Dual time-resolved temperature-jump fluorescence and infrared spectroscopy for the study of fast protein dynamics.

Science.gov (United States)

Davis, Caitlin M; Reddish, Michael J; Dyer, R Brian

2017-05-05

Time-resolved temperature-jump (T-jump) coupled with fluorescence and infrared (IR) spectroscopy is a powerful technique for monitoring protein dynamics. Although IR spectroscopy of the polypeptide amide I mode is more technically challenging, it offers complementary information because it directly probes changes in the protein backbone, whereas, fluorescence spectroscopy is sensitive to the environment of specific side chains. With the advent of widely tunable quantum cascade lasers (QCL) it is possible to efficiently probe multiple IR frequencies with high sensitivity and reproducibility. Here we describe a dual time-resolved T-jump fluorescence and IR spectrometer and its application to study protein folding dynamics. A Q-switched Ho:YAG laser provides the T-jump source for both time-resolved IR and fluorescence spectroscopy, which are probed by a QCL and Ti:Sapphire laser, respectively. The Ho:YAG laser simultaneously pumps the time-resolved IR and fluorescence spectrometers. The instrument has high sensitivity, with an IR absorbance detection limit of jump induced difference spectrum from 50ns to 0.5ms. This study demonstrates the power of the dual time-resolved T-jump fluorescence and IR spectroscopy to resolve complex folding mechanisms by complementary IR absorbance and fluorescence measurements of protein dynamics. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultra-broadband THz time-domain spectroscopy of common polymers using THz air photonics

DEFF Research Database (Denmark)

D’Angelo, Francesco; Mics, Zoltán; Bonn, Mischa

2014-01-01

-domain spectrometer employing air-photonics for the generation and detection of single-cycle sub-50 fs THz transients. The time domain measurements provide direct access to both the absorption and refractive index spectra. The polymers LDPE and TOPAS® demonstrate negligible absorption and spectrally-flat refractive...... index across the entire spectroscopy window, revealing the high potential of these polymers for applications in THz photonics such as ultra-broadband polymer-based dielectric mirrors, waveguides, and fibers. Resonant high-frequency polar vibrational modes are observed and assigned in polymers PA6...... and PTFE, and their dielectric functions in the complete frequency window 2-15 THz are theoretically reproduced. Our results demonstrate the potential of ultrabroadband air-photonics-based THz time domain spectroscopy as a valuable analytic tool for materials science....

Plasma polarization spectroscopy. Time resolved spectroscopy in soft x-ray region on recombining plasma

International Nuclear Information System (INIS)

Iwamae, Atsushi; Hasuo, Masahiro; Atake, Makoto; Hasegawa, Noboru; Kawachi, Tetsuya

2007-01-01

We present an experimental study of polarization of emission radiations from recombining plasmas generated by the interaction of 60 fs ultra-short laser pulses with a gas jet. Time-resolved spectroscopy with a temporal resolution of 5 ps with repetitive accumulation is used to follow the recombination time histories. (author)

Generation of pulsed far-infrared radiation and its application for far-infrared time-resolved spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Kondo, Yasuhiro [Tohoku Univ., Sendai (Japan). Faculty of Engineering

1996-07-01

So-called time-resolved spectroscopy technique has been used from old time as the means for studying the dynamic optical property, light-induced reaction and so on of matters. As an example, there is the method called pump and probe, and here, the wavelength of this probe light is the problem. If the object energy region is limited to about 0.1 eV, fast time-resolved spectroscopy is feasible relatively easily. However, energy region is extended to low energy region, the light source which is available as the pulsed probe light having sufficient intensity is limited. In this paper, the attempt of time-resolved spectroscopy utilizing coherent radiation, which has ended in failure, and the laser pulse-induced far-infrared radiation which can be utilized as new far-infrared probe light are reported. The reason why far-infrared radiation is used is explained. The attempt of time-resolved spectroscopy using NaCl crystals is reported on the equipment, the method of measuring absorption spectra and the results. Laser pulse-induced far-infrared radiation and the method of generating it are described. The multi-channel detector for far-infrared radiation which was made for trial is shown. (K.I.)

Time-resolved and doppler-reduced laser spectroscopy on atoms

International Nuclear Information System (INIS)

Bergstroem, H.

1991-10-01

Radiative lifetimes have been studied in neutral boron, carbon, silicon and strontium, in singly ionized gadolinium and tantalum and in molecular carbon monoxide and C 2 . The time-resolved techniques were based either on pulsed lasers or pulse-modulated CW lasers. Several techniques have been utilized for the production of free atoms and ions such as evaporation into an atomic beam, sputtering in hollow cathodes and laser-produced plasmas. Hyperfine interactions in boron, copper and strontium have been examined using quantum beat spectroscopy, saturation spectroscopy and collimated atomic beam spectroscopy. Measurement techniques based on effusive hollow cathodes as well as laser produced plasmas in atomic physics have been developed. Investigations on laser produced plasmas using two colour beam deflection tomography for determination of electron densities have been performed. Finally, new possibilities for view-time-expansion in light-in-flight holography using mode-locked CW lasers have been demonstrated. (au)

Space- and time-resolved raman and breakdown spectroscopy: advanced lidar techniques

Science.gov (United States)

Silviu, Gurlui; Marius Mihai, Cazacu; Adrian, Timofte; Oana, Rusu; Georgiana, Bulai; Dimitriu, Dan

2018-04-01

DARLIOES - the advanced LIDAR is based on space- and time-resolved RAMAN and breakdown spectroscopy, to investigate chemical and toxic compounds, their kinetics and physical properties at high temporal (2 ns) and spatial (1 cm) resolution. The high spatial and temporal resolution are needed to resolve a large variety of chemical troposphere compounds, emissions from aircraft, the self-organization space charges induced light phenomena, temperature and humidity profiles, ice nucleation, etc.

Hexamethylcyclopentadiene: time-resolved photoelectron spectroscopy and ab initio multiple spawning simulations

DEFF Research Database (Denmark)

Wolf, T. J. A.; Kuhlman, Thomas Scheby; Schalk, O.

2014-01-01

comparing time-resolved photoelectron spectroscopy (TRPES) with ab initio multiple spawning (AIMS) simulations on the MS-MR-CASPT2 level of theory. We disentangle the relationship between two phenomena that dominate the immediate molecular response upon light absorption: a spectrally dependent delay...

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

Energy Technology Data Exchange (ETDEWEB)

Boschini, F.; Hedayat, H.; Piovera, C.; Dallera, C. [Dipartimento di Fisica, Politecnico di Milano, p.zza Leonardo da Vinci 32, 20133 Milano (Italy); Gupta, A. [Department of Chemistry, University of Alabama, Tuscaloosa, Alabama 35487 (United States); Carpene, E., E-mail: ettore.carpene@polimi.it [CNR-IFN, Dipartimento di Fisica, Politecnico di Milano, p.zza Leonardo da Vinci 32, 20133 Milano (Italy)

2015-01-15

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

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

International Nuclear Information System (INIS)

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

2015-01-01

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

Theory of sum-frequency generation spectroscopy of adsorbed molecules using the density matrix method-broadband vibrational sum-frequency generation and applications

International Nuclear Information System (INIS)

Bonn, M; Ueba, H; Wolf, M

2005-01-01

A generalized theory of frequency- and time-resolved vibrational sum-frequency generation (SFG) spectroscopy of adsorbates at surfaces is presented using the density matrix formalism. Our theoretical treatment is specifically aimed at addressing issues that accompany the relatively novel SFG approach using broadband infrared pulses. The ultrashort duration of these pulses makes them ideally suited for time-resolved investigations, for which we present a complete theoretical treatment. A second key characteristic of these pulses is their large bandwidth and high intensity, which allow for highly non-linear effects, including vibrational ladder climbing of surface vibrations. We derive general expressions relating the density matrix to SFG spectra, and apply these expressions to specific experimental results by solving the coupled optical Bloch equations of the density matrix elements. Thus, we can theoretically reproduce recent experimentally demonstrated hot band SFG spectra using femtosecond broadband infrared excitation of carbon monoxide (CO) on a Ru(001) surface

Development of soft x-ray time-resolved photoemission spectroscopy system with a two-dimensional angle-resolved time-of-flight analyzer at SPring-8 BL07LSU

Energy Technology Data Exchange (ETDEWEB)

Ogawa, Manami; Yamamoto, Susumu; Nakamura, Fumitaka; Yukawa, Ryu; Fukushima, Akiko; Harasawa, Ayumi; Kakizaki, Akito; Matsuda, Iwao [Institute for Solid State Physics, University of Tokyo, 5-1-5 Kashiwanoha, Chiba 277-8581 (Japan); Kousa, Yuka; Kondoh, Hiroshi [Department of Chemistry, Keio University, Yokohama 223-8522 (Japan); Tanaka, Yoshihito [RIKEN/SPring-8 Center, 1-1-1, Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148 (Japan)

2012-02-15

We have developed a soft x-ray time-resolved photoemission spectroscopy system using synchrotron radiation (SR) at SPring-8 BL07LSU and an ultrashort pulse laser system. Two-dimensional angle-resolved measurements were performed with a time-of-flight-type analyzer. The photoemission spectroscopy system is synchronized to light pulses of SR and laser using a time control unit. The performance of the instrument is demonstrated by mapping the band structure of a Si(111) crystal over the surface Brillouin zones and observing relaxation of the surface photo-voltage effect using the pump (laser) and probe (SR) method.

Time-resolved VUV spectroscopy in the EXTRAP-T2 reversed field pinch

International Nuclear Information System (INIS)

Hedqvist, A.; Rachlew-Kaellne, E.

1998-01-01

Time-resolved VUV spectroscopy has been used to investigate the effects of impurities in a reversed field pinch operating with a resistive shell. Results of electron temperature, impurity ion densities, particle confinement time and Z eff together with a description of the interpretation and the equipment are presented. (author)

Time-resolved tunable diode laser absorption spectroscopy of pulsed plasma

Czech Academy of Sciences Publication Activity Database

Adámek, Petr; Olejníček, Jiří; Čada, Martin; Kment, Š.; Hubička, Zdeněk

2013-01-01

Roč. 38, č. 14 (2013), s. 2428-2430 ISSN 0146-9592 R&D Projects: GA MŠk LH12045; GA ČR(CZ) GAP205/11/0386; GA MŠk LD12002; GA MŠk LH12043 Institutional support: RVO:68378271 Keywords : diode laser s * plasma diagnostics * absorption spectroscopy * time resolved Subject RIV: BL - Plasma and Gas Discharge Physics Impact factor: 3.179, year: 2013

Time-resolved spectroscopy using a chopper wheel as a fast shutter

International Nuclear Information System (INIS)

Wang, Shicong; Wendt, Amy E.; Boffard, John B.; Lin, Chun C.

2015-01-01

Widely available, small form-factor, fiber-coupled spectrometers typically have a minimum exposure time measured in milliseconds, and thus cannot be used directly for time-resolved measurements at the microsecond level. Spectroscopy at these faster time scales is typically done with an intensified charge coupled device (CCD) system where the image intensifier acts as a “fast” electronic shutter for the slower CCD array. In this paper, we describe simple modifications to a commercially available chopper wheel system to allow it to be used as a “fast” mechanical shutter for gating a fiber-coupled spectrometer to achieve microsecond-scale time-resolved optical measurements of a periodically pulsed light source. With the chopper wheel synchronized to the pulsing of the light source, the time resolution can be set to a small fraction of the pulse period by using a chopper wheel with narrow slots separated by wide spokes. Different methods of synchronizing the chopper wheel and pulsing of the light sources are explored. The capability of the chopper wheel system is illustrated with time-resolved measurements of pulsed plasmas

Time-resolved VUV spectroscopy in the EXTRAP-T2 reversed field pinch

Science.gov (United States)

Hedqvist, Anders; Rachlew-Källne, Elisabeth

1998-09-01

Time-resolved VUV spectroscopy has been used to investigate the effects of impurities in a reversed field pinch operating with a resistive shell. Results of electron temperature, impurity ion densities, particle confinement time and 0741-3335/40/9/004/img1 together with a description of the interpretation and the equipment are presented.

TIME-RESOLVED INFRARED SPECTROSCOPY IN THE U121R BEAMLINE AT THE NSLS

International Nuclear Information System (INIS)

CARR, G.L.; LAVEIGNE, J.D.; LOBO, R.P.S.M.; REITZE, D.H.; TANNER, D.B.

1999-01-01

A facility for performing time-resolved infrared spectroscopy has been developed at the NSLS, primarily at beamline U12IR. The pulsed IR light from the synchrotron is used to perform pump-probe spectroscopy. The authors present here a description of the facility and results for the relaxation of photoexcitations in both a semiconductor and superconductor

Spectrally resolved, broadband frequency response characterization of photodetectors using continuous-wave supercontinuum sources

Science.gov (United States)

Choudhury, Vishal; Prakash, Roopa; Nagarjun, K. P.; Supradeepa, V. R.

2018-02-01

A simple and powerful method using continuous wave supercontinuum lasers is demonstrated to perform spectrally resolved, broadband frequency response characterization of photodetectors in the NIR Band. In contrast to existing techniques, this method allows for a simple system to achieve the goal, requiring just a standard continuous wave(CW) high-power fiber laser source and an RF spectrum analyzer. From our recent work, we summarize methods to easily convert any high-power fiber laser into a CW supercontinuum. These sources in the time domain exhibit interesting properties all the way down to the femtosecond time scale. This enables measurement of broadband frequency response of photodetectors while the wide optical spectrum of the supercontinuum can be spectrally filtered to obtain this information in a spectrally resolved fashion. The method involves looking at the RF spectrum of the output of a photodetector under test when incident with the supercontinuum. By using prior knowledge of the RF spectrum of the source, the frequency response can be calculated. We utilize two techniques for calibration of the source spectrum, one using a prior measurement and the other relying on a fitted model. Here, we characterize multiple photodetectors from 150MHz bandwidth to >20GHz bandwidth at multiple bands in the NIR region. We utilize a supercontinuum source spanning over 700nm bandwidth from 1300nm to 2000nm. For spectrally resolved measurement, we utilize multiple wavelength bands such as around 1400nm and 1600nm. Interesting behavior was observed in the frequency response of the photodetectors when comparing broadband spectral excitation versus narrower band excitation.

Time-resolved photoelectron spectroscopy of nitrobenzene and its aldehydes

Science.gov (United States)

Schalk, Oliver; Townsend, Dave; Wolf, Thomas J. A.; Holland, David M. P.; Boguslavskiy, Andrey E.; Szöri, Milan; Stolow, Albert

2018-01-01

We report the first femtosecond time-resolved photoelectron spectroscopy study of 2-, 3- and 4-nitrobenzaldehyde (NBA) and nitrobenzene (NBE) in the gas phase upon excitation at 200 nm. In 3- and 4-NBA, the dynamics follow fast intersystem crossing within 1-2 picoseconds. In 2-NBA and NBE, the dynamics are faster (∼ 0.5 ps). 2-NBA undergoes hydrogen transfer similar to solution phase dynamics. NBE either releases NO2 in the excited state or converts internally back to the ground state. We discuss why these channels are suppressed in the other nitrobenzaldehydes.

Transient photoconductivity in InGaN/GaN multiple quantum wells, measured by time-resolved terahertz spectroscopy

DEFF Research Database (Denmark)

Porte, Henrik; Turchinovich, Dmitry; Cooke, David

2009-01-01

Terahertz conductivity of InGaN/GaN MQWs was studied by time-resolved terahertz spectroscopy. Restoration of the built-in piezoelectric field leads to a nonexponential carrier density decay. Terahertz conductivity spectrum is described by the Drude-Smith......Terahertz conductivity of InGaN/GaN MQWs was studied by time-resolved terahertz spectroscopy. Restoration of the built-in piezoelectric field leads to a nonexponential carrier density decay. Terahertz conductivity spectrum is described by the Drude-Smith...

Time-resolved x-ray absorption spectroscopy: Watching atoms dance

Science.gov (United States)

Milne, Chris J.; Pham, Van-Thai; Gawelda, Wojciech; van der Veen, Renske M.; El Nahhas, Amal; Johnson, Steven L.; Beaud, Paul; Ingold, Gerhard; Lima, Frederico; Vithanage, Dimali A.; Benfatto, Maurizio; Grolimund, Daniel; Borca, Camelia; Kaiser, Maik; Hauser, Andreas; Abela, Rafael; Bressler, Christian; Chergui, Majed

2009-11-01

The introduction of pump-probe techniques to the field of x-ray absorption spectroscopy (XAS) has allowed the monitoring of both structural and electronic dynamics of disordered systems in the condensed phase with unprecedented accuracy, both in time and in space. We present results on the electronically excited high-spin state structure of an Fe(II) molecular species, [FeII(bpy)3]2+, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 Å. In addition an analysis technique using the reduced χ2 goodness of fit between FEFF EXAFS simulations and the experimental transient absorption signal in energy space has been successfully tested as a function of excited state population and chemical shift, demonstrating its applicability in situations where the fractional excited state population cannot be determined through other measurements. Finally by using a novel ultrafast hard x-ray 'slicing' source the question of how the molecule relaxes after optical excitation has been successfully resolved using femtosecond XANES.

Gain-assisted broadband ring cavity enhanced spectroscopy

Science.gov (United States)

Selim, Mahmoud A.; Adib, George A.; Sabry, Yasser M.; Khalil, Diaa

2017-02-01

Incoherent broadband cavity enhanced spectroscopy can significantly increase the effective path length of light-matter interaction to detect weak absorption lines over broad spectral range, for instance to detect gases in confined environments. Broadband cavity enhancement can be based on the decay time or the intensity drop technique. Decay time measurement is based on using tunable laser source that is expensive and suffers from long scan time. Intensity dependent measurement is usually reported based on broadband source using Fabry-Perot cavity, enabling short measurement time but suffers from the alignment tolerance of the cavity and the cavity insertion loss. In this work we overcome these challenges by using an alignment-free ring cavity made of an optical fiber loop and a directional coupler, while having a gain medium pumped below the lasing threshold to improve the finesse and reduce the insertion loss. Acetylene (C2H2) gas absorption is measured around 1535 nm wavelength using a semiconductor optical amplifier (SOA) gain medium. The system is analyzed for different ring resonator forward coupling coefficient and loses, including the 3-cm long gas cell insertion loss and fiber connector losses used in the experimental verification. The experimental results are obtained for a coupler ratio of 90/10 and a fiber length of 4 m. The broadband source is the amplified spontaneous emission of another SOA and the output is measured using a 70pm-resolution optical spectrum analyzer. The absorption depth and the effective interaction length are improved about an order of magnitude compared to the direct absorption of the gas cell. The presented technique provides an engineering method to improve the finesse and, consequently the effective length, while relaxing the technological constraints on the high reflectivity mirrors and free-space cavity alignment.

Time-resolved resonance fluorescence spectroscopy for study of chemical reactions in laser-induced plasmas.

Science.gov (United States)

Liu, Lei; Deng, Leimin; Fan, Lisha; Huang, Xi; Lu, Yao; Shen, Xiaokang; Jiang, Lan; Silvain, Jean-François; Lu, Yongfeng

2017-10-30

Identification of chemical intermediates and study of chemical reaction pathways and mechanisms in laser-induced plasmas are important for laser-ablated applications. Laser-induced breakdown spectroscopy (LIBS), as a promising spectroscopic technique, is efficient for elemental analyses but can only provide limited information about chemical products in laser-induced plasmas. In this work, time-resolved resonance fluorescence spectroscopy was studied as a promising tool for the study of chemical reactions in laser-induced plasmas. Resonance fluorescence excitation of diatomic aluminum monoxide (AlO) and triatomic dialuminum monoxide (Al 2 O) was used to identify these chemical intermediates. Time-resolved fluorescence spectra of AlO and Al 2 O were used to observe the temporal evolution in laser-induced Al plasmas and to study their formation in the Al-O 2 chemistry in air.

Frame-Transfer Gating Raman Spectroscopy for Time-Resolved Multiscalar Combustion Diagnostics

Science.gov (United States)

Nguyen, Quang-Viet; Fischer, David G.; Kojima, Jun

2011-01-01

Accurate experimental measurement of spatially and temporally resolved variations in chemical composition (species concentrations) and temperature in turbulent flames is vital for characterizing the complex phenomena occurring in most practical combustion systems. These diagnostic measurements are called multiscalar because they are capable of acquiring multiple scalar quantities simultaneously. Multiscalar diagnostics also play a critical role in the area of computational code validation. In order to improve the design of combustion devices, computational codes for modeling turbulent combustion are often used to speed up and optimize the development process. The experimental validation of these codes is a critical step in accepting their predictions for engine performance in the absence of cost-prohibitive testing. One of the most critical aspects of setting up a time-resolved stimulated Raman scattering (SRS) diagnostic system is the temporal optical gating scheme. A short optical gate is necessary in order for weak SRS signals to be detected with a good signal- to-noise ratio (SNR) in the presence of strong background optical emissions. This time-synchronized optical gating is a classical problem even to other spectroscopic techniques such as laser-induced fluorescence (LIF) or laser-induced breakdown spectroscopy (LIBS). Traditionally, experimenters have had basically two options for gating: (1) an electronic means of gating using an image intensifier before the charge-coupled-device (CCD), or (2) a mechanical optical shutter (a rotary chopper/mechanical shutter combination). A new diagnostic technology has been developed at the NASA Glenn Research Center that utilizes a frame-transfer CCD sensor, in conjunction with a pulsed laser and multiplex optical fiber collection, to realize time-resolved Raman spectroscopy of turbulent flames that is free from optical background noise (interference). The technology permits not only shorter temporal optical gating (down

Time resolved optical emission spectroscopy of cross-beam pulsed laser ablation on graphite targets

International Nuclear Information System (INIS)

Sangines, R.; Sanchez Ake, C.; Sobral, H.; Villagran-Muniz, M.

2007-01-01

Cross-beam pulsed laser ablation with two delayed lasers is performed on two perpendicular graphite targets. The time delay between lasers is varied by up to 5 μs, and physical changes on the second plasma, due to the interaction with the first generated one, are determined by time resolved optical emission spectroscopy

Photophysical characterization and time-resolved spectroscopy of a anthradithiophene dimer: exploring the role of conformation in singlet fission

KAUST Repository

Dean, Jacob C.; Zhang, Ruomeng; Hallani, Rawad K.; Pensack, Ryan D.; Sanders, Samuel N.; Oblinsky, Daniel G.; Parkin, Sean R.; Campos, Luis M.; Anthony, John E.; Scholes, Gregory D.

2017-01-01

carried out in toluene and acetone solution via absorption and fluorescence spectroscopy, and their photo-initiated dynamics were investigated with time-resolved fluorescence (TRF) and transient absorption (TA) spectroscopy. In accordance

Time-resolved terahertz spectroscopy of conjugated polymer/CdSe nanorod composites

DEFF Research Database (Denmark)

Cooke, David; Lek, Jun Y.; Krebs, Frederik C

2010-01-01

report ultrafast carrier dynamics in hybrid CdSe nanorod / poly(3-hexythiophene) (P3HT) bulk heterojunction films measured by time-resolved terahertz spectroscopy, and compare to the well studied P3HT/phenyl-C61-butyric acid methyl ester (PCBM) blend. Both films show an improved peak...... photoconductivity compared to P3HT alone, consistent with efficient charge transfer. The photoconductivity dynamics show fast, picosecond trapping or recombination in the hybrid blend while the all-organic film shows no such loss of mobile charge over ns time scales. The ac conductivity for all samples is well...

Speciation of actinides in aqueous solution by time-resolved laser-induced fluorescence spectroscopy (TRLFS)

International Nuclear Information System (INIS)

Kimura, Takaumi; Kato, Yoshiharu; Meinrath, G.; Yoshida, Zenko; Choppin, G.R.

1995-01-01

Time-resolved laser-induced fluorescence spectroscopy (TRLFS) as a sensitive and selective method has been applied to the speciation of actinides in aqueous solution. Studies on hydrolysis and carbonate complexation of U(VI) and on determination of hydration number of Cm(III) are reported. (author)

Scanning, non-contact, hybrid broadband diffuse optical spectroscopy and diffuse correlation spectroscopy system.

Science.gov (United States)

Johansson, Johannes D; Mireles, Miguel; Morales-Dalmau, Jordi; Farzam, Parisa; Martínez-Lozano, Mar; Casanovas, Oriol; Durduran, Turgut

2016-02-01

A scanning system for small animal imaging using non-contact, hybrid broadband diffuse optical spectroscopy (ncDOS) and diffuse correlation spectroscopy (ncDCS) is presented. The ncDOS uses a two-dimensional spectrophotometer retrieving broadband (610-900 nm) spectral information from up to fifty-seven source-detector distances between 2 and 5 mm. The ncDCS data is simultaneously acquired from four source-detector pairs. The sample is scanned in two dimensions while tracking variations in height. The system has been validated with liquid phantoms, demonstrated in vivo on a human fingertip during an arm cuff occlusion and on a group of mice with xenoimplanted renal cell carcinoma.

Characterization of type I, II, III, IV, and V collagens by time-resolved laser-induced fluorescence spectroscopy

Science.gov (United States)

Marcu, Laura; Cohen, David; Maarek, Jean-Michel I.; Grundfest, Warren S.

2000-04-01

The relative proportions of genetically distinct collagen types in connective tissues vary with tissue type and change during disease progression, development, wound healing, aging. This study aims to 1) characterize the spectro- temporal fluorescence emission of fiber different types of collagen and 2) assess the ability of time-resolved laser- induced fluorescence spectroscopy to distinguish between collagen types. Fluorescence emission of commercially available purified samples was induced with nitrogen laser excitation pulses and detected with a MCP-PMT connected to a digital storage oscilloscope. The recorded time-resolved emission spectra displayed distinct fluorescence emission characteristics for each collagen type. The time domain information complemented the spectral domain intensity data for improved discrimination between different collagen types. Our results reveal that analysis of the fluorescence emission can be used to characterize different species of collagen. Also, the results suggest that time-resolved spectroscopy can be used for monitoring of connective tissue matrix composition changes due to various pathological and non-pathological conditions.

Time-resolved ultraviolet laser-induced breakdown spectroscopy for organic material analysis

Energy Technology Data Exchange (ETDEWEB)

Baudelet, Matthieu; Boueri, Myriam [Laboratoire de Spectrometrie Ionique et Moleculaire, Universite Claude Bernard Lyon 1, UMR CNRS 5579, 43, Bd. du 11 Novembre 1918, F-69622 Villeurbanne Cedex (France); Yu Jin [Laboratoire de Spectrometrie Ionique et Moleculaire, Universite Claude Bernard Lyon 1, UMR CNRS 5579, 43, Bd. du 11 Novembre 1918, F-69622 Villeurbanne Cedex (France)], E-mail: jin.yu@lasim.univ-lyon1.fr; Mao, Samuel S; Piscitelli, Vincent; Xianglei, Mao; Russo, Richard E [Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

2007-12-15

Ultraviolet pulses (266 nm) delivered by a quadrupled Nd:YAG laser were used to analyze organic samples with laser-induced breakdown spectroscopy (LIBS). We present characteristics of the spectra obtained from organic samples with special attentions on the emissions of organic elements, O and N, and molecular bonds CN. The choice of these atomic or molecular species is justified on one hand, by the importance of these species to specify organic or biological materials; and on the other hand by the possible interferences with ambient air when laser ablation takes place in the atmosphere. Time-resolved LIBS was used to determine the time-evolution of line intensity emitted from these species. We demonstrate different kinetic behaviors corresponding to different origins of emitters: native atomic or molecular species directly vaporized from the sample or those generated through dissociation or recombination due to interaction between laser-induced plasma and air molecules. Our results show the ability of time-resolved UV-LIBS for detection and identification of native atomic or molecular species from an organic sample.

Time-resolved fluorescence spectroscopy

International Nuclear Information System (INIS)

Gustavsson, Thomas; Mialocq, Jean-Claude

2007-01-01

This article addresses the evolution in time of light emitted by a molecular system after a brief photo-excitation. The authors first describe fluorescence from a photo-physical point of view and discuss the characterization of the excited state. Then, they explain some basic notions related to fluorescence characterization (lifetime and decays, quantum efficiency, so on). They present the different experimental methods and techniques currently used to study time-resolved fluorescence. They discuss basic notions of time resolution and spectral reconstruction. They briefly present some conventional methods: intensified Ccd cameras, photo-multipliers and photodiodes associated with a fast oscilloscope, and phase modulation. Other methods and techniques are more precisely presented: time-correlated single photon counting (principle, examples, and fluorescence lifetime imagery), streak camera (principle, examples), and optical methods like the Kerr optical effect (principle and examples) and fluorescence up-conversion (principle and theoretical considerations, examples of application)

Time-resolved x-ray laser induced photoelectron spectroscopy of isochoric heated copper

International Nuclear Information System (INIS)

Nelson, A.J.; Dunn, J.; Hunter, J.; Widmann, K.

2005-01-01

Time-resolved x-ray photoelectron spectroscopy is used to probe the nonsteady-state evolution of the valence band electronic structure of laser heated ultrathin (50 nm) copper. A metastable phase is studied using a 527 nm wavelength 400 fs laser pulse containing 0.1-2.5 mJ laser energy focused in a large 500x700 μm 2 spot to create heated conditions of 0.07-1.8x10 12 W cm -2 intensity. Valence band photoemission spectra are presented showing the changing occupancy of the Cu 3d level with heating are presented. These picosecond x-ray laser induced time-resolved photoemission spectra of laser-heated ultrathin Cu foil show dynamic changes in the electronic structure. The ultrafast nature of this technique lends itself to true single-state measurements of shocked and heated materials

Time-resolved X-ray spectroscopies of chemical systems: New perspectives

Directory of Open Access Journals (Sweden)

Majed Chergui

2016-05-01

Full Text Available The past 3–5 years have witnessed a dramatic increase in the number of time-resolved X-ray spectroscopic studies, mainly driven by novel technical and methodological developments. The latter include (i the high repetition rate optical pump/X-ray probe studies, which have greatly boosted the signal-to-noise ratio for picosecond (ps X-ray absorption spectroscopy studies, while enabling ps X-ray emission spectroscopy (XES at synchrotrons; (ii the X-ray free electron lasers (XFELs are a game changer and have allowed the first femtosecond (fs XES and resonant inelastic X-ray scattering experiments to be carried out; (iii XFELs are also opening the road to the development of non-linear X-ray methods. In this perspective, I will mainly focus on the most recent technical developments and briefly address some examples of scientific questions that have been addressed thanks to them. I will look at the novel opportunities in the horizon.

Broadband stimulated Raman spectroscopy in the deep ultraviolet region

Science.gov (United States)

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 (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.

Laser induced breakdown spectroscopy of the uranium including calcium. Time resolved measurement spectroscopic analysis (Contract research)

International Nuclear Information System (INIS)

Akaoka, Katsuaki; Maruyama, Youichiro; Oba, Masaki; Miyabe, Masabumi; Otobe, Haruyoshi; Wakaida, Ikuo

2010-05-01

For the remote analysis of low DF TRU (Decontamination Factor Transuranic) fuel, Laser Breakdown Spectroscopy (LIBS) was applied to uranium oxide including a small amount of calcium oxide. The characteristics, such as spectrum intensity and plasma excitation temperature, were measured using time-resolved spectroscopy. As a result, in order to obtain the stable intensity of calcium spectrum for the uranium spectrum, it was found out that the optimum observation delay time of spectrum is 4 microseconds or more after laser irradiation. (author)

Challenge for real-time and real-space resolved spectroscopy of surface chemical reactions. Aiming at trace of irreversible and inhomogeneous reactions

International Nuclear Information System (INIS)

Amemiya, Kenta

2015-01-01

A novel experimental technique, time-resolved wavelength-dispersive soft X-ray imaging spectroscopy, is proposed in order to achieve real-time and real-space resolved spectroscopy for the observation of irreversible and inhomogeneous surface chemical reactions. By combining the wavelength-dispersed soft X rays, in which the X-ray wavelength (photon energy) changes as a function of position on the sample, with the photoelectron emission microscope, the soft X-ray absorption spectra are separately obtained at different positions on the sample without scanning the X-ray monochromator. Therefore, the real-time resolved measurement of site-selective soft X-ray absorption spectroscopy is realized in one event without repeating the chemical reaction. It is expected that the spatial distribution of different chemical species is traced during the surface chemical reaction, which is essential to understand the reaction mechanism. (author)

Ionic classification of Xe laser lines: A new approach through time resolved spectroscopy

International Nuclear Information System (INIS)

Schinca, D.; Duchowicz, R.; Gallardo, M.

1992-01-01

Visible and UV laser emission from a highly ionized pulsed Xe plasma was studied in relation to the ionic assignment of the laser lines. Time-resolved spectroscopy was used to determine the ionic origin of the studied lines. The results are in agreement with an intensity versus pressure analysis performed over the same wavelength range. From the temporal behaviour of the spontaneous emission, a probable classification can be obtained. (author). 7 refs, 7 figs, 1 tab

Broadband Rotational Spectroscopy

Science.gov (United States)

Pate, Brooks

2014-06-01

The past decade has seen several major technology advances in electronics operating at microwave frequencies making it possible to develop a new generation of spectrometers for molecular rotational spectroscopy. High-speed digital electronics, both arbitrary waveform generators and digitizers, continue on a Moore's Law-like development cycle that started around 1993 with device bandwidth doubling about every 36 months. These enabling technologies were the key to designing chirped-pulse Fourier transform microwave (CP-FTMW) spectrometers which offer significant sensitivity enhancements for broadband spectrum acquisition in molecular rotational spectroscopy. A special feature of the chirped-pulse spectrometer design is that it is easily implemented at low frequency (below 8 GHz) where Balle-Flygare type spectrometers with Fabry-Perot cavity designs become technologically challenging due to the mirror size requirements. The capabilities of CP-FTMW spectrometers for studies of molecular structure will be illustrated by the collaborative research effort we have been a part of to determine the structures of water clusters - a project which has identified clusters up to the pentadecamer. A second technology trend that impacts molecular rotational spectroscopy is the development of high power, solid state sources in the mm-wave/THz regions. Results from the field of mm-wave chirped-pulse Fourier transform spectroscopy will be described with an emphasis on new problems in chemical dynamics and analytical chemistry that these methods can tackle. The third (and potentially most important) technological trend is the reduction of microwave components to chip level using monolithic microwave integrated circuits (MMIC) - a technology driven by an enormous mass market in communications. Some recent advances in rotational spectrometer designs that incorporate low-cost components will be highlighted. The challenge to the high-resolution spectroscopy community - as posed by Frank De

Temperature Measurements in Reacting Flows Using Time-Resolved Femtosecond Coherent Anti-Stokes Raman Scattering (fs-CARS) Spectroscopy (Postprint)

National Research Council Canada - National Science Library

Roy, Sukesh; Kinnius, Paul J; Lucht, Robert P; Gord, James R

2007-01-01

Time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of the nitrogen molecule is used for the measurement of temperature in atmospheric-pressure, near-adiabatic, hydrogen-air diffusion flames...

Microcontroller based resonance tracking unit for time resolved continuous wave cavity-ringdown spectroscopy measurements.

Science.gov (United States)

Votava, Ondrej; Mašát, Milan; Parker, Alexander E; Jain, Chaithania; Fittschen, Christa

2012-04-01

We present in this work a new tracking servoloop electronics for continuous wave cavity-ringdown absorption spectroscopy (cw-CRDS) and its application to time resolved cw-CRDS measurements by coupling the system with a pulsed laser photolysis set-up. The tracking unit significantly increases the repetition rate of the CRDS events and thus improves effective time resolution (and/or the signal-to-noise ratio) in kinetics studies with cw-CRDS in given data acquisition time. The tracking servoloop uses novel strategy to track the cavity resonances that result in a fast relocking (few ms) after the loss of tracking due to an external disturbance. The microcontroller based design is highly flexible and thus advanced tracking strategies are easy to implement by the firmware modification without the need to modify the hardware. We believe that the performance of many existing cw-CRDS experiments, not only time-resolved, can be improved with such tracking unit without any additional modification to the experiment. © 2012 American Institute of Physics

Time-resolved pump-probe X-ray absorption fine structure spectroscopy of Gaq3

International Nuclear Information System (INIS)

Dicke, Benjamin

2013-01-01

Gallium(tris-8-hydroxyquinoline) (Gaq 3 ) belongs to a class of metal organic compounds, used as electron transport layer and emissive layer in organic light emitting diodes. Many research activities have concentrated on the optical and electronic properties, especially of the homologue molecule aluminum(tris-8-hydroxyquinoline) (Alq 3 ). Knowledge of the first excited state S 1 structure of these molecules could provide deeper insight into the processes involved into the operation of electronic devices, such as OLEDs and, hence, it could further improve their efficiency and optical properties. Until now the excited state structure could not be determined experimentally. Most of the information about this structure mainly arises from theoretical calculations. X-ray absorption fine structure (XAFS) spectroscopy is a well developed technique to determine both, the electronic and the geometric properties of a sample. The connection of ultrashort pulsed X-ray sources with a pulsed laser system offers the possibility to use XAFS as a tool for studying the transient changes of a sample induced by a laser pulse. In the framework of this thesis a new setup for time-resolved pump-probe X-ray absorption spectroscopy at PETRA III beamline P11 was developed for measuring samples in liquid form. In this setup the sample is pumped into its photo-excited state by a femtosecond laser pump pulse with 343 nm wavelength and after a certain time delay probed by an X-ray probe pulse. In this way the first excited singlet state S 1 of Gaq 3 dissolved in benzyl alcohol was analyzed. A structural model for the excited state structure of the Gaq 3 molecule based on the several times reproduced results of the XAFS experiments is proposed. According to this model it was found that the Ga-N A bond length is elongated, while the Ga-O A bond length is shortened upon photoexcitation. The dynamics of the structural changes were not the focus of this thesis. Nevertheless the excited state lifetime

Time-resolved luminescent spectroscopy of YAG:Ce single crystal and single crystalline films

International Nuclear Information System (INIS)

Zorenko, Yu.; Gorbenko, V.; Savchyn, V.; Vozniak, T.; Puzikov, V.; Danko, A.; Nizhankovski, S.

2010-01-01

The peculiarities of the luminescence and energy transfer from YAG host to the emission centers formed by the Y Al antisite defects and Ce 3+ ions have been studied in YAG:Ce single crystals, grown from the melt by modified Bridgman method in Ar and CO 2 + H 2 atmospheres, and YAG:Ce single crystalline film, grown by liquid phase epitaxy method, using the comparative time-resolved luminescent spectroscopy under excitation by synchrotron radiation in the range of fundamental adsorption of this garnet.

Time-resolved resonance Raman spectroscopy of radiation-chemical processes

International Nuclear Information System (INIS)

Tripathi, G.N.R.

1983-01-01

A tunable pulsed laser Raman spectrometer for time resolved Raman studies of radiation-chemical processes is described. This apparatus utilizes the state of art optical multichannel detection and analysis techniques for data acquisition and electron pulse radiolysis for initiating the reactions. By using this technique the resonance Raman spectra of intermediates with absorption spectra in the 248-900 nm region, and mean lifetimes > 30 ns can be examined. This apparatus can be used to time resolve the vibrational spectral overlap between transients absorbing in the same region, and to follow their decay kinetics by monitoring the well resolved Raman peaks. For kinetic measurements at millisecond time scale, the Raman technique is preferable over optical absorption method where low frequency noise is quite bothersome. A time resolved Raman study of the pulse radiolytic oxidation of aqueous tetrafluorohydroquinone and p-methoxyphenol is briefly discussed. 15 references, 5 figures

NO kinetics in pulsed low-pressure nitrogen plasmas studied by time resolved quantum cascade laser absorption spectroscopy

NARCIS (Netherlands)

Welzel, S.; Guaitella, O.; Lazzaroni, C.; Pintassilgo, C.; Rousseau, A.; Röpcke, J.

2011-01-01

Time-resolved quantum cascade laser absorption spectroscopy at 1897 cm-1 (5.27 µm) has been applied to study the NO(X) kinetics on the micro- and millisecond time scale in pulsed low-pressure N2/NO dc discharges. Experiments have been performed under flowing and static gas conditions to infer the

Exploring the Dynamics of Superconductors by Time-Resolved Far-Infrared Spectroscopy

International Nuclear Information System (INIS)

Carr, G. L.; Lobo, R. P. S. M.; LaVeigne, J.; Reitze, D. H.; Tanner, D. B.

