wang, Tao; Quan, Wei; Yuan, Heng; Zhang, Hong; Li, Yang; Zou, Sheng

2014-06-01

A novel method to compensate the residual magnetic field for an atomic magnetometer consisting of two perpendicular beams of polarizations was demonstrated in this paper. The method can realize magnetic compensation in the case where the pumping rate of the probe beam cannot be ignored. In the experiment, the probe beam is always linearly polarized, whereas, the probe beam contains a residual circular component due to the imperfection of the polarizer, which leads to the pumping effect of the probe beam. A simulation of the probe beam's optical rotation and pumping rate was demonstrated. At the optimized points, the wavelength of the probe beam was optimized to achieve the largest optical rotation. Although, there is a small circular component in the linearly polarized probe beam, the pumping rate of the probe beam was non-negligible at the optimized wavelength which if ignored would lead to inaccuracies in the magnetic field compensation. Therefore, the dynamic equation of spin evolution was solved by considering the pumping effect of the probe beam. Based on the quasi-static solution, a novel magnetic compensation method was proposed, which contains two main steps: (1) the non-pumping compensation and (2) the sequence compensation with a very specific sequence. After these two main steps, a three-axis in situ magnetic compensation was achieved. The compensation method was suitable to design closed-loop spin-exchange relaxation-free magnetometer. By a combination of the magnetic compensation and the optimization, the magnetic field sensitivity was approximately 4 fT/Hz(1/2), which was mainly dominated by the noise of the magnetic shield.
Ti : sapphire laser synchronised with femtosecond Yb pump laser via nonlinear pulse coupling in Ti : sapphire active medium

NASA Astrophysics Data System (ADS)

Didenko, N. V.; Konyashchenko, A. V.; Konyashchenko, D. A.; Kostryukov, P. V.; Kuritsyn, I. I.; Lutsenko, A. P.; Mavritskiy, A. O.

2017-02-01

A laser system utilising the method of synchronous pumping of a Ti : sapphire laser by a high-power femtosecond Yb3+-doped laser is described. The pulse repetition rate of the Ti : sapphire laser is successfully locked to the repetition rate of the Yb laser for more than 6 hours without the use of any additional electronics. The measured timing jitter is shown to be less than 1 fs. A simple qualitative model addressing the synchronisation mechanism utilising the cross-phase modulation of oscillation and pump pulses within a Ti : sapphire active medium is proposed. Output parameters of the Ti : sapphire laser as functions of its cavity length are discussed in terms of this model.
Initial Atomic Motion Immediately Following Femtosecond-Laser Excitation in Phase-Change Materials.

PubMed

Matsubara, E; Okada, S; Ichitsubo, T; Kawaguchi, T; Hirata, A; Guan, P F; Tokuda, K; Tanimura, K; Matsunaga, T; Chen, M W; Yamada, N

2016-09-23

Despite the fact that phase-change materials are widely used for data storage, no consensus exists on the unique mechanism of their ultrafast phase change and its accompanied large and rapid optical change. By using the pump-probe observation method combining a femtosecond optical laser and an x-ray free-electron laser, we substantiate experimentally that, in both GeTe and Ge_{2}Sb_{2}Te_{5} crystals, rattling motion of mainly Ge atoms takes place with keeping the off-center position just after femtosecond-optical-laser irradiation, which eventually leads to a higher symmetry or disordered state. This very initial rattling motion in the undistorted lattice can be related to instantaneous optical change due to the loss of resonant bonding that characterizes GeTe-based phase change materials. Based on the amorphous structure derived by first-principles molecular dynamics simulation, we infer a plausible ultrafast amorphization mechanism via nonmelting.

CW and femtosecond operation of a diode-pumped Yb:BaY(2)F(8) laser.

PubMed

Galzerano, G; Coluccelli, N; Gatti, D; Di Lieto, A; Tonelli, M; Laporta, P

2010-03-15

We report for the first time on laser action of a diode-pumped Yb:BaY(2)F(8) crystal. Both CW and femtosecond operations have been demonstrated at room-temperature conditions. A maximum output power of 0.56 W, a slope efficiency of 34%, and a tunability range from 1013 to 1067 nm have been obtained in CW regime. Transform-limited pulse trains with a minimum duration of 275 fs, an average power of 40 mW, and a repetition rate of 83 MHz have been achieved in a passive mode-locked regime using a semiconductor saturable absorber mirror.
Use of the Femtosecond Lasers in Ophthalmology

NASA Astrophysics Data System (ADS)

Roszkowska, Anna M.; Urso, Mario; Signorino, Alberto; Aragona, Pasquale

2018-01-01

Femtosecond laser (FSL) is an infrared laser with a wavelength of 1053 nm. FS laser works producing photodisruption or photoionization of the optically transparent tissue such as cornea. Currently FS lasers have a wide range of applications in ophthalmic surgery. They are used above all in corneal surgery in refractive procedures and keratoplasty, and recently in cataract surgery. The use of the FSL in corneal refractive surgery includes LASIK flap creation, astigmatic keratotomy, Femtosecond Lenticule Extraction (FLEx), Small Incision Lenticule Extraction (SMILE) and channels creation for implantation of the intrastromal corneal rings. As to the corneal grafting, the FS lasers are used in laser-assisted anterior and posterior lamellar keratoplasty and customized trephination in the penetrating keratoplasty. FS Laser Assisted Cataract Surgery (FLACS) includes capsulorrhexis and nuclear fragmentation that enhance safety and efficacy of the procedure.
Femtosecond few- to single-electron point-projection microscopy for nanoscale dynamic imaging

PubMed Central

Bainbridge, A. R.; Barlow Myers, C. W.; Bryan, W. A.

2016-01-01

Femtosecond electron microscopy produces real-space images of matter in a series of ultrafast snapshots. Pulses of electrons self-disperse under space-charge broadening, so without compression, the ideal operation mode is a single electron per pulse. Here, we demonstrate femtosecond single-electron point projection microscopy (fs-ePPM) in a laser-pump fs-e-probe configuration. The electrons have an energy of only 150 eV and take tens of picoseconds to propagate to the object under study. Nonetheless, we achieve a temporal resolution with a standard deviation of 114 fs (equivalent to a full-width at half-maximum of 269 ± 40 fs) combined with a spatial resolution of 100 nm, applied to a localized region of charge at the apex of a nanoscale metal tip induced by 30 fs 800 nm laser pulses at 50 kHz. These observations demonstrate real-space imaging of reversible processes, such as tracking charge distributions, is feasible whilst maintaining femtosecond resolution. Our findings could find application as a characterization method, which, depending on geometry, could resolve tens of femtoseconds and tens of nanometres. Dynamically imaging electric and magnetic fields and charge distributions on sub-micron length scales opens new avenues of ultrafast dynamics. Furthermore, through the use of active compression, such pulses are an ideal seed for few-femtosecond to attosecond imaging applications which will access sub-optical cycle processes in nanoplasmonics. PMID:27158637
Time-resolved polarization imaging by pump-probe (stimulated emission) fluorescence microscopy.

PubMed Central

Buehler, C; Dong, C Y; So, P T; French, T; Gratton, E

2000-01-01

We report the application of pump-probe fluorescence microscopy in time-resolved polarization imaging. We derived the equations governing the pump-probe stimulated emission process and characterized the pump and probe laser power levels for signal saturation. Our emphasis is to use this novel methodology to image polarization properties of fluorophores across entire cells. As a feasibility study, we imaged a 15-microm orange latex sphere and found that there is depolarization that is possibly due to energy transfer among fluorescent molecules inside the sphere. We also imaged a mouse fibroblast labeled with CellTracker Orange CMTMR (5-(and-6)-(((4-chloromethyl)benzoyl)amino)tetramethyl-rhodamine). We observed that Orange CMTMR complexed with gluthathione rotates fast, indicating the relatively low fluid-phase viscosity of the cytoplasmic microenvironment as seen by Orange CMTMR. The measured rotational correlation time ranged from approximately 30 to approximately 150 ps. This work demonstrates the effectiveness of stimulated emission measurements in acquiring high-resolution, time-resolved polarization information across the entire cell. PMID:10866979
In situ magnetic compensation for potassium spin-exchange relaxation-free magnetometer considering probe beam pumping effect

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

Fang, Jiancheng; Wang, Tao, E-mail: wangtaowt@aspe.buaa.edu.cn; Quan, Wei

2014-06-15

A novel method to compensate the residual magnetic field for an atomic magnetometer consisting of two perpendicular beams of polarizations was demonstrated in this paper. The method can realize magnetic compensation in the case where the pumping rate of the probe beam cannot be ignored. In the experiment, the probe beam is always linearly polarized, whereas, the probe beam contains a residual circular component due to the imperfection of the polarizer, which leads to the pumping effect of the probe beam. A simulation of the probe beam's optical rotation and pumping rate was demonstrated. At the optimized points, the wavelengthmore » of the probe beam was optimized to achieve the largest optical rotation. Although, there is a small circular component in the linearly polarized probe beam, the pumping rate of the probe beam was non-negligible at the optimized wavelength which if ignored would lead to inaccuracies in the magnetic field compensation. Therefore, the dynamic equation of spin evolution was solved by considering the pumping effect of the probe beam. Based on the quasi-static solution, a novel magnetic compensation method was proposed, which contains two main steps: (1) the non-pumping compensation and (2) the sequence compensation with a very specific sequence. After these two main steps, a three-axis in situ magnetic compensation was achieved. The compensation method was suitable to design closed-loop spin-exchange relaxation-free magnetometer. By a combination of the magnetic compensation and the optimization, the magnetic field sensitivity was approximately 4 fT/Hz{sup 1/2}, which was mainly dominated by the noise of the magnetic shield.« less
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.
Photoinduced electron-transfer in perylenediimide triphenylamine-based dendrimers: single photon timing and femtosecond transient absorption spectroscopy.

PubMed

Fron, Eduard; Pilot, Roberto; Schweitzer, Gerd; Qu, Jianqiang; Herrmann, Andreas; Müllen, Klaus; Hofkens, Johan; Van der Auweraer, Mark; De Schryver, Frans C

2008-05-01

The excited state dynamics of two generations perylenediimide chromophores substituted in the bay area with dendritic branches bearing triphenylamine units as well as those of the respective reference compounds are investigated. Using single photon timing and multi-pulse femtosecond transient absorption experiments a direct proof of a reversible charge transfer occurring from the peripheral triphenylamine to the electron acceptor perylenediimide core is revealed. Femtosecond pump-dump-probe experiments provide evidence for the ground state dynamics by populating excited vibronic levels. It is found by the means of both techniques that the rotational isomerization of the dendritic branches occurs on a time scale that ranges up to 1 ns. This time scale of the isomerization depends on the size of the dendritic arms and is similar both in the ground and excited state.
The changing landscape of dermatology practice: melanoma and pump-probe laser microscopy.

PubMed

Puza, Charles J; Mosca, Paul J

2017-11-01

To present current melanoma diagnosis, staging, prognosis, and treatment algorithms and how recent advances in laser pump-probe microscopy will fill in the gaps in our clinical understanding. Expert opinion and significantly cited articles identified in SCOPUS were used in conjunction with a pubmed database search on Melanoma practice guidelines from the last 10 years. Significant advances in melanoma treatment have been made over the last decade. However, proper treatment algorithm and prognostic information per melanoma stage remain controversial. The next step for providers will involve the identification of patient population(s) that can benefit from recent advances. One method of identifying potential patients is through new laser imaging techniques. Pump-probe laser microscopy has been shown to correctly identify nevi from melanoma and furthermore stratify melanoma by aggressiveness. The recent development of effective adjuvant therapies for melanoma is promising and should be utilized on appropriate patient populations that can potentially be identified using pump-probe laser microscopy.
Femtosecond time-resolved MeV electron diffraction

DOE PAGES

Zhu, Pengfei; Zhu, Y.; Hidaka, Y.; ...

2015-06-02

We report the experimental demonstration of femtosecond electron diffraction using high-brightness MeV electron beams. High-quality, single-shot electron diffraction patterns for both polycrystalline aluminum and single-crystal 1T-TaS 2 are obtained utilizing a 5 fC (~3 × 10 4 electrons) pulse of electrons at 2.8 MeV. The high quality of the electron diffraction patterns confirms that electron beam has a normalized emittance of ~50 nm rad. The transverse and longitudinal coherence length is ~11 and ~2.5 nm, respectively. The timing jitter between the pump laser and probe electron beam was found to be ~100 fs (rms). The temporal resolution is demonstrated bymore » observing the evolution of Bragg and superlattice peaks of 1T-TaS 2 following an 800 nm optical pump and was found to be 130 fs. Lastly, our results demonstrate the advantages of MeV electrons, including large elastic differential scattering cross-section and access to high-order reflections, and the feasibility of ultimately realizing below 10 fs time-resolved electron diffraction.« less
Using ultrashort terahertz pulses to directly probe spin dynamics in insulating antiferromagnets

NASA Astrophysics Data System (ADS)

Bowlan, P.; Trugman, S. A.; Yarotski, D. A.; Taylor, A. J.; Prasankumar, R. P.

2018-05-01

Terahertz pulses are a direct and general probe of ultrafast spin dynamics in insulating antiferromagnets (AFM). This is shown by using optical-pump, THz-probe spectroscopy to directly track AFM spin dynamics in the hexagonal multiferroic HoMnO3 and the orthorhombic multiferroic TbMnO3. Our studies show that despite the different structural and spin orders in these materials, THz pulses can unambiguously resolve spin dynamics after optical photoexcitation. We believe that this approach is quite general and can be applied to a broad range of materials with different AFM spin alignments, providing a novel non-contact approach for probing AFM order with femtosecond temporal resolution.
Femtosecond nonlinear ultrasonics in gold probed with ultrashort surface plasmons.

PubMed

Temnov, Vasily V; Klieber, Christoph; Nelson, Keith A; Thomay, Tim; Knittel, Vanessa; Leitenstorfer, Alfred; Makarov, Denys; Albrecht, Manfred; Bratschitsch, Rudolf

2013-01-01

Fundamental interactions induced by lattice vibrations on ultrafast time scales have become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the terahertz-frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here we report on the generation and nonlinear propagation of giant (1 per cent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for unambiguous characterization of arbitrary ultrafast acoustic transients. The giant acoustic pulses experience substantial nonlinear reshaping after a propagation distance of only 100 nm in a crystalline gold layer. Excellent agreement with the Korteveg-de Vries model points to future quantitative nonlinear femtosecond terahertz-ultrasonics at the nano-scale in metals at room temperature.
Broadband two-dimensional electronic spectroscopy in an actively phase stabilized pump-probe configuration.

PubMed

Zhu, Weida; Wang, Rui; Zhang, Chunfeng; Wang, Guodong; Liu, Yunlong; Zhao, Wei; Dai, Xingcan; Wang, Xiaoyong; Cerullo, Giulio; Cundiff, Steven; Xiao, Min

2017-09-04

We introduce a novel configuration for two-dimensional electronic spectroscopy (2DES) that combines the partially collinear pump-probe geometry with active phase locking. We demonstrate the method on a solution sample of CdSe/ZnS nanocrystals by employing two non-collinear optical parametric amplifiers as the pump and probe sources. The two collinear pump pulse replicas are created using a Mach-Zehnder interferometer phase stabilized by active feedback electronics. Taking the advantage of separated paths of the two pump pulses in the interferometer, we improve the signal-to-noise ratio with double modulation of the individual pump beams. In addition, a quartz wedge pair manipulates the phase difference between the two pump pulses, enabling the recovery of the rephasing and non-rephasing signals. Our setup integrates many advantages of available 2DES techniques with robust phase stabilization, ultrafast time resolution, two-color operation, long delay scan, individual polarization manipulation and the ease of implementation.
Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons.

PubMed

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

2016-02-05

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.
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.
Pump-probe differencing technique for cavity-enhanced, noise-canceling saturation laser spectroscopy.

PubMed

de Vine, Glenn; McClelland, David E; Gray, Malcolm B; Close, John D

2005-05-15

We present an experimental technique that permits mechanical-noise-free, cavity-enhanced frequency measurements of an atomic transition and its hyperfine structure. We employ the 532-nm frequency-doubled output from a Nd:YAG laser and an iodine vapor cell. The cell is placed in a folded ring cavity (FRC) with counterpropagating pump and probe beams. The FRC is locked with the Pound-Drever-Hall technique. Mechanical noise is rejected by differencing the pump and probe signals. In addition, this differenced error signal provides a sensitive measure of differential nonlinearity within the FRC.
Time-resolved investigations of the non-thermal ablation process of graphite induced by femtosecond laser pulses

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

Kalupka, C., E-mail: christian.kalupka@llt.rwth-aachen.de; Finger, J.; Reininghaus, M.

2016-04-21

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 ofmore » 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.« less
Pump-probe study of the formation of rubidium molecules by ultrafast photoassociation of ultracold atoms

NASA Astrophysics Data System (ADS)

McCabe, David J.; England, Duncan G.; Martay, Hugo E. L.; Friedman, Melissa E.; Petrovic, Jovana; Dimova, Emiliya; Chatel, Béatrice; Walmsley, Ian A.

2009-09-01

An experimental pump-probe study of the photoassociative creation of translationally ultracold rubidium molecules is presented together with numerical simulations of the process. The formation of loosely bound excited-state dimers is observed as a first step toward a fully coherent pump-dump approach to the stabilization of Rb2 into its lowest ground vibrational states. The population that contributes to the pump-probe process is characterized and found to be distinct from a background population of preassociated molecules.
Properties of optical breakdown in BK7 glass induced by an extended-cavity femtosecond laser oscillator.

PubMed

Do, Binh T; Phillips, Mark C; Miller, Paul A; Kimmel, Mark W; Britsch, Justin; Cho, Seong-Ho

2009-02-16

Using an extended-cavity femtosecond oscillator, we investigated optical breakdown in BK7 glass caused by the accumulated action of many laser pulses. By using a pump-probe experiment and collecting the transmitted pump along with the reflected pump and the broadband light generated by the optical breakdown, we measured the build-up time to optical breakdown as a function of the pulse energy, and we also observed the instability of the plasma due to the effect of defocusing and shielding created by the electron gas. The spectrum of the broadband light emitted by the optical breakdown and the origin of the material modification in BK7 glass was studied. We developed a simple model of electromagnetic wave propagation in plasma that is consistent with the observed behavior of the reflection, absorption, and transmission of the laser light.
Resolution enhancement of pump-probe microscope with an inverse-annular filter

NASA Astrophysics Data System (ADS)

Kobayashi, Takayoshi; Kawasumi, Koshi; Miyazaki, Jun; Nakata, Kazuaki

2018-04-01

Optical pump-probe microscopy can provide images by detecting changes in probe light intensity induced by stimulated emission, photoinduced absorbance change, or photothermal-induced refractive index change in either transmission or reflection mode. Photothermal microscopy, which is one type of optical pump-probe microscopy, has intrinsically super resolution capability due to the bilinear dependence of signal intensity of pump and probe. We introduce new techniques for further resolution enhancement and fast imaging in photothermal microscope. First, we introduce a new pupil filter, an inverse-annular pupil filter in a pump-probe photothermal microscope, which provides resolution enhancement in three dimensions. The resolutions are proved to be improved in lateral and axial directions by imaging experiment using 20-nm gold nanoparticles. The improvement in X (perpendicular to the common pump and probe polarization direction), Y (parallel to the polarization direction), and Z (axial direction) are by 15 ± 6, 8 ± 8, and 21 ± 2% from the resolution without a pupil filter. The resolution enhancement is even better than the calculation using vector field, which predicts the corresponding enhancement of 11, 8, and 6%. The discussion is made to explain the unexpected results. We also demonstrate the photothermal imaging of thick biological samples (cells from rabbit intestine and kidney) stained with hematoxylin and eosin dye with the inverse-annular filter. Second, a fast, high-sensitivity photothermal microscope is developed by implementing a spatially segmented balanced detection scheme into a laser scanning microscope using a Galvano mirror. We confirm a 4.9 times improvement in signal-to-noise ratio in the spatially segmented balanced detection compared with that of conventional detection. The system demonstrates simultaneous bi-modal photothermal and confocal fluorescence imaging of transgenic mouse brain tissue with a pixel dwell time of 20 µs. The
Femtosecond laser spectroscopy of the rhodopsin photochromic reaction: a concept for ultrafast optical molecular switch creation (ultrafast reversible photoreaction of rhodopsin).

PubMed

Smitienko, Olga; Nadtochenko, Victor; Feldman, Tatiana; Balatskaya, Maria; Shelaev, Ivan; Gostev, Fedor; Sarkisov, Oleg; Ostrovsky, Mikhail

2014-11-11

Ultrafast reverse photoreaction of visual pigment rhodopsin in the femtosecond time range at room temperature is demonstrated. Femtosecond two-pump probe experiments with a time resolution of 25 fs have been performed. The first рump pulse at 500 nm initiated cis-trans photoisomerization of rhodopsin chromophore, 11-cis retinal, which resulted in the formation of the primary ground-state photoproduct within a mere 200 fs. The second pump pulse at 620 nm with a varying delay of 200 to 3750 fs relative to the first рump pulse, initiated the reverse phototransition of the primary photoproduct to rhodopsin. The results of this photoconversion have been observed on the differential spectra obtained after the action of two pump pulses at a time delay of 100 ps. It was found that optical density decreased at 560 nm in the spectral region of bathorhodopsin absorption and increased at 480 nm, where rhodopsin absorbs. Rhodopsin photoswitching efficiency shows oscillations as a function of the time delay between two рump pulses. The quantum yield of reverse photoreaction initiated by the second pump pulse falls within the range 15%±1%. The molecular mechanism of the ultrafast reversible photoreaction of visual pigment rhodopsin may be used as a concept for the development of an ultrafast optical molecular switch.

Ultrafast quantum control of ionization dynamics in krypton.

PubMed

Hütten, Konrad; Mittermair, Michael; Stock, Sebastian O; Beerwerth, Randolf; Shirvanyan, Vahe; Riemensberger, Johann; Duensing, Andreas; Heider, Rupert; Wagner, Martin S; Guggenmos, Alexander; Fritzsche, Stephan; Kabachnik, Nikolay M; Kienberger, Reinhard; Bernhardt, Birgitta

2018-02-19

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.
Mode coupling enhancement by astigmatism compensation in a femtosecond laser cavity

NASA Astrophysics Data System (ADS)

Castro-Olvera, Gustavo; Garduño-Mejía, Jesus; Rosete-Aguilar, Martha; Roman-Moreno, Carlos J.

2016-09-01

In this work we present a numerical analysis of the mode coupling between the pump-beam and the laser-beam in a Ti:Sapphire crystal used as a gain medium of a femtosecond laser. Using the Matrix ABCD and propagation gaussian beam models, we obtained an optimal configuration for compensate the astigmatism in the output beam laser. Also we analysed pump-beam propagation and got the settings to fix the astigmatism in the crystal. Furthermore we apply this configuration to a homemade femtosecond laser, accomplishing an overall efficiency of laser to 20% in continuum wave (CW) and 16% in mode looking (ML) operation. The femtosecond laser have 30 nm bandwidth to FWHM at 810 nm corresponding 30fs.
Proton transfer mediated by the vibronic coupling in oxygen core ionized states of glyoxalmonoxime studied by infrared-X-ray pump-probe spectroscopy.

PubMed

Felicíssimo, V C; Guimarães, F F; Cesar, A; Gel'mukhanov, F; Agren, H

2006-11-30

The theory of IR-X-ray pump-probe spectroscopy beyond the Born-Oppenheimer approximation is developed and applied to the study of the dynamics of intramolecular proton transfer in glyoxalmonoxime leading to the formation of the tautomer 2-nitrosoethenol. Due to the IR pump pulses the molecule gains sufficient energy to promote a proton to a weakly bound well. A femtosecond X-ray pulse snapshots the wave packet route and, hence, the dynamics of the proton transfer. The glyoxalmonoxime molecule contains two chemically nonequivalent oxygen atoms that possess distinct roles in the hydrogen bond, a hydrogen donor and an acceptor. Core ionizations of these form two intersecting core-ionized states, the vibronic coupling between which along the OH stretching mode partially delocalizes the core hole, resulting in a hopping of the core hole from one site to another. This, in turn, affects the dynamics of the proton transfer in the core-ionized state. The quantum dynamical simulations of X-ray photoelectron spectra of glyoxalmonoxime driven by strong IR pulses demonstrate the general applicability of the technique for studies of intramolecular proton transfer in systems with vibronic coupling.
Time and frequency pump-probe multiplexing to enhance the signal response of Brillouin optical time-domain analyzers.

PubMed

Soto, Marcelo A; Ricchiuti, Amelia Lavinia; Zhang, Liang; Barrera, David; Sales, Salvador; Thévenaz, Luc

2014-11-17

A technique to enhance the response and performance of Brillouin distributed fiber sensors is proposed and experimentally validated. The method consists in creating a multi-frequency pump pulse interacting with a matching multi-frequency continuous-wave probe. To avoid nonlinear cross-interaction between spectral lines, the method requires that the distinct pump pulse components and temporal traces reaching the photo-detector are subject to wavelength-selective delaying. This way the total pump and probe powers launched into the fiber can be incrementally boosted beyond the thresholds imposed by nonlinear effects. As a consequence of the multiplied pump-probe Brillouin interactions occurring along the fiber, the sensor response can be enhanced in exact proportion to the number of spectral components. The method is experimentally validated in a 50 km-long distributed optical fiber sensor augmented to 3 pump-probe spectral pairs, demonstrating a signal-to-noise ratio enhancement of 4.8 dB.
Acceleration of a ground-state reaction by selective femtosecond-infrared-laser-pulse excitation

NASA Astrophysics Data System (ADS)

Stensitzki, Till; Yang, Yang; Kozich, Valeri; Ahmed, Ashour A.; Kössl, Florian; Kühn, Oliver; Heyne, Karsten

2018-02-01

Infrared (IR) excitation of vibrations that participate in the reaction coordinate of an otherwise thermally driven chemical reaction are believed to lead to its acceleration. Attempts at the practical realization of this concept have been hampered so far by competing processes leading to sample heating. Here we demonstrate, using femtosecond IR-pump IR-probe experiments, the acceleration of urethane and polyurethane formation due to vibrational excitation of the reactants for 1:1 mixtures of phenylisocyanate and cyclohexanol, and toluene-2,4-diisocyanate and 2,2,2-trichloroethane-1,1-diol, respectively. We measured reaction rate changes upon selective vibrational excitation with negligible heating of the sample and observed an increase of the reaction rate up to 24%. The observation is rationalized using reactant and transition-state structures obtained from quantum chemical calculations. We subsequently used IR-driven reaction acceleration to write a polyurethane square on sample windows using a femtosecond IR pulse.
Double photoionization of the Be isoelectronic sequence

NASA Astrophysics Data System (ADS)

Barmaki, S.; Albert, M. A.; Belliveau, J.; Laulan, S.

2018-05-01

We investigate the double photoionization (DPI) process along the Be isoelectronic sequence (Be‑Ne6+) by solving the time-dependent Schrödinger equation with a spectral method of configuration interaction type. The results that we obtain of the DPI cross sections are in a good agreement with other reported data. We also present the first results of double-to-single photoionization cross sections ratios for Be-like ions in support of possible photofragmentation experiments with x-ray free electron lasers. Finally, we probe the mutual interaction of the valence electrons at different photon energies and examine the subsequent redistribution of the excess photon energy among them.
High-power Femtosecond Optical Parametric Amplification at 1 kHz in BiB(3)O(6) pumped at 800 nm.

PubMed

Petrov, Valentin; Noack, Frank; Tzankov, Pancho; Ghotbi, Masood; Ebrahim-Zadeh, Majid; Nikolov, Ivailo; Buchvarov, Ivan

2007-01-22

Substantial power scaling of a travelling-wave femtosecond optical parametric amplifier, pumped near 800 nm by a 1 kHz Ti:sapphire laser amplifier, is demonstrated using monoclinic BiB(3)O(6) in a two stage scheme with continuum seeding. Total energy output (signal plus idler) exceeding 1 mJ is achieved, corresponding to an intrinsic conversion efficiency of approximately 32% for the second stage. The tunability extends from 1.1 to 2.9 microm. The high parametric gain and broad amplification bandwidth of this crystal allowed the maintenance of the pump pulse duration, leading to pulse lengths less than 140 fs, both for the signal and idler pulses, even at such high output levels.
Pump/Probe Angular Dependence of Hanle Electromagnetically Induced Transparency

NASA Astrophysics Data System (ADS)

Jackson, Richard; Campbell, Kaleb; Crescimanno, Michael; Bali, Samir

2015-05-01

We investigate the dependence of Hanle Electromagnetically Induced Transparency (EIT) on angular separation between pump and probe field propagation directions in room-temperature Rb vapor. We observe the FWHM of the probe transmission spectrum and the amplitude of the EIT signal while varying the angular separation from 0 to 1 milliradian. Following the work of Ref., we examine potential applications in information storage and retrieval. We are grateful to Miami University for their generous financial support, and to the Miami University Instrumentation lab for their invaluable contributions.
Single laser based pump-probe technique to study plasma shielding during nanosecond laser ablation of copper thin films

NASA Astrophysics Data System (ADS)

Nammi, Srinagalakshmi; Vasa, Nilesh J.; Gurusamy, Balaganesan; Mathur, Anil C.

2017-09-01

A plasma shielding phenomenon and its influence on micromachining is studied experimentally and theoretically for laser wavelengths of 355 nm, 532 nm and 1064 nm. A time resolved pump-probe technique is proposed and demonstrated by splitting a single nanosecond Nd3+:YAG laser into an ablation laser (pump laser) and a probe laser to understand the influence of plasma shielding on laser ablation of copper (Cu) clad on polyimide thin films. The proposed nanosecond pump-probe technique allows simultaneous measurement of the absorption characteristics of plasma produced during Cu film ablation by the pump laser. Experimental measurements of the probe intensity distinctly show that the absorption by the ablated plume increases with increase in the pump intensity, as a result of plasma shielding. Theoretical estimation of the intensity of the transmitted pump beam based on the thermo-temporal modeling is in qualitative agreement with the pump-probe based experimental measurements. The theoretical estimate of the depth attained for a single pulse with high pump intensity value on a Cu thin film is limited by the plasma shielding of the incident laser beam, similar to that observed experimentally. Further, the depth of micro-channels produced shows a similar trend for all three wavelengths, however, the channel depth achieved is lesser at the wavelength of 1064 nm.
Femtosecond diffraction dynamics of laser-induced periodic surface structures on fused silica

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

Hoehm, S.; Rosenfeld, A.; Krueger, J.

2013-02-04

The formation of laser-induced periodic surface structures (LIPSS) on fused silica upon irradiation with linearly polarized fs-laser pulses (50 fs pulse duration, 800 nm center wavelength) is studied experimentally using a transillumination femtosecond time-resolved (0.1 ps-1 ns) pump-probe diffraction approach. This allows to reveal the generation dynamics of near-wavelength-sized LIPSS showing a transient diffraction at specific spatial frequencies even before a corresponding permanent surface relief was observed. The results confirm that the ultrafast energy deposition to the materials surface plays a key role and triggers subsequent physical mechanisms such as carrier scattering into self-trapped excitons.
Ultrafast dynamics of electrons in ammonia.

PubMed

Vöhringer, Peter

2015-04-01

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

PubMed

Sukhoivanov, Igor A; Iakushev, Sergii O; Shulika, Oleksiy V; Díez, Antonio; Andrés, Miguel

2013-07-29

Formation of parabolic pulses at femtosecond time scale by means of passive nonlinear reshaping in normally dispersive optical fibers is analyzed. Two approaches are examined and compared: the parabolic waveform formation in transient propagation regime and parabolic waveform formation in the steady-state propagation regime. It is found that both approaches could produce parabolic pulses as short as few hundred femtoseconds applying commercially available fibers, specially designed all-normal dispersion photonic crystal fiber and modern femtosecond lasers for pumping. The ranges of parameters providing parabolic pulse formation at the femtosecond time scale are found depending on the initial pulse duration, chirp and energy. Applicability of different fibers for femtosecond pulse shaping is analyzed. Recommendation for shortest parabolic pulse formation is made based on the analysis presented.
Mapping CTTS dynamics of Na- in tetrahydrofurane with ultrafast multichannel pump-probe spectroscopy.

PubMed

Shoshana, O; Pérez Lustres, J L; Ernsting, N P; Ruhman, S

2006-06-14

Using multichannel femtosecond spectroscopy we have followed Na- charge transfer to solvent (CTTS) dynamics in THF solution. Absorption of the primary photoproducts in the visible, resolved here for the first time, consists of an asymmetric triplet centered at 595 nm, which we assign to a metastable incompletely solvated neutral atomic sodium species. Decay of this feature within approximately 1 ps to a broad and structureless solvated neutral is accompanied by broadening and loss of spectral detail. Kinetic analysis shows that both the spectral structure and the decay of this band are independent of the excitation photon frequency in the range 400-800 nm. With different pump-probe polarizations the anisotropy in transient transmission has been charted and its variation with excitation wavelength surveyed. The anisotropies are assigned to the reactant bleach, indicating that due to solvent-induced symmetry breaking, the CTTS absorption band of Na- is made up of discreet orthogonally polarized sub bands. None of the anisotropy in transient absorption could be associated with the photoproduct triplet band even at the earliest measurable time delays. Along with the documented differences in the spatial distribution of ejected electrons across the tested excitation wavelength range, these results lead us to conclude that photoejection is extremely rapid, and that loss of correlations between the departing electron and its neutral core is faster than our time resolution of approximately 60 fs.
Efficient neutron generation from solid-nanoparticle explosions driven by DPSSL-pumped high-repetition rate femtosecond laser pulse

NASA Astrophysics Data System (ADS)

Watari, T.; Matsukado, K.; Sekine, T.; Takeuchi, Y.; Hatano, Y.; Yoshimura, R.; Satoh, N.; Nishihara, K.; Takagi, M.; Kawashima, T.

2016-03-01

We propose novel neutron source using high-intensity laser based on the cluster fusion scheme. We developed DPSSL-pumped high-repetition-rate 20-TW laser system and solid nanoparticle target for neutron generation demonstration. In our neutron generation experiment, high-energy deuterons were generated from coulomb explosion of CD solid- nanoparticles and neutrons were generated by DD fusion reaction. Efficient and stable neutron generation was obtained by irradiating an intense femtosecond laser pulse of >2×1018 W/cm2. A yield of ∼105 neutrons per shot was stably observed during 0.1-1 Hz continuous operation.
Generation and subsequent amplification of few-cycle femtosecond pulses from a picosecond pump laser

NASA Astrophysics Data System (ADS)

Mukhin, I. B.; Kuznetsov, I. I.; Palashov, O. V.

2018-04-01

Using a new approach, in which generation of femtosecond pulses as short as a few field cycles is implemented directly from the radiation of a picosecond pump laser, pulses with the microjoule energy, the repetition rate 10 kHz, and the duration less than 26 fs are generated in the spectral range 1.3 ‑ 1.4 μm. In the process of generating this radiation, use was made of a method providing passive phase stabilisation of the carrier oscillation of the electromagnetic field and its slow envelope. The radiation spectrum was converted into the range of parametric amplification in the BBO crystal by the broadband second harmonic generation; the pulse was parametrically amplified up to the microjoule level and compressed by chirped mirrors to a duration of 28 fs.
Simulating Energy Relaxation in Pump-Probe Vibrational Spectroscopy of Hydrogen-Bonded Liquids.

PubMed

Dettori, Riccardo; Ceriotti, Michele; Hunger, Johannes; Melis, Claudio; Colombo, Luciano; Donadio, Davide

2017-03-14

We introduce a nonequilibrium molecular dynamics simulation approach, based on the generalized Langevin equation, to study vibrational energy relaxation in pump-probe spectroscopy. A colored noise thermostat is used to selectively excite a set of vibrational modes, leaving the other modes nearly unperturbed, to mimic the effect of a monochromatic laser pump. Energy relaxation is probed by analyzing the evolution of the system after excitation in the microcanonical ensemble, thus providing direct information about the energy redistribution paths at the molecular level and their time scale. The method is applied to hydrogen-bonded molecular liquids, specifically deuterated methanol and water, providing a robust picture of energy relaxation at the molecular scale.
Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.

PubMed

Loh, Zhi-Heng; Khalil, Munira; Correa, Raoul E; Santra, Robin; Buth, Christian; Leone, Stephen R

2007-04-06

Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m quantum state distribution of Xe+ produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution rhoj,|m| of rho3/2,1/2ratiorho1/2,1/2ratiorho3/2,3/2=75+/-6 :12+/-3 :13+/-6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.
Discriminating Bio-aerosols from Non-Bio-aerosols in Real-Time by Pump-Probe Spectroscopy

PubMed Central

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

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

PubMed

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

2016-09-13

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.

Communication: hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering thermometry using a narrowband time-asymmetric probe pulse.

PubMed

Stauffer, Hans U; Miller, Joseph D; Roy, Sukesh; Gord, James R; Meyer, Terrence R

2012-03-21

A narrowband, time-asymmetric probe pulse is introduced into the hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering (fs/ps RCARS) technique to provide accurate and precise single-shot, high-repetition-rate gas-phase thermometric measurements. This narrowband pulse-generated by inserting a Fabry-Pérot étalon into the probe-pulse beam path-enables frequency-domain detection of pure-rotational transitions. The unique time-asymmetric nature of this pulse, in turn, allows for detection of resonant Raman-active rotational transitions free of signal contamination by nonresonant four-wave-mixing processes while still allowing detection at short probe-pulse delays, where collisional dephasing processes are negligible. We demonstrate that this approach provides excellent single-shot thermometric accuracy (<1% error) and precision (~2.5%) in gas-phase environments. © 2012 American Institute of Physics
Pump-probe microscopy of respiratory chain pigments: towards non-fluorescent label-free metabolic imaging

NASA Astrophysics Data System (ADS)

Domingue, Scott R.; Chicco, Adam J.; Bartels, Randy A.; Wilson, Jesse W.