2000-01-01

We have examined the recombination of excess quasiparticles in superconducting Pb by time-resolved far-infrared spectroscopy using a pulsed synchrotron source. The energy gap shift calculated by Owen and Scalapino [Phys. Rev. Lett. 28, 1559 (1972)] is directly observed, as is the associated reduction in the Cooper pair density. The relaxation process involves a two-component decay; the faster (∼200 ps) is associated with the actual (effective) recombination process, while the slower (∼10 to 100ns) is due to heat transport across the film/substrate interface. The temperature dependence of the recombination process between 0.5T c and 0.85T c is in good agreement with theory

Time-resolved spectroscopy of plasma resonances in highly excited silicon and germanium

International Nuclear Information System (INIS)

Huang, C.Y.; Malvezzi, A.M.; Bloembergen, N.; Kurz, H.

1985-01-01

The dynamics of the electron-hole plasma in silicon and germanium samples irradiated by 20 ps. 532 nm laser pulses has been investigated in the near infrared by the time-resolved picosecond optical spectroscopy. The experimental reflectivities and transmission are compared with the predictions of the thermal model for degenerate carrier distributions through the Drude formalism. Above a certain fluence, a significant deviation between measured and calculated values indicates a strong increase of the recombination rate as soon as the plasma resonances become comparable with the band gaps. These new plasmon-aided recombination channels are particularly pronounced in germanium. 15 refs., 8 figs

Time-resolved X-ray photoelectron spectroscopy techniques for the study of interfacial charge dynamics

Energy Technology Data Exchange (ETDEWEB)

Neppl, Stefan, E-mail: sneppl@lbl.gov; Gessner, Oliver

2015-04-15

Highlights: • Ultrafast interfacial charge transfer is probed with atomic site specificity. • Femtosecond X-ray photoelectron spectroscopy using a free electron laser. • Efficient and flexible picosecond X-ray photoelectron pump–probe scheme using synchrotron radiation. - Abstract: X-ray photoelectron spectroscopy (XPS) is one of the most powerful techniques to quantitatively analyze the chemical composition and electronic structure of surfaces and interfaces in a non-destructive fashion. Extending this technique into the time domain has the exciting potential to shed new light on electronic and chemical dynamics at surfaces by revealing transient charge configurations with element- and site-specificity. Here, we describe prospects and challenges that are associated with the implementation of picosecond and femtosecond time-resolved X-ray photoelectron spectroscopy at third-generation synchrotrons and X-ray free-electron lasers, respectively. In particular, we discuss a series of laser-pump/X-ray-probe photoemission experiments performed on semiconductor surfaces, molecule-semiconductor interfaces, and films of semiconductor nanoparticles that demonstrate the high sensitivity of time-resolved XPS to light-induced charge carrier generation, diffusion and recombination within the space charge layers of these materials. Employing the showcase example of photo-induced electronic dynamics in a dye-sensitized semiconductor system, we highlight the unique possibility to probe heterogeneous charge transfer dynamics from both sides of an interface, i.e., from the perspective of the molecular electron donor and the semiconductor acceptor, simultaneously. Such capabilities will be crucial to improve our microscopic understanding of interfacial charge redistribution and associated chemical dynamics, which are at the heart of emerging energy conversion, solar fuel generation, and energy storage technologies.

Hole emission from Ge/Si quantum dots studied by time-resolved capacitance spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Kapteyn, C.M.A.; Lion, M.; Heitz, R.; Bimberg, D. [Technische Univ. Berlin (Germany). Inst. fuer Festkoerperphysik; Miesner, C.; Asperger, T.; Brunner, K.; Abstreiter, G. [Technische Univ. Muenchen, Garching (Germany). Walter-Schottky-Inst. fuer Physikalische Grundlagen der Halbleiterelektronik

2001-03-01

Emission of holes from self-organized Ge quantum dots (QDs) embedded in Si Schottky diodes is studied by time-resolved capacitance spectroscopy (DLTS). The DLTS signal is rather broad and depends strongly on the filling and detection bias conditions. The observed dependence is interpreted in terms of carrier emission from many-hole states of the QDs. The activation energies obtained from the DLTS measurements are a function of the amount of stored charge and the position of the Fermi level in the QDs. (orig.)

Development of time-resolved electron momentum spectroscopy. Toward real-time imaging of frontier electrons in molecular reactions

International Nuclear Information System (INIS)

Yamazaki, M.; Takahashi, M.

2016-01-01

This report will introduce a new experimental technique to readers, which we would like to propose towards advances in the field of molecular reaction dynamics. It is time-resolved electron momentum spectroscopy and aims to take in momentum space snapshots of the rapid change of molecular orbitals, which is the driving force behind any structural changes occurring in transient molecules. Following a description of the working principle of the technique, some preliminary result will be presented in order to illustrate the current performance of the apparatus. (author)

Recent trends in spin-resolved photoelectron spectroscopy

Science.gov (United States)

Okuda, Taichi

2017-12-01

Since the discovery of the Rashba effect on crystal surfaces and also the discovery of topological insulators, spin- and angle-resolved photoelectron spectroscopy (SARPES) has become more and more important, as the technique can measure directly the electronic band structure of materials with spin resolution. In the same way that the discovery of high-Tc superconductors promoted the development of high-resolution angle-resolved photoelectron spectroscopy, the discovery of this new class of materials has stimulated the development of new SARPES apparatus with new functions and higher resolution, such as spin vector analysis, ten times higher energy and angular resolution than conventional SARPES, multichannel spin detection, and so on. In addition, the utilization of vacuum ultra violet lasers also opens a pathway to the realization of novel SARPES measurements. In this review, such recent trends in SARPES techniques and measurements will be overviewed.

Time-resolved absorption measurements on OMEGA

International Nuclear Information System (INIS)

Jaanimagi, P.A.; DaSilva, L.; Delettrez, J.; Gregory, G.G.; Richardson, M.C.

1986-01-01

Time-resolved measurements of the incident laser light that is scattered and/or refracted from targets irradiated by the 24 uv-beam OMEGA laser at LLE, have provided some interesting features related to time-resolved absorption. The decrease in laser absorption characteristic of irradiating a target that implodes during the laser pulse has been observed. The increase in absorption expected as the critical density surface moves from a low to a high Z material in the target has also been noted. The detailed interpretation of these results is made through comparisons with simulation using the code LILAC, as well as with streak data from time-resolved x-ray imaging and spectroscopy. In addition, time and space-resolved imaging of the scattered light yields information on laser irradiation uniformity conditions on the target. The report consists of viewgraphs

Charge transport in nanostructured materials for solar energy conversion studied by time-resolved terahertz spectroscopy

Czech Academy of Sciences Publication Activity Database

Němec, Hynek; Kužel, Petr; Sundström, V.

2010-01-01

Roč. 215, 2-3 (2010), s. 123-139 ISSN 1010-6030 R&D Projects: GA ČR(CZ) GP202/09/P099; GA AV ČR(CZ) IAA100100902; GA MŠk LC512 Institutional research plan: CEZ:AV0Z10100520 Keywords : time-resolved terahertz spectroscopy * ultrafast dynamics * bulk heterojunction * semiconductor nanostructures * transport * mobility Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 2.243, year: 2010

Broadband integrated mid infrared light sources as enabling technology for point of care mid-infrared spectroscopy

Science.gov (United States)

2017-08-20

AFRL-AFOSR-JP-TR-2017-0061 Broadband integrated mid-infrared light sources as enabling technology for point-of-care mid- infrared spectroscopy Alex...mid-infrared light sources as enabling technology for point-of-care mid-infrared spectroscopy 5a.  CONTRACT NUMBER 5b.  GRANT NUMBER FA2386-16-1-4037...Broadband integrated mid-infrared light sources as enabling technology for point-of-care mid- infrared spectroscopy ” Date: 16th August 2017 Name

Time-resolved spectroscopy of the probe fluorescence in the study of human blood protein dynamic structure on SR beam

International Nuclear Information System (INIS)

Dobretsov, G.E.; Kurek, N.K.; Syrejshchikova, T.I.; Yakimenko, M.N.; Clarke, D.T.; Jones, G.R.; Munro, I.H.

2000-01-01

Time-resolved spectroscopy on the SRS of the Daresbury Laboratory was used for the study of the human serum lipoproteins and human blood albumins with fluorescent probes K-37 and K-35, developed in Russia. The probe K-37 was found sensitive to the difference in dynamic properties of the lipid objects. Two sets of the parameters were used for the description of lipid dynamic structure: (1) time-resolved fluorescence spectra and (2) time-resolved fluorescence depolarization as a function of rotational mobility of lipid molecules. Each measured dynamic parameter reflected the monotonous changes of dynamic properties in the range: lipid spheres-very low density lipoproteins-low density lipoproteins-high density lipoproteins-phospholipid liposomes. The range is characterized by the increase of the ratio polar/ nonpolar lipids. Thus, time-resolved fluorescence could be used to detect some structural modifications in lipoproteins related to atherosclerosis and subsequent cardiovascular diseases development

Ultra-Broadband Infrared Pulses from a Potassium-Titanyl Phosphate Optical Parametric Amplifier for VIS-IR-SFG Spectroscopy

Science.gov (United States)

Isaienko, Oleksandr; Borguet, Eric

A non-collinear KTP-OPA to provide ultra-broadband mid-infrared pulses was designed and characterized. With proper pulse-front and phase correction, the system has a potential for high-time resolution vibrational VIS-IR-SFG spectroscopy.

Photolytic interruptions of the bacteriorhodopsin photocycle examined by time-resolved resonance raman spectroscopy.

Science.gov (United States)

Grieger, I; Atkinson, G H

1985-09-24

An investigation of the photolytic conditions used to initiate and spectroscopically monitor the bacteriorhodopsin (BR) photocycle utilizing time-resolved resonance Raman (TR3) spectroscopy has revealed and characterized two photoinduced reactions that interrupt the thermal pathway. One reaction involves the photolytic interconversion of M-412 and M', and the other involves the direct photolytic conversion of the BR-570/K-590 photostationary mixture either to M-412 and M' or to M-like intermediates within 10 ns. The photolytic threshold conditions describing both reactions have been quantitatively measured and are discussed in terms of experimental parameters.

The application of time-resolved luminescence spectroscopy to a remote uranyl sensor

International Nuclear Information System (INIS)

Varineau, P.T.; Duesing, R.; Wangen, L.E.

1991-01-01

Time resolved luminescence spectroscopy is an effective method for the determination of a wide range of uranyl concentrations in aqueous samples. We have applied this technique to the development of a remote sensing device using fiber optic cables coupled with a micro flow cell in order to probe for uranyl in aqueous samples. This sensor incorporates a Nafion membrane through which UO 2 2+ can diffuse in to a reaction/analysis chamber which holds phosphoric acid, a reagent which enhances the uranyl luminescence intensity and lifetime. With this device, anionic and fluorescing organic interferences could be eliminated, allowing for the determination of uranyl over a concentration range of 10 4 to 10 -9 M. 17 refs., 5 figs

Ultrafast time-resolved spectroscopy of the light-harvesting complex 2 (LH2) from the photosynthetic bacterium Thermochromatium tepidum.

Science.gov (United States)

Niedzwiedzki, Dariusz M; Fuciman, Marcel; Kobayashi, Masayuki; Frank, Harry A; Blankenship, Robert E

2011-10-01

The light-harvesting complex 2 from the thermophilic purple bacterium Thermochromatium tepidum was purified and studied by steady-state absorption and fluorescence, sub-nanosecond-time-resolved fluorescence and femtosecond time-resolved transient absorption spectroscopy. The measurements were performed at room temperature and at 10 K. The combination of both ultrafast and steady-state optical spectroscopy methods at ambient and cryogenic temperatures allowed the detailed study of carotenoid (Car)-to-bacteriochlorophyll (BChl) as well BChl-to-BChl excitation energy transfer in the complex. The studies show that the dominant Cars rhodopin (N=11) and spirilloxanthin (N=13) do not play a significant role as supportive energy donors for BChl a. This is related with their photophysical properties regulated by long π-electron conjugation. On the other hand, such properties favor some of the Cars, particularly spirilloxanthin (N=13) to play the role of the direct quencher of the excited singlet state of BChl. © Springer Science+Business Media B.V. 2011

Structure-activity relationships of heterogeneous catalysts from time-resolved X-ray absorption spectroscopy

International Nuclear Information System (INIS)

Ressler, T.; Jentoft, R.E.; Wienold, J.; Girgsdies, F.; Neisius, T.; Timpe, O.

2003-01-01

Knowing the composition and the evolution of the bulk structure of a heterogeneous catalyst under working conditions (in situ) is a pre-requisite for understanding structure-activity relationships. X-ray absorption spectroscopy can be employed to study a catalytically active material in situ. In addition to steady-state investigations, the technique permits experiments with a time-resolution in the sub-second range to elucidate the solid-state kinetics of the reactions involved. Combined with mass spectrometry, the evolution of the short-range order structure of a heterogeneous catalyst, the average valence of the constituent metals, and the phase composition can be obtained. Here we present results obtained from time-resolved studies on the reduction of MoO 3 in propene and in propene and oxygen

Decay time shortening of fluorescence from donor-acceptor pair proteins using ultrafast time-resolved fluorescence resonance energy transfer spectroscopy

International Nuclear Information System (INIS)

Baba, Motoyoshi; Suzuki, Masayuki; Ganeev, Rashid A.; Kuroda, Hiroto; Ozaki, Tsuneyuki; Hamakubo, Takao; Masuda, Kazuyuki; Hayashi, Masahiro; Sakihama, Toshiko; Kodama, Tatsuhiko; Kozasa, Tohru

2007-01-01

We improved an ultrafast time-resolved fluorescence resonance energy transfer (FRET) spectroscopy system and measured directly the decrease in the fluorescence decay time of the FRET signal, without any entanglement of components in the picosecond time scale from the donor-acceptor protein pairs (such as cameleon protein for calcium ion indicator, and ligand-activated GRIN-Go proteins pair). The drastic decrease in lifetime of the donor protein fluorescence under the FRET condition (e.g. a 47.8% decrease for a GRIN-Go protein pair) proves the deformation dynamics between donor and acceptor fluorescent proteins in an activated state of a mixed donor-acceptor protein pair. This study is the first clear evidence of physical contact of the GRIN-Go proteins pair using time-resolved FRET system. G protein-coupled receptors (GPCRs) are the most important protein family for the recognition of many chemical substances at the cell surface. They are the targets of many drugs. Simultaneously, we were able to observe the time-resolved spectra of luminous proteins at the initial stage under the FRET condition, within 10 ns from excitation. This new FRET system allows us to trace the dynamics of the interaction between proteins at the ligand-induced activated state, molecular structure change and combination or dissociation. It will be a key technology for the development of protein chip technology

Development of in situ time-resolved Raman spectroscopy facility for dynamic shock loading in materials

Science.gov (United States)

Chaurasia, S.; Rastogi, V.; Rao, U.; Sijoy, C. D.; Mishra, V.; Deo, M. N.

2017-11-01

The transient state of excitation and relaxation processes in materials under shock compression can be investigated by coupling the laser driven shock facility with Raman spectroscopy. For this purpose, a time resolved Raman spectroscopy setup has been developed to monitor the physical and the chemical changes such as phase transitions, chemical reactions, molecular kinetics etc., under shock compression with nanosecond time resolution. This system consist of mainly three parts, a 2 J/8 ns Nd:YAG laser system used for generation of pump and probe beams, a Raman spectrometer with temporal and spectral resolution of 1.2 ns and 3 cm-1 respectively and a target holder in confinement geometry assembly. Detailed simulation for the optimization of confinement geometry targets is performed. Time resolved measurement of polytetrafluoroethylene (PTFE) targets at focused laser intensity of 2.2 GW/cm2 has been done. The corresponding pressure in the Aluminum and PTFE are 3.6 and 1.7 GPa respectively. At 1.7 GPa in PTFE, a red shift of 5 cm-1 is observed for the CF2 twisting mode (291 cm-1). Shock velocity in PTFE is calculated by measuring rate of change of ratios of the intensity of Raman lines scattered from shocked volume to total volume of sample in the laser focal spot along the laser axis. The calculated shock velocity in PTFE is found to be 1.64 ± 0.16 km/s at shock pressure of 1.7 GPa, for present experimental conditions.

Time-resolved spectroscopy of nonequilibrium ionization in laser-produced plasmas

International Nuclear Information System (INIS)

Marjoribanks, R.S.

1988-01-01

The highly transient ionization characteristic of laser-produced plasmas at high energy densities has been investigated experimentally, using x-ray spectroscopy with time resolution of less than 20 ps. Spectroscopic diagnostics of plasma density and temperature were used, including line ratios, line profile broadening and continuum emission, to characterize the plasma conditions without relying immediately on ionization modeling. The experimentally measured plasma parameters were used as independent variables, driving an ionization code, as a test of ionization modeling, divorced from hydrodynamic calculations. Several state-of-the-art streak spectrographs, each recording a fiducial of the laser peak along with the time-resolved spectrum, characterized the laser heating of thin signature layers of different atomic numbers imbedded in plastic targets. A novel design of crystal spectrograph, with a conically curved crystal, was developed. Coupled with a streak camera, it provided high resolution (λ/ΔΛ > 1000) and a collection efficiency roughly 20-50 times that of planar crystal spectrographs, affording improved spectra for quantitative reduction and greater sensitivity for the diagnosis of weak emitters. Experimental results were compared to hydrocode and ionization code simulations, with poor agreement. The conclusions question the appropriateness of describing electron velocity distributions by a temperature parameter during the time of laser illumination and emphasis the importance of characterizing the distribution more generally

Direct Imaging of Transient Fano Resonances in N_{2} Using Time-, Energy-, and Angular-Resolved Photoelectron Spectroscopy.

Science.gov (United States)

Eckstein, Martin; Yang, Chung-Hsin; Frassetto, Fabio; Poletto, Luca; Sansone, Giuseppe; Vrakking, Marc J J; Kornilov, Oleg

2016-04-22

Autoionizing Rydberg states of molecular N_{2} are studied using time-, energy-, and angular-resolved photoelectron spectroscopy. A femtosecond extreme ultraviolet pulse with a photon energy of 17.5 eV excites the resonance and a subsequent IR pulse ionizes the molecule before the autoionization takes place. The angular-resolved photoelectron spectra depend on pump-probe time delay and allow for the distinguishing of two electronic states contributing to the resonance. The lifetime of one of the contributions is determined to be 14±1  fs, while the lifetime of the other appears to be significantly shorter than the time resolution of the experiment. These observations suggest that the Rydberg states in this energy region are influenced by the effect of interference stabilization and merge into a complex resonance.

Time-resolved diode laser infrared absorption spectroscopy of the nascent HCl in the infrared laser chemistry of 1,2-dichloro-1,1-difluoroethane

Science.gov (United States)

Dietrich, Peter; Quack, Martin; Seyfang, George

1990-04-01

The IR multiphoton excitation and the frequency, fluence and intensity dependence of the IR-laser chemical yields of CF 2ClCH 2Cl have been studied in the fluence range of 1 to 10 J cm -2 yielding a steady-state constant k(st)/ I=0.74×10 6 s -1 MW -1 cm 2 which is approximately independent of intensity. Time-resolved IR absorption spectroscopy with diode laser sources has been used to observe the nascent HCl during the first few 100 ns indicating a population inversion between the levels ν=1, J=4 and ν=2, J=5. At low reactant pressures ( p⩽10 Pa) the time-resolved measurement gives a steady-state rate constant consistent with the theoretical result adjusted to the static yield measurements. The capability of state-selective and time-resolved IR spectroscopy is thus demonstrated, giving real-time determinations of rate constants.

A high-efficiency spin-resolved photoemission spectrometer combining time-of-flight spectroscopy with exchange-scattering polarimetry

Energy Technology Data Exchange (ETDEWEB)

Jozwiak, Chris M.; Graff, Jeff; Lebedev, Gennadi; Andresen, Nord; Schmid, Andreas; Fedorov, Alexei; El Gabaly, Farid; Wan, Weishi; Lanzara, Alessandra; Hussain, Zahid

2010-04-13

We describe a spin-resolved electron spectrometer capable of uniquely efficient and high energy resolution measurements. Spin analysis is obtained through polarimetry based on low-energy exchange scattering from a ferromagnetic thin-film target. This approach can achieve a similar analyzing power (Sherman function) as state-of-the-art Mott scattering polarimeters, but with as much as 100 times improved efficiency due to increased reflectivity. Performance is further enhanced by integrating the polarimeter into a time-of-flight (TOF) based energy analysis scheme with a precise and flexible electrostatic lens system. The parallel acquisition of a range of electron kinetic energies afforded by the TOF approach results in an order of magnitude (or more) increase in efficiency compared to hemispherical analyzers. The lens system additionally features a 90 degrees bandpass filter, which by removing unwanted parts of the photoelectron distribution allows the TOF technique to be performed at low electron drift energy and high energy resolution within a wide range of experimental parameters. The spectrometer is ideally suited for high-resolution spin- and angle-resolved photoemission spectroscopy (spin-ARPES), and initial results are shown. The TOF approach makes the spectrometer especially ideal for time-resolved spin-ARPES experiments.

Time-resolved photoelectron spectroscopy using synchrotron radiation time structure

International Nuclear Information System (INIS)

Bergeard, N.; Silly, M.G.; Chauvet, C.; Guzzo, M.; Ricaud, J.P.; Izquierdo, M.; Sirotti, F.; Krizmancic, D.; Guzzo, M.; Stebel, L.; Pittana, P.; Sergo, R.; Cautero, G.; Dufour, G.; Rochet, F.

2011-01-01

Synchrotron radiation time structure is becoming a common tool for studying dynamic properties of materials. The main limitation is often the wide time domain the user would like to access with pump-probe experiments. In order to perform photoelectron spectroscopy experiments over time scales from milliseconds to picoseconds it is mandatory to measure the time at which each measured photoelectron was created. For this reason the usual CCD camera based two-dimensional detection of electron energy analyzers has been replaced by a new delay-line detector adapted to the time structure of the SOLEIL synchrotron radiation source. The new two-dimensional delay-line detector has a time resolution of 5 ns and was installed on a Scienta SES 2002 electron energy analyzer. The first application has been to characterize the time of flight of the photo emitted electrons as a function of their kinetic energy and the selected pass energy. By repeating the experiment as a function of the available pass energy and of the kinetic energy, a complete characterization of the analyzer behaviour in the time domain has been obtained. Even for kinetic energies as low as 10 eV at 2 eV pass energy, the time spread of the detected electrons is lower than 140 ns. These results and the time structure of the SOLEIL filling modes assure the possibility of performing pump-probe photoelectron spectroscopy experiments with the time resolution given by the SOLEIL pulse width, the best performance of the beamline and of the experimental station. (authors)

Insights into the charge carrier terahertz mobility in polyfluorenes from large-scale atomistic simulations and time-resolved terahertz spectroscopy

Czech Academy of Sciences Publication Activity Database

Vukmirović, N.; Ponseca, C.S.; Němec, Hynek; Yartsev, A.; Sundström, V.

2012-01-01

Roč. 116, č. 37 (2012), s. 19665-1972 ISSN 1932-7447 Institutional research plan: CEZ:AV0Z10100520 Keywords : charge carrier mobility * time-resolved terahertz spectroscopy * multiscale atomistic calculations Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 4.814, year: 2012

Kinetics of the reaction F+NO+M->FNO+M studied by pulse radiolysis combined with time-resolved IR and UV spectroscopy

DEFF Research Database (Denmark)

Pagsberg, Palle Bjørn; Sillesen, A.; Jodkowski, J.T.

1996-01-01

The title reaction was initiated by pulse radiolysis of SF6/NO gas mixtures, and the formation of FNO was studied by time-resolved IR and UV spectroscopy. At SF6 pressures of 10-320 mbar at 298 K, the formation of FNO was studied by infrared diode laser spectroscopy at 1857.324 cm(-1). Comparative...

System for time-resolved laser absorption spectroscopy and its application to high-power impulse magnetron sputtering

Czech Academy of Sciences Publication Activity Database

Adámek, Petr; Olejníček, Jiří; Hubička, Zdeněk; Čada, Martin; Kment, Štěpán; Kohout, Michal; Do, H.T.

2017-01-01

Roč. 88, č. 2 (2017), 1-8, č. článku 023105. ISSN 0034-6748 R&D Projects: GA TA ČR(CZ) TF01000084; GA ČR(CZ) GA15-00863S Institutional support: RVO:68378271 Keywords : plasma diagnostics * HiPIMS * time resolved measurement * laser absorption spectroscopy Subject RIV: BL - Plasma and Gas Discharge Physics OBOR OECD: Fluids and plasma physics (including surface physics) Impact factor: 1.515, year: 2016

Quantitative terahertz time-domain spectroscopy and analysis in chemistry and biology

DEFF Research Database (Denmark)

Jepsen, Peter Uhd

2005-01-01

I will describe how Terahertz Time-Domain Spectroscopy (THz-TDS) can be used for quantitative, broadband spectroscopy in the far-infrared spectral region. Thz-TDS is sensitive to long-range, non-covalent interactions in the condensed phase, for instance intermolecular hydrogen bonding in molecula...

Rapid high-resolution spin- and angle-resolved photoemission spectroscopy with pulsed laser source and time-of-flight spectrometer

Science.gov (United States)

Gotlieb, K.; Hussain, Z.; Bostwick, A.; Lanzara, A.; Jozwiak, C.

2013-09-01

A high-efficiency spin- and angle-resolved photoemission spectroscopy (spin-ARPES) spectrometer is coupled with a laboratory-based laser for rapid high-resolution measurements. The spectrometer combines time-of-flight (TOF) energy measurements with low-energy exchange scattering spin polarimetry for high detection efficiencies. Samples are irradiated with fourth harmonic photons generated from a cavity-dumped Ti:sapphire laser that provides high photon flux in a narrow bandwidth, with a pulse timing structure ideally matched to the needs of the TOF spectrometer. The overall efficiency of the combined system results in near-EF spin-resolved ARPES measurements with an unprecedented combination of energy resolution and acquisition speed. This allows high-resolution spin measurements with a large number of data points spanning multiple dimensions of interest (energy, momentum, photon polarization, etc.) and thus enables experiments not otherwise possible. The system is demonstrated with spin-resolved energy and momentum mapping of the L-gap Au(111) surface states, a prototypical Rashba system. The successful integration of the spectrometer with the pulsed laser system demonstrates its potential for simultaneous spin- and time-resolved ARPES with pump-probe based measurements.

Time-resolved photoelectron spectrometry of a dephasing process in pyrazine

International Nuclear Information System (INIS)

Pavlov, R.L.; Pavlov, L.I.; Delchev, Ya.I.; Pavlova, S.I.

2001-01-01

The first femtosecond time-resolved photoelectron imaging (PEI) is presented. The method is characterized by photoionization of NO and further applied to ultrafast dephasing in pyrazine. Intermediate case behaviour in radiationless transition is clearly observed in time-resolved photoelectron kinetic energy distribution. Femtosecond PEI is with much improved efficiency than conventional photoelectron spectroscopies. It is anticipated that the unifield approach of time-resolved photoelectron and photoion imaging opens the possibility of observing photon-induced dynamics in real time

Noninvasive observation of skeletal muscle contraction using near-infrared time-resolved reflectance and diffusing-wave spectroscopy

Science.gov (United States)

Belau, Markus; Ninck, Markus; Hering, Gernot; Spinelli, Lorenzo; Contini, Davide; Torricelli, Alessandro; Gisler, Thomas

2010-09-01

We introduce a method for noninvasively measuring muscle contraction in vivo, based on near-infrared diffusing-wave spectroscopy (DWS). The method exploits the information about time-dependent shear motions within the contracting muscle that are contained in the temporal autocorrelation function g(1)(τ,t) of the multiply scattered light field measured as a function of lag time, τ, and time after stimulus, t. The analysis of g(1)(τ,t) measured on the human M. biceps brachii during repetitive electrical stimulation, using optical properties measured with time-resolved reflectance spectroscopy, shows that the tissue dynamics giving rise to the speckle fluctuations can be described by a combination of diffusion and shearing. The evolution of the tissue Cauchy strain e(t) shows a strong correlation with the force, indicating that a significant part of the shear observed with DWS is due to muscle contraction. The evolution of the DWS decay time shows quantitative differences between the M. biceps brachii and the M. gastrocnemius, suggesting that DWS allows to discriminate contraction of fast- and slow-twitch muscle fibers.

Probing the influence of X-rays on aqueous copper solutions using time-resolved in situ combined video/X-ray absorption near-edge/ultraviolet-visible spectroscopy

NARCIS (Netherlands)

Mesu, J. Gerbrand; Beale, Andrew M.; de Groot, Frank M. F.; Weckhuysen, Bert M.

2006-01-01

Time-resolved in situ video monitoring and ultraviolet-visible spectroscopy in combination with X-ray absorption near-edge spectroscopy (XANES) have been used for the first time in a combined manner to study the effect of synchrotron radiation on a series of homogeneous aqueous copper solutions in a

Underresolved absorption spectroscopy of OH radicals in flames using broadband UV LEDs

Science.gov (United States)

White, Logan; Gamba, Mirko

2018-04-01

A broadband absorption spectroscopy diagnostic based on underresolution of the spectral absorption lines is evaluated for the inference of species mole fraction and temperature in combustion systems from spectral fitting. The approach uses spectrally broadband UV light emitting diodes and leverages low resolution, small form factor spectrometers. Through this combination, the method can be used to develop high precision measurement sensors. The challenges of underresolved spectroscopy are explored and addressed using spectral derivative fitting, which is found to generate measurements with high precision and accuracy. The diagnostic is demonstrated with experimental measurements of gas temperature and OH mole fraction in atmospheric air/methane premixed laminar flat flames. Measurements exhibit high precision, good agreement with 1-D flame simulations, and high repeatability. A newly developed model of uncertainty in underresolved spectroscopy is applied to estimate two-dimensional confidence regions for the measurements. The results of the uncertainty analysis indicate that the errors in the outputs of the spectral fitting procedure are correlated. The implications of the correlation between uncertainties for measurement interpretation are discussed.

Study of the Bulk Charge Carrier Dynamics in Anatase and Rutile TiO2 Single Crystals by Femtosecond Time Resolved Spectroscopy

KAUST Repository

Maity, Partha; Mohammed, Omar F.; Katsiev, Khabiboulakh; Idriss, Hicham

2018-01-01

as the best model for fundamental studies. Their ultrafast charge carrier dynamics especially on TiO2 anatase single crystal (the most active phase) are unresolved. Here femtosecond time resolved spectroscopy (TRS) was carried out to explore the dynamics

Distortion dependent intersystem crossing: A femtosecond time-resolved photoelectron spectroscopy study of benzene, toluene, and p-xylene

Directory of Open Access Journals (Sweden)

Anne B. Stephansen

2017-07-01

Full Text Available The competition between ultrafast intersystem crossing and internal conversion in benzene, toluene, and p-xylene is investigated with time-resolved photoelectron spectroscopy and quantum chemical calculations. By exciting to S2 out-of-plane symmetry breaking, distortions are activated at early times whereupon spin-forbidden intersystem crossing becomes (partly allowed. Natural bond orbital analysis suggests that the pinnacle carbon atoms distorting from the aromatic plane change hybridization between the planar Franck-Condon geometry and the deformed (boat-shaped S2 equilibrium geometry. The effect is observed to increase in the presence of methyl-groups on the pinnacle carbon-atoms, where largest extents of σ and π orbital-mixing are observed. This is fully consistent with the time-resolved spectroscopy data: Toluene and p-xylene show evidence for ultrafast triplet formation competing with internal conversion, while benzene appears to only decay via internal conversion within the singlet manifold. For toluene and p-xylene, internal conversion to S1 and intersystem crossing to T3 occur within the time-resolution of our instrument. The receiver triplet state (T3 is found to undergo internal conversion in the triplet manifold within ≈100–150 fs (toluene or ≈180–200 fs (p-xylene as demonstrated by matching rise and decay components of upper and lower triplet states. Overall, the effect of methylation is found to both increase the intersystem crossing probability and direct the molecular axis of the excited state dynamics.

Femtosecond time-resolved impulsive stimulated Raman spectroscopy using sub-7-fs pulses: Apparatus and applications

Energy Technology Data Exchange (ETDEWEB)

Kuramochi, Hikaru [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako 351-0198 (Japan); Takeuchi, Satoshi; Tahara, Tahei, E-mail: tahei@riken.jp [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako 351-0198 (Japan); Ultrafast Spectroscopy Research Team, RIKEN Center for Advanced Photonics (RAP), 2-1 Hirosawa, Wako 351-0198 (Japan)

2016-04-15

We describe details of the setup for time-resolved impulsive stimulated Raman spectroscopy (TR-ISRS). In this method, snapshot molecular vibrational spectra of the photoreaction transients are captured via time-domain Raman probing using ultrashort pulses. Our instrument features transform-limited sub-7-fs pulses to impulsively excite and probe coherent nuclear wavepacket motions, allowing us to observe vibrational fingerprints of transient species from the terahertz to 3000-cm{sup −1} region with high sensitivity. Key optical components for the best spectroscopic performance are discussed. The TR-ISRS measurements for the excited states of diphenylacetylene in cyclohexane are demonstrated, highlighting the capability of our setup to track femtosecond dynamics of all the Raman-active fundamental molecular vibrations.

Ultrafast optical responses of {beta}-carotene and lycopene probed by sub-20-fs time-resolved coherent spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Fujiwara, M.; Sugisaki, M. [CREST-JST and Department of Physics, Osaka City University, Osaka 558-8585 (Japan); Gall, A.; Robert, B. [CEA, Institut de Biologie et Technologies de Saclay, and CNRS, Gif-sur-Yvette F-91191 (France); Cogdell, R.J. [IBLS, Glasgow Biomedical Research Centre, University of Glasgow, Glasgow G12 8QQ, Scotland (United Kingdom); Hashimoto, H., E-mail: hassy@sci.osaka-cu.ac.j [CREST-JST and Department of Physics, Osaka City University, Osaka 558-8585 (Japan)

2009-12-15

We investigate how structural distortions in carotenoid cause decoherences of its high-frequency vibrational modes by applying the sub-20-fs time-resolved transient grating spectroscopy to {beta}-carotene and lycopene. The results indicate that the C=C central stretching mode shows significant loss of coherence under the effects of the steric hindrance between {beta}-ionone ring and polyene backbone, whereas the other high-frequency modes do not show such dependency on the structural distortions.

Ultrafast optical responses of β-carotene and lycopene probed by sub-20-fs time-resolved coherent spectroscopy

International Nuclear Information System (INIS)

Fujiwara, M.; Sugisaki, M.; Gall, A.; Robert, B.; Cogdell, R.J.; Hashimoto, H.

2009-01-01

We investigate how structural distortions in carotenoid cause decoherences of its high-frequency vibrational modes by applying the sub-20-fs time-resolved transient grating spectroscopy to β-carotene and lycopene. The results indicate that the C=C central stretching mode shows significant loss of coherence under the effects of the steric hindrance between β-ionone ring and polyene backbone, whereas the other high-frequency modes do not show such dependency on the structural distortions.

Studies of Minerals, Organic and Biogenic Materials through Time-Resolved Raman Spectroscopy

Science.gov (United States)

Garcia, Christopher S.; Abedin, M. Nurul; Ismail, Syed; Sharma, Shiv K.; Misra, Anupam K.; Nyugen, Trac; Elsayed-Ali, hani

2009-01-01

A compact remote Raman spectroscopy system was developed at NASA Langley Research center and was previously demonstrated for its ability to identify chemical composition of various rocks and minerals. In this study, the Raman sensor was utilized to perform time-resolved Raman studies of various samples such as minerals and rocks, Azalea leaves and a few fossil samples. The Raman sensor utilizes a pulsed 532 nm Nd:YAG laser as excitation source, a 4-inch telescope to collect the Raman-scattered signal from a sample several meters away, a spectrograph equipped with a holographic grating, and a gated intensified CCD (ICCD) camera system. Time resolved Raman measurements were carried out by varying the gate delay with fixed short gate width of the ICCD camera, allowing measurement of both Raman signals and fluorescence signals. Rocks and mineral samples were characterized including marble, which contain CaCO3. Analysis of the results reveals the short (approx.10-13 s) lifetime of the Raman process, and shows that Raman spectra of some mineral samples contain fluorescence emission due to organic impurities. Also analyzed were a green (pristine) and a yellow (decayed) sample of Gardenia leaves. It was observed that the fluorescence signals from the green and yellow leaf samples showed stronger signals compared to the Raman lines. Moreover, it was also observed that the fluorescence of the green leaf was more intense and had a shorter lifetime than that of the yellow leaf. For the fossil samples, Raman shifted lines could not be observed due the presence of very strong short-lived fluorescence.

Frequency-comb-assisted broadband precision spectroscopy with cascaded diode lasers

DEFF Research Database (Denmark)

Liu, Junqiu; Brasch, Victor; Pfeiffer, Martin H. P.

2016-01-01

Frequency-comb-assisted diode laser spectroscopy, employing both the accuracy of an optical frequency comb and the broad wavelength tuning range of a tunable diode laser, has been widely used in many applications. In this Letter, we present a novel method using cascaded frequency agile diode lasers......, which allows us to extend the measurement bandwidth to 37.4 THz (1355-1630 nm) at megahertz resolution with scanning speeds above 1 THz/s. It is demonstrated as a useful tool to characterize a broadband spectrum for molecular spectroscopy, and in particular it enables us to characterize the dispersion...

Time- and Space-Resolved Spectroscopic Investigation on Pi-Conjugated Nanostructures - 2

Science.gov (United States)

2016-01-12

Defocused wide-field fluorescence (DWFI) microscopy suggests that molecular heterogeneities and flexibilities clearly depend on ring size and that site... Confocal   Microscopy   Setup Wild‐field  Microscopy   Setup Femtosecond Z‐scan  experiment Setup Figure 3. Instruments of Time- and space-resolved...approved for public release. 3. Space-Resolved Laser Spectroscopy - Confocal Microscopy - Wild-field Microscopy 4. Non-Linear Spectroscopy

Femtosecond time-resolved transient absorption spectroscopy of xanthophylls.

Science.gov (United States)

Niedzwiedzki, Dariusz M; Sullivan, James O; Polívka, Tomás; Birge, Robert R; Frank, Harry A

2006-11-16

Xanthophylls are a major class of photosynthetic pigments that participate in an adaptation mechanism by which higher plants protect themselves from high light stress. In the present work, an ultrafast time-resolved spectroscopic investigation of all the major xanthophyll pigments from spinach has been performed. The molecules are zeaxanthin, lutein, violaxanthin, and neoxanthin. beta-Carotene was also studied. The experimental data reveal the inherent spectral properties and ultrafast dynamics including the S(1) state lifetimes of each of the pigments. In conjunction with quantum mechanical computations the results address the molecular features of xanthophylls that control the formation and decay of the S* state in solution. The findings provide compelling evidence that S* is an excited state with a conformational geometry twisted relative to the ground state. The data indicate that S* is formed via a branched pathway from higher excited singlet states and that its yield depends critically on the presence of beta-ionylidene rings in the polyene system of pi-electron conjugated double bonds. The data are expected to be beneficial to researchers employing ultrafast time-resolved spectroscopic methods to investigate the mechanisms of both energy transfer and nonphotochemical quenching in higher plant preparations.

Broadband spectroscopy of magnetic response in a nano-scale magnetic wire

International Nuclear Information System (INIS)

Yamaguchi, A.; Motoi, K.; Miyajima, H.; Utsumi, Y.

2014-01-01

We measure the broadband spectra of magnetic response in a single layered ferromagnetic nano-scale wire in order to investigate the size effect on the ferromagnetic resonance. We found that the resonance frequency difference between 300-nm- and 5-μm-wide wires was varied by about 5 GHz due to the shape anisotropy. Furthermore, we experimentally detected the magnetization precession induced by the thermal fluctuation via the rectification of a radio-frequency (rf) current by incorporating an additional direct current (dc) by using Wheatstone bridge circuit. Our investigation renders that the shape anisotropy is of great importance to control the resonance frequency and to provide thermal stability of the microwave devices. - Highlights: • We describe an experimental investigation of the magnetic response of a single layered ferromagnetic nano-scale wire. • We present the conventional broadband microwave spectroscopy with a vector network analyzer and rectifying spectroscopy obtained with a Wheatstone bridge technique. • The investigation enables us to characterize the size effect on the ferromagnetic response and also to detect the magnetization precession induced by the thermal fluctuations

Exploration of CdTe quantum dots as mesoscale pressure sensors via time-resolved shock-compression photoluminescent emission spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Kang, Zhitao [Georgia Tech Research Institute, Georgia Institute of Technology, Atlanta, Georgia 30332-0826 (United States); School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0245 (United States); Banishev, Alexandr A.; Christensen, James; Dlott, Dana D. [School of Chemical Sciences and Fredrick Seitz Materials Research Laboratory, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801 (United States); Lee, Gyuhyon; Scripka, David A.; Breidenich, Jennifer; Summers, Christopher J.; Thadhani, Naresh N., E-mail: naresh.thadhani@mse.gatech.edu [School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0245 (United States); Xiao, Pan [LNM, Institute of Mechanics, Chinese Academy of Sciences, Beijing 100190 (China); George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0405 (United States); Zhou, Min [George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0405 (United States)

2016-07-28

The nanometer size of CdTe quantum dots (QDs) and their unique optical properties, including size-tunable narrow photoluminescent emission, broad absorption, fast photoluminescence decay, and negligible light scattering, are ideal features for spectrally tagging the shock response of localized regions in highly heterogeneous materials such as particulate media. In this work, the time-resolved laser-excited photoluminescence response of QDs to shock-compression was investigated to explore their utilization as mesoscale sensors for pressure measurements and in situ diagnostics during shock loading experiments. Laser-driven shock-compression experiments with steady-state shock pressures ranging from 2.0 to 13 GPa were performed on nanocomposite films of CdTe QDs dispersed in a soft polyvinyl alcohol polymer matrix and in a hard inorganic sodium silicate glass matrix. Time-resolved photoluminescent emission spectroscopy was used to correlate photoluminescence changes with the history of shock pressure and the dynamics of the matrix material surrounding the QDs. The results revealed pressure-induced blueshifts in emitted wavelength, decreases in photoluminescent emission intensity, reductions in peak width, and matrix-dependent response times. Data obtained for these QD response characteristics serve as indicators for their use as possible time-resolved diagnostics of the dynamic shock-compression response of matrix materials in which such QDs are embedded as in situ sensors.

Exploration of CdTe quantum dots as mesoscale pressure sensors via time-resolved shock-compression photoluminescent emission spectroscopy

International Nuclear Information System (INIS)

Kang, Zhitao; Banishev, Alexandr A.; Christensen, James; Dlott, Dana D.; Lee, Gyuhyon; Scripka, David A.; Breidenich, Jennifer; Summers, Christopher J.; Thadhani, Naresh N.; Xiao, Pan; Zhou, Min

2016-01-01

The nanometer size of CdTe quantum dots (QDs) and their unique optical properties, including size-tunable narrow photoluminescent emission, broad absorption, fast photoluminescence decay, and negligible light scattering, are ideal features for spectrally tagging the shock response of localized regions in highly heterogeneous materials such as particulate media. In this work, the time-resolved laser-excited photoluminescence response of QDs to shock-compression was investigated to explore their utilization as mesoscale sensors for pressure measurements and in situ diagnostics during shock loading experiments. Laser-driven shock-compression experiments with steady-state shock pressures ranging from 2.0 to 13 GPa were performed on nanocomposite films of CdTe QDs dispersed in a soft polyvinyl alcohol polymer matrix and in a hard inorganic sodium silicate glass matrix. Time-resolved photoluminescent emission spectroscopy was used to correlate photoluminescence changes with the history of shock pressure and the dynamics of the matrix material surrounding the QDs. The results revealed pressure-induced blueshifts in emitted wavelength, decreases in photoluminescent emission intensity, reductions in peak width, and matrix-dependent response times. Data obtained for these QD response characteristics serve as indicators for their use as possible time-resolved diagnostics of the dynamic shock-compression response of matrix materials in which such QDs are embedded as in situ sensors.

A Q-switched Ho:YAG laser assisted nanosecond time-resolved T-jump transient mid-IR absorbance spectroscopy with high sensitivity

Energy Technology Data Exchange (ETDEWEB)

Li, Deyong; Li, Yunliang; Li, Hao; Weng, Yuxiang, E-mail: yxweng@iphy.ac.cn [Key Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190 (China); Wu, Xianyou [Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031 (China); Yu, Qingxu [School of Physics and Optoelectronic Technology, Dalian University of Technology, No. 2, Linggong Road, Dalian 116023 (China)

2015-05-15

Knowledge of dynamical structure of protein is an important clue to understand its biological function in vivo. Temperature-jump (T-jump) time-resolved transient mid-IR absorbance spectroscopy is a powerful tool in elucidating the protein dynamical structures and the folding/unfolding kinetics of proteins in solution. A home-built setup of T-jump time-resolved transient mid-IR absorbance spectroscopy with high sensitivity is developed, which is composed of a Q-switched Cr, Tm, Ho:YAG laser with an output wavelength at 2.09 μm as the T-jump heating source, and a continuous working CO laser tunable from 1580 to 1980 cm{sup −1} as the IR probe. The results demonstrate that this system has a sensitivity of 1 × 10{sup −4} ΔOD for a single wavelength detection, and 2 × 10{sup −4} ΔOD for spectral detection in amide I′ region, as well as a temporal resolution of 20 ns. Moreover, the data quality coming from the CO laser is comparable to the one using the commercial quantum cascade laser.

Isotope effect on hydrated electron relaxation dynamics studied with time-resolved liquid jet photoelectron spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Elkins, Madeline H.; Williams, Holly L. [Department of Chemistry, University of California, Berkeley, California 94720 (United States); Neumark, Daniel M., E-mail: dneumark@berkeley.edu [Department of Chemistry, University of California, Berkeley, California 94720 (United States); Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

2016-05-14

The excited state relaxation dynamics of the solvated electron in H{sub 2}O and D{sub 2}O are investigated using time-resolved photoelectron spectroscopy in a liquid microjet. The data show that the initial excited state decays on a time scale of 75 ± 12 fs in H{sub 2}O and 102 ± 8 fs in D{sub 2}O, followed by slower relaxation on time scales of 400 ± 70 fs and 390 ± 70 fs that are isotopically invariant within the precision of our measurements. Based on the time evolution of the transient signals, the faster and slower time constants are assigned to p → s internal conversion (IC) of the hydrated electron and relaxation on the ground electronic state, respectively. This assignment is consistent with the non-adiabatic mechanism for relaxation of the hydrated electron and yields an isotope effect of 1.4 ± 0.2 for IC of the hydrated electron.

Isotope effect on hydrated electron relaxation dynamics studied with time-resolved liquid jet photoelectron spectroscopy

Science.gov (United States)

Elkins, Madeline H.; Williams, Holly L.; Neumark, Daniel M.

2016-05-01

The excited state relaxation dynamics of the solvated electron in H2O and D2O are investigated using time-resolved photoelectron spectroscopy in a liquid microjet. The data show that the initial excited state decays on a time scale of 75 ± 12 fs in H2O and 102 ± 8 fs in D2O, followed by slower relaxation on time scales of 400 ± 70 fs and 390 ± 70 fs that are isotopically invariant within the precision of our measurements. Based on the time evolution of the transient signals, the faster and slower time constants are assigned to p → s internal conversion (IC) of the hydrated electron and relaxation on the ground electronic state, respectively. This assignment is consistent with the non-adiabatic mechanism for relaxation of the hydrated electron and yields an isotope effect of 1.4 ± 0.2 for IC of the hydrated electron.

Direct angle resolved photoemission spectroscopy and ...

Indian Academy of Sciences (India)

Since 1997 we systematically perform direct angle resolved photoemission spectroscopy (ARPES) on in-situ grown thin (< 30 nm) cuprate films. Specifically, we probe low-energy electronic structure and properties of high-c superconductors (HTSC) under different degrees of epitaxial (compressive vs. tensile) strain.

Time resolved measurement of laser-ablated particles by LAPXAS (Laser Plasma Soft X-ray Absorption Spectroscopy)

International Nuclear Information System (INIS)

Miyashita, Atsumi; Yoda, Osamu; Murakami, Kouichi

1999-01-01

The time- and spatially-resolved properties of laser ablated carbon, boron and silicon particles were measured by LAPXAS (Laser Plasma Soft X-ray Absorption Spectroscopy). The maximum speed of positively charged ions is higher than those of neutral atoms and negatively charged ions. The spatial distributions of the laser-ablated particles in the localized rare gas environment were measured. In helium gas environment, by the helium cloud generated on the top of ablation plume depressed the ablation plume. There is no formation of silicon clusters till 15 μs after laser ablation in the argon gas environment. (author)

Indoor Measurement of Angle Resolved Light Absorption by Black Silicon

DEFF Research Database (Denmark)

Amdemeskel, Mekbib Wubishet; Iandolo, Beniamino; Davidsen, Rasmus Schmidt

2017-01-01

Angle resolved optical spectroscopy of photovoltaic (PV) samples gives crucial information on PV panels under realistic working conditions. Here, we introduce measurements of angle resolved light absorption by PV cells, performed indoors using a collimated high radiance broadband light source. Our...... indoor method offers a significant simplification as compared to measurements by solar trackers. As a proof-of-concept demonstration, we show characterization of black silicon solar cells. The experimental results showed stable and reliable optical responses that makes our setup suitable for indoor......, angle resolved characterization of solar cells....

Wide-field time-resolved luminescence imaging and spectroscopy to decipher obliterated documents in forensic science

Science.gov (United States)

Suzuki, Mototsugu; Akiba, Norimitsu; Kurosawa, Kenji; Kuroki, Kenro; Akao, Yoshinori; Higashikawa, Yoshiyasu

2016-01-01

We applied a wide-field time-resolved luminescence (TRL) method with a pulsed laser and a gated intensified charge coupled device (ICCD) for deciphering obliterated documents for use in forensic science. The TRL method can nondestructively measure the dynamics of luminescence, including fluorescence and phosphorescence lifetimes, which prove to be useful parameters for image detection. First, we measured the TRL spectra of four brands of black porous-tip pen inks on paper to estimate their luminescence lifetimes. Next, we acquired the TRL images of 12 obliterated documents at various delay times and gate times of the ICCD. The obliterated contents were revealed in the TRL images because of the difference in the luminescence lifetimes of the inks. This method requires no pretreatment, is nondestructive, and has the advantage of wide-field imaging, which makes it is easy to control the gate timing. This demonstration proves that TRL imaging and spectroscopy are powerful tools for forensic document examination.

Creation of free excitons in solid krypton investigated by time-resolved luminescence spectroscopy

International Nuclear Information System (INIS)

Kisand, Vambola; Kirm, Marco; Negodin, Evgeni; Sombrowski, Elke; Steeg, Barbara; Vielhauer, Sebastian; Zimmerer, Georg

2003-01-01

The creation and relaxation of secondary excitons in solid Kr was investigated using energy-and time-resolved luminescence spectroscopy in the vacuum ultraviolet region. The spectrally selected emission of the free exciton (FE) was used as a probe for an investigation of the different exciton creation processes. Delayed FE creation via electron-hole recombination and 'prompt' (in terms of the time-resolution of the experiment) creation of excitons were separated. The 'prompt' creation of a FE appears in the region above threshold energy E th , which is equal to the sum of the band gap energy and the free exciton energy. 'Prompt' creation of excitons above E th is ascribed to a superposition of two processes: (i) creation of the electronic polaron complex (one-step process) and (ii) inelastic scattering of photoelectrons described in the framework of the multiple-parabolic-branch band model (two-step process). In addition, the ratio spectrum of the time-integrated FE and self-trapped exciton (STE) emission was analysed. The behaviour of the ratio spectrum is a proof that electron-hole recombination leads to STE states through FE states as precursors

Time-resolved tunable diode laser absorption spectroscopy of excited argon and ground-state titanium atoms in pulsed magnetron discharges

Czech Academy of Sciences Publication Activity Database

Sushkov, V.; Do, H.T.; Čada, Martin; Hubička, Zdeněk; Hippler, R.

2013-01-01

Roč. 22, č. 1 (2013), 1-10 ISSN 0963-0252 R&D Projects: GA ČR(CZ) GAP205/11/0386; GA ČR GAP108/12/2104 Institutional research plan: CEZ:AV0Z10100522 Keywords : absorption spectroscopy * diode laser * magnetron * argon metastable * HiPIMS * titanium * time-resolved Subject RIV: BH - Optics, Masers, Lasers Impact factor: 3.056, year: 2013 http://iopscience.iop.org/0963-0252/22/1/015002/

Dynamics of Al/Fe{sub 2}O{sub 3} MIC combustion from short single-pulse photothermal initiation and time-resolved spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Stiegman, Albert E.; Park, Chi-Dong; Mileham, Melissa; Van de Burgt, Lambertus J. [Department of Chemistry and Biochemistry, Florida State University Tallahassee, FL (United States); Kramer, Michael P. [AFRL/MNME Eglin AFB, FL (United States)

2009-08-15

Time-resolved spectroscopy was used to study the dynamics of the photothermal ignition of Al/Fe{sub 2}O{sub 3} metastable intermolecular composites after single short-pulse laser initiation. The dynamics were recorded in several time domains from nanosecond to microsecond to quantify the dynamics from initial laser excitation to combustion. Time-averaged spectral data were also collected for the overall emission occurring during combustion. (Abstract Copyright [2009], Wiley Periodicals, Inc.)

Improved Fast, Deep Record Length, Time-Resolved Visible Spectroscopy of Plasmas Using Fiber Grids

Science.gov (United States)

Brockington, S.; Case, A.; Cruz, E.; Williams, A.; Witherspoon, F. D.; Horton, R.; Klauser, R.; Hwang, D.

2017-10-01

HyperV Technologies is developing a fiber-coupled, deep record-length, low-light camera head for performing high time resolution spectroscopy on visible emission from plasma events. By coupling the output of a spectrometer to an imaging fiber bundle connected to a bank of amplified silicon photomultipliers, time-resolved spectroscopic imagers of 100 to 1,000 pixels can be constructed. A second generation prototype 32-pixel spectroscopic imager employing this technique was constructed and successfully tested at the University of California at Davis Compact Toroid Injection Experiment (CTIX). Pixel performance of 10 Megaframes/sec with record lengths of up to 256,000 frames ( 25.6 milliseconds) were achieved. Pixel resolution was 12 bits. Pixel pitch can be refined by using grids of 100 μm to 1000 μm diameter fibers. Experimental results will be discussed, along with future plans for this diagnostic. Work supported by USDOE SBIR Grant DE-SC0013801.

SmB6 electron-phonon coupling constant from time- and angle-resolved photoelectron spectroscopy

Science.gov (United States)

Sterzi, A.; Crepaldi, A.; Cilento, F.; Manzoni, G.; Frantzeskakis, E.; Zacchigna, M.; van Heumen, E.; Huang, Y. K.; Golden, M. S.; Parmigiani, F.

2016-08-01

SmB6 is a mixed valence Kondo system resulting from the hybridization between localized f electrons and delocalized d electrons. We have investigated its out-of-equilibrium electron dynamics by means of time- and angle-resolved photoelectron spectroscopy. The transient electronic population above the Fermi level can be described by a time-dependent Fermi-Dirac distribution. By solving a two-temperature model that well reproduces the relaxation dynamics of the effective electronic temperature, we estimate the electron-phonon coupling constant λ to range from 0.13 ±0.03 to 0.04 ±0.01 . These extremes are obtained assuming a coupling of the electrons with either a phonon mode at 10 or 19 meV. A realistic value of the average phonon energy will give an actual value of λ within this range. Our results provide an experimental report on the material electron-phonon coupling, contributing to both the electronic transport and the macroscopic thermodynamic properties of SmB6.

Broadband terahertz spectroscopy: principles, fundamental research and potential for industrial applications

International Nuclear Information System (INIS)

Zouaghi, W; Thomson, M D; Rabia, K; Hahn, R; Blank, V; Roskos, H G

2013-01-01

Terahertz radiation (also called T-rays) can be employed for spectroscopy and imaging, from the laboratory to industrial applications. In this paper we give an overview of how broadband optoelectronic THz techniques (i.e. using optical lasers to achieve THz generation and detection) can be implemented, and give examples of their unique use in solid-state physics, and in biological and industrial applications. (paper)

Time resolved infrared spectroscopy of femtosecond proton dynamics in the liquid phase

International Nuclear Information System (INIS)

Amir, W.

2003-12-01

This work of thesis aims to understand the strong mobility of protons in water. Water is fundamental to life and mediates many chemical and biological processes. However this liquid is poorly understood at the molecular level. The richness of interdisciplinary sciences allows us to study the properties which make it so unique. The technique used for this study was the femtosecond time resolved vibrational spectroscopy. Several experiments were carried out to characterize the femtosecond proton dynamics in water. The visualization of the rotation of water molecules obtained by anisotropy measurements will be presented. This experiment is carried out in isotopic water HDO/D 2 O for reasons of experimental and theoretical suitability. However this is not water. Pure water H 2 O was also studied without thermal effects across vibrations modes. An intermolecular energy resonant transfer was observed. Finally the localized structure of the proton in water (called Eigen form) was clearly experimentally observed. This molecule is implicated in the abnormal mobility of the proton in water (Grotthuss mechanism). (author)

Coherent spectroscopies on ultrashort time and length scales

Directory of Open Access Journals (Sweden)

Schneider C.

2013-03-01

Full Text Available Three spectroscopic techniques are presented that provide simultaneous spatial and temporal resolution: modified confocal microscopy with heterodyne detection, space-time-resolved spectroscopy using coherent control concepts, and coherent two-dimensional nano-spectroscopy. Latest experimental results are discussed.

Time- and angle-resolved photoemission spectroscopy with optimized high-harmonic pulses using frequency-doubled Ti:Sapphire lasers

International Nuclear Information System (INIS)

Eich, S.; Stange, A.; Carr, A.V.; Urbancic, J.; Popmintchev, T.; Wiesenmayer, M.; Jansen, K.; Ruffing, A.; Jakobs, S.; Rohwer, T.; Hellmann, S.; Chen, C.; Matyba, P.; Kipp, L.; Rossnagel, K.; Bauer, M.; Murnane, M.M.; Kapteyn, H.C.; Mathias, S.; Aeschlimann, M.

2014-01-01

Highlights: • We present a scheme to generate high intensity XUV pulses from HHG with variable time-bandwidth product. • Shorter-wavelength driven high-harmonic XUV trARPES provides higher photon flux and increased energy resolution. • High-quality high-harmonic XUV trARPES data with sub 150 meV energy and sub 30 fs time resolution is presented. - Abstract: Time- and angle-resolved photoemission spectroscopy (trARPES) using femtosecond extreme ultraviolet high harmonics has recently emerged as a powerful tool for investigating ultrafast quasiparticle dynamics in correlated-electron materials. However, the full potential of this approach has not yet been achieved because, to date, high harmonics generated by 800 nm wavelength Ti:Sapphire lasers required a trade-off between photon flux, energy and time resolution. Photoemission spectroscopy requires a quasi-monochromatic output, but dispersive optical elements that select a single harmonic can significantly reduce the photon flux and time resolution. Here we show that 400 nm driven high harmonic extreme-ultraviolet trARPES is superior to using 800 nm laser drivers since it eliminates the need for any spectral selection, thereby increasing photon flux and energy resolution to <150 meV while preserving excellent time resolution of about 30 fs

Broadband dielectric spectroscopy and calorimetric investigations of D-lyxose.

Science.gov (United States)

Singh, Lokendra P; Alegría, A; Colmenero, J

2011-10-18

Using broadband dielectric spectroscopy, we have studied different types of relaxation processes, namely, primary (α), secondary (β), and another sub-T(g) process called γ-process, in the supercooled state of D-lyxose, over a wide frequency (10(-2)-10(9) Hz) and temperature range (120-340 K). In addition, the same sample was analyzed by differential scanning calorimeter. The temperature dependence of the relaxation times as well as the dielectric strength of different processes has been critically examined. It has been observed that the slower secondary relaxation (designated as β-) process shifts to lower frequencies with increasing applied pressure, but not the faster one. This pressure dependence indicates that the observed slower secondary relaxation (β-) is Johari-Goldstein relaxation process and faster one (γ-process) is probably the rotation of hydroxymethyl (-CH(2)OH) side group attached to the sugar ring, that is, of intramolecular origin. Copyright © 2011 Elsevier Ltd. All rights reserved.

Determination of quenching coefficients by time resolved emission spectroscopy

International Nuclear Information System (INIS)

Gans, T.; Schulz-von der Gathen, V.; Doebele, H.F.

2001-01-01

Capacitively coupled RF discharges (CCRF discharges) at 13.56 MHz in hydrogen exhibit a field reversal phase of about 10 ns during which an intense electron current provides collisional excitation, within the sheath region. After this strongly dominant short pulsed electron impact excitation, it is possible to determine quenching coefficients from the lifetime of the fluorescence at various pressures by time resolved OES even for high energy levels and without any restrictions of optical selection rules. This novel technique allows the measurement of quenching coefficients for atomic and molecular emission lines of hydrogen itself, as well as for emission lines of small admixtures (e.g. noble gases) to the hydrogen discharge, since with a fast gate-able ICCD camera operating at 13.56 MHz it is possible to measure even faint emission lines temporally resolved

Determination of quenching coefficients by time resolved emission spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Gans, T.; Schulz-von der Gathen, V.; Doebele, H.F. [Essen Univ. (Gesamthochschule) (Germany). Inst. fuer Laser- und Plasmaphysik

2001-07-01

Capacitively coupled RF discharges (CCRF discharges) at 13.56 MHz in hydrogen exhibit a field reversal phase of about 10 ns during which an intense electron current provides collisional excitation, within the sheath region. After this strongly dominant short pulsed electron impact excitation, it is possible to determine quenching coefficients from the lifetime of the fluorescence at various pressures by time resolved OES even for high energy levels and without any restrictions of optical selection rules. This novel technique allows the measurement of quenching coefficients for atomic and molecular emission lines of hydrogen itself, as well as for emission lines of small admixtures (e.g. noble gases) to the hydrogen discharge, since with a fast gate-able ICCD camera operating at 13.56 MHz it is possible to measure even faint emission lines temporally resolved.

Relaxations and fast dynamics of the plastic crystal cyclo-octanol investigated by broadband dielectric spectroscopy

OpenAIRE

Lunkenheimer, Peter

1997-01-01

Relaxations and fast dynamics of the plastic crystal cyclo-octanol investigated by broadband dielectric spectroscopy / R. Brand, P. Lunkenheimer, A. Loidl. - In: Physical review. B. 56. 1997. S. R5713-R5716

Linearity of Air-Biased Coherent Detection for Terahertz Time-Domain Spectroscopy

DEFF Research Database (Denmark)

Wang, Tianwu; Iwaszczuk, Krzysztof; Wrisberg, Emil Astrup

2016-01-01

The performance of air-biased coherent detection (ABCD) in a broadband two-color laser-induced air plasma system for terahertz time-domain spectroscopy (THz-TDS) has been investigated. Fundamental parameters of the ABCD detection, including signal-to-noise ratio (SNR), dynamic range (DR), and lin...

Highly Resolved Sub-Terahertz Vibrational Spectroscopy of Biological Macromolecules and Bacteria Cells

Science.gov (United States)

2016-07-01

HIGHLY RESOLVED SUB-TERAHERTZ VIBRATIONAL SPECTROSCOPY OF BIOLOGICAL MACROMOLECULES AND BACTERIA CELLS ECBC...SUBTITLE Highly Resolved Sub-Terahertz Vibrational Spectroscopy of Biological Macromolecules and Bacteria Cells 5a. CONTRACT NUMBER W911SR-14-P...22 4.3 Bacteria THz Study

Resolving molecular vibronic structure using high-sensitivity two-dimensional electronic spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Bizimana, Laurie A.; Brazard, Johanna; Carbery, William P.; Gellen, Tobias; Turner, Daniel B., E-mail: dturner@nyu.edu [Department of Chemistry, New York University, 100 Washington Square East, New York, New York 10003 (United States)

2015-10-28

Coherent multidimensional optical spectroscopy is an emerging technique for resolving structure and ultrafast dynamics of molecules, proteins, semiconductors, and other materials. A current challenge is the quality of kinetics that are examined as a function of waiting time. Inspired by noise-suppression methods of transient absorption, here we incorporate shot-by-shot acquisitions and balanced detection into coherent multidimensional optical spectroscopy. We demonstrate that implementing noise-suppression methods in two-dimensional electronic spectroscopy not only improves the quality of features in individual spectra but also increases the sensitivity to ultrafast time-dependent changes in the spectral features. Measurements on cresyl violet perchlorate are consistent with the vibronic pattern predicted by theoretical models of a highly displaced harmonic oscillator. The noise-suppression methods should benefit research into coherent electronic dynamics, and they can be adapted to multidimensional spectroscopies across the infrared and ultraviolet frequency ranges.

Detecting aromatic compounds on planetary surfaces using ultraviolet time-resolved fluorescence spectroscopy

Science.gov (United States)

Eshelman, E.; Daly, M. G.; Slater, G.; Cloutis, E.

2018-02-01

Many aromatic organic molecules exhibit strong and characteristic fluorescence when excited with ultraviolet radiation. As laser excitation in the ultraviolet generates both fluorescence and resonantly enhanced Raman scattering of aromatic vibrational modes, combined Raman and fluorescence instruments have been proposed to search for organic compounds on Mars. In this work the time-resolved fluorescence of a suite of 24 compounds composed of 2-5 ringed alternant, non-alternant, and heterocyclic PAHs was measured. Fluorescence instrumentation with similar specifications to a putative flight instrument was capable of observing the fluorescence decay of these compounds with a sub-ns resolution. Incorporating time-resolved capabilities was also found to increase the ability to discriminate between individual PAHs. Incorporating time-resolved fluorescence capabilities into an ultraviolet gated Raman system intended for a rover or lander can increase the ability to detect and characterize PAHs on planetary surfaces.

Spectroscopie de Fourier par peignes de fréquences femtosecondes

OpenAIRE

Mandon , Julien

2009-01-01

This work presents results towards the development of a novel frequency-comb based Fourier transform spectroscopy (FTS). Since 1970, due to its exceptional qualities, FTS has offered a simple way for spectral analysis and has assumed a position of dominance for the measurement of broadband well-resolved accurate spectra. However, FTS doesn't satisfy the new requirements in molecular physics. Acquisition time at the limit, extreme resolution, broad spectral extension, high sensitivity, and acc...

Nonadiabatic Dynamics May Be Probed through Electronic Coherence in Time-Resolved Photoelectron Spectroscopy.

Science.gov (United States)

Bennett, Kochise; Kowalewski, Markus; Mukamel, Shaul

2016-02-09

We present a hierarchy of Fermi golden rules (FGRs) that incorporate strongly coupled electronic/nuclear dynamics in time-resolved photoelectron spectroscopy (TRPES) signals at different levels of theory. Expansion in the joint electronic and nuclear eigenbasis yields the numerically most challenging exact FGR (eFGR). The quasistatic Fermi Golden Rule (qsFGR) neglects nuclear motion during the photoionization process but takes into account electronic coherences as well as populations initially present in the pumped matter as well as those generated internally by coupling between electronic surfaces. The standard semiclassical Fermi Golden Rule (scFGR) neglects the electronic coherences and the nuclear kinetic energy during the ionizing pulse altogether, yielding the classical Condon approximation. The coherence contributions depend on the phase-profile of the ionizing field, allowing coherent control of TRPES signals. The photoelectron spectrum from model systems is simulated using these three levels of theory. The eFGR and the qsFGR show temporal oscillations originating from the electronic or vibrational coherences generated as the nuclear wave packet traverses a conical intersection. These oscillations, which are missed by the scFGR, directly reveal the time-evolving splitting between electronic states of the neutral molecule in the curve-crossing regime.

Time-resolved materials science opportunities using synchrotron x-ray sources

International Nuclear Information System (INIS)

Larson, B.C.; Tischler, J.Z.

1995-06-01

The high brightness, high intensity, and pulsed time-structure of synchrotron sources provide new opportunities for time-resolved x-ray diffraction investigations. With third generation synchrotron sources coming on line, high brilliance and high brightness are now available in x-ray beams with the highest flux. In addition to the high average flux, the instantaneous flux available in synchrotron beams is greatly enhanced by the pulsed time structure, which consists of short bursts of x-rays that are separated by ∼tens to hundreds of nanoseconds. Time-resolved one- and two-dimensional position sensitive detection techniques that take advantage of synchrotron radiation for materials science x-ray diffraction investigations are presented, and time resolved materials science applications are discussed in terms of recent diffraction and spectroscopy results and materials research opportunities

Time resolved super continuum Cavity Ring-Down Spectroscopy for multicomponent gas detection

International Nuclear Information System (INIS)

Nakaema, Walter Morinobu

2010-01-01

In this work, we present a variation of the technique CRDS (Cavity Ring-Down Spectroscopy) to obtain simultaneously a multicomponent absorption spectrum in a broad visible range. This new approach uses the Supercontinuum (SC) spectrum (resulting from irradiation of nonlinear media by femtosecond lasers, or simply generated by compact sources) as a light source to illuminate the cavity. In this context it is described the features of the modules assembling a MC-SC-CRDS (Multicomponent Supercontinuum Cavity Ring-Down Spectroscopy): a set of high reflectivity mirrors, the resonant cavity and the detection system. Some problems related to the multimode excitation, stray light, effective use of the dynamic range of the detector, the poor resolution of the instrument to resolve narrow absorption lines are issued. We present the absorption spectra of H 2 O (polyads 4υ, 4υ + δ) and O 2 (spin-forbidden b-X branch) measured simultaneously by this technique in the visible range and a comparison with the absorption lines based on HITRAN database is made to demonstrate the functionality of this method. (author)

Studies of the reactions of hydrogen atoms by time-resolved E. S. R. spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Fessenden, R W; Verma, N C [Carnegie-Mellon Univ., Pittsburgh, Pa. (USA). Dept. of Chemistry

1977-01-01

Time-resolved e.s.r. spectroscopy has been used to follow directly the reactions of H atoms produced by pulse radiolysis of acid solutions. Detailed analysis of the time profile of the e.s.r. signal was carried out by means of modified Bloch equations. The increased signal found when a scavenger for OH such as t-butyl alcohol is present is shown to be mainly the result of slower H atom decay by radical-radical reaction. The reaction H + OH does not appear to produce any signal polarization. The decay curves observed in the presence of solute are readily accounted for by the treatment, and good plots of pseudo first-order rate constant against solute concentration are obtained. The absolute rate constants for reaction with H atoms are for methanol 2.5 x10/sup 6/, for ethanol 2.1 X 10/sup 7/, for isopropanol 6.8 x 10/sup 7/, and for succinic acid 3.0 x 10/sup 6/ dm/sup 3/ mol/sup -1/s/sup -1/. These values are in good agreement with the earlier chemical measurements.

Laser plasma x-ray source for ultrafast time-resolved x-ray absorption spectroscopy

Directory of Open Access Journals (Sweden)

L. Miaja-Avila

2015-03-01

Full Text Available We describe a laser-driven x-ray plasma source designed for ultrafast x-ray absorption spectroscopy. The source is comprised of a 1 kHz, 20 W, femtosecond pulsed infrared laser and a water target. We present the x-ray spectra as a function of laser energy and pulse duration. Additionally, we investigate the plasma temperature and photon flux as we vary the laser energy. We obtain a 75 μm FWHM x-ray spot size, containing ∼106 photons/s, by focusing the produced x-rays with a polycapillary optic. Since the acquisition of x-ray absorption spectra requires the averaging of measurements from >107 laser pulses, we also present data on the source stability, including single pulse measurements of the x-ray yield and the x-ray spectral shape. In single pulse measurements, the x-ray flux has a measured standard deviation of 8%, where the laser pointing is the main cause of variability. Further, we show that the variability in x-ray spectral shape from single pulses is low, thus justifying the combining of x-rays obtained from different laser pulses into a single spectrum. Finally, we show a static x-ray absorption spectrum of a ferrioxalate solution as detected by a microcalorimeter array. Altogether, our results demonstrate that this water-jet based plasma source is a suitable candidate for laboratory-based time-resolved x-ray absorption spectroscopy experiments.

BROADBAND X-RAY IMAGING AND SPECTROSCOPY OF THE CRAB NEBULA AND PULSAR WITH NuSTAR

International Nuclear Information System (INIS)

Madsen, Kristin K.; Harrison, Fiona; Grefenstette, Brian W.; Reynolds, Stephen; An, Hongjun; Boggs, Steven; Craig, William W.; Zoglauer, Andreas; Christensen, Finn E.; Fryer, Chris L.; Hailey, Charles J.; Nynka, Melania; Markwardt, Craig; Zhang, William; Stern, Daniel

2015-01-01

We present broadband (3-78 keV) NuSTAR X-ray imaging and spectroscopy of the Crab nebula and pulsar. We show that while the phase-averaged and spatially integrated nebula + pulsar spectrum is a power law in this energy band, spatially resolved spectroscopy of the nebula finds a break at ∼9 keV in the spectral photon index of the torus structure with a steepening characterized by ΔΓ ∼ 0.25. We also confirm a previously reported steepening in the pulsed spectrum, and quantify it with a broken power law with break energy at ∼12 keV and ΔΓ ∼ 0.27. We present spectral maps of the inner 100'' of the remnant and measure the size of the nebula as a function of energy in seven bands. These results find that the rate of shrinkage with energy of the torus size can be fitted by a power law with an index of γ = 0.094 ± 0.018, consistent with the predictions of Kennel and Coroniti. The change in size is more rapid in the NW direction, coinciding with the counter-jet where we find the index to be a factor of two larger. NuSTAR observed the Crab during the latter part of a γ-ray flare, but found no increase in flux in the 3-78 keV energy band

In situ time-resolved X-ray near-edge absorption spectroscopy of selenite reduction by siderite

International Nuclear Information System (INIS)

Badaut, V.; Schlegel, M.L.; Descostes, M.; Moutiers, G.

2012-01-01

The reduction oxidation-reaction between aqueous selenite (SeO 3 2- ) and siderite (FeCO 3 (s)) was monitored by in situ, time-resolved X-ray absorption near-edge structure (XANES) spectroscopy at the selenium K edge in a controlled electrochemical environment. Spectral evolutions showed that more than 60% of selenite was reduced at the siderite surface after 20 h of experiment, at which time the reaction was still incomplete. Fitting of XANES spectra by linear combination of reference spectra showed that selenite reaction with siderite is essentially a two-step process, selenite ions being immobilized on siderite surface prior to their reduction. A kinetic model of the reduction step is proposed, allowing to identify the specific contribution of surface reduction. These results have strong implications for the retention of selenite by corrosion products in nuclear waste repositories and in a larger extent for the fate of selenium in the environment. (authors)

Time domain diffuse optical spectroscopy: In vivo quantification of collagen in breast tissue

Science.gov (United States)

Taroni, Paola; Pifferi, Antonio; Quarto, Giovanna; Farina, Andrea; Ieva, Francesca; Paganoni, Anna Maria; Abbate, Francesca; Cassano, Enrico; Cubeddu, Rinaldo

2015-05-01

Time-resolved diffuse optical spectroscopy provides non-invasively the optical characterization of highly diffusive media, such as biological tissues. Light pulses are injected into the tissue and the effects of light propagation on re-emitted pulses are interpreted with the diffusion theory to assess simultaneously tissue absorption and reduced scattering coefficients. Performing spectral measurements, information on tissue composition and structure is derived applying the Beer law to the measured absorption and an empiric approximation to Mie theory to the reduced scattering. The absorption properties of collagen powder were preliminarily measured in the range of 600-1100 nm using a laboratory set-up for broadband time-resolved diffuse optical spectroscopy. Optical projection images were subsequently acquired in compressed breast geometry on 218 subjects, either healthy or bearing breast lesions, using a portable instrument for optical mammography that operates at 7 wavelengths selected in the range 635-1060 nm. For all subjects, tissue composition was estimated in terms of oxy- and deoxy-hemoglobin, water, lipids, and collagen. Information on tissue microscopic structure was also derived. Good correlation was obtained between mammographic breast density (a strong risk factor for breast cancer) and an optical index based on collagen content and scattering power (that accounts mostly for tissue collagen). Logistic regression applied to all optically derived parameters showed that subjects at high risk for developing breast cancer for their high breast density can effectively be identified based on collagen content and scattering parameters. Tissue composition assessed in breast lesions with a perturbative approach indicated that collagen and hemoglobin content are significantly higher in malignant lesions than in benign ones.

Broadband sub-THz spectroscopy modules integrated in 65-nm CMOS technology

NARCIS (Netherlands)

Matters-Kammerer, M.K.; van Goor, D.; Tripodi, L.

2017-01-01

The design and characterization of a broadband 20-480 GHz continuously tuneable on-chip spectrometer based on non-linear transmission lines in 65-nm CMOS technology is presented. The design procedure of the sampler that detects the ultra-broadband signal from the transmitter in time and frequency

Frequency-resolved measurement of the orbital angular momentum spectrum of femtosecond ultra-broadband optical-vortex pulses based on field reconstruction

International Nuclear Information System (INIS)

Yamane, Keisaku; Yang, Zhili; Toda, Yasunori; Morita, Ryuji

2014-01-01

We propose a high-precision method for measuring the orbital angular momentum (OAM) spectrum of ultra-broadband optical-vortex (OV) pulses from fork-like interferograms between OV pulses and a reference plane-wave pulse. It is based on spatial reconstruction of the electric fields of the pulses to be measured from the frequency-resolved interference pattern. Our method is demonstrated experimentally by obtaining the OAM spectra for different spectral components of the OV pulses, enabling us to characterize the frequency dispersion of the topological charge of the OAM spectrum by a simple experimental setup. Retrieval is carried out in quasi-real time, allowing us to investigate OAM spectra dynamically. Furthermore, we determine the relative phases (including the sign) of the topological-charge-resolved electric-field amplitudes, which are significant for evaluating OVs or OV pulses with arbitrarily superposed modes. (paper)

Photoelectron spectroscopy at a free-electron laser. Investigation of space-charge effects in angle-resolved and core-level spectroscopy and realizaton of a time-resolved core-level photoemission experiment

International Nuclear Information System (INIS)

Marczynski-Buehlow, Martin

2012-01-01

The free-electron laser (FEL) in Hamburg (FLASH) is a very interesting light source with which to perform photoelectron spectroscopy (PES) experiments. Its special characteristics include highly intense photon pulses (up to 100 J/pulse), a photon energy range of 30 eV to 1500 eV, transverse coherence as well as pulse durations of some ten femtoseconds. Especially in terms of time-resolved PES (TRPES), the deeper lying core levels can be reached with photon energies up to 1500 eV with acceptable intensity now and, therefore, element-specific, time-resolved core-level PES (XPS) is feasible at FLASH. During the work of this thesis various experimental setups were constructed in order to realize angle-resolved (ARPES), core-level (XPS) as well as time-resolved PES experiments at the plane grating monochromator beamline PG2 at FLASH. Existing as well as newly developed systems for online monitoring of FEL pulse intensities and generating spatial and temporal overlap of FEL and optical laser pulses for time-resolved experiments are successfully integrated into the experimental setup for PES. In order to understand space-charge effects (SCEs) in PES and, therefore, being able to handle those effects in future experiments using highly intense and pulsed photon sources, the origin of energetic broadenings and shifts in photoelectron spectra are studied by means of a molecular dynamic N-body simulation using a modified Treecode Algorithm for sufficiently fast and accurate calculations. It turned out that the most influencing parameter is the ''linear electron density'' - the ratio of the number of photoelectrons to the diameter of the illuminated spot on the sample. Furthermore, the simulations could reproduce the observations described in the literature fairly well. Some rules of thumb for XPS and ARPES measurements could be deduced from the simulations. Experimentally, SCEs are investigated by means of ARPES as well as XPS measurements as a function of FEL pulse

Photoelectron spectroscopy at a free-electron laser. Investigation of space-charge effects in angle-resolved and core-level spectroscopy and realizaton of a time-resolved core-level photoemission experiment

Energy Technology Data Exchange (ETDEWEB)

Marczynski-Buehlow, Martin

2012-01-30

The free-electron laser (FEL) in Hamburg (FLASH) is a very interesting light source with which to perform photoelectron spectroscopy (PES) experiments. Its special characteristics include highly intense photon pulses (up to 100 J/pulse), a photon energy range of 30 eV to 1500 eV, transverse coherence as well as pulse durations of some ten femtoseconds. Especially in terms of time-resolved PES (TRPES), the deeper lying core levels can be reached with photon energies up to 1500 eV with acceptable intensity now and, therefore, element-specific, time-resolved core-level PES (XPS) is feasible at FLASH. During the work of this thesis various experimental setups were constructed in order to realize angle-resolved (ARPES), core-level (XPS) as well as time-resolved PES experiments at the plane grating monochromator beamline PG2 at FLASH. Existing as well as newly developed systems for online monitoring of FEL pulse intensities and generating spatial and temporal overlap of FEL and optical laser pulses for time-resolved experiments are successfully integrated into the experimental setup for PES. In order to understand space-charge effects (SCEs) in PES and, therefore, being able to handle those effects in future experiments using highly intense and pulsed photon sources, the origin of energetic broadenings and shifts in photoelectron spectra are studied by means of a molecular dynamic N-body simulation using a modified Treecode Algorithm for sufficiently fast and accurate calculations. It turned out that the most influencing parameter is the ''linear electron density'' - the ratio of the number of photoelectrons to the diameter of the illuminated spot on the sample. Furthermore, the simulations could reproduce the observations described in the literature fairly well. Some rules of thumb for XPS and ARPES measurements could be deduced from the simulations. Experimentally, SCEs are investigated by means of ARPES as well as XPS measurements as a function of

Time-resolved spectroscopy of laser-induced breakdown in water

Science.gov (United States)

Thomas, Robert J.; Hammer, Daniel X.; Noojin, Gary D.; Stolarski, David J.; Rockwell, Benjamin A.; Roach, William P.