2017-02-01

Current label-free metabolic microscopy techniques are limited to obtaining contrast from fluorescent molecules NAD(P)H and FAD+, and are unable to determine redox state along the mitochondrial respiratory chain itself. The respiratory chain electron carriers do not fluoresce, but some are heme proteins that have redox-dependent absorption spectra. The most prominent of these, cytochrome c, has been extensively characterized by transient absorption spectroscopy, which suggests that pump-probe measurements in the vicinity of 450 - 600 nm can provide strong contrast between its redox states. Motivated by the success of pump-probe microscopy targeting another heme protein, hemoglobin, we seek to extend the technique to the cytochromes, with the ultimate goal of dissecting respiratory chain function of individual cells in live tissue. To that end, we have developed a new optical system producing ultrafast, visible, independently-tunable pulse pairs via sum-frequency generation of nonlinearly broadened pulses in periodically-poled lithium niobate. The system is pumped by a homebuilt fiber-based oscillator/amplifier emitting 1060 nm pulses at 1.3 W (63 MHz repetition rate), and produces tunable pulses in the vicinity of 488 and 532 nm. Pump-probe spectroscopy of cytochrome c with this source reveals differences in excited-state absorption relaxation times between redox states. Though redox contrast is weak with this setup, we argue that this can be improved with a resonant galvo-scanning microscope. Moreover, pump-probe images were acquired of brown adipose tissue (which contains dense mitochondria), demonstrating label-free contrast from excited-state absorption in respiratory chain hemes.
Efficient terahertz wave generation from GaP crystals pumped by chirp-controlled pulses from femtosecond photonic crystal fiber amplifier

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

Li, Jiang; Shi, Junkai; Xu, Baozhong

2014-01-20

A chirp-tunable femtosecond 10 W, 42 MHz photonic-crystal-fiber oscillator-amplifier system that is capable of delivering sub-60 fs light pulses at 1040 nm is used to demonstrate high-efficiency terahertz radiation generation via optical rectification in GaP crystals only a few millimeters in length. The optimization of the chirp of the fiber-laser pulses is shown to radically enhance the terahertz output, indicating one possible way to more efficiently use these extended nonlinear crystals in compact fiber-pumped terahertz radiation sources.
Exploring Ultrafast Structural Dynamics for Energetic Enhancement or Disruption

DTIC Science & Technology

2016-03-01

it. In a pump -push/ dump probe experiment, a secondary laser pulse (push/ dump ) is used after the initial perturbation due to the pump pulse. The...increased. The pump -push/ dump probe technique is a difficult experiment that requires a highly stable laser source. Ultrafast pump -probe experiments...decomposition of solids. Journal of Applied Physics. 2001;89:4156–4166. 17. Kee TW. Femtosecond pump -push-probe and pump - dump -probe spectroscopy of
Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra

DOE PAGES

Wolf, Thomas; Holzmeier, Fabian; Wagner, Isabella; ...

2017-07-01

Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine's neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependentmore » dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.« less
Vibrational dynamics of adsorbed molecules under conditions of photodesorption: Pump-probe SFG spectra of CO/Pt(111)

NASA Astrophysics Data System (ADS)

Fournier, Frédéric; Zheng, Wanquan; Carrez, Serge; Dubost, Henri; Bourguignon, Bernard

2004-09-01

Interaction of CO adsorbed on Pt(111) with electrons and phonons is studied experimentally by means of a pump-probe experiment where CO is probed by IR+visible sum frequency generation under a pump laser intensity that allows photodesorption. Vibrational spectra of CO internal stretch are obtained as a function of pump-probe delay. A two-temperature and anharmonic coupling model is used to extract from the spectra the real time variations of CO peak frequency and dephasing time. The main conclusions are the following: (i) The CO stretch is perturbed by two low-frequency modes, assigned to frustrated rotation and frustrated translation. (ii) The frustrated rotation is directly coupled to electrons photoexcited in Pt(111) by the pump laser. (iii) There is no evidence of Pt-CO stretch excitation in the spectra. The implications for the photodesorption dynamics are discussed.
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.
Polarized pump-probe spectroscopy of exciton transport in bacteriochlorophyll a- protein from Prosthecochloris aestuarii

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

Causgrove, T.P.; Yang, S.; Struve, W.S.

1988-11-17

The polarization of the Q/sub x/ electronic transition in the BChl a-protein complex from the green sulfur bacterium Prosthecochloris aestuarii was monitored by pump-probe spectroscopy with approx. 1.5-ps resolution at 598, 603, and 609 nm. At 603 nm, the polarization decays with a mean lifetime of 4.78 ps. Substantial residual polarization appears at long times (the ratio A/sub parallel//A/sub perpendicular/ of optical densities for probe pulses polarized parallel and perpendicular to the excitation pulse is approx. 1.7) in consequence of the nonrandom chromophore orientations. The polarized pump-probe transients have been analyzed in terms of an exciton hopping model that incorporatesmore » the known geometry of the BChl a-protein.« less
Determination of photoionization cross-sections of different organic molecules using gas chromatography coupled to single-photon ionization (SPI) time-of-flight mass spectrometry (TOF-MS) with an electron-beam-pumped rare gas excimer light source (EBEL): influence of molecular structure and analytical implications.

PubMed

Eschner, Markus S; Zimmermann, Ralf

2011-07-01

This work describes a fast and reliable method for determination of photoionization cross-sections (PICS) by means of gas chromatography (GC) coupled to single-photon ionization mass spectrometry (SPI-MS). Photoionization efficiency (PIE) data for 69 substances was obtained at a photon energy of 9.8 ± 0.4 eV using an innovative electron-beam-pumped rare gas excimer light source (EBEL) filled with argon. The investigated analytes comprise 12 alkylbenzenes as well as 11 other substituted benzenes, 23 n-alkanes, ten polyaromatic hydrocarbons, seven aromatic heterocycles, and six polyaromatic heterocycles. Absolute PICS for each substance at 9.8 eV are calculated from the relative photoionization efficiencies of the compounds with respect to benzene, whose photoionization cross-section data is well known. Furthermore, a direct correlation between the type of benzene substituents and their absolute PICS is presented and discussed in depth. Finally, comparison of previously measured photoionization cross-sections for 20 substances shows good agreement with the data of the present work.
Vibrational dynamics of adsorbed molecules under conditions of photodesorption: pump-probe SFG spectra of CO/Pt(111).

PubMed

Fournier, Frédéric; Zheng, Wanquan; Carrez, Serge; Dubost, Henri; Bourguignon, Bernard

2004-09-08

Interaction of CO adsorbed on Pt(111) with electrons and phonons is studied experimentally by means of a pump-probe experiment where CO is probed by IR + visible sum frequency generation under a pump laser intensity that allows photodesorption. Vibrational spectra of CO internal stretch are obtained as a function of pump-probe delay. A two-temperature and anharmonic coupling model is used to extract from the spectra the real time variations of CO peak frequency and dephasing time. The main conclusions are the following: (i) The CO stretch is perturbed by two low-frequency modes, assigned to frustrated rotation and frustrated translation. (ii) The frustrated rotation is directly coupled to electrons photoexcited in Pt(111) by the pump laser. (iii) There is no evidence of Pt-CO stretch excitation in the spectra. The implications for the photodesorption dynamics are discussed. Copyright 2004 American Institute of Physics
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.
Dynamics of Hollow Atom Formation in Intense X-Ray Pulses Probed by Partial Covariance Mapping

NASA Astrophysics Data System (ADS)

Frasinski, L. J.; Zhaunerchyk, V.; Mucke, M.; Squibb, R. J.; Siano, M.; Eland, J. H. D.; Linusson, P.; v. d. Meulen, P.; Salén, P.; Thomas, R. D.; Larsson, M.; Foucar, L.; Ullrich, J.; Motomura, K.; Mondal, S.; Ueda, K.; Osipov, T.; Fang, L.; Murphy, B. F.; Berrah, N.; Bostedt, C.; Bozek, J. D.; Schorb, S.; Messerschmidt, M.; Glownia, J. M.; Cryan, J. P.; Coffee, R. N.; Takahashi, O.; Wada, S.; Piancastelli, M. N.; Richter, R.; Prince, K. C.; Feifel, R.

2013-08-01

When exposed to ultraintense x-radiation sources such as free electron lasers (FELs) the innermost electronic shell can efficiently be emptied, creating a transient hollow atom or molecule. Understanding the femtosecond dynamics of such systems is fundamental to achieving atomic resolution in flash diffraction imaging of noncrystallized complex biological samples. We demonstrate the capacity of a correlation method called “partial covariance mapping” to probe the electron dynamics of neon atoms exposed to intense 8 fs pulses of 1062 eV photons. A complete picture of ionization processes competing in hollow atom formation and decay is visualized with unprecedented ease and the map reveals hitherto unobserved nonlinear sequences of photoionization and Auger events. The technique is particularly well suited to the high counting rate inherent in FEL experiments.
Synchrotron Photoionization Investigation of the Oxidation of Ethyl tert-Butyl Ether.

PubMed

Winfough, Matthew; Yao, Rong; Ng, Martin; Catani, Katherine; Meloni, Giovanni

2017-02-23

The oxidation of ethyl tert-butyl ether (ETBE), a widely used fuel oxygenated additive, is investigated using Cl atoms as initiators in the presence of oxygen. The reaction is carried out at 293, 550, and 700 K. Reaction products are probed by a multiplexed chemical kinetics photoionization mass spectrometer coupled with the synchrotron radiation produced at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory. Products are identified on the basis of mass-to-charge ratio, ionization energies, and shape of photoionization spectra. Reaction pathways are proposed together with detected primary products.
Femtosecond crystallography with ultrabright electrons and x-rays: capturing chemistry in action.

PubMed

Miller, R J Dwayne

2014-03-07

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

PubMed

Richardson, Daniel R; Stauffer, Hans U; Roy, Sukesh; Gord, James R

2017-04-10

A comparison is made between two ultrashort-pulse coherent anti-Stokes Raman scattering (CARS) thermometry techniques-hybrid femtosecond/picosecond (fs/ps) CARS and chirped-probe-pulse (CPP) fs-CARS-that have become standards for high-repetition-rate thermometry in the combustion diagnostics community. These two variants of fs-CARS differ only in the characteristics of the ps-duration probe pulse; in hybrid fs/ps CARS a spectrally narrow, time-asymmetric probe pulse is used, whereas a highly chirped, spectrally broad probe pulse is used in CPP fs-CARS. Temperature measurements were performed using both techniques in near-adiabatic flames in the temperature range 1600-2400 K and for probe time delays of 0-30 ps. Under these conditions, both techniques are shown to exhibit similar temperature measurement accuracies and precisions to previously reported values and to each other. However, it is observed that initial calibration fits to the spectrally broad CPP results require more fitting parameters and a more robust optimization algorithm and therefore significantly increased computational cost and complexity compared to the fitting of hybrid fs/ps CARS data. The optimized model parameters varied more for the CPP measurements than for the hybrid fs/ps measurements for different experimental conditions.
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.
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.
Control of photodissociation and photoionization of the NaI molecule by dynamic Stark effect.

PubMed

Han, Yong-Chang; Yuan, Kai-Jun; Hu, Wen-Hui; Cong, Shu-Lin

2009-01-28

The diabatic photodissociation and photoionization processes of the NaI molecule are studied theoretically using the quantum wave packet method. A pump laser pulse is used to prepare a dissociation wave packet that propagates through both the ionic channel (NaI-->Na(+)+I(-)) and the covalent channel (NaI-->Na+I). A Stark pulse is used to control the diabatic dissociation dynamics and a probe pulse is employed to ionize the products from the two channels. Based on the first order nonresonant nonperturbative dynamic Stark effect, the dissociation probabilities and the branching ratio of the products from the two channels can be controlled. Moreover the final photoelectron kinetic energy distribution can also be affected by the Stark pulse. The influences of the delay time, intensity, frequency, and carrier-envelope phase of the Stark pulse on the dissociation and ionization dynamics of the NaI molecule are discussed in detail.
Biomedical applications of laser photoionization

NASA Astrophysics Data System (ADS)

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

1991-07-01

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

NASA Astrophysics Data System (ADS)

Juhasz, Tibor; Nagy, Zoltan; Sarayba, Melvin; Kurtz, Ronald M.

2010-02-01

The human eye is a favored target for laser surgery due to its accessibility via the optically transparent ocular tissue. Femtosecond lasers with confined tissue effects and minimized collateral tissue damage are primary candidates for high precision intraocular surgery. The advent of compact diode-pumped femtosecond lasers, coupled with computer controlled beam delivery devices, enabled the development of high precision femtosecond laser for ophthalmic surgery. In this article, anterior segment femtosecond laser applications currently in clinical practice and investigation are reviewed. Corneal procedures evolved first and remain dominant due to easy targeting referenced from a contact surface, such as applanation lenses placed on the eye. Adding a high precision imaging technique, such as optical coherence tomography (OCT), can enable accurate targeting of tissue beyond the cornea, such as the crystalline lens. Initial clinical results of femtosecond laser cataract surgery are discussed in detail in the latter portion part of the article.

The initial pump-probe polarization anisotropy of colloidal PbS quantum dots

DOE PAGES

Park, Samuel; Baranov, Dmitry; Ryu, Jisu; ...

2016-07-20

Pump-probe polarization anisotropy measurements with 15 fs pulses are employed to investigate the electronic structure of PbS quantum dots. Here, the initial anisotropy at the bandgap is anomalously low (<0.1) and suggests large electronic couplings.
Photoionization of rare gas clusters

NASA Astrophysics Data System (ADS)

Zhang, Huaizhen

This thesis concentrates on the study of photoionization of van der Waals clusters with different cluster sizes. The goal of the experimental investigation is to understand the electronic structure of van der Waals clusters and the electronic dynamics. These studies are fundamental to understand the interaction between UV-X rays and clusters. The experiments were performed at the Advanced Light Source at Lawrence Berkeley National Laboratory. The experimental method employs angle-resolved time-of-flight photoelectron spectrometry, one of the most powerful methods for probing the electronic structure of atoms, molecules, clusters and solids. The van der Waals cluster photoionization studies are focused on probing the evolution of the photoelectron angular distribution parameter as a function of photon energy and cluster size. The angular distribution has been known to be a sensitive probe of the electronic structure in atoms and molecules. However, it has not been used in the case of van der Waals clusters. We carried out outer-valence levels, inner-valence levels and core-levels cluster photoionization experiments. Specifically, this work reports on the first quantitative measurements of the angular distribution parameters of rare gas clusters as a function of average cluster sizes. Our findings for xenon clusters is that the overall photon-energy-dependent behavior of the photoelectrons from the clusters is very similar to that of the corresponding free atoms. However, distinct differences in the angular distribution point at cluster-size-dependent effects were found. For krypton clusters, in the photon energy range where atomic photoelectrons have a high angular anisotropy, our measurements show considerably more isotropic angular distributions for the cluster photoelectrons, especially right above the 3d and 4p thresholds. For the valence electrons, a surprising difference between the two spin-orbit components was found. For argon clusters, we found that the
Arbitrary-detuning asynchronous optical sampling pump-probe spectroscopy of bacterial reaction centers.

PubMed

Antonucci, Laura; Bonvalet, Adeline; Solinas, Xavier; Jones, Michael R; Vos, Marten H; Joffre, Manuel

2013-09-01

A recently reported variant of asynchronous optical sampling compatible with arbitrary unstabilized laser repetition rates is applied to pump-probe spectroscopy. This makes possible the use of a 5.1 MHz chirped pulse oscillator as the pump laser, thus extending the available time window to almost 200 ns with a time resolution as good as about 320 fs. The method is illustrated with the measurement in a single experiment of the complete charge transfer dynamics of the reaction center from Rhodobacter sphaeroides.
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.
Coherent evolution of parahydrogen induced polarisation using laser pump, NMR probe spectroscopy: Theoretical framework and experimental observation.

PubMed

Halse, Meghan E; Procacci, Barbara; Henshaw, Sarah-Louise; Perutz, Robin N; Duckett, Simon B

2017-05-01

We recently reported a pump-probe method that uses a single laser pulse to introduce parahydrogen (p-H 2 ) into a metal dihydride complex and then follows the time-evolution of the p-H 2 -derived nuclear spin states by NMR. We present here a theoretical framework to describe the oscillatory behaviour of the resultant hyperpolarised NMR signals using a product operator formalism. We consider the cases where the p-H 2 -derived protons form part of an AX, AXY, AXYZ or AA'XX' spin system in the product molecule. We use this framework to predict the patterns for 2D pump-probe NMR spectra, where the indirect dimension represents the evolution during the pump-probe delay and the positions of the cross-peaks depend on the difference in chemical shift of the p-H 2 -derived protons and the difference in their couplings to other nuclei. The evolution of the NMR signals of the p-H 2 -derived protons, as well as the transfer of hyperpolarisation to other NMR-active nuclei in the product, is described. The theoretical framework is tested experimentally for a set of ruthenium dihydride complexes representing the different spin systems. Theoretical predictions and experimental results agree to within experimental error for all features of the hyperpolarised 1 H and 31 P pump-probe NMR spectra. Thus we establish the laser pump, NMR probe approach as a robust way to directly observe and quantitatively analyse the coherent evolution of p-H 2 -derived spin order over micro-to-millisecond timescales. Copyright © 2017 The Authors. Published by Elsevier Inc. All rights reserved.
Infrared x-ray pump-probe spectroscopy of the NO molecule

NASA Astrophysics Data System (ADS)

Guimarães, F. F.; Kimberg, V.; Felicíssimo, V. C.; Gel'Mukhanov, F.; Cesar, A.; Ågren, H.

2005-07-01

Two color infrared x-ray pump-probe spectroscopy of the NO molecule is studied theoretically and numerically in order to obtain a deeper insight of the underlying physics and of the potential of this suggested technology. From the theoretical investigation a number of conclusions could be drawn: It is found that the phase of the infrared field strongly influences the trajectory of the nuclear wave packet, and hence, the x-ray spectrum. The trajectory experiences fast oscillations with the vibrational frequency with a modulation due to the anharmonicity of the potential. The dependences of the x-ray spectra on the delay time, the duration, and the shape of the pulses are studied in detail. It is shown that the x-ray spectrum keep memory about the infrared phase after the pump field left the system. This memory effect is sensitive to the time of switching-off the pump field and the Rabi frequency. The phase effect takes maximum value when the duration of the x-ray pulse is one-fourth of the infrared field period, and can be enhanced by a proper control of the duration and intensity of the pump pulse. The manifestation of the phase is different for oriented and disordered molecules and depends strongly on the intensity of the pump radiation.
Photoionization of furan from the ground and excited electronic states.

PubMed

Ponzi, Aurora; Sapunar, Marin; Angeli, Celestino; Cimiraglia, Renzo; Došlić, Nađa; Decleva, Piero

2016-02-28

Here we present a comparative computational study of the photoionization of furan from the ground and the two lowest-lying excited electronic states. The study aims to assess the quality of the computational methods currently employed for treating bound and continuum states in photoionization. For the ionization from the ground electronic state, we show that the Dyson orbital approach combined with an accurate solution of the continuum one particle wave functions in a multicenter B-spline basis, at the density functional theory (DFT) level, provides cross sections and asymmetry parameters in excellent agreement with experimental data. On the contrary, when the Dyson orbitals approach is combined with the Coulomb and orthogonalized Coulomb treatments of the continuum, the results are qualitatively different. In excited electronic states, three electronic structure methods, TDDFT, ADC(2), and CASSCF, have been used for the computation of the Dyson orbitals, while the continuum was treated at the B-spline/DFT level. We show that photoionization observables are sensitive probes of the nature of the excited states as well as of the quality of excited state wave functions. This paves the way for applications in more complex situations such as time resolved photoionization spectroscopy.
Understanding Intense Laser Interactions with Solid Density Plasma

DTIC Science & Technology

2017-01-04

obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter...with negligible pump-probe jitter being possible with future laser- wakefield-accelerator ultrafast-electron-diffraction schemes. Distribution
The polarization anisotropy of vibrational quantum beats in resonant pump-probe experiments: Diagrammatic calculations for square symmetric molecules.

PubMed

Farrow, Darcie A; Smith, Eric R; Qian, Wei; Jonas, David M

2008-11-07

By analogy to the Raman depolarization ratio, vibrational quantum beats in pump-probe experiments depend on the relative pump and probe laser beam polarizations in a way that reflects vibrational symmetry. The polarization signatures differ from those in spontaneous Raman scattering because the order of field-matter interactions is different. Since pump-probe experiments are sensitive to vibrations on excited electronic states, the polarization anisotropy of vibrational quantum beats can also reflect electronic relaxation processes. Diagrammatic treatments, which expand use of the symmetry of the two-photon tensor to treat signal pathways with vibrational and vibronic coherences, are applied to find the polarization anisotropy of vibrational and vibronic quantum beats in pump-probe experiments for different stages of electronic relaxation in square symmetric molecules. Asymmetric vibrational quantum beats can be distinguished from asymmetric vibronic quantum beats by a pi phase jump near the center of the electronic spectrum and their disappearance in the impulsive limit. Beyond identification of vibrational symmetry, the vibrational quantum beat anisotropy can be used to determine if components of a doubly degenerate electronic state are unrelaxed, dephased, population exchanged, or completely equilibrated.
Monomolecular layer of squarylium dye J aggregates exhibiting a femtosecond optical response of delocalized excitons

NASA Astrophysics Data System (ADS)

Furuki, Makoto; Pu, Lyong Sun; Sasaki, Fumio; Kobayashi, Shyunsuke; Tani, Toshiro

1998-05-01

We report on the demonstration of the femtosecond nonlinear optical response from a two-dimensional monomolecular layer of squarylium dye J aggregate at 5 °C. The formation of a monomolecular layer Langmuir film was achieved by spreading squarylium dye modified by two propyl and two hexyl groups at the air-water interface, which resulted in a very strong J band (o.d.=0.3) at 777 nm. The transient absorption spectra in a resonant pump-probe measurement showed a low absorption saturation power (9.7×106W/cm2) and an ultrafast response (300 fs), which are indicative of exciton delocalization over 18 molecules in this J aggregate, even at 5 °C.
Alignment, vibronic level splitting, and coherent coupling effects on the pump-probe polarization anisotropy.

PubMed

Smith, Eric R; Jonas, David M

2011-04-28

The pump-probe polarization anisotropy is computed for molecules with a nondegenerate ground state, two degenerate or nearly degenerate excited states with perpendicular transition dipoles, and no resonant excited-state absorption. Including finite pulse effects, the initial polarization anisotropy at zero pump-probe delay is predicted to be r(0) = 3/10 with coherent excitation. During pulse overlap, it is shown that the four-wave mixing classification of signal pathways as ground or excited state is not useful for pump-probe signals. Therefore, a reclassification useful for pump-probe experiments is proposed, and the coherent anisotropy is discussed in terms of a more general transition dipole and molecular axis alignment instead of experiment-dependent ground- versus excited-state pathways. Although coherent excitation enhances alignment of the transition dipole, the molecular axes are less aligned than for a single dipole transition, lowering the initial anisotropy. As the splitting between excited states increases beyond the laser bandwidth and absorption line width, the initial anisotropy increases from 3/10 to 4/10. Asymmetric vibrational coordinates that lift the degeneracy control the electronic energy gap and off-diagonal coupling between electronic states. These vibrations dephase coherence and equilibrate the populations of the (nearly) degenerate states, causing the anisotropy to decay (possibly with oscillations) to 1/10. Small amounts of asymmetric inhomogeneity (2 cm(-1)) cause rapid (130 fs) suppression of both vibrational and electronic anisotropy beats on the excited state, but not vibrational beats on the ground electronic state. Recent measurements of conical intersection dynamics in a silicon napthalocyanine revealed anisotropic quantum beats that had to be assigned to asymmetric vibrations on the ground electronic state only [Farrow, D. A.; J. Chem. Phys. 2008, 128, 144510]. Small environmental asymmetries likely explain the observed absence
Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering temperature and concentration measurements using two different picosecond-duration probes.

PubMed

Kearney, Sean P; Scoglietti, Daniel J; Kliewer, Christopher J

2013-05-20

A hybrid fs/ps pure-rotational CARS scheme is characterized in furnace-heated air at temperatures from 290 to 800 K. Impulsive femtosecond excitation is used to prepare a rotational Raman coherence that is probed with a ps-duration beam generated from an initially broadband fs pulse that is bandwidth limited using air-spaced Fabry-Perot etalons. CARS spectra are generated using 1.5- and 7.0-ps duration probe beams with corresponding coarse and narrow spectral widths. The spectra are fitted using a simple phenomenological model for both shot-averaged and single-shot measurements of temperature and oxygen mole fraction. Our single-shot temperature measurements exhibit high levels of precision and accuracy when the spectrally coarse 1.5-ps probe beam is used, demonstrating that high spectral resolution is not required for thermometry. An initial assessment of concentration measurements in air is also provided, with best results obtained using the higher resolution 7.0-ps probe. This systematic assessment of the hybrid CARS technique demonstrates its utility for practical application in low-temperature gas-phase systems.
Vibrational dynamics of hydrogen-bonded complexes in solutions studied with ultrafast infrared pump-probe spectroscopy.

PubMed

Banno, Motohiro; Ohta, Kaoru; Yamaguchi, Sayuri; Hirai, Satori; Tominaga, Keisuke

2009-09-15

In aqueous solution, the basis of all living processes, hydrogen bonding exerts a powerful effect on chemical reactivity. The vibrational energy relaxation (VER) process in hydrogen-bonded complexes in solution is sensitive to the microscopic environment around the oscillator and to the geometrical configuration of the hydrogen-bonded complexes. In this Account, we describe the use of time-resolved infrared (IR) pump-probe spectroscopy to study the vibrational dynamics of (i) the carbonyl CO stretching modes in protic solvents and (ii) the OH stretching modes of phenol and carboxylic acid. In these cases, the carbonyl group acts as a hydrogen-bond acceptor, whereas the hydroxyl group acts as a hydrogen-bond donor. These vibrational modes have different properties depending on their respective chemical bonds, suggesting that hydrogen bonding may have different mechanisms and effects on the VER of the CO and OH modes than previously understood. The IR pump-probe signals of the CO stretching mode of 9-fluorenone and methyl acetate in alcohol, as well as that of acetic acid in water, include several components with different time constants. Quantum chemical calculations indicate that the dynamical components are the result of various hydrogen-bonded complexes that form between solute and solvent molecules. The acceleration of the VER is due to the increasing vibrational density of states caused by the formation of hydrogen bonds. The vibrational dynamics of the OH stretching mode in hydrogen-bonded complexes were studied in several systems. For phenol-base complexes, the decay time constant of the pump-probe signal decreases as the band peak of the IR absorption spectrum shifts to lower wavenumbers (the result of changing the proton acceptor). For phenol oligomers, the decay time constant of the pump-probe signal decreases as the probe wavenumber decreases. These observations show that the VER time strongly correlates with the strength of hydrogen bonding. This
Spin-exchange relaxation-free magnetometer with nearly parallel pump and probe beams

DOE PAGES

Karaulanov, Todor; Savukov, Igor; Kim, Young Jin

2016-03-22

We constructed a spin-exchange relaxation-free (SERF) magnetometer with a small angle between the pump and probe beams facilitating a multi-channel design with a flat pancake cell. This configuration provides almost complete overlap of the beams in the cell, and prevents the pump beam from entering the probe detection channel. By coupling the lasers in multi-mode fibers, without an optical isolator or field modulation, we demonstrate a sensitivity of 10 fTmore » $$/\\sqrt{\\text{Hz}}$$ for frequencies between 10 Hz and 100 Hz. In addition to the experimental study of sensitivity, we present a theoretical analysis of SERF magnetometer response to magnetic fields for small-angle and parallel-beam configurations, and show that at optimal DC offset fields the magnetometer response is comparable to that in the orthogonal-beam configuration. Based on the analysis, we also derive fundamental and probe-limited sensitivities for the arbitrary non-orthogonal geometry. The expected practical and fundamental sensitivities are of the same order as those in the orthogonal geometry. As a result, we anticipate that our design will be useful for magnetoencephalography (MEG) and magnetocardiography (MCG) applications.« less
Progress in Cherenkov femtosecond fiber lasers

PubMed Central

Liu, Xiaomin; Svane, Ask S.; Lægsgaard, Jesper; Tu, Haohua; Boppart, Stephen A.; Turchinovich, Dmitry

2016-01-01

We review the recent developments in the field of ultrafast Cherenkov fiber lasers. Two essential properties of such laser systems – broad wavelength tunability and high efficiency of Cherenkov radiation wavelength conversion are discussed. The exceptional performance of the Cherenkov fiber laser systems are highlighted - dependent on the realization scheme, the Cherenkov lasers can generate the femtosecond output tunable across the entire visible and even the UV range, and for certain designs more than 40 % conversion efficiency from the pump to Cherenkov signal can be achieved. The femtosecond Cherenkov laser with all-fiber architecture is presented and discussed. Operating in the visible range, it delivers 100–200 fs wavelength-tunable pulses with multimilliwatt output power and exceptionally low noise figure an order of magnitude lower than the traditional wavelength tunable supercontinuum-based femtosecond sources. The applications for Cherenkov laser systems in practical biophotonics and biomedical applications, such as bio-imaging and microscopy, are discussed. PMID:27110037
Progress in Cherenkov femtosecond fiber lasers.

PubMed

Liu, Xiaomin; Svane, Ask S; Lægsgaard, Jesper; Tu, Haohua; Boppart, Stephen A; Turchinovich, Dmitry

2016-01-20

We review the recent developments in the field of ultrafast Cherenkov fiber lasers. Two essential properties of such laser systems - broad wavelength tunability and high efficiency of Cherenkov radiation wavelength conversion are discussed. The exceptional performance of the Cherenkov fiber laser systems are highlighted - dependent on the realization scheme, the Cherenkov lasers can generate the femtosecond output tunable across the entire visible and even the UV range, and for certain designs more than 40 % conversion efficiency from the pump to Cherenkov signal can be achieved. The femtosecond Cherenkov laser with all-fiber architecture is presented and discussed. Operating in the visible range, it delivers 100-200 fs wavelength-tunable pulses with multimilliwatt output power and exceptionally low noise figure an order of magnitude lower than the traditional wavelength tunable supercontinuum-based femtosecond sources. The applications for Cherenkov laser systems in practical biophotonics and biomedical applications, such as bio-imaging and microscopy, are discussed.
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)
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
High repetition pump-and-probe photoemission spectroscopy based on a compact fiber laser system.

PubMed

Ishida, Y; Otsu, T; Ozawa, A; Yaji, K; Tani, S; Shin, S; Kobayashi, Y

2016-12-01

The paper describes a time-resolved photoemission (TRPES) apparatus equipped with a Yb-doped fiber laser system delivering 1.2-eV pump and 5.9-eV probe pulses at the repetition rate of 95 MHz. Time and energy resolutions are 11.3 meV and ∼310 fs, respectively, the latter is estimated by performing TRPES on a highly oriented pyrolytic graphite (HOPG). The high repetition rate is suited for achieving high signal-to-noise ratio in TRPES spectra, thereby facilitating investigations of ultrafast electronic dynamics in the low pump fluence (p) region. TRPES of polycrystalline bismuth (Bi) at p as low as 30 nJ/mm 2 is demonstrated. The laser source is compact and is docked to an existing TRPES apparatus based on a 250-kHz Ti:sapphire laser system. The 95-MHz system is less prone to space-charge broadening effects compared to the 250-kHz system, which we explicitly show in a systematic probe-power dependency of the Fermi cutoff of polycrystalline gold. We also describe that the TRPES response of an oriented Bi(111)/HOPG sample is useful for fine-tuning the spatial overlap of the pump and probe beams even when p is as low as 30 nJ/mm 2 .
Controlling the femtosecond laser-driven transformation of dicyclopentadiene into cyclopentadiene

PubMed Central

Goswami, Tapas; Das, Dipak K.; Goswami, Debabrata

2013-01-01

Dynamics of the chemical transformation of dicyclopentadiene into cyclopentadiene in a supersonic molecular beam is elucidated using femtosecond time-resolved degenerate pump–probe mass spectrometry. Control of this ultrafast chemical reaction is achieved by using linearly chirped frequency modulated pulses. We show that negatively chirped femtosecond laser pulses enhance the cyclopentadiene photoproduct yield by an order of magnitude as compared to that of the unmodulated or the positively chirped pulses. This demonstrates that the phase structure of femtosecond laser pulse plays an important role in determining the outcome of a chemical reaction. PMID:24098059

Histotripsy Lesion Formation using an Ultrasound Imaging Probe Enabled by a Low-Frequency Pump Transducer

PubMed Central

Lin, Kuang-Wei; Hall, Timothy L.; Xu, Zhen; Cain, Charles A.

2015-01-01

When applying histotripsy pulses shorter than 2 cycles, the formation of a dense bubble cloud only relies on the applied peak negative pressure (p-) exceeding the “intrinsic threshold” of the medium (absolute value of 26 – 30 MPa in most soft tissue). A previous study conducted by our research group showed that a sub-threshold high-frequency probe pulse (3 MHz) can be enabled by a sub-threshold low-frequency pump pulse (500 kHz) where the sum exceeds the intrinsic threshold, thus generating lesion-producing dense bubble clouds (“dual-beam histotripsy”). This paper investigates the feasibility of using an imaging transducer to provide the high-frequency probe pulse in the dual-beam histotripsy approach. More specifically, an ATL L7–4 imaging transducer, pulsed by a Verasonics V-1 Data Acquisition System, was used to generate the high-frequency probe pulses. The low-frequency pump pulses were generated by a 20-element 345 kHz array transducer, driven by a custom high voltage pulser. These dual-beam histotripsy pulses were applied to red-blood-cell (RBC) tissue-mimicking phantoms at a pulse repetition frequency of 1 Hz, and optical imaging was used to visualize bubble clouds and lesions generated in the RBC phantoms. The results showed that dense bubble clouds (and resulting lesions) were generated when the p- of the sub-threshold pump and probe pulses combined constructively to exceed the intrinsic threshold. The average size of the smallest reproducible lesions using the imaging probe pulse enabled by the sub-threshold pump pulse was 0.7 × 1.7 mm while that using the supra-threshold pump pulse alone was 1.4 × 3.7 mm. When the imaging transducer was steered laterally, bubble clouds and lesions were steered correspondingly until the combined p- no longer exceeded the intrinsic threshold. These results were also validated with ex vivo porcine liver experiments. Using an imaging transducer for dual-beam histotripsy can have two advantages, 1) lesion
Case study on the dynamics of ultrafast laser heating and ablation of gold thin films by ultrafast pump-probe reflectometry and ellipsometry

NASA Astrophysics Data System (ADS)

Pflug, T.; Wang, J.; Olbrich, M.; Frank, M.; Horn, A.

2018-02-01

To increase the comprehension of ultrafast laser ablation, the ablation process has to be portrayed with sufficient temporal resolution. For example, the temporal modification of the complex refractive index {\\tilde{n}} and the relative reflectance of a sample material after irradiation with ultrafast single-pulsed laser radiation can be measured with a pump-probe setup. This work describes the construction and validation of a pump-probe setup enabling spatially, temporally, and spectroscopically resolved Brewster angle microscopy, reflectometry, ellipsometry, and shadow photography. First pump-probe reflectometry and ellipsometry measurements are performed on gold at λ _{probe}= 440 nm and three fluences of the single-pulsed pump radiation at λ _{pump}= 800 nm generating no, gentle, and strong ablation. The relative reflectance overall increases at no and gentle ablation. At strong ablation, the relative reflectance locally decreases, presumable caused by emitted thermal electrons, ballistic electrons, and ablating material. The refractive index n is slightly decreasing after excitation, while the extinction coefficient k is increasing.
Ultrafast molecular processes mapped by femtosecond x-ray diffraction

NASA Astrophysics Data System (ADS)

Elsaesser, Thomas

2012-02-01

X-ray diffraction with a femtosecond time resolution allows for mapping photoinduced structural dynamics on the length scale of a chemical bond and in the time domain of atomic and molecular motion. In a pump-probe approach, a femtosecond excitation pulse induces structural changes which are probed by diffracting a femtosecond hard x-ray pulse from the excited sample. The transient angular positions and intensities of diffraction peaks give insight into the momentary atomic or molecular positions and into the distribution of electronic charge density. The simultaneous measurement of changes on different diffraction peaks is essential for determining atom positions and charge density maps with high accuracy. Recent progress in the generation of ultrashort hard x-ray pulses (Cu Kα, wavelength λ=0.154 nm) in laser-driven plasma sources has led to the implementation of the powder diffraction and the rotating crystal method with a time resolution of 100 fs. In this contribution, we report new results from powder diffraction studies of molecular materials. A first series of experiments gives evidence of a so far unknown concerted transfer of electrons and protons in ammonium sulfate [(NH4)2SO4], a centrosymmetric structure. Charge transfer from the sulfate groups results in the sub-100 fs generation of a confined electron channel along the c-axis of the unit cell which is stabilized by transferring protons from the adjacent ammonium groups into the channel. Time-dependent charge density maps display a periodic modulation of the channel's charge density by low-frequency lattice motions with a concerted electron and proton motion between the channel and the initial proton binding site. A second study addresses atomic rearrangements and charge dislocations in the non-centrosymmetric potassium dihydrogen phosphate [KH2PO4, KDP]. Photoexcitation generates coherent low-frequency motions along the LO and TO phonon coordinates, leaving the average atomic positions unchanged
Excited-State Dynamics of a DNA Duplex in a Deep Eutectic Solvent Probed by Femtosecond Time-Resolved IR Spectroscopy.

PubMed

de La Harpe, Kimberly; Kohl, Forrest R; Zhang, Yuyuan; Kohler, Bern

2018-03-08

To better understand how the solvent influences excited-state deactivation in DNA strands, femtosecond time-resolved IR (fs-TRIR) pump-probe measurements were performed on a d(AT) 9 ·d(AT) 9 duplex dissolved in a deep eutectic solvent (DES) made from choline chloride and ethylene glycol in a 1:2 mol ratio. This solvent, known as ethaline, is a member of a class of ionic liquids capable of solubilizing DNA with minimal disruption to its secondary structure. UV melting analysis reveals that the duplex studied here melts at 18 °C in ethaline compared to 50 °C in aqueous solution. Ethaline has an excellent transparency window that facilitates TRIR measurements in the double-bond stretching region. Transient spectra recorded in deuterated ethaline at room temperature indicate that photoinduced intrastrand charge transfer occurs from A to T, yielding the same exciplex state previously detected in aqueous solution. This state decays via charge recombination with a lifetime of 380 ± 10 ps compared to the 300 ± 10 ps lifetime measured earlier in D 2 O solution. The TRIR data strongly suggest that the long-lived exciplex forms exclusively in the solvated duplex, and not in the denatured single strands, which appear to have little, if any, base stacking. The longer lifetime of the exciplex state in the DES compared to aqueous solution is suggested to arise from reduced stabilization of the charge transfer state, resulting in slower charge recombination on account of Marcus inverted behavior.
Isomer-dependent fragmentation dynamics of inner-shell photoionized difluoroiodobenzene

DOE PAGES

Ablikim, Utuq; Bomme, Cédric; Savelyev, Evgeny; ...