1996-05-01

Laser pulses of 60-ps and 80-ps at a wavelength of 532-nm and 1064-nm respectively were used to produce laser induced breakdown in triple-distilled water. The resulting luminescent flash from the plasma was captured with an imaging spectrograph coupled to a streak camera with a 5-ps time resolution. The wavelength range was 350 to 900-nm. We present the resulting experimental data which gives plasma duration and time-resolved spectral information. Plasma temperature is also computed from the data. All parameters are presented at a pulse energy of 1-mJ and are compared with time-integrated spectra at the same pulse duration and at 5 to 7-ns pulse duration in a similar energy range.

Spectral characterization of crude oil using fluorescence (synchronous and time-resolved) and NIR (Near Infrared Spectroscopy); Caracterizacao espectral do petroleo utilizando fluorescencia (sincronizada e resolvida no tempo) e NIR (Near Infrared Spectroscopy)

Energy Technology Data Exchange (ETDEWEB)

Falla Sotelo, F.; Araujo Pantoja, P.; Lopez-Gejo, J.; Le Roux, G.A.C.; Nascimento, C.A.O. [Universidade de Sao Paulo (USP), SP (Brazil). Dept. de Engenharia Quimica. Lab. de Simulacao e Controle de Processos; Quina, F.H. [Universidade de Sao Paulo (USP), SP (Brazil). Inst. de Quimica. Centro de Capacitacao e Pesquisa em Meio Ambiente (CEPEMA)

2008-07-01

The objective of the present work is to evaluate the performance of two spectroscopic techniques employed in the crude oil characterization: NIR spectroscopy and fluorescence spectroscopy (Synchronous fluorescence - SF and Time Resolved Fluorescence - TRF) for the development of correlation models between spectral profiles of crude oil samples and both physical properties (viscosity and API density) and physico-chemical properties (SARA analysis: Saturated, Aromatic, Resins and Asphaltenes). The better results for viscosity and density were obtained using NIR whose prediction capacity was good (1.5 cP and 0.5 deg API, respectively). For SARA analysis, fluorescence spectroscopy revealed its potential in the model calibration showing good results (R2 coefficients greater than 0.85). TRF spectroscopy had better performance than SF spectroscopy. (author)

Ultrafast time-resolved spectroscopy of lead halide perovskite films

Science.gov (United States)

Idowu, Mopelola A.; Yau, Sung H.; Varnavski, Oleg; Goodson, Theodore

2015-09-01

Recently, lead halide perovskites which are organic-inorganic hybrid structures, have been discovered to be highly efficient as light absorbers. Herein, we show the investigation of the excited state dynamics and emission properties of non-stoichiometric precursor formed lead halide perovskites grown by interdiffusion method using steady-state and time-resolved spectroscopic measurements. The influence of the different ratios of the non-stoichiometric precursor solution was examined. The observed photoluminescence properties were correlated with the femtosecond transient absorption measurements.

Time-resolved Chemical Imaging of Molecules by High-order Harmonics and Ultrashort Rescattering Electrons

Energy Technology Data Exchange (ETDEWEB)

Lin, Chii Dong [Kansas State Univ., Manhattan, KS (United States)

2016-03-21

Directly monitoring atomic motion during a molecular transformation with atomic-scale spatio-temporal resolution is a frontier of ultrafast optical science and physical chemistry. Here we provide the foundation for a new imaging method, fixed-angle broadband laser-induced electron scattering, based on structural retrieval by direct one-dimensional Fourier transform of a photoelectron energy distribution observed along the polarization direction of an intense ultrafast light pulse. The approach exploits the scattering of a broadband wave packet created by strong-field tunnel ionization to self-interrogate the molecular structure with picometre spatial resolution and bond specificity. With its inherent femtosecond resolution, combining our technique with molecular alignment can, in principle, provide the basis for time-resolved tomography for multi-dimensional transient structural determination.

Advances in high-order harmonic generation sources for time-resolved investigations

Energy Technology Data Exchange (ETDEWEB)

Reduzzi, Maurizio [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Institute of Photonics and Nanotechnologies, CNR-IFN, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Carpeggiani, Paolo [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Kühn, Sergei [ELI-ALPS, ELI-Hu Kft., Dugonics ter 13, H-6720 Szeged (Hungary); Calegari, Francesca [Institute of Photonics and Nanotechnologies, CNR-IFN, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Nisoli, Mauro; Stagira, Salvatore [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Institute of Photonics and Nanotechnologies, CNR-IFN, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Vozzi, Caterina [Institute of Photonics and Nanotechnologies, CNR-IFN, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Dombi, Peter [ELI-ALPS, ELI-Hu Kft., Dugonics ter 13, H-6720 Szeged (Hungary); Wigner Research Center for Physics, 1121 Budapest (Hungary); Kahaly, Subhendu [ELI-ALPS, ELI-Hu Kft., Dugonics ter 13, H-6720 Szeged (Hungary); Tzallas, Paris; Charalambidis, Dimitris [ELI-ALPS, ELI-Hu Kft., Dugonics ter 13, H-6720 Szeged (Hungary); Foundation for Research and Technology – Hellas, Institute of Electronic Structure and Lasers, P.O. Box 1527, GR-711 10 Heraklion, Crete (Greece); Varju, Katalin [ELI-ALPS, ELI-Hu Kft., Dugonics ter 13, H-6720 Szeged (Hungary); Department of Optics and Quantum Electronics, University of Szeged, Dóm tér 9, 6720 Szeged (Hungary); Osvay, Karoly [ELI-ALPS, ELI-Hu Kft., Dugonics ter 13, H-6720 Szeged (Hungary); and others

2015-10-15

We review the main research directions ongoing in the development of extreme ultraviolet sources based on high-harmonic generation for the synthesization and application of trains and isolated attosecond pulses to time-resolved spectroscopy. A few experimental and theoretical works will be discussed in connection to well-established attosecond techniques. In this context, we present the unique possibilities offered for time-resolved investigations on the attosecond timescale by the new Extreme Light Infrastructure Attosecond Light Pulse Source, which is currently under construction.

Advances in high-order harmonic generation sources for time-resolved investigations

International Nuclear Information System (INIS)

Reduzzi, Maurizio; Carpeggiani, Paolo; Kühn, Sergei; Calegari, Francesca; Nisoli, Mauro; Stagira, Salvatore; Vozzi, Caterina; Dombi, Peter; Kahaly, Subhendu; Tzallas, Paris; Charalambidis, Dimitris; Varju, Katalin; Osvay, Karoly

2015-01-01

We review the main research directions ongoing in the development of extreme ultraviolet sources based on high-harmonic generation for the synthesization and application of trains and isolated attosecond pulses to time-resolved spectroscopy. A few experimental and theoretical works will be discussed in connection to well-established attosecond techniques. In this context, we present the unique possibilities offered for time-resolved investigations on the attosecond timescale by the new Extreme Light Infrastructure Attosecond Light Pulse Source, which is currently under construction.

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

Energy Technology Data Exchange (ETDEWEB)

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

2015-10-01

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

Adaptive sampling dual terahertz comb spectroscopy using dual free-running femtosecond lasers.

Science.gov (United States)

Yasui, Takeshi; Ichikawa, Ryuji; Hsieh, Yi-Da; Hayashi, Kenta; Cahyadi, Harsono; Hindle, Francis; Sakaguchi, Yoshiyuki; Iwata, Tetsuo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Minoshima, Kaoru; Inaba, Hajime

2015-06-02

Terahertz (THz) dual comb spectroscopy (DCS) is a promising method for high-accuracy, high-resolution, broadband THz spectroscopy because the mode-resolved THz comb spectrum includes both broadband THz radiation and narrow-line CW-THz radiation characteristics. In addition, all frequency modes of a THz comb can be phase-locked to a microwave frequency standard, providing excellent traceability. However, the need for stabilization of dual femtosecond lasers has often hindered its wide use. To overcome this limitation, here we have demonstrated adaptive-sampling THz-DCS, allowing the use of free-running femtosecond lasers. To correct the fluctuation of the time and frequency scales caused by the laser timing jitter, an adaptive sampling clock is generated by dual THz-comb-referenced spectrum analysers and is used for a timing clock signal in a data acquisition board. The results not only indicated the successful implementation of THz-DCS with free-running lasers but also showed that this configuration outperforms standard THz-DCS with stabilized lasers due to the slight jitter remained in the stabilized lasers.

Exhaled breath profiling using broadband quantum cascade laser-based spectroscopy in healthy children and children with asthma and cystic fibrosis.

Science.gov (United States)

van Mastrigt, E; Reyes-Reyes, A; Brand, K; Bhattacharya, N; Urbach, H P; Stubbs, A P; de Jongste, J C; Pijnenburg, M W

2016-04-08

Exhaled breath analysis is a potential non-invasive tool for diagnosing and monitoring airway diseases. Gas chromatography-mass spectrometry and electrochemical sensor arrays are the main techniques to detect volatile organic compounds (VOC) in exhaled breath. We developed a broadband quantum cascade laser spectroscopy technique for VOC detection and identification. The objective of this study was to assess the repeatability of exhaled breath profiling with broadband quantum cascade laser-based spectroscopy and to explore the clinical applicability by comparing exhaled breath samples from healthy children with those from children with asthma or cystic fibrosis (CF). Healthy children and children with stable asthma or stable CF, aged 6-18 years, were included. Two to four exhaled breath samples were collected in Tedlar bags and analyzed by quantum cascade laser spectroscopy to detect VOCs with an absorption profile in the wavenumber region between 832 and 1262.55 cm(-1). We included 35 healthy children, 39 children with asthma and 15 with CF. Exhaled breath VOC profiles showed poor repeatability (Spearman's rho  =  0.36 to 0.46) and agreement of the complete profiles. However, we were able to discriminate healthy children from children with stable asthma or stable CF and identified VOCs that were responsible for this discrimination. Broadband quantum cascade laser-based spectroscopy detected differences in VOC profiles in exhaled breath samples between healthy children and children with asthma or CF. The combination of a relatively easy and fast method and the possibility of molecule identification makes broadband quantum cascade laser-based spectroscopy attractive to investigate the diagnostic and prognostic potential of volatiles in exhaled breath.

Broadband enhancement of local density of states using silicon-compatible hyperbolic metamaterials

Energy Technology Data Exchange (ETDEWEB)

Wang, Yu; Inampudi, Sandeep; Capretti, Antonio [Department of Electrical and Computer Engineering and Photonics Center, Boston University, 8 Saint Mary' s Street Boston, Massachusetts 02215 (United States); Sugimoto, Hiroshi [Department of Electrical and Computer Engineering and Photonics Center, Boston University, 8 Saint Mary' s Street Boston, Massachusetts 02215 (United States); Department of Electrical and Electronic Engineering, Graduate School of Engineering, Kobe University, Rokkodai, Nada, Kobe 657-8501 (Japan); Fujii, Minoru [Department of Electrical and Electronic Engineering, Graduate School of Engineering, Kobe University, Rokkodai, Nada, Kobe 657-8501 (Japan); Dal Negro, Luca, E-mail: dalnegro@bu.edu [Department of Electrical and Computer Engineering and Photonics Center, Boston University, 8 Saint Mary' s Street Boston, Massachusetts 02215 (United States); Division of Materials Science and Engineering, Boston University, 15 Saint Mary' s Street, Brookline, Massachusetts 02446 (United States)

2015-06-15

Light emitting silicon quantum dots by colloidal synthesis were uniformly spin-coated into a 20 nm-thick film and deposited atop a hyperbolic metamaterial of alternating TiN and SiO{sub 2} sub-wavelength layers. Using steady-state and time-resolved photoluminescence spectroscopy as a function of the emission wavelength in partnership with rigorous electromagnetic modeling of dipolar emission, we demonstrate enhanced Local Density of States and coupling to high-k modes in a broad spectral range. These findings provide an alternative approach for the engineering of novel Si-compatible broadband sources that leverage the control of radiative transitions in hyperbolic metamaterials and the flexibility of the widespread Si platform.

Dynamic Time-Resolved Chirped-Pulse Rotational Spectroscopy of Vinyl Cyanide Photoproducts in a Room Temperature Flow Reactor

Science.gov (United States)

Zaleski, Daniel P.; Prozument, Kirill

2017-06-01

Chirped-pulsed (CP) Fourier transform rotational spectroscopy invented by Brooks Pate and coworkers a decade ago is an attractive tool for gas phase chemical dynamics and kinetics studies. A good reactor for such a purpose would have well-defined (and variable) temperature and pressure conditions to be amenable to accurate kinetic modeling. Furthermore, in low pressure samples with large enough number of molecular emitters, reaction dynamics can be observable directly, rather than mediated by supersonic expansion. In the present work, we are evaluating feasibility of in situ time-resolved CP spectroscopy in a room temperature flow tube reactor. Vinyl cyanide (CH_2CHCN), neat or mixed with inert gasses, flows through the reactor at pressures 1-50 μbar (0.76-38 mTorr) where it is photodissociated by a 193 nm laser. Millimeter-wave beam of the CP spectrometer co-propagates with the laser beam along the reactor tube and interacts with nascent photoproducts. Rotational transitions of HCN, HNC, and HCCCN are detected, with ≥10 μs time-steps for 500 ms following photolysis of CH_2CHCN. The post-photolysis evolution of the photoproducts' rotational line intensities is investigated for the effects of rotational and vibrational thermalization of energized photoproducts. Possible contributions from bimolecular and wall-mediated chemistry are evaluated as well.

Equilibrium constants in aqueous lanthanide and actinide chemistry from time-resolved fluorescence spectroscopy: The role of ground and excited state reactions

International Nuclear Information System (INIS)

Billard, I.; Luetzenkirchen, K.

2003-01-01

Equilibrium constants for aqueous reactions between lanthanide or actinide ions and (in-) organic ligands contain important information for various radiochemical problems, such as nuclear reprocessing or the migration of radioelements in the geosphere. We study the conditions required to determine equilibrium constants by time-resolved fluorescence spectroscopy measurements. Based on a simulation study it is shown that the possibility to determine equilibrium constants depends upon the reaction rates in the photoexcited states of the lanthanide or actinide ions. (orig.)

Validation of a high-power, time-resolved, near-infrared spectroscopy system for measurement of superficial and deep muscle deoxygenation during exercise.

Science.gov (United States)

Koga, Shunsaku; Barstow, Thomas J; Okushima, Dai; Rossiter, Harry B; Kondo, Narihiko; Ohmae, Etsuko; Poole, David C

2015-06-01

Near-infrared assessment of skeletal muscle is restricted to superficial tissues due to power limitations of spectroscopic systems. We reasoned that understanding of muscle deoxygenation may be improved by simultaneously interrogating deeper tissues. To achieve this, we modified a high-power (∼8 mW), time-resolved, near-infrared spectroscopy system to increase depth penetration. Precision was first validated using a homogenous optical phantom over a range of inter-optode spacings (OS). Coefficients of variation from 10 measurements were minimal (0.5-1.9%) for absorption (μa), reduced scattering, simulated total hemoglobin, and simulated O2 saturation. Second, a dual-layer phantom was constructed to assess depth sensitivity, and the thickness of the superficial layer was varied. With a superficial layer thickness of 1, 2, 3, and 4 cm (μa = 0.149 cm(-1)), the proportional contribution of the deep layer (μa = 0.250 cm(-1)) to total μa was 80.1, 26.9, 3.7, and 0.0%, respectively (at 6-cm OS), validating penetration to ∼3 cm. Implementation of an additional superficial phantom to simulate adipose tissue further reduced depth sensitivity. Finally, superficial and deep muscle spectroscopy was performed in six participants during heavy-intensity cycle exercise. Compared with the superficial rectus femoris, peak deoxygenation of the deep rectus femoris (including the superficial intermedius in some) was not significantly different (deoxyhemoglobin and deoxymyoglobin concentration: 81.3 ± 20.8 vs. 78.3 ± 13.6 μM, P > 0.05), but deoxygenation kinetics were significantly slower (mean response time: 37 ± 10 vs. 65 ± 9 s, P ≤ 0.05). These data validate a high-power, time-resolved, near-infrared spectroscopy system with large OS for measuring the deoxygenation of deep tissues and reveal temporal and spatial disparities in muscle deoxygenation responses to exercise. Copyright © 2015 the American Physiological Society.

Static and time-resolved mid-infrared spectroscopy of Hg0.95Cd0.05Cr2Se4 spinel.

Science.gov (United States)

Barsaume, S; Telegin, A V; Sukhorukov, Yu P; Stavrias, N; Fedorov, V A; Menshchikova, T K; Kimel, A V

2017-08-16

Static and time-resolved mid-infrared spectroscopy of ferromagnetic single crystal Hg 0.95 Cd 0.05 Cr 2 Se 4 was performed below the absorption edge, in order to reveal the origin of the electronic transitions contributing to the magneto-optical properties of this material. The mid-infrared spectroscopy reveals a strong absorption peak around 0.236 eV which formerly was assigned to a transition within the selenide-chromium complexes ([Formula: see text] Se -Cr 2+ ). To reveal the sensitivity of the transition to the magnetic order, we performed the studies in a temperature range across the Curie temperature and magnetic fields across the value at which the saturation of ferromagnetic magnetization occurs. Despite the fact that the Curie temperature of this ferromagnetic semiconductor is around 107 K, the intensity of the mid-infrared transition reduces substantially increasing the temperature, so that already at 70 K the absorption peak is hardly visible. Such a dramatic decrease of the oscillator strength is observed simultaneously with the strong red-shift of the absorption edge in the magnetic semiconductor. Employing a time-resolved pump-and-probe technique enabled us to determine the lifetime of the electrons in the excited state of this optical transition. In the temperature range from 7 K to 80 K, the lifetime changes from 3 ps to 6 ps. This behavior agrees with the phenomenon of giant oscillator strength described earlier for weakly bound excitons in nonmagnetic semiconductors.

Vibrational dynamics of aqueous hydroxide solutions probed using broadband 2DIR spectroscopy

International Nuclear Information System (INIS)

Mandal, Aritra; Tokmakoff, Andrei

2015-01-01

We employed ultrafast transient absorption and broadband 2DIR spectroscopy to study the vibrational dynamics of aqueous hydroxide solutions by exciting the O–H stretch vibrations of the strongly hydrogen-bonded hydroxide solvation shell water and probing the continuum absorption of the solvated ion between 1500 and 3800 cm −1 . We observe rapid vibrational relaxation processes on 150–250 fs time scales across the entire probed spectral region as well as slower vibrational dynamics on 1–2 ps time scales. Furthermore, the O–H stretch excitation loses its frequency memory in 180 fs, and vibrational energy exchange between bulk-like water vibrations and hydroxide-associated water vibrations occurs in ∼200 fs. The fast dynamics in this system originate in strong nonlinear coupling between intra- and intermolecular vibrations and are explained in terms of non-adiabatic vibrational relaxation. These measurements indicate that the vibrational dynamics of the aqueous hydroxide complex are faster than the time scales reported for long-range transport of protons in aqueous hydroxide solutions

Ultrafast photo-initiated molecular quantum dynamics in the DNA dinucleotide d(ApG) revealed by broadband transient absorption spectroscopy.

Science.gov (United States)

Stuhldreier, Mayra C; Temps, Friedrich

2013-01-01

The ultrafast photo-initiated quantum dynamics of the adenine-guanine dinucleotide d(ApG) in aqueous solution (pH 7) has been studied by femtosecond time-resolved spectroscopy after excitation at lambda = 260 nm. The results reveal a hierarchy of processes on time scales from tau 100 ps. Characteristic spectro-temporal signatures are observed indicating the transformation of the molecules in the electronic relaxation from the photo-excited state to a long-lived exciplex. In particular, broadband UV/VIS excited-state absorption (ESA) measurements detected a distinctive absorption by the excited dinucleotide around lambda = 335 nm, approximately 0.5 eV to the blue compared to the maximum of the broad and unstructured ESA spectrum after excitation of an equimolar mixture of the mononucleotides dAMP and dGMP. A similar feature has been identified as signature of the excimer in the dynamics of the adenine dinucleotide d(ApA). The lifetime of the d(ApG) exciplex was found to be tau = 124 +/- 4 ps both from the ESA decay time and from the ground-state recovery time, far longer than the sub-picosecond lifetimes of excited dAMP or dGMP. Fluorescence-time profiles measured by the up-conversion technique indicate that the exciplex state is reached around approximately 6 ps after excitation. Very weak residual fluorescence at longer times red-shifted to the emission from the photo-excited state shows that the exciplex is almost optically dark, but still has enough oscillator strength to give rise to the dual fluorescence of the dinucleotide in the static fluorescence spectrum.

Ultrabroadband time-resolved THz spectroscopy of polymer-based solar cells

DEFF Research Database (Denmark)

Cooke, David G.; Krebs, Frederik C; Jepsen, Peter Uhd

2011-01-01

We have developed ultrabroadband THz spectroscopy in reflection mode for characterization of conductivity dynamics in conductive polymer samples used in organic solar cells. The spectrometer is designed to have a time resolution limited only by the duration of the optical pump pulse, thus enabling...

Factors affecting measurement of optic parameters by time-resolved near-infrared spectroscopy in breast cancer

Science.gov (United States)

Yoshizawa, Nobuko; Ueda, Yukio; Mimura, Tetsuya; Ohmae, Etsuko; Yoshimoto, Kenji; Wada, Hiroko; Ogura, Hiroyuki; Sakahara, Harumi

2018-02-01

The purpose of this study was to evaluate the effects of the thickness and depth of tumors on hemoglobin measurements in breast cancer by optical spectroscopy and to demonstrate tissue oxygen saturation (SO2) and reduced scattering coefficient (μs‧) in breast tissue and breast cancer in relation to the skin-to-chest wall distance. We examined 53 tumors from 44 patients. Total hemoglobin concentration (tHb), SO2, and μs‧ were measured by time-resolved spectroscopy (TRS). The skin-to-chest wall distance and the size and depth of tumors were measured by ultrasonography. There was a positive correlation between tHb and tumor thickness, and a negative correlation between tHb and tumor depth. SO2 in breast tissue decreased when the skin-to-chest wall distance decreased, and SO2 in tumors tended to be lower than in breast tissue. In breast tissue, there was a negative correlation between μs‧ and the skin-to-chest wall distance, and μs‧ in tumors was higher than in breast tissue. Measurement of tHb in breast cancer by TRS was influenced by tumor thickness and depth. Although SO2 seemed lower and μs‧ was higher in breast cancer than in breast tissue, the skin-to-chest wall distance may have affected the measurements.

Diagnosis of laser ablated carbon particles measured by time-resolved X-ray absorption spectroscopy

International Nuclear Information System (INIS)

Miyashita, Atsumi; Yoda, Osamu; Ohyanagi, T.; Murakami, K.

1995-01-01

The time and space resolved properties of laser ablated carbon particles were measured by X-ray absorption spectroscopy using LPX as an X-ray source. The energy density of the irradiation laser on the sample was in the range of 0.5-20J/cm 2 and the time delay was varied between 0 and 120ns. The absorption spectra exhibited several peaks originated from level to level transitions and an intense broad absorption in the energy range of C-K edge. At a delay time of 120ns, the absorption peak from 1s→2p transition of neutral carbon atom (C 0 ), C - , C + and C 2+ ions were observed. The absorption peak from C 0 was stronger as the probing position was closer to the sample surface and decreased rapidly with distance from the sample surface. The absorption peak C 2+ ion was observed only at comparatively distant positions from surface. The maximum speeds of highly charged ions were faster than that of neutral atoms and negative charged ions. The neutral atom and lower charged ions were emitted from the sample even after laser irradiation. The spatial distributions of the laser ablated carbon particles in the localized helium gas environment were measured. In the helium gas environment, the ablation plume was depressed by the helium cloud generated on the top of ablation plume. (author)

Femtosecond time-resolved vibrational SFG spectroscopy of CO/Ru( 0 0 1 )

Science.gov (United States)

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.

Time-Resolved Spectroscopy and Near Infrared Imaging for Prostate Cancer Detection: Receptor-targeted and Native Biomarker

Science.gov (United States)

Pu, Yang

Optical spectroscopy and imaging using near-infrared (NIR) light provides powerful tools for non-invasive detection of cancer in tissue. Optical techniques are capable of quantitative reconstructions maps of tissue absorption and scattering properties, thus can map in vivo the differences in the content of certain marker chromophores and/or fluorophores in normal and cancerous tissues (for example: water, tryptophan, collagen and NADH contents). Potential clinical applications of optical spectroscopy and imaging include functional tumor detection and photothermal therapeutics. Optical spectroscopy and imaging apply contrasts from intrinsic tissue chromophores such as water, collagen and NADH, and extrinsic optical contrast agents such as Indocyanine Green (ICG) to distinguish disease tissue from the normal one. Fluorescence spectroscopy and imaging also gives high sensitivity and specificity for biomedical diagnosis. Recent developments on specific-targeting fluorophores such as small receptor-targeted dye-peptide conjugate contrast agent offer high contrast between normal and cancerous tissues hence provide promising future for early tumour detection. This thesis focus on a study to distinguish the cancerous prostate tissue from the normal prostate tissues with enhancement of specific receptor-targeted prostate cancer contrast agents using optical spectroscopy and imaging techniques. The scattering and absorption coefficients, and anisotropy factor of cancerous and normal prostate tissues were investigated first as the basis for the biomedical diagnostic and optical imaging. Understanding the receptors over-expressed prostate cancer cells and molecular target mechanism of ligand, two small ICG-derivative dye-peptides, namely Cypate-Bombesin Peptide Analogue Conjugate (Cybesin) and Cypate-Octreotate Peptide Conjugate (Cytate), were applied to study their clinical potential for human prostate cancer detection. In this work, the steady-state and time-resolved

Spectrally interleaved, comb-mode-resolved spectroscopy using swept dual terahertz combs.

Science.gov (United States)

Hsieh, Yi-Da; Iyonaga, Yuki; Sakaguchi, Yoshiyuki; Yokoyama, Shuko; Inaba, Hajime; Minoshima, Kaoru; Hindle, Francis; Araki, Tsutomu; Yasui, Takeshi

2014-01-22

Optical frequency combs are innovative tools for broadband spectroscopy because a series of comb modes can serve as frequency markers that are traceable to a microwave frequency standard. However, a mode distribution that is too discrete limits the spectral sampling interval to the mode frequency spacing even though individual mode linewidth is sufficiently narrow. Here, using a combination of a spectral interleaving and dual-comb spectroscopy in the terahertz (THz) region, we achieved a spectral sampling interval equal to the mode linewidth rather than the mode spacing. The spectrally interleaved THz comb was realized by sweeping the laser repetition frequency and interleaving additional frequency marks. In low-pressure gas spectroscopy, we achieved an improved spectral sampling density of 2.5 MHz and enhanced spectral accuracy of 8.39 × 10(-7) in the THz region. The proposed method is a powerful tool for simultaneously achieving high resolution, high accuracy, and broad spectral coverage in THz spectroscopy.

Spectrally interleaved, comb-mode-resolved spectroscopy using swept dual terahertz combs

Science.gov (United States)

Hsieh, Yi-Da; Iyonaga, Yuki; Sakaguchi, Yoshiyuki; Yokoyama, Shuko; Inaba, Hajime; Minoshima, Kaoru; Hindle, Francis; Araki, Tsutomu; Yasui, Takeshi

2014-01-01

Optical frequency combs are innovative tools for broadband spectroscopy because a series of comb modes can serve as frequency markers that are traceable to a microwave frequency standard. However, a mode distribution that is too discrete limits the spectral sampling interval to the mode frequency spacing even though individual mode linewidth is sufficiently narrow. Here, using a combination of a spectral interleaving and dual-comb spectroscopy in the terahertz (THz) region, we achieved a spectral sampling interval equal to the mode linewidth rather than the mode spacing. The spectrally interleaved THz comb was realized by sweeping the laser repetition frequency and interleaving additional frequency marks. In low-pressure gas spectroscopy, we achieved an improved spectral sampling density of 2.5 MHz and enhanced spectral accuracy of 8.39 × 10-7 in the THz region. The proposed method is a powerful tool for simultaneously achieving high resolution, high accuracy, and broad spectral coverage in THz spectroscopy.

Orbital Evolution and Orbital Phase Resolved Spectroscopy of the ...

Indian Academy of Sciences (India)

binary. We have carried out orbital phase resolved spectroscopy to mea- ... agreement with a simple model of a spherically symmetric stellar wind from the .... has a set of Narrow Field Instruments (NFI) comprising one Low Energy Concen-.

Broadband cavity-enhanced absorption spectroscopy in the ultraviolet spectral region for measurements of nitrogen dioxide and formaldehyde

Science.gov (United States)

Washenfelder, R. A.; Attwood, A. R.; Flores, J. M.; Zarzana, K. J.; Rudich, Y.; Brown, S. S.

2016-01-01

Formaldehyde (CH2O) is the most abundant aldehyde in the atmosphere, and it strongly affects photochemistry through its photolysis. We describe simultaneous measurements of CH2O and nitrogen dioxide (NO2) using broadband cavity-enhanced absorption spectroscopy in the ultraviolet spectral region. The light source consists of a continuous-wave diode laser focused into a Xenon bulb to produce a plasma that emits high-intensity, broadband light. The plasma discharge is optically filtered and coupled into a 1 m optical cavity. The reflectivity of the cavity mirrors is 0.99930 ± 0.00003 (1- reflectivity = 700 ppm loss) at 338 nm, as determined from the known Rayleigh scattering of He and zero air. This mirror reflectivity corresponds to an effective path length of 1.43 km within the 1 m cell. We measure the cavity output over the 315-350 nm spectral region using a grating monochromator and charge-coupled device array detector. We use published reference spectra with spectral fitting software to simultaneously retrieve CH2O and NO2 concentrations. Independent measurements of NO2 standard additions by broadband cavity-enhanced absorption spectroscopy and cavity ring-down spectroscopy agree within 2 % (slope for linear fit = 1.02 ± 0.03 with r2 = 0.998). Standard additions of CH2O measured by broadband cavity-enhanced absorption spectroscopy and calculated based on flow dilution are also well correlated, with r2 = 0.9998. During constant mixed additions of NO2 and CH2O, the 30 s measurement precisions (1σ) of the current configuration were 140 and 210 pptv, respectively. The current 1 min detection limit for extinction measurements at 315-350 nm provides sufficient sensitivity for measurement of trace gases in laboratory experiments and ground-based field experiments. Additionally, the instrument provides highly accurate, spectroscopically based trace gas detection that may complement higher precision techniques based on non-absolute detection methods. In addition to

Electronic resonances in broadband stimulated Raman spectroscopy

Science.gov (United States)

Batignani, G.; Pontecorvo, E.; Giovannetti, G.; Ferrante, C.; Fumero, G.; Scopigno, T.

2016-01-01

Spontaneous Raman spectroscopy is a formidable tool to probe molecular vibrations. Under electronic resonance conditions, the cross section can be selectively enhanced enabling structural sensitivity to specific chromophores and reaction centers. The addition of an ultrashort, broadband femtosecond pulse to the excitation field allows for coherent stimulation of diverse molecular vibrations. Within such a scheme, vibrational spectra are engraved onto a highly directional field, and can be heterodyne detected overwhelming fluorescence and other incoherent signals. At variance with spontaneous resonance Raman, however, interpreting the spectral information is not straightforward, due to the manifold of field interactions concurring to the third order nonlinear response. Taking as an example vibrational spectra of heme proteins excited in the Soret band, we introduce a general approach to extract the stimulated Raman excitation profiles from complex spectral lineshapes. Specifically, by a quantum treatment of the matter through density matrix description of the third order nonlinear polarization, we identify the contributions which generate the Raman bands, by taking into account for the cross section of each process.

Time-resolved photoluminescence spectroscopy of semiconductors for optical applications beyond the visible spectral range

Energy Technology Data Exchange (ETDEWEB)

Chernikov, Alexey A.

2011-07-01

The work discussed in this thesis is focused on the experimental studies regarding these three steps: (1) investigation of the fundamental effects, (2) characterization of new material systems, and (3) optimization of the semiconductor devices. In all three cases, the experimental technique of choice is photoluminescence (PL) spectroscopy. The thesis is organized as follows. Chapter 2 gives a summary of the PL properties of semiconductors relevant for this work. The first section deals with the intrinsic processes in an ideal direct band gap material, starting with a brief summary of the theoretical background followed by the overview of a typical PL scenario. In the second part of the chapter, the role of the lattice-vibrations, the internal electric fields as well as the influence of the band-structure and the dielectric environment are discussed. Finally, extrinsic PL properties are presented in the third section, focusing on defects and disorder in real materials. In chapter 3, the experimental realization of the spectroscopic studies is discussed. The time-resolved photoluminescence (TRPL) setup is presented, focusing on the applied excitation source, non-linear frequency mixing, and the operation of the streak camera used for the detection. In addition, linear spectroscopy setup for continous-wave (CW) PL and absorption measurements is illustrated. Chapter 4 aims at the study of the interactions between electrons and lattice-vibrations in semiconductor crystals relevant for the proper description of carrier dynamics as well as the heat-transfer processes. The presented discussion covers the experimental studies of many-body effects in phonon-assisted emission of semiconductors due to the carriercarrier Coulomb-interaction. The corresponding theoretical background is discussed in detail in chapter 2. The investigations are focused on the two main questions regarding electron-hole plasma contributions to the phonon-assisted light-matter interaction as well as

Covariance J-resolved spectroscopy: Theory and application in vivo.

Science.gov (United States)

Iqbal, Zohaib; Verma, Gaurav; Kumar, Anand; Thomas, M Albert

2017-08-01

Magnetic resonance spectroscopy (MRS) is a powerful tool capable of investigating the metabolic status of several tissues in vivo. In particular, single-voxel-based 1 H spectroscopy provides invaluable biochemical information from a volume of interest (VOI) and has therefore been used in a variety of studies. Unfortunately, typical one-dimensional MRS data suffer from severe signal overlap and thus important metabolites are difficult to distinguish. One method that is used to disentangle overlapping resonances is the two-dimensional J-resolved spectroscopy (JPRESS) experiment. Due to the long acquisition duration of the JPRESS experiment, a limited number of points are acquired in the indirect dimension, leading to poor spectral resolution along this dimension. Poor spectral resolution is problematic because proper peak assignment may be hindered, which is why the zero-filling method is often used to improve resolution as a post-processing step. However, zero-filling leads to spectral artifacts, which may affect visualization and quantitation of spectra. A novel method utilizing a covariance transformation, called covariance J-resolved spectroscopy (CovJ), was developed in order to improve spectral resolution along the indirect dimension (F 1 ). Comparison of simulated data demonstrates that peak structures remain qualitatively similar between JPRESS and the novel method along the diagonal region (F 1 = 0 Hz), whereas differences arise in the cross-peak (F 1 ≠0 Hz) regions. In addition, quantitative results of in vivo JPRESS data acquired on a 3T scanner show significant correlations (r 2 >0.86, pCOVariance Spectral Evaluation of 1 H Acquisitions using Representative prior knowledge' (Cov-SEHAR), was developed in order to quantify γ-aminobutyric acid and glutamate from the CovJ spectra. These preliminary findings indicate that the CovJ method may be used to improve spectral resolution without hindering metabolite quantitation for J-resolved spectra

Near-Infrared Spatially Resolved Spectroscopy for Tablet Quality Determination.

Science.gov (United States)

Igne, Benoît; Talwar, Sameer; Feng, Hanzhou; Drennen, James K; Anderson, Carl A

2015-12-01

Near-infrared (NIR) spectroscopy has become a well-established tool for the characterization of solid oral dosage forms manufacturing processes and finished products. In this work, the utility of a traditional single-point NIR measurement was compared with that of a spatially resolved spectroscopic (SRS) measurement for the determination of tablet assay. Experimental designs were used to create samples that allowed for calibration models to be developed and tested on both instruments. Samples possessing a poor distribution of ingredients (highly heterogeneous) were prepared by under-blending constituents prior to compaction to compare the analytical capabilities of the two NIR methods. The results indicate that SRS can provide spatial information that is usually obtainable only through imaging experiments for the determination of local heterogeneity and detection of abnormal tablets that would not be detected with single-point spectroscopy, thus complementing traditional NIR measurement systems for in-line, and in real-time tablet analysis. © 2015 Wiley Periodicals, Inc. and the American Pharmacists Association.

Investigation of Co nanoparticle formation using time-dependent and spatially-resolved X-ray absorption spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Zinoveva, S

2008-04-15

A crucial step towards controlled synthesis of nanoparticles is the detailed understanding of the various chemical processes that take place during the synthesis. X-ray Absorption Spectroscopy (XAS) is especially suitable for elucidating the type and structure of the intermediate metal species. It is applicable to materials that have no long range order and provides information on both electronic and geometric structures. Here a comparative study is reported of the formation of cobalt nanoparticles via thermolysis of two organometallic precursors dicobalt octacarbonyl (DCO) and alkyne-bridged dicobalt hexacarbonyl (ADH) in the presence of aluminum organics. Using time-dependent XAS a reaction pathway different from both the atom based La Mer model and the Watzky and Finsky autocatalytic surface growth model is observed. Where prior to the nucleation several intermediates are formed and the initial nucleus is composed of Co atoms coordinated with ligands Co{sub n}(CO){sub m} with n=2-3, m=3-5. The formation of Co nanoparticles was also investigated using a reaction different from thermolysis of cobalt carbonyls, namely reduction of Co (II) acetate by sodium borohydrate. Here the combination of microreactor system and spatially resolved XAS allowed ''in situ'' monitoring of the wet chemical synthesis. Several steps of the reaction were spatially resolved in the microreactor. The vertical size of the X-ray beam (50 {mu}m) focused with Kirkpatrick-Baez mirror system, determines the time resolution (better than 2 ms). The results provide direct insight into rapid process of nanoparticles formation and demonstrate the potential of this new technique for the fundamental studies of such type of processes where miniaturization and timeresolution are important. Like in the carbonyls thermolysis no evidence for the reduction of the starting complex to isolated Co{sup 0} atoms followed by nucleation of Co{sup 0} atoms was observed. (orig.)

Investigation of Co nanoparticle formation using time-dependent and spatially-resolved X-ray absorption spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Zinoveva, S.

2008-04-15

A crucial step towards controlled synthesis of nanoparticles is the detailed understanding of the various chemical processes that take place during the synthesis. X-ray Absorption Spectroscopy (XAS) is especially suitable for elucidating the type and structure of the intermediate metal species. It is applicable to materials that have no long range order and provides information on both electronic and geometric structures. Here a comparative study is reported of the formation of cobalt nanoparticles via thermolysis of two organometallic precursors dicobalt octacarbonyl (DCO) and alkyne-bridged dicobalt hexacarbonyl (ADH) in the presence of aluminum organics. Using time-dependent XAS a reaction pathway different from both the atom based La Mer model and the Watzky and Finsky autocatalytic surface growth model is observed. Where prior to the nucleation several intermediates are formed and the initial nucleus is composed of Co atoms coordinated with ligands Co{sub n}(CO){sub m} with n=2-3, m=3-5. The formation of Co nanoparticles was also investigated using a reaction different from thermolysis of cobalt carbonyls, namely reduction of Co (II) acetate by sodium borohydrate. Here the combination of microreactor system and spatially resolved XAS allowed ''in situ'' monitoring of the wet chemical synthesis. Several steps of the reaction were spatially resolved in the microreactor. The vertical size of the X-ray beam (50 {mu}m) focused with Kirkpatrick-Baez mirror system, determines the time resolution (better than 2 ms). The results provide direct insight into rapid process of nanoparticles formation and demonstrate the potential of this new technique for the fundamental studies of such type of processes where miniaturization and timeresolution are important. Like in the carbonyls thermolysis no evidence for the reduction of the starting complex to isolated Co{sup 0} atoms followed by nucleation of Co{sup 0} atoms was observed. (orig.)