2017-05-11

The fragmentation dynamics of 2,6- and 3,5-difluoroiodobenzene after iodine 4d inner-shell photoionization with soft X-rays are studied using coincident electron and ion momentum imaging. By analyzing the momentum correlation between iodine and fluorine cations in three-fold ion coincidence events, we can distinguish the two isomers experimentally. Classical Coulomb explosion simulations are in overall agreement with the experimentally determined fragment ion kinetic energies and momentum correlations and point toward different fragmentation mechanisms and time scales. Finally, while most three-body fragmentation channels show clear evidence for sequential fragmentation on a time scale larger than the rotational period of the fragments, the breakupmore » into iodine and fluorine cations and a third charged co-fragment appears to occur within several hundred femtoseconds.« less
Optimal Dynamic Detection of Explosives (ODD-EX)

DTIC Science & Technology

2011-12-29

2. Control of nitromethane photoionization efficiency with shaped femtosecond pulses, J. Roslund, O. Shir, A. Dogariu, R. Miles, H. Rabitz, J. Chem...feedback loop. 2. Control of nitromethane photoionization efficiency with shaped femtosecond pulses, J. Roslund, O. Shir, A. Dogariu, R. Miles, H. Rabitz...resonances that allow a significant increase in the photoionization efficiency of nitromethane with shaped near-infrared femtosecond pulses. The
Femtosecond gas phase electron diffraction with MeV electrons.

PubMed

Yang, Jie; Guehr, Markus; Vecchione, Theodore; Robinson, Matthew S; Li, Renkai; Hartmann, Nick; Shen, Xiaozhe; Coffee, Ryan; Corbett, Jeff; Fry, Alan; Gaffney, Kelly; Gorkhover, Tais; Hast, Carsten; Jobe, Keith; Makasyuk, Igor; Reid, Alexander; Robinson, Joseph; Vetter, Sharon; Wang, Fenglin; Weathersby, Stephen; Yoneda, Charles; Wang, Xijie; Centurion, Martin

2016-12-16

We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.
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.
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
"Intact" Carrier Doping by Pump-Pump-Probe Spectroscopy in Combination with Interfacial Charge Transfer: A Case Study of CsPbBr3 Nanocrystals.

PubMed

Wang, Junhui; Ding, Tao; Leng, Jing; Jin, Shengye; Wu, Kaifeng

2018-06-21

Carrier doping is important for semiconductor nanocrystals (NCs) as it offers a new knob to tune NCs' functionalities, in addition to size and shape control. Also, extensive studies on NC devices have revealed that under operating conditions NCs are often unintentionally doped with electrons or holes. Thus, it is essential to be able to control the doping of NCs and study the carrier dynamics of doped NCs. The extension of previously reported redox-doping methods to chemically sensitive materials, such as recently introduced perovskite NCs, has remained challenging. We introduce an "intact" carrier-doping method by performing pump-pump-probe transient absorption spectroscopy on NC-acceptor complexes. The first pump pulse is used to trigger charge transfer from the NC to the acceptor, leading to NCs doped with a band edge carrier; the following pump-probe pulses measure the dynamics of carrier-doped NCs. We performed this measurement on CsPbBr 3 NCs and deduced positive and negative trion lifetimes of 220 ± 50 and 150 ± 40 ps, respectively, for 10 nm diameter NCs, both dominated by Auger recombination. It also allowed us to identify randomly photocharged excitons in CsPbBr 3 NCs as positive trions.
Serial Femtosecond Crystallography and Ultrafast Absorption Spectroscopy of the Photoswitchable Fluorescent Protein IrisFP.

PubMed

Colletier, Jacques-Philippe; Sliwa, Michel; Gallat, François-Xavier; Sugahara, Michihiro; Guillon, Virginia; Schirò, Giorgio; Coquelle, Nicolas; Woodhouse, Joyce; Roux, Laure; Gotthard, Guillaume; Royant, Antoine; Uriarte, Lucas Martinez; Ruckebusch, Cyril; Joti, Yasumasa; Byrdin, Martin; Mizohata, Eiichi; Nango, Eriko; Tanaka, Tomoyuki; Tono, Kensuke; Yabashi, Makina; Adam, Virgile; Cammarata, Marco; Schlichting, Ilme; Bourgeois, Dominique; Weik, Martin

2016-03-03

Reversibly photoswitchable fluorescent proteins find growing applications in cell biology, yet mechanistic details, in particular on the ultrafast photochemical time scale, remain unknown. We employed time-resolved pump-probe absorption spectroscopy on the reversibly photoswitchable fluorescent protein IrisFP in solution to study photoswitching from the nonfluorescent (off) to the fluorescent (on) state. Evidence is provided for the existence of several intermediate states on the pico- and microsecond time scales that are attributed to chromophore isomerization and proton transfer, respectively. Kinetic modeling favors a sequential mechanism with the existence of two excited state intermediates with lifetimes of 2 and 15 ps, the second of which controls the photoswitching quantum yield. In order to support that IrisFP is suited for time-resolved experiments aiming at a structural characterization of these ps intermediates, we used serial femtosecond crystallography at an X-ray free electron laser and solved the structure of IrisFP in its on state. Sample consumption was minimized by embedding crystals in mineral grease, in which they remain photoswitchable. Our spectroscopic and structural results pave the way for time-resolved serial femtosecond crystallography aiming at characterizing the structure of ultrafast intermediates in reversibly photoswitchable fluorescent proteins.
Time-resolved measurement of single pulse femtosecond laser-induced periodic surface structure formation induced by a pre-fabricated surface groove.

PubMed

Kafka, K R P; Austin, D R; Li, H; Yi, A Y; Cheng, J; Chowdhury, E A

2015-07-27

Time-resolved diffraction microscopy technique has been used to observe the formation of laser-induced periodic surface structures (LIPSS) from the interaction of a single femtosecond laser pulse (pump) with a nano-scale groove mechanically formed on a single-crystal Cu substrate. The interaction dynamics (0-1200 ps) was captured by diffracting a time-delayed, frequency-doubled pulse (probe) from nascent LIPSS formation induced by the pump with an infinity-conjugate microscopy setup. The LIPSS ripples are observed to form asynchronously, with the first one forming after 50 ps and others forming sequentially outward from the groove edge at larger time delays. A 1-D analytical model of electron heating including both the laser pulse and surface plasmon polariton excitation at the groove edge predicts ripple period, melt spot diameter, and qualitatively explains the asynchronous time-evolution of LIPSS formation.
Holography and thermalization in optical pump-probe spectroscopy

NASA Astrophysics Data System (ADS)

Bagrov, A.; Craps, B.; Galli, F.; Keränen, V.; Keski-Vakkuri, E.; Zaanen, J.

2018-04-01

Using holography, we model experiments in which a 2 +1 D strange metal is pumped by a laser pulse into a highly excited state, after which the time evolution of the optical conductivity is probed. We consider a finite-density state with mildly broken translation invariance and excite it by oscillating electric field pulses. At zero density, the optical conductivity would assume its thermalized value immediately after the pumping has ended. At finite density, pulses with significant dc components give rise to slow exponential relaxation, governed by a vector quasinormal mode. In contrast, for high-frequency pulses the amplitude of the quasinormal mode is strongly suppressed, so that the optical conductivity assumes its thermalized value effectively instantaneously. This surprising prediction may provide a stimulus for taking up the challenge to realize these experiments in the laboratory. Such experiments would test a crucial open question faced by applied holography: are its predictions artifacts of the large N limit or do they enjoy sufficient UV independence to hold at least qualitatively in real-world systems?
Effects of Electronic-State-Dependent Solute Polarizability: Application to Solute-Pump/Solvent-Probe Spectra.

PubMed

Sun, Xiang; Ladanyi, Branka M; Stratt, Richard M

2015-07-23

Experimental studies of solvation dynamics in liquids invariably ask how changing a solute from its electronic ground state to an electronically excited state affects a solution's dynamics. With traditional time-dependent-fluorescence experiments, that means looking for the dynamical consequences of the concomitant change in solute-solvent potential energy. But if one follows the shift in the dynamics through its effects on the macroscopic polarizability, as recent solute-pump/solvent-probe spectra do, there is another effect of the electronic excitation that should be considered: the jump in the solute's own polarizability. We examine the spectroscopic consequences of this solute polarizability change in the classic example of the solvation dye coumarin 153 dissolved in acetonitrile. After demonstrating that standard quantum chemical methods can be used to construct accurate multisite models for the polarizabilities of ground- and excited-state solvation dyes, we show via simulation that this polarizability change acts as a contrast agent, significantly enhancing the observable differences in optical-Kerr spectra between ground- and excited-state solutions. A comparison of our results with experimental solute-pump/solvent-probe spectra supports our interpretation and modeling of this spectroscopy. We predict, in particular, that solute-pump/solvent-probe spectra should be sensitive to changes in both the solvent dynamics near the solute and the electronic-state-dependence of the solute's own rotational dynamics.
rotational Raman spectroscopy methods for probing energy thermalisation processes during spin-exchange optical pumping

NASA Astrophysics Data System (ADS)

Newton, Hayley; Walkup, Laura L.; Whiting, Nicholas; West, Linda; Carriere, James; Havermeyer, Frank; Ho, Lawrence; Morris, Peter; Goodson, Boyd M.; Barlow, Michael J.

2014-05-01

Spin-exchange optical pumping (SEOP) has been widely used to produce enhancements in nuclear spin polarisation for hyperpolarised noble gases. However, some key fundamental physical processes underlying SEOP remain poorly understood, particularly in regards to how pump laser energy absorbed during SEOP is thermalised, distributed and dissipated. This study uses in situ ultra-low frequency Raman spectroscopy to probe rotational temperatures of nitrogen buffer gas during optical pumping under conditions of high resonant laser flux and binary Xe/N2 gas mixtures. We compare two methods of collecting the Raman scattering signal from the SEOP cell: a conventional orthogonal arrangement combining intrinsic spatial filtering with the utilisation of the internal baffles of the Raman spectrometer, eliminating probe laser light and Rayleigh scattering, versus a new in-line modular design that uses ultra-narrowband notch filters to remove such unwanted contributions. We report a ~23-fold improvement in detection sensitivity using the in-line module, which leads to faster data acquisition and more accurate real-time monitoring of energy transport processes during optical pumping. The utility of this approach is demonstrated via measurements of the local internal gas temperature (which can greatly exceed the externally measured temperature) as a function of incident laser power and position within the cell.
Development of Two-Photon Pump Polarization Spectroscopy Probe Technique Tpp-Psp for Measurements of Atomic Hydrogen .

NASA Astrophysics Data System (ADS)

Satija, Aman; Lucht, Robert P.

2015-06-01

Atomic hydrogen (H) is a key radical in combustion and plasmas. Accurate knowledge of its concentration can be used to better understand transient phenomenon such as ignition and extinction in combustion environments. Laser induced polarization spectroscopy is a spatially resolved absorption technique which we have adapted for quantitative measurements of H atom. This adaptation is called two-photon pump, polarization spectroscopy probe technique (TPP-PSP) and it has been implemented using two different laser excitation schemes. The first scheme involves the two-photon excitation of 1S-2S transitions using a linearly polarized 243-nm beam. An anisotropy is created amongst Zeeman states in 2S-3P levels using a circularly polarized 656-nm pump beam. This anisotropy rotates the polarization of a weak, linearly polarized probe beam at 656 nm. As a result, the weak probe beam "leaks" past an analyzer in the detection channel and is measured using a PMT. This signal can be related to H atom density in the probe volume. The laser beams were created by optical parametric generation followed by multiple pulse dye amplification stages. This resulted in narrow linewidth beams which could be scanned in frequency domain and varied in energy. This allowed us to systematically investigate saturation and Stark effect in 2S-3P transitions with the goal of developing a quantitative H atom measurement technique. The second scheme involves the two-photon excitation of 1S-2S transitions using a linearly polarized 243-nm beam. An anisotropy is created amongst Zeeman states in 2S-4P transitions using a circularly polarized 486-nm pump beam. This anisotropy rotates the polarization of a weak, linearly polarized probe beam at 486 nm. As a result the weak probe beam "leaks" past an analyzer in the detection channel and is measured using a PMT. This signal can be related to H atom density in the probe volume. A dye laser was pumped by third harmonic of a Nd:YAG laser to create a laser beam
Amplitude mode oscillations in pump-probe photoemission spectra from a d -wave superconductor

NASA Astrophysics Data System (ADS)

Nosarzewski, B.; Moritz, B.; Freericks, J. K.; Kemper, A. F.; Devereaux, T. P.

2017-11-01

Recent developments in the techniques of ultrafast pump-probe photoemission have made possible the search for collective modes in strongly correlated systems out of equilibrium. Including inelastic scattering processes and a retarded interaction, we simulate time- and angle-resolved photoemission spectroscopy (trARPES) to study the amplitude mode of a d -wave superconductor, a collective mode excited through the nonlinear light-matter coupling to the pump pulse. We find that the amplitude mode oscillations of the d -wave order parameter occur in phase at a single frequency that is twice the quasi-steady-state maximum gap size after pumping. We comment on the necessary conditions for detecting the amplitude mode in trARPES experiments.
Improved optical efficiency of bulk laser amplifiers with femtosecond written waveguides

NASA Astrophysics Data System (ADS)

Bukharin, Mikhail A.; Lyashedko, Andrey; Skryabin, Nikolay N.; Khudyakov, Dmitriy V.; Vartapetov, Sergey K.

2016-04-01

In the paper we proposed improved technique of three-dimensional waveguides writing with direct femtosecond laser inscription technology. The technique allows, for the first time of our knowledge, production of waveguides with mode field diameter larger than 200 μm. This result broadens field of application of femtosecond writing technology into bulk laser schemes and creates an opportunity to develop novel amplifiers with increased efficiency. We proposed a novel architecture of laser amplifier that combines free-space propagation of signal beam with low divergence and propagation of pump irradiation inside femtosecond written waveguide with large mode field diameter due to total internal reflection effect. Such scheme provides constant tight confinement of pump irradiation over the full length of active laser element (3-10 cm). The novel amplifier architecture was investigated numerically and experimentally in Nd:phosphate glass. Waveguides with 200 μm mode field diameter were written with high frequency femtosecond oscillator. Proposed technique of three-dimensional waveguides writing based on decreasing and compensation of spherical aberration effect due to writing in heat cumulative regime and dynamic pulse energy adjustment at different depths of writing. It was shown, that written waveguides could increase optical efficiency of amplifier up to 4 times compared with corresponding usual free-space schemes. Novelty of the results consists in technique of femtosecond writing of waveguides with large mode field diameter. Actuality of the results consists in originally proposed architecture allows to improve up to 4 times optical efficiency of conventional bulk laser schemes and especially ultrafast pulse laser amplifiers.
Elliptical polarization of near-resonant linearly polarized probe light in optically pumped alkali metal vapor

PubMed Central

Li, Yingying; Wang, Zhiguo; Jin, Shilong; Yuan, Jie; Luo, Hui

2017-01-01

Optically pumped alkali metal atoms currently provide a sensitive solution for magnetic microscopic measurements. As the most practicable plan, Faraday rotation of linearly polarized light is extensively used in spin polarization measurements of alkali metal atoms. In some cases, near-resonant Faraday rotation is applied to improve the sensitivity. However, the near-resonant linearly polarized probe light is elliptically polarized after passing through optically pumped alkali metal vapor. The ellipticity of transmitted near-resonant probe light is numerically calculated and experimentally measured. In addition, we also analyze the negative impact of elliptical polarization on Faraday rotation measurements. From our theoretical estimate and experimental results, the elliptical polarization forms an inevitable error in spin polarization measurements. PMID:28216649
Reinterpretation of femtosecond laser pump-probe and thermomodulation optical spectroscopy results on HTSC materials in terms of the resonant negative-U model

NASA Astrophysics Data System (ADS)

Wilson, John A.

2000-01-01

The laser pump/probe spectroscopy from Stevens et al (on YBCO7 ) and the thermomodulation optical data and analysis from Holcomb et al (on a selection of HTSC materials) are examined in terms of the resonant negative-U mechanism for high temperature superconductivity (HTSC) in the mixed-valent cuprates. The work centres on the universal 1.5-2 eV features becoming visible below Tc upon the optical `charge-transfer' edge. These it is argued are not simple p-to-d band-to-band excitations but are to be associated with the mixed-valent and negative-U states that instigate HTSC. This argument is supported both by the decay characteristics apparent in the new data recorded by Stevens et al and also in the outcome of the Eliashberg analysis developed by Holcomb et al to accommodate their own thermomodulation data. The interpretation provided is in line with that offered recently of the highly characteristic thermoelectric behaviour exhibited by all HTSC systems.

Observation of Ultrafast Magnon Dynamics in Antiferromagnetic Nickel Oxide by Optical Pump-Probe and Terahertz Time-Domain Spectroscopies

NASA Astrophysics Data System (ADS)

Kohmoto, T.; Moriyasu, T.; Wakabayashi, S.; Jinn, H.; Takahara, M.; Kakita, K.

2018-01-01

We have studied the ultrafast magnon dynamics in an antiferromagnetic 3d-transition-metal monoxide, nickel oxide (NiO), using optical pump-probe spectroscopy and terahertz time-domain spectroscopy (THz-TDS). THz damped magnon oscillations were observed in the Faraday rotation signal and in the transmitted THz electric field via optical pump-probe spectroscopy and THz-TDS, respectively. The magnon signals were observed in both the optical pump-probe spectroscopy and THz-TDS experiments, which shows that both Raman- and infrared-active modes are included in the NiO magnon modes. The magnon relaxation rate observed using THz-TDS was found to be almost constant up to the Néel temperature T N (= 523 K) and to increase abruptly near that temperature. This shows that temperature-independent spin-spin relaxation dominates up to T N . In our experiment, softening of the magnon frequency near T N was clearly observed. This result shows that the optical pump-probe spectroscopy and THz-TDS have high frequency resolution and a high signal to noise ratio in the THz region. We discuss the observed temperature dependence of the magnon frequencies using three different molecular field theories. The experimental results suggest that the biquadratic contribution of the exchange interaction plays an important role in the temperature dependence of the sublattice magnetization and the magnon frequency in cubic antiferromagnetic oxides.
Femtosecond optical reflectivity measurements of lattice-mediated spin repulsions in photoexcited LaCoO3 thin films

NASA Astrophysics Data System (ADS)

Bielecki, J.; Rata, A. D.; Börjesson, L.

2014-01-01

We present results on the temperature dependence of ultrafast electron and lattice dynamics, measured with pump-probe transient reflectivity experiments, of an epitaxially grown LaCoO3 thin film under tensile strain. Probing spin-polarized transitions into the antibonding eg band provides a measure of the low-spin fraction, both as a function of temperature and time after photoexcitation. It is observed that femtosecond laser pulses destabilize the constant low-spin fraction (˜63%-64%) in equilibrium into a thermally activated state, driven by a subpicosecond change in spin gap Δ. From the time evolution of the low-spin fraction, it is possible to disentangle the thermal and lattice contributions to the spin state. A lattice mediated spin repulsion, identified as the governing factor determining the equilibrium spin state in thin-film LaCoO3, is observed. These results suggests that time-resolved spectroscopy is a sensitive probe of the spin state in LaCoO3 thin films, with the potential to bring forward quantitative insight into the complicated interplay between structure and spin state in LaCoO3.
Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering.

PubMed

Miller, Joseph D; Roy, Sukesh; Slipchenko, Mikhail N; Gord, James R; Meyer, Terrence R

2011-08-01

High-repetition-rate, single-laser-shot measurements are important for the investigation of unsteady flows where temperature and species concentrations can vary significantly. Here, we demonstrate single-shot, pure-rotational, hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps RCARS) thermometry based on a kHz-rate fs laser source. Interferences that can affect nanosecond (ns) and ps CARS, such as nonresonant background and collisional dephasing, are eliminated by selecting an appropriate time delay between the 100-fs pump/Stokes pulses and the pulse-shaped 8.4-ps probe. A time- and frequency-domain theoretical model is introduced to account for rotational-level dependent collisional dephasing and indicates that the optimal probe-pulse time delay is 13.5 ps to 30 ps. This time delay allows for uncorrected best-fit N2-RCARS temperature measurements with ~1% accuracy. Hence, the hybrid fs/ps RCARS approach can be performed with kHz-rate laser sources while avoiding corrections that can be difficult to predict in unsteady flows.
Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

NASA Astrophysics Data System (ADS)

Miller, Joseph D.; Roy, Sukesh; Slipchenko, Mikhail N.; Gord, James R.; Meyer, Terrence R.

2011-08-01

High-repetition-rate, single-laser-shot measurements are important for the investigation of unsteady flows where temperature and species concentrations can vary significantly. Here, we demonstrate single-shot, pure-rotational, hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps RCARS) thermometry based on a kHz-rate fs laser source. Interferences that can affect nanosecond (ns) and ps CARS, such as nonresonant background and collisional dephasing, are eliminated by selecting an appropriate time delay between the 100-fs pump/Stokes pulses and the pulse-shaped 8.4-ps probe. A time- and frequency-domain theoretical model is introduced to account for rotational-level dependent collisional dephasing and indicates that the optimal probe-pulse time delay is 13.5 ps to 30 ps. This time delay allows for uncorrected best-fit N2-RCARS temperature measurements with ~1% accuracy. Hence, the hybrid fs/ps RCARS approach can be performed with kHz-rate laser sources while avoiding corrections that can be difficult to predict in unsteady flows.
Histotripsy Lesion Formation Using an Ultrasound Imaging Probe Enabled by a Low-Frequency Pump Transducer.

PubMed

Lin, Kuang-Wei; Hall, Timothy L; Xu, Zhen; Cain, Charles A

2015-08-01

When histotripsy pulses shorter than 2 cycles are applied, the formation of a dense bubble cloud relies only on the applied peak negative pressure (p-) exceeding the "intrinsic threshold" of the medium (absolute value of 26-30 MPa in most soft tissues). It has been found that a sub-threshold high-frequency probe pulse (3 MHz) can be enabled by a sub-threshold low-frequency pump pulse (500 kHz) where the sum exceeds the intrinsic threshold, thus generating lesion-producing dense bubble clouds ("dual-beam histotripsy"). Here, the feasibility of using an imaging transducer to provide the high-frequency probe pulse in the dual-beam histotripsy approach is investigated. More specifically, an ATL L7-4 imaging transducer (Philips Healthcare, Andover, MA, USA), pulsed by a V-1 Data Acquisition System (Verasonics, Redmond, WA, USA), was used to generate the high-frequency probe pulses. The low-frequency pump pulses were generated by a 20-element 345-kHz array transducer, driven by a custom high-voltage pulser. These dual-beam histotripsy pulses were applied to red blood cell tissue-mimicking phantoms at a pulse repetition frequency of 1 Hz, and optical imaging was used to visualize bubble clouds and lesions generated in the red blood cell phantoms. The results indicated that dense bubble clouds (and resulting lesions) were generated when the p- of the sub-threshold pump and probe pulses combined constructively to exceed the intrinsic threshold. The average size of the smallest reproducible lesions using the imaging probe pulse enabled by the sub-threshold pump pulse was 0.7 × 1.7 mm, whereas that using the supra-threshold pump pulse alone was 1.4 × 3.7 mm. When the imaging transducer was steered laterally, bubble clouds and lesions were steered correspondingly until the combined p- no longer exceeded the intrinsic threshold. These results were also validated with ex vivo porcine liver experiments. Using an imaging transducer for dual-beam histotripsy can have two
Photoinduced electron transfer in a molecular dyad by nanosecond pump-pump-probe spectroscopy.

PubMed

Ha-Thi, M-H; Pham, V-T; Pino, T; Maslova, V; Quaranta, A; Lefumeux, C; Leibl, W; Aukauloo, A

2018-06-01

The design of robust and inexpensive molecular photocatalysts for the conversion of abundant stable molecules like H2O and CO2 into an energetic carrier is one of the major fundamental questions for scientists nowadays. The outstanding challenge is to couple single photoinduced charge separation events with the sequential accumulation of redox equivalents at the catalytic unit for performing multielectronic catalytic reactions. Herein, double excitation by nanosecond pump-pump-probe experiments was used to interrogate the photoinduced charge transfer and charge accumulation on a molecular dyad composed of a porphyrin chromophore and a ruthenium-based catalyst in the presence of a reversible electron acceptor. An accumulative charge transfer state is unattainable because of rapid reverse electron transfer to the photosensitizer upon the second excitation and the low driving force of the forward photodriven electron transfer reaction. Such a method allows the fundamental understanding of the relaxation mechanism after two sequential photon absorptions, deciphering the undesired electron transfer reactions that limit the charge accumulation efficiency. This study is a step toward the improvement of synthetic strategies of molecular photocatalysts for light-induced charge accumulation and more generally, for solar energy conversion.
Amplitude mode oscillations in pump-probe photoemission spectra from a d -wave superconductor

DOE PAGES

Nosarzewski, B.; Moritz, B.; Freericks, J. K.; ...

2017-11-20

Recent developments in the techniques of ultrafast pump-probe photoemission have made possible the search for collective modes in strongly correlated systems out of equilibrium. Including inelastic scattering processes and a retarded interaction, we simulate time- and angle-resolved photoemission spectroscopy (trARPES) to study the amplitude mode of a d-wave superconductor, a collective mode excited through the nonlinear light-matter coupling to the pump pulse. We find that the amplitude mode oscillations of the d-wave order parameter occur in phase at a single frequency that is twice the quasi-steady-state maximum gap size after pumping. As a result, we comment on the necessary conditionsmore » for detecting the amplitude mode in trARPES experiments.« less
Amplitude mode oscillations in pump-probe photoemission spectra from a d -wave superconductor

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

Nosarzewski, B.; Moritz, B.; Freericks, J. K.

Recent developments in the techniques of ultrafast pump-probe photoemission have made possible the search for collective modes in strongly correlated systems out of equilibrium. Including inelastic scattering processes and a retarded interaction, we simulate time- and angle-resolved photoemission spectroscopy (trARPES) to study the amplitude mode of a d-wave superconductor, a collective mode excited through the nonlinear light-matter coupling to the pump pulse. We find that the amplitude mode oscillations of the d-wave order parameter occur in phase at a single frequency that is twice the quasi-steady-state maximum gap size after pumping. As a result, we comment on the necessary conditionsmore » for detecting the amplitude mode in trARPES experiments.« less
Ultrafast carrier dynamics in bilayer graphene studied by broadband infrared pump-probe spectroscopy

NASA Astrophysics Data System (ADS)

Limmer, Thomas; da Como, Enrico; Niggebaum, Alexander; Feldmann, Jochen

2010-03-01

Recently, bilayer graphene gained a large interest because of its electrically tunable gap appearing in the middle infrared part of the electromagnetic spectrum. This feature is expected to open a number of applications of bilayer graphene in optoelectronics. In this communication we report on the first pump-probe experiment on a single bilayer flake with an unprecedented probe photon energy interval (0.25 -- 1.3 eV). Single flakes were prepared by mechanical exfoliation of graphite and transferred to calcium fluoride substrates. When illuminated with 800 nm (1.5 eV) pump pulses the induced change in transmission shows an ultrafast saturation of the interband transitions from 1.3 to 0.5 eV. In this energy range the saturation recovery occurs within 3 ps and is consistent with an ultrafast relaxation of hot carriers. Interestingly, we report on the observation of a resonance at 0.4 eV characterized by a longer dynamics. The results are discussed considering many-body interactions.
Ultrafast internal conversion dynamics of highly excited pyrrole studied with VUV/UV pump probe spectroscopy.

PubMed

Horton, Spencer L; Liu, Yusong; Chakraborty, Pratip; Matsika, Spiridoula; Weinacht, Thomas

2017-02-14

We study the relaxation dynamics of pyrrole after excitation with an 8 eV pump pulse to a state just 0.2 eV below the ionization potential using vacuum ultraviolet/ultraviolet pump probe spectroscopy. Our measurements in conjunction with electronic structure calculations indicate that pyrrole undergoes rapid internal conversion to the ground state in less than 300 fs. We find that internal conversion to the ground state dominates over dissociation.
Diode-laser pumping into the emitting level for efficient lasing of depressed cladding waveguides realized in Nd:YVO4 by the direct femtosecond-laser writing technique.

PubMed

Pavel, Nicolaie; Salamu, Gabriela; Jipa, Florin; Zamfirescu, Marian

2014-09-22

Depressed cladding waveguides have been realized in Nd:YVO(4) employing direct writing technique with a femtosecond-laser beam. It was shown that the output performances of such laser devices are improved by the reduction of the quantum defect between the pump wavelength and the laser wavelength. Thus, under the classical pump at 808 nm (i.e. into the (4)F(5/2) level), a 100-μm diameter circular waveguide inscribed in a 0.7-at.% Nd:YVO(4) outputted 1.06-μm laser pulses with 3.0-mJ energy, at 0.30 optical efficiency and slope efficiency of 0.32. The pump at 880 nm (i.e.directly into the (4)F(3/2) emitting level) increased the pulse energy at 3.8 mJ and improved both optical efficiency and slope efficiency at 0.36 and 0.39, respectively. The same waveguide yielded continuous-wave 1.5-W output power at 1.06 μm under the pump at 880 nm. Laser emission at 1.34 μm was also improved using the pump into the (4)F(3/2) emitting level of Nd:YVO(4).
Double photoionization of atoms

NASA Astrophysics Data System (ADS)

Wiedenhoeft, Marco

2003-10-01

Double photoionization studies of atoms and molecules are new state-of-the-art studies providing a deeper knowledge of multi-electron excitations. This type of work advances the understanding of many-body problems. Double photoionization of atoms is of great interest to learn about electron-electron correlation and relaxation effects in atoms and molecules. In order to study double photoionization processes, a new electron-electron coincidence apparatus was built to carry out the measurements. I will present the apparatus I built as well as the results of the measurement of the triply-differential-cross-section (TDCS) for the predicted interference and Post-Collision-Interaction (PCI) effects in the Xenon N5O2,3 O2,3 Auger decay after 4d5/2 photoionization. Furthermore I present measurements for direct double photoionization of Helium at various photon energies.
DOE Office of Scientific and Technical Information (OSTI.GOV)

Fang, Li; Xiong, Hui; Kukk, Edwin

Molecular dynamics is of fundamental interest in natural science research. The capability of investigating molecular dynamics is one of the various motivations for ultrafast optics. Here, we present our investigation of photoionization and nuclear dynamics in methyl iodine (CH 3I) molecule with an X-ray pump X-ray probe scheme. The pump–probe experiment was realized with a two-mirror X-ray split and delay apparatus. Time-of-flight mass spectra at various pump–probe delay times were recorded to obtain the time profile for the creation of high charge states via sequential ionization and for molecular dissociation. We observed high charge states of atomic iodine up tomore » 29+, and visualized the evolution of creating these high atomic ion charge states, including their population suppression and enhancement as the arrival time of the second X-ray pulse was varied. We also show the evolution of the kinetics of the high charge states upon the timing of their creation during the ionization-dissociation coupled dynamics. We demonstrate the implementation of X-ray pump–probe methodology for investigating X-ray induced molecular dynamics with femtosecond temporal resolution. The results indicate the footprints of ionization that lead to high charge states, probing the long-range potential curves of the high charge states.« less
Coherent vs Incoherent Emission from Semiconductor Structures after Resonant Femtosecond Excitation

NASA Astrophysics Data System (ADS)

Gurioli, Massimo; Bogani, Franco; Ceccherini, Simone; Colocci, Marcello

1997-04-01

We show that an interferometric correlation measurement with fs time resolution provides an unambiguous discrimination between coherent and incoherent emission after resonant femtosecond excitation. The experiment directly probes the most important difference between the two emissions, that is, the phase correlation with the excitation pulse. The comparison with cw frequency resolved measurements demonstrates that the relationship between coherent and incoherent emission is similar under femtosecond and steady-state excitation.
Mercury Amalgam Diffusion in Human Teeth Probed Using Femtosecond LIBS.

PubMed

Bello, Liciane Toledo; da Ana, Patricia Aparecida; Santos, Dário; Krug, Francisco José; Zezell, Denise Maria; Vieira, Nilson Dias; Samad, Ricardo Elgul

2017-04-01

In this work the diffusion of mercury and other elements from amalgam tooth restorations through the surrounding dental tissue (dentin) was evaluated using femtosecond laser-induced breakdown spectroscopy (fs-LIBS). To achieve this, seven deciduous and eight permanent extracted human molar teeth with occlusal amalgam restorations were half-sectioned and analyzed using pulses from a femtosecond laser. The measurements were performed from the amalgam restoration along the amalgam/dentin interface to the apical direction. It was possible to observe the presence of metallic elements (silver, mercury, copper and tin) emission lines, as well as dental constituent ones, providing fingerprints of each material and comparable data for checking the consistence of the results. It was also shown that the elements penetration depth values in each tooth are usually similar and consistent, for both deciduous and permanent teeth, indicating that all the metals diffuse into the dentin by the same mechanism. We propose that this diffusion mechanism is mainly through liquid dragging inside the dentin tubules. The mercury diffused further in permanent teeth than in deciduous teeth, probably due to the longer diffusion times due to the age of the restorations. It was possible to conclude that the proposed femtosecond-LIBS system can detect the presence of metals in the dental tissue, among the tooth constituent elements, and map the distribution of endogenous and exogenous chemical elements, with a spatial resolution that can be brought under 100 µm.
Terahertz radiation driven by two-color laser pulses at near-relativistic intensities: Competition between photoionization and wakefield effects.

PubMed

González de Alaiza Martínez, P; Davoine, X; Debayle, A; Gremillet, L; Bergé, L

2016-06-03

We numerically investigate terahertz (THz) pulse generation by linearly-polarized, two-color femtosecond laser pulses in highly-ionized argon. Major processes consist of tunneling photoionization and ponderomotive forces associated with transverse and longitudinal field excitations. By means of two-dimensional particle-in-cell (PIC) simulations, we reveal the importance of photocurrent mechanisms besides transverse and longitudinal plasma waves for laser intensities >10(15) W/cm(2). We demonstrate the following. (i) With two-color pulses, photoionization prevails in the generation of GV/m THz fields up to 10(17) W/cm(2) laser intensities and suddenly loses efficiency near the relativistic threshold, as the outermost electron shell of ionized Ar atoms has been fully depleted. (ii) PIC results can be explained by a one-dimensional Maxwell-fluid model and its semi-analytical solutions, offering the first unified description of the main THz sources created in plasmas. (iii) The THz power emitted outside the plasma channel mostly originates from the transverse currents.
Terahertz radiation driven by two-color laser pulses at near-relativistic intensities: Competition between photoionization and wakefield effects

PubMed Central

González de Alaiza Martínez, P.; Davoine, X.; Debayle, A.; Gremillet, L.; Bergé, L.

2016-01-01

We numerically investigate terahertz (THz) pulse generation by linearly-polarized, two-color femtosecond laser pulses in highly-ionized argon. Major processes consist of tunneling photoionization and ponderomotive forces associated with transverse and longitudinal field excitations. By means of two-dimensional particle-in-cell (PIC) simulations, we reveal the importance of photocurrent mechanisms besides transverse and longitudinal plasma waves for laser intensities >1015 W/cm2. We demonstrate the following. (i) With two-color pulses, photoionization prevails in the generation of GV/m THz fields up to 1017 W/cm2 laser intensities and suddenly loses efficiency near the relativistic threshold, as the outermost electron shell of ionized Ar atoms has been fully depleted. (ii) PIC results can be explained by a one-dimensional Maxwell-fluid model and its semi-analytical solutions, offering the first unified description of the main THz sources created in plasmas. (iii) The THz power emitted outside the plasma channel mostly originates from the transverse currents. PMID:27255689
Collective Modes and Structural Modulation in Ni-Mn-Ga(Co) Martensite Thin Films Probed by Femtosecond Spectroscopy and Scanning Tunneling Microscopy.

PubMed

Schubert, M; Schaefer, H; Mayer, J; Laptev, A; Hettich, M; Merklein, M; He, C; Rummel, C; Ristow, O; Großmann, M; Luo, Y; Gusev, V; Samwer, K; Fonin, M; Dekorsy, T; Demsar, J

2015-08-14

The origin of the martensitic transition in the magnetic shape memory alloy Ni-Mn-Ga has been widely discussed. While several studies suggest it is electronically driven, the adaptive martensite model reproduced the peculiar nonharmonic lattice modulation. We used femtosecond spectroscopy to probe the temperature and doping dependence of collective modes, and scanning tunneling microscopy revealed the corresponding static modulations. We show that the martensitic phase can be described by a complex charge-density wave tuned by magnetic ordering and strong electron-lattice coupling.
Collective Modes and Structural Modulation in Ni-Mn-Ga(Co) Martensite Thin Films Probed by Femtosecond Spectroscopy and Scanning Tunneling Microscopy

NASA Astrophysics Data System (ADS)

Schubert, M.; Schaefer, H.; Mayer, J.; Laptev, A.; Hettich, M.; Merklein, M.; He, C.; Rummel, C.; Ristow, O.; Großmann, M.; Luo, Y.; Gusev, V.; Samwer, K.; Fonin, M.; Dekorsy, T.; Demsar, J.

2015-08-01

The origin of the martensitic transition in the magnetic shape memory alloy Ni-Mn-Ga has been widely discussed. While several studies suggest it is electronically driven, the adaptive martensite model reproduced the peculiar nonharmonic lattice modulation. We used femtosecond spectroscopy to probe the temperature and doping dependence of collective modes, and scanning tunneling microscopy revealed the corresponding static modulations. We show that the martensitic phase can be described by a complex charge-density wave tuned by magnetic ordering and strong electron-lattice coupling.
Pump-probe STM light emission spectroscopy for detection of photo-induced semiconductor-metal phase transition of VO2

NASA Astrophysics Data System (ADS)

Sakai, Joe; Katano, Satoshi; Kuwahara, Masashi; Uehara, Yoichi

2017-10-01

We attempted to observe pump-probe scanning tunneling microscopy (STM)-light emission (LE) from a VO2 thin film grown on a rutile TiO2(0 0 1) substrate, with an Ag tip fixed over a semiconducting domain. Laser pulses from a Ti:sapphire laser (wavelength 920 nm pulse width less than 1.5 ps) irradiated the tip-sample gap as pump and probe light sources. With a photon energy of 2.7 eV, suggesting phase transition from semiconducting monoclinic (M) to metallic rutile (R) phases in relation to the electronic band structure, faint LE was observed roughly 30 ps after the irradiation of the pump pulse, followed by retention for roughly 20 ps. The incident energy fluence of the pump pulse at the gap was five orders of magnitude lower than the threshold value for reported photo-induced M-R phase transition. The mechanism that makes it possible to reduce the threshold fluence is discussed.

Pump-probe STM light emission spectroscopy for detection of photo-induced semiconductor-metal phase transition of VO2.

PubMed

Sakai, Joe; Katano, Satoshi; Kuwahara, Masashi; Uehara, Yoichi

2017-10-11

We attempted to observe pump-probe scanning tunneling microscopy (STM)-light emission (LE) from a VO 2 thin film grown on a rutile TiO 2 (0 0 1) substrate, with an Ag tip fixed over a semiconducting domain. Laser pulses from a Ti:sapphire laser (wavelength 920 nm; pulse width less than 1.5 ps) irradiated the tip-sample gap as pump and probe light sources. With a photon energy of 2.7 eV, suggesting phase transition from semiconducting monoclinic (M) to metallic rutile (R) phases in relation to the electronic band structure, faint LE was observed roughly 30 ps after the irradiation of the pump pulse, followed by retention for roughly 20 ps. The incident energy fluence of the pump pulse at the gap was five orders of magnitude lower than the threshold value for reported photo-induced M-R phase transition. The mechanism that makes it possible to reduce the threshold fluence is discussed.
User oriented end-station on VUV pump-probe magneto-optical ellipsometry at ELI beamlines

NASA Astrophysics Data System (ADS)

Espinoza, Shirly; Neuber, Gerd; Brooks, Christopher D.; Besner, Bastian; Hashemi, Maryam; Rübhausen, Michael; Andreasson, Jakob

2017-11-01

A state of the art ellipsometer for user operations is being implemented at ELI Beamlines in Prague, Czech Republic. It combines three of the most promising and exotic forms of ellipsometry: VUV, pump-probe and magneto-optical ellipsometry. This new ellipsometer covers a spectral operational range from the NIR up to the VUV, with high through-put between 1 and 40 eV. The ellipsometer also allows measurements of magneto-optical spectra with a 1 kHz switchable magnetic field of up to 1.5 T across the sample combining ellipsometry and Kerr spectroscopy measurements in an unprecedented spectral range. This form of generalized ellipsometry enables users to address diagonal and off-diagonal components of the dielectric tensor within one measurement. Pump-probe measurements enable users to study the dynamic behaviour of the dielectric tensor in order to resolve the time-domain phenomena in the femto to 100 ns range.
Femtosecond transient absorption dynamics of close-packed gold nanocrystal monolayer arrays*1

NASA Astrophysics Data System (ADS)

Eah, Sang-Kee; Jaeger, Heinrich M.; Scherer, Norbert F.; Lin, Xiao-Min; Wiederrecht, Gary P.

2004-03-01

Femtosecond transient absorption spectroscopy is used to investigate hot electron dynamics of close-packed 6 nm gold nanocrystal monolayers. Morphology changes of the monolayer caused by the laser pump pulse are monitored by transmission electron microscopy. At low pump power, the monolayer maintains its structural integrity. Hot electrons induced by the pump pulse decay through electron-phonon (e-ph) coupling inside the nanocrystals with a decay constant that is similar to the value for bulk films. At high pump power, irreversible particle aggregation and sintering occur in the nanocrystal monolayer, which cause damping and peak shifting of the transient bleach signal.
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.
Near shot-noise limited time-resolved circular dichroism pump-probe spectrometer

NASA Astrophysics Data System (ADS)

Stadnytskyi, Valentyn; Orf, Gregory S.; Blankenship, Robert E.; Savikhin, Sergei

2018-03-01

We describe an optical near shot-noise limited time-resolved circular dichroism (TRCD) pump-probe spectrometer capable of reliably measuring circular dichroism signals in the order of μdeg with nanosecond time resolution. Such sensitivity is achieved through a modification of existing TRCD designs and introduction of a new data processing protocol that eliminates approximations that have caused substantial nonlinearities in past measurements and allows the measurement of absorption and circular dichroism transients simultaneously with a single pump pulse. The exceptional signal-to-noise ratio of the described setup makes the TRCD technique applicable to a large range of non-biological and biological systems. The spectrometer was used to record, for the first time, weak TRCD kinetics associated with the triplet state energy transfer in the photosynthetic Fenna-Matthews-Olson antenna pigment-protein complex.
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.
Carrier-phase control among subharmonic pulses in a femtosecond optical parametric oscillator.

PubMed

Kobayashi, Y; Torizuka, K

2001-08-15

We have generated femtosecond subharmonic pulses by using an optical parametric oscillator. The optical frequencies of the idler and the signal are one third and two thirds, respectively, of the optical frequency of the pump pulse. The carrier phase of the signal pulse relative to that of the pump pulse was locked by electronic feedback. The carrier-envelope phase slip frequency of the signal pulse relative to that of the pump was locked to F/6 , where F is defined as the repetition frequency.
Photoionization bands of rubidium molecule

NASA Astrophysics Data System (ADS)

Rakić, M.; Pichler, G.

2018-03-01

We studied the absorption spectrum of dense rubidium vapor generated in a T-type sapphire cell with a special emphasis on the structured photoionization continuum observed in the 200-300 nm spectral region. The photoionization spectrum has a continuous atomic contribution with a pronounced Seaton-Cooper minimum at about 250 nm and a molecular photoionization contribution with many broad bands. We discuss the possible origin of the photoionization bands as stemming from the absorption from the ground state of the Rb2 molecule to excited states of Rb2+* and to doubly excited autoionizing states of Rb2** molecule. All these photoionization bands are located above the Rb+ and Rb2+ ionization limits.
Distinguishing between relaxation pathways by combining dissociative ionization pump probe spectroscopy and ab initio calculations: a case study of cytosine.

PubMed

Kotur, Marija; Weinacht, Thomas C; Zhou, Congyi; Kistler, Kurt A; Matsika, Spiridoula

2011-05-14

We present a general method for tracking molecular relaxation along different pathways from an excited state down to the ground state. We follow the excited state dynamics of cytosine pumped near the S(0)-S(1) resonance using ultrafast laser pulses in the deep ultraviolet and probed with strong field near infrared pulses which ionize and dissociate the molecules. The fragment ions are detected via time of flight mass spectroscopy as a function of pump probe delay and probe pulse intensity. Our measurements reveal that different molecular fragments show different timescales, indicating that there are multiple relaxation pathways down to the ground state. We interpret our measurements with the help of ab initio electronic structure calculations of both the neutral molecule and the molecular cation for different conformations en route to relaxation back down to the ground state. Our measurements and calculations show passage through two seams of conical intersections between ground and excited states and demonstrate the ability of dissociative ionization pump probe measurements in conjunction with ab initio electronic structure calculations to track molecular relaxation through multiple pathways.
Miniature fiber-optic multiphoton microscopy system using frequency-doubled femtosecond Er-doped fiber laser

PubMed Central

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

2016-01-01

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

NASA Technical Reports Server (NTRS)

Aikin, A. C.; Maier, E. J. R.

1978-01-01

A balloon-borne photoionization mass spectrometer used to measure stratospheric trace gases is described. Ions are created with photons from high-intensity krypton discharge lamps and a quadrupole mass analyzer is employed for ion identification. Differential pumping is achieved with liquid helium cryopumping. To insure measurement of unperturbed stratospheric air, the entire system is contained in a sealed gondola and the atmospheric sample is taken some distance away during descent. The photoionization technique allows the detection of a low ionization potential constituent, such as nitric oxide, at less than a part in one billion in the presence of the major atmospheric gases and their isotopes. Operation of the mass spectrometer system was demonstrated during a daytime flight from Palestine, Texas on 26 April 1977. The sensitivity achieved and the unique selectivity afforded by this technique offer a capability for trace constituent measurement not possible with the more conventional electron impact ionization approach.
Photoionization Rate of Atomic Oxygen

NASA Astrophysics Data System (ADS)

Meier, R. R.; McLaughlin, B. M.; Warren, H. P.; Bishop, J.

2006-05-01

Accurate knowledge of the photoionization rate of atomic oxygen is important for the study and understanding of the ionospheres and emission processes of terrestrial, planetary, and cometary atmospheres. Past calculations of the photoionization rate have been carried out at various spectral resolutions, but none were at sufficiently high resolution to accommodate accidental resonances between solar emission lines and highly structured auto-ionization features in the photoionization cross section. A new version of the NRLEUV solar spectral irradiance model (at solar minimum) and a new model of the O photoionization cross section enable calculations at very high spectral resolution. We find unattenuated photoionization rates computed at 0.001 nm resolution are larger than those at moderate resolution (0.1 nm) by amounts approaching 20%. Allowing for attenuation in the terrestrial atmosphere, we find differences in photoionization rates computed at high and moderate resolution to vary with altitude, especially below 200 km where deviations of plus or minus 20% occur between the two cases.
Raman conversion in intense femtosecond Bessel beams in air

NASA Astrophysics Data System (ADS)

Scheller, Maik; Chen, Xi; Ariunbold, Gombojav O.; Born, Norman; Moloney, Jerome; Kolesik, Miroslav; Polynkin, Pavel

2014-05-01

We demonstrate experimentally that bright and nearly collimated radiation can be efficiently generated in air pumped by an intense femtosecond Bessel beam. We show that this nonlinear conversion process is driven by the rotational Raman response of air molecules. Under optimum conditions, the conversion efficiency from the Bessel pump into the on-axis propagating beam exceeds 15% and is limited by the onset of intensity clamping and plasma refraction on the beam axis. Our experimental findings are in excellent agreement with numerical simulations based on the standard model for the ultrafast nonlinear response of air.
FAST TRACK COMMUNICATION: Generalized geometrical model for photoionization of polarized atoms: II. Magnetic dichroism in the 3p photoemission from the K 3p64s 2S1/2 ground state

NASA Astrophysics Data System (ADS)

Grum-Grzhimailo, A. N.; Cubaynes, D.; Heinecke, E.; Hoffmann, P.; Zimmermann, P.; Meyer, M.

2010-10-01

The generalized geometrical model for photoionization from polarized atoms is extended to include mixing of configurations in the initial atomic and/or the final photoion states. The theoretical results for angle-resolved linear and circular magnetic dichroism are in good agreement with new high-resolution photoelectron data for 3p-1 photoionization of potassium atoms polarized in the K 3p64s 2S1/2 ground state by laser optical pumping.
Measurement of the photoionization cross section from the laser-populated 3D metastable levels in barium

NASA Technical Reports Server (NTRS)

Carlsten, J. L.; Mcilrath, T. J.; Parkinson, W. H.

1974-01-01

Measurements of the absolute photoionization cross section from the 6s5d 3D metastable level of barium are presented. The 3D levels were selectively populated with a high-power tuneable dye laser. The number density was determined by observing the resulting depopulation of the ground state when pumping occurred.
Time-resolved study of femtosecond laser induced micro-modifications inside transparent brittle materials

NASA Astrophysics Data System (ADS)

Hendricks, F.; Matylitsky, V. V.; Domke, M.; Huber, Heinz P.

2016-03-01

Laser processing of optically transparent or semi-transparent, brittle materials is finding wide use in various manufacturing sectors. For example, in consumer electronic devices such as smartphones or tablets, cover glass needs to be cut precisely in various shapes. The unique advantage of material processing with femtosecond lasers is efficient, fast and localized energy deposition in nearly all types of solid materials. When an ultra-short laser pulse is focused inside glass, only the localized region in the neighborhood of the focal volume absorbs laser energy by nonlinear optical absorption. Therefore, the processing volume is strongly defined, while the rest of the target stays unaffected. Thus ultra-short pulse lasers allow cutting of the chemically strengthened glasses such as Corning Gorilla glass without cracking. Non-ablative cutting of transparent, brittle materials, using the newly developed femtosecond process ClearShapeTM from Spectra-Physics, is based on producing a micron-sized material modification track with well-defined geometry inside. The key point for development of the process is to understand the induced modification by a single femtosecond laser shot. In this paper, pump-probe microscopy techniques have been applied to study the defect formation inside of transparent materials, namely soda-lime glass samples, on a time scale between one nanosecond to several tens of microseconds. The observed effects include acoustic wave propagation as well as mechanical stress formation in the bulk of the glass. Besides better understanding of underlying physical mechanisms, our experimental observations have enabled us to find optimal process parameters for the glass cutting application and lead to better quality and speed for the ClearShapeTM process.
Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization.

PubMed

Germann, Matthias; Willitsch, Stefan

2016-07-28

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

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

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

2016-07-28

We develop a model for predicting fine- and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra, we derive highly symmetrized forms of the squared photoionization dipole matrix elements from which we derive the salient selection and propensity rules for fine- and hyperfine resolved photoionizing transitions. Our theoretical results are validated by the analysis of the fine-structure resolved photoelectron spectrum of O{sub 2} reported by Palm and Merkt [Phys. Rev. Lett. 81, 1385 (1998)] and are used for predicting hyperfine populations of molecular ionsmore » produced by photoionization.« less
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.
Fiber-based modulated optical reflectance configuration allowing for offset pump and probe beams

NASA Astrophysics Data System (ADS)

Fleming, A.; Folsom, C.; Jensen, C.; Ban, H.

2016-12-01

A new fiber-based modulated optical reflectance configuration is developed in this work. The technique maintains the fiber-based heating laser (pump) and detection laser (probe) in close proximity at a fixed separation distance in a ceramic ferrule. The pump beam periodically heats the sample inducing thermal waves into the sample. The probe beam measures the temperature response at a known distance from the pump beam over a range of heating modulation frequencies. The thermal diffusivity of the sample may be calculated from the phase response between the input heat flux and the temperature response of a sample having a reflective surface. The unique measurement configuration is ideal for in situ measurements and has many advantages for laboratory-based systems. The design and development of the system are reported along with theoretical justification for the experimental design. The thermal diffusivities of Ge and SiC are measured and found to be within 10% of reported literature values. The diffusivity for SiO2 is measured with a relative difference of approximately 100% from the literature value when the ferrule is in contact with the sample. An additional measurement was made on the SiO2 sample with the ferrule not in contact resulting in a difference of less than 2% from the literature value. The difference in the SiO2 measurement when the ferrule is in contact with the sample is likely due to a parallel heat transfer path through the dual-fiber ferrule assembly.

Fiber-based modulated optical reflectance configuration allowing for offset pump and probe beams.

PubMed

Fleming, A; Folsom, C; Jensen, C; Ban, H

2016-12-01

A new fiber-based modulated optical reflectance configuration is developed in this work. The technique maintains the fiber-based heating laser (pump) and detection laser (probe) in close proximity at a fixed separation distance in a ceramic ferrule. The pump beam periodically heats the sample inducing thermal waves into the sample. The probe beam measures the temperature response at a known distance from the pump beam over a range of heating modulation frequencies. The thermal diffusivity of the sample may be calculated from the phase response between the input heat flux and the temperature response of a sample having a reflective surface. The unique measurement configuration is ideal for in situ measurements and has many advantages for laboratory-based systems. The design and development of the system are reported along with theoretical justification for the experimental design. The thermal diffusivities of Ge and SiC are measured and found to be within 10% of reported literature values. The diffusivity for SiO 2 is measured with a relative difference of approximately 100% from the literature value when the ferrule is in contact with the sample. An additional measurement was made on the SiO 2 sample with the ferrule not in contact resulting in a difference of less than 2% from the literature value. The difference in the SiO 2 measurement when the ferrule is in contact with the sample is likely due to a parallel heat transfer path through the dual-fiber ferrule assembly.
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.
Pump-probe imaging of laser-induced periodic surface structures after ultrafast irradiation of Si

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

Murphy, Ryan D.; Torralva, Ben; Adams, David P.

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

Picón, A.; Lehmann, C. S.; Bostedt, C.

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 XeF 2 molecules following X-ray absorption at the Xe site.« less
Attosecond Spectroscopy Probing Electron Correlation Dynamics

NASA Astrophysics Data System (ADS)

Winney, Alexander H.

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

PubMed

Smolentsev, Grigory; Guda, Alexander; Zhang, Xiaoyi; Haldrup, Kristoffer; Andreiadis, Eugen; Chavarot-Kerlidou, Murielle; Canton, Sophie E; Nachtegaal, Maarten; Artero, Vincent; Sundstrom, Villy

2013-08-29

A new setup for pump-flow-probe X-ray absorption spectroscopy has been implemented at the SuperXAS beamline of the Swiss Light Source. It allows recording X-ray absorption spectra with a time resolution of tens of microseconds and high detection efficiency for samples with sub-mM concentrations. A continuous wave laser is used for the photoexcitation, with the distance between laser and X-ray beams and velocity of liquid flow determining the time delay, while the focusing of both beams and the flow speed define the time resolution. This method is compared with the alternative measurement technique that utilizes a 1 kHz repetition rate laser and multiple X-ray probe pulses. Such an experiment was performed at beamline 11ID-D of the Advanced Photon Source. Advantages, limitations and potential for improvement of the pump-flow-probe setup are discussed by analyzing the photon statistics. Both methods, with Co K-edge probing were applied to the investigation of a cobaloxime-based photo-catalytic reaction. The interplay between optimizing for efficient photoexcitation and time resolution as well as the effect of sample degradation for these two setups are discussed.
Pump-Flow-Probe X-Ray Absorption Spectroscopy as a Tool for Studying Intermediate States of Photocatalytic Systems

PubMed Central

Smolentsev, Grigory; Guda, Alexander; Zhang, XIaoyi; Haldrup, Kristoffer; Andreiadis, Eugen; Chavarot-Kerlidou, Murielle; Canton, Sophie E.; Nachtegaal, Maarten; Artero, Vincent; Sundstrom, Villy

2014-01-01

A new setup for pump-flow-probe X-ray absorption spectroscopy has been implemented at the SuperXAS beamline of the Swiss Light Source. It allows recording X-ray absorption spectra with a time resolution of tens of microseconds and high detection efficiency for samples with sub-mM concentrations. A continuous wave laser is used for the photoexcitation, with the distance between laser and X-ray beams and velocity of liquid flow determining the time delay, while the focusing of both beams and the flow speed define the time resolution. This method is compared with the alternative measurement technique that utilizes a 1 kHz repetition rate laser and multiple X-ray probe pulses. Such an experiment was performed at beamline 11ID-D of the Advanced Photon Source. Advantages, limitations and potential for improvement of the pump-flow-probe setup are discussed by analyzing the photon statistics. Both methods, with Co K-edge probing were applied to the investigation of a cobaloxime-based photo-catalytic reaction. The interplay between optimizing for efficient photoexcitation and time resolution as well as the effect of sample degradation for these two setups are discussed. PMID:24443663
Probing the nuclear susceptibility of mesoionic compounds using two-beam coupling with chirp-controlled pulses

NASA Astrophysics Data System (ADS)

Bosco, Carlos A. C.; Maciel, Glauco S.; Rakov, Nikifor; de Araújo, Cid B.; Acioli, Lúcio H.; Simas, Alfredo M.; Athayde-Filho, Petrônio F.; Miller, Joseph

2007-11-01

The third-order non-linear optical response of mesoionic compounds (MIC) in dimethylsulfoxide (DMSO) and methanol solutions was investigated by use of collinear pump and probe technique with chirp-controlled femtosecond pulses. The experiments allowed the investigation of non-instantaneous nuclear processes and thermal effects induced by two-photon absorption (TPA). We found that the nuclear non-linearity of MIC in DMSO is ˜1/5 the benzene, which was used as a reference material. This result is attributed to the large inertia of MIC to rotation, compared to benzene. The results for MIC in methanol indicate the influence of thermal effects due to TPA.
THz pulse doubler at FLASH: double pulses for pump-probe experiments at X-ray FELs.

PubMed

Zapolnova, Ekaterina; Golz, Torsten; Pan, Rui; Klose, Karsten; Schreiber, Siegfried; Stojanovic, Nikola

2018-01-01

FLASH, the X-ray free-electron laser in Hamburg, Germany, employs a narrowband high-field accelerator THz source for unique THz pump X-ray probe experiments. However, the large difference in optical paths of the THz and X-ray beamlines prevents utilization of the machine's full potential (e.g. extreme pulse energies in the soft X-ray range). To solve this issue, lasing of double electron bunches, separated by 28 periods of the driving radiofrequency (at 1.3 GHz), timed for the temporal overlap of THz and X-ray pulses at the experimental station has been employed. In order to optimize conditions for a typical THz pump X-ray probe experiment, X-ray lasing of the first bunch to one-sixth of that of the second has been suppressed. Finally, synchronization of THz radiation pulses was measured to be ∼20 fs (r.m.s.), and a solution for monitoring the arrival time for achieving higher temporal resolution is presented.
Label-Free Imaging of Female Genital Tract Melanocytic Lesions With Pump-Probe Microscopy: A Promising Diagnostic Tool.

PubMed

Robles, Francisco E; Deb, Sanghamitra; Fischer, Martin C; Warren, Warren S; Selim, Maria Angelica

2017-04-01

Melanomas of the female genital tract present a unique clinical challenge. Not only are these lesions in an anatomically sensitive area, but also they tend to be multifocal and have high recurrence rates. Furthermore, several benign melanocytic proliferations resemble early-stage melanoma clinically and/or histopathologically. Thus, there is a significant need for additional tools that can help correctly diagnose and stage these lesions. Here, we quantitatively and nondestructively analyze the chemical composition of melanin in excised pigmented lesions of the female genital tract using pump-probe microscopy, a high-resolution optical imaging technique that is sensitive to many biochemical properties of melanin. Thirty-one thin (~5 μm) tissue sections previously excised from female genital tract melanocytic lesions were imaged with pump-probe microscopy and analyzed. We find significant quantitative differences in melanin type and structure between melanoma and nonmalignant melanocytic proliferations. Our analysis also suggests a link between the molecular signatures of melanins and lesion-specific genetic mutations. Finally, significant differences are found between metastatic and nonmetastatic melanomas. The limitations of this work include the fact that molecular information is restricted to melanin pigment and the sample size is relatively small. Pump-probe microscopy provides unique information regarding the biochemical composition of genital tract melanocytic lesions, which can be used to improve the diagnosis and staging of vulvar melanomas.
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.
Dynamical interferences to probe short-pulse photoassociation of Rb atoms and stabilization of Rb{sub 2} dimers

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

Mur-Petit, Jordi; Luc-Koenig, Eliane; Masnou-Seeuws, Francoise

2007-06-15

We analyze the formation of Rb{sub 2} molecules with short photoassociation pulses applied to a cold {sup 85}Rb sample. A pump laser pulse couples a continuum level of the ground electronic state X {sup 1}{sigma}{sub g}{sup +} with bound levels in the 0{sub u}{sup +}(5S+5P{sub 1/2}) and 0{sub u}{sup +}(5S+5P{sub 3/2}) vibrational series. The nonadiabatic coupling between the two excited channels induces time-dependent beatings in the populations. We propose to take advantage of these oscillations to design further laser pulses that probe the photoassociation process via photoionization or that optimize the stabilization in deep levels of the ground state.
Vibrational spectroscopy of water in hydrated lipid multi-bilayers. I. Infrared spectra and ultrafast pump-probe observables.

PubMed

Gruenbaum, S M; Skinner, J L

2011-08-21

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 H(2)O. 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
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
Molecular dynamics simulation of shock wave and spallation phenomena in metal foils irradiated by femtosecond laser pulse

NASA Astrophysics Data System (ADS)

Zhakhovsky, Vasily; Demaske, Brian; Inogamov, Nail; Oleynik, Ivan

2010-03-01

Femtosecond laser irradiation of metals is an effective technique to create a high-pressure frontal layer of 100-200 nm thickness. The associated ablation and spallation phenomena can be studied in the laser pump-probe experiments. We present results of a large-scale MD simulation of ablation and spallation dynamics developing in 1,2,3μm thick Al and Au foils irradiated by a femtosecond laser pulse. Atomic-scale mechanisms of laser energy deposition, transition from pressure wave to shock, reflection of the shock from the rear-side of the foil, and the nucleation of cracks in the reflected tensile wave, having a very high strain rate, were all studied. To achieve a realistic description of the complex phenomena induced by strong compression and rarefaction waves, we developed new embedded atom potentials for Al and Au based on cold pressure curves. MD simulations revealed the complex interplay between spallation and ablation processes: dynamics of spallation depends on the pressure profile formed in the ablated zone at the early stage of laser energy absorption. It is shown that the essential information such as material properties at high strain rate and spall strength can be extracted from the simulated rear-side surface velocity as a function of time.
Novel electronic ferroelectricity in an organic charge-order insulator investigated with terahertz-pump optical-probe spectroscopy

PubMed Central

Yamakawa, H.; Miyamoto, T.; Morimoto, T.; Yada, H.; Kinoshita, Y.; Sotome, M.; Kida, N.; Yamamoto, K.; Iwano, K.; Matsumoto, Y.; Watanabe, S.; Shimoi, Y.; Suda, M.; Yamamoto, H. M.; Mori, H.; Okamoto, H.

2016-01-01

In electronic-type ferroelectrics, where dipole moments produced by the variations of electron configurations are aligned, the polarization is expected to be rapidly controlled by electric fields. Such a feature can be used for high-speed electric-switching and memory devices. Electronic-type ferroelectrics include charge degrees of freedom, so that they are sometimes conductive, complicating dielectric measurements. This makes difficult the exploration of electronic-type ferroelectrics and the understanding of their ferroelectric nature. Here, we show unambiguous evidence for electronic ferroelectricity in the charge-order (CO) phase of a prototypical ET-based molecular compound, α-(ET)2I3 (ET:bis(ethylenedithio)tetrathiafulvalene), using a terahertz pulse as an external electric field. Terahertz-pump second-harmonic-generation(SHG)-probe and optical-reflectivity-probe spectroscopy reveal that the ferroelectric polarization originates from intermolecular charge transfers and is inclined 27° from the horizontal CO stripe. These features are qualitatively reproduced by the density-functional-theory calculation. After sub-picosecond polarization modulation by terahertz fields, prominent oscillations appear in the reflectivity but not in the SHG-probe results, suggesting that the CO is coupled with molecular displacements, while the ferroelectricity is electronic in nature. The results presented here demonstrate that terahertz-pump optical-probe spectroscopy is a powerful tool not only for rapidly controlling polarizations, but also for clarifying the mechanisms of ferroelectricity. PMID:26864779
Novel electronic ferroelectricity in an organic charge-order insulator investigated with terahertz-pump optical-probe spectroscopy.

PubMed

Yamakawa, H; Miyamoto, T; Morimoto, T; Yada, H; Kinoshita, Y; Sotome, M; Kida, N; Yamamoto, K; Iwano, K; Matsumoto, Y; Watanabe, S; Shimoi, Y; Suda, M; Yamamoto, H M; Mori, H; Okamoto, H

2016-02-11

In electronic-type ferroelectrics, where dipole moments produced by the variations of electron configurations are aligned, the polarization is expected to be rapidly controlled by electric fields. Such a feature can be used for high-speed electric-switching and memory devices. Electronic-type ferroelectrics include charge degrees of freedom, so that they are sometimes conductive, complicating dielectric measurements. This makes difficult the exploration of electronic-type ferroelectrics and the understanding of their ferroelectric nature. Here, we show unambiguous evidence for electronic ferroelectricity in the charge-order (CO) phase of a prototypical ET-based molecular compound, α-(ET)2I3 (ET:bis(ethylenedithio)tetrathiafulvalene), using a terahertz pulse as an external electric field. Terahertz-pump second-harmonic-generation(SHG)-probe and optical-reflectivity-probe spectroscopy reveal that the ferroelectric polarization originates from intermolecular charge transfers and is inclined 27° from the horizontal CO stripe. These features are qualitatively reproduced by the density-functional-theory calculation. After sub-picosecond polarization modulation by terahertz fields, prominent oscillations appear in the reflectivity but not in the SHG-probe results, suggesting that the CO is coupled with molecular displacements, while the ferroelectricity is electronic in nature. The results presented here demonstrate that terahertz-pump optical-probe spectroscopy is a powerful tool not only for rapidly controlling polarizations, but also for clarifying the mechanisms of ferroelectricity.
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.
Confocal ultrafast pump-probe spectroscopy: a new technique to explore nanoscale composites.

PubMed

Virgili, Tersilla; Grancini, Giulia; Molotokaite, Egle; Suarez-Lopez, Inma; Rajendran, Sai Kiran; Liscio, Andrea; Palermo, Vincenzo; Lanzani, Guglielmo; Polli, Dario; Cerullo, Giulio

2012-04-07

This article is devoted to the exploration of the benefits of a new ultrafast confocal pump-probe technique, able to study the photophysics of different structured materials with nanoscale resolution. This tool offers many advantages over standard stationary microscopy techniques because it directly interrogates excited state dynamics in molecules, providing access to both radiative and non-radiative deactivation processes at a local scale. In this paper we present a few different examples of its application to organic semiconductor systems. The first two are focussed on the study of the photophysics of phase-separated polymer blends: (i) a blue-emitting polyfluorene (PFO) in an inert matrix of PMMA and (ii) an electron donor polythiophene (P3HT) mixed with an electron acceptor fullerene derivative (PCBM). The experimental results on these samples demonstrate the capability of the technique to unveil peculiar interfacial dynamics at the border region between phase-segregated domains, which would be otherwise averaged out using conventional pump-probe spectroscopy. The third example is the study of the photophysics of isolated mesoscopic crystals of the PCBM molecule. Our ultrafast microscope could evidence the presence of two distinctive regions within the crystals. In particular, we could pinpoint for the first time areas within the crystals showing photobleaching/stimulated emission signals from a charge-transfer state. This journal is © The Royal Society of Chemistry 2012
Probing Intermolecular Interactions in Binary Liquid Mixtures Using Femtosecond Laser-Induced Self-Defocusing.

PubMed

Maurya, Sandeep Kumar; Das, Dhiman; Goswami, Debabrata

2016-06-13

Photo-thermal behavior of binary liquid mixtures has been studied by high repetition rate (HRR) Z-scan technique with femtosecond laser pulses. Changes in the peak-valley difference in transmittance (ΔT P-V ) for closed aperture Z-scan experiments are indicative of thermal effects induced by HRR femtosecond laser pulses. We show such indicative results can have a far-reaching impact on molecular properties and intermolecular interactions in binary liquid mixtures. Spectroscopic parameters derived from this experimental technique show that the combined effect of physical and molecular properties of the constituent binary liquids can be related to the components of the binary liquid. © The Author(s) 2016.

Design of Portable Mass Spectrometers with Handheld Probes: Aspects of the Sampling and Miniature Pumping Systems

NASA Astrophysics Data System (ADS)

Chen, Chien-Hsun; Chen, Tsung-Chi; Zhou, Xiaoyu; Kline-Schoder, Robert; Sorensen, Paul; Cooks, R. Graham; Ouyang, Zheng

2015-02-01

Miniature mass spectrometry analytical systems of backpack configuration fitted with sampling probes could potentially be of significant interest for in-field, real-time chemical analysis. In this study, various configurations were explored in which a long narrow tube was used to connect the turbo and backing pumps used to create and maintain vacuum. Also, for the first time we introduced two new types of pumps for miniature mass spectrometers, the Creare 130 g drag pump and Creare 350 g scroll backing pump. These pumps, along with another Creare 550 turbo pump and the commercially available Pfeiffer HiPace 10 turbo and KnF diaphragm backing pumps, were tested with the backpack configurations. The system performance, especially the scan time, was characterized when used with a discontinuous atmospheric pressure interface (DAPI) for ion introduction. The pumping performance in the pressure region above 1 mtorr is critical for DAPI operation. The 550 g turbo pump was shown to have a relatively higher pumping speed above 1 mtorr and gave a scan time of 300 ms, almost half the value obtained with the larger, heavier HiPace 10 often used with miniature mass spectrometers. The 350 g scroll pump was also found to be an improvement over the diaphragm pumps generally used as backing pumps. With a coaxial low temperature plasma ion source, direct analysis of low volatility compounds glass slides was demonstrated, including 1 ng DNP (2,4-Dinitrophenol) and 10 ng TNT (2,4,6-trinitrotoluene) with Creare 550 g turbo pump as well as 10 ng cocaine and 20 ng DNP with Creare 130 g drag pump.
Design of Portable Mass Spectrometers with Handheld Probes: Aspects of the Sampling and Miniature Pumping Systems

PubMed Central

Chen, Chien-Hsun; Chen, Tsung-Chi; Zhou, Xiaoyu; Kline-Schoder, Robert; Sorensen, Paul; Cooks, R. Graham; Ouyang, Zheng

2014-01-01

Miniature mass spectrometry analytical systems of backpack configuration fitted with sampling probes could potentially be of significant interest for in-field, real-time chemical analysis. In this study, various configurations were explored in which a long narrow tube was used to connect the turbo and backing pumps used to create and maintain vacuum. Also, for the first time we introduced two new types of pumps for miniature mass spectrometers, the Creare 130g drag pump and Creare 350g scroll backing pump. These pumps, along with another Creare 550 turbo pump and the commercially available Pfeiffer HiPace 10 turbo and KnF diaphragm backing pumps, were tested with the backpack configurations. The system performance, especially the scan time, was characterized when used with a discontinuous atmospheric pressure interface (DAPI) for ion introduction. The pumping performance in the pressure region above 1 mtorr is critical for DAPI operation. The 550g turbo pump was shown to have a relatively higher pumping speed above 1 mtorr and gave a scan time of 300 ms, almost half the value obtained with the larger, heavier HiPace 10 often used with miniature mass spectrometers. The 350 g scroll pump was also found to be an improvement over the diaphragm pumps generally used as backing pumps. With a coaxial low temperature plasma ion source, direct analysis of low volatility compounds glass slides was demonstrated, including 1 ng DNP (2,4-Dinitrophenol) and 10ng TNT (2,4,6-trinitrotoluene) with Creare 550g turbo pump as well as 10 ng cocaine and 20 ng DNP with Creare 130g drag pump. PMID:25404157
Design of portable mass spectrometers with handheld probes: aspects of the sampling and miniature pumping systems.

PubMed

Chen, Chien-Hsun; Chen, Tsung-Chi; Zhou, Xiaoyu; Kline-Schoder, Robert; Sorensen, Paul; Cooks, R Graham; Ouyang, Zheng

2015-02-01

Miniature mass spectrometry analytical systems of backpack configuration fitted with sampling probes could potentially be of significant interest for in-field, real-time chemical analysis. In this study, various configurations were explored in which a long narrow tube was used to connect the turbo and backing pumps used to create and maintain vacuum. Also, for the first time we introduced two new types of pumps for miniature mass spectrometers, the Creare 130 g drag pump and Creare 350 g scroll backing pump. These pumps, along with another Creare 550 turbo pump and the commercially available Pfeiffer HiPace 10 turbo and KnF diaphragm backing pumps, were tested with the backpack configurations. The system performance, especially the scan time, was characterized when used with a discontinuous atmospheric pressure interface (DAPI) for ion introduction. The pumping performance in the pressure region above 1 mtorr is critical for DAPI operation. The 550 g turbo pump was shown to have a relatively higher pumping speed above 1 mtorr and gave a scan time of 300 ms, almost half the value obtained with the larger, heavier HiPace 10 often used with miniature mass spectrometers. The 350 g scroll pump was also found to be an improvement over the diaphragm pumps generally used as backing pumps. With a coaxial low temperature plasma ion source, direct analysis of low volatility compounds glass slides was demonstrated, including 1 ng DNP (2,4-Dinitrophenol) and 10 ng TNT (2,4,6-trinitrotoluene) with Creare 550 g turbo pump as well as 10 ng cocaine and 20 ng DNP with Creare 130 g drag pump.
Using acoustic levitation in synchrotron based laser pump hard x-ray probe experiments

NASA Astrophysics Data System (ADS)

Hu, Bin; Lerch, Jason; Suthar, Kamlesh; Dichiara, Anthony

Acoustic levitation provides a platform to trap and hold a small amount of material by using standing pressure waves without a container. The technique has a potential to be used for laser pump x-ray probe experiments; x-ray scattering and laser distortion from the container can be avoided, sample consumption can be minimized, and unwanted chemistry that may occur at the container interface can be avoided. The method has been used at synchrotron sources for studying protein and pharmaceutical solutions using x-ray diffraction (XRD) and small angle x-ray scattering (SAXS). However, pump-probe experiments require homogeneously excited samples, smaller than the absorption depth of the material that must be held stably at the intersection of both the laser and x-ray beams. We discuss 1) the role of oscillations in acoustic levitation and the optimal acoustic trapping conditions for x-ray/laser experiments, 2) opportunities to automate acoustic levitation for fast sample loading and manipulation, and 3) our experimental results using SAXS to monitor laser induced thermal expansion in gold nanoparticles solution. We also performed Finite Element Analysis to optimize the trapping performance and stability of droplets ranging from 0.4 mm to 2 mm. Our early x-ray/laser demonstrated the potential of the technique for time-resolved X-ray science.
Regenerative Amplification of Femtosecond Pulses: Design andConstruction of a sub-100fs, muon J Laser System

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

Schumacher, Andreas B.

1996-10-01

Femtosecond lasers are a powerful tool for a wealth of applications in physics, chemistry and biology. In most cases, however, their use is fundamentally restricted to a rather narrow spectral range. This thesis deals with the construction and characterization of a femtosecond light source for spectroscopic applications which overcomes that restriction. It is demonstrated how the output of a continuously pumped Ti:sapphire femtosecond oscillator is amplified to the μJ level,while the pulse duration remains below 100 fs. A combination of continuous pumping, acousto-optic switching and Ti:Al 2O 3 as a gain medium allows amplification at high repetition rates. By focusingmore » the high energy pulses into a sapphire crystal, a broad-band continuum can be generated, extended in wavelengths over several hundred nanometers. To accomplish amplification of three orders of magnitude while maintaining the pulse length, a regenerative multipass amplifier system was built. The thesis describes theoretical design, realization and characterization of the system. Theoretical calculations and preliminary measurements were carried out and allow a critical evaluation of the final performance.« less
Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

DOE PAGES

Seo, Minah; Yamaguchi, Hisato; Mohite, Aditya D.; ...

2016-02-15

We performed ultrafast optical microscopy on single flakes of atomically thin CVD-grown molybdenum disulfide, using non-degenerate femtosecond pump-probe spectroscopy to excite and probe carriers above and below the indirect and direct band gaps. These measurements reveal the influence of layer thickness on carrier dynamics when probing near the band gap. Furthermore, fluence-dependent measurements indicate that carrier relaxation is primarily influenced by surface-related defect and trap states after above-bandgap photoexcitation. Furthermore, the ability to probe femtosecond carrier dynamics in individual flakes can thus give much insight into light-matter interactions in these two-dimensional nanosystems.
Research on spectrum broadening covering visible light of a fiber femtosecond optical frequency comb for absolute frequency measurement

NASA Astrophysics Data System (ADS)

Xing, Shuai; Wu, Tengfei; Li, Shuyi; Xia, Chuanqing; Han, Jibo; Zhang, Lei; Zhao, Chunbo

2018-03-01

As a bridge connecting microwave frequency and optical frequency, femtosecond laser has important significance in optical frequency measurement. Compared with the traditional Ti-sapphire femtosecond optical frequency comb, with the advantages of compact structure, strong anti-interference ability and low cost, the fiber femtosecond optical frequency comb has a wider application prospect. An experiment of spectrum broadening in a highly nonlinear photonic crystal fiber pumped by an Er-fiber mode-locked femtosecond laser is studied in this paper. Based on optical amplification and frequency doubling, the central wavelength of the output spectrum is 780nm and the average power is 232mW. With the femtosecond pulses coupled into two different photonic crystal fibers, the coverage of visible spectrum is up to 500nm-960nm. The spectral shape and width can be optimized by changing the polarization state for satisfying the requirments of different optical frequencies measurement.
Narrow-bandwidth tunable picosecond pulses in the visible produced by noncollinear optical parametric amplification with a chirped blue pump.