Revealing the ultrafast charge carrier dynamics in organo metal halide perovskite solar cell materials using time resolved THz spectroscopy

Science.gov (United States)

Ponseca, C. S., Jr.; Sundström, V.

2016-03-01

Ultrafast charge carrier dynamics in organo metal halide perovskite has been probed using time resolved terahertz (THz) spectroscopy (TRTS). Current literature on its early time characteristics is unanimous: sub-ps charge carrier generation, highly mobile charges and very slow recombination rationalizing the exceptionally high power conversion efficiency for a solution processed solar cell material. Electron injection from MAPbI3 to nanoparticles (NP) of TiO2 is found to be sub-ps while Al2O3 NPs do not alter charge dynamics. Charge transfer to organic electrodes, Spiro-OMeTAD and PCBM, is sub-ps and few hundreds of ps respectively, which is influenced by the alignment of energy bands. It is surmised that minimizing defects/trap states is key in optimizing charge carrier extraction from these materials.

Time-resolved imaging of purely valence-electron dynamics during a chemical reaction

DEFF Research Database (Denmark)

Hockett, Paul; Bisgaard, Christer Z.; Clarkin, Owen J.

2011-01-01

Chemical reactions are manifestations of the dynamics of molecular valence electrons and their couplings to atomic motions. Emerging methods in attosecond science can probe purely electronic dynamics in atomic and molecular systems(1-6). By contrast, time-resolved structural-dynamics methods...... such as electron(7-10) or X-ray diffraction(11) and X-ray absorption(12) yield complementary information about the atomic motions. Time-resolved methods that are directly sensitive to both valence-electron dynamics and atomic motions include photoelectron spectroscopy(13-15) and high-harmonic generation(16......,17): in both cases, this sensitivity derives from the ionization-matrix element(18,19). Here we demonstrate a time-resolved molecular-frame photoelectron-angular-distribution (TRMFPAD) method for imaging the purely valence-electron dynamics during a chemical reaction. Specifically, the TRMFPADs measured during...

Josephson admittance spectroscopy application for frequency analysis of broadband THz antennas

International Nuclear Information System (INIS)

Volkov, O Yu; Divin, Yu Yu; Gubankov, V N; Gundareva, I I; Pavlovskiy, V V

2010-01-01

Application of Josephson admittance spectroscopy for the spectral analysis of a broad-band log-periodic superconducting antenna was demonstrated at the frequency range from 50 to 700 GHz. The [001]-tilt YBa 2 Cu 3 O 7-x bicrystal Josephson junctions, integrated with sinuous log-periodic YBa 2 Cu 3 O 7-x antennas, were fabricated on NdGaO 3 bicrystal substrates. A real part of the antenna admittance ReY(f) as a function of the frequency f was reconstructed from the modification of the dc current-voltage characteristic of the junction, induced by the antenna. Resonance features were observed in the recovered ReY(f)-spectra with a periodicity in the logarithmic frequency scale, corresponding to log-periodic geometry of the antenna. The ReY(f)-spectra, recovered by Josephson spectroscopy, were compared with the ReY(f)-spectra, obtained by CAD simulation, and both spectra were shown to be similar in their main features. A value of 23 was obtained for an effective permittivity of the NdGaO3 bicrystal substrates by fitting simulated data to those obtained from Josephson spectroscopy.

Dissociation dynamics of CH3I in electric spark induced breakdown revealed by time-resolved laser induced breakdown spectroscopy

International Nuclear Information System (INIS)

Wang, Yang; Liu, Wei-long; Song, Yun-fei; Duo, Li-ping; Liu, Yu-qiang; Yang, Yan-qiang

2015-01-01

Highlights: • Emission of electric spark dissociation of CH 3 I is similar to its fs LIBS. • We use fs laser induced breakdown as a simulation for electric spark dissociation. • The I 2 molecule formation is directly observed in the time-resolved LIBS. • Bimolecular collision of I ∗ and CH 3 I is responsible for the formation of I 2 . - Abstract: The electric discharge spark dissociation of gas CH 3 I is found to be similar to its femtosecond laser photodissociation. The almost identical spectra of the two processes show that their initial ionization conditions are very similar. The initial ionization followed by molecular fragmentation is proposed as the dissociation mechanism, in which the characteristic emissions of I + , CH 3 , CH 2 , CH, H, and I 2 are identified as the dissociation products. The emission band of 505 nm I 2 is clearly observed in the time-resolved laser induced breakdown spectroscopy (LIBS). The dynamic curve indicates that I 2 ∗ molecules are formed after the delay time of ∼4.7 ns. The formation of I 2 ∗ molecule results from the bimolecular collision of the highly excited iodine atom I ∗ ( 4 P) and CH 3 I molecule. This dynamical information can help understand the process of electric discharge spark dissociation of CH 3 I

Surface State Dynamics of Topological Insulators Investigated by Femtosecond Time- and Angle-Resolved Photoemission Spectroscopy

Directory of Open Access Journals (Sweden)

Hamoon Hedayat

2018-04-01

Full Text Available Topological insulators (TI are known for striking quantum phenomena associated with their spin-polarized topological surface state (TSS. The latter in particular forms a Dirac cone that bridges the energy gap between valence and conduction bands, providing a unique opportunity for prospective device applications. In TI of the BixSb2−xTeySe3−y (BSTS family, stoichiometry determines the morphology and position of the Dirac cone with respect to the Fermi level. In order to engineer specific transport properties, a careful tuning of the TSS is highly desired. Therefore, we have systematically explored BSTS samples with different stoichiometries by time- and angle-resolved photoemission spectroscopy (TARPES. This technique provides snapshots of the electronic structure and discloses the carrier dynamics in surface and bulk states, providing crucial information for the design of electro-spin current devices. Our results reveal the central role of doping level on the Dirac cone structure and its femtosecond dynamics. In particular, an extraordinarily long TSS lifetime is observed when the the vertex of the Dirac cone lies at the Fermi level.

Mapping of calf muscle oxygenation and haemoglobin content during dynamic plantar flexion exercise by multi-channel time-resolved near-infrared spectroscopy

International Nuclear Information System (INIS)

Torricelli, Alessandro; Quaresima, Valentina; Pifferi, Antonio; Biscotti, Giovanni; Spinelli, Lorenzo; Taroni, Paola; Ferrari, Marco; Cubeddu, Rinaldo

2004-01-01

A compact and fast multi-channel time-resolved near-infrared spectroscopy system for tissue oximetry was developed. It employs semiconductor laser and fibre optics for delivery of optical signals. Photons are collected by eight 1 mm fibres and detected by a multianode photomultiplier. A time-correlated single photon counting board is used for the parallel acquisition of time-resolved reflectance curves. Estimate of the reduced scattering coefficient is achieved by fitting with a standard model of diffusion theory, while the modified Lambert-Beer law is used to assess the absorption coefficient. In vivo measurements were performed on five healthy volunteers to monitor spatial changes in calf muscle (medial and lateral gastrocnemius; MG, LG) oxygen saturation (SmO 2 ) and total haemoglobin concentration (tHb) during dynamic plantar flexion exercise performed at 50% of the maximal voluntary contraction. At rest SmO 2 was 73.0 ± 0.9 and 70.5 ± 1.7% in MG and LG, respectively (P = 0.045). At the end of the exercise, SmO 2 decreased (69.1 ± 1.8 and 63.8 ± 2.1% in MG and LG, respectively; P 2 and tHb

Time-resolved terahertz spectroscopy of electrically conductive metal-organic frameworks doped with redox active species

Science.gov (United States)

Alberding, Brian G.; Heilweil, Edwin J.

2015-09-01

Metal-Organic Frameworks (MOFs) are three-dimensional coordination polymers that are well known for large pore surface area and their ability to adsorb molecules from both the gaseous and solution phases. In general, MOFs are electrically insulating, but promising opportunities for tuning the electronic structure exist because MOFs possess synthetic versatility; the metal and organic ligand subunits can be exchanged or dopant molecules can be introduced into the pore space. Two such MOFs with demonstrated electrical conductivity are Cu3(1,3,5-benzenetricarboxylate)2, a.k.a HKUST-1, and Cu[Ni(pyrazine-2,3-dithiolate)2]. Herein, these two MOFs have been infiltrated with the redox active species 7,7,8,8-tetracyanoquinodimethane (TCNQ) and iodine under solution phase conditions and shown to produce redox products within the MOF pore space. Vibrational bands assignable to TCNQ anion and triiodide anion have been observed in the Mid-IR and Terahertz ranges using FTIR Spectroscopy. The MOF samples have been further investigated by Time-Resolved Terehertz Spectroscopy (TRTS). Using this technique, the charge mobility, separation, and recombination dynamics have been followed on the picosecond time scale following photoexcitation with visible radiation. The preliminary results show that the MOF samples have small inherent photoconductivity with charge separation lifetimes on the order of a few picoseconds. In the case of HKUST-1, the MOF can also be supported by a TiO2 film and initial results show that charge injection into the TiO2 layer occurs with a comparable efficiency to the dye sensitizer N3, [cis-Bis(isothiocyanato)-bis(2,2'-bipyridyl-4,4'-dicarboxylato ruthenium(II)], and therefore this MOF has potential as a new light absorbing and charge conducting material in photovoltaic devices.

Application of microfluidic devices for time resolved FTIR spectroscopy

International Nuclear Information System (INIS)

Wagner, C.

2012-01-01

Within this thesis, micro fluidic mixers, operated in continuous flow mode, were used for time resolved FTIR studies of chemical reactions in aqueous solution. Any chemical reaction, that can be started upon mixing two reagents, can be examined with this technique. The mixing channel also serves as the observation window for the IR measurements. The actual measurements take place at well defined spots along this channel, corresponding to specific reaction times: moving the measurement spot (100 × 100 μm 2 ) towards the entry yields shorter reaction times, moving it towards the channel's end gives longer reaction times. The temporal resolution of the experiment depends on the flow rate inside the mixing channel and the spacing between subsequent measurement points. Fast flow rates, limited by the back pressure of the mixer leading to leakages, allow time resolutions in the sub-millisecond time range using a standard FTIR microscope, whereas slow flow rates allow the measurement of reaction times up to 1000 ms. Evaluating the mixer using a fast chemical reaction resulted in mixing times of approximately 5 ms and a homogeneous distribution of the liquids across the width of the mixing channel. The mixer was then used for the measurement of the H/D exchange on carbohydrates, the complex formaldehyde sulfite clock reaction, and the folding of the protein ubiquitin from its native to the ''A'' state, induced by mixing it with an acidified methanol solution. For cleaning the mixer a software tool, called ATLAS, was developed in LabVIEW, which was used to automatize the necessary cleaning steps performed by a dedicated flow system. Additionally, the micro mixer technology was combined with the step scan measurement technique using a beam condenser focusing the IR beam of an FTIR spectrometer down to a spot size of 1 mm diameter and through the mixer. The laser light, initiating the chemical reaction inside the mixing channel, was coupled into the focusing unit using a

Sol-to-Gel Transition in Fast Evaporating Systems Observed by in Situ Time-Resolved Infrared Spectroscopy.

Science.gov (United States)

Innocenzi, Plinio; Malfatti, Luca; Carboni, Davide; Takahashi, Masahide

2015-06-22

The in situ observation of a sol-to-gel transition in fast evaporating systems is a challenging task and the lack of a suitable experimental design, which includes the chemistry and the analytical method, has limited the observations. We synthesise an acidic sol, employing only tetraethylorthosilicate, SiCl4 as catalyst and deuterated water; the absence of water added to the sol allows us to follow the absorption from the external environment and the evaporation of deuterated water. The time-resolved data, obtained by attenuated total reflection infrared spectroscopy on an evaporating droplet, enables us to identify four different stages during evaporation. They are linked to specific hydrolysis and condensation rates that affect the uptake of water from external environment. The second stage is characterized by a decrease in hydroxyl content, a fast rise of condensation rate and an almost stationary absorption of water. This stage has been associated with the sol-to-gel transition. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Pump laser-induced space-charge effects in HHG-driven time- and angle-resolved photoelectron spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Oloff, L.-P., E-mail: oloff@physik.uni-kiel.de; Hanff, K.; Stange, A.; Rohde, G.; Diekmann, F.; Bauer, M.; Rossnagel, K., E-mail: rossnagel@physik.uni-kiel.de [Institut für Experimentelle und Angewandte Physik, Christian-Albrechts-Universität zu Kiel, D-24098 Kiel (Germany)

2016-06-14

With the advent of ultrashort-pulsed extreme ultraviolet sources, such as free-electron lasers or high-harmonic-generation (HHG) sources, a new research field for photoelectron spectroscopy has opened up in terms of femtosecond time-resolved pump-probe experiments. The impact of the high peak brilliance of these novel sources on photoemission spectra, so-called vacuum space-charge effects caused by the Coulomb interaction among the photoemitted probe electrons, has been studied extensively. However, possible distortions of the energy and momentum distributions of the probe photoelectrons caused by the low photon energy pump pulse due to the nonlinear emission of electrons have not been studied in detail yet. Here, we systematically investigate these pump laser-induced space-charge effects in a HHG-based experiment for the test case of highly oriented pyrolytic graphite. Specifically, we determine how the key parameters of the pump pulse—the excitation density, wavelength, spot size, and emitted electron energy distribution—affect the measured time-dependent energy and momentum distributions of the probe photoelectrons. The results are well reproduced by a simple mean-field model, which could open a path for the correction of pump laser-induced space-charge effects and thus toward probing ultrafast electron dynamics in strongly excited materials.

Rapid and economical data acquisition in ultrafast frequency-resolved spectroscopy using choppers and a microcontroller.

Science.gov (United States)

Guo, Liang; Monahan, Daniele M; Fleming, Graham

2016-08-08

Spectrometers and cameras are used in ultrafast spectroscopy to achieve high resolution in both time and frequency domains. Frequency-resolved signals from the camera pixels cannot be processed by common lock-in amplifiers, which have only a limited number of input channels. Here we demonstrate a rapid and economical method that achieves the function of a lock-in amplifier using mechanical choppers and a programmable microcontroller. We demonstrate the method's effectiveness by performing a frequency-resolved pump-probe measurement on the dye Nile Blue in solution.

Sensitivity enhancement of 13C nuclei in 2D J-resolved NMR spectroscopy using a recycled-flow system

International Nuclear Information System (INIS)

Ha, S.T.K.; Lee, R.W.K.; Wilkins, C.L.

1987-01-01

Recycled-flow nuclear magnetic resonance for sensitivity enhancement in 1/2 spin nuclei has been reported previously, achieving several-fold signal enhancement. The success of the method depends upon premagnetization of nuclei prior to flowing into the detector region, obviating the need for delays following data acquisition to allow spin-lattice relaxation and reduce experiment time. The actual gains of sensitivity enhancement for 13 C- 1 H 2D J-resolved NMR using a recycled-flow method are evaluated. Possible enhancements for two types of J-resolved measurements, namely, one-bond 13 C- 1 H and long range J-resolved spectroscopy, are estimated using a simple Carr-Purcell spin-echo approach to quantify the 13 C signals. The pulse sequence is simply 90 0 -t /sub 1/2/-180 0 -t/sub 1/2/-AT-t/sub d/, where t/sub 1/2/ is half the evolution time, AT is the acquisition time, and t/sub d/ the experiment repetition time. In a static 2D NMR experiment, t/sub d/ usually must be the same order of the longest spin-lattice relaxation time (T 1 ) of nuclei. Quantitative measurements using a recycled-flow system indicate t/dub d/ can be reduced to a fraction of T 1 ; hence significant time savings can be achieved. Time-savings of between 2 and 25 can be anticipated for 2D spectroscopy under flow measurement conditions used in the present study. Other types of 2D NMR spectroscopy (autocorrelation and double quantum NMR) are discussed

Investigations of suspension stability of iron oxide nanoparticles using time-resolved UV–visible spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Vikram, S.; Vasanthakumari, R. [B. S. Abdur Rahman University, Polymer Nanotechnology Centre (India); Tsuzuki, Takuya [Australian National University, Research School of Engineering, College of Engineering and Computer Science (Australia); Rangarajan, Murali, E-mail: r-murali@cb.amrita.edu [Amrita University, Center of Excellence in Advanced Materials and Green Technologies, Amrita School of Engineering Coimbatore (India)

2016-09-15

This study examines the suspension stability of iron oxide nanoparticles of different sizes, magnetic susceptibility, and saturation magnetization over long time scales in dilute systems using time-resolved UV–visible spectroscopy. The effects of citric acid as a chelating agent and applied external magnetic field are also studied. UV–visible spectra are obtained at different times for citric-acid-stabilized nanoparticles dispersed in water, and the peak absorbance is tracked with time, in the presence and absence of external magnetic fields. It is seen that the nanoparticles sediment slowly even in the absence of chain formation, with the phenomenon occurring in two-to-three regimes for the systems studied. Sedimentation exhibits either exponential or power-law behavior of maximum absorbance with time. In the dilute dispersions studied, thermal dispersion is about two orders of magnitude stronger than van der Waals interactions, and chain formation is not easy. Yet, it is likely that local anisotropic structures of the nanoparticles form, through which the attractive interactions result in sedimentation. Citric acid gradually stabilizes the aggregating particles; after an initial faster sedimentation, electrostatic repulsion causes the particles to segregate, as observed by a linear increase in the concentration of the nanoparticles at long times. In the presence of magnetic field, stabilization effects are significantly reduced. It is seen that though the attractive force between the nanoparticles and the external field is smaller than Brownian forces, together with van der Waals interactions, these attractive forces likely act as directing agents facilitating sedimentation. This study demonstrates that aggregation-induced sedimentation of magnetic nanoparticles is likely to play a significant role in magnetic drug targeting even when the particles are stabilized with chelating agents.Graphical abstract.

Investigations of suspension stability of iron oxide nanoparticles using time-resolved UV–visible spectroscopy

International Nuclear Information System (INIS)

Vikram, S.; Vasanthakumari, R.; Tsuzuki, Takuya; Rangarajan, Murali

2016-01-01

This study examines the suspension stability of iron oxide nanoparticles of different sizes, magnetic susceptibility, and saturation magnetization over long time scales in dilute systems using time-resolved UV–visible spectroscopy. The effects of citric acid as a chelating agent and applied external magnetic field are also studied. UV–visible spectra are obtained at different times for citric-acid-stabilized nanoparticles dispersed in water, and the peak absorbance is tracked with time, in the presence and absence of external magnetic fields. It is seen that the nanoparticles sediment slowly even in the absence of chain formation, with the phenomenon occurring in two-to-three regimes for the systems studied. Sedimentation exhibits either exponential or power-law behavior of maximum absorbance with time. In the dilute dispersions studied, thermal dispersion is about two orders of magnitude stronger than van der Waals interactions, and chain formation is not easy. Yet, it is likely that local anisotropic structures of the nanoparticles form, through which the attractive interactions result in sedimentation. Citric acid gradually stabilizes the aggregating particles; after an initial faster sedimentation, electrostatic repulsion causes the particles to segregate, as observed by a linear increase in the concentration of the nanoparticles at long times. In the presence of magnetic field, stabilization effects are significantly reduced. It is seen that though the attractive force between the nanoparticles and the external field is smaller than Brownian forces, together with van der Waals interactions, these attractive forces likely act as directing agents facilitating sedimentation. This study demonstrates that aggregation-induced sedimentation of magnetic nanoparticles is likely to play a significant role in magnetic drug targeting even when the particles are stabilized with chelating agents.Graphical abstract

Ultrafast time-resolved spectroscopy of xanthophylls at low temperature.

Science.gov (United States)

Cong, Hong; Niedzwiedzki, Dariusz M; Gibson, George N; Frank, Harry A

2008-03-20

Many of the spectroscopic features and photophysical properties of xanthophylls and their role in energy transfer to chlorophyll can be accounted for on the basis of a three-state model. The characteristically strong visible absorption of xanthophylls is associated with a transition from the ground state S0 (1(1)Ag-) to the S2 (1(1)Bu+) excited state. The lowest lying singlet state denoted S1 (2(1)Ag-), is a state into which absorption from the ground state is symmetry forbidden. Ultrafast optical spectroscopic studies and quantum computations have suggested the presence of additional excited singlet states in the vicinity of S1 (2(1)Ag-) and S2 (1(1)Bu+). One of these is denoted S* and has been suggested in previous work to be associated with a twisted molecular conformation of the molecule in the S1 (2(1)Ag-) state. In this work, we present the results of a spectroscopic investigation of three major xanthophylls from higher plants: violaxanthin, lutein, and zeaxanthin. These molecules have systematically increasing extents of pi-electron conjugation from nine to eleven conjugated carbon-carbon double bonds. All-trans isomers of the molecules were purified by high-performance liquid chromatography (HPLC) and studied by steady-state and ultrafast time-resolved optical spectroscopy at 77 K. Analysis of the data using global fitting techniques has revealed the inherent spectral properties and ultrafast dynamics of the excited singlet states of each of the molecules. Five different global fitting models were tested, and it was found that the data are best explained using a kinetic model whereby photoexcitation results in the promotion of the molecule into the S2 (1(1)Bu+) state that subsequently undergoes decay to a vibrationally hot S1 (1(1)Ag-) state and with the exception of violaxanthin also to the S* state. The vibrationally hot S1 (1(1)Ag-) state then cools to a vibrationally relaxed S1 (2(1)Ag-) state in less than a picosecond. It was also found that a portion

Time-Resolved Diffuse Optical Spectroscopy and Imaging Using Solid-State Detectors: Characteristics, Present Status, and Research Challenges.

Science.gov (United States)

Alayed, Mrwan; Deen, M Jamal

2017-09-14

Diffuse optical spectroscopy (DOS) and diffuse optical imaging (DOI) are emerging non-invasive imaging modalities that have wide spread potential applications in many fields, particularly for structural and functional imaging in medicine. In this article, we review time-resolved diffuse optical imaging (TR-DOI) systems using solid-state detectors with a special focus on Single-Photon Avalanche Diodes (SPADs) and Silicon Photomultipliers (SiPMs). These TR-DOI systems can be categorized into two types based on the operation mode of the detector (free-running or time-gated). For the TR-DOI prototypes, the physical concepts, main components, figures-of-merit of detectors, and evaluation parameters are described. The performance of TR-DOI prototypes is evaluated according to the parameters used in common protocols to test DOI systems particularly basic instrumental performance (BIP). In addition, the potential features of SPADs and SiPMs to improve TR-DOI systems and expand their applications in the foreseeable future are discussed. Lastly, research challenges and future developments for TR-DOI are discussed for each component in the prototype separately and also for the entire system.

Semiconductor Nonlinear Dynamics Study by Broadband Terahertz Spectroscopy

Science.gov (United States)

Ho, I.-Chen

Semiconductor nonlinearity in the terahertz (THz) frequency range has been attracting considerable attention due to the recent development of high-power semiconductor-based nanodevices. However, the underlying physics concerning carrier dynamics in the presence of high-field THz transients is still obscure. This thesis introduces an ultrafast, time-resolved THz pump/THz probe approach to the study of semiconductor properties in the nonlinear regime. The carrier dynamics regarding two mechanisms, intervalley scattering and impact ionization, is observed for doped InAs on a sub-picosecond time scale. In addition, polaron modulation driven by intense THz pulses is experimentally and theoretically investigated. The observed polaron dynamics verifies the interaction between energetic electrons and a phonon field. In contrast to previous work which reports optical phonon responses, acoustic phonon modulations are addressed in this study. A further understanding of the intense field interacting with solid materials will accelerate the development of semiconductor devices. This thesis starts with the design and performance of a table-top THz spectrometer which has the advantages of ultra-broad bandwidth (one order higher bandwidth compared to a conventional ZnTe sensor) and high electric field strength (>100 kV/cm). Unlike the conventional THz time-domain spectroscopy, the spectrometer integrates a novel THz air-biased-coherent-detection (THz-ABCD) technique and utilizes selected gases as THz emitters and sensors. In comparison with commonly used electro-optic (EO) crystals or photoconductive (PC) dipole antennas, the gases have the benefits of no phonon absorption as existing in EO crystals and no carrier life time limitation as observed in PC dipole antennas. The newly development THz-ABCD spectrometer with a strong THz field strength capability provides a platform for various research topics especially on the nonlinear carrier dynamics of semiconductors. Two mechanisms

Sensitivity Analysis and Requirements for Temporally and Spatially Resolved Thermometry Using Neutron Resonance Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Fernandez, Juan Carlos [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Barnes, Cris William [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Mocko, Michael Jeffrey [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Zavorka, Lukas [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2018-01-31

This report is intended to examine the use of neutron resonance spectroscopy (NRS) to make time- dependent and spatially-resolved temperature measurements of materials in extreme conditions. Specifically, the sensitivities of the temperature estimate on neutron-beam and diagnostic parameters is examined. Based on that examination, requirements are set on a pulsed neutron-source and diagnostics to make a meaningful measurement.

Structure in nascent carbon nanotubes revealed by spatially resolved Raman spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Landois, Périne [CEA, IRAMIS, SPAM, Laboratoire Francis Perrin (CNRS URA 2453), 91191 Gif-sur-Yvette (France); Laboratoire de Physique des Solides, UMR CNRS 8502, Université Paris Sud 11, 91405 Orsay (France); Pinault, Mathieu [CEA, IRAMIS, SPAM, Laboratoire Francis Perrin (CNRS URA 2453), 91191 Gif-sur-Yvette (France); Huard, Mickaël [Laboratoire de Physique des Solides, UMR CNRS 8502, Université Paris Sud 11, 91405 Orsay (France); Reita, Valérie [Univ. Grenoble Alpes, Inst NEEL, F-38042 Grenoble (France); CNRS, Inst NEEL, F-38042 Grenoble (France); Rouzière, Stéphan; Launois, Pascale [Laboratoire de Physique des Solides, UMR CNRS 8502, Université Paris Sud 11, 91405 Orsay (France); Mayne-L' Hermite, Martine [CEA, IRAMIS, SPAM, Laboratoire Francis Perrin (CNRS URA 2453), 91191 Gif-sur-Yvette (France); Bendiab, Nedjma, E-mail: nedjma.bendiab@grenoble.cnrs.fr [Univ. Grenoble Alpes, Inst NEEL, F-38042 Grenoble (France); CNRS, Inst NEEL, F-38042 Grenoble (France)

2014-10-01

The understanding of carbon nanotube (CNT) growth is crucial for the control of their production. In particular, the identification of structural changes of carbon possibly occurring near the catalyst particle in the very early stages of their formation is of high interest. In this study, samples of nascent CNT obtained during nucleation step and samples of vertically aligned CNT obtained during growth step are analysed by combined spatially resolved Raman spectroscopy and X-ray diffraction measurements. Spatially resolved Raman spectroscopy reveals that iron-based phases and carbon phases are co-localized at the same position, and indicates that sp{sup 2} carbon nucleates preferentially on iron-based particles during this nucleation step. Depth scan Raman spectroscopy analysis, performed on nascent CNT, highlights that carbon structural organisation is significantly changing from defective graphene layers surrounding the iron-based particles at their base up to multi-walled nanotube structures in the upper part of iron-based particles. - Highlights: • Spatial co-localization of iron and carbon structures in nascent carbon nanotubes • Imaging local carbon structure changes along catalyst particles by Raman spectroscopy. • In nascent nanotubes, significant structural changes occur along catalyst particle.

Time-resolved far-infrared experiments at the National Synchrotron Light Source. Final report

International Nuclear Information System (INIS)

Tanner, D.B.; Reitze, D.H.; Carr, G.L.

1999-01-01

A facility for time-resolved infrared and far-infrared spectroscopy has been built and commissioned at the National Synchrotron Light Source. This facility permits the study of time dependent phenomena over a frequency range from 2-8000cm -1 (0.25 meV-1 eV). Temporal resolution is approximately 200 psec and time dependent phenomena in the time range out to 100 nsec can be investigated

Broadband 2D Electronic Spectroscopy Reveals Coupling Between Dark 1Bu- State of Carotenoid and Qx State of Bacteriochlorophyll

Directory of Open Access Journals (Sweden)

Scholes Gregory D.

2013-03-01

Full Text Available The study of LH2 protein of purple bacteria by broadband 2D electronic spectroscopy is presented. The dark 1Bu- carotenoid state is directly observed in 2D spectra and its role in carotenoid-bacteriochlorophyll interaction is discussed.

Light adaptation of the unicellular red alga, Cyanidioschyzon merolae, probed by time-resolved fluorescence spectroscopy.

Science.gov (United States)

Ueno, Yoshifumi; Aikawa, Shimpei; Kondo, Akihiko; Akimoto, Seiji

2015-08-01

Photosynthetic organisms change the quantity and/or quality of their pigment-protein complexes and the interactions among these complexes in response to light conditions. In the present study, we analyzed light adaptation of the unicellular red alga Cyanidioschyzon merolae, whose pigment composition is similar to that of cyanobacteria because its phycobilisomes (PBS) lack phycoerythrin. C. merolae were grown under different light qualities, and their responses were measured by steady-state absorption, steady-state fluorescence, and picosecond time-resolved fluorescence spectroscopies. Cells were cultivated under four monochromatic light-emitting diodes (blue, green, yellow, and red), and changes in pigment composition and energy transfer were observed. Cells grown under blue and green light increased their relative phycocyanin levels compared with cells cultured under white light. Energy-transfer processes to photosystem I (PSI) were sensitive to yellow and red light. The contribution of direct energy transfer from PBS to PSI increased only under yellow light, while red light induced a reduction in energy transfer from photosystem II to PSI and an increase in energy transfer from light-harvesting chlorophyll protein complex I to PSI. Differences in pigment composition, growth, and energy transfer under different light qualities are discussed.

Femtosecond optical parametric oscillators toward real-time dual-comb spectroscopy

Science.gov (United States)

Jin, Yuwei; Cristescu, Simona M.; Harren, Frans J. M.; Mandon, Julien

2015-04-01

We demonstrate mid-infrared dual-comb spectroscopy with an optical parametric oscillator (OPO) toward real-time field measurement. A singly resonant OPO based on a MgO-doped periodically poled lithium niobate (PPLN) crystal is demonstrated. Chirped mirrors are used to compensate the dispersion caused by the optical cavity and the crystal. A low threshold of 17 mW has been achieved. The OPO source generates a tunable idler frequency comb between 2.7 and 4.7 μm. Dual-comb spectroscopy is achieved by coupling two identical Yb-fiber mode-locked lasers to this OPO with slightly different repetition frequencies. A measured absorption spectrum of methane is presented with a spectral bandwidth of , giving an instrumental resolution of . In addition, a second OPO containing two MgO-doped PPLN crystals in a singly resonant ring cavity is demonstrated. As such, this OPO generates two idler combs (average power up to 220 mW), covering a wavelength range between 2.7 and 4.2 μm, from which a mid-infrared dual-comb Fourier transform spectrometer is constructed. By detecting the heterodyned signal between the two idler combs, broadband spectra of molecular gases can be observed over a spectral bandwidth of more than . This special cavity design allows the spectral resolution to be improved to without locking the OPO cavity, indicating that this OPO represents an ideal high-power broadband mid-infrared source for real-time gas sensing.

Real-time observation of intersystem crossing induced by charge recombination during bimolecular electron transfer reactions

KAUST Repository

Alsam, Amani Abdu

2016-09-21

Real-time probing of intersystem crossing (ISC) and triplet-state formation after photoinduced electron transfer (ET) is a particularly challenging task that can be achieved by time-resolved spectroscopy with broadband capability. Here, we examine the mechanism of charge separation (CS), charge recombination (CR) and ISC of bimolecular photoinduced electron transfer (PET) between poly[(9,9-di(3,3′-N,N’-trimethyl-ammonium) propyl fluorenyl-2,7-diyl)-alt-co-(9,9-dioctyl-fluorenyl-2,7-diyl)] diiodide salt (PFN) and dicyanobenzene (DCB) using time-resolved spectroscopy. PET from PFN to DCB is confirmed by monitoring the transient absorption (TA) and infrared spectroscopic signatures for the radical ion pair (DCB─•-PFN+•). In addition, our time-resolved results clearly demonstrate that CS takes place within picoseconds followed by CR within nanoseconds. The ns-TA data exhibit the clear spectroscopic signature of PFN triplet-triplet absorption, induced by the CR of the radical ion pairs (DCB─•-PFN+•). As a result, the triplet state of PFN (3PFN*) forms and subsequently, the ground singlet state is replenished within microseconds. © 2016

Time-resolved spectroscopy and fluorescence resonance energy transfer in the study of excimer laser damage of chromatin

Energy Technology Data Exchange (ETDEWEB)

Radu, L. [Department of Molecular Genetics and Radiobiology, Babes National Institute, Bucharest (Romania)], E-mail: lilianajradu@yahoo.fr; Mihailescu, I. [Department of Lasers, Laser, Plasma and Radiation Physics Institute, Bucharest (Romania); Radu, S. [Department of Computer Science, Polytechnics University, Bucharest (Romania); Gazdaru, D. [Department of Biophysics, Bucharest University (Romania)

2007-09-21

The analysis of chromatin damage produced by a 248 nm excimer laser radiation, for doses of 0.3-3 MJ/m{sup 2} was carried out by time-resolved spectroscopy and fluorescence resonance energy transfer (FRET). The chromatin was extracted from a normal and a tumoral tissue of Wistar rats. The decrease with laser dose of the relative contribution of the excited state lifetimes of ethidium bromide (EtBr) bounded to chromatin constitutes an evidence of the reduction of chromatin deoxyribonucleic acid (DNA) double-strand structure. FRET was performed from dansyl chloride to acridine orange, both coupled to chromatin. The increase of the average distance between these ligands, under the action of laser radiation, reflects a loosening of the chromatin structure. The radiosensitivity of tumor tissue chromatin is higher than that of a normal tissue. The determination of the chromatin structure modification in an excimer laser field can be of interest in laser therapy.

Time-resolved spectroscopy and fluorescence resonance energy transfer in the study of excimer laser damage of chromatin

International Nuclear Information System (INIS)

Radu, L.; Mihailescu, I.; Radu, S.; Gazdaru, D.

2007-01-01

The analysis of chromatin damage produced by a 248 nm excimer laser radiation, for doses of 0.3-3 MJ/m 2 was carried out by time-resolved spectroscopy and fluorescence resonance energy transfer (FRET). The chromatin was extracted from a normal and a tumoral tissue of Wistar rats. The decrease with laser dose of the relative contribution of the excited state lifetimes of ethidium bromide (EtBr) bounded to chromatin constitutes an evidence of the reduction of chromatin deoxyribonucleic acid (DNA) double-strand structure. FRET was performed from dansyl chloride to acridine orange, both coupled to chromatin. The increase of the average distance between these ligands, under the action of laser radiation, reflects a loosening of the chromatin structure. The radiosensitivity of tumor tissue chromatin is higher than that of a normal tissue. The determination of the chromatin structure modification in an excimer laser field can be of interest in laser therapy

Time resolved techniques: An overview

International Nuclear Information System (INIS)

Larson, B.C.; Tischler, J.Z.

1990-06-01

Synchrotron sources provide exceptional opportunities for carrying out time-resolved x-ray diffraction investigations. The high intensity, high angular resolution, and continuously tunable energy spectrum of synchrotron x-ray beams lend themselves directly to carrying out sophisticated time-resolved x-ray scattering measurements on a wide range of materials and phenomena. When these attributes are coupled with the pulsed time-structure of synchrotron sources, entirely new time-resolved scattering possibilities are opened. Synchrotron beams typically consist of sub-nanosecond pulses of x-rays separated in time by a few tens of nanoseconds to a few hundred nanoseconds so that these beams appear as continuous x-ray sources for investigations of phenomena on time scales ranging from hours down to microseconds. Studies requiring time-resolution ranging from microseconds to fractions of a nanosecond can be carried out in a triggering mode by stimulating the phenomena under investigation in coincidence with the x-ray pulses. Time resolution on the picosecond scale can, in principle, be achieved through the use of streak camera techniques in which the time structure of the individual x-ray pulses are viewed as quasi-continuous sources with ∼100--200 picoseconds duration. Techniques for carrying out time-resolved scattering measurements on time scales varying from picoseconds to kiloseconds at present and proposed synchrotron sources are discussed and examples of time-resolved studies are cited. 17 refs., 8 figs

Energy- and angled-resolved photoelectron spectroscopy of negative ions

International Nuclear Information System (INIS)

Pegg, D.J.; Thompson, J.S.; Compton, R.N.; Alton, G.D.

1988-01-01

Energy- and angle-resolved photoelectron detachment spectroscopy is currently being used to investigate the structure of negative ions and their interaction with radiation. Measurements of the electron affinity of the Ca atom and the partial cross sections for photodetachment of the metastable negative ion, He - (1s2s2p 4 P), are reported. 5 refs., 5 figs

Femtosecond time-resolved transient absorption spectroscopy of xanthophylls

Czech Academy of Sciences Publication Activity Database

Niedzwiedzki, D.; Sullivan, J.O.; Polívka, Tomáš; Birge, R.R.; Frank, H.A.

2006-01-01

Roč. 110, č. 45 (2006), s. 22872-22885 ISSN 1520-6106 Institutional research plan: CEZ:AV0Z50510513 Keywords : xanthophyll * spectroscopy study Subject RIV: BO - Biophysics Impact factor: 4.115, year: 2006

Broadband time-resolved elliptical crystal spectrometer for X-ray spectroscopic measurements in laser-produced plasmas

International Nuclear Information System (INIS)

Wang Rui-Rong; Jia Guo; Fang Zhi-Heng; Wang Wei; Meng Xiang-Fu; Xie Zhi-Yong; Zhang Fan

2014-01-01

The X-ray spectrometer used in high-energy-density plasma experiments generally requires both broad X-ray energy coverage and high temporal, spatial, and spectral resolutions for overcoming the difficulties imposed by the X-ray background, debris, and mechanical shocks. By using an elliptical crystal together with a streak camera, we resolve this issue at the SG-II laser facility. The carefully designed elliptical crystal has a broad spectral coverage with high resolution, strong rejection of the diffuse and/or fluorescent background radiation, and negligible source broadening for extended sources. The spectra that are Bragg reflected (23° < θ < 38°) from the crystal are focused onto a streak camera slit 18 mm long and about 80 μm wide, to obtain a time-resolved spectrum. With experimental measurements, we demonstrate that the quartz(1011) elliptical analyzer at the SG-II laser facility has a single-shot spectral range of (4.64–6.45) keV, a typical spectral resolution of E/ΔE = 560, and an enhanced focusing power in the spectral dimension. For titanium (Ti) data, the lines of interest show a distribution as a function of time and the temporal variations of the He-α and Li-like Ti satellite lines and their spatial profiles show intensity peak red shifts. The spectrometer sensitivity is illustrated with a temporal resolution of better than 25 ps, which satisfies the near-term requirements of high-energy-density physics experiments. (atomic and molecular physics)

Large Molecule Structures by Broadband Fourier Transform Molecular Rotational Spectroscopy

Science.gov (United States)

Evangelisti, Luca; Seifert, Nathan A.; Spada, Lorenzo; Pate, Brooks

2016-06-01

Fourier transform molecular rotational resonance spectroscopy (FT-MRR) using pulsed jet molecular beam sources is a high-resolution spectroscopy technique that can be used for chiral analysis of molecules with multiple chiral centers. The sensitivity of the molecular rotational spectrum pattern to small changes in the three dimensional structure makes it possible to identify diastereomers without prior chemical separation. For larger molecules, there is the additional challenge that different conformations of each diastereomer may be present and these need to be differentiated from the diastereomers in the spectral analysis. Broadband rotational spectra of several larger molecules have been measured using a chirped-pulse FT-MRR spectrometer. Measurements of nootkatone (C15H22O), cedrol (C15H26O), ambroxide (C16H28O) and sclareolide (C16H26O2) are presented. These spectra are measured with high sensitivity (signal-to-noise ratio near 1,000:1) and permit structure determination of the most populated isomers using isotopic analysis of the 13C and 18O isotopologues in natural abundance. The accuracy of quantum chemistry calculations to identify diastereomers and conformers and to predict the dipole moment properties needed for three wave mixing measurements is examined.