PubMed

Co, Dick T; Lockard, Jenny V; McCamant, David W; Wasielewski, Michael R

2010-04-01

Narrow-bandwidth (approximately 27 cm(-1)) tunable picosecond pulses from 480 nm-780 nm were generated from the output of a 1 kHz femtosecond titanium:sapphire laser system using a type I noncollinear optical parametric amplifier (NOPA) with chirped second-harmonic generation (SHG) pumping. Unlike a femtosecond NOPA, this system utilizes a broadband pump beam, the chirped 400 nm SHG of the Ti:sapphire fundamental, to amplify a monochromatic signal beam (spectrally-filtered output of a type II collinear OPA). Optimum geometric conditions for simultaneous phase- and group-velocity matching were calculated in the visible spectrum. This design is an efficient and simple method for generating tunable visible picosecond pulses that are synchronized to the femtosecond pulses.
Photoionization Efficiencies of Five Polycyclic Aromatic Hydrocarbons.

PubMed

Johansson, K Olof; Campbell, Matthew F; Elvati, Paolo; Schrader, Paul E; Zádor, Judit; Richards-Henderson, Nicole K; Wilson, Kevin R; Violi, Angela; Michelsen, Hope A

2017-06-15

We have measured photoionization-efficiency curves for pyrene, fluoranthene, chrysene, perylene, and coronene in the photon energy range of 7.5-10.2 eV and derived their photoionization cross-section curves in this energy range. All measurements were performed using tunable vacuum ultraviolet (VUV) radiation generated at the Advanced Light Source synchrotron at Lawrence Berkeley National Laboratory. The VUV radiation was used for photoionization, and detection was performed using a time-of-flight mass spectrometer. We measured the photoionization efficiency of 2,5-dimethylfuran simultaneously with those of pyrene, fluoranthene, chrysene, perylene, and coronene to obtain references of the photon flux during each measurement from the known photoionization cross-section curve of 2,5-dimethylfuran.
Spectrally-broad coherent anti-Stokes Raman scattering hyper-microscopy utilizing a Stokes supercontinuum pumped at 800 nm

PubMed Central

Porquez, Jeremy G.; Cole, Ryan A.; Tabarangao, Joel T.; Slepkov, Aaron D.

2016-01-01

We demonstrate spectral-focusing based coherent anti-Stokes Raman scattering (SF-CARS) hyper-microscopy capable of probing vibrational frequencies from 630 cm−1 to 3250 cm−1 using a single Ti:Sapphire femtosecond laser operating at 800 nm, and a commercially-available supercontinuum-generating fibre module. A broad Stokes supercontinuum with significant spectral power at wavelengths between 800 nm and 940 nm is generated by power tuning the fibre module using atypically long and/or chirped ~200 fs pump pulses, allowing convenient access to lower vibrational frequencies in the fingerprint spectral region. This work significantly reduces the instrumental and technical requirements for multimodal CARS microscopy, while expanding the spectral capabilities of an established approach to SF-CARS. PMID:27867735
Inverting pump-probe spectroscopy for state tomography of excitonic systems.

PubMed

Hoyer, Stephan; Whaley, K Birgitta

2013-04-28

We propose a two-step protocol for inverting ultrafast spectroscopy experiments on a molecular aggregate to extract the time-evolution of the excited state density matrix. The first step is a deconvolution of the experimental signal to determine a pump-dependent response function. The second step inverts this response function to obtain the quantum state of the system, given a model for how the system evolves following the probe interaction. We demonstrate this inversion analytically and numerically for a dimer model system, and evaluate the feasibility of scaling it to larger molecular aggregates such as photosynthetic protein-pigment complexes. Our scheme provides a direct alternative to the approach of determining all Hamiltonian parameters and then simulating excited state dynamics.
Surface and interface effects on non-radiative exciton recombination and relaxation dynamics in CdSe/Cd,Zn,S nanocrystals

NASA Astrophysics Data System (ADS)

Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M.; Nick, Robert; Coe-Sullivan, Seth; Kambhampati, Patanjali

2016-06-01

Excitonic state-resolved pump/probe spectroscopy and time correlate single photon counting were used to study exciton dynamics from the femtosecond to nanosecond time scales in CdSe/Cd,Zn,S nanocrystals. These measurements reveal the role of the core/shell interface as well as surface on non-radiative excitonic processes over three time regimes. Time resolved photoluminescence reports on how the interface controls slow non-radiative processes that dictate emission at the single excitonic level. Heterogeneity in decay is minimized by interfacial structure. Pump/probe measurements explore the non-radiative multiexcitonic recombination processes on the picosecond timescale. These Auger based non-radiative processes dictate lifetimes of multiexcitonic states. Finally state-resolved pump/probe measurements on the femtosecond timescale reveal the influence of the interface on electron and hole relaxation dynamics. We find that the interface has a profound influence on all three types of non-radiative processes which ultimately control light emission from nanocrystals.
Ultrafast Charge Transfer in Nickel Phthalocyanine Probed by Femtosecond Raman-Induced Kerr Effect Spectroscopy

PubMed Central

2015-01-01

The recently developed technique of femtosecond stimulated Raman spectroscopy, and its variant, femtosecond Raman-induced Kerr effect spectroscopy (FRIKES), offer access to ultrafast excited-state dynamics via structurally specific vibrational spectra. We have used FRIKES to study the photoexcitation dynamics of nickel(II) phthalocyanine with eight butoxy substituents, NiPc(OBu)8. NiPc(OBu)8 is reported to have a relatively long-lived ligand-to-metal charge-transfer (LMCT) state, an essential characteristic for efficient electron transfer in photocatalysis. Following photoexcitation, vibrational transitions in the FRIKES spectra, assignable to phthalocyanine ring modes, evolve on the femtosecond to picosecond time scales. Correlation of ring core size with the frequency of the ν10 (asymmetric C–N stretching) mode confirms the identity of the LMCT state, which has a ∼500 ps lifetime, as well as that of a precursor d-d excited state. An even earlier (∼0.2 ps) transient is observed and tentatively assigned to a higher-lying Jahn–Teller-active LMCT state. This study illustrates the power of FRIKES spectroscopy in elucidating ultrafast molecular dynamics. PMID:24841906
Investigation of the dynamics of a nonlinear optical response in glassy chalcogenide semiconductors by the pump–probe method

NASA Astrophysics Data System (ADS)

Romanova, E. A.; Kuzyutkina, Yu S.; Shiryaev, V. S.; Guizard, S.

2018-03-01

An analysis of the results of measurements by using the pump–probe method with a femtosecond resolution in time and computer simulation of the charge carrier kinetics have revealed two types of a nonlinear optical response in samples of chalcogenide glasses belonging to the As – S – Se system, irradiated by 50-fs laser pulses with a wavelength of 0.79 μm. The difference in the nonlinear dynamics is due to the difference in the photoexcitation character, because laser radiation can be absorbed either through bound states in the band gap or without their participation, depending on the ratio of the pump photon energy to the bandgap energy.
Calculation of femtosecond pulse laser induced damage threshold for broadband antireflective microstructure arrays.

PubMed

Jing, Xufeng; Shao, Jianda; Zhang, Junchao; Jin, Yunxia; He, Hongbo; Fan, Zhengxiu

2009-12-21

In order to more exactly predict femtosecond pulse laser induced damage threshold, an accurate theoretical model taking into account photoionization, avalanche ionization and decay of electrons is proposed by comparing respectively several combined ionization models with the published experimental measurements. In addition, the transmittance property and the near-field distribution of the 'moth eye' broadband antireflective microstructure directly patterned into the substrate material as a function of the surface structure period and groove depth are performed by a rigorous Fourier model method. It is found that the near-field distribution is strongly dependent on the periodicity of surface structure for TE polarization, but for TM wave it is insensitive to the period. What's more, the femtosecond pulse laser damage threshold of the surface microstructure on the pulse duration taking into account the local maximum electric field enhancement was calculated using the proposed relatively accurate theoretical ionization model. For the longer incident wavelength of 1064 nm, the weak linear damage threshold on the pulse duration is shown, but there is a surprising oscillation peak of breakdown threshold as a function of the pulse duration for the shorter incident wavelength of 532 nm.
A wavelength dependent investigation of the indole photophysics via ionization and fragmentation pump-probe spectroscopies.

PubMed

Godfrey, T J; Yu, Hui; Biddle, Michael S; Ullrich, Susanne

2015-10-14

A wavelength dependent study investigating the low-lying (1)La and (1)Lb states, both possessing (1)ππ* character, and the (1)πσ* state in the deactivation process of indole is presented here. Relaxation dynamics following excitation at 241, 250, 260, 270, 273, and 282 nm are examined using three gas-phase, pump-probe spectroscopic techniques: (1) hydrogen atom (H-atom) time-resolved kinetic energy release (TR-KER), (2) time-resolved photoelectron spectroscopy (TR-PES), and (3) time-resolved ion yield (TR-IY). Applied in combination, a more complete picture of the indole relaxation dynamics may be gleaned. For instance, TR-PES experiments directly observe all relaxation pathways by probing the evolution of the excited states following photoexcitation; whereas, TR-KER measurements indirectly, yet specifically, probe for (1)πσ*-state activity through the detection of H-atoms eliminated along the indole nitrogen-hydrogen (N-H) stretch coordinate-a possible outcome of (1)πσ*-state relaxation in indole. In addition, mass information obtained via TR-IY monitors fragmentation dynamics that may occur within the neutral electronically excited and/or cationic states. The work herein assesses the onset and importance of the (1)πσ* state at various pump wavelengths by systematically tuning across the ultraviolet absorption spectrum of indole with a particular focus on those pump wavelengths longer than 263 nm, where the involvement of the (1)πσ* state is under current debate. As far as this experimental work is concerned, there does not appear to be any significant involvement by the (1)πσ* state in the indole relaxation processes following excitation at 270, 273, or 282 nm. This investigation also evaluates the primary orbital promotions contributing to the (1)La, (1)Lb, and (1)πσ* transitions based on ionization preferences observed in TR-PES spectra. Relaxation time constants associated with dynamics along these states are also reported for excitation at all
Tuning the frequency of ultrashort laser pulses by a cross-phase-modulation-induced shift in a photonic crystal fiber.

PubMed

Konorov, S O; Akimov, D A; Zheltikov, A M; Ivanov, A A; Alfimov, M V; Scalora, M

2005-06-15

Femtosecond pulses of fundamental Cr:forsterite laser radiation are used as a pump field to tune the frequency of copropagating second-harmonic pulses of the same laser through cross-phase modulation in a photonic crystal fiber. Sub-100-kW femtosecond pump pulses coupled into a photonic crystal fiber with an appropriate dispersion profile can shift the central frequency of the probe field by more than 100 nm, suggesting a convenient way to control propagation and spectral transformations of ultrashort laser pulses.
Photoionization Efficiencies of Five Polycyclic Aromatic Hydrocarbons

DOE PAGES

Johansson, K. Olof; Campbell, Matthew F.; Elvati, Paolo; ...

2017-05-18

We have measured photoionization-efficiency curves for pyrene, fluoranthene, chrysene, perylene, and coronene in the photon energy range of 7.5-10.2 eV and derived their photoionization cross-section curves in this energy range. All measurements were performed using tunable vacuum ultraviolet (VUV) radiation generated at the Advanced Light Source synchrotron at Lawrence Berkeley National Laboratory. The VUV radiation was used for photoionization, and detection was performed using a time-of-flight mass spectrometer. We measured the photoionization efficiency of 2,5-dimethylfuran simultaneously with those of pyrene, fluoranthene, chrysene, perylene, and coronene to obtain references of the photon flux during each measurement from the known photoionization cross-sectionmore » curve of 2,5- dimethylfuran.« less
Two-color pump-probe laser spectroscopy instrument with picosecond time-resolved electronic delay and extended scan range

NASA Astrophysics Data System (ADS)

Yu, Anchi; Ye, Xiong; Ionascu, Dan; Cao, Wenxiang; Champion, Paul M.

2005-11-01

An electronically delayed two-color pump-probe instrument was developed using two synchronized laser systems. The instrument has picosecond time resolution and can perform scans over hundreds of nanoseconds without the beam divergence and walk-off effects that occur using standard spatial delay systems. A unique picosecond Ti :sapphire regenerative amplifier was also constructed without the need for pulse stretching and compressing optics. The picosecond regenerative amplifier has a broad wavelength tuning range, which suggests that it will make a significant contribution to two-color pump-probe experiments. To test this instrument we studied the rotational correlation relaxation of myoglobin (τr=8.2±0.5ns) in water as well as the geminate rebinding kinetics of oxygen to myoglobin (kg1=1.7×1011s-1, kg2=3.4×107s-1). The results are consistent with, and improve upon, previous studies.
Photoionization and pseudopotentials

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

Costa, Romarly F. da; Lima, Marco A.P.; Ferreira, Luiz G.

2003-05-01

Transferability of norm-conserving pseudopotentials to low-energy electron-molecule scattering processes has been very successful [Bettega et al., Phys. Rev. A 47, 1111 (1993)]. In this paper we discuss the possibility of using effective potentials in calculations of valence electrons photoionization cross sections. Through atomic targets, we illustrate that pseudopotentials can be optimized to give cross sections in good agreement with all-electron calculations. The present work represents a first step towards more elaborate computer programs for photoionization of molecular targets containing heavy atoms.

Plasma dynamics and structural modifications induced by femtosecond laser pulses in quartz

NASA Astrophysics Data System (ADS)

Hernandez-Rueda, J.; Puerto, D.; Siegel, J.; Galvan-Sosa, M.; Solis, J.

2012-09-01

We have investigated plasma formation and relaxation dynamics induced by single femtosecond laser pulses at the surface of crystalline SiO2 (quartz) along with the corresponding topography modifications. The use of fs-resolved pump-probe microscopy allows combining spatial and temporal resolution and simultaneous access to phenomena occurring in adjacent regions excited with different local fluences. The results show the formation of a transient free-electron plasma ring surrounding the location of the inner ablation crater. Optical microscopy measurements reveal a 30% reflectivity decrease in this region, consistent with local amorphization. The accompanying weak depression of ≈15 nm in this region is explained by gentle material removal via Coulomb explosion. Finally, we discuss the timescales of the plasma dynamics and its role in the modifications produced, by comparing the results with previous studies obtained in amorphous SiO2 (fused silica). For this purpose, we have conceived a new representation concept of time-resolved microscopy image stacks in a single graph, which allows visualizing quickly suble differences of the overall similar dynamic response of both materials.
Single-shot transient absorption spectroscopy with a 45 ps pump-probe time delay range.

PubMed

Wilson, Kelly S; Wong, Cathy Y

2018-02-01

We report a single-shot transient absorption apparatus that successfully uses a tilted pump pulse to spatially encode a 45 ps pump-probe time delay. The time delay range is significantly improved over other reported instruments by using a spatial light modulator to flatten the intensity of the excitation field at the sample position. The full time delay range of the instrument is demonstrated by measuring a long-lived dye. A signal-to-noise ratio of >35 is attained in 8 s. This advance will enable the measurement of excited state dynamics of systems that are not at structural equilibrium.
Photoionization of the Buckminsterfullerene Cation.

PubMed

Douix, Suzie; Duflot, Denis; Cubaynes, Denis; Bizau, Jean-Marc; Giuliani, Alexandre

2017-01-05

Photoionization of a buckminsterfullerene ion is investigated using an ion trap and a merged beam setup coupled to synchrotron radiation beamlines and compared to theoretical calculations. Absolute measurements derived from the ion trap experiment allow discrepancies concerning the photoionization cross section of C 60 + to be solved.
Photoionization of calcium

NASA Astrophysics Data System (ADS)

Deshmukh, Pranawa C.; Johnson, W. R.

1983-01-01

A study of the photoionization of calcium in the relativistic random-phase approximation is reported. Predictions of photoionization cross sections, angular distribution asymmetry parameters, and spin-polarization parameters for the 4s, 3p, and 3s subshells are made with emphasis on the energy region above the 3p32 threshold where multiconfigurational effects are not expected to be very important. Autoionization resonances below the 3s threshold and between the 3p32 and 3p12 thresholds are analyzed using the relativistic multichannel quantum-defect theory.
Probing Photoexcited Carriers in a Few-Layer MoS2 Laminate by Time-Resolved Optical Pump-Terahertz Probe Spectroscopy.

PubMed

Kar, Srabani; Su, Y; Nair, R R; Sood, A K

2015-12-22

We report the dynamics of photoinduced carriers in a free-standing MoS2 laminate consisting of a few layers (1-6 layers) using time-resolved optical pump-terahertz probe spectroscopy. Upon photoexcitation with the 800 nm pump pulse, the terahertz conductivity increases due to absorption by the photoinduced charge carriers. The relaxation of the non-equilibrium carriers shows fast as well as slow decay channels, analyzed using a rate equation model incorporating defect-assisted Auger scattering of photoexcited electrons, holes, and excitons. The fast relaxation time occurs due to the capture of electrons and holes by defects via Auger processes, resulting in nonradiative recombination. The slower relaxation arises since the excitons are bound to the defects, preventing the defect-assisted Auger recombination of the electrons and the holes. Our results provide a comprehensive understanding of the non-equilibrium carrier kinetics in a system of unscreened Coulomb interactions, where defect-assisted Auger processes dominate and should be applicable to other 2D systems.
On the absolute photoionization cross section and dissociative photoionization of cyclopropenylidene.

PubMed

Holzmeier, Fabian; Fischer, Ingo; Kiendl, Benjamin; Krueger, Anke; Bodi, Andras; Hemberger, Patrick

2016-04-07

We report the determination of the absolute photoionization cross section of cyclopropenylidene, c-C3H2, and the heat of formation of the C3H radical and ion derived by the dissociative ionization of the carbene. Vacuum ultraviolet (VUV) synchrotron radiation as provided by the Swiss Light Source and imaging photoelectron photoion coincidence (iPEPICO) were employed. Cyclopropenylidene was generated by pyrolysis of a quadricyclane precursor in a 1 : 1 ratio with benzene, which enabled us to derive the carbene's near threshold absolute photoionization cross section from the photoionization yield of the two pyrolysis products and the known cross section of benzene. The cross section at 9.5 eV, for example, was determined to be 4.5 ± 1.4 Mb. Upon dissociative ionization the carbene decomposes by hydrogen atom loss to the linear isomer of C3H(+). The appearance energy for this process was determined to be AE(0K)(c-C3H2; l-C3H(+)) = 13.67 ± 0.10 eV. The heat of formation of neutral and cationic C3H was derived from this value via a thermochemical cycle as Δ(f)H(0K)(C3H) = 725 ± 25 kJ mol(-1) and Δ(f)H(0K)(C3H(+)) = 1604 ± 19 kJ mol(-1), using a previously reported ionization energy of C3H.
Determining the partial photoionization cross-sections of ethyl radicals.

PubMed

FitzPatrick, B L; Maienschein-Cline, M; Butler, L J; Lee, S-H; Lin, J J

2007-12-13

Using a crossed laser-molecular beam scattering apparatus, these experiments photodissociate ethyl chloride at 193 nm and detect the Cl and ethyl products, resolved by their center-of-mass recoil velocities, with vacuum ultraviolet photoionization. The data determine the relative partial cross-sections for the photoionization of ethyl radicals to form C2H5+, C2H4+, and C2H3+ at 12.1 and 13.8 eV. The data also determine the internal energy distribution of the ethyl radical prior to photoionization, so we can assess the internal energy dependence of the photoionization cross-sections. The results show that the C2H4++H and C2H3++H2 dissociative photoionization cross-sections strongly depend on the photoionization energy. Calibrating the ethyl radical partial photoionization cross-sections relative to the bandwidth-averaged photoionization cross-section of Cl atoms near 13.8 eV allows us to use these data in conjunction with literature estimates of the Cl atom photoionization cross-sections to put the present bandwidth-averaged cross-sections on an absolute scale. The resulting bandwidth-averaged cross-section for the photoionization of ethyl radicals to C2H5+ near 13.8 eV is 8+/-2 Mb. Comparison of our 12.1 eV data with high-resolution ethyl radical photoionization spectra allows us to roughly put the high-resolution spectrum on the same absolute scale. Thus, one obtains the photoionization cross-section of ethyl radicals to C2H5+ from threshold to 12.1 eV. The data show that the onset of the C2H4++H dissociative photoionization channel is above 12.1 eV; this result offers a simple way to determine whether the signal observed in photoionization experiments on complex mixtures is due to ethyl radicals. We discuss an application of the results for resolving the product branching in the O+allyl bimolecular reaction.
Vibrational dynamics of acetate in D2O studied by infrared pump-probe spectroscopy.

PubMed

Banno, Motohiro; Ohta, Kaoru; Tominaga, Keisuke

2012-05-14

Solute-solvent interactions between acetate and D(2)O were investigated by vibrational spectroscopic methods. The vibrational dynamics of the COO asymmetric stretching mode in D(2)O was observed by time-resolved infrared (IR) pump-probe spectroscopy. The pump-probe signal contained both decay and oscillatory components. The time dependence of the decay component could be explained by a double exponential function with time constants of 200 fs and 2.6 ps, which are the same for both the COO asymmetric and symmetric stretching modes. The Fourier spectrum of the oscillatory component contained a band around 80 cm(-1), which suggests that the COO asymmetric stretching mode couples to a low-frequency vibrational mode with a wavenumber of 80 cm(-1). Based on quantum chemistry calculations, we propose that a bridged complex comprising an acetate ion and one D(2)O molecule, in which the two oxygen atoms in the acetate anion form hydrogen bonds with the two deuterium atoms in D(2)O, is the most stable structure. The 80 cm(-1) low-frequency mode was assigned to the asymmetric stretching vibration of the hydrogen bond in the bridged complex. This journal is © the Owner Societies 2012
Photoelectron photoion molecular beam spectroscopy

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

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.
Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory.

PubMed

De Giovannini, Umberto; Brunetto, Gustavo; Castro, Alberto; Walkenhorst, Jessica; Rubio, Angel

2013-05-10

Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experiment, provide additional information about electronic structure and dynamics that improve characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Evaluation of the UFXC32k photon-counting detector for pump-probe experiments using synchrotron radiation.

PubMed

Koziol, Anna; Bordessoule, Michel; Ciavardini, Alessandra; Dawiec, Arkadiusz; Da Silva, Paulo; Desjardins, Kewin; Grybos, Pawel; Kanoute, Brahim; Laulhe, Claire; Maj, Piotr; Menneglier, Claude; Mercere, Pascal; Orsini, Fabienne; Szczygiel, Robert

2018-03-01

This paper presents the performance of a single-photon-counting hybrid pixel X-ray detector with synchrotron radiation. The camera was evaluated with respect to time-resolved experiments, namely pump-probe-probe experiments held at SOLEIL. The UFXC camera shows very good energy resolution of around 1.5 keV and allows the minimum threshold setting to be as low as 3 keV keeping the high-count-rate capabilities. Measurements of a synchrotron characteristic filling mode prove the proper separation of an isolated bunch of photons and the usability of the detector in time-resolved experiments.
Absolute photoionization cross-section of the methyl radical.

PubMed

Taatjes, Craig A; Osborn, David L; Selby, Talitha M; Meloni, Giovanni; Fan, Haiyan; Pratt, Stephen T

2008-10-02

The absolute photoionization cross-section of the methyl radical has been measured using two completely independent methods. The CH3 photoionization cross-section was determined relative to that of acetone and methyl vinyl ketone at photon energies of 10.2 and 11.0 eV by using a pulsed laser-photolysis/time-resolved synchrotron photoionization mass spectrometry method. The time-resolved depletion of the acetone or methyl vinyl ketone precursor and the production of methyl radicals following 193 nm photolysis are monitored simultaneously by using time-resolved synchrotron photoionization mass spectrometry. Comparison of the initial methyl signal with the decrease in precursor signal, in combination with previously measured absolute photoionization cross-sections of the precursors, yields the absolute photoionization cross-section of the methyl radical; sigma(CH3)(10.2 eV) = (5.7 +/- 0.9) x 10(-18) cm(2) and sigma(CH3)(11.0 eV) = (6.0 +/- 2.0) x 10(-18) cm(2). The photoionization cross-section for vinyl radical determined by photolysis of methyl vinyl ketone is in good agreement with previous measurements. The methyl radical photoionization cross-section was also independently measured relative to that of the iodine atom by comparison of ionization signals from CH3 and I fragments following 266 nm photolysis of methyl iodide in a molecular-beam ion-imaging apparatus. These measurements gave a cross-section of (5.4 +/- 2.0) x 10(-18) cm(2) at 10.460 eV, (5.5 +/- 2.0) x 10(-18) cm(2) at 10.466 eV, and (4.9 +/- 2.0) x 10(-18) cm(2) at 10.471 eV. The measurements allow relative photoionization efficiency spectra of methyl radical to be placed on an absolute scale and will facilitate quantitative measurements of methyl concentrations by photoionization mass spectrometry.
Ultrafast exciton dynamics in cadmium selenide nanocrystals determined by femtosecond fluorescence upconversion spectroscopy

NASA Astrophysics Data System (ADS)

Underwood, David Frederick

Femtosecond fluorescence upconversion spectroscopy is a technique that allows the unambiguous determination of the excited state dynamics of an analyte. Combining this method with the use of tunable laser excitation, the exciton dynamics in semiconducting nanocrystals (NC's) of cadmium selenide (CdSe) have been determined, devoid of the complications arising from more common spectroscopic methods such as pump-probe. The results of this investigation were used to construct a model to fully describe the three-level system comprising of the valence and conduction bands and surface states, which have been calculated by others to lie mid-gap in energy. Smaller NC's showed faster decay components due to increased interaction between the exciton and surface states. The deep trap emission, which has never before been measured by ultrafast fluorescence techniques, shows a rapid rise time (˜2 ps), which is attributed to surface selenium dangling bonds relaxing to the valence band and radiatively combining with the photo-generated hole. The band edge fluorescence decays as the deep trap emission grows in, inherently coupling the two processes. An experiment which measured the dependence of the excitation energy showed that increased energy imparted to the NC's resulted in increased rise times, yielding the timescales for exciton relaxation through the valence and conduction band states to the lowest emitting state. Surface-oxidized and normally-passivated NC's display the same decay dynamics in time but differ in relative amplitude; the latter point agrees with steady-state measurements. The rotational anisotrophy of the NC's was measured and agrees with previous pump-probe data. Upconversion on the red and blue sides of the static fluorescence spectrum showed no discernable differences, which is either and inherent limitation of the experimental apparatus, or the possibility that lower-lying triplet states are populated on a timescale below the instrument resolution.
Two-color vibrational, femtosecond, fully resonant electronically enhanced CARS (FREE-CARS) of gas-phase nitric oxide.

PubMed

Stauffer, Hans U; Roy, Sukesh; Schmidt, Jacob B; Wrzesinski, Paul J; Gord, James R

2016-09-28

A resonantly enhanced, two-color, femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) approach is demonstrated and used to explore the nature of the frequency- and time-dependent signals produced by gas-phase nitric oxide (NO). Through careful selection of the input pulse wavelengths, this fully resonant electronically enhanced CARS (FREE-CARS) scheme allows rovibronic-state-resolved observation of time-dependent rovibrational wavepackets propagating on the vibrationally excited ground-state potential energy surface of this diatomic species. Despite the use of broadband, ultrafast time-resolved input pulses, high spectral resolution of gas-phase rovibronic transitions is observed in the FREE-CARS signal, dictated by the electronic dephasing timescales of these states. Analysis and computational simulation of the time-dependent spectra observed as a function of pump-Stokes and Stokes-probe delays provide insight into the rotationally resolved wavepacket motion observed on the excited-state and vibrationally excited ground-state potential energy surfaces of NO, respectively.
Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry.

PubMed

Marceau, Claude; Makhija, Varun; Platzer, Dominique; Naumov, A Yu; Corkum, P B; Stolow, Albert; Villeneuve, D M; Hockett, Paul

2017-08-25

Photoionization of molecular species is, essentially, a multipath interferometer with both experimentally controllable and intrinsic molecular characteristics. In this work, XUV photoionization of impulsively aligned molecular targets (N_{2}) is used to provide a time-domain route to "complete" photoionization experiments, in which the rotational wave packet controls the geometric part of the photoionization interferometer. The data obtained is sufficient to determine the magnitudes and phases of the ionization matrix elements for all observed channels, and to reconstruct molecular frame interferograms from lab frame measurements. In principle, this methodology provides a time-domain route to complete photoionization experiments and the molecular frame, which is generally applicable to any molecule (no prerequisites), for all energies and ionization channels.
Ultrafast time-resolved pump-probe spectroscopy of PYP by a sub-8 fs pulse laser at 400 nm.

PubMed

Liu, Jun; Yabushita, Atsushi; Taniguchi, Seiji; Chosrowjan, Haik; Imamoto, Yasushi; Sueda, Keiichi; Miyanaga, Noriaki; Kobayashi, Takayoshi

2013-05-02

Impulsive excitation of molecular vibration is known to induce wave packets in both the ground state and excited state. Here, the ultrafast dynamics of PYP was studied by pump-probe spectroscopy using a sub-8 fs pulse laser at 400 nm. The broadband spectrum of the UV pulse allowed us to detect the pump-probe signal covering 360-440 nm. The dependence of the vibrational phase of the vibrational mode around 1155 cm(-1) on the probe photon energy was observed for the first time to our knowledge. The vibrational mode coupled to the electronic transition observed in the probe spectral ranges of 2.95-3.05 and 3.15-3.35 eV was attributed to the wave packets in the ground state and the excited state, respectively. The frequencies in the ground state and excited state were determined to be 1155 ± 1 and 1149 ± 1 cm(-1), respectively. The frequency difference is due to change after photoexcitation. This means a reduction of the bond strength associated with π-π* excitation, which is related to the molecular structure change associated with the primary isomerization process in the photocycle in PYP. Real-time vibrational modes at low frequency around 138, 179, 203, 260, and 317 cm(-1) were also observed and compared with the Raman spectrum for the assignment of the vibrational wave packet.
Tracking of the nuclear wavepacket motion in cyanine photoisomerization by ultrafast pump-dump-probe spectroscopy.

PubMed

Wei, Zhengrong; Nakamura, Takumi; Takeuchi, Satoshi; Tahara, Tahei

2011-06-01

Understanding ultrafast reactions, which proceed on a time scale of nuclear motions, requires a quantitative characterization of the structural dynamics. To track such structural changes with time, we studied a nuclear wavepacket motion in photoisomerization of a prototype cyanine dye, 1,1'-diethyl-4,4'-cyanine, by ultrafast pump-dump-probe measurements in solution. The temporal evolution of wavepacket motion was examined by monitoring the efficiency of stimulated emission dumping, which was obtained from the recovery of a ground-state bleaching signal. The dump efficiency versus pump-dump delay exhibited a finite rise time, and it became longer (97 fs → 330 fs → 390 fs) as the dump pulse was tuned to longer wavelengths (690 nm → 950 nm → 1200 nm). This result demonstrates a continuous migration of the leading edge of the wavepacket on the excited-state potential from the Franck-Condon region toward the potential minimum. A slowly decaying feature of the dump efficiency indicated a considerable broadening of the wavepacket over a wide range of the potential, which results in the spread of a population distribution on the flat S(1) potential energy surface. The rapid migration as well as broadening of the wavepacket manifests a continuous nature of the structural dynamics and provides an intuitive visualization of this ultrafast reaction. We also discussed experimental strategies to evaluate reliable dump efficiencies separately from other ultrafast processes and showed a high capability and possibility of the pump-dump-probe method for spectroscopic investigation of unexplored potential regions such as conical intersections. © 2011 American Chemical Society
Photoionization studies with molecular beams

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

Ng, C.Y.

1976-09-01

A molecular beam photoionization apparatus which combines the advantages of both the molecular beam method with photoionization mass spectrometry has been designed and constructed for carrying out some unique photoionization experiments. Rotational cooling during the supersonic expansion has resulted in high resolution photoionization efficiency curves for NO, ICl, C/sub 2/H/sub 2/ and CH/sub 3/I. The analysis of these spectra has yielded ionization potentials for these molecules to an accuracy of +- 3 MeV. Detailed autoionization structures were also resolved. This allows the investigation of the selection rules for autoionization, and the identification of the Rydberg series which converge to themore » excited states of the molecular ions. The degree of relaxation for thermally populated excited states has been examined using NO and ICl as examples. As a result of adiabatic cooling, a small percentage of dimers is also formed during the expansion. The photoionization efficiency curves for (NO)/sub 2/, ArICl, Ar/sub 2/, Kr/sub 2/ and Xe/sub 2/ have been obtained near the thresholds. Using the known dissociation energies of the (NO)/sub 2/, Ar/sub 2/, Kr/sub 2/ and Xe/sub 2/ van der Waals molecules, the corresponding dissociation energies for NO-NO/sup +/, Ar/sub 2//sup +/, Kr/sub 2//sup +/, and Xe/sub 2//sup +/ have been determined. The ionization mechanisms for this class of molecules are examined and discussed.« less
Terahertz imaging with sub-wavelength resolution by femtosecond laser filament in air

PubMed Central

Zhao, Jiayu; Chu, Wei; Guo, Lanjun; Wang, Zhi; Yang, Jing; Liu, Weiwei; Cheng, Ya; Xu, Zhizhan

2014-01-01

Terahertz (THz) imaging provides cutting edge technique in biology, medical sciences and non-destructive evaluation. However, due to the long wavelength of the THz wave, the obtained resolution of THz imaging is normally a few hundred microns and is much lower than that of the traditional optical imaging. We introduce a sub-wavelength resolution THz imaging technique which uses the THz radiation generated by a femtosecond laser filament in air as the probe. This method is based on the fact that the femtosecond laser filament forms a waveguide for the THz wave in air. The diameter of the THz beam, which propagates inside the filament, varies from 20 μm to 50 μm, which is significantly smaller than the wavelength of the THz wave. Using this highly spatially confined THz beam as the probe, THz imaging with resolution as high as 20 μm (~λ/38 at 0.4 THz) can be realized. PMID:24457525
A transmission-grating-modulated pump-probe absorption spectroscopy and demonstration of diffusion dynamics of photoexcited carriers in bulk intrinsic GaAs film.

PubMed

Chen, Ke; Wang, Wenfang; Chen, Jianming; Wen, Jinhui; Lai, Tianshu

2012-02-13

A transmission-grating-modulated time-resolved pump-probe absorption spectroscopy is developed and formularized. The spectroscopy combines normal time-resolved pump-probe absorption spectroscopy with a binary transmission grating, is sensitive to the spatiotemporal evolution of photoinjected carriers, and has extensive applicability in the study of diffusion transport dynamics of photoinjected carriers. This spectroscopy has many advantages over reported optical methods to measure diffusion dynamics, such as simple experimental setup and operation, and high detection sensitivity. The measurement of diffusion dynamics is demonstrated on bulk intrinsic GaAs films. A carrier density dependence of carrier diffusion coefficient is obtained and agrees well with reported results.

Femtosecond diode-pumped mode-locked neodymium lasers

NASA Astrophysics Data System (ADS)

Kubeček, Václav; Jelínek, Michal; Čech, Miroslav; Vyhlídal, David; Su, Liangbi; Jiang, Dapeng; Ma, Fengkai; Qian, Xiaobo; Wang, Jingya; Xu, Jun

2016-12-01

Fluoride-type crystals (CaF2, SrF2) doped with neodymium Nd3+ and codoped with buffer ions for breaking clusters of active ions and increasing fluorescence efficiency, present interesting alternative as laser active media for the diode-pumped mode-locked lasers. In comparison with widely used materials as Nd:YAG or Nd:YVO4, they have broad emission spectra as well as longer fluorescence lifetime, in comparison with Nd:glass, SrF2 and CaF2 have better thermal conductivity. In spite of the fact, that this thermal conductivity decreases with Nd3+ doping concentration, these crystals are alternative for the Nd:glass in subpicosecond mode-locked laser systems. In this paper we review the basic results reported recently on these active materials and in the second part we present our results achieved in low power diode pumped passively mode locked lasers with Nd,La:CaF2 and Nd,Y:SrF2 crystals. The pulses as short as 258 fs at wavelength of 1057 nm were obtained in the first case, while 5 ps long pulses at 1065 nm were generated from the second laser system.
Impact of pumping configuration on all-fibered femtosecond chirped pulse amplification

NASA Astrophysics Data System (ADS)

Lecourt, Jean-Bernard; Duterte, Charles; Bertrand, Anthony; Liégeois, Flavien; Hernandez, Yves; Giannone, Domenico

2008-04-01

We experimentally compared the co- and counter-propagative pumping scheme for the amplification of ultra-short optical pulses. According to pumping direction we show that optical pulses with a duration of 75 fs and 100mW of average output power can be obtained for co-propagative pumping, while pulse duration is never shorter than 400 fs for the counter-propagative case. We show that the impact of non-linear effects on pulse propagation is different for the two pumping configurations. We assume that Self Phase Modulation (SPM) is the main effect in the copropagative case, whereas the impact of Stimulated Raman Scattering is bigger for the counter-propagative case.
Communication: nanosecond folding dynamics of an alpha helix: time-dependent 2D-IR cross peaks observed using polarization-sensitive dispersed pump-probe spectroscopy.

PubMed

Panman, Matthijs R; van Dijk, Chris N; Meuzelaar, Heleen; Woutersen, S

2015-01-28

We present a simple method to measure the dynamics of cross peaks in time-resolved two-dimensional vibrational spectroscopy. By combining suitably weighted dispersed pump-probe spectra, we eliminate the diagonal contribution to the 2D-IR response, so that the dispersed pump-probe signal contains the projection of only the cross peaks onto one of the axes of the 2D-IR spectrum. We apply the method to investigate the folding dynamics of an alpha-helical peptide in a temperature-jump experiment and find characteristic folding and unfolding time constants of 260 ± 30 and 580 ± 70 ns at 298 K.
Femtosecond mega-electron-volt electron microdiffraction

DOE PAGES

Shen, X.; Li, R. K.; Lundstrom, U.; ...

2017-09-01

To understand and control the basic functions of physical, chemical and biological processes from micron to nano-meter scale, an instrument capable of visualizing transient structural changes of inhomogeneous materials with atomic spatial and temporal resolutions, is required. One such technique is femtosecond electron microdiffraction, in which a short electron pulse with femtosecond-scale duration is focused into a micron-scale spot and used to obtain diffraction images to resolve ultrafast structural dynamics over a localized crystalline domain. In this letter, we report the experimental demonstration of time-resolved mega-electron-volt electron microdiffraction which achieves a 5 μm root-mean-square (rms) beam size on the samplemore » and a 110 fs rms temporal resolution. Using pulses of 10k electrons at 4.2 MeV energy with a normalized emittance 3 nm-rad, we obtained high quality diffraction from a single 10 μm paraffin ( C 44 H 90) crystal. The phonon softening mode in optical-pumped polycrystalline Bi was also time-resolved, demonstrating the temporal resolution limits of the instrument. In conclusion, this new characterization capability will open many research opportunities in material and biological sciences.« less
Femtosecond mega-electron-volt electron microdiffraction

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

Shen, X.; Li, R. K.; Lundstrom, U.