Hemodynamic measurements in deep brain tissues of humans by near-infrared time-resolved spectroscopy

Science.gov (United States)

Suzuki, Hiroaki; Oda, Motoki; Yamaki, Etsuko; Suzuki, Toshihiko; Yamashita, Daisuke; Yoshimoto, Kenji; Homma, Shu; Yamashita, Yutaka

2014-03-01

Using near-infrared time-resolved spectroscopy (TRS), we measured the human head in transmittance mode to obtain the optical properties, tissue oxygenation, and hemodynamics of deep brain tissues in 50 healthy adult volunteers. The right ear canal was irradiated with 3-wavelengths of pulsed light (760, 795, and 835nm), and the photons passing through the human head were collected at the left ear canal. Optical signals with sufficient intensity could be obtained from 46 of the 50 volunteers. By analyzing the temporal profiles based on the photon diffusion theory, we successfully obtained absorption coefficients for each wavelength. The levels of oxygenated hemoglobin (HbO2), deoxygenated hemoglobin (Hb), total hemoglobin (tHb), and tissue oxygen saturation (SO2) were then determined by referring to the hemoglobin spectroscopic data. Compared with the SO2 values for the forehead measurements in reflectance mode, the SO2 values of the transmittance measurements of the human head were approximately 10% lower, and tHb values of the transmittance measurements were always lower than those of the forehead reflectance measurements. Moreover, the level of hemoglobin and the SO2 were strongly correlated between the human head measurements in transmittance mode and the forehead measurements in the reflectance mode, respectively. These results demonstrated a potential application of this TRS system in examining deep brain tissues of humans.

Positron annihilation response and broadband dielectric spectroscopy: salol.

Science.gov (United States)

Bartoš, J; Iskrová, M; Köhler, M; Wehn, R; Sauša, O; Lunkenheimer, P; Krištiak, J; Loidl, A

2011-09-01

A phenomenological analysis of the ortho-positronium (o-Ps) annihilation from positron annihilation lifetime spectroscopy (PALS) and the dynamics from broadband dielectric spectroscopy (BDS) are reported on a small molecular glass former of intermediate H-bonding and fragility: salol. The dielectric spectra extend over a very broad frequency range of about 2 × 10(-2)-3.5 × 10(11) Hz, providing information on the α-relaxation, the secondary relaxation giving rise to the excess wing, and the shallow high-frequency minimum in the micro- to milli-meter wave range. A number of empirical correlations between the o-Ps lifetime, τ(3)(T), and the various spectral and relaxation features have been observed. Thus, the phenomenological evaluation of the τ(3)(T) dependence of the PALS response of the amorphous sample reveals three characteristic PALS temperatures: T(g)(PALS), T(b1)(L) = 1.15T(g)(PALS) and T(b2)(L) = 1.25T(g)(PALS), which are discussed in relation to similar findings for some typical small molecular vdW- and H-bonded glass formers. A slighter change of the slope at T(b1)(L) appears to be related to the transition from excess wing to the primary α-process-dominated behavior, with the secondary process dominating in the deeply supercooled liquid state below T(b1)(L). The high-temperature plateau effect in the τ (3)(T) plot occurs at T(b2)(L) and agrees with the characteristic Stickel temperature, T(B)(ST), marking a qualitative change of the primary α process, but it does not follow the relation T(b2)(L) application of the two-order parameter (TOP) model to the structural relaxation as represented by the primary α relaxation times from BDS leads to the characteristic TOP temperature, T(m)(c), close to T(b1) from PALS. Within this model the phenomenological interpretation is offered based on changes in the probability of occurrence of solid-like and liquid-like domains to explain the dynamic as well as PALS responses. In summary, all the empirical

Time-resolved pump and probe x-ray absorption fine structure spectroscopy at beamline P11 at PETRA III

Energy Technology Data Exchange (ETDEWEB)

Göries, D., E-mail: dennis.goeries@desy.de; Roedig, P.; Stübe, N.; Meyer, J.; Warmer, M.; Weckert, E.; Meents, A., E-mail: alke.meents@desy.de [DESY Photon Science, Deutsches Elektronen-Synchrotron (DESY), Notkestraße 85, 22607 Hamburg (Germany); Dicke, B.; Naumova, M.; Rübhausen, M. [Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg (Germany); Galler, A.; Gawelda, W.; Geßler, P.; Sotoudi Namin, H.; Beckmann, A. [European XFEL, Albert-Einstein Ring 19, 22761 Hamburg (Germany); Britz, A.; Bressler, C. [European XFEL, Albert-Einstein Ring 19, 22761 Hamburg (Germany); The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg (Germany); Schlie, M. [Institut für Experimentalphysik, University of Hamburg, Luruper Chaussee 149, 22761 Hamburg (Germany)

2016-05-15

We report about the development and implementation of a new setup for time-resolved X-ray absorption fine structure spectroscopy at beamline P11 utilizing the outstanding source properties of the low-emittance PETRA III synchrotron storage ring in Hamburg. Using a high intensity micrometer-sized X-ray beam in combination with two positional feedback systems, measurements were performed on the transition metal complex fac-Tris[2-phenylpyridinato-C2,N]iridium(III) also referred to as fac-Ir(ppy){sub 3}. This compound is a representative of the phosphorescent iridium(III) complexes, which play an important role in organic light emitting diode (OLED) technology. The experiment could directly prove the anticipated photoinduced charge transfer reaction. Our results further reveal that the temporal resolution of the experiment is limited by the PETRA III X-ray bunch length of ∼103 ps full width at half maximum (FWHM).

Direct Structural and Chemical Characterization of the Photolytic Intermediates of Methylcobalamin Using Time-Resolved X-ray Absorption Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Subramanian, Ganesh; Zhang, Xiaoyi; Kodis, Gerdenis; Kong, Qingyu; Liu, Cunming; Chizmeshya, Andrew; Weierstall, Uwe; Spence, John

2018-04-05

Cobalt−carbon bond cleavage is crucial to most natural and synthetic applications of the cobalamin class of compounds, and here we present the first direct electronic and geometric structural characteristics of intermediates formed following photoexcitation of methylcobalamin (MeCbl) using time-resolved X-ray absorption spectroscopy (XAS). We catch transients corresponding to two intermediates, in the hundreds of picoseconds and a few microseconds. Highlights of the picosecond intermediate, which is reduced in comparison to the ground state, are elongation of the upper axial Co−C bond and relaxation of the corrin ring. This is not so with the recombining photocleaved products captured at a few microseconds, where the Co−C bond almost (yet not entirely) reverts to its ground state configuration and a substantially elongated lower axial Co−NIm bond is observed. The reduced cobalt site here confirms formation of methyl radical as the photoproduct.

Investigations of lateral and vertical compositional gradients in Cu(In,Ga)Se{sub 2} by highly spatially, spectrally and time resolved cathodoluminescence spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Mueller, Mathias; Ribbe, Stefan; Hempel, Thomas; Bertram, Frank; Christen, Juergen [Institute for Experimental Physics, Otto-von-Guericke-University, Magdeburg (Germany); Witte, Wolfram; Hariskos, Dimitrios [Zentrum fuer Sonnenenergie- und Wasserstoff-Forschung Baden-Wuerttemberg (ZSW), Stuttgart (Germany)

2011-07-01

Luminescence properties of Cu(In,Ga)Se{sub 2} (CIGS) layers with different thicknesses were investigated by means of highly spatially, spectrally and time resolved cathodoluminescence (CL) spectroscopy at low temperature (T=5 K). A polycrystalline CIGS thin film with a thickness of 2.4 {mu}m was grown using an in-line co-evaporation process with a final Cu-poor composition on top of a sputtered Mo layer on a soda lime glass substrate. The layer thickness was then reduced by highly controlled bromine methanol etching. The typical grainy (d{sub average}=3 {mu}m) structure of the untouched sample develops thin longish structures under the influence of the etchant. Integral CL spectra of the samples are dominated by donor-acceptor pair (DAP) luminescence. The peak energies of these spectra are ranging from 1.13 eV to 1.22 eV with decreasing layer thickness. The lateral distribution of the luminescence is inhomogeneous regarding the intensity as well as the peak energy. Time resolved CL shows a strong dependence of the initial lifetime from the emission energy.

Rare Earth Elements as Potential Biosignatures on Mars in SuperCam Time Resolved Laser Fluorescence Spectroscopy Data

Science.gov (United States)

Ollila, A.; Beyssac, O.; Sharma, S. K.; Misra, A. K.; Clegg, S. M.; Gauthier, M.; Wiens, R. C.; Maurice, S.; Gasnault, O.; Lanza, N.

2017-12-01

The rare earth elements (REE, La to Lu) are a group of elements with similar chemical properties that are generally present in geologic materials at trace concentrations. REEs may be concentrated via processes such as igneous fractional crystallization in accessory minerals, e.g. apatite, zircon, and titanite. Additionally, however, concentrations of REE may serve to identify regions of high astrobiological interest. For example, Fe-oxyhydroxide deposits in hydrothermal vent systems and biologically related manganese nodules may be enriched in REEs. REEs have not been measured in situ on Mars, therefore their prevalence and distribution on Mars is as yet unknown, except as observed in martian meteorites. SuperCam is a survey instrument that will analyze materials around the Mars 2020 rover using a variety of spectral techniques including laser-induced breakdown spectroscopy (LIBS), Raman, VIS-IR, and time-resolved laser fluorescence (TRLF) spectroscopy. Recently, the SuperCam Engineering Development Unit was tested at the Los Alamos National Laboratory for its capabilities to detect REEs in minerals using TRLF spectroscopy. While this instrument was not designed to precisely replicate the flight model, the spectral resolution and light transmission was sufficient to obtain TRLF spectra on a number of minerals demonstrating a variety of REE luminescent centers. These include apatite (Sm3+, Nd3+, Eu3+, Dy3+), fluorite (Ho3+, Sm3+, Dy3+, Nd3+), and zircon (Er3+, Pr3+, Nd3+). Future work includes expanding this suite to include minerals associated with biological activities, for example Mn-oxides (desert varnish and manganese nodules), hydrothermal Fe-oxides, and stromatolite-associated carbonates. In this way and in combination with its other techniques, SuperCam may direct the rover team to perform further analyses of similar samples by the in situ chemical and mineralogical suite of instruments, or aid in prioritization for sample return.

Time-Resolved Synchronous Fluorescence for Biomedical Diagnosis

Science.gov (United States)

Zhang, Xiaofeng; Fales, Andrew; Vo-Dinh, Tuan

2015-01-01

This article presents our most recent advances in synchronous fluorescence (SF) methodology for biomedical diagnostics. The SF method is characterized by simultaneously scanning both the excitation and emission wavelengths while keeping a constant wavelength interval between them. Compared to conventional fluorescence spectroscopy, the SF method simplifies the emission spectrum while enabling greater selectivity, and has been successfully used to detect subtle differences in the fluorescence emission signatures of biochemical species in cells and tissues. The SF method can be used in imaging to analyze dysplastic cells in vitro and tissue in vivo. Based on the SF method, here we demonstrate the feasibility of a time-resolved synchronous fluorescence (TRSF) method, which incorporates the intrinsic fluorescent decay characteristics of the fluorophores. Our prototype TRSF system has clearly shown its advantage in spectro-temporal separation of the fluorophores that were otherwise difficult to spectrally separate in SF spectroscopy. We envision that our previously-tested SF imaging and the newly-developed TRSF methods will combine their proven diagnostic potentials in cancer diagnosis to further improve the efficacy of SF-based biomedical diagnostics. PMID:26404289

Time-resolved laser fluorescence spectroscopy of organic ligands by europium: Fluorescence quenching and lifetime properties

Science.gov (United States)

Nouhi, A.; Hajjoul, H.; Redon, R.; Gagné, J. P.; Mounier, S.

2018-03-01

Time-resolved Laser Fluorescence Spectroscopy (TRLFS) has proved its usefulness in the fields of biophysics, life science and geochemistry to characterize the fluorescence probe molecule with its chemical environment. The purpose of this study is to demonstrate the applicability of this powerful technique combined with Steady-State (S-S) measurements. A multi-mode factor analysis, in particular CP/PARAFAC, was used to analyze the interaction between Europium (Eu) and Humic substances (HSs) extracted from Saint Lawrence Estuary in Canada. The Saint Lawrence system is a semi-enclosed water stream with connections to the Atlantic Ocean and is an excellent natural laboratory. CP/PARAFAC applied to fluorescence S-S data allows introspecting ligands-metal interactions and the one-site 1:1 modeling gives information about the stability constants. From the spectral signatures and decay lifetimes data given by TRLFS, one can deduce the fluorescence quenching which modifies the fluorescence and discuss its mechanisms. Results indicated a relatively strong binding ability between europium and humic substances samples (Log K value varies from 3.38 to 5.08 at pH 7.00). Using the Stern-Volmer plot, it has been concluded that static and dynamic quenching takes places in the case of salicylic acid and europium interaction while for HSs interaction only a static quenching is observed.

Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system.

Science.gov (United States)

Falge, Mirjam; Fröbel, Friedrich Georg; Engel, Volker; Gräfe, Stefanie

2017-08-02

If the adiabatic approximation is valid, electrons smoothly adapt to molecular geometry changes. In contrast, as a characteristic of diabatic dynamics, the electron density does not follow the nuclear motion. Recently, we have shown that the asymmetry in time-resolved photoelectron spectra serves as a tool to distinguish between these dynamics [Falge et al., J. Phys. Chem. Lett., 2012, 3, 2617]. Here, we investigate the influence of an additional, moderately intense infrared (IR) laser field, as often applied in attosecond time-resolved experiments, on such asymmetries. This is done using a simple model for coupled electronic-nuclear motion. We calculate time-resolved photoelectron spectra and their asymmetries and demonstrate that the spectra directly map the bound electron-nuclear dynamics. From the asymmetries, we can trace the IR field-induced population transfer and both the field-driven and intrinsic (non-)adiabatic dynamics. This holds true when considering superposition states accompanied by electronic coherences. The latter are observable in the asymmetries for sufficiently short XUV pulses to coherently probe the coupled states. It is thus documented that the asymmetry is a measure for phases in bound electron wave packets and non-adiabatic dynamics.

STROBE-X: X-ray Timing & Spectroscopy on Dynamical Timescales from Milliseconds to Years

Science.gov (United States)

Wilson-Hodge, Colleen A.; Ray, P. S.; Maccarone, T; Chakrabarty, D.; Gendreau, K.; Arzoumanian, Z.; Jenke, P.; Ballantyne, D.; Bozzo, E.; Brandt, S.;

Direct and quantitative broadband absorptance spectroscopy with multilayer cantilever probes

Science.gov (United States)

Hsu, Wei-Chun; Tong, Jonathan Kien-Kwok; Liao, Bolin; Chen, Gang

2015-04-21

A system for measuring the absorption spectrum of a sample is provided that includes a broadband light source that produces broadband light defined within a range of an absorptance spectrum. An interferometer modulates the intensity of the broadband light source for a range of modulation frequencies. A bi-layer cantilever probe arm is thermally connected to a sample arm having at most two layers of materials. The broadband light modulated by the interferometer is directed towards the sample and absorbed by the sample and converted into heat, which causes a temperature rise and bending of the bi-layer cantilever probe arm. A detector mechanism measures and records the deflection of the probe arm so as to obtain the absorptance spectrum of the sample.

Ionomer Dynamics: Insights from Broadband Dielectric Spectroscopy

Science.gov (United States)

Runt, James

2015-03-01

Ionomers (polymers containing ionic functionality) have been traditionally used as packaging materials and in molding applications, and are now of increasing interest as candidate single ion conductors for energy storage devices, in energy conversion, and for other electroactive materials applications. The focus of this presentation is on the insight that broadband dielectric (impedance) spectroscopy brings to our understanding of ion and polymer dynamics of this family of materials. As an example of our recent work on relatively conductive ionomers, the first portion of the presentation will focus on anion conducting polyphosphazene ionomers, in which polymer bound cations are quaternized with either short alkyl or short ether oxygen chains. The low Tg, amorphous nature, and cation-solvating backbone distinguish polyphosphazenes as promising materials for ion conduction, the iodide variants being of particular interest in solar cells. In the second part of this overview, the first findings on the molecular dynamics of linear precise polyethylene-based ionomers containing 1-methylimidazolium bromide pendants on exactly every 9th, 15th, or 21st carbon atom will be summarized. In order to develop a robust interpretation of the dynamics of these materials, it is imperative to develop a thorough understanding of microphase separation (e.g. ion aggregation), and each of the above studies is complimented by multiangle X-ray scattering experiments. Supported by the NSF Polymers Program and DOE Basic Energy Sciences.

Kinetics of methane-ethane gas replacement in clathrate-hydrates studied by time-resolved neutron diffraction and Raman spectroscopy.

Science.gov (United States)

Murshed, M Mangir; Schmidt, Burkhard C; Kuhs, Werner F

2010-01-14

The kinetics of CH(4)-C(2)H(6) replacement in gas hydrates has been studied by in situ neutron diffraction and Raman spectroscopy. Deuterated ethane structure type I (C(2)H(6) sI) hydrates were transformed in a closed volume into methane-ethane mixed structure type II (CH(4)-C(2)H(6) sII) hydrates at 5 MPa and various temperatures in the vicinity of 0 degrees C while followed by time-resolved neutron powder diffraction on D20 at ILL, Grenoble. The role of available surface area of the sI starting material on the formation kinetics of sII hydrates was studied. Ex situ Raman spectroscopic investigations were carried out to crosscheck the gas composition and the distribution of the gas species over the cages as a function of structure type and compared to the in situ neutron results. Raman micromapping on single hydrate grains showed compositional and structural gradients between the surface and core of the transformed hydrates. Moreover, the observed methane-ethane ratio is very far from the one expected for a formation from a constantly equilibrated gas phase. The results also prove that gas replacement in CH(4)-C(2)H(6) hydrates is a regrowth process involving the nucleation of new crystallites commencing at the surface of the parent C(2)H(6) sI hydrate with a progressively shrinking core of unreacted material. The time-resolved neutron diffraction results clearly indicate an increasing diffusion limitation of the exchange process. This diffusion limitation leads to a progressive slowing down of the exchange reaction and is likely to be responsible for the incomplete exchange of the gases.

The Fourteenth International Meeting on Time-Resolved Vibrational Spectroscopy (TRVS XIV)

Science.gov (United States)

2010-02-03

conferences covering the use of advanced vibrational spectroscopy for the use of studying time-dependent molecular processes in chemistry, physics ...Netherlands a.huertaviga@uva.nl Neil Hunt Dept of  Physics , University of Strathclyde United Kingdom nhunt@phys.strath.ac Koichi Iwata Gakushuin University...Dasgupta Mark Creelman Sangdeok Shim Biochemical Reaction Dynamics, , , UC B k ler e ey 11:50 AM C W. Zinth, W. J. Schreier, J. Kubon, N. Regner, K

Photophysical characterization and time-resolved spectroscopy of a anthradithiophene dimer: exploring the role of conformation in singlet fission

KAUST Repository

Dean, Jacob C.

2017-08-18

Quantitative singlet fission has been observed for a variety of acene derivatives such as tetracene and pentacene, and efforts to extend the library of singlet fission compounds is of current interest. Preliminary calculations suggest anthradithiophenes exhibit significant exothermicity between the first optically-allowed singlet state, S1, and 2 × T1 with an energy difference of >5000 cm−1. Given the fulfillment of this ingredient for singlet fission, here we investigate the singlet fission capability of a difluorinated anthradithiophene dimer (2ADT) covalently linked by a (dimethylsilyl)ethane bridge and derivatized by triisobutylsilylethynyl (TIBS) groups. Photophysical characterization of 2ADT and the single functionalized ADT monomer were carried out in toluene and acetone solution via absorption and fluorescence spectroscopy, and their photo-initiated dynamics were investigated with time-resolved fluorescence (TRF) and transient absorption (TA) spectroscopy. In accordance with computational predictions, two conformers of 2ADT were observed via fluorescence spectroscopy and were assigned to structures with the ADT cores trans or cis to one another about the covalent bridge. The two conformers exhibited markedly different excited state deactivation mechanisms, with the minor trans population being representative of the ADT monomer showing primarily radiative decay, while the dominant cis population underwent relaxation into an excimer geometry before internally converting to the ground state. The excimer formation kinetics were found to be solvent dependent, yielding time constants of ∼1.75 ns in toluene, and ∼600 ps in acetone. While the difference in rates elicits a role for the solvent in stabilizing the excimer structure, the rate is still decidedly long compared to most singlet fission rates of analogous dimers, suggesting that the excimer is neither a kinetic nor a thermodynamic trap, yet singlet fission was still not observed. The result

Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study

Energy Technology Data Exchange (ETDEWEB)

Wu, Guorong [National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 (Canada); State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023 (China); Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026 (China); Neville, Simon P. [Department of Chemistry, University of Ottawa, 10 Marie Curie, Ottawa, Ontario K1N 6N5 (Canada); Schalk, Oliver [National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 (Canada); Department of Physics, AlbaNova University Center, Stockholm University, Roslagstullsbacken 21, 106 91 Stockholm (Sweden); Sekikawa, Taro [Department of Applied Physics, Hokkaido University, Kita-13 Nishi-8, Kita-ku, Sapporo 060-8628 (Japan); Ashfold, Michael N. R. [School of Chemistry, University of Bristol, Bristol BS8 1TS (United Kingdom); Worth, Graham A. [School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT (United Kingdom); Stolow, Albert, E-mail: astolow@uottawa.ca [National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 (Canada); Department of Chemistry, University of Ottawa, 10 Marie Curie, Ottawa, Ontario K1N 6N5 (Canada); Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5 (Canada)

2016-01-07

The dynamics of N-methylpyrrole following excitation at wavelengths in the range 241.5-217.0 nm were studied using a combination of time-resolved photoelectron spectroscopy (TRPES), ab initio quantum dynamics calculations using the multi-layer multi-configurational time-dependent Hartree method, as well as high-level photoionization cross section calculations. Excitation at 241.5 and 236.2 nm results in population of the A{sub 2}(πσ{sup ∗}) state, in agreement with previous studies. Excitation at 217.0 nm prepares the previously neglected B{sub 1}(π3p{sub y}) Rydberg state, followed by prompt internal conversion to the A{sub 2}(πσ{sup ∗}) state. In contrast with the photoinduced dynamics of pyrrole, the lifetime of the wavepacket in the A{sub 2}(πσ{sup ∗}) state was found to vary with excitation wavelength, decreasing by one order of magnitude upon tuning from 241.5 nm to 236.2 nm and by more than three orders of magnitude when excited at 217.0 nm. The order of magnitude difference in lifetimes measured at the longer excitation wavelengths is attributed to vibrational excitation in the A{sub 2}(πσ{sup ∗}) state, facilitating wavepacket motion around the potential barrier in the N–CH{sub 3} dissociation coordinate.

Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study

International Nuclear Information System (INIS)

Wu, Guorong; Neville, Simon P.; Schalk, Oliver; Sekikawa, Taro; Ashfold, Michael N. R.; Worth, Graham A.; Stolow, Albert

2016-01-01

The dynamics of N-methylpyrrole following excitation at wavelengths in the range 241.5-217.0 nm were studied using a combination of time-resolved photoelectron spectroscopy (TRPES), ab initio quantum dynamics calculations using the multi-layer multi-configurational time-dependent Hartree method, as well as high-level photoionization cross section calculations. Excitation at 241.5 and 236.2 nm results in population of the A 2 (πσ ∗ ) state, in agreement with previous studies. Excitation at 217.0 nm prepares the previously neglected B 1 (π3p y ) Rydberg state, followed by prompt internal conversion to the A 2 (πσ ∗ ) state. In contrast with the photoinduced dynamics of pyrrole, the lifetime of the wavepacket in the A 2 (πσ ∗ ) state was found to vary with excitation wavelength, decreasing by one order of magnitude upon tuning from 241.5 nm to 236.2 nm and by more than three orders of magnitude when excited at 217.0 nm. The order of magnitude difference in lifetimes measured at the longer excitation wavelengths is attributed to vibrational excitation in the A 2 (πσ ∗ ) state, facilitating wavepacket motion around the potential barrier in the N–CH 3 dissociation coordinate

Time-resolved X-ray transmission microscopy on magnetic microstructures

International Nuclear Information System (INIS)

Puzic, Aleksandar

2007-01-01

Three excitation schemes were designed for stroboscopic imaging of magnetization dynamics with time-resolved magnetic transmission X-ray microscopy (TR-MTXM). These techniques were implemented into two types of X-ray microscopes, namely the imaging transmission X-ray microscope (ITXM) and the scanning transmission X-ray microscope (STXM), both installed at the electron storage ring of the Advanced Light Source in Berkeley, USA. Circular diffraction gratings (Fresnel zone plates) used in both microscopes as focusing and imaging elements presently allow for lateral resolution down to 30 nm. Magnetic imaging is performed by using the X-ray magnetic circular dichroism (XMCD) as element specific contrast mechanism. The developed methods have been successfully applied to the experimental investigation of magnetization dynamics in ferromagnetic microstructures. A temporal resolution well below 100 ps was achieved. A conventional pump-probe technique was implemented first. The dynamic response of the magnetization excited by a broadband pulsed magnetic field was imaged spatially resolved using focused X-ray flashes. As a complementary method, the spatially resolved ferromagnetic resonance (SR-FMR) technique was developed for experimental study of magnetization dynamics in the frequency domain. As a third excitation mode, the burst excitation was implemented. The performance and efficiency of the developed methods have been demonstrated by imaging the local magnetization dynamics in laterally patterned ferromagnetic thin-film elements and three-layer stacks. The existence of multiple eigenmodes in the excitation spectra of ferromagnetic microstructures has been verified by using the pump-probe technique. Magnetostatic spin waves were selectively excited and detected with a time resolution of 50 ps using the SR-FMR technique. Thorough analysis of 20 in most cases independently prepared samples has verified that vortices which exhibit a low-amplitude switching of their core

Insights into the Structural Changes Occurring upon Photoconversion in the Orange Carotenoid Protein from Broadband Two-Dimensional Electronic Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

De Re, Eleonora; Schlau-Cohen, Gabriela S.; Leverenz, Ryan L.; Huxter, Vanessa M.; Oliver, Thomas A. A.; Mathies, Richard A.; Fleming, Graham R.

2014-05-22

Carotenoids play an essential role in photoprotection, interacting with other pigments to safely dissipate excess absorbed energy as heat. In cyanobacteria, the short time scale photoprotective mechanisms involve the photoactive orange carotenoid protein (OCP), which binds a single carbonyl carotenoid. Blue-green light induces the photoswitching of OCP from its ground state form (OCPO) to a metastable photoproduct (OCPR). OCPR can bind to the phycobilisome antenna and induce fluorescence quenching. The photoswitching is accompanied by structural and functional changes at the level of the protein and of the bound carotenoid. In this study, we use broadband two-dimensional electronic spectroscopy to look at the differences in excited state dynamics of the carotenoid in the two forms of OCP. Our results provide insight into the origin of the pronounced vibrational lineshape and oscillatory dynamics observed in linear absorption and 2D electronic spectroscopy of OCPO and the large inhomogeneous broadening in OCPR, with consequences for the chemical function of the two forms.

Probing specific molecular processes and intermediates by time-resolved Fourier transform infrared spectroscopy: application to the bacteriorhodopsin photocycle.

Science.gov (United States)

Lórenz-Fonfría, Víctor A; Kandori, Hideki; Padrós, Esteve

2011-06-23

We present a general approach for probing the kinetics of specific molecular processes in proteins by time-resolved Fourier transform infrared (IR) spectroscopy. Using bacteriorhodopsin (bR) as a model we demonstrate that by appropriately monitoring some selected IR bands it is possible obtaining the kinetics of the most important events occurring in the photocycle, namely changes in the chromophore and the protein backbone conformation, and changes in the protonation state of the key residues implicated in the proton transfers. Besides confirming widely accepted views of the bR photocycle, our analysis also sheds light into some disputed issues: the degree of retinal torsion in the L intermediate to respect the ground state; the possibility of a proton transfer from Asp85 to Asp212; the relationship between the protonation/deprotonation of Asp85 and the proton release complex; and the timing of the protein backbone dynamics. By providing a direct way to estimate the kinetics of photocycle intermediates the present approach opens new prospects for a robust quantitative kinetic analysis of the bR photocycle, which could also benefit the study of other proteins involved in photosynthesis, in phototaxis, or in respiratory chains.

Interest in broadband dielectric spectroscopy to study the electronic transport in materials for lithium batteries

Energy Technology Data Exchange (ETDEWEB)

Badot, Jean-Claude, E-mail: jc.badot@chimie-paristech.fr [Institut de Recherche de Chimie Paris, UMR CNRS 8247, Réseau sur le Stockage Electrochimique de l' Energie (RS2E), Chimie Paris Tech, PSL*, 11 rue P. et M. Curie, 75231 Cedex 05 Paris (France); Lestriez, Bernard [Institut des Matériaux Jean Rouxel, UMR CNRS 6502, Université de Nantes, 2 rue de la Houssinière, BP32229, 44322 Nantes (France); Dubrunfaut, Olivier [GeePs | Group of electrical engineering – Paris, UMR CNRS 8507, CentraleSupélec, Univ. Paris-Sud, Université Paris-Saclay, Sorbonne Universités, UPMC Univ Paris 06, 3 & 11 rue Joliot-Curie, Plateau de Moulon, 91192 Gif-sur-Yvette CEDEX, Paris (France)

2016-11-15

Highlights: • Broadband dielectric spectroscopy measures the multiscale electronic conductivity from macroscopic to interatomic sizes. • There is an influence of the surface states on the electronic transfer of powdered materials (e.g. thin insulating layer of Li{sub 2}CO{sub 3} on LiNiO{sub 2} and carbon coating on LiFePO{sub 4}). • Electrical relaxations resulting from the interfacial polarizations at the different scales of the carbon black network are evidenced. - Abstract: Broadband dielectric spectroscopy (BDS) is used to measure complex permittivity and conductivity of conducting materials for lithium batteries at frequencies from a few Hz to several GHz with network and impedance analysers. Under the influence of an electric field, there will be charge density fluctuations in the conductor mainly due to electronic transfer. These fluctuations result in dielectric relaxations for frequencies below 100 GHz. The materials are compacted powders in which each element (particles, agglomerates of particles) can have different sizes and morphologies. In the present review, studies are reported on the influence of surface states in LiNiO{sub 2} (ageing and degradation in air) and LiFePO{sub 4} (carbon coating thin layer), and on a composite electrode based on the lithium trivanadate (Li{sub 1.1}V{sub 3}O{sub 8}) active material. The results have shown that the BDS technique is very sensitive to the different scales of materials architectures involved in electronic transport, from interatomic distances to macroscopic sizes.

Interest in broadband dielectric spectroscopy to study the electronic transport in materials for lithium batteries

International Nuclear Information System (INIS)

Badot, Jean-Claude; Lestriez, Bernard; Dubrunfaut, Olivier

2016-01-01

Highlights: • Broadband dielectric spectroscopy measures the multiscale electronic conductivity from macroscopic to interatomic sizes. • There is an influence of the surface states on the electronic transfer of powdered materials (e.g. thin insulating layer of Li_2CO_3 on LiNiO_2 and carbon coating on LiFePO_4). • Electrical relaxations resulting from the interfacial polarizations at the different scales of the carbon black network are evidenced. - Abstract: Broadband dielectric spectroscopy (BDS) is used to measure complex permittivity and conductivity of conducting materials for lithium batteries at frequencies from a few Hz to several GHz with network and impedance analysers. Under the influence of an electric field, there will be charge density fluctuations in the conductor mainly due to electronic transfer. These fluctuations result in dielectric relaxations for frequencies below 100 GHz. The materials are compacted powders in which each element (particles, agglomerates of particles) can have different sizes and morphologies. In the present review, studies are reported on the influence of surface states in LiNiO_2 (ageing and degradation in air) and LiFePO_4 (carbon coating thin layer), and on a composite electrode based on the lithium trivanadate (Li_1_._1V_3O_8) active material. The results have shown that the BDS technique is very sensitive to the different scales of materials architectures involved in electronic transport, from interatomic distances to macroscopic sizes.

Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy

Directory of Open Access Journals (Sweden)

Georgi L. Dakovski

2015-09-01

Full Text Available A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy, which significantly limits the accessible momentum space. Using 20.15 eV, 12 fs pulses, we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate that non-monotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in stark contrast to the monotonic relaxation in the nodal and off-nodal regions.

A time resolved microfocus XEOL facility at the Diamond Light Source

International Nuclear Information System (INIS)

Mosselmans, J F W; Taylor, R P; Quinn, P D; Cibin, G; Gianolio, D; Finch, A A; Sapelkin, A V

2013-01-01

We have constructed a Time-Resolved X-ray Excited Optical Luminescence (TR-XEOL) detection system at the Microfocus Spectroscopy beamline I18 at the Diamond Light Source. Using the synchrotron in h ybrid bunch mode , the data collection is triggered by the RF clock, and we are able to record XEOL photons with a time resolution of 6.1 ps during the 230 ns gap between the hybrid bunch and the main train of electron bunches. We can detect photons over the range 180-850 nm using a bespoke optical fibre, with X-ray excitation energies between 2 and 20 keV. We have used the system to study a range of feldspars. The detector is portable and has also been used on beamline B18 to collect Optically Determined X-ray Absorption Spectroscopy (OD-XAS) in QEXAFS mode.

A time resolved microfocus XEOL facility at the Diamond Light Source

Science.gov (United States)

Mosselmans, J. F. W.; Taylor, R. P.; Quinn, P. D.; Finch, A. A.; Cibin, G.; Gianolio, D.; Sapelkin, A. V.

2013-03-01

We have constructed a Time-Resolved X-ray Excited Optical Luminescence (TR-XEOL) detection system at the Microfocus Spectroscopy beamline I18 at the Diamond Light Source. Using the synchrotron in "hybrid bunch mode", the data collection is triggered by the RF clock, and we are able to record XEOL photons with a time resolution of 6.1 ps during the 230 ns gap between the hybrid bunch and the main train of electron bunches. We can detect photons over the range 180-850 nm using a bespoke optical fibre, with X-ray excitation energies between 2 and 20 keV. We have used the system to study a range of feldspars. The detector is portable and has also been used on beamline B18 to collect Optically Determined X-ray Absorption Spectroscopy (OD-XAS) in QEXAFS mode.

New techniques of time-resolved infrared and Raman spectroscopy using ultrashort laser pulses

International Nuclear Information System (INIS)

Laubereau, A.

1986-01-01

Considerable progress has been made in recent years in the field of spectroscopic applications of ultrashort laser pulses. This paper examines two approaches toward studying ultrafast relaxation processes in condensed matter: an IR technique which complements coherent Raman scattering; and a Fourier Raman method with high frequency resolution. The time domain IR spectroscopy technique has been applied to various vibration-rotation transitions of pure HCl gas and in mixtures with Ar buffer gas. The advantage of the time domain measurements instead of frequency spectroscopy is readily visualized when one recalls that a frequency resolution of 10 -3 cm -1 corresponds to time observations over 10 -8 , which are readily feasible. As a first demonstration of the FT-Raman technique the author presents experimental data on the Q-branch of the v 1 -vibrational mode of methane. An example for the experimental data obtained approximately 2 mm behind the nozzle is presented; the coherent anti-Stokes Raman signal is plotted versus delay time. A complicated beating structure and the decay of the signal envelope are readily seen. The desired spectroscopic information is obtained by numerical Fourier transformation of the experimental points presented

Detection of rhodopsin dimerization in situ by PIE-FCCS, a time-resolved fluorescence spectroscopy.

Science.gov (United States)

Smith, Adam W

2015-01-01

Rhodopsin self-associates in the plasma membrane. At low concentrations, the interactions are consistent with a monomer-dimer equilibrium (Comar et al., J Am Chem Soc 136(23):8342-8349, 2014). At high concentrations in native tissue, higher-order clusters have been observed (Fotiadis et al., Nature 421:127-128, 2003). The physiological role of rhodopsin dimerization is still being investigated, but it is clear that a quantitative assessment is essential to determining the function of rhodopsin clusters in vision. To quantify rhodopsin interactions, I will outline the theory and methodology of a specialized time-resolved fluorescence spectroscopy for measuring membrane protein-protein interactions called pulsed-interleaved excitation fluorescence cross-correlation spectroscopy (PIE-FCCS). The strength of this technique is its ability to quantify rhodopsin interactions in situ (i.e., a live cell plasma membrane). There are two reasons for restricting the scope to live cell membranes. First, the compositional heterogeneity of the plasma membrane creates a complex milieu with thousands of lipid, protein, and carbohydrate species. This makes it difficult to infer quaternary interactions from detergent solubilized samples or construct a model phospholipid bilayer that recapitulates all of the interactions present in native membranes. Second, organizational structure and dynamics is a key feature of the plasma membrane, and fixation techniques like formaldehyde cross-linking and vitrification will modulate the interactions. PIE-FCCS is based on two-color fluorescence imaging with time-correlated single-photon counting (TCSPC) (Becker et al., Rev Sci Instrum 70:1835-1841, 1999). By time-tagging every detected photon, the data can be analyzed as a fluorescence intensity distribution, fluorescence lifetime histogram, or fluorescence (cross-)correlation spectra (FCS/FCCS) (Becker, Advanced time-correlated single-photon counting techniques, Springer, Berlin, 2005). These

Time-resolved laser spectroscopy in the UV/VUV spectral region

International Nuclear Information System (INIS)

Bengtsson, J.

1992-01-01

Radiative lifetimes ranging from 3 to 500 ns were measured on various states of Ag, N, Se, Te and As, by recording the fluorescence light decay after excitation by a laser pulse. Ag was supplied by a collimated atomic beam while Se, Te and As were contained in quartz cells. Pulsed laser radiation, with a wavelength down to 185 nm, was generated by different set-ups, using Nd-YAG pumped dye lasers combined with non-linear crystals and Raman shifting. Short laser pulses were produced by a nitrogen laser or a distributed feedback dye laser. Two-photon processes and stepwise excitation were used to populate high-lying levels. Depletion spectroscopy, quantum-beat spectroscopy and optical double resonance spectroscopy were also performed

Comb-Resolved Dual-Comb Spectroscopy Stabilized by Free-Running Continuous-Wave Lasers

Science.gov (United States)

Kuse, Naoya; Ozawa, Akira; Kobayashi, Yohei

2012-11-01

We demonstrate dual-comb spectroscopy with relatively phase-locked two frequency combs, instead of frequency combs firmly fixed to the absolute frequency references. By stabilizing two beat frequencies between two mode-locked lasers at different wavelengths observed via free-running continuous-wave (CW) lasers, two combs are tightly phase locked to each other. The frequency noise of the CW lasers barely affects the performance of dual-comb spectroscopy because of the extremely fast common-mode noise rejection. Transform-limited comb-resolved dual-comb spectroscopy with a 6 Hz radio frequency linewidth is demonstrated by the use of Yb-fiber oscillators.

Chemical sensitivity of InP/In0.48Ga0.52P surface quantum dots studied by time-resolved photoluminescence spectroscopy

International Nuclear Information System (INIS)

De Angelis, Roberta; Casalboni, Mauro; De Matteis, Fabio; Hatami, Fariba; Masselink, William T.; Zhang, Hong; Prosposito, Paolo

2015-01-01

InP/InGaP surface quantum dots represent an attractive material for optical chemical sensors since they show a remarkable near infra-red emission at room temperature, whose intensity increases rapidly and reversibly depending on the composition of the environmental atmosphere. We show here their emission properties by time resolved photoluminescence spectroscopy investigation. Photoluminescence transients with and without chemical solvent vapours (methanol, clorophorm, acetone and water) were fitted with a 3-exponential decay law with times of about 0.5 ns, 2 ns and 7 ns. The measurements revealed a weak effect on clorophorm, acetone and water, while the initial decay time of InP surface quantum dots increases (up to 15%) upon methanol vapour exposure, indicating that the organic molecules efficiently saturate QD non-radiative surface states. - Highlights: • InP SQDs emission depends on the presence of solvent vapours in the atmosphere. • TR photoluminescence transients were fitted with a 3-exponential decay law. • The initial decay time increases (up to 15%) upon methanol vapour exposure. • Organic molecules efficiently saturate QD non-radiative surface states.

Kinetics of the F+NO2+M->FNO2+M reaction studied by pulse radiolysis combined with time-resolved IR and UV spectroscopy

DEFF Research Database (Denmark)

Pagsberg, Palle Bjørn; Sillesen, A.; Jodkowski, J.T.