To understand and control the basic functions of physical, chemical and biological processes from micron to nano-meter scale, an instrument capable of visualizing transient structural changes of inhomogeneous materials with atomic spatial and temporal resolutions, is required. One such technique is femtosecond electron microdiffraction, in which a short electron pulse with femtosecond-scale duration is focused into a micron-scale spot and used to obtain diffraction images to resolve ultrafast structural dynamics over a localized crystalline domain. In this letter, we report the experimental demonstration of time-resolved mega-electron-volt electron microdiffraction which achieves a 5 μm root-mean-square (rms) beam size on the samplemore » and a 110 fs rms temporal resolution. Using pulses of 10k electrons at 4.2 MeV energy with a normalized emittance 3 nm-rad, we obtained high quality diffraction from a single 10 μm paraffin ( C 44 H 90) crystal. The phonon softening mode in optical-pumped polycrystalline Bi was also time-resolved, demonstrating the temporal resolution limits of the instrument. In conclusion, this new characterization capability will open many research opportunities in material and biological sciences.« less
Two-Color Pump-Probe Measurement of Photonic Quantum Correlations Mediated by a Single Phonon

NASA Astrophysics Data System (ADS)

Anderson, Mitchell D.; Tarrago Velez, Santiago; Seibold, Kilian; Flayac, Hugo; Savona, Vincenzo; Sangouard, Nicolas; Galland, Christophe

2018-06-01

We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally resolved, time-correlated photon counting. Following pulsed laser excitation, the n =1 phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with subpicosecond time resolution. We observe strongly nonclassical Stokes-anti-Stokes correlations, whose decay maps the single phonon dynamics. Our scheme can be applied to any Raman-active vibrational mode. It can be modified to measure the lifetime of n ≥1 Fock states or the phonon quantum coherences through the preparation and detection of two-mode entangled vibrational states.
Two-Color Pump-Probe Measurement of Photonic Quantum Correlations Mediated by a Single Phonon.

PubMed

Anderson, Mitchell D; Tarrago Velez, Santiago; Seibold, Kilian; Flayac, Hugo; Savona, Vincenzo; Sangouard, Nicolas; Galland, Christophe

2018-06-08

We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally resolved, time-correlated photon counting. Following pulsed laser excitation, the n=1 phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with subpicosecond time resolution. We observe strongly nonclassical Stokes-anti-Stokes correlations, whose decay maps the single phonon dynamics. Our scheme can be applied to any Raman-active vibrational mode. It can be modified to measure the lifetime of n≥1 Fock states or the phonon quantum coherences through the preparation and detection of two-mode entangled vibrational states.
Dissociative Photoionization of Diethyl Ether.

PubMed

Voronova, Krisztina; Mozaffari Easter, Chrissa M; Covert, Kyle J; Bodi, Andras; Hemberger, Patrick; Sztáray, Bálint

2015-10-29

The dissociative photoionization of internal energy selected diethyl ether ions was investigated by imaging photoelectron photoion coincidence spectroscopy. In a large, 5 eV energy range Et2O(+) cations decay by two parallel and three sequential dissociative photoionization channels, which can be modeled well using statistical theory. The 0 K appearance energies of the CH3CHOCH2CH3(+) (H-loss, m/z = 73) and CH3CH2O═CH2(+) (methyl-loss, m/z = 59) fragment ions were determined to be 10.419 ± 0.015 and 10.484 ± 0.008 eV, respectively. The reemergence of the hydrogen-loss ion above 11 eV is attributed to transition-state (TS) switching, in which the second, outer TS is rate-determining at high internal energies. At 11.81 ± 0.05 eV, a secondary fragment of the CH3CHOCH2CH3(+) (m/z = 73) ion, protonated acetaldehyde, CH3CH═OH(+) (m/z = 45) appears. On the basis of the known thermochemical onset of this fragment, a reverse barrier of 325 meV was found. Two more sequential dissociation reactions were examined, namely, ethylene and formaldehyde losses from the methyl-loss daughter ion. The 0 K appearance energies of 11.85 ± 0.07 and 12.20 ± 0.08 eV, respectively, indicate no reverse barrier in these processes. The statistical model of the dissociative photoionization can also be used to predict the fractional ion abundances in threshold photoionization at large temperatures, which could be of use in, for example, combustion diagnostics.
Tunable femtosecond near-infrared source based on a Yb:LYSO-laser-pumped optical parametric oscillator

NASA Astrophysics Data System (ADS)

Wen-Long, Tian; Zhao-Hua, Wang; Jiang-Feng, Zhu; Zhi-Yi, Wei

2016-01-01

We demonstrate a widely tunable near-infrared source from 767 nm to 874 nm generated by the intracavity second harmonic generation (SHG) in an optical parametric oscillator pumped by a Yb:LYSO solid-state laser. The home-made Yb:LYSO oscillator centered at 1035 nm delivers an average power of 2 W and a pulse duration as short as 351 fs. Two MgO doped periodically poled lithium niobates (MgO:PPLN) with grating periods of 28.5-31.5 μm in steps of 0.5 μm and 19.5-21.3 μm in steps of 0.2 μm are used for the OPO and intracavity SHG, respectively. The maximum average output power of 180 mW at 798 nm was obtained and the output pulses have pulse duration of 313 fs at 792 nm if a sech2-pulse shape was assumed. In addition, tunable signal femtosecond pulses from 1428 nm to 1763 nm are also realized with the maximum average power of 355 mW at 1628 nm. Project supported by the National Key Basic Research Program of China (Grant No. 2013CB922402), the National Key Scientific Instruments Development Program of China (Grant No. 2012YQ120047), the National Natural Science Foundation of China (Grant Nos. 61205130 and 11174361), and the Key Deployment Project of Chinese Academy of Sciences (Grant No. KJZD-EW-L11-03).
Rotational Dynamics of Solutes with Multiple Single Bond Axes Studied by Infrared Pump-Probe Spectroscopy.

PubMed

Okuda, Masaki; Ohta, Kaoru; Tominaga, Keisuke

2018-02-01

To investigate the relationship between the structural degrees of freedom around a vibrational probe and the rotational relaxation process of a solute in solution, we studied the anisotropy decays of three different N 3 -derivatized amino acids in primary alcohol solutions. By performing polarization-controlled IR pump-probe measurements, we reveal that the anisotropy decays of the vibrational probe molecules in 1-alcohol solutions possess two decay components, at subpicosecond and picosecond time scales. On the basis of results showing that the fast relaxation component is insensitive to the vibrational probe molecule, we suggest that the anisotropy decay of the N 3 group on a subpicosecond time scale results from a local, small-amplitude fluctuation of the flexible vibrational probe, which does not depend on the details of its molecular structure. However, the slow relaxation component depends on the solute: with longer alkyl chains attached to the N 3 group, the anisotropy decay of the slow component is faster. Consequently, we conclude that the slow relaxation component corresponds to the reorientational motion of the N 3 group correlated with other intramolecular rotational motions (e.g., rotational motions of the neighboring alkyl chain). Our experimental results provide important insight into understanding the rotational dynamics of solutes with multiple single bond axes in solution.
Extension of supercontinuum spectrum, generated in polarization-maintaining photonic crystal fiber, using chirped femtosecond pulses

NASA Astrophysics Data System (ADS)

Vengelis, Julius; Jarutis, Vygandas; Sirutkaitis, Valdas

2018-01-01

We present results of experimental and numerical investigation of supercontinuum (SC) generation in polarization-maintaining photonic crystal fiber (PCF) using chirped femtosecond pulses. The initial unchirped pump pulse source was a mode-locked Yb:KGW laser generating 52-nJ energy, 110-fs duration pulses at 1030 nm with a 76-MHz repetition rate. The nonlinear medium was a 32-cm-long polarization-maintaining PCF manufactured by NKT Photonics A/S. We demonstrated the influence of pump pulse chirp on spectral characteristics of a SC. We showed that by chirping pump pulses positively or negatively one can obtain a broader SC spectrum than in the case of unchirped pump pulses at the same peak power. Moreover, the extension can be controlled by changing the amount of pump pulse chirp. Numerical simulation results also indicated that pump pulse chirp yields an extension of SC spectrum.
Probing photoelectron multiple interferences via Fourier spectroscopy in energetic photoionization of Xe@C60

NASA Astrophysics Data System (ADS)

Potter, Andrea; McCune, Matthew A.; de, Ruma; Madjet, Mohamed E.; Chakraborty, Himadri S.

2010-09-01

Considering the photoionization of the Xe@C60 endohedral compound, we study in detail the ionization cross sections of various levels of the system at energies higher than the plasmon resonance region. Five classes of single-electron levels are identified depending on their spectral character. Each class engenders distinct oscillations in the cross section, emerging from the interference between active ionization modes specific to that class. Analysis of the cross sections based on their Fourier transforms unravels oscillation frequencies that carry unique fingerprints of the emitting level.
Terahertz dielectric response of photoexcited carriers in Si revealed via single-shot optical-pump and terahertz-probe spectroscopy

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

Minami, Yasuo; Horiuchi, Kohei; Masuda, Kaisei

We have demonstrated accurate observations of terahertz (THz) dielectric response due to photoexcited carriers in a Si plate via single-shot optical-pump and THz-probe spectroscopy. In contrast to conventional THz time-domain spectroscopy, this spectroscopic technique allows single-shot detection of the THz response of materials at a given delay time between the pump and THz pulses, thereby sufficiently extending the time interval between the pump pulses. As a result, we can accurately measure the dielectric properties of materials, while avoiding artifacts in the response caused by the accumulation of long-lived photoexcited carriers. Using our single-shot scheme, the transmittance of a Si platemore » was measured in the range of 0.5–2.5 THz with different pump fluences. Based on a Drude model analysis, the optically induced complex dielectric constant, plasma frequency, and damping rate in the THz region were quantitatively evaluated.« less
Development of a femtosecond micromachining workstation by use of spectral interferometry.

PubMed

Bera, Sudipta; Sabbah, A J; Durfee, Charles G; Squier, Jeff A

2005-02-15

A workstation that permits real-time measurement of ablation depth while micromachining with femtosecond laser pulses is demonstrated. This method incorporates the unamplified pulse train that is available in a chirped-pulse amplification system as the probe in an arrangement that uses spectral interferometry to measure the ablation depth while cutting with the amplified pulse in thin metal films.
New topics in coherent anti-stokes raman scattering gas-phase diagnostics : femtosecond rotational CARS and electric-field measurements.

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

Lempert, Walter R.; Barnat, Edward V.; Kearney, Sean Patrick

2010-07-01

We discuss two recent diagnostic-development efforts in our laboratory: femtosecond pure-rotational Coherent anti-Stokes Raman scattering (CARS) for thermometry and species detection in nitrogen and air, and nanosecond vibrational CARS measurements of electric fields in air. Transient pure-rotational fs-CARS data show the evolution of the rotational Raman polarization in nitrogen and air over the first 20 ps after impulsive pump/Stokes excitation. The Raman-resonant signal strength at long time delays is large, and we additionally observe large time separation between the fs-CARS signatures of nitrogen and oxygen, so that the pure-rotational approach to fs-CARS has promise for simultaneous species and temperature measurementsmore » with suppressed nonresonant background. Nanosecond vibrational CARS of nitrogen for electric-field measurements is also demonstrated. In the presence of an electric field, a dipole is induced in the otherwise nonpolar nitrogen molecule, which can be probed with the introduction of strong collinear pump and Stokes fields, resulting in CARS signal radiation in the infrared. The electric-field diagnostic is demonstrated in air, where the strength of the coherent infrared emission and sensitivity our field measurements is quantified, and the scaling of the infrared signal with field strength is verified.« less
Carrier-envelope phase effects for a dipolar molecule interacting with two-color pump-probe laser pulses

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

Cheng Taiwang; Brown, Alex

2004-12-01

The interaction of a two-level dipolar molecule with two laser pulses, where one laser's frequency is tuned to the energy level separation (pump laser) while the second laser's frequency is extremely small (probe laser), is investigated. A dipolar molecule is one with a nonzero difference between the permanent dipole moments of the molecular states. As shown previously [A. Brown, Phys. Rev. A 66, 053404 (2002)], the final population transfer between the two levels exhibits a dependence on the carrier-envelope phase of the probe laser. Based on the rotating-wave approximation (RWA), an effective Hamiltonian is derived to account for the basicmore » characteristics of the carrier-envelope phase dependence effect. By analysis of the effective Hamiltonian, scaling properties of the system are found with regard to field strengths, pulse durations, and frequencies. According to these scaling properties, the final-state population transfer can be controlled by varying the carrier-envelope phase of the probe laser field using lasers with weak field strengths (low intensities) and relatively long pulse durations. In order to examine the possible roles of background states, the investigation is extended to a three-level model. It is demonstrated that the carrier-envelope phase effect still persists in a well-defined manner even when neighboring energy levels are present. These results illustrate the potential of utilizing excitation in dipolar molecules as a means of measuring the carrier-envelope phase of a laser pulse or if one can manipulate the carrier envelope phase, as a method of controlling population transfer in dipolar molecules. The results also suggest that the carrier-envelope phases must be taken into account properly when performing calculations involving pump-probe excitation schemes with laser frequencies which differ widely in magnitude.« less
Monolithic optofluidic ring resonator lasers created by femtosecond laser nanofabrication.

PubMed

Chandrahalim, Hengky; Chen, Qiushu; Said, Ali A; Dugan, Mark; Fan, Xudong

2015-05-21

We designed, fabricated, and characterized a monolithically integrated optofluidic ring resonator laser that is mechanically, thermally, and chemically robust. The entire device, including the ring resonator channel and sample delivery microfluidics, was created in a block of fused-silica glass using a 3-dimensional femtosecond laser writing process. The gain medium, composed of Rhodamine 6G (R6G) dissolved in quinoline, was flowed through the ring resonator. Lasing was achieved at a pump threshold of approximately 15 μJ mm(-2). Detailed analysis shows that the Q-factor of the optofluidic ring resonator is 3.3 × 10(4), which is limited by both solvent absorption and scattering loss. In particular, a Q-factor resulting from the scattering loss can be as high as 4.2 × 10(4), suggesting the feasibility of using a femtosecond laser to create high quality optical cavities.
Near-Field Infrared Pump-Probe Imaging of Surface Phonon Coupling in Boron Nitride Nanotubes.

PubMed

Gilburd, Leonid; Xu, Xiaoji G; Bando, Yoshio; Golberg, Dmitri; Walker, Gilbert C

2016-01-21

Surface phonon modes are lattice vibrational modes of a solid surface. Two common surface modes, called longitudinal and transverse optical modes, exhibit lattice vibration along or perpendicular to the direction of the wave. We report a two-color, infrared pump-infrared probe technique based on scattering type near-field optical microscopy (s-SNOM) to spatially resolve coupling between surface phonon modes. Spatially varying couplings between the longitudinal optical and surface phonon polariton modes of boron nitride nanotubes are observed, and a simple model is proposed.
Simple efficient travelin-wave excitation of short-wavelength lasers using a conical pumping geometry.

PubMed

Silfvast, W T; Ii, O R

1989-01-01

A conically shaped pumping geometry can produce an efficient burst of laser radiation, without the need for an optical cavity, by restricting amplified spontaneous emission losses to a small region near the apex of the cone. Requirements on the active medium and on the size and intensity of the pumping source to make such a burst laser are derived. We calculate that a 15-mJ pulse of energy at 37.2 nm at an efficiency of 0.15% can be extracted from sodium vapor photoionized with radiation from a 1.06-microm-laser-produced plasma using this pumping geometry.
Nonlinear nonlocal infrared plasmonic arrays for pump-probe studies on protein monolayers

NASA Astrophysics Data System (ADS)

Erramilli, Shyamsunder; Adato, Ronen; Gabel, Alan; Yanik, Ahmet Ali; Altug, Hatice; Hong, Mi K.

2010-03-01

Infrared spectroscopy is an exquisite bond-specific tool for studying biomolecules with characteristic vibrational normal modes that serve as a molecular ``fingerprint''. Intrinsic absorption cross-sections for proteins are significant (˜10-19 -10-21 cm^2), although small compared to label-based fluorescence methods. We have shown that carefully designed plasmonic nanoantenna arrays can enhance the vibrational signatures by ˜ 10^5 (Adato et al, Proc Natl Acad Sci USA, 2009). Theoretical modeling combined with polarized FTIR-microscopy show that enhancement is due both to localized effects and nonlocal collective effects, governed by the dielectric properties of silicon and gold nanoantennae, coupled to protein molecules. The resonance properties can be modulated by photoinduced excitation of charge carriers and excitons, causing both a shift in the resonance frequency and a change in the enhancement factor. An ultrafast visible pump laser can then be used to extend visible pump-infrared probe studies to protein molecules even when the molecules lack a chromophore. This provides a toolkit for biophysical studies in which the nonlinear, nonlocal interaction between a 35-fs visible or near-infrared laser and the designed plasmonic nanoantenna arrays are used to study dynamics of protein molecules.

Multiparameter spatio-thermochemical probing of flame–wall interactions advanced with coherent Raman imaging

DOE PAGES

Bohlin, Gustav Alexis; Jainski, Christopher; Patterson, Brian D.; ...

2016-08-10

Ultrabroadband coherent anti-Stokes Ra man spectroscopy (CARS) has been developed for one -dimensional imaging of temperature and major species distributions simultaneously in the near-wall region of a methane/air flame supported on a side-wall-quenching (SWQ) burner. Automatic temporal and spatial overlap of the ~7 femtosecond pump and Stokes pulses is achieved utilizing a two-beam CARS phase-matching scheme, and the crossed ~75 picosecond probe beam provide s excellent spatial sectioning of the probed location. Concurrent detection of N 2, O 2, H 2, CO, CO 2, and CH 4 is demonstrated while high-fidelity flame thermometry is assessed from the N 2 puremore » rotational S-branch in a one-dimensional -CARS imaging configuration. A methane/air premixed flame at lean, stoichiometric, and rich conditions ( Φ = 0.83, 1.0 , and 1.2) and Reynolds number = 5,000 is probed as it quenches against a cooled steel side- wall parallel to the flow providing a persistent flame-wall interaction. Here, an imaging resolution of better than 40 μm is achieved across the field -of-view, thus allowing thermochemical states (temperature and major species) of the thermal boundary layer to be resolved to within ~30 μm of the interface.« less
Multiparameter spatio-thermochemical probing of flame–wall interactions advanced with coherent Raman imaging

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

Bohlin, Gustav Alexis; Jainski, Christopher; Patterson, Brian D.

Ultrabroadband coherent anti-Stokes Ra man spectroscopy (CARS) has been developed for one -dimensional imaging of temperature and major species distributions simultaneously in the near-wall region of a methane/air flame supported on a side-wall-quenching (SWQ) burner. Automatic temporal and spatial overlap of the ~7 femtosecond pump and Stokes pulses is achieved utilizing a two-beam CARS phase-matching scheme, and the crossed ~75 picosecond probe beam provide s excellent spatial sectioning of the probed location. Concurrent detection of N 2, O 2, H 2, CO, CO 2, and CH 4 is demonstrated while high-fidelity flame thermometry is assessed from the N 2 puremore » rotational S-branch in a one-dimensional -CARS imaging configuration. A methane/air premixed flame at lean, stoichiometric, and rich conditions ( Φ = 0.83, 1.0 , and 1.2) and Reynolds number = 5,000 is probed as it quenches against a cooled steel side- wall parallel to the flow providing a persistent flame-wall interaction. Here, an imaging resolution of better than 40 μm is achieved across the field -of-view, thus allowing thermochemical states (temperature and major species) of the thermal boundary layer to be resolved to within ~30 μm of the interface.« less
Optically Guided Photoactivity: Coordinating Tautomerization, Photoisomerization, Inhomogeneity, and Reactive Intermediates within the RcaE Cyanobacteriochrome.

PubMed

Gottlieb, Sean M; Chang, Che-Wei; Martin, Shelley S; Rockwell, Nathan C; Lagarias, J Clark; Larsen, Delmar S

2014-05-01

The RcaE cyanobacteriochrome uses a linear tetrapyrrole chromophore to sense the ratio of green and red light to enable the Fremyella diplosiphon cyanobacterium to control the expression of the photosynthetic infrastructure for efficient utilization of incident light. The femtosecond photodynamics of the embedded phycocyanobilin chromophore within RcaE were characterized with dispersed femtosecond pump-dump-probe spectroscopy, which resolved a complex interplay of excited-state proton transfer, photoisomerization, multilayered inhomogeneity, and reactive intermediates. These reactions were integrated within a central model that incorporated a rapid (200 fs) excited-state Le Châtelier redistribution between parallel evolving populations ascribed to different tautomers. Three photoproducts were resolved and originates from four independent subpopulations, each with different dump-induced behavior: Lumi-Go was depleted, Lumi-Gr was unaffected, and Lumi-Gf was enhanced. This suggests that RcaE may be engineered to act either as an in vivo fluorescent probe (after single-pump excitation) or as an in vivo optogenetic sample (after pump and dump excitation).
Effects of Different Quantum Coherence on the Pump-Probe Polarization Anisotropy of Photosynthetic Light-Harvesting Complexes: A Computational Study.

PubMed

Bai, Shuming; Song, Kai; Shi, Qiang

2015-05-21

Observations of oscillatory features in the 2D spectra of several photosynthetic complexes have led to diverged opinions on their origins, including electronic coherence, vibrational coherence, and vibronic coherence. In this work, effects of these different types of quantum coherence on ultrafast pump-probe polarization anisotropy are investigated and distinguished. We first simulate the isotropic pump-probe signal and anisotropy decay of the Fenna-Matthews-Olson (FMO) complex using a model with only electronic coherence at low temperature and obtain the same coherence time as in the previous experiment. Then, three model dimer systems with different prespecified quantum coherence are simulated, and the results show that their different spectral characteristics can be used to determine the type of coherence during the spectral process. Finally, we simulate model systems with different electronic-vibrational couplings and reveal the condition in which long time vibronic coherence can be observed in systems like the FMO complex.
Theoretical modeling and experiments on a DBR waveguide laser fabricated by the femtosecond laser direct-write technique.

PubMed

Duan, Yuwen; McKay, Aaron; Jovanovic, Nemanja; Ams, Martin; Marshall, Graham D; Steel, M J; Withford, Michael J

2013-07-29

We present a model for a Yb-doped distributed Bragg reflector (DBR) waveguide laser fabricated in phosphate glass using the femtosecond laser direct-write technique. The model gives emphasis to transverse integrals to investigate the energy distribution in a homogenously doped glass, which is an important feature of femtosecond laser inscribed waveguide lasers (WGLs). The model was validated with experiments comparing a DBR WGL and a fiber laser, and then used to study the influence of distributed rare earth dopants on the performance of such lasers. Approximately 15% of the pump power was absorbed by the doped "cladding" in the femtosecond laser inscribed Yb doped WGL case with the length of 9.8 mm. Finally, we used the model to determine the parameters that optimize the laser output such as the waveguide length, output coupler reflectivity and refractive index contrast.
Superresolution fluorescence imaging by pump-probe setup using repetitive stimulated transition process

NASA Astrophysics Data System (ADS)

Dake, Fumihiro; Fukutake, Naoki; Hayashi, Seri; Taki, Yusuke

2018-02-01

We proposed superresolution nonlinear fluorescence microscopy with pump-probe setup that utilizes repetitive stimulated absorption and stimulated emission caused by two-color laser beams. The resulting nonlinear fluorescence that undergoes such a repetitive stimulated transition is detectable as a signal via the lock-in technique. As the nonlinear fluorescence signal is produced by the multi-ply combination of incident beams, the optical resolution can be improved. A theoretical model of the nonlinear optical process is provided using rate equations, which offers phenomenological interpretation of nonlinear fluorescence and estimation of the signal properties. The proposed method is demonstrated as having the scalability of optical resolution. Theoretical resolution and bead image are also estimated to validate the experimental result.
Application of the R-matrix method to photoionization of molecules.

PubMed

Tashiro, Motomichi

2010-04-07

The R-matrix method has been used for theoretical calculation of electron collision with atoms and molecules for long years. The method was also formulated to treat photoionization process, however, its application has been mostly limited to photoionization of atoms. In this work, we implement the R-matrix method to treat molecular photoionization problem based on the UK R-matrix codes. This method can be used for diatomic as well as polyatomic molecules, with multiconfigurational description for electronic states of both target neutral molecule and product molecular ion. Test calculations were performed for valence electron photoionization of nitrogen (N(2)) as well as nitric oxide (NO) molecules. Calculated photoionization cross sections and asymmetry parameters agree reasonably well with the available experimental results, suggesting usefulness of the method for molecular photoionization.
Double Photoionization Near Threshold

NASA Technical Reports Server (NTRS)

Wehlitz, Ralf

2007-01-01

The threshold region of the double-photoionization cross section is of particular interest because both ejected electrons move slowly in the Coulomb field of the residual ion. Near threshold both electrons have time to interact with each other and with the residual ion. Also, different theoretical models compete to describe the double-photoionization cross section in the threshold region. We have investigated that cross section for lithium and beryllium and have analyzed our data with respect to the latest results in the Coulomb-dipole theory. We find that our data support the idea of a Coulomb-dipole interaction.
Stark-assisted population control of coherent CS(2) 4f and 5p Rydberg wave packets studied by femtosecond time-resolved photoelectron spectroscopy.

PubMed

Knappenberger, Kenneth L; Lerch, Eliza-Beth W; Wen, Patrick; Leone, Stephen R

2007-09-28

A two-color (3+1(')) pump-probe scheme is employed to investigate Rydberg wave packet dynamics in carbon disulfide (CS(2) (*)). The state superpositions are created within the 4f and 5p Rydberg manifolds by three photons of the 400 nm pump pulse, and their temporal evolution is monitored with femtosecond time-resolved photoelectron spectroscopy using an 800 nm ionizing probe pulse. The coherent behavior of the non-stationary superpositions are observed through wavepacket revivals upon ionization to either the upper (12) or lower (32) spin-orbit components of CS(2) (+). The results show clearly that the composition of the wavepacket can be efficiently controlled by the power density of the excitation pulse over a range from 500 GWcm(2) to 10 TWcm(2). The results are consistent with the anticipated ac-Stark shift for 400 nm light and demonstrate an effective method for population control in molecular systems. Moreover, it is shown that Rydberg wavepackets can be formed in CS(2) with excitation power densities up to 10 TWcm(2) without significant fragmentation. The exponential 1e population decay (T(1)) of specific excited Rydberg states are recovered by analysis of the coherent part of the signal. The dissociation lifetimes of these states are typically 1.5 ps. However, a region exhibiting a more rapid decay ( approximately 800 fs) is observed for states residing in the energy range of 74 450-74 550 cm(-1), suggestive of an enhanced surface crossing in this region.
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.
Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging

NASA Astrophysics Data System (ADS)

Cocker, Tyler L.; Peller, Dominik; Yu, Ping; Repp, Jascha; Huber, Rupert

2016-11-01

Watching a single molecule move on its intrinsic timescale has been one of the central goals of modern nanoscience, and calls for measurements that combine ultrafast temporal resolution with atomic spatial resolution. Steady-state experiments access the requisite spatial scales, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution. But tracking the intrinsic dynamics of a single molecule directly in the time domain faces the challenge that interactions with the molecule must be confined to a femtosecond time window. For individual nanoparticles, such ultrafast temporal confinement has been demonstrated by combining scanning tunnelling microscopy with so-called lightwave electronics, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on timescales faster even than a single cycle of light. Here we build on ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state. It thereby removes a single electron from an individual pentacene molecule’s highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record approximately 100-femtosecond snapshot images of the orbital structure with sub-ångström spatial resolution, and to reveal, through pump/probe measurements, coherent molecular vibrations at terahertz frequencies directly in the time domain. We anticipate that the combination of lightwave electronics and the atomic resolution of our approach will open the door to visualizing ultrafast photochemistry and the operation of molecular electronics on the single-orbital scale.
PHOTOIONIZATION IN THE SOLAR WIND

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

Landi, E.; Lepri, S. T., E-mail: elandi@umich.edu

2015-10-20

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 withoutmore » 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 O{sup 7+}/O{sup 6+} 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 O{sup 7+}/O{sup 6+} ratio needs to be used with caution for solar wind classification and coronal temperature estimates, and recommend the C{sup 6+}/C{sup 4+} ratio for these purposes.« less
Atomic photoionization processes under magnification

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

Lepine, F.; Bordas, Ch.; Nicole, C.

2004-09-01

Recently, classical simulations of threshold photoionization in the presence of an electric field have shown that a clear distinction between direct and indirect trajectories followed by the outgoing electron can be observed in the patterns of electron impacts on a two-dimensional detector. Subsequently, slow photoelectron imaging experiments have been reported where this distinction could be observed in atomic xenon. Furthermore, using a magnifying electrostatic lens to improve the velocity-map imaging technique, oscillatory patterns were observed modulating the classical envelope that was measured in the experiments of Nicole et al. [Phys. Rev. Lett. 88, 133001 (2002)]. This extension of slow photoelectronmore » imaging, called photoionization microscopy, relies on the existence of interferences between various trajectories by which the electron moves from the atom to the plane of observation. In this article we present the main experimental results obtained both in slow photoelectron imaging and in photoionization microscopy. The formation of the interference pattern is discussed in the framework of a semiclassical model that is described in detail elsewhere. The qualitative information that can be drawn from the experiments is discussed, and the potential applications of photoionization microscopy are considered. Particular attention is paid to the role of continuum Stark resonances that appear between the saddle point in the Coulomb+dc field potential and the field-free ionization limit.« less
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
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.
Dissociative Photoionization of the Elusive Vinoxy Radical.

PubMed

Adams, Jonathan D; Scrape, Preston G; Lee, Shih-Huang; Butler, Laurie J

2017-08-24

These experiments report the dissociative photoionization of vinoxy radicals to m/z = 15 and 29. In a crossed laser-molecular beam scattering apparatus, we induce C-Cl bond fission in 2-chloroacetaldehyde by photoexcitation at 157 nm. Our velocity measurements, combined with conservation of angular momentum, show that 21% of the C-Cl photofission events form vinoxy radicals that are stable to subsequent dissociation to CH 3 + CO or H + ketene. Photoionization of these stable vinoxy radicals, identified by their velocities, which are momentum-matched with the higher-kinetic-energy Cl atom photofragments, shows that the vinoxy radicals dissociatively photoionize to give signal at m/z = 15 and 29. We calibrated the partial photoionization cross section of vinoxy to CH 3 + relative to the bandwidth-averaged photoionization cross section of the Cl atom at 13.68 eV to put the partial photoionization cross sections on an absolute scale. The resulting bandwidth-averaged partial cross sections are 0.63 and 1.3 Mb at 10.5 and 11.44 eV, respectively. These values are consistent with the upper limit to the cross section estimated from a study by Savee et al. on the O( 3 P) + propene bimolecular reaction. We note that the uncertainty in these values is primarily dependent on the signal attributed to C-Cl primary photofission in the m/z = 35 (Cl + ) time-of-flight data. While the value is a rough estimate, the bandwidth-averaged partial photoionization cross section of vinoxy to HCO + calculated from the signal at m/z = 29 at 11.53 eV is approximately half that of vinoxy to CH 3 + . We also present critical points on the potential energy surface of the vinoxy cation calculated at the G4//B3LYP/6-311++G(3df,2p) level of theory to support the observation of dissociative ionization of vinoxy to both CH 3 + and HCO + .
Characteristics of optical parametric oscillator synchronously pumped by Yb:KGW laser and based on periodically poled potassium titanyl phosphate crystal

NASA Astrophysics Data System (ADS)

Vengelis, Julius; Tumas, Adomas; Pipinytė, Ieva; Kuliešaitė, Miglė; Tamulienė, Viktorija; Jarutis, Vygandas; Grigonis, Rimantas; Sirutkaitis, Valdas

2018-03-01

We present experimental data and numerical simulation results obtained during investigation of synchronously pumped optical parametric oscillator (SPOPO) pumped by femtosecond Yb:KGW laser (central wavelength at 1033 nm). The nonlinear medium for parametric generation was periodically poled potassium titanyl phosphate crystal (PPKTP). Maximum parametric light conversion efficiency from pump power to signal power was more than 37.5% at λs=1530 nm wavelength, whereas the achieved signal wave continuous tuning range was from 1470 nm to 1970 nm with signal pulse durations ranging from 91 fs to roughly 280 fs. We demonstrated wavelength tuning by changing cavity length and PPKTP crystal grating period and also discussed net cavity group delay dispersion (GDD) influence on SPOPO output radiation characteristics. The achieved high pump to signal conversion efficiency and easy wavelength tuning make this device a very promising alternative to Ti:sapphire based SPOPOs as a source of continuously tunable femtosecond laser radiation in the near and mid-IR range.
Rovibrational hybrid fs/ps CARS using a volume Bragg grating for N₂ thermometry.

PubMed

Scherman, M; Nafa, M; Schmid, T; Godard, A; Bresson, A; Attal-Tretout, B; Joubert, P

2016-02-01

Coherent anti-Stokes Raman scattering (CARS) spectra of N2 in the hybrid femtosecond/picosecond regime have been recorded with 0.7 cm(-1) resolution. The Q-branch rovibrational structure has been resolved, making it suitable for gas-phase simultaneous rotational and vibrational thermometry applications. Resolving this spectral structure requires synchronization of a narrowband picosecond probe pulse with a broadband femtosecond pair of pump and Stokes pulses. It is achieved using a single femtosecond ytterbium-laser source and a volume Bragg grating in a compact experimental arrangement.
Picosecond dynamics of photoexcited DNO-bound myoglobin probed by femtosecond vibrational spectroscopy.

PubMed

Lee, Taegon; Hwang, Sungu; Lim, Manho

2015-02-05

Like nitric oxide (NO), nitroxyl (HNO), a reduced form of NO, plays many biologically important roles including neurological function and vascular regulation. Although HNO is unstable in aqueous solution, it is exceptionally stable on binding to ferrous myoglobin (Mb) to form MbHNO. Various experimental and theoretical investigations has been carried out to unveil the structure of the active site and binding characteristics of MbHNO that can explain its functioning mechanism and the origin of its unusual stability. However, the binding dynamics of HNO to Mb, as well as the photochemical and photophysical processes associated with binding, have not been fully established. Herein, femtosecond vibrational spectroscopy was used to probe the photoexcitation dynamics of excited MbDNO in D2O solution at 294 K with a 575 nm pulse. Time-resolved spectra were described by three vibrational bands near 1380 cm(-1), in the expected N-O stretching (νN-O) mode of MbDNO, and all three bands showed instantaneous bleach that decays on a picosecond time scale. The three bands were assigned based on isotope shifts upon (15)N substitution and ab initio calculation of the vibrational frequency on a DNO-bound model heme. These three bands likely arise from Fermi interactions between the strong νN-O mode and the weak overtone and combination modes of the N atom-related modes. The immediate appearance of the bleach in these bands and the picosecond decay of the bleach indicate that most of the photoexcited MbDNO undergoes picosecond geminate rebinding (GR) of DNO to Mb subsequent to its immediate deligation. Ultrafast and efficient GR of DNO likely arises from the bonding structure of the ligand and high reactivity between DNO and Mb.
Angular dependence of EWS time delay for photoionization of @Xe

NASA Astrophysics Data System (ADS)

Mandal, Ankur; Deshmukh, Pranawa; Kheifets, Anatoli; Dolmatov, Valeriy; Manson, Steven

2017-04-01

Interference between photoionization channels leads to angular dependence in photoionization time delay. Angular dependence is found to be a common effect for two-photon absorption experiments very recently. The effect of confinement on the time delay where each partial wave contributions to the ionization are studied. In this work we report angular dependence and confinement effects on Eisenbud-Wigner-Smith (EWS) time delay in atomic photoionization. Using and we computed the EWS time delay for free and confined Xe atom for photoionization from inner 4d3/2 and 4d5/2 and outer 5p1/2 and 5p3/2 subshells at various angles. The calculated EWS time delay is few tens to few hundreds of attoseconds (10-18 second). The photoionization time delay for @Xe follows that in the free Xe atom on which the confinement oscillations are built. The present work reveals the effect of confinement on the photoionization time delay at different angles between photoelectron ejection and the photon polarization.

Femtosecond-laser-written superficial cladding waveguides in Nd:CaF2 crystal

NASA Astrophysics Data System (ADS)

Li, Rang; Nie, Weijie; Lu, Qingming; Cheng, Chen; Shang, Zhen; Vázquez de Aldana, Javier R.; Chen, Feng

2017-07-01

We report on the superficial cladding waveguides fabricated by direct femtosecond laser writing in Nd: CaF2 crystal with three different groups of parameters. The lowest propagation loss of waveguides has been determined to be 0.7 dB/cm at wavelength of 632.8 nm along TE polarization. The near fundamental modal distributions have been imaged through the end-face coupling technique. The guidance of the waveguides is found to possess low sensitivity on polarization of the probe light. By using a confocal microscope system, the micro-photoluminescence mappings and micro-fluorescence spectra are also obtained, which indicates the photoluminescence features of the Nd3+ ions are well preserved in the waveguide cores after direct femtosecond laser writing.
Consistent characterization of semiconductor saturable absorber mirrors with single-pulse and pump-probe spectroscopy.

PubMed

Fleischhaker, R; Krauss, N; Schättiger, F; Dekorsy, T

2013-03-25

We study the comparability of the two most important measurement methods used for the characterization of semiconductor saturable absorber mirrors (SESAMs). For both methods, single-pulse spectroscopy (SPS) and pump-probe spectroscopy (PPS), we analyze in detail the time-dependent saturation dynamics inside a SESAM. Based on this analysis, we find that fluence-dependent PPS at complete spatial overlap and zero time delay is equivalent to SPS. We confirm our findings experimentally by comparing data from SPS and PPS of two samples. We show how to interpret this data consistently and we give explanations for possible deviations.
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.
Femtosecond laser for cavity preparation in enamel and dentin: ablation efficiency related factors.