1996-01-01

was studied with SF6 pressures of 5-1000 mbar at 298 K. Comparative studies were carried out by monitoring the decay kinetics of NO2 at 445 nm using pressures of 100-1000 mbar at 295 and 341 K. The observed pressure dependence is represented in terms of a fall-off curve with the following values......The title reaction was initiated by the pulse radiolysis of SF6/NO2 gas mixtures, and the formation of FNO2 was studied by time-resolved infrared spectroscopy employing strong rotational transitions within the nu(1) and nu(4) bands of FNO2. The pressure dependence of the formation kinetics...

Photo-Induced Spin-State Conversion in Solvated Transition Metal Complexes Probed via Time-Resolved Soft X-ray Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Huse, Nils; Kim, Tae Kyu; Jamula, Lindsey; McCusker, James K.; de Groot, Frank M. F.; Schoenlein, Robert W.

2010-04-30

Solution-phase photoinduced low-spin to high-spin conversion in the FeII polypyridyl complex [Fe(tren(py)3)]2+ (where tren(py)3 is tris(2-pyridylmethyliminoethyl)amine) has been studied via picosecond soft X-ray spectroscopy. Following 1A1 --> 1MLCT (metal-to-ligand charge transfer) excitation at 560 nm, changes in the iron L2- and L3-edges were observed concomitant with formation of the transient high-spin 5T2 state. Charge-transfer multiplet calculations coupled with data acquired on low-spin and high-spin model complexes revealed a reduction in ligand field splitting of 1 eV in the high-spin state relative to the singlet ground state. A significant reduction in orbital overlap between the central Fe-3d and the ligand N-2p orbitals was directly observed, consistent with the expected ca. 0.2 Angstrom increase in Fe-N bond length upon formation of the high-spin state. The overall occupancy of the Fe-3d orbitals remains constant upon spin crossover, suggesting that the reduction in sigma-donation is compensated by significant attenuation of pi-back-bonding in the metal-ligand interactions. These results demonstrate the feasibility and unique potential of time-resolved soft X-ray absorption spectroscopy to study ultrafast reactions in the liquid phase by directly probing the valence orbitals of first-row metals as well as lighter elements during the course of photochemical transformations.

Broadband dielectric spectroscopy of oxidized porous silicon

International Nuclear Information System (INIS)

Axelrod, Ekaterina; Urbach, Benayahu; Sa'ar, Amir; Feldman, Yuri

2006-01-01

Dielectric measurements accompanied by infrared absorption and photoluminescence (PL) spectroscopy were used to investigate the electrical and optical properties of oxidized porous silicon (PS). As opposed to non-oxidized PS, only high temperature relaxation processes could be resolved for oxidized PS. Two relaxation processes have been observed. The first process is related to dc-conductivity that dominates at high temperatures and low frequencies. After subtraction of dc-conductivity we could analyse a second high-temperature relaxation process that is related to interface polarization induced by charge carriers trapped at the host matrix-pore interfaces. We found that, while the main effect of the oxidation on the PL appears to be a size reduction in the silicon nanocrystals that gives rise to a blue shift of the PL spectrum, its main contribution to the dielectric properties turns out to be blocking of transport channels in the host tissue and activation of hopping conductivity between silicon nanocrystals

Broadband dielectric spectroscopy of oxidized porous silicon

Energy Technology Data Exchange (ETDEWEB)

Axelrod, Ekaterina [Department of Applied Physics, Hebrew University of Jerusalem, Jerusalem, 91904 (Israel); Urbach, Benayahu [Racah Institute of Physics and the Center for Nanoscience and Nanotechnology, Hebrew University of Jerusalem, Jerusalem, 91904 (Israel); Sa' ar, Amir [Racah Institute of Physics and the Center for Nanoscience and Nanotechnology, Hebrew University of Jerusalem, Jerusalem, 91904 (Israel); Feldman, Yuri [Department of Applied Physics, Hebrew University of Jerusalem, Jerusalem, 91904 (Israel)

2006-04-07

Dielectric measurements accompanied by infrared absorption and photoluminescence (PL) spectroscopy were used to investigate the electrical and optical properties of oxidized porous silicon (PS). As opposed to non-oxidized PS, only high temperature relaxation processes could be resolved for oxidized PS. Two relaxation processes have been observed. The first process is related to dc-conductivity that dominates at high temperatures and low frequencies. After subtraction of dc-conductivity we could analyse a second high-temperature relaxation process that is related to interface polarization induced by charge carriers trapped at the host matrix-pore interfaces. We found that, while the main effect of the oxidation on the PL appears to be a size reduction in the silicon nanocrystals that gives rise to a blue shift of the PL spectrum, its main contribution to the dielectric properties turns out to be blocking of transport channels in the host tissue and activation of hopping conductivity between silicon nanocrystals.

Ultrafast time-resolved faraday rotation in EuO thin films.

Science.gov (United States)

Liu, F; Makino, T; Yamasaki, T; Ueno, K; Tsukazaki, A; Fukumura, T; Kong, Y; Kawasaki, M

2012-06-22

We have investigated the ultrafast spin dynamics in EuO thin films by time-resolved Faraday rotation spectroscopy. The photoinduced magnetization is found to be increased in a transient manner, accompanied with subsequent demagnetization. The dynamical magnetization enhancement showed a maximum slightly below the Curie temperature with prolonged tails toward both lower and higher temperatures and dominates the demagnetization counterpart at 55 K. The magnetization enhancement component decays in ~1 ns. The realization of the transient collective ordering is attributable to the enhancement of the f-d exchange interaction.

Atomic column resolved electron energy-loss spectroscopy

International Nuclear Information System (INIS)

Duscher, G.; Pennycook, S.J.; Browning, N.D.

1998-01-01

Spatially resolved electron energy-loss spectroscopy (EELS) is rapidly developing into a unique and powerful tool to characterize internal interfaces. Because atomic column resolved Z-contrast imaging can be performed simultaneously with EELS in the scanning transmission electron microscope, this combination allows the atomic structure to be correlated with the electronic structure, and thus the local properties of interfaces or defects can be determined directly. However, the ability to characterize interfaces and defects at that level requires not only high spatial resolution but also the exact knowledge of the beam location, from where the spectrum is obtained. Here we discuss several examples progressing from cases where the limitation in spatial resolution is given by the microscopes or the nature of the sample, to one example of impurity atoms at a grain boundary, which show intensity and fine structure changes from atomic column to atomic column. Such data can be interpreted as changes in valence of the impurity, depending on its exact site in the boundary plane. Analysis ofthis nature is a valuable first step in understanding the microscopic structural, optical and electronic properties of materials. (orig.)

Exciplex formation in bimolecular photoinduced electron-transfer investigated by ultrafast time-resolved infrared spectroscopy.

Science.gov (United States)

Koch, Marius; Letrun, Romain; Vauthey, Eric

2014-03-12

The dynamics of bimolecular photoinduced electron-transfer reactions has been investigated with three donor/acceptor (D/A) pairs in tetrahydrofuran (THF) and acetonitrile (ACN) using a combination of ultrafast spectroscopic techniques, including time-resolved infrared absorption. For the D/A pairs with the highest driving force of electron transfer, all transient spectroscopic features can be unambiguously assigned to the excited reactant and the ionic products. For the pair with the lowest driving force, three additional transient infrared bands, more intense in THF than in ACN, with a time dependence that differs from those of the other bands are observed. From their frequency and solvent dependence, these bands can be assigned to an exciplex. Moreover, polarization-resolved measurements point to a relatively well-defined mutual orientation of the constituents and to a slower reorientational time compared to those of the individual reactants. Thanks to the minimal overlap of the infrared signature of all transient species in THF, a detailed reaction scheme including the relevant kinetic and thermodynamic parameters could be deduced for this pair. This analysis reveals that the formation and recombination of the ion pair occur almost exclusively via the exciplex.

Externally calibrated parallel imaging for 3D multispectral imaging near metallic implants using broadband ultrashort echo time imaging.

Science.gov (United States)

Wiens, Curtis N; Artz, Nathan S; Jang, Hyungseok; McMillan, Alan B; Reeder, Scott B

2017-06-01

To develop an externally calibrated parallel imaging technique for three-dimensional multispectral imaging (3D-MSI) in the presence of metallic implants. A fast, ultrashort echo time (UTE) calibration acquisition is proposed to enable externally calibrated parallel imaging techniques near metallic implants. The proposed calibration acquisition uses a broadband radiofrequency (RF) pulse to excite the off-resonance induced by the metallic implant, fully phase-encoded imaging to prevent in-plane distortions, and UTE to capture rapidly decaying signal. The performance of the externally calibrated parallel imaging reconstructions was assessed using phantoms and in vivo examples. Phantom and in vivo comparisons to self-calibrated parallel imaging acquisitions show that significant reductions in acquisition times can be achieved using externally calibrated parallel imaging with comparable image quality. Acquisition time reductions are particularly large for fully phase-encoded methods such as spectrally resolved fully phase-encoded three-dimensional (3D) fast spin-echo (SR-FPE), in which scan time reductions of up to 8 min were obtained. A fully phase-encoded acquisition with broadband excitation and UTE enabled externally calibrated parallel imaging for 3D-MSI, eliminating the need for repeated calibration regions at each frequency offset. Significant reductions in acquisition time can be achieved, particularly for fully phase-encoded methods like SR-FPE. Magn Reson Med 77:2303-2309, 2017. © 2016 International Society for Magnetic Resonance in Medicine. © 2016 International Society for Magnetic Resonance in Medicine.

Turbulent Statistics From Time-Resolved PIV Measurements of a Jet Using Empirical Mode Decomposition

Science.gov (United States)

Dahl, Milo D.

2013-01-01

Empirical mode decomposition is an adaptive signal processing method that when applied to a broadband signal, such as that generated by turbulence, acts as a set of band-pass filters. This process was applied to data from time-resolved, particle image velocimetry measurements of subsonic jets prior to computing the second-order, two-point, space-time correlations from which turbulent phase velocities and length and time scales could be determined. The application of this method to large sets of simultaneous time histories is new. In this initial study, the results are relevant to acoustic analogy source models for jet noise prediction. The high frequency portion of the results could provide the turbulent values for subgrid scale models for noise that is missed in large-eddy simulations. The results are also used to infer that the cross-correlations between different components of the decomposed signals at two points in space, neglected in this initial study, are important.

Time-Resolved Fluorescence Spectroscopy and Fluorescence Lifetime Imaging Microscopy for Characterization of Dendritic Polymer Nanoparticles and Applications in Nanomedicine

Directory of Open Access Journals (Sweden)

Alexander Boreham

2016-12-01

Full Text Available The emerging field of nanomedicine provides new approaches for the diagnosis and treatment of diseases, for symptom relief and for monitoring of disease progression. One route of realizing this approach is through carefully constructed nanoparticles. Due to the small size inherent to the nanoparticles a proper characterization is not trivial. This review highlights the application of time-resolved fluorescence spectroscopy and fluorescence lifetime imaging microscopy (FLIM for the analysis of nanoparticles, covering aspects ranging from molecular properties to particle detection in tissue samples. The latter technique is particularly important as FLIM allows for distinguishing of target molecules from the autofluorescent background and, due to the environmental sensitivity of the fluorescence lifetime, also offers insights into the local environment of the nanoparticle or its interactions with other biomolecules. Thus, these techniques offer highly suitable tools in the fields of particle development, such as organic chemistry, and in the fields of particle application, such as in experimental dermatology or pharmaceutical research.

Time-Resolved Fluorescence Spectroscopy and Fluorescence Lifetime Imaging Microscopy for Characterization of Dendritic Polymer Nanoparticles and Applications in Nanomedicine.

Science.gov (United States)

Boreham, Alexander; Brodwolf, Robert; Walker, Karolina; Haag, Rainer; Alexiev, Ulrike

2016-12-24

The emerging field of nanomedicine provides new approaches for the diagnosis and treatment of diseases, for symptom relief and for monitoring of disease progression. One route of realizing this approach is through carefully constructed nanoparticles. Due to the small size inherent to the nanoparticles a proper characterization is not trivial. This review highlights the application of time-resolved fluorescence spectroscopy and fluorescence lifetime imaging microscopy (FLIM) for the analysis of nanoparticles, covering aspects ranging from molecular properties to particle detection in tissue samples. The latter technique is particularly important as FLIM allows for distinguishing of target molecules from the autofluorescent background and, due to the environmental sensitivity of the fluorescence lifetime, also offers insights into the local environment of the nanoparticle or its interactions with other biomolecules. Thus, these techniques offer highly suitable tools in the fields of particle development, such as organic chemistry, and in the fields of particle application, such as in experimental dermatology or pharmaceutical research.

Service Differentiation in Residential Broadband Networks

DEFF Research Database (Denmark)

Sigurdsson, Halldór Matthias

2004-01-01

As broadband gains widespread adoption with residential users, revenue generating voice- and video-services have not yet taken off. This slow uptake is often attributed to lack of Quality of Service management in residential broadband networks. To resolve this and induce service variety, network...... access providers are implementing service differentiation in their networks where voice and video gets prioritised before data. This paper discusses the role of network access providers in multipurpose packet based networks and the available migration strategies for supporting multimedia services...... in digital subscriber line (DSL) based residential broadband networks. Four possible implementation scenarios and their technical characteristics and effects are described. To conclude, the paper discusses how network access providers can be induced to open their networks for third party service providers....

Time resolved plasma characterization in a long conduction time planar plasma opening switch

International Nuclear Information System (INIS)

Adler, L.K.; Greenly, J.B.; Qi, N.; Hammer, D.A.

1989-01-01

The authors discuss additional experiments in which the plasma dynamics and properties will be monitored in detail before and during opening. Space and time resolved density, temperature and motion information about the plasma and neutrals is given by emission spectroscopy and streak photography and correlated to the current and voltage traces. Specifically, we will look for the effects of neutrals evolving off of surfaces, stagnation of the switch plasma, and rvec J x rvec B motion of the plasma downstream of the switch. Diagnostics include current and voltage monitors, a multi-aperture biased Faraday cup, emission spectroscopy and streak photography. Pairs of B dot loops are positioned in the stripline just upstream and downstream of the POS. Also, two single B loops were placed further downstream to look for bulk plasma motion. An inductive monitor gives the voltage at the upstream side of the POS and the Faraday cup monitors the gun plasma consistency from shot to shot

Proceedings of the Third Symposium Optical Spectroscopy SOS-84

International Nuclear Information System (INIS)

Fassler, D.; Feller, K.H.; Wilhelmi, B.

1985-01-01

The main topics of the symposium were: 1) new developments and applications of laser spectroscopy including time resolved UV/VIS spectroscopy, time resolved fluorescence spectroscopy, and laser Raman spectroscopy, 2) dynamics and photokinetics of molecular systems, and 3) spectroscopy and photoprocesses in organized biological systems

Time-resolved and steady-state studies of biologically and chemically relevant systems using laser, absorption, and fluorescence spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Barnes, Charles Ashley [Iowa State Univ., Ames, IA (United States)

2014-12-20

In Chapter 2 several experimental and data analysis methods used in this thesis are described. In Chapter 3 steady-state fluorescence spectroscopy was used to determine the concentration of the efflux pump inhibitors (EPIs), pheophorbide a and pyropheophorbide a, in the feces of animals and it was found that their levels far exceed those reported to be inhibitory to efflux pumps. In Chapter 4 the solvation dynamics of 6-Propionyl-2-(N,Ndimethyl) aminonaphthalene (PRODAN) was studied in reverse micelles. The two fluorescent states of PRODAN solvate on different time scales and as such care must be exercised in solvation dynamic studies involving it and its analogs. In Chapter 5 we studied the experimental and theoretical solvation dynamics of coumarin 153 (C153) in wild-type (WT) and modified myoglobins. Based on the nuclear magnetic resonance (NMR) spectroscopy and time-resolved fluorescence studies, we have concluded that it is important to thoroughly characterize the structure of a protein and probe system before comparing the theoretical and experimental results. In Chapter 6 the photophysical and spectral properties of a derivative of the medically relevant compound curcumin called cyclocurcumin was studied. Based on NMR, fluorescence, and absorption studies, the ground- and excited-states of cyclocurcumin are complicated by the existence of multiple structural isomers. In Chapter 7 the hydrolysis of cellulose by a pure form of cellulase in an ionic liquid, HEMA, and its aqueous mixtures at various temperatures were studied with the goal of increasing the cellulose to glucose conversion for biofuel production. It was found that HEMA imparts an additional stability to cellulase and can allow for faster conversion of cellulose to glucose using a pre-treatment step in comparison to only buffer.

Relationship between time-resolved and non-time-resolved Beer-Lambert law in turbid media.

Science.gov (United States)

Nomura, Y; Hazeki, O; Tamura, M

1997-06-01

The time-resolved Beer-Lambert law proposed for oxygen monitoring using pulsed light was extended to the non-time-resolved case in a scattered medium such as living tissues with continuous illumination. The time-resolved Beer-Lambert law was valid for the phantom model and living tissues in the visible and near-infrared regions. The absolute concentration and oxygen saturation of haemoglobin in rat brain and thigh muscle could be determined. The temporal profile of rat brain was reproduced by Monte Carlo simulation. When the temporal profiles of rat brain under different oxygenation states were integrated with time, the absorbance difference was linearly related to changes in the absorption coefficient. When the simulated profiles were integrated, there was a linear relationship within the absorption coefficient which was predicted for fractional inspiratory oxygen concentration from 10 to 100% and, in the case beyond the range of the absorption coefficient, the deviation from linearity was slight. We concluded that an optical pathlength which is independent of changes in the absorption coefficient is a good approximation for near-infrared oxygen monitoring.

Development of a method for the in situ measurement of polycyclic aromatic hydrocarbons with time resolved laser fluorescence spectroscopy. Final report

International Nuclear Information System (INIS)

Jaeger, E.; Weissbach, A.; Koenig, F.; Paul, T.

1994-01-01

A method was developed for the detection of polycyclic aromatic hydrocarbons (PAH) in water on the basis of time resolved laser fluorescence spectroscopy. The detection of the sum of PAH in ground- and surfacewater is possible with high sensitivity and selectivity. The fluorescence of other substances like chlorophyll or dissolved organic matter is suppressed by a special choice of spectral and temporal windows. The method works without any sample preparation and gives the results in a very short time. On the basis of this method a first device was built with a sensitivity of 0,1 μg/1 PAH in water. The measuring time was less than one minute. The on site use of this prototype is possible because of the use of a battery driven nitrogen laser together with a notebook computer for system control The application of fiberoptic cables up to 30 meter length makes it possible to use the system for screening and monitoring of polluted areas both in existing wells and without any well by using geological probe techniques. (orig.) [de

Broadband Spectroscopy of Nanoporous-Gold Promoter

Directory of Open Access Journals (Sweden)

S. K. Nakatani

2014-02-01

Full Text Available The efficiency of UV photocatalysis on TiO2 particles was increased by mixing TiO2 particles with nanoporous gold (NPG with pore diameters of 10–40 nm. This means that NPG acts as a promoter in the photocatalytic reaction of TiO2. Broadband spectroscopic results from millimeter wave to ultra violet of NPG membrane are discussed to estimate plasmonic effect on the catalysis.

Time-resolved broadband analysis of slow-light propagation and superluminal transmission of electromagnetic waves in three-dimensional photonic crystals

NARCIS (Netherlands)

Gómez Rivas, J.; Farré Benet, A.; Niehusmann, J.; Haring Bolivar, P.; Kurz, H.

2005-01-01

A time-resolved analysis of the amplitude and phase of THz pulses propagating through three-dimensional photonic crystals is presented. Single-cycle pulses of THz radiation allow measurements over a wide frequency range, spanning more than an octave below, at and above the bandgap of strongly

Noncontact blood species identification method based on spatially resolved near-infrared transmission spectroscopy

Science.gov (United States)

Zhang, Linna; Sun, Meixiu; Wang, Zhennan; Li, Hongxiao; Li, Yingxin; Li, Gang; Lin, Ling

2017-09-01

The inspection and identification of whole blood are crucially significant for import-export ports and inspection and quarantine departments. In our previous research, we proved Near-Infrared diffuse transmitted spectroscopy method was potential for noninvasively identifying three blood species, including macaque, human and mouse, with samples measured in the cuvettes. However, in open sampling cases, inspectors may be endangered by virulence factors in blood samples. In this paper, we explored the noncontact measurement for classification, with blood samples measured in the vacuum blood vessels. Spatially resolved near-infrared spectroscopy was used to improve the prediction accuracy. Results showed that the prediction accuracy of the model built with nine detection points was more than 90% in identification between all five species, including chicken, goat, macaque, pig and rat, far better than the performance of the model built with single-point spectra. The results fully supported the idea that spatially resolved near-infrared spectroscopy method can improve the prediction ability, and demonstrated the feasibility of this method for noncontact blood species identification in practical applications.

Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

Science.gov (United States)

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.

Unfolding of Ubiquitin Studied by Picosecond Time-Resolved Fluorescence of the Tyrosine Residue

OpenAIRE

Noronha, Melinda; Lima, João C.; Bastos, Margarida; Santos, Helena; Maçanita, António L.

2004-01-01

The photophysics of the single tyrosine in bovine ubiquitin (UBQ) was studied by picosecond time-resolved fluorescence spectroscopy, as a function of pH and along thermal and chemical unfolding, with the following results: First, at room temperature (25°C) and below pH 1.5, native UBQ shows single-exponential decays. From pH 2 to 7, triple-exponential decays were observed and the three decay times were attributed to the presence of tyrosine, a tyrosine-carboxylate hydrogen-bonded complex, and...

Studies on Ternary Complex Formation of U(VI)-salicylate by Using Time-resolved Fluorescence Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Cha, Wan Sik; Cho, H. R.; Park, K. K.; Kim, W. H.; Jung, E. C. [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

2010-05-15

Organic ligands containing carboxylic and phenolic functional groups naturally occur in groundwater environment, particularly in forms of polyelectrolytes such as humic and fulvic acids, from microbial degradation of biomass, e.g., plant and animal tissues. These ligands play important roles in dissolution and migration of actinide radionuclide species since they can form stable ternary actinide complexes with common inorganic ions like hydroxides and carbonates. Therefore, model ternary complexes of lanthanides and actinides have been targets of studies to understand their chemical behaviors under near-neutral pH groundwater conditions. Previous model carboxylic ligands include phthalates, maleic acids, or alpha- substituted carboxylic acids. However, majority of previous studies investigated binary systems or used potentiometric titration method that requires high ligand concentration in mM levels. Recently, highly sensitive time-resolved laserinduced fluorescence spectroscopy (TRLFS) has been used to investigate lower concentration (e.g., a few {mu}M levels) reactions of binary complexes between of ligands and metal ions. This technique provides information regarding electronic structures and complexation constants as well as fluorescence quenching mechanism. In the present study, we studied the U(VI)-OH-salicylate (SA) ternary complex formation at higher pH (> 4) via TRLF spectrum and UV-Vis absorbance measurement. Preliminary studies show that the fluorescence (FL) intensity of hydroxouranyl species at pH 4.5 decreases as SA concentration elevates in aqueous solution. Fluorescence quenching mechanism by SA is suggested based on FL intensity (I) and lifetime (tau) measurement via TRLFS

Spatially resolved x-ray fluorescence spectroscopy of beryllium capsule implosions at the NIF

Science.gov (United States)

MacDonald, M. J.; Bishel, D. T.; Saunders, A. M.; Scott, H. A.; Kyrala, G.; Kline, J.; MacLaren, S.; Thorn, D. B.; Yi, S. A.; Zylstra, A. B.; Falcone, R. W.; Doeppner, T.

2017-10-01

Beryllium ablators used in indirectly driven inertial confinement fusion implosions are doped with copper to prevent preheat of the cryogenic hydrogen fuel. Here, we present analysis of spatially resolved copper K- α fluorescence spectra from the beryllium ablator layer. It has been shown that K- α fluorescence spectroscopy can be used to measure plasma conditions of partially ionized dopants in high energy density systems. In these experiments, K-shell vacancies in the copper dopant are created by the hotspot emission at stagnation, resulting in K-shell fluorescence at bang time. Spatially resolved copper K- α emission spectra are compared to atomic kinetics and radiation code simulations to infer density and temperature profiles. This work was supported by the US DOE under Grant No. DE-NA0001859, under the auspices of the US DOE by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344, and by Los Alamos National Laboratory under contract DE-AC52-06NA52396.

Thermo-oxidative degradation study of melt-processed polyethylene and its blend with polyamide using time-resolved rheometry

CSIR Research Space (South Africa)

Salehiyan, Reza

2017-05-01

Full Text Available Time-resolved mechanical spectroscopy (TRMS) was conducted to study the thermo-oxidative degradation of linear low density polyethylene (LLDPE) samples with different thermal histories and their blends with a polyamide (PA6) in the melt state. Neat...

Time-resolved study of formate on Ni( 1 1 1 ) by picosecond SFG spectroscopy

Science.gov (United States)

Kusafuka, K.; Noguchi, H.; Onda, K.; Kubota, J.; Domen, K.; Hirose, C.; Wada, A.

2002-04-01

Time-resolved vibrational measurements were carried out on formate (HCOO) adsorbed on Ni(1 1 1) surface by combining the sum-frequency generation method and picosecond laser system (time resolution of 6 ps). Rapid intensity decrease (within the time resolution) followed by intensity recovery (time constant of several tens of ps) of CH stretching signal was observed when picosecond 800 nm pulse was irradiated on the sample surface. From the results of temperature and pump fluence dependences of temporal behaviour of signal intensity, we concluded that the observed intensity change was induced by non-thermal process. Mechanism of the temporal intensity change was discussed.

Fully phase-encoded MRI near metallic implants using ultrashort echo times and broadband excitation.

Science.gov (United States)

Wiens, Curtis N; Artz, Nathan S; Jang, Hyungseok; McMillan, Alan B; Koch, Kevin M; Reeder, Scott B

2018-04-01

To develop a fully phase-encoded MRI method for distortion-free imaging near metallic implants, in clinically feasible acquisition times. An accelerated 3D fully phase-encoded acquisition with broadband excitation and ultrashort echo times is presented, which uses a broadband radiofrequency pulse to excite the entire off-resonance induced by the metallic implant. Furthermore, fully phase-encoded imaging is used to prevent distortions caused by frequency encoding, and to obtain ultrashort echo times for rapidly decaying signal. Phantom and in vivo acquisitions were used to describe the relationship among excitation bandwidth, signal loss near metallic implants, and T 1 weighting. Shorter radiofrequency pulses captured signal closer to the implant by improving spectral coverage and allowing shorter echo times, whereas longer pulses improved T 1 weighting through larger maximum attainable flip angles. Comparisons of fully phase-encoded acquisition with broadband excitation and ultrashort echo times to T 1 -weighted multi-acquisition with variable resonance image combination selective were performed in phantoms and subjects with metallic knee and hip prostheses. These acquisitions had similar contrast and acquisition efficiency. Accelerated fully phase-encoded acquisitions with ultrashort echo times and broadband excitation can generate distortion free images near metallic implants in clinically feasible acquisition times. Magn Reson Med 79:2156-2163, 2018. © 2017 International Society for Magnetic Resonance in Medicine. © 2017 International Society for Magnetic Resonance in Medicine.

Polymer chain dynamics in epoxy based composites as investigated by broadband dielectric spectroscopy

Directory of Open Access Journals (Sweden)

Mohammad K. Hassan

2016-03-01

Full Text Available Epoxy networks of the diglycidyl ether of bisphenol A (DGEBA were prepared using 3,3′- and 4,4′-diaminodiphenyl sulfone isomer crosslinkers. Secondary relaxations and the glass transitions of resultant networks were probed using broadband dielectric spectroscopy (BDS. A sub-Tg γ relaxation peak for both networks shifts to higher frequencies (f with increasing temperature in Arrhenius fashion, both processes having the same activation energy and being assigned to phenyl ring flipping in DGEBA chains. A β relaxation is assigned to local motions of dipoles that were created during crosslinking reactions. 4,4′-based networks exhibited higher Tg relative to 3,3′-based networks as per dynamic mechanical as well as BDS analyses. The Vogel–Fulcher–Tammann–Hesse equation fitted well to relaxation time vs. temperature data and comparison of Vogel temperatures suggests lower free volume per mass for the 3,3′-based network. The Kramers–Krönig transformation was used to directly calculate dc-free ɛ″ vs. f data from experimental ɛ′ vs. f data. Distribution of relaxation times (DRT curves are bi-modal for the 3,3′-crosslinked resin suggesting large-scale microstructural heterogeneity as opposed to homogeneity for the 4,4′-based network whose DRT consists of a single peak.

Time-resolved x-ray spectra from laser-generated high-density plasmas

Science.gov (United States)

Andiel, U.; Eidmann, Klaus; Witte, Klaus-Juergen

2001-04-01

We focused frequency doubled ultra short laser pulses on solid C, F, Na and Al targets, K-shell emission was systematically investigated by time resolved spectroscopy using a sub-ps streak camera. A large number of laser shots can be accumulated when triggering the camera with an Auston switch system at very high temporal precision. The system provides an outstanding time resolution of 1.7ps accumulating thousands of laser shots. The time duration of the He-(alpha) K-shell resonance lines was observed in the range of (2-4)ps and shows a decrease with the atomic number. The experimental results are well reproduced by hydro code simulations post processed with an atomic kinetics code.

Time-resolved soft x-ray absorption setup using multi-bunch operation modes at synchrotrons

International Nuclear Information System (INIS)

Stebel, L.; Sigalotti, P.; Ressel, B.; Cautero, G.; Malvestuto, M.; Capogrosso, V.; Bondino, F.; Magnano, E.; Parmigiani, F.

2011-01-01

Here, we report on a novel experimental apparatus for performing time-resolved soft x-ray absorption spectroscopy in the sub-ns time scale using non-hybrid multi-bunch mode synchrotron radiation. The present setup is based on a variable repetition rate Ti:sapphire laser (pump pulse) synchronized with the ∼500 MHz x-ray synchrotron radiation bunches and on a detection system that discriminates and singles out the significant x-ray photon pulses by means of a custom made photon counting unit. The whole setup has been validated by measuring the time evolution of the L 3 absorption edge during the melting and the solidification of a Ge single crystal irradiated by an intense ultrafast laser pulse. These results pave the way for performing synchrotron time-resolved experiments in the sub-ns time domain with variable repetition rate exploiting the full flux of the synchrotron radiation.

Toward practical terahertz time-domain spectroscopy

Science.gov (United States)

Brigada, David J.

Terahertz time-domain spectroscopy is a promising technology for the identification of explosive and pharmaceutical substances in adverse conditions. It interacts strongly with intermolecular vibrational and rotational modes. Terahertz also passes through many common dielectric covering materials, allowing for the identification of substances in envelopes, wrapped in opaque plastic, or otherwise hidden. However, there are several challenges preventing the adoption of terahertz spectroscopy outside the laboratory. This dissertation examines the problems preventing widespread adoption of terahertz technology and attempts to resolve them. In order to use terahertz spectroscopy to identify substances, a spectrum measured of the target sample must be compared to the spectra of various known standard samples. This dissertation examines various methods that can be employed throughout the entire process of acquiring and transforming terahertz waveforms to improve the accuracy of these comparisons. The concepts developed in this dissertation directly apply to terahertz spectroscopy, but also carry implications for other spectroscopy methods, from Raman to mass spectrometry. For example, these techniques could help to lower the rate of false positives at airport security checkpoints. This dissertation also examines the implementation of several of these methods as a way to realize a fully self-contained, handheld, battery-operated terahertz spectrometer. This device also employs techniques to allow minimally-trained operators use terahertz to detect different substances of interest. It functions as a proof-of-concept of the true benefits of the improvements that have been developed in this dissertation.

Study on the interaction of phthalate esters to human serum albumin by steady-state and time-resolved fluorescence and circular dichroism spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Xie, Xiaoyun [National Key Laboratory of Organic Chemistry, Lanzhou University, Lanzhou 730000 (China); College of Earth and Environmental Sciences, Lanzhou University, Lanzhou 730000 (China); Wang, Zhaowei [College of Earth and Environmental Sciences, Lanzhou University, Lanzhou 730000 (China); Zhou, Ximin; Wang, Xiaoru [National Key Laboratory of Organic Chemistry, Lanzhou University, Lanzhou 730000 (China); Chen, Xingguo, E-mail: chenxg@lzu.edu.cn [National Key Laboratory of Organic Chemistry, Lanzhou University, Lanzhou 730000 (China); Department of Chemistry, Lanzhou University, Lanzhou 730000 (China)

2011-09-15

Highlights: {center_dot} Molecular docking revealed PAEs to be located in the hydrophobic pocket of HSA. {center_dot} HSA-DMP had one class of binding sites while HSA-BBP and HSA-DEHP had two types. {center_dot} Hydrophobic and hydrogen interactions dominated in the association of HSA-PAEs. {center_dot} The lifetime of Trp residue of HSA decreased after the addition of PAEs. {center_dot} The presences of PAEs could alter the second structure of HSA. - Abstract: Phthalate esters (PAEs) are globally pervasive contaminants that are considered to be endocrine disruptor chemicals and toxic environmental priority pollutants. In this paper, the interactions between PAEs and human serum albumin (HSA) were examined by molecular modelling, steady state and time-resolved fluorescence, ultraviolet-visible spectroscopy (UV-vis) and circular dichroism spectroscopy (CD). The association constants between PAEs and HSA were determined using the Stern-Volmer and Scatchard equations. The binding of dimethyl phthalate (DMP) to HSA has a single class of binding site and its binding constants (K) are 4.08 x 10{sup 3}, 3.97 x 10{sup 3}, 3.45 x 10{sup 3}, and 3.20 x 10{sup 3} L mol{sup -1} at 289, 296, 303, and 310 K, respectively. The Stern-Volmer and Scatchard plots both had two regression curves for HSA-butylbenzyl phthalate (BBP) and HSA-di-2-ethylhexyl phthalate (DEHP), which indicated that these bindings were via two types of binding sites: the numbers of binding site for the first type were lower than for the second type. The binding constants of the first type binding site were higher than those of the second type binding site at corresponding temperatures, the results suggesting that the first type of binding site had high affinity and the second binding site involved other sites with lower binding affinity and selectivity. The thermodynamic parameters of the binding reactions ({Delta}G{sup o}, {Delta}H{sup o} and {Delta}S{sup o}) were measured, and they indicated the presences

Sequence-Dependent Mechanism of DNA Oligonucleotide Dehybridization Resolved through Infrared Spectroscopy.

Science.gov (United States)

Sanstead, Paul J; Stevenson, Paul; Tokmakoff, Andrei

2016-09-14

Despite its important role in biology and nanotechnology, many questions remain regarding the molecular mechanism and dynamics by which oligonucleotides recognize and hybridize to their complementary sequence. The thermodynamics and kinetics of DNA oligonucleotide hybridization and dehybridization are often assumed to involve an all-or-nothing two-state dissociation pathway, but deviations from this behavior can be considerable even for short sequences. We introduce a new strategy to characterize the base-pair-specific thermal dissociation mechanism of DNA oligonucleotides through steady-state and time-resolved infrared spectroscopy. Experiments are interpreted with a lattice model to provide a structure-specific interpretation. This method is applied to a model set of self-complementary 10-base-pair sequences in which the placement of GC base pairs is varied in an otherwise AT strand. Through a combination of Fourier transform infrared and two-dimensional infrared spectroscopy, experiments reveal varying degrees of deviation from simple two-state behavior. As the temperature is increased, duplexes dissociate through a path in which the terminal bases fray, without any significant contribution from loop configurations. Transient temperature jump experiments reveal time scales of 70-100 ns for fraying and 10-30 μs for complete dissociation near the melting temperature. Whether or not frayed states are metastable intermediates or short-lived configurations during the full dissociation of the duplex is dictated by the nucleobase sequence.

Efficient Implementation of a Symbol Timing Estimator for Broadband PLC.

Science.gov (United States)

Nombela, Francisco; García, Enrique; Mateos, Raúl; Hernández, Álvaro

2015-08-21

Broadband Power Line Communications (PLC) have taken advantage of the research advances in multi-carrier modulations to mitigate frequency selective fading, and their adoption opens up a myriad of applications in the field of sensory and automation systems, multimedia connectivity or smart spaces. Nonetheless, the use of these multi-carrier modulations, such as Wavelet-OFDM, requires a highly accurate symbol timing estimation for reliably recovering of transmitted data. Furthermore, the PLC channel presents some particularities that prevent the direct use of previous synchronization algorithms proposed in wireless communication systems. Therefore more research effort should be involved in the design and implementation of novel and robust synchronization algorithms for PLC, thus enabling real-time synchronization. This paper proposes a symbol timing estimator for broadband PLC based on cross-correlation with multilevel complementary sequences or Zadoff-Chu sequences and its efficient implementation in a FPGA; the obtained results show a 90% of success rate in symbol timing estimation for a certain PLC channel model and a reduced resource consumption for its implementation in a Xilinx Kyntex FPGA.

Efficient Implementation of a Symbol Timing Estimator for Broadband PLC

Directory of Open Access Journals (Sweden)

Francisco Nombela

2015-08-01

Full Text Available Broadband Power Line Communications (PLC have taken advantage of the research advances in multi-carrier modulations to mitigate frequency selective fading, and their adoption opens up a myriad of applications in the field of sensory and automation systems, multimedia connectivity or smart spaces. Nonetheless, the use of these multi-carrier modulations, such as Wavelet-OFDM, requires a highly accurate symbol timing estimation for reliably recovering of transmitted data. Furthermore, the PLC channel presents some particularities that prevent the direct use of previous synchronization algorithms proposed in wireless communication systems. Therefore more research effort should be involved in the design and implementation of novel and robust synchronization algorithms for PLC, thus enabling real-time synchronization. This paper proposes a symbol timing estimator for broadband PLC based on cross-correlation with multilevel complementary sequences or Zadoff-Chu sequences and its efficient implementation in a FPGA; the obtained results show a 90% of success rate in symbol timing estimation for a certain PLC channel model and a reduced resource consumption for its implementation in a Xilinx Kyntex FPGA.

Energy and angle resolved ion scattering spectroscopy: new possibilities for surface analysis

International Nuclear Information System (INIS)

Hellings, G.J.A.

1986-01-01

In this thesis the design and development of a novel, very sensitive and high-resolving spectrometer for surface analysis is described. This spectrometer is designed for Energy and Angle Resolved Ion Scattering Spectroscopy (EARISS). There are only a few techniques that are sensitive enough to study the outermost atomic layer of surfaces. One of these techniques, Low-Energy Ion Scattering (LEIS), is discussed in chapter 2. Since LEIS is destructive, it is important to make a very efficient use of the scattered ions. This makes it attractive to simultaneously carry out energy and angle dependent measurements (EARISS). (Auth.)

Effects of cations and cholesterol with sphingomyelin membranes investigated by high-resolution broadband sum frequency vibrational spectroscopy

Science.gov (United States)

Zhang, Zhen; Feng, Rong-juan; Li, Yi-yi; Liu, Ming-hua; Guo, Yuan

2017-08-01

Sphingomyelin(SM) is specifically enriched in the plasma membrane of mammalian cells. Its molecular structure is compose by N-acyl-Derythro-sphingosylphosphorylcholine. The function of the SM related to membrane signaling and protein trafficking are relied on the interactions of the SM, cations, cholesterol and proteins. In this report, the interaction of three different nature SMs, cations and cholesterol at air/aqueous interfaces studied by high-resolution broadband sum frequency vibrational spectroscopy, respectively. Our results shed lights on understanding the relationship between SMs monolayer, cholesterol and Cations.

Application of two-dimensional J-resolved nuclear magnetic resonance spectroscopy to differentiation of beer

International Nuclear Information System (INIS)

Khatib, Alfi; Wilson, Erica G.; Kim, Hye Kyong; Lefeber, Alfons W.M.; Erkelens, Cornelis; Choi, Young Hae; Verpoorte, Robert

2006-01-01

A number of ingredients in beer that directly or indirectly affect its quality require an unbiased wide-spectrum analytical method that allows for the determination of a wide array of compounds for its efficient control. 1 H nuclear magnetic resonance (NMR) spectroscopy is a method that clearly meets this description as the broad range of compounds in beer is detectable. However, the resulting congestion of signals added to the low resolution of 1 H NMR spectra makes the identification of individual components very difficult. Among two-dimensional (2D) NMR techniques that increase the resolution, J-resolved NMR spectra were successfully applied to the analysis of 2-butanol extracts of beer as overlapping signals in 1 H NMR spectra were fully resolved by the additional axis of the coupling constant. Principal component analysis based on the projected J-resolved NMR spectra showed a clear separation between all of the six brands of pilsner beer evaluated in this study. The compounds responsible for the differentiation were identified by 2D NMR spectra including correlated spectroscopy and heteronuclear multiple bond correlation spectra together with J-resolved spectra. They were identified as nucleic acid derivatives (adenine, uridine and xanthine), amino acids (tyrosine and proline), organic acid (succinic and lactic acid), alcohol (tyrosol and isopropanol), cholines and carbohydrates

Picosecond Time-Resolved Temperature and Density Measurements with K-Shell Spectroscopy

Science.gov (United States)

Stillman, C. R.; Nilson, P. M.; Ivancic, S. T.; Mileham, C.; Froula, D. H.; Golovkin, I. E.