PubMed

Chen, H; Li, H; Sun, Yc; Wang, Y; Lü, Pj

2016-02-11

To study the effects of laser fluence (laser energy density), scanning line spacing and ablation depth on the efficiency of a femtosecond laser for three-dimensional ablation of enamel and dentin. A diode-pumped, thin-disk femtosecond laser (wavelength 1025 nm, pulse width 400 fs) was used for the ablation of enamel and dentin. The laser spot was guided in a series of overlapping parallel lines on enamel and dentin surfaces to form a three-dimensional cavity. The depth and volume of the ablated cavity was then measured under a 3D measurement microscope to determine the ablation efficiency. Different values of fluence, scanning line spacing and ablation depth were used to assess the effects of each variable on ablation efficiency. Ablation efficiencies for enamel and dentin were maximized at different laser fluences and number of scanning lines and decreased with increases in laser fluence or with increases in scanning line spacing beyond spot diameter or with increases in ablation depth. Laser fluence, scanning line spacing and ablation depth all significantly affected femtosecond laser ablation efficiency. Use of a reasonable control for each of these parameters will improve future clinical application.
Following coherent multichannel nuclear wave packets in pump-probe studies of O2 with ultrashort laser pulses

NASA Astrophysics Data System (ADS)

Xue, Shan; Du, Hongchuan; Hu, Bitao; Lin, C. D.; Le, Anh-Thu

2018-04-01

We reexamine the recent pump-probe experiment with O2 using short intense infrared laser pulses theoretically. Using parameters that closely mimic the experimental conditions and taking into account the angle-dependent population redistribution due to resonant coupling between the relevant states, we show that the observed kinetic energy release spectra, including the energy-dependent structure and the quantum beat frequencies, can be accurately reproduced. Our results reveal additional important channels that were missed earlier. In particular, the strong contributions from O2+a 4Πu and b 4Σg- states lead to the possibility of observing the interchannel beating. We further demonstrate that, by varying the laser parameters, the coherent nuclear wave-packet motions on different potential energy surfaces (PESs) can be probed and the properties of the PES can be examined. Future experiments with different wavelength lasers are proposed for better probing and controlling nuclear dynamics on different PESs.
Separation of High Order Harmonics with Fluoride Windows

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

Allison, Tom; van Tilborg, Jeroen; Wright, Travis

2010-08-02

The lower orders produced in high order harmonic generation can be effciently temporally separated into monochromatic pulses by propagation in a Fluoride window while still preserving their femtosecond pulse duration. We present calculations for MgF2, CaF2, and LiF windows for the third, fifth, and seventh harmonics of 800 nm. We demonstrate the use of this simple and inexpensive technique in a femtosecond pump/probe experiment using the fifth harmonic.
Domain of validity of the perturbative approach to femtosecond optical spectroscopy

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

Gelin, Maxim F.; Rao, B. Jayachander; Nest, Mathias

2013-12-14

We have performed numerical nonperturbative simulations of transient absorption pump-probe responses for a series of molecular model systems. The resulting signals as a function of the laser field strength and the pump-probe delay time are compared with those obtained in the perturbative response function formalism. The simulations and their theoretical analysis indicate that the perturbative description remains valid up to moderately strong laser pulses, corresponding to a rather substantial depopulation (population) of the initial (final) electronic states.
Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer

DOE PAGES

Dell'Angela, M.; Anniyev, T.; Beye, M.; ...

2015-03-01

Vacuum space charge-induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse.
Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer.

PubMed

Dell'Angela, M; Anniyev, T; Beye, M; Coffee, R; Föhlisch, A; Gladh, J; Kaya, S; Katayama, T; Krupin, O; Nilsson, A; Nordlund, D; Schlotter, W F; Sellberg, J A; Sorgenfrei, F; Turner, J J; Öström, H; Ogasawara, H; Wolf, M; Wurth, W

2015-03-01

Vacuum space charge induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse.
Wavelength dependence of femtosecond laser-induced damage threshold of optical materials

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

Gallais, L., E-mail: laurent.gallais@fresnel.fr; Douti, D.-B.; Commandré, M.

2015-06-14

An experimental and numerical study of the laser-induced damage of the surface of optical material in the femtosecond regime is presented. The objective of this work is to investigate the different processes involved as a function of the ratio of photon to bandgap energies and compare the results to models based on nonlinear ionization processes. Experimentally, the laser-induced damage threshold of optical materials has been studied in a range of wavelengths from 1030 nm (1.2 eV) to 310 nm (4 eV) with pulse durations of 100 fs with the use of an optical parametric amplifier system. Semi-conductors and dielectrics materials, in bulk or thinmore » film forms, in a range of bandgap from 1 to 10 eV have been tested in order to investigate the scaling of the femtosecond laser damage threshold with the bandgap and photon energy. A model based on the Keldysh photo-ionization theory and the description of impact ionization by a multiple-rate-equation system is used to explain the dependence of laser-breakdown with the photon energy. The calculated damage fluence threshold is found to be consistent with experimental results. From these results, the relative importance of the ionization processes can be derived depending on material properties and irradiation conditions. Moreover, the observed damage morphologies can be described within the framework of the model by taking into account the dynamics of energy deposition with one dimensional propagation simulations in the excited material and thermodynamical considerations.« less
Palm-top-size, 1.5 kW peak-power, and femtosecond (160 fs) diode-pumped mode-locked Yb+3:KY(WO4)2 solid-state laser with a semiconductor saturable absorber mirror.

PubMed

Yamazoe, Shogo; Katou, Masaki; Adachi, Takashi; Kasamatsu, Tadashi

2010-03-01

We report a palm-top-size femtosecond diode-pumped mode-locked Yb(+3):KY(WO(4))(2) solid-state laser with a semiconductor saturable absorber mirror utilizing soliton mode locking for shortening the cavity to 50 mm. An average output power of 680 mW and a pulse width of 162 fs were obtained at 1045 nm with a repetition rate of 2.8 GHz, which led to a peak power of 1.5 kW. Average power fluctuations of a modularized laser source were found to be +/-10% for the free-running 3000 h operation and +/-1% for the power-controlled 2000 h operation.
All-optical modulation in Mid-Wavelength Infrared using porous Si membranes

PubMed Central

Park, Sung Jin; Zakar, Ammar; Zerova, Vera L.; Chekulaev, Dimitri; Canham, Leigh T.; Kaplan, Andre

2016-01-01

We demonstrate for the first time the possibility of all-optical modulation of self-standing porous Silicon (pSi) membrane in the Mid-Wavelength Infrared (MWIR) range using femtosecond pump-probe techniques. To study optical modulation, we used pulses of an 800 nm, 60 femtosecond for pump and a MWIR tunable probe in the spectral range between 3.5 and 4.4 μm. We show that pSi possesses a natural transparency window centred around 4 μm. Yet, about 55% of modulation contrast can be achieved by means of optical excitation at the pump power of 60 mW (4.8 mJ/cm2). Our analysis shows that the main mechanism of the modulation is interaction of the MWIR signal with the free charge carrier excited by the pump. The time-resolved measurements showed a sub-picosecond rise time and a recovery time of about 66 ps, which suggests a modulation speed performance of ~15 GHz. This optical modulation of pSi membrane in MWIR can be applied to a variety of applications such as thermal imaging and free space communications. PMID:27440224
Exploring exciton relaxation and multiexciton generation in PbSe nanocrystals using hyperspectral near-IR probing.

PubMed

Gdor, Itay; Sachs, Hanan; Roitblat, Avishy; Strasfeld, David B; Bawendi, Moungi G; Ruhman, Sanford

2012-04-24

Hyperspectral femtosecond transient absorption spectroscopy is employed to record exciton relaxation and recombination in colloidal lead selenide (PbSe) nanocrystals in unprecedented detail. Results obtained with different pump wavelengths and fluences are scrutinized with regard to three issues: (1) early subpicosecond spectral features due to "hot" excitons are analyzed in terms of suggested underlying mechanisms; (2) global kinetic analysis facilitates separation of the transient difference spectra into single, double, and triple exciton state contributions, from which individual band assignments can be tested; and (3) the transient spectra are screened for signatures of multiexciton generation (MEG) by comparing experiments with excitation pulses both below and well above the theoretical threshold for multiplication. For the latter, a recently devised ultrafast pump-probe spectroscopic approach is employed. Scaling sample concentrations and pump pulse intensities inversely with the extinction coefficient at each excitation wavelength overcomes ambiguities due to direct multiphoton excitation, uncertainties of absolute absorption cross sections, and low signal levels. As observed in a recent application of this method to InAs core/shell/shell nanodots, no sign of MEG was detected in this sample up to photon energy 3.7 times the band gap. Accordingly, numerous reports of efficient MEG in other samples of PbSe suggest that the efficiency of this process varies from sample to sample and depends on factors yet to be determined.
Electron-nuclear spin dynamics of Ga centers in GaAsN dilute nitride semiconductors probed by pump-probe spectroscopy

NASA Astrophysics Data System (ADS)

Sandoval-Santana, J. C.; Ibarra-Sierra, V. G.; Azaizia, S.; Carrère, H.; Bakaleinikov, L. A.; Kalevich, V. K.; Ivchenko, E. L.; Marie, X.; Amand, T.; Balocchi, A.; Kunold, A.

2018-03-01

We propose an experimental procedure to track the evolution of electronic and nuclear spins in Ga2+ centers in GaAsN dilute semiconductors. The method is based on a pump-probe scheme that enables to monitor the time evolution of the three components of the electronic and nuclear spin variables. In contrast to other characterization methods, as nuclear magnetic resonance, this one only needs moderate magnetic fields (B≈ 10 mT), and does not require microwave irradiation. Specifically, we carry out a series of tests for different experimental conditions in order to optimize the procedure for maximum sensitivity in the measurement of the circular degree of polarization. Based on previous experimental results and the theoretical calculations presented here, we estimate that the method could yield a time resolution of about 10ps.
Femtosecond laser-ablated Fresnel zone plate fiber probe and sensing applications

NASA Astrophysics Data System (ADS)

Tan, Xiaoling; Geng, Youfu; Chen, Yan; Li, Shiguo; Wang, Xinzhong

2018-02-01

We investigate the Fresnel zone plate (FZP) inscribed on multimode fiber endface using femtosecond laser ablation and its application in sensing. The mode transmission through fiber tips with FZP is investigated both by the beam propagation method theoretically and by measuring the beam images with a charge-coupled device camera experimentally, which show a good agreement. Such devices are tested for surface-enhanced Raman scattering (SERS) using the aqueous solution of rhodamine 6G under a Raman spectroscopy. The experimental results demonstrate that the SERS signal is enhanced benefiting from focal ability of FZP, which is a promising method for the particular biochemical spectra sensing applications.
Pump-Probe Imaging Differentiates Melanoma from Melanocytic Nevi

PubMed Central

Matthews, Thomas E.; Piletic, Ivan R.; Selim, M. Angelica; Simpson, Mary Jane; Warren, Warren S.

2012-01-01

Melanoma diagnosis is clinically challenging; the accuracy of visual inspection by dermatologists is highly variable and heavily weighted toward false positives. Even the current gold standard of biopsy results in varying diagnoses among pathologists. We have developed a multiphoton technique (based on pump-probe spectroscopy) that directly determines the microscopic distribution of eumelanin and pheomelanin in pigmented lesions of human skin. Our initial results showed a marked difference in the chemical variety of melanin between nonmalignant nevi and melanoma, as well as a number of substantial architectural differences. We examined slices from 42 pigmented lesions and found that melanomas had an increased eumelanin content compared to nonmalignant nevi. When used as a diagnostic criterion, the ratio of eumelanin to pheomelanin captured all investigated melanomas but excluded three-quarters of dysplastic nevi and all benign dermal nevi. Evaluating architectural and cytological features revealed by multiphoton imaging, including the maturation of melanocytes, presence of pigmented melanocytes in the dermis, number and location of melanocytic nests, and confluency of pigmented cells in the epidermis, further increased specificity, allowing rejection of more than half of the remaining false-positive results. We then adapted this multiphoton imaging technique to hematoxylin and eosin (H&E)–stained slides. By adding melanin chemical contrast to H&E-stained slides, pathologists will gain complementary information to increase the ease and accuracy of melanoma diagnosis. PMID:21346168
Continuous-wave modulation of a femtosecond oscillator using coherent molecules.

PubMed

Gold, D C; Karpel, J T; Mueller, E A; Yavuz, D D

2018-03-01

We describe a new method to broaden the frequency spectrum of a femtosecond oscillator in the continuous-wave (CW) domain. The method relies on modulating the femtosecond laser using four-wave mixing inside a Raman-based optical modulator. We prepare the modulator by placing deuterium molecules inside a high-finesse cavity and driving their fundamental vibrational transition using intense pump and Stokes lasers that are locked to the cavity modes. With the molecules prepared, any laser within the optical region of the spectrum can pass through the system and be modulated in a single pass. This constitutes a CW optical modulator at a frequency of 90 THz with a steady-state single-pass efficiency of ∼10 -6 and transient (10 μs-time-scale) single-pass efficiency of ∼10 -4 . Using our modulator, we broaden the initial Ti:sapphire spectrum centered at 800 nm and produce upshifted and downshifted sidebands centered at wavelengths of 650 nm and 1.04 μm, respectively.
Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

NASA Astrophysics Data System (ADS)

Boguslavskiy, Andrey E.; Schalk, Oliver; Gador, Niklas; Glover, William J.; Mori, Toshifumi; Schultz, Thomas; Schuurman, Michael S.; Martínez, Todd J.; Stolow, Albert

2018-04-01

The ultrafast excited state dynamics of the smallest polyene, trans-1,3-butadiene, were studied by femtosecond time-resolved photoelectron-photoion coincidence (TRPEPICO) spectroscopy. The evolution of the excited state wavepacket, created by pumping the bright 1Bu (ππ*) electronic state at its origin of 216 nm, is projected via one- and two-photon ionization at 267 nm onto several ionization continua. The results are interpreted in terms of Koopmans' correlations and Franck-Condon factors for the excited and cationic states involved. The known predissociative character of the cation excited states is utilized to assign photoelectron bands to specific continua using TRPEPICO spectroscopy. This permits us to report the direct observation of the famously elusive S1(21Ag) dark electronic state during the internal conversion of trans 1,3-butadiene. Our phenomenological analysis permits the spectroscopic determination of several important time constants. We report the overall decay lifetimes of the 11Bu and 21Ag states and observe the re-appearance of the hot ground state molecule. We argue that the apparent dephasing time of the S2(11Bu) state, which leads to the extreme breadth of the absorption spectrum, is principally due to large amplitude torsional motion on the 1Bu surface in conjunction with strong non-adiabatic couplings via conical intersections, whereupon nuclear wavepacket revivals to the initial Franck-Condon region become effectively impossible. In Paper II [W. J. Glover et al., J. Chem. Phys. 148, 164303 (2018)], ab initio multiple spawning is used for on-the-fly computations of the excited state non-adiabatic wavepacket dynamics and their associated TRPEPICO observables, allowing for direct comparisons of experiment with theory.
Molecular photoionization processes of astrophysical and aeronomical interest

NASA Technical Reports Server (NTRS)

Langhoff, P. W.

1985-01-01

An account is given of aspects of photoionization processes in molecules, with particular reference to recent theoretical and experimental studies of partial cross sections for production of specific final electronic states and of parent and fragment ions. Such cross sections help provide a basis for specifying the state of excitation of the ionized medium, are useful for estimating the kinetic energy distributions of photoejected electrons and fragment ions, provide parent-and fragment-ion yields, and clarify the possible origins of neutral fragments in highly excited rovibronic states. A descriptive account is given of photoionization phenomena, including tabulation of valence- and inner-shell potentials for some molecules of astrophysical and aeronomical interest. Cross sectional expressions are given. Various approximations currently employed in computational studies are described briefly, threshold laws and high-energy limits are indicated, and distinction is drawn between resonant and direct photoionization phenomena. Recent experimental and theoretical studies of partial photoionization cross sections in selected compounds of astrophysical and aeronomical relevance are described and discussed.
Photoionization and electron-impact ionization of Ar5+

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

Wang, J.C.; Lu, M.; Esteves, D.

2007-02-27

Absolute cross sections for photoionization andelectron-impact Photionization of Ar5+ have been measuredusing twodifferent interacting-beams setups. The spectra consist of measurementsof the yield of products dueto single ionization as a function ofelectron or photon energy. In addition, absolute photoionization andelectron-impact ionization cross sections were measured to normalize themeasured Ar6+ product-ion yield spectra. In the energy range from 90 to111 eV, both electron-impact ionization and photoionization of Ar5+aredominated by indirect 3s subshell excitation-autoionization. In theenergy range from 270 to 285 eV, resonances due to 2p-3dexcitation-autoionization are prominent in the photoionization spectrum.In the range from 225 to 335 eV, an enhancement due tomore » 2p-nl (n>2>excitations are evident in the electron-impactionization cross section.The electron and photon impact data show some features due to excitationof the same intermediate autoionizing states.« less

Ultrabright femtosecond source of biphotons based on a spatial mode inverter.

PubMed

Jarutis, Vygandas; Juodkazis, Saulius; Mizeikis, Vygantas; Sasaki, Keiji; Misawa, Hiroaki

2005-02-01

A method of enhancing the efficiency of entangled biphoton sources based on a type II femtosecond spontaneous parametric downconversion (SPDC) process is proposed and implemented experimentally. Enhancement is obtained by mode inversion of one of the SPDC output beams, which allows the beams to overlap completely, thus maximizing the number of SPDC photon pairs with optimum spatiotemporal overlap. By use of this method, biphoton count rates as high as 16 kHz from a single 0.5-mm-long beta-barium borate crystal pumped by second-harmonic radiation from a Ti:sapphire laser were obtained.
Femtosecond laser ablation of dentin and enamel: relationship between laser fluence and ablation efficiency.

PubMed

Chen, Hu; Liu, Jing; Li, Hong; Ge, Wenqi; Sun, Yuchun; Wang, Yong; Lü, Peijun

2015-02-01

The objective was to study the relationship between laser fluence and ablation efficiency of a femtosecond laser with a Gaussian-shaped pulse used to ablate dentin and enamel for prosthodontic tooth preparation. A diode-pumped thin-disk femtosecond laser with wavelength of 1025 nm and pulse width of 400 fs was used for the ablation of dentin and enamel. The laser spot was guided in a line on the dentin and enamel surfaces to form a groove-shaped ablation zone under a series of laser pulse energies. The width and volume of the ablated line were measured under a three-dimensional confocal microscope to calculate the ablation efficiency. Ablation efficiency for dentin reached a maximum value of 0.020 mm3∕J when the laser fluence was set at 6.51 J∕cm2. For enamel, the maximum ablation efficiency was 0.009 mm3∕J at a fluence of 7.59 J∕cm2.Ablation efficiency of the femtosecond laser on dentin and enamel is closely related to the laser fluence and may reach a maximum when the laser fluence is set to an appropriate value. © 2015 Society of Photo-Optical Instrumentation Engineers (SPIE)
Broadband stimulated Raman spectroscopy in the deep ultraviolet region

NASA Astrophysics Data System (ADS)

Kuramochi, Hikaru; Fujisawa, Tomotsumi; Takeuchi, Satoshi; Tahara, Tahei

2017-09-01

We report broadband stimulated Raman measurements in the deep ultraviolet (DUV) region, which enables selective probing of the aromatic amino acid residues inside proteins through the resonance enhancement. We combine the narrowband DUV Raman pump pulse (<10 cm-1) at wavelengths as short as 240 nm and the broadband DUV probe pulse (>1000 cm-1) to realize stimulated Raman measurements covering a >1500 cm-1 spectral window. The stimulated Raman measurements for neat solvents, tryptophan, tyrosine, and glucose oxidase are performed using 240- and 290-nm Raman pump, highlighting the high potential of the DUV stimulated Raman probe for femtosecond time-resolved study of proteins.
Terahertz demultiplexing by a single-shot time-to-space conversion using a film of squarylium dye J aggregates

NASA Astrophysics Data System (ADS)

Furuki, Makoto; Tian, Minquan; Sato, Yasuhiro; Pu, Lyong Sun; Tatsuura, Satoshi; Wada, Osamu

2000-07-01

We applied time-to-space conversion using femtosecond nonlinear-optical response of squarylium-dye (SQ) J-aggregates film. A pump pulse and a train of four probe pulses were illuminated on the same area (10 mm φ) of the film in direction of oblique and normal to the film plane, respectively. Due to the oblique illumination, the pump pulse met probe pulses (interval time: 1 ps) at separate places. The film picked out part of each probe pulse by its transmittance change, which was observed for a transmitted image of spatially separated four lines. Response time of the SQ J aggregates is enough for the single-shot 1 THz demultiplexing.
Optical spectroscopy and ultrafast pump-probe studies on the heavy-fermion compound CePt 2 In 7

DOE PAGES

Chen, R. Y.; Zhang, S. J.; Bauer, E. D.; ...

2016-07-29

We report optical spectroscopy and ultrafast pump-probe measurements on the antiferromagnetic heavy-fermion compound CePt 2 In 7 , a member showing stronger two dimensionality than other compounds in the CeIn 3 -derived heavy-fermion family. Here, we identify clear and typical hybridization spectral structures at low temperature from the two different spectroscopy probes. But, the strength and related energy scale of the hybridization are much weaker and smaller than that in the superconducting compounds CeCoIn 5 and CeIrIn 5 . The features are more similar to observations on the antiferromagnetic compounds CeIn 3 and CeRhIn 5 in the same family. Ourmore » results clearly indicate that the Kondo interaction and hybridizations exist in the antiferromagnetic compounds but with weaker strength.« less
Optomechanical oscillator pumped and probed by optically two isolated photonic crystal cavity systems.

PubMed

Tian, Feng; Sumikura, Hisashi; Kuramochi, Eiichi; Taniyama, Hideaki; Takiguchi, Masato; Notomi, Masaya

2016-11-28

Optomechanical control of on-chip emitters is an important topic related to integrated all-optical circuits. However, there is neither a realization nor a suitable optomechanical structure for this control. The biggest obstacle is that the emission signal can hardly be distinguished from the pump light because of the several orders' power difference. In this study, we designed and experimentally verified an optomechanical oscillation system, in which a lumped mechanical oscillator connected two optically isolated pairs of coupled one-dimensional photonic crystal cavities. As a functional device, the two pairs of coupled cavities were respectively used as an optomechanical pump for the lumped oscillator (cavity pair II, wavelengths were designed to be within a 1.5 μm band) and a modulation target of the lumped oscillator (cavity pair I, wavelengths were designed to be within a 1.2 μm band). By conducting finite element method simulations, we found that the lumped-oscillator-supported configurations of both cavity pairs enhance the optomechanical interactions, especially for higher order optical modes, compared with their respective conventional side-clamped configurations. Besides the desired first-order in-plane antiphase mechanical mode, other mechanical modes of the lumped oscillator were investigated and found to possibly have optomechanical applications with a versatile degree of freedom. In experiments, the oscillator's RF spectra were probed using both cavity pairs I and II, and the results matched those of the simulations. Dynamic detuning of the optical spectrum of cavity pair I was then implemented with a pumped lumped oscillator. This was the first demonstration of an optomechanical lumped oscillator connecting two optically isolated pairs of coupled cavities, whose biggest advantage is that one cavity pair can be modulated with an lumped oscillator without interference from the pump light in the other cavity pair. Thus, the oscillator is a suitable
Effect of an ultrafast laser induced plasma on a relativistic electron beam to determine temporal overlap in pump-probe experiments.

PubMed

Scoby, Cheyne M; Li, R K; Musumeci, P

2013-04-01

In this paper we report on a simple and robust method to measure the absolute temporal overlap of the laser and the electron beam at the sample based on the effect of a laser induced plasma on the electron beam transverse distribution, successfully extending a similar method from keV to MeV electron beams. By pumping a standard copper TEM grid to form the plasma, we gain timing information independent of the sample under study. In experiments discussed here the optical delay to achieve temporal overlap between the pump electron beam and probe laser can be determined with ~1 ps precision. Copyright © 2012 Elsevier B.V. All rights reserved.
Goniometer-based femtosecond X-ray diffraction of mutant 30S ribosomal subunit crystals

DOE PAGES

Dao, E. Han; Sierra, Raymond G.; Laksmono, Hartawan; ...

2015-04-30

In this work, we collected radiation-damage-free data from a set of cryo-cooled crystals for a novel 30S ribosomal subunit mutant using goniometer-based femtosecond crystallography. Crystal quality assessment for these samples was conducted at the X-ray Pump Probe end-station of the Linac Coherent Light Source (LCLS) using recently introduced goniometer-based instrumentation. These 30S subunit crystals were genetically engineered to omit a 26-residue protein, Thx, which is present in the wild-type Thermus thermophilus 30S ribosomal subunit. We are primarily interested in elucidating the contribution of this ribosomal protein to the overall 30S subunit structure. To assess the viability of this study, femtosecondmore » X-ray diffraction patterns from these crystals were recorded at the LCLS during a protein crystal screening beam time. During our data collection, we successfully observed diffraction from these difficult-to-grow 30S ribosomal subunit crystals. Most of our crystals were found to diffract to low resolution, while one crystal diffracted to 3.2 Å resolution. These data suggest the feasibility of pursuing high-resolution data collection as well as the need to improve sample preparation and handling in order to collect a complete radiation-damage-free data set using an X-ray Free Electron Laser.« less
Fabrication of nanofibers reinforced polymer microstructures using femtosecond laser material processing

NASA Astrophysics Data System (ADS)

Alubaidy, Mohammed-Amin

A new method has been introduced for the formation of microfeatures made of nanofibers reinforced polymer, using femtosecond laser material processing. The Femtosecond laser is used for the generation of three-dimensional interweaved nanofibers and the construction of microfeatures, like microchannels and voxels, through multi photon polymerization of nanofiber dispersed polymer resin. A new phenomenon of multiphoton polymerization induced by dual wavelength irradiation was reported for the first time. A significant improvement in the spatial resolution, compared to the two photon absorption (2PA) and the three photon absorption (3PA) processes has been achieved. Conductive polymer microstructures and magnetic polymer microstructures have been fabricated through this method. The mechanical properties of nanofiber reinforced polymer microstructures has been investigated by means of nanoindentation and the volume fraction of the generated nanofibers in the nanocomposite was calculated by using nanoindentation analysis. The results showed significant improvement in strength of the material. The electrical conductivity of the two photon polymerization (TPP) generated microfeatures was measured by a two-probe system at room temperature and the conductivity-temperature relationship was measured at a certain temperature range. The results suggest that the conductive polymer microstructure is reproducible and has a consistent conductivity-temperature relation. The magnetic strength has been characterized using Guassmeter. To demonstrate the potential application of the new fabrication method, a novel class of DNA-functionalized three-dimensional (3D), stand-free, and nanostructured electrodes were fabricated. The developed nanofibrous DNA biosensor has been characterized by cyclic voltammetry with the use of ferrocyanide as an electrochemical redox indicator. Results showed that the probe--target recognition has been improved. This research demonstrated that femtosecond
Double-pulse femtosecond laser peening of aluminum alloy AA5038: Effect of inter-pulse delay on transient optical plume emission and final surface micro-hardness

NASA Astrophysics Data System (ADS)

Ageev, E. I.; Bychenkov, V. Yu.; Ionin, A. A.; Kudryashov, S. I.; Petrov, A. A.; Samokhvalov, A. A.; Veiko, V. P.

2016-11-01

Double-pulse ablative femtosecond laser peening of the AA5038 aluminum alloy surface in the phase explosion regime results in its enhanced microhardness, which monotonously decreases till the initial value versus inter-pulse delay, increasing on a sub-nanosecond timescale. Optical emission spectroscopy of the double-pulse ablative plume reveals the same trend in the yield of the corresponding atomic and ion emission versus inter-pulse delay, enlightening the interaction of the second femtosecond laser pump pulse with the surface and the resulting plume.
Key stages of material expansion in dielectrics upon femtosecond laser ablation revealed by double-color illumination time-resolved microscopy

NASA Astrophysics Data System (ADS)

Garcia-Lechuga, Mario; Solis, Javier; Siegel, Jan

2018-03-01

The physical origin of material removal in dielectrics upon femtosecond laser pulse irradiation (800 nm, 120 fs pulse duration) has been investigated at fluences slightly above ablation threshold. Making use of a versatile pump-probe microscopy setup, the dynamics and different key stages of the ablation process in lithium niobate have been monitored. The use of two different illumination wavelengths, 400 and 800 nm, and a rigorous image analysis combined with theoretical modelling, enables drawing a clear picture of the material excitation and expansion stages. Immediately after excitation, a dense electron plasma is generated. Few picoseconds later, direct evidence of a rarefaction wave propagating into the bulk is obtained, with an estimated speed of 3650 m/s. This process marks the onset of material expansion, which is confirmed by the appearance of transient Newton rings, which dynamically change during the expansion up to approximately 1 ns. Exploring delays up to 15 ns, a second dynamic Newton ring pattern is observed, consistent with the formation of a second ablation front propagating five times slower than the first one.
Widely tunable two-colour seeded free-electron laser source for resonant-pump resonant-probe magnetic scattering

PubMed Central

Ferrari, Eugenio; Spezzani, Carlo; Fortuna, Franck; Delaunay, Renaud; Vidal, Franck; Nikolov, Ivaylo; Cinquegrana, Paolo; Diviacco, Bruno; Gauthier, David; Penco, Giuseppe; Ribič, Primož Rebernik; Roussel, Eleonore; Trovò, Marco; Moussy, Jean-Baptiste; Pincelli, Tommaso; Lounis, Lounès; Manfredda, Michele; Pedersoli, Emanuele; Capotondi, Flavio; Svetina, Cristian; Mahne, Nicola; Zangrando, Marco; Raimondi, Lorenzo; Demidovich, Alexander; Giannessi, Luca; De Ninno, Giovanni; Danailov, Miltcho Boyanov; Allaria, Enrico; Sacchi, Maurizio

2016-01-01

The advent of free-electron laser (FEL) sources delivering two synchronized pulses of different wavelengths (or colours) has made available a whole range of novel pump–probe experiments. This communication describes a major step forward using a new configuration of the FERMI FEL-seeded source to deliver two pulses with different wavelengths, each tunable independently over a broad spectral range with adjustable time delay. The FEL scheme makes use of two seed laser beams of different wavelengths and of a split radiator section to generate two extreme ultraviolet pulses from distinct portions of the same electron bunch. The tunability range of this new two-colour source meets the requirements of double-resonant FEL pump/FEL probe time-resolved studies. We demonstrate its performance in a proof-of-principle magnetic scattering experiment in Fe–Ni compounds, by tuning the FEL wavelengths to the Fe and Ni 3p resonances. PMID:26757813
Ultrafast vibrational dynamics of BH{sub 4}{sup −} ions in liquid and crystalline environments

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

Tyborski, Tobias, E-mail: tyborski@mbi-berlin.de; Costard, Rene; Woerner, Michael

2014-07-21

Ultrafast vibrational dynamics of BH{sub 4}{sup −} ions, the key units in boron hydride materials for hydrogen storage, are studied in diluted polar liquid solution and in NaBH{sub 4} crystallites by femtosecond infrared spectroscopy. Two-color pump-probe experiments reveal v = 1 lifetimes of 3 ps for the asymmetric BH{sub 4}{sup −} stretching mode ν{sub 3} and of 3.6 ps for the asymmetric bending mode ν{sub 4} in the solvent isopropylamine. We provide direct evidence for the BH{sub 4}{sup −} stretching relaxation pathway via the asymmetric bending mode ν{sub 4} by probing the latter after femtosecond excitation of ν{sub 3}. Pump-probemore » traces measured in the crystalline phase show signatures of radiative coupling between the densely packed BH{sub 4}{sup −} oscillators, most clearly manifested in an accelerated subpicosecond depopulation of the v = 1 state of the ν{sub 4} mode. The radiative decay is followed by incoherent vibrational relaxation similar to the liquid phase. The excess energy released in the relaxation processes of the BH{sub 4}{sup −} intramolecular modes is transferred into the environment with thermal pump-probe signals being much more pronounced in the dense solid than in the diluted solution.« less
New resonances from the coherence of Auger and intercoulombic (ICD) processes in the photoionization of endohedral fullerenes

NASA Astrophysics Data System (ADS)

Chakraborty, Himadri; Wise, Jacob; de, Ruma; Javani, Mohammad; Manson, Steve; Madjet, Mohamed

2014-05-01

Considering the photoionization of Ar@C60 , we predict resonant femtosecond decays of both Ar and C60 vacancies through the continua of atom-fullerene hybrid final states. The resulting resonances emerge from the interference between simultaneous autoionizing and intercoulombic decay (ICD) processes. For Ar 3s --> np excitations, these resonances are far stronger than the Ar-to-C60 resonant ICDs, while for C60 excitations they are strikingly larger than the corresponding Auger features. The results indicate the power of hybridization to enhance decay rates, and modify lifetimes and line profiles. These decays are also likely to exist generally in the ionization of molecules, nano-dimers and -polymers, and fullerene onions that support hybridized electrons as well. A jellium based time-dependent local density approximation (TDLDA), with the Leeuwen and Baerends exchange-correlation functional to produce accurate asymptotic behavior, is employed to calculate the dynamical response of the system to the photon field.
Rovibrational photoionization dynamics of methyl and its isotopomers studied by high-resolution photoionization and photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Schulenburg, A. M.; Alcaraz, Ch.; Grassi, G.; Merkt, F.

2006-09-01

High-resolution photoionization and pulsed-field-ionization zero-kinetic-energy photoelectron spectra of CH3, CH2D, CHD2, and CD3 have been recorded in the vicinity of the first adiabatic ionization threshold following single-photon excitation from the ground neutral state using a narrow-bandwidth vacuum-ultraviolet laser. The radicals were produced from the precursor molecules methyl-bromide, methyl-iodide, dimethyl-thioether, acetone, and nitromethane by 193nm excimer photolysis in a quartz capillary and were subsequently cooled to a rotational temperature Trot≈30K in a supersonic expansion. Nitromethane was identified as a particularly suitable photolytic precursor of methyl for studies by photoionization and threshold photoelectron spectroscopy. Thanks to the cold rotational temperature reached in the supersonic expansion, the rotational structure of the threshold ionization spectra could be resolved, and the photoionization dynamics investigated. Rydberg series converging on excited rotational levels of CH3+ could be observed in the range of principal quantum number n =30-50, and both rotational autoionization and predissociation were identified as decay processes in the threshold region. The observed photoionization transitions can be understood in the realm of an orbital model for direct ionization but the intensity distributions can only be fully accounted for if the rotational channel interactions mediated by the quadrupole of the cation are considered. Improved values of the adiabatic ionization thresholds were derived for all isotopomers [CH3: 79356.2(15)cm-1, CH2D: 79338.8(15)cm-1, CHD2: 79319.1(15)cm-1, and CD3: 79296.4(15)cm-1].
Construction of a magnetic bottle spectrometer and its application to pulse duration measurement of X-ray laser using a pump-probe method

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

Namba, S., E-mail: namba@hiroshima-u.ac.jp; Hasegawa, N.; Kishimoto, M.

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

PubMed

Zhang, Jihua; He, Yizhuo; Lam, Billy; Guo, Chunlei

2017-08-21

Femtosecond-laser surface structuring on metals is investigated in real time by both fundamental and second harmonic generation (SHG) signals. The onset of surface modification and its progress can be monitored by both the fundamental and SHG probes. However, the dynamics of femtosecond-laser-induced periodic surface structures (FLIPSSs) formation can only be revealed by SHG but not fundamental because of the higher sensitivity of SHG to structural geometry on metal. Our technique provides a simple and effective way to monitor the surface modification and FLIPSS formation thresholds and allows us to obtain the optimal FLIPSS for SHG enhancement.
Optical pump terahertz probe studies of semiconducting polymers

NASA Astrophysics Data System (ADS)

Cunningham, Paul D.

Optical-pump terahertz-probe spectroscopy (OPTP) has been applied to study charge generation, transport and the evolution of the photo-induced excited states in thin film organic semiconductors, with emphasis on their relevance to photovoltaic technology. In these experiments the response of the photoexcited material to the AC electric field of a terahertz (THz) pulse was measured. From this response, the evolution of the complex conductivity in the far-infrared was monitored. OPTP presents advantages over other techniques by being an all-optical probe of the complex conductivity over nanometer scale distances with sub-picosecond resolution and exhibits particular sensitivity to carrier scattering rates, which typically lay in the THz range. Conductivity models were applied to the extracted conductivity curves in order to determine technologically relevant quantities like the charge carrier mobility and external quantum yield of charge carrier generation. We observed charge carriers generated on a subpicosecond time scale in thin films of polyhexylthiophene (P3HT). Through application of the Drude-Smith model (DSM) over the 0-2 THz band, we determined a room temperature intrinsic mobility of about 30 cm2/Vs. The temperature dependence of the conductivity dynamics showed signs of thermally activated polaron hopping influenced by torsional disorder. Both above and below gap excitation resulted in similar dynamics, showing that the majority of carriers recombine within 1 ps. We were able to observe charge transfer occurring on a sub-ps timescale to the soluble fullerene, PCBM, for both excited states, demonstrating that narrow gap polymers can be blended with PCBM for photovoltaic applications. We observed charge carrier generated on a sub-ps time scale in thin amorphous films of metalated polymers. The time evolution of the conductivity showed that charge carriers recombine and only excitons persist after 100 ps. This characteristic appears to be common to amorphous
Photon-assisted Beam Probes for Low Temperature Plasmas and Installation of Neutral Beam Probe in Helimak

NASA Astrophysics Data System (ADS)

Garcia de Gorordo, Alvaro; Hallock, Gary A.; Kandadai, Nirmala

2008-11-01

The Heavy Ion Beam Probe (HIBP) diagnostic has successfully measured the electric potential in a number of major plasma devices in the fusion community. In contrast to a Langmuir probe, the HIBP measures the exact electric potential rather than the floating potential. It is also has the advantage of being a very nonperturbing diagnostic. We propose a new photon-assisted beam probe technique that would extend the HIBP type of diagnostics into the low temperature plasma regime. We expect this method to probe plasmas colder than 10 eV. The novelty of the proposed diagnostic is a VUV laser that ionizes the probing particle. Excimer lasers produce the pulsed VUV radiation needed. The lasers on the market don't have a short enough wavelength too ionize any ion directly and so we calculate the population density of excited states in a NLTE plasma. These new photo-ionization techniques can take an instantaneous one-dimensional potential measurement of a plasma and are ideal for nonmagnitized plasmas where continuous time resolution is not required. Also the status of the Neutral Beam Probe installation on the Helimak experiment will be presented.
Stochastic Liouville equations for femtosecond stimulated Raman spectroscopy

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

Agarwalla, Bijay Kumar; Ando, Hideo; Dorfman, Konstantin E.

2015-01-14

Electron and vibrational dynamics of molecules are commonly studied by subjecting them to two interactions with a fast actinic pulse that prepares them in a nonstationary state and after a variable delay period T, probing them with a Raman process induced by a combination of a broadband and a narrowband pulse. This technique, known as femtosecond stimulated Raman spectroscopy (FSRS), can effectively probe time resolved vibrational resonances. We show how FSRS signals can be modeled and interpreted using the stochastic Liouville equations (SLE), originally developed for NMR lineshapes. The SLE provide a convenient simulation protocol that can describe complex dynamicsmore » caused by coupling to collective bath coordinates at much lower cost than a full dynamical simulation. The origin of the dispersive features that appear when there is no separation of timescales between vibrational variations and the dephasing time is clarified.« less

Photoionization of Ne8+

NASA Astrophysics Data System (ADS)

Pindzola, M. S.; Abdel-Naby, Sh. A.; Robicheaux, F.; Colgan, J.

2014-05-01

Single and double photoionization cross sections for Ne8+ are calculated using a non-perturbative fully relativistic time-dependent close-coupling method. A Bessel function expansion is used to include both dipole and quadrupole effects in the radiation field interaction and the repulsive interaction between electrons includes both the Coulomb and Gaunt interactions. The fully correlated ground state of Ne8+ is obtained by solving a time-independent inhomogeneous set of close-coupled equations. Propagation of the time-dependent close-coupled equations yields single and double photoionization cross sections for Ne8+ at energies easily accessible at advanced free electron laser facilities. 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.
Photoionization of atoms and molecules. [of hydrogen, helium, and xenon

NASA Technical Reports Server (NTRS)

Samson, J. A. R.

1976-01-01

A literature review on the present state of knowledge in photoionization is presented. Various experimental techniques that have been developed to study photoionization, such as fluorescence and photoelectron spectroscopy, mass spectroscopy, are examined. Various atoms and molecules were chosen to illustrate these techniques, specifically helium and xenon atoms and hydrogen molecules. Specialized photoionization such as in positive and negative ions, excited states, and free radicals is also treated. Absorption cross sections and ionization potentials are also discussed.
Solar photoionization as a loss mechanism of neutral interstellar hydrogen in interplanetary space

NASA Technical Reports Server (NTRS)

Ogawa, H. S.; Wu, C. Y. Robert; Gangopadhyay, P.; Judge, D. L.

1995-01-01

Two primary loss mechanisms of interstellar neutral hydrogen in interplanetary space are resonance charge exchange ionization with solar wind protons and photoionization by solar EUV radiation. The later process has often been neglected since the average photoionization rate has been estimated to be as much as 5 to 10 times smaller than the charge exchange rate. These factors are based on ionization rates from early measurements of solar EUV and solar wind fluxes. Using revised solar EUV and solar wind fluxes measured near the ecliptic plane we have reinvestigated the ionization rates of interplanetary hydrogen. The result of our analysis indicates that indeed the photoionization rate during solar minimum can be smaller than charge exchange by a factor of 5; however, during solar maximum conditions when solar EUV fluxes are high, and solar wind fluxes are low, photoionization can be over 60% of the charge exchange rate at Earth orbit. To obtain an accurate estimate of the importance of photoionization relative to charge exchange, we have included photoionization from both the ground and metastable states of hydrogen. We find, however, that the photoionization from the metastable state does not contribute significantly to the overall photoionization rate.
Surface states in the photoionization of high-quality CdSe core/shell nanocrystals.

PubMed

Li, Shu; Steigerwald, Michael L; Brus, Louis E

2009-05-26

We use electric force microscopy (EFM) to study single nanocrystal photoionization in two classes of high-quality nanocrystals whose exciton luminescence quantum yields approach unity in solution. The CdSe/CdS/ZnS core/shell nanocrystals do not photoionize, while the CdSe/CdS nanocrystals do show substantial photoionization. This verifies the theoretical prediction that the ZnS shell confines the excited electron within the nanocrystal. Despite the high luminescence quantum yield, photoionization varies substantially among the CdSe/CdS nanocrystals. We have studied the nanocrystal photoionization with both UV (396 nm) and green (532 nm) light, and we have found that the magnitude of the charge due to photoionization per absorbed photon is greater for UV excitation than for green excitation. A fraction of the photoionization occurs directly via a "hot electron" process, using trap states that are either on the particle surface, within the ligand sphere, or within the silicon oxide layer. This must occur without relaxation to the thermalized, lowest-energy, emitting exciton. We discuss the occurrence of hot carrier processes that are common to photoionization, luminescence blinking, and the fast transient optical absorption that is associated with multiple exciton generation MEG studies.
Photoionization and heating of a supernova-driven turbulent interstellar medium

NASA Astrophysics Data System (ADS)

Barnes, J. E.; Wood, Kenneth; Hill, Alex S.; Haffner, L. M.

2014-06-01

The diffuse ionized gas (DIG) in galaxies traces photoionization feedback from massive stars. Through three-dimensional photoionization simulations, we study the propagation of ionizing photons, photoionization heating and the resulting distribution of ionized and neutral gas within snapshots of magnetohydrodynamic simulations of a supernova-driven turbulent interstellar medium. We also investigate the impact of non-photoionization heating on observed optical emission line ratios. Inclusion of a heating term which scales less steeply with electron density than photoionization is required to produce diagnostic emission line ratios similar to those observed with the Wisconsin Hα Mapper. Once such heating terms have been included, we are also able to produce temperatures similar to those inferred from observations of the DIG, with temperatures increasing to above 15 000 K at heights |z| ≳ 1 kpc. We find that ionizing photons travel through low-density regions close to the mid-plane of the simulations, while travelling through diffuse low-density regions at large heights. The majority of photons travel small distances (≲100 pc); however some travel kiloparsecs and ionize the DIG.
Total internal reflection-based side-pumping configuration for terawatt ultraviolet amplifier and laser oscillator development

NASA Astrophysics Data System (ADS)

Cadatal-Raduban, Marilou; Pham, Minh Hong; Pham, Duong Van; Bui, Duong Thi Thuy; Yamanoi, Kohei; Takeda, Kohei; Empizo, Melvin John F.; Mui, Luong Viet; Shimizu, Toshihiko; Nguyen, Hung Dai; Sarukura, Nobuhiko; Fukuda, Tsuguo

2018-06-01

A two-side-pumping scheme that is based on total internal reflection in a diamond-cut Ce3+:LiCaAlF6 crystal suitable for the development of an ultraviolet laser and femtosecond amplifier system is proposed. Experimental fluorescence images and lasing results that demonstrate total internal reflection of the excitation beam using this diamond-cut crystal are presented. Calculations for the optimized crystal geometry that facilitate high extraction efficiency and homogeneity of the absorbed excitation beam are also discussed. About 50% increase in extraction efficiency compared to previously reported chirped-pulse femtosecond ultraviolet amplifier operating at 50-GW peak power is expected using this total internal reflection-based two-side-pumping configuration and a diamond-cut Ce3+:LiCaAlF6 crystal with a geometry of {φ _1} = 103°, {φ _2} = {φ _4} = 82°, {φ _3} = 93°, a length of 1.23 cm, a height of 2 cm, and an absorption coefficient of 1.5 cm-1. Our results can be used as a guide during the crystal growth process by providing the appropriate crystal geometry and size for a particular absorption coefficient to achieve high extraction efficiency. With the appropriate crystal combined with multiple-beam pumping afforded by the side-pumping scheme, the development of an all-solid-state ultraviolet laser operating at terawatt level would be within reach.
Photoionization research on atomic beams. 2: The photoionization cross section of atomic oxygen

NASA Technical Reports Server (NTRS)

Comes, F. J.; Speier, F.; Elzer, A.

1982-01-01

An experiment to determine the absolute value of the photo-ionization cross section of atomic oxygen is described. The atoms are produced in an electrical discharge in oxygen gas with 1% hydrogen added. In order to prevent recombination a crossed beam technique is employed. The ions formed are detected by a time-of-flight mass spectrometer. The concentration of oxygen atoms in the beam is 57%. The measured photoionization cross section of atomic oxygen is compared with theoretical data. The results show the participation of autoionization processes in ionization. The cross section at the autoionizing levels detected is considerably higher than the absorption due to the unperturbed continuum. Except for wavelengths where autoionization occurs, the measured ionization cross section is in fair agreement with theory. This holds up to 550 A whereas for shorter wavelengths the theoretical values are much higher.
Neuroscience imaging enabled by new highly tunable and high peak power femtosecond lasers

NASA Astrophysics Data System (ADS)

Hakulinen, T.; Klein, J.

2017-02-01

Neuroscience applications benefit from recent developments in industrial femtosecond laser technology. New laser sources provide several megawatts of peak power at wavelength of 1040 nm, which enables simultaneous optogenetics photoactivation of tens or even hundreds of neurons using red shifted opsins. Another recent imaging trend is to move towards longer wavelengths, which would enable access to deeper layers of tissue due to lower scattering and lower absorption in the tissue. Femtosecond lasers pumping a non-collinear optical parametric amplifier (NOPA) enable the access to longer wavelengths with high peak powers. High peak powers of >10 MW at 1300 nm and 1700 nm allow effective 3-photon excitation of green and red shifted calcium indicators respectively and access to deeper, sub-cortex layers of the brain. Early results include in vivo detection of spontaneous activity in hippocampus within an intact mouse brain, where neurons express GCaMP6 activated in a 3-photon process at 1320 nm.
Serial femtosecond crystallography: A revolution in structural biology.

PubMed

Martin-Garcia, Jose M; Conrad, Chelsie E; Coe, Jesse; Roy-Chowdhury, Shatabdi; Fromme, Petra

2016-07-15

Macromolecular crystallography at synchrotron sources has proven to be the most influential method within structural biology, producing thousands of structures since its inception. While its utility has been instrumental in progressing our knowledge of structures of molecules, it suffers from limitations such as the need for large, well-diffracting crystals, and radiation damage that can hamper native structural determination. The recent advent of X-ray free electron lasers (XFELs) and their implementation in the emerging field of serial femtosecond crystallography (SFX) has given rise to a remarkable expansion upon existing crystallographic constraints, allowing structural biologists access to previously restricted scientific territory. SFX relies on exceptionally brilliant, micro-focused X-ray pulses, which are femtoseconds in duration, to probe nano/micrometer sized crystals in a serial fashion. This results in data sets comprised of individual snapshots, each capturing Bragg diffraction of single crystals in random orientations prior to their subsequent destruction. Thus structural elucidation while avoiding radiation damage, even at room temperature, can now be achieved. This emerging field has cultivated new methods for nanocrystallogenesis, sample delivery, and data processing. Opportunities and challenges within SFX are reviewed herein. Published by Elsevier Inc.
Sensitivity of nonlinear photoionization to resonance substructure in collective excitation

PubMed Central

Mazza, T.; Karamatskou, A.; Ilchen, M.; Bakhtiarzadeh, S.; Rafipoor, A. J.; O'Keeffe, P.; Kelly, T. J.; Walsh, N.; Costello, J. T.; Meyer, M.; Santra, R.

2015-01-01

Collective behaviour is a characteristic feature in many-body systems, important for developments in fields such as magnetism, superconductivity, photonics and electronics. Recently, there has been increasing interest in the optically nonlinear response of collective excitations. Here we demonstrate how the nonlinear interaction of a many-body system with intense XUV radiation can be used as an effective probe for characterizing otherwise unresolved features of its collective response. Resonant photoionization of atomic xenon was chosen as a case study. The excellent agreement between experiment and theory strongly supports the prediction that two distinct poles underlie the giant dipole resonance. Our results pave the way towards a deeper understanding of collective behaviour in atoms, molecules and solid-state systems using nonlinear spectroscopic techniques enabled by modern short-wavelength light sources. PMID:25854939
Sensitivity of nonlinear photoionization to resonance substructure in collective excitation

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

Mazza, T.; Karamatskou, A.; Ilchen, M.

Collective behaviour is a characteristic feature in many-body systems, important for developments in fields such as magnetism, superconductivity, photonics and electronics. Recently, there has been increasing interest in the optically nonlinear response of collective excitations. Here we demonstrate how the nonlinear interaction of a many-body system with intense XUV radiation can be used as an effective probe for characterizing otherwise unresolved features of its collective response. Resonant photoionization of atomic xenon was chosen as a case study. The excellent agreement between experiment and theory strongly supports the prediction that two distinct poles underlie the giant dipole resonance. Our results pavemore » the way towards a deeper understanding of collective behaviour in atoms, molecules and solid-state systems using nonlinear spectroscopic techniques enabled by modern short-wavelength light sources.« less
Time-dependent local density approximation study of iodine photoionization delay

NASA Astrophysics Data System (ADS)

Magrakvelidze, Maia; Chakraborty, Himadri

2017-04-01

We investigate dipole quantum phases and Wigner-Smith (WS) time delays in the photoionization of iodine using Kohn-Sham time-dependent local density approximation (TDLDA) with the Leeuwen and Baerends exchange-correlation functional. Study of the effects of electron correlations on the absolute as well as relative delays in emissions from both valence 5p and 5s, and core 4d, 4p and 4s levels has been carried out. Particular emphasis is paid to unravel the role of correlations to induce structures in the delay as a function of energy at resonances and Cooper minima. The results should encourage attosecond measurements of iodine photoemission and probe the WS-temporal landscape of an open-shell atomic system. This work was supported by the U.S. National Science Foundation.
Sensitivity of nonlinear photoionization to resonance substructure in collective excitation

DOE PAGES

Mazza, T.; Karamatskou, A.; Ilchen, M.; ...

2015-04-09

Collective behaviour is a characteristic feature in many-body systems, important for developments in fields such as magnetism, superconductivity, photonics and electronics. Recently, there has been increasing interest in the optically nonlinear response of collective excitations. Here we demonstrate how the nonlinear interaction of a many-body system with intense XUV radiation can be used as an effective probe for characterizing otherwise unresolved features of its collective response. Resonant photoionization of atomic xenon was chosen as a case study. The excellent agreement between experiment and theory strongly supports the prediction that two distinct poles underlie the giant dipole resonance. Our results pavemore » the way towards a deeper understanding of collective behaviour in atoms, molecules and solid-state systems using nonlinear spectroscopic techniques enabled by modern short-wavelength light sources.« less
Near-Resonant Raman Amplification in the Rotational Quantum Wave Packets of Nitrogen Molecular Ions Generated by Strong Field Ionization

NASA Astrophysics Data System (ADS)

Liu, Zhaoxiang; Yao, Jinping; Chen, Jinming; Xu, Bo; Chu, Wei; Cheng, Ya

2018-02-01

The generation of laserlike narrow bandwidth emissions from nitrogen molecular ions (N2+ ) generated in intense near- and mid infrared femtosecond laser fields has aroused much interest because of the mysterious physics underlying such a phenomenon. Here, we perform a pump-probe measurement on the nonlinear interaction of rotational quantum wave packets of N2+ generated in midinfrared (e.g., at a wavelength centered at 1580 nm) femtosecond laser fields with an ultrashort probe pulse whose broad spectrum overlaps both P - and R -branch rotational transition lines between the electronic states N2+(B2Σu+,v'=0 ) and N2+(X2Σg+,v =0 ) . The results indicate the occurrence of highly efficient near-resonant stimulated Raman scattering in the quantum wave packets of N2+ ions generated in strong laser fields in the midinfrared region, of which the underlying mechanism is different from that of the air lasers generated in atmospheric environment when pumping with 800 nm intense pulses.
Nonlinear femtosecond near infrared laser structuring in oxide glasses

NASA Astrophysics Data System (ADS)

Royon, Arnaud

nonlinear third-order susceptibility properties have been measured. Moreover, the structuring of fused silica at the subwavelength scale into "nanogratings" is observed and the form of birefringence induced by these structures is discussed. In addition to the fused silica samples, several oxide glasses presenting very distinct chemical compositions have been studied. A sodium-borophosphate glass containing niobium oxide exhibits micro-cracks and nano-crystallites following irradiation. A silicate glass with or without a silver component reveals fluorescent rings or "nanograting" structures. A zinc phosphate glass containing silver also presents fluorescent ring structures, with a size of the order of 80 nm, well below the diffraction limit. Pump-probe microscope techniques have been performed on this glass to investigate the laser-glass interaction. The absorption mechanism is determined to be four-photon absorption. The generated free electron density is ˜ 1017 cm-3, which suggests the conclusion that an electron gas rather than a plasma is formed during the laser irradiation.
Picosecond transient backward stimulated Raman scattering and pumping of femtosecond dye lasers

NASA Astrophysics Data System (ADS)

Arrivo, Steven M.; Spears, Kenneth G.; Sipior, Jeffrey

1995-02-01

We report studies of transient, backward stimulated, Raman scattering (TBSRS) in solvents with a 10 Hz, 27 ps, 532 nm pump laser. The TBSRS effect was used to create pulses at 545 nm and 630 nm with durations of 2-3 ps and 5-10 μJ of energy. The duration, energy and fluctuations of the Raman pulse were studied as a function of pump energy and focal parameters. A 5 μJ Raman pulse was amplified in either a Raman amplifier or two stage dye amplifier to 1 mJ levels. A 545 nm pulse of 3 ps duration was generated in CCl 4 and was then used to pump a short cavity dye laser (SCDL). The SCDL oscillator and a 5 stage dye amplifier provided a pulse of 700 fs and 400 μJ that was tunable near 590 nm.
Laser-pump/X-ray-probe experiments with electrons ejected from a Cu(111) target: space-charge acceleration.

PubMed

Schiwietz, G; Kühn, D; Föhlisch, A; Holldack, K; Kachel, T; Pontius, N

2016-09-01

A comprehensive investigation of the emission characteristics for electrons induced by X-rays of a few hundred eV at grazing-incidence angles on an atomically clean Cu(111) sample during laser excitation is presented. Electron energy spectra due to intense infrared laser irradiation are investigated at the BESSY II slicing facility. Furthermore, the influence of the corresponding high degree of target excitation (high peak current of photoemission) on the properties of Auger and photoelectrons liberated by a probe X-ray beam is investigated in time-resolved pump and probe measurements. Strong electron energy shifts have been found and assigned to space-charge acceleration. The variation of the shift with laser power and electron energy is investigated and discussed on the basis of experimental as well as new theoretical results.
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.
Terahertz Optical Gain Based on Intersubband Transitions in Optically-Pumped Semiconductor Quantum Wells: Coherent Pumped-Probe Interactions

NASA Technical Reports Server (NTRS)

Liu, Ansheng; Ning, Cun-Zheng

1999-01-01

Terahertz optical gain due to intersubband transitions in optically-pumped semiconductor quantum wells (QW's) is calculated nonperturbatively. We solve the pump- field-induced nonequilibrium distribution function for each subband of the QW system from a set of rate equations that include both intrasubband and intersubband relaxation processes. The gain arising from population inversion and stimulated Raman processes is calculated in a unified manner. We show that the coherent pump and signal wave interactions contribute significantly to the THz gain. Because of the optical Stark effect and pump-induced population redistribution, optical gain saturation at larger pump intensities is predicted.
Coherent Acoustic Vibration of Metal Nanoshells

NASA Astrophysics Data System (ADS)

Guillon, C.; Langot, P.; Del Fatti, N.; Vallée, F.; Kirakosyan, A. S.; Shahbazyan, T. V.; Cardinal, T.; Treguer, M.

2007-01-01

Using time-resolved pump-probe spectroscopy we have performed the first investigation of the vibrational modes of gold nanoshells. The fundamental isotropic mode launched by a femtosecond pump pulse manifests itself in a pronounced time-domain modulation of the differential transmission probed at the frequency of nanoshell surface plasmon resonance. The modulation amplitude is significantly stronger and the period is longer than in a gold nanoparticle of the same overall size, in agreement with theoretical calculations. This distinct acoustical signature of nanoshells provides a new and efficient method for identifying these versatile nanostructures and for studying their mechanical and structural properties.

Measurement and control of the frequency chirp rate of high-order harmonic pulses

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

Mauritsson, J.; Johnsson, P.; Lopez-Martens, R.

2004-08-01

We measure the chirp rate of harmonics 13 to 23 in argon by cross correlation with a 12 femtosecond probe pulse. Under low ionization conditions, we directly measure the negative chirp due to the atomic dipole phase, and show that an additional chirp on the pump pulse is transferred to the qth harmonic as q times the fundamental chirp. Our results are in accord with simulations using the experimentally measured 815 nm pump and probe pulses. The ability to measure and manipulate the harmonic chirp rate is essential for the characterization and optimization of attosecond pulse trains.
DOE Office of Scientific and Technical Information (OSTI.GOV)

Ingold, G., E-mail: gerhard.ingold@psi.ch; Rittmann, J., E-mail: jochen.rittmann@psi.ch; Beaud, P.

The ESB instrument at the SwissFEL ARAMIS hard X-ray free electron laser is designed to perform pump-probe experiments in condensed matter and material science employing photon-in and photon-out techniques. It includes a femtosecond optical laser system to generate a variety of pump beams, a X-ray optical scheme to tailor the X-ray probe beam, shot-to-shot diagnostics to monitor the X-ray intensity and arrival time, and two endstations operated at a single focus position that include multi-purpose sample environments and 2D pixel detectors for data collection.
Measurements of sound velocity in iron-nickel alloys by femtosecond laser pulses in a diamond anvil cell

NASA Astrophysics Data System (ADS)

Wakamatsu, Tatsuya; Ohta, Kenji; Yagi, Takashi; Hirose, Kei; Ohishi, Yasuo

2018-01-01

By comparing the seismic wave velocity profile in the Earth with laboratory data of the sound velocity of iron alloys, we can infer the chemical composition of materials in the Earth's core. The sound velocity of pure iron (Fe) has been sufficiently measured using various techniques, while experimental study on the sound velocity of iron-nickel (Fe-Ni) alloys is limited. Here, we measured longitudinal wave velocities of hexagonal-close-packed (hcp) structured Fe up to 29 GPa, Fe-5 wt% Ni, and Fe-15 wt% Ni up to 64 GPa via a combination of the femtosecond pulse laser pump-probe technique and a diamond anvil cell at room temperature condition. We found that the effect of Ni on the sound velocity of an Fe-based alloy is weaker than that determined by previous experimental study. In addition, we obtained the parameters of Birch's law to be V P = 1146(57)ρ - 3638(567) for Fe-5 wt% Ni and V P = 1141(45)ρ- 3808(446) for Fe-15 wt% Ni, respectively, where V P is longitudinal wave velocity (m/s) and ρ is density (g/cm3).
Measurements of sound velocity in iron-nickel alloys by femtosecond laser pulses in a diamond anvil cell

NASA Astrophysics Data System (ADS)

Wakamatsu, Tatsuya; Ohta, Kenji; Yagi, Takashi; Hirose, Kei; Ohishi, Yasuo

2018-06-01

By comparing the seismic wave velocity profile in the Earth with laboratory data of the sound velocity of iron alloys, we can infer the chemical composition of materials in the Earth's core. The sound velocity of pure iron (Fe) has been sufficiently measured using various techniques, while experimental study on the sound velocity of iron-nickel (Fe-Ni) alloys is limited. Here, we measured longitudinal wave velocities of hexagonal-close-packed (hcp) structured Fe up to 29 GPa, Fe-5 wt% Ni, and Fe-15 wt% Ni up to 64 GPa via a combination of the femtosecond pulse laser pump-probe technique and a diamond anvil cell at room temperature condition. We found that the effect of Ni on the sound velocity of an Fe-based alloy is weaker than that determined by previous experimental study. In addition, we obtained the parameters of Birch's law to be V P = 1146(57) ρ - 3638(567) for Fe-5 wt% Ni and V P = 1141(45) ρ- 3808(446) for Fe-15 wt% Ni, respectively, where V P is longitudinal wave velocity (m/s) and ρ is density (g/cm3).
Blue two-photon fluorescence metal cluster probe precisely marking cell nuclei of two cell lines.

PubMed

Wang, Yaling; Cui, Yanyan; Liu, Ru; Wei, Yueteng; Jiang, Xinglu; Zhu, Huarui; Gao, Liang; Zhao, Yuliang; Chai, Zhifang; Gao, Xueyun

2013-11-25

A bifunctional peptide was designed to in situ reduce Cu ions and anchor a Cu cluster. The peptide-Cu cluster probe, mainly composed of Cu14, emitted blue two-photon fluorescence under femtosecond laser excitation. Most important, the probe can specifically mark the nuclei of HeLa and A549 cells, respectively.
Investigating vibrational relaxation in cyanide-bridged transition metal mixed-valence complexes using two-dimensional infrared and infrared pump-probe spectroscopies

PubMed Central

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

2016-01-01

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

PubMed

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

2016-03-01

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

NASA Technical Reports Server (NTRS)

Zhang, Zhengyu; Kuo, Szu-Cherng; Klemm, R. Bruce; Monks, Paul S.; Stief, Louis J.

1994-01-01

Photoionization efficiency spectra of FO were measured over the wavelength range 80.0-100.0 nm and in the ionization threshold region, 94.0-100.0 nm, using a discharge flow-photoionization mass spectrometer apparatus coupled to a synchrotron radiation source. FO was generated by the reaction of F2P atoms with NO3 and via a F2O2 discharge. A value of 12.78 +/- 0.03 eV was obtained for the adiabatic ionization energy of FO from photoion thresholds which corresponds to FO(+)(X 3 Sigma -) from FO(X 2 Pi i). These results, which are the first to be obtained by direct Photo-ionization mass spectrometry (PIMS) measurements, corroborate those of a photoelectron spectroscopy (PES) study; however, the ionization energy determined here is free from interferences due to other species which complicated the PES measurement. A value of 109.5 +/- 8.0 kJ/mol for Delta f H 0 298(FO) is computed from the present value of IE(FO) and a previous appearance energy measurement, and a value for the proton affinity of FO is calculated to be 511.5 +/- 10.0 kJ/mol.
Ti:sapphire-pumped diamond Raman laser with sub-100-fs pulse duration.

PubMed

Murtagh, Michelle; Lin, Jipeng; Mildren, Richard P; Spence, David J

2014-05-15

We report a synchronously pumped femtosecond diamond Raman laser operating at 895 nm with a 33% slope efficiency. Pumped using a mode-locked Ti:sapphire laser at 800 nm with a duration of 170 fs, the bandwidth of the Stokes output is broadened and chirped to enable subsequent pulse compression to 95 fs using a prism pair. Modeling results indicate that self-phase modulation drives the broadening of the Stokes spectrum in this highly transient laser. Our results demonstrate the potential for Raman conversion to extend the wavelength coverage and pulse shorten Ti:sapphire lasers.
Dissociative photoionization of 1,3-butadiene: experimental and theoretical insights.

PubMed

Fang, Wenzheng; Gong, Lei; Zhang, Qiang; Shan, Xiaobin; Liu, Fuyi; Wang, Zhenya; Sheng, Liusi

2011-05-07

The vacuum-ultraviolet photoionization and dissociative photoionization of 1,3-butadiene in a region ∼8.5-17 eV have been investigated with time-of-flight photoionization mass spectrometry using tunable synchrotron radiation. The adiabatic ionization energy of 1,3-butadiene and appearance energies for its fragment ions, C(4)H(5)(+), C(4)H(4)(+), C(4)H(3)(+), C(3)H(3)(+), C(2)H(4)(+), C(2)H(3)(+), and C(2)H(2)(+), are determined to be 9.09, 11.72, 13.11, 15.20, 11.50, 12.44, 15.15, and 15.14 eV, respectively, by measurements of photoionization efficiency spectra. Ab initio molecular orbital calculations have been performed to investigate the reaction mechanism of dissociative photoionization of 1,3-butadiene. On the basis of experimental and theoretical results, seven dissociative photoionization channels are proposed: C(4)H(5)(+) + H, C(4)H(4)(+) + H(2), C(4)H(3)(+) + H(2) + H, C(3)H(3)(+) + CH(3), C(2)H(4)(+) + C(2)H(2), C(2)H(3)(+) + C(2)H(2) + H, and C(2)H(2)(+) + C(2)H(2) + H(2). Channel C(3)H(3)(+) + CH(3) is found to be the dominant one, followed by C(4)H(5)(+) + H and C(2)H(4)(+) + C(2)H(2). The majority of these channels occur via isomerization prior to dissociation. Transition structures and intermediates for those isomerization processes were also determined.
Vacuum ultraviolet photoionization cross section of the hydroxyl radical.

PubMed

Dodson, Leah G; Savee, John D; Gozem, Samer; Shen, Linhan; Krylov, Anna I; Taatjes, Craig A; Osborn, David L; Okumura, Mitchio

2018-05-14

The absolute photoionization spectrum of the hydroxyl (OH) radical from 12.513 to 14.213 eV was measured by multiplexed photoionization mass spectrometry with time-resolved radical kinetics. Tunable vacuum ultraviolet (VUV) synchrotron radiation was generated at the Advanced Light Source. OH radicals were generated from the reaction of O( 1 D) + H 2 O in a flow reactor in He at 8 Torr. The initial O( 1 D) concentration, where the atom was formed by pulsed laser photolysis of ozone, was determined from the measured depletion of a known concentration of ozone. Concentrations of OH and O( 3 P) were obtained by fitting observed time traces with a kinetics model constructed with literature rate coefficients. The absolute cross section of OH was determined to be σ(13.436 eV) = 3.2 ± 1.0 Mb and σ(14.193 eV) = 4.7 ± 1.6 Mb relative to the known cross section for O( 3 P) at 14.193 eV. The absolute photoionization spectrum was obtained by recording a spectrum at a resolution of 8 meV (50 meV steps) and scaling to the single-energy cross sections. We computed the absolute VUV photoionization spectrum of OH and O( 3 P) using equation-of-motion coupled-cluster Dyson orbitals and a Coulomb photoelectron wave function and found good agreement with the observed absolute photoionization spectra.
Vacuum ultraviolet photoionization cross section of the hydroxyl radical

NASA Astrophysics Data System (ADS)

Dodson, Leah G.; Savee, John D.; Gozem, Samer; Shen, Linhan; Krylov, Anna I.; Taatjes, Craig A.; Osborn, David L.; Okumura, Mitchio

2018-05-01

The absolute photoionization spectrum of the hydroxyl (OH) radical from 12.513 to 14.213 eV was measured by multiplexed photoionization mass spectrometry with time-resolved radical kinetics. Tunable vacuum ultraviolet (VUV) synchrotron radiation was generated at the Advanced Light Source. OH radicals were generated from the reaction of O(1D) + H2O in a flow reactor in He at 8 Torr. The initial O(1D) concentration, where the atom was formed by pulsed laser photolysis of ozone, was determined from the measured depletion of a known concentration of ozone. Concentrations of OH and O(3P) were obtained by fitting observed time traces with a kinetics model constructed with literature rate coefficients. The absolute cross section of OH was determined to be σ(13.436 eV) = 3.2 ± 1.0 Mb and σ(14.193 eV) = 4.7 ± 1.6 Mb relative to the known cross section for O(3P) at 14.193 eV. The absolute photoionization spectrum was obtained by recording a spectrum at a resolution of 8 meV (50 meV steps) and scaling to the single-energy cross sections. We computed the absolute VUV photoionization spectrum of OH and O(3P) using equation-of-motion coupled-cluster Dyson orbitals and a Coulomb photoelectron wave function and found good agreement with the observed absolute photoionization spectra.
Vacuum Ultraviolet Photoionization of Complex Chemical Systems

DOE PAGES

Kostko, Oleg; Bandyopadhyay, Biswajit; Ahmed, Musahid

2016-02-24

Tunable vacuum ultraviolet (VUV) radiation coupled to mass spectrometry is applied to the study of complex chemical systems in this paper. The identification of novel reactive intermediates and radicals is revealed in flame, pulsed photolysis, and pyrolysis reactors, leading to the elucidation of spectroscopy, reaction mechanisms, and kinetics. Mass-resolved threshold photoelectron photoion coincidence measurements provide unprecedented access to vibrationally resolved spectra of free radicals present in high-temperature reactors. Photoionization measurements in water clusters, nucleic acid base dimers, and their complexes with water provide signatures of proton transfer in hydrogen-bonded and π-stacked systems. Experimental and theoretical methods to track ion–molecule reactionsmore » and fragmentation pathways in intermolecular and intramolecular hydrogen-bonded systems in sugars and alcohols are described. Photoionization of laser-ablated molecules, clusters, and their reaction products inform thermodynamics and spectroscopy that are relevant to astrochemistry and catalysis. Finally, new directions in coupling VUV radiation to interrogate complex chemical systems are discussed.« less
Photoionization of Se+ and Se2+ Ions: Experiment and Theory

NASA Astrophysics Data System (ADS)

Esteves, D. A.; Sterling, N. C.; Alna'Washi, Ghassan; Aguilar, A.; Kilcoyne, A. L. D.; Balance, C. P.; Norrington, P. H.; McLaughlin, B. M.

2007-06-01

The determination of elemental abundances in astrophysical nebulae are highly dependent on the accuracy of the available atomic data. Numerical simulations show that derived Se abundances in ionized nebulae can be uncertain by factors of two or more from atomic data uncertainties alone. Of these uncertainties, photoionization cross section data are the most important, particularly in the near threshold region of the valence shell. Absolute photoionization cross sections for Se^+ and Se^2+ ions near their thresholds have been measured at the Advanced Light Source in Berkeley, using the merged beams photo-ion technique. Theoretical photoionization cross sections calculations were performed for both of these Se ions using the state-of-the-art fully relativistic Dirac R-matrix code (DARC). The calculations show encouraging agreement with the experimental measurements. A more comprehensive set of results will be presented at the meeting.
Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

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

Boguslavskiy, Andrey E.; Schalk, Oliver; Gador, Niklas

The ultrafast excited state dynamics of the smallest polyene, trans-1,3-butadiene, were studied by femtosecond time-resolved photoelectron-photoion coincidence (TRPEPICO) spectroscopy. The evolution of the excited state wavepacket, created by pumping the bright 1B u (ππ*) electronic state at its origin of 216 nm, is projected via one- and two-photon ionization at 267 nm onto several ionization continua. The results are interpreted in terms of Koopmans’ correlations and Franck-Condon factors for the excited and cationic states involved. The known predissociative character of the cation excited states is utilized to assign photoelectron bands to specific continua using TRPEPICO spectroscopy. This permits us tomore » report the direct observation of the famously elusive S 1(2 1A g) dark electronic state during the internal conversion of trans 1,3-butadiene. Our phenomenological analysis permits the spectroscopic determination of several important time constants. We report the overall decay lifetimes of the 1 1B u and 2 1A g states and observe the re-appearance of the hot ground state molecule. We argue that the apparent dephasing time of the S 2(1 1B u) state, which leads to the extreme breadth of the absorption spectrum, is principally due to large amplitude torsional motion on the 1B u surface in conjunction with strong non-adiabatic couplings via conical intersections, whereupon nuclear wavepacket revivals to the initial Franck-Condon region become effectively impossible. Lastly, in Paper II [W. J. Glover et al., J. Chem. Phys. 148, 164303 (2018)], ab initio multiple spawning is used for on-the-fly computations of the excited state non-adiabatic wavepacket dynamics and their associated TRPEPICO observables, allowing for direct comparisons of experiment with theory.« less
Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

DOE PAGES

Boguslavskiy, Andrey E.; Schalk, Oliver; Gador, Niklas; ...

2018-04-27

The ultrafast excited state dynamics of the smallest polyene, trans-1,3-butadiene, were studied by femtosecond time-resolved photoelectron-photoion coincidence (TRPEPICO) spectroscopy. The evolution of the excited state wavepacket, created by pumping the bright 1B u (ππ*) electronic state at its origin of 216 nm, is projected via one- and two-photon ionization at 267 nm onto several ionization continua. The results are interpreted in terms of Koopmans’ correlations and Franck-Condon factors for the excited and cationic states involved. The known predissociative character of the cation excited states is utilized to assign photoelectron bands to specific continua using TRPEPICO spectroscopy. This permits us tomore » report the direct observation of the famously elusive S 1(2 1A g) dark electronic state during the internal conversion of trans 1,3-butadiene. Our phenomenological analysis permits the spectroscopic determination of several important time constants. We report the overall decay lifetimes of the 1 1B u and 2 1A g states and observe the re-appearance of the hot ground state molecule. We argue that the apparent dephasing time of the S 2(1 1B u) state, which leads to the extreme breadth of the absorption spectrum, is principally due to large amplitude torsional motion on the 1B u surface in conjunction with strong non-adiabatic couplings via conical intersections, whereupon nuclear wavepacket revivals to the initial Franck-Condon region become effectively impossible. Lastly, in Paper II [W. J. Glover et al., J. Chem. Phys. 148, 164303 (2018)], ab initio multiple spawning is used for on-the-fly computations of the excited state non-adiabatic wavepacket dynamics and their associated TRPEPICO observables, allowing for direct comparisons of experiment with theory.« less
Continuous wave channel waveguide lasers in Nd:LuVO4 fabricated by direct femtosecond laser writing.

PubMed

Ren, Yingying; Dong, Ningning; Macdonald, John; Chen, Feng; Zhang, Huaijin; Kar, Ajoy K

2012-01-30

Buried channel waveguides in Nd:LuVO<4 were fabricated by femtosecond laser writing with the double-line technique. The photoluminescence properties of the bulk materials were found to be well preserved within the waveguide core region. Continuous-wave laser oscillation at 1066.4 nm was observed from the waveguide under ~809 nm optical excitation, with the absorbed pump power at threshold and laser slope efficiency of 98 mW and 14%, respectively.
Carrier dynamics in silicon nanowires studied using optical-pump terahertz-probe spectroscopy

NASA Astrophysics Data System (ADS)

Beaudoin, Alexandre; Salem, Bassem; Baron, Thierry; Gentile, Pascal; Morris, Denis

2014-03-01

The advance of non-contact measurements involving pulsed terahertz radiation presents great interests for characterizing electrical properties of a large ensemble of nanowires. In this work, N-doped and undoped silicon nanowires (SiNWs) grown by chemical vapour deposition (CVD) on quartz substrate were characterized using optical-pump terahertz probe (OPTP) transmission experiments. Our results show that defects and ionized impurities introduced by N-doping the CVD-grown SiNWs tend to reduce the photoexcited carrier lifetime and degrade their conductivity properties. Capture mechanisms by the surface trap states play a key role on the photocarrier dynamics in theses small diameters' (~100 nm) SiNWs and the doping level is found to alter this dynamics. We propose convincing capture and recombination scenarios that explain our OPTP measurements. Fits of our photoconductivity data curves, from 0.5 to 2 THz, using a Drude-plasmon conductivity model allow determining photocarrier mobility values of 190 and 70 cm2/V .s, for the undoped and N-doped NWs samples, respectively.
The X-ray Pump–Probe instrument at the Linac Coherent Light Source

DOE PAGES

Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco; ...

2015-04-21

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.
Dual-wavelength waveguide lasers at 1064 and 1079 nm in Nd:YAP crystal by direct femtosecond laser writing.

PubMed

Nie, Weijie; Cheng, Chen; Jia, Yuechen; Romero, Carolina; Vázquez de Aldana, Javier R; Chen, Feng

2015-05-15

Low-loss depressed cladding waveguides have been produced in Nd:YAP laser crystal by using direct femtosecond laser writing. Under optical pump at 812 nm at room temperature, continuous-wave simultaneous dual-wavelength laser oscillations at 1064 and 1079 nm, both along TM polarization, have been realized in the waveguiding structures. It has been found that, with the variation of pump polarization, the intensity ratio of 1064 and 1079 nm emissions varies periodically, while the polarization of output dual-wavelength laser remains unchanged. The maximum output power achieved for the Nd:YAP waveguide lasers is ∼200 mW with a slope efficiency of 33.4%.

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