2017-10-01

The thermal x-ray emission from rapidly heated solid targets containing a buried-aluminum layer was measured to track the evolution of the bulk plasma conditions. The targets were driven by high-contrast 1 ω laser pulses at focused intensities up to 1 × 1019 W/cm2. A streaked x-ray spectrometer recorded the AlHeα and lithium-like satellite lines with 2-ps temporal resolution and moderate resolving power (E E ΔE 1000 ΔE 1000) . Time-integrated measurements over the same spectral range were used to correct the streaked data for variations in photocathode sensitivity. Linewidths and intensity ratios from the streaked data were interpreted using a collisional radiative atomic kinetics model to provide the average plasma conditions in the buried layer as a function of time. Experimental uncertainties in the measured plasma conditions are quantified within a consistent model-dependent framework. The data demonstrate the production of a 330 +/-56 eV, 0.9 +/-0.3 g/cm3 plasma that evolves slowly during peak Heα emission. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

Broadband pump-probe spectroscopy with sub-10-fs resolution for probing ultrafast internal conversion and coherent phonons in carotenoids

International Nuclear Information System (INIS)

Polli, D.; Antognazza, M.R.; Brida, D.; Lanzani, G.; Cerullo, G.; De Silvestri, S.

2008-01-01

We use pump-probe spectroscopy with broadband detection to study electronic energy relaxation and coherent vibrational dynamics in carotenoids. A fast optical multichannel analyzer combined with a non-collinear optical parametric amplifier allows simultaneous acquisition of the differential transmission dynamics on the 500-700 nm wavelength range with sub-10-fs temporal resolution. The broad spectral coverage enables on the one hand a detailed study of the ultrafast bright-to-dark state internal conversion process; on the other hand, the tracking of the motion of the vibrational wavepacket launched on the ground state multidimensional potential energy surface. We present results on all-trans β-carotene and on a long-chain polyene in solution. The developed experimental setup enables the straightforward acquisition and analysis of coherent vibrational dynamics, highlighting time-frequency domain features with extreme resolution

Real-time monitoring of airborne beryllium, at OSHA limit levels, by time-resolved laser-induced breakdown spectroscopy

International Nuclear Information System (INIS)

Radziemski, L.J.; Loree, T.R.; Cremers, D.A.

1982-01-01

Real-time detection of beryllium particulate is being investigated by the new technique of laser-induced breakdown spectroscopy. For beryllium detection we monitor the 313.1-nm feature of once ionized beryllium (Be II). Numerous publications describe the technique, our beryllium results, and other applications. Here we summarize the important points and describe our experiments with beryllium

Time-resolved optical spectrometer based on a monolithic array of high-precision TDCs and SPADs

Science.gov (United States)

Tamborini, Davide; Markovic, Bojan; Di Sieno, Laura; Contini, Davide; Bassi, Andrea; Tisa, Simone; Tosi, Alberto; Zappa, Franco

2013-12-01

We present a compact time-resolved spectrometer suitable for optical spectroscopy from 400 nm to 1 μm wavelengths. The detector consists of a monolithic array of 16 high-precision Time-to-Digital Converters (TDC) and Single-Photon Avalanche Diodes (SPAD). The instrument has 10 ps resolution and reaches 70 ps (FWHM) timing precision over a 160 ns full-scale range with a Differential Non-Linearity (DNL) better than 1.5 % LSB. The core of the spectrometer is the application-specific integrated chip composed of 16 pixels with 250 μm pitch, containing a 20 μm diameter SPAD and an independent TDC each, fabricated in a 0.35 μm CMOS technology. In front of this array a monochromator is used to focus different wavelengths into different pixels. The spectrometer has been used for fluorescence lifetime spectroscopy: 5 nm spectral resolution over an 80 nm bandwidth is achieved. Lifetime spectroscopy of Nile blue is demonstrated.

Monitoring angiogenesis using a human compatible calibration for broadband near-infrared spectroscopy

Science.gov (United States)

Yang, Runze; Zhang, Qiong; Wu, Ying; Dunn, Jeff F.

2013-01-01

Angiogenesis is a hallmark of many conditions, including cancer, stroke, vascular disease, diabetes, and high-altitude exposure. We have previously shown that one can study angiogenesis in animal models by using total hemoglobin (tHb) as a marker of cerebral blood volume (CBV), measured using broadband near-infrared spectroscopy (bNIRS). However, the method was not suitable for patients as global anoxia was used for the calibration. Here we determine if angiogenesis could be detected using a calibration method that could be applied to patients. CBV, as a marker of angiogenesis, is quantified in a rat cortex before and after hypoxia acclimation. Rats are acclimated at 370-mmHg pressure for three weeks, while rats in the control group are housed under the same conditions, but under normal pressure. CBV increased in each animal in the acclimation group. The mean CBV (%volume/volume) is 3.49%±0.43% (mean±SD) before acclimation for the experimental group, and 4.76%±0.29% after acclimation. The CBV for the control group is 3.28%±0.75%, and 3.09%±0.48% for the two measurements. This demonstrates that angiogenesis can be monitored noninvasively over time using a bNIRS system with a calibration method that is compatible with human use and less stressful for studies using animals.

Extended wavelength anisotropy resolved multidimensional emission spectroscopy (ARMES) measurements: better filters, validation standards, and Rayleigh scatter removal methods

Science.gov (United States)

Casamayou-Boucau, Yannick; Ryder, Alan G.

2017-09-01

Anisotropy resolved multidimensional emission spectroscopy (ARMES) provides valuable insights into multi-fluorophore proteins (Groza et al 2015 Anal. Chim. Acta 886 133-42). Fluorescence anisotropy adds to the multidimensional fluorescence dataset information about the physical size of the fluorophores and/or the rigidity of the surrounding micro-environment. The first ARMES studies used standard thin film polarizers (TFP) that had negligible transmission between 250 and 290 nm, preventing accurate measurement of intrinsic protein fluorescence from tyrosine and tryptophan. Replacing TFP with pairs of broadband wire grid polarizers enabled standard fluorescence spectrometers to accurately measure anisotropies between 250 and 300 nm, which was validated with solutions of perylene in the UV and Erythrosin B and Phloxine B in the visible. In all cases, anisotropies were accurate to better than ±1% when compared to literature measurements made with Glan Thompson or TFP polarizers. Better dual wire grid polarizer UV transmittance and the use of excitation-emission matrix measurements for ARMES required complete Rayleigh scatter elimination. This was achieved by chemometric modelling rather than classical interpolation, which enabled the acquisition of pure anisotropy patterns over wider spectral ranges. In combination, these three improvements permit the accurate implementation of ARMES for studying intrinsic protein fluorescence.

Coherent cavity-enhanced dual-comb spectroscopy

OpenAIRE

Fleisher, Adam J.; Long, David A.; Reed, Zachary D.; Hodges, Joseph T.; Plusquellic, David F.

2016-01-01

Dual-comb spectroscopy allows for the rapid, multiplexed acquisition of high-resolution spectra without the need for moving parts or low-resolution dispersive optics. This method of broadband spectroscopy is most often accomplished via tight phase locking of two mode-locked lasers or via sophisticated signal processing algorithms, and therefore, long integration times of phase coherent signals are difficult to achieve. Here we demonstrate an alternative approach to dual-comb spectroscopy usin...

Angle-resolved photoelectron spectroscopy of formaldehyde and methanol

Science.gov (United States)

Keller, P. R.; Taylor, J. W.; Grimm, F. A.; Carlson, Thomas A.

1984-10-01

Angle-resolved photoelectron spectroscopy was employed to obtain the angular distribution parameter, β, for the valence orbitals (IP < 21.1 eV) of formaldehyde and methanol over the 10-30 eV photon energy range using dispersed polarized synchrotron radiation as the excitation source. It was found that the energy dependence of β in the photoelectron energy range between 2 and 10 eV can be related to the molecular-orbital type from which ionization occurs. This generalized energy behavior is discussed with regard to earlier energy-dependence studies on molecules of different orbital character. Evidence is presented for the presence of resonance photoionization phenomena in formaldehyde in agreement with theoretical cross-section calculations.

Angle-resolved photoemission spectroscopy on iron-chalcogenide superconductors

Energy Technology Data Exchange (ETDEWEB)

Maletz, Janek; Zabolotnyy, Volodymyr; Evtushinsky, Daniil; Thirupathaiah, Setti; Wolter-Giraud, Anja; Harnagea, Luminita; Kordyuk, Alexander; Borisenko, Sergey [IFW Dresden (Germany); Yaresko, Alexander [MPI-FKF, Stuttgart (Germany); Vasiliev, Alexander [Moscow State University (Russian Federation); Chareev, Dimitri [RAS, Chernogolovka (Russian Federation); Rienks, Emile [Helmholtz-Zentrum Berlin (Germany); Buechner, Bernd [IFW Dresden (Germany); TU Dresden (Germany); Shermadini, Zurab; Luetkens, Hubertus; Sedlak, Kamil; Khasanov, Rustem; Amato, Alex; Krzton-Maziopa, Anna; Conder, Kazimierz; Pomjakushina, Ekaterina [Paul Scherrer Institute (Switzerland); Klauss, Hans-Henning [TU Dresden (Germany)

2014-07-01

The electronic structure of the iron chalcogenide superconductors FeSe{sub 1-x} and Rb{sub 0.77}Fe{sub 1.61}Se{sub 2} was investigated by high-resolution angle-resolved photoemission spectroscopy (ARPES). The results were compared to DFT calculations and μSR measurements. Both compounds share ''cigar-shaped'' Fermi surface sheets in their electronic structure, that can be found in almost all iron-pnictide superconductors. These features originate from a strong interplay of two hole- and electron-like bands in the Brillouin zone center, leading to a pronounced singularity in the density of states just below the Fermi level. This facilitates the coupling to a bosonic mode responsible for superconductivity.

Amplifier with time-invariant trapezoidal shaping and shape-sensitive pileup rejector for high-rate spectroscopy

International Nuclear Information System (INIS)

Drndarevic, V.; Ryge, P.; Gozani, T.

1989-01-01

An amplifier with trapezoidal pulse shaping was developed for high-rate high-energy gamma spectroscopy using NaI(T1) scintillation detectors. It employs a double delay-line technique for producing a nearly triangular pulse shape combined with a linear circuit for producing a flattopped pulse. Good energy resolution and short resolving time make this amplifier especially suitable for high count rate gamma ray spectroscopy. To provide a versatile high-performance system, it includes a pileup rejector based on inspection of a pileup signal obtained by combining the slow output signal and fast-shaped input signal. The trapezoidal shape provides a short resolving time for minimal occurrence of pileup with a width suitable for presentation to a standard multichannel analyzer. The performance of the system was tested, and the results are presented

Active control of time-varying broadband noise and vibrations using a sliding-window Kalman filter

NARCIS (Netherlands)

van Ophem, S.; Berkhoff, Arthur P.; Sas, P.; Moens, D.; Denayer, H.

2014-01-01

Recently, a multiple-input/multiple-output Kalman filter technique was presented to control time-varying broadband noise and vibrations. By describing the feed-forward broadband active noise control problem in terms of a state estimation problem it was possible to achieve a faster rate of

Time-resolved cathodoluminescence microscopy with sub-nanosecond beam blanking for direct evaluation of the local density of states

NARCIS (Netherlands)

Moerland, R.J.; Weppelman, I.G.C.; Garming, M.W.H.; Kruit, P.; Hoogenboom, J.P.

2016-01-01

We show cathodoluminescence-based time-resolved electron beam spectroscopy in order to directly probe the spontaneous emission decay rate that is modified by the local density of states in a nanoscale environment. In contrast to dedicated laser-triggered electron-microscopy setups, we use commercial

Continuous wave and time resolved spectroscopy of InAsN/GaAsN based quantum dots

International Nuclear Information System (INIS)

Taliercio, T.; Valvin, P.; Intartaglia, R.; Guillet, T.; Lefebvre, P.; Bretagnon, T.; Gil, B.; Sallet, V.; Harmand, J.C.

2005-01-01

We present a study of the optical properties of quantum dots based on a new family of semiconductors: III-V dilute nitrides such as (In,Ga)(N,As). Continuous wave and time resolved photoluminescence (PL) experiments allowed us to evaluate the impact of N incorporation during the growth of InAs/GaAs quantum dots. Previous work [V. Sallet et al., to be submitted to J. Cryst. Growth (2005); O. Schumann et al., J. Appl. Phys. 96, 2832 (2004)] showed that increasing the flux of N atoms into the growth chamber modifies drastically the size of the dots which leads to a bimodal growth. Two populations of dots with different sizes appear. The quantum dot PL line broadens and a second PL line appears at higher energy. Time resolved PL allows us to identify the nature of this second PL line: second population of quantum dots. A second decay time is observed which we interpret as being the consequence of the perturbation of the electronic states of the quantum dots. (copyright 2005 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

Solid-phase nano-extraction and laser-excited time-resolved Shpol'skii spectroscopy for the analysis of polycyclic aromatic hydrocarbons in drinking water samples.

Science.gov (United States)

Wang, Huiyong; Yu, Shenjiang; Campiglia, Andres D

2009-02-15

A unique method for screening polycyclic aromatic hydrocarbons in drinking water samples is reported. Water samples (500 microl) are mixed and centrifuged with 950 microl of a commercial solution of 20 nm gold nanoparticles for pollutants extraction. The precipitate is treated with 2 microl of 1-pentanethiol and 48 microl of n-octane, and the supernatant is then analyzed via laser-excited time-resolved Shpol'skii spectroscopy. Fifteen priority pollutants are directly determined at liquid helium temperature (4.2 K) with the aid of a cryogenic fiber-optic probe. Unambiguous pollutant determination is carried out via spectral and lifetime analysis. Limits of detection are at the parts-per-trillion level. Analytical recoveries are similar to those obtained via high-performance liquid chromatography. The simplicity of the experimental procedure, use of microliters of organic solvent, short analysis time, selectivity, and excellent analytical figures of merit demonstrate the advantages of this environmentally friendly approach for routine analysis of numerous samples.

Spatially resolved sulfur K-edge XANES spectroscopy of wheat leaves infected by Puccinia triticina

International Nuclear Information System (INIS)

Lichtenberg, H; Prange, A; Hormes, J; Steiner, U; Oerke, E-C

2009-01-01

In this study, wheat leaves infected with brown rust, a plant disease of serious economic concern caused by the fungus Puccinia triticina, were investigated using spatially resolved XANES (X-ray Absorption Near Edge Structure) spectroscopy at the sulfur K-absorption edge.

Spatially resolved sulfur K-edge XANES spectroscopy of wheat leaves infected by Puccinia triticina

Energy Technology Data Exchange (ETDEWEB)

Lichtenberg, H; Prange, A; Hormes, J [CAMD, Louisiana State University, 6980 Jefferson Hwy, Baton Rouge, LA 70806 (United States); Steiner, U; Oerke, E-C, E-mail: lichtenberg@lsu.ed [INRES-Phytomedicine, University of Bonn, Nussallee 9, 53115 Bonn (Germany)

2009-11-15

In this study, wheat leaves infected with brown rust, a plant disease of serious economic concern caused by the fungus Puccinia triticina, were investigated using spatially resolved XANES (X-ray Absorption Near Edge Structure) spectroscopy at the sulfur K-absorption edge.

Ultrafast pump-probe reflectance spectroscopy: Why sodium makes Cu(In,Ga)Se2 solar cells better

KAUST Repository

Eid, Jessica; Usman, Anwar; Gereige, Issam; Duren, Jeroen Van; Lyssenko, Vadim; Leo, Karl; Mohammed, Omar F.

2015-01-01

Although Cu(In,Ga)Se2 (CIGS) solar cells have the highest efficiency of any thin-film solar cell, especially when sodium is incorporated, the fundamental device properties of ultrafast carrier transport and recombination in such cells remain not fully understood. Here, we explore the dynamics of charge carriers in CIGS absorber layers with varying concentrations of Na by femtosecond (fs) broadband pump-probe reflectance spectroscopy with 120 fs time resolution. By analyzing the time-resolved transient spectra in a different time domain, we show that a small amount of Na integrated by NaF deposition on top of sputtered Cu(In,Ga) prior to selenization forms CIGS, which induces slower recombination of the excited carriers. Here, we provide direct evidence for the elongation of carrier lifetimes by incorporating Na into CIGS.

Ultrafast pump-probe reflectance spectroscopy: Why sodium makes Cu(In,Ga)Se2 solar cells better

KAUST Repository

Eid, Jessica

2015-04-14

Although Cu(In,Ga)Se2 (CIGS) solar cells have the highest efficiency of any thin-film solar cell, especially when sodium is incorporated, the fundamental device properties of ultrafast carrier transport and recombination in such cells remain not fully understood. Here, we explore the dynamics of charge carriers in CIGS absorber layers with varying concentrations of Na by femtosecond (fs) broadband pump-probe reflectance spectroscopy with 120 fs time resolution. By analyzing the time-resolved transient spectra in a different time domain, we show that a small amount of Na integrated by NaF deposition on top of sputtered Cu(In,Ga) prior to selenization forms CIGS, which induces slower recombination of the excited carriers. Here, we provide direct evidence for the elongation of carrier lifetimes by incorporating Na into CIGS.

Space-resolved vacuum ultra-violet spectroscopy on T.F.R. Tokamak plasmas

International Nuclear Information System (INIS)

1978-01-01

Results are reported of space-resolved vacuum-ultraviolet spectroscopy (between 100 A and 2000A) on T.F.R. Tokamak plasmas and examples are given of profiles for both heavy and light impurity ions. The experimental method and the associated uncertainties and problems are stressed. The great importance of numerical calculations in the interpretation of the impurity profiles is pointed out. (author)

Photodissociation of CH3CHO at 248 nm by time-resolved Fourier-transform infrared emission spectroscopy: Verification of roaming and triple fragmentation

Science.gov (United States)

Hung, Kai-Chan; Tsai, Po-Yu; Li, Hou-Kuan; Lin, King-Chuen

2014-02-01

By using time-resolved Fourier-transform infrared emission spectroscopy, the HCO fragment dissociated from acetaldehyde (CH3CHO) at 248 nm is found to partially decompose to H and CO. The fragment yields are enhanced by the Ar addition that facilitates the collision-induced internal conversion. The channels to CH2CO + H2 and CH3CO + H are not detected significantly. The rotational population distribution of CO, after removing the Ar collision effect, shows a bimodal feature comprising both low- and high-rotational (J) components, sharing a fraction of 19% and 81%, respectively, for the vibrational state v = 1. The low-J component is ascribed to both roaming pathway and triple fragmentation. They are determined to have a branching ratio of 0.06, respectively, relative to the whole v = 1 population. The CO roaming is accompanied by a highly vibrational population of CH4 that yields a vibrational bimodality.

Time-resolved quantitative phosphoproteomics

DEFF Research Database (Denmark)

Verano-Braga, Thiago; Schwämmle, Veit; Sylvester, Marc

2012-01-01

proteins involved in the Ang-(1-7) signaling, we performed a mass spectrometry-based time-resolved quantitative phosphoproteome study of human aortic endothelial cells (HAEC) treated with Ang-(1-7). We identified 1288 unique phosphosites on 699 different proteins with 99% certainty of correct peptide...

Numerical simulations of time-resolved quantum electronics

International Nuclear Information System (INIS)

Gaury, Benoit; Weston, Joseph; Santin, Matthieu; Houzet, Manuel; Groth, Christoph; Waintal, Xavier

2014-01-01

Numerical simulation has become a major tool in quantum electronics both for fundamental and applied purposes. While for a long time those simulations focused on stationary properties (e.g. DC currents), the recent experimental trend toward GHz frequencies and beyond has triggered a new interest for handling time-dependent perturbations. As the experimental frequencies get higher, it becomes possible to conceive experiments which are both time-resolved and fast enough to probe the internal quantum dynamics of the system. This paper discusses the technical aspects–mathematical and numerical–associated with the numerical simulations of such a setup in the time domain (i.e. beyond the single-frequency AC limit). After a short review of the state of the art, we develop a theoretical framework for the calculation of time-resolved observables in a general multiterminal system subject to an arbitrary time-dependent perturbation (oscillating electrostatic gates, voltage pulses, time-varying magnetic fields, etc.) The approach is mathematically equivalent to (i) the time-dependent scattering formalism, (ii) the time-resolved non-equilibrium Green’s function (NEGF) formalism and (iii) the partition-free approach. The central object of our theory is a wave function that obeys a simple Schrödinger equation with an additional source term that accounts for the electrons injected from the electrodes. The time-resolved observables (current, density, etc.) and the (inelastic) scattering matrix are simply expressed in terms of this wave function. We use our approach to develop a numerical technique for simulating time-resolved quantum transport. We find that the use of this wave function is advantageous for numerical simulations resulting in a speed up of many orders of magnitude with respect to the direct integration of NEGF equations. Our technique allows one to simulate realistic situations beyond simple models, a subject that was until now beyond the simulation

Developments in time-resolved x-ray research at APS beamline 7ID

Energy Technology Data Exchange (ETDEWEB)

Walko, D. A., E-mail: d-walko@anl.gov; Adams, B. W.; Doumy, G.; Dufresne, E. M.; Li, Yuelin; March, A. M.; Sandy, A. R.; Wang, Jin; Wen, Haidan; Zhu, Yi [Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439 (United States)

2016-07-27

The 7ID beamline of the Advanced Photon Source (APS) is dedicated to time-resolved research using x-ray imaging, scattering, and spectroscopy techniques. Time resolution is achieved via gated detectors and/or mechanical choppers in conjunction with the time structure of the x-ray beam. Three experimental hutches allow for a wide variety of experimental setups. Major areas of research include atomic, molecular, and optical physics; chemistry; condensed matter physics in the bulk, thin film, and surface regimes; and fluid-spray dynamics. Recent developments in facilities at 7ID include a high-power, high-repetition-rate picosecond laser to complement the 1 kHz ultrafast laser. For the ultrafast laser, a newly commissioned optical parametric amplifier provides pump wavelength from 0.2 to 15 µm with energy per pulse up to 200 µJ. A nanodiffraction station has also been commissioned, using Fresnel zone-plate optics to achieve a focused x-ray spot of 300 nm. This nanoprobe is not only used to spatially resolve the evolution of small features in samples after optical excitation, but also has been combined with an intense THz source to study material response under ultrafast electric fields.

Applications of a table-top time-resolved luminescence spectrometer with nanosecond soft X-ray pulse excitation

Czech Academy of Sciences Publication Activity Database

Brůža, P.; Pánek, D.; Fidler, V.; Benedikt, P.; Čuba, V.; Gbur, T.; Boháček, Pavel; Nikl, Martin

2014-01-01

Roč. 61, č. 1 (2014), s. 448-451 ISSN 0018-9499 R&D Projects: GA ČR GA13-09876S Institutional support: RVO:68378271 Keywords : LiCaAlF 6 * luminescence * scintillators * soft x-ray * SrHfO 3 * time-resolved spectroscopy * ZnO :Ga Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.283, year: 2014

Novel lanthanide doped micro- and mesoporous solids. Characterization of ion-host-interactions, species distribution and luminescence properties using time-resolved luminescence spectroscopy

International Nuclear Information System (INIS)

Gessner, Andre

2010-12-01

In this work lanthanide-doped microporous zeolites, microporous-mesoporous hybrid materials and mesoporous silicates were investigated regarding their luminescence properties and the ion-host-interactions using time-resolved luminescence spectroscopy. Thereby, time-resolved emission spectra (TRES) provide information in the wavelength and time domain. For the analysis of the TRES a broad set of analytic methods was applied and thus a corresponding ''toolbox'' developed. Fitting of the luminescence decays was performed with a discrete number of exponentials and supported by luminescence decay times distributions. Time-resolved area normalized emission spectra (TRANES), an advancement of TRES, could be used for the determination of the number of emissive lanthanide species in porous materials for the first time. Calculation of the decay-associated spectra (DAS) allowed the correlation of spectral information with luminescence decay times and thus delivered the luminescence spectra of the different europium species. For europium(III) we could use in addition the time-dependent asymmetry ratio and spectral evolution of the 5 D 0 - 7 F 0 -transition with time to obtain further information about the distribution of the lanthanide ions in the host material. Luminescence decay times and spectra allowed conclusions on the number of OH-oscillators in and the symmetry of the first coordination sphere. For the microporous and microporous-mesoporous materials were found different lanthanide species, which were characterized by the above mentioned methods. These lanthanide species can be found on different positions in the host material. One position is located deep in the pore system. Here, lanthanide ions are hardly accessible for water and mainly coordinated by framework oxygens. This results in long luminescence decay times and distorted coordination spheres. The second position can be found near or on the outer surface or in the mesopores. Lanthanide ions located here, are

A versatile setup for ultrafast broadband optical spectroscopy of coherent collective modes in strongly correlated quantum systems

Directory of Open Access Journals (Sweden)

Edoardo Baldini

2016-11-01

Full Text Available A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide temperature range. By combining high temporal resolution and a broad detection window, this apparatus can investigate the interplay between coherent collective modes and high-energy electronic excitations, which is a distinctive characteristic of correlated electron systems. Using a single-shot readout array detector at frame rates of 10 kHz allows resolving coherent oscillations with amplitudes <10−4. We demonstrate its operation on the charge-transfer insulator La2CuO4, revealing coherent phonons with frequencies up to 13 THz and providing access into their Raman matrix elements.

Broadband Dielectric Spectroscopy and Quasi-Elastic Neutron Scattering on Single-Ion Polymer Conductors

Science.gov (United States)

Soles, Christopher; Peng, Hua-Gen; Page, Kirt; Snyder, Chad; Pandy, Ashoutosh; Jeong, Youmi; Runt, James; NIST Collaboration; Pennsylvania Collaboration

2011-03-01

The application of solid polymer electrolytes in rechargeable batteries has not been fully realized after decades of research due to its low conductivity. Dramatic increases of the ion conductivity are needed and this progress requires the understanding of conduction mechanism. We address this topic in two fronts, namely, the effect of plasticizer additives and geometric confinement on the charge transfer mechanism. To this end, we combine broadband dielectric spectroscopy (BDS) to characterize the ion mobility and quasi-elastic neutron scattering (QENS) to quantify segmental motion on a single-ion model polymer electrolyte. Deuterated small molecules were used as plasticizers so that the segmental motion of the polymer electrolyte could be monitored by QENS to understand the mechanism behind the increased conductivity. Anodic aluminum oxide (AAO) membranes with well defined channel sizes are used as the matrix to study the transport of ions solvated in a 1D polymer electrolyte.

Real-time reflectance-difference spectroscopy of GaAs molecular beam epitaxy homoepitaxial growth

Energy Technology Data Exchange (ETDEWEB)

Lastras-Martínez, A., E-mail: alm@cactus.iico.uaslp.mx, E-mail: alastras@gmail.com; Ortega-Gallegos, J.; Guevara-Macías, L. E.; Nuñez-Olvera, O.; Balderas-Navarro, R. E.; Lastras-Martínez, L. F. [Instituto de Investigación en Comunicación Optica, Universidad Autónoma de San Luis Potosí, Alvaro Obregón 64, San Luis Potosí, SLP 78000 (Mexico); Lastras-Montaño, L. A. [IBM T. J. Watson Research Center, Yorktown Heights, New York 10598 (United States); Lastras-Montaño, M. A. [Department of Electrical and Computer Engineering, University of California, Santa Barbara, Santa Barbara, California 93106 (United States)

2014-03-01

We report on real time-resolved Reflectance-difference (RD) spectroscopy of GaAs(001) grown by molecular beam epitaxy, with a time-resolution of 500 ms per spectrum within the 2.3–4.0 eV photon energy range. Through the analysis of transient RD spectra we demonstrated that RD line shapes are comprised of two components with different physical origins and determined their evolution during growth. Such components were ascribed to the subsurface strain induced by surface reconstruction and to surface stoichiometry. Results reported in this paper render RD spectroscopy as a powerful tool for the study of fundamental processes during the epitaxial growth of zincblende semiconductors.

Real-time visualization of the vibrational wavepacket dynamics in electronically excited pyrimidine via femtosecond time-resolved photoelectron imaging

Science.gov (United States)

Li, Shuai; Long, Jinyou; Ling, Fengzi; Wang, Yanmei; Song, Xinli; Zhang, Song; Zhang, Bing

2017-07-01

The vibrational wavepacket dynamics at the very early stages of the S1-T1 intersystem crossing in photoexcited pyrimidine is visualized in real time by femtosecond time-resolved photoelectron imaging and time-resolved mass spectroscopy. A coherent superposition of the vibrational states is prepared by the femtosecond pump pulse at 315.3 nm, resulting in a vibrational wavepacket. The composition of the prepared wavepacket is directly identified by a sustained quantum beat superimposed on the parent-ion transient, possessing a frequency in accord with the energy separation between the 6a1 and 6b2 states. The dephasing time of the vibrational wavepacket is determined to be 82 ps. More importantly, the variable Franck-Condon factors between the wavepacket components and the dispersed cation vibrational levels are experimentally illustrated to identify the dark state and follow the energy-flow dynamics on the femtosecond time scale. The time-dependent intensities of the photoelectron peaks originated from the 6a1 vibrational state exhibit a clear quantum beating pattern with similar periodicity but a phase shift of π rad with respect to those from the 6b2 state, offering an unambiguous picture of the restricted intramolecular vibrational energy redistribution dynamics in the 6a1/6b2 Fermi resonance.

Time-resolved studies. Ch. 9

International Nuclear Information System (INIS)

Mills, Dennis M.; Argonne National Lab., IL

1991-01-01

Synchrotron radiation, with its unique properties, offers a tool to extend X-ray measurements from the static to the time-resolved regime. The most straight-forward application of synchrotron radiation to the study of transient phenomena is directly through the possibility of decreased data-collection times via the enormous increase in flux over that of a laboratory X-ray system. Even further increases in intensity can be obtained through the use of novel X-ray optical devices. Wide-bandpass monochromators, e.g., that utilize the continuous spectral distribution of synchrotron radiation, can increase flux on the sample several orders of magnitude over conventional X-ray optical systems thereby allowing a further shortening of the data-collection time. Another approach that uses the continuous spectral nature of synchrotron radiation to decrease data-collection times is the 'parallel data collection' method. Using this technique, intensities as a function of X-ray energy are recorded simultaneously for all energies rather than sequentially recording data at each energy, allowing for a dramatic decrease in data-collection time. Perhaps the most exciting advances in time-resolved X-ray studies will be made by those methods that exploit the pulsed nature of the radiation emitted from storage rings. Pulsed techniques have had an enormous impact in the study of the temporal evolution of transient phenomena. The extension from continuous to modulated sources for use in time-resolved work has been carried over in a host of fields that use both pulsed particle and pulsed electro-magnetic beams. In this chapter the new experimental techniques are reviewed and illustrated with some experiments. (author). 98 refs.; 20 figs.; 5 tabs

Broadband demonstrations of true-time delay using linear sideband chirped programming and optical coherent transients

International Nuclear Information System (INIS)

Reibel, R.R.; Barber, Z.W.; Fischer, J.A.; Tian, M.; Babbitt, W.R.

2004-01-01

Linear sideband chirped (LSC) programming is introduced as a means of configuring spatial-spectral holographic gratings for optical coherent transient processors. Similar to linear frequency chirped programming, LSC programming allows the use of broadband integrated electro-optic phase modulators to produce chirps instead of using elaborate broadband chirped lasers. This approach has several advantages including the ability to use a stabilized laser for the optical carrier as well as stable, reproducible chirped optical signals when the modulator is driven digitally. Using LSC programming, we experimentally demonstrate broadband true-time delay as a proof of principle for the optical control of phased array radars. Here both cw phase modulated and binary phase shift keyed probe signals are true-time delayed with bandwidths of 1 GHz and delay resolutions better than 60 ps

Time resolved IR-LIGS experiments for gas-phase trace detection and temperature measurements

Energy Technology Data Exchange (ETDEWEB)

Fantoni, R.; Giorgi, M. [ENEA, Centro Ricerche Frascati, Rome (Italy). Dip. Innovazione; Snels, M. [CNR, Tito Scalo, Potenza (Italy). Istituto per i Materiali Speciali; Latzel, H.

1997-01-01

Time resolved Laser Induced Grating Spectroscopy (LIGS) has been performed to detect different gases in mixtures at atmospheric pressure or higher. The possibility of trace detection of minor species and of temperature measurements has been demonstrated for various molecular species either of environmental interest or involved in combustion processes. In view of the application of tracing unburned hydrocarbons in combustion chambers, the coupling of the IR-LIGS technique with imaging detection has been considered and preliminary results obtained in small size ethylene/air flames are shown.

Deflection evaluation using time-resolved radiography

International Nuclear Information System (INIS)

Fry, D.A.; Lucero, J.P.

1990-01-01

Time-resolved radiography is the creation of an x-ray image for which both the start-exposure and stop-exposure times are known with respect to the event under study. The combination of image and timing are used to derive information about the event. The authors have applied time-resolved radiography to evaluate motions of explosive-driven events. In the particular application discussed in this paper, the author's intent is to measure maximum deflections of the components involved. Exposures are made during the time just before to just after the event of interest occurs. A smear or blur of motion out to its furthest extent is recorded on the image. Comparison of the dynamic images with static images allows deflection measurements to be made

[A new measurement method of time-resolved spectrum].

Science.gov (United States)

Shi, Zhi-gang; Huang, Shi-hua; Liang, Chun-jun; Lei, Quan-sheng

2007-02-01

A new method for measuring time-resolved spectrum (TRS) is brought forward. Programming with assemble language controlled the micro-control-processor (AT89C51), and a kind of peripheral circuit constituted the drive circuit, which drived the stepping motor to run the monochromator. So the light of different kinds of expected wavelength could be obtained. The optical signal was transformed to electrical signal by optical-to-electrical transform with the help of photomultiplier tube (Hamamatsu 1P28). The electrical signal of spectrum data was transmitted to the oscillograph. Connecting the two serial interfaces of RS232 between the oscillograph and computer, the electrical signal of spectrum data could be transmitted to computer for programming to draw the attenuation curve and time-resolved spectrum (TRS) of the swatch. The method for measuring time-resolved spectrum (TRS) features parallel measurement in time scale but serial measurement in wavelength scale. Time-resolved spectrum (TRS) and integrated emission spectrum of Tb3+ in swatch Tb(o-BBA)3 phen were measured using this method. Compared with the real time-resolved spectrum (TRS). It was validated to be feasible, credible and convenient. The 3D spectra of fluorescence intensity-wavelength-time, and the integrated spectrum of the swatch Tb(o-BBA)3 phen are given.

Broadband spectral observation of a dMe star radio flare

International Nuclear Information System (INIS)

Guedel, M.; Benz, A.O.; Fuerst, E.; Simett, G.M.; Davis, R.J.

1989-01-01

A flare on the dMe star AD Leonis was simultaneously observed with the radio telescopes in Effelsberg, Jodrell Bank, and Arecibo using spectrometers at 1665, 166 and 1415 MHz with bandwidths of 25, 100 and 40 MHz respectively. The time coincidence confirms the stellar origin of the radiation. The flare emission was resolved into a multitude of broadband pulsations. The e-folding rise and decay times were of the order of the time resolution of the Effelsberg data (125 ms), or less. The circular polarization was ∼ 100%. Similar bursts, but 4 orders of magnitude less powerful, have been observed from the sun at lower frequencies

New approaches for a time- and position-resolved detector for positron annihilation spectroscopy at PLEPS

Energy Technology Data Exchange (ETDEWEB)

Ackermann, Ulrich; Egger, Werner; Sperr, Peter; Loewe, Benjamin; Ravelli, Luca; Koegel, Gottfried; Dollinger, Guenther [Universitaet der Bundeswehr Muenchen, LRT2 (Germany); Jagutzki, Ottmar [Universitaet Frankfurt, RoentDek GmbH (Germany)

2013-07-01

The pulsed low energy positron system PLEPS at NEPOMUC at the FRM II is a tool for depth resolved positron lifetime measurements. Besides positron lifetime measurements 2D-AMOC (two dimensional age momentum correlation) experiments are also possible. 2D-AMOC provides in coincidence the lifetime of the positron and the longitudinal momentum distribution of the annihilating electron. It would be of great scientific concern to measure simultaneously the entire 3D-momentum distribution of the annihilating electron and the corresponding lifetime of the positron (4D-AMOC). To perform 4D-AMOC measurements, a time and spatially resolving detector with a time resolution of about 100 ps (FWHM) and a spatial resolution of circa 2 mm over an area of about 12 cm{sup 2} is required in coincidence with a pixelated Ge-detector and currently under development at our institute. It is intended to use a MCP-based UV-light detector with two MCP-stages coupled to a BaF{sub 2} scintillator. To achieve the spatial resolution the centroid information of the photoelectron-cloud is detected with a position sensitive anode installed outside the housing of the MCP detector. As an alternative to a MCP-based detector, silicon photomultipliers are also envisaged.

Time-resolved studies at PETRA III with a highly repetitive synchronized laser system

Energy Technology Data Exchange (ETDEWEB)

Schlie, Mortiz

2013-09-15

Atomic and molecular processes can nowadays be directly followed in the time domain. This is a core technique for a better understanding of the involved fundamental physics, thus auguring new applications in the future as well. Usually the so-called pump-probe technique making use of two synchronized ultrashort light pulses is utilized to obtain this time-resolved data. In this work, the development and characterization of a synchronization system enabling such pump-probe studies at the storage ring PETRA III in combination with an external, then synchronized fs-laser system is described. The synchronization is based on an extended PLL approach with three interconnected feedback loops allowing to monitor short-time losses of the lock and thus prevent them. This way, the jitter between the laser PHAROS and the PETRA III reference signal is reduced to {sigma} <5 ps. Thus the system allows to conduct experiments at a repetition rate of 130 kHz with a temporal resolution limited only by the X-ray pulse length. A major emphasis in the fundamental introductory chapters is an intuitive explanation of the basic principles of phase locked loops and the different aspects of phase noise to allow a deeper understanding of the synchronization. Furthermore, first pump-probe experiments conducted at different beamlines at PETRA III are presented, demonstrating the usability of the laser system in a scientific environment as well. In first characterizing experiments the pulse duration of PETRA III X-ray pulses has been measured to be 90 ps FWHM. In particular, there have been time resolved X-ray absorption spectroscopy experiments on Gaq3 and Znq2 conducted at beamline P11. First results show dynamics of the electronic excitation on the timescale of a few hundred pico seconds up to a few nano seconds and provide a basic understanding for further research on those molecules. For Gaq3 this data is analyzed in detail and compared with visible fluorescence measurements suggesting at

Time-resolved studies at PETRA III with a highly repetitive synchronized laser system

International Nuclear Information System (INIS)

Schlie, Mortiz

2013-09-01

Atomic and molecular processes can nowadays be directly followed in the time domain. This is a core technique for a better understanding of the involved fundamental physics, thus auguring new applications in the future as well. Usually the so-called pump-probe technique making use of two synchronized ultrashort light pulses is utilized to obtain this time-resolved data. In this work, the development and characterization of a synchronization system enabling such pump-probe studies at the storage ring PETRA III in combination with an external, then synchronized fs-laser system is described. The synchronization is based on an extended PLL approach with three interconnected feedback loops allowing to monitor short-time losses of the lock and thus prevent them. This way, the jitter between the laser PHAROS and the PETRA III reference signal is reduced to σ <5 ps. Thus the system allows to conduct experiments at a repetition rate of 130 kHz with a temporal resolution limited only by the X-ray pulse length. A major emphasis in the fundamental introductory chapters is an intuitive explanation of the basic principles of phase locked loops and the different aspects of phase noise to allow a deeper understanding of the synchronization. Furthermore, first pump-probe experiments conducted at different beamlines at PETRA III are presented, demonstrating the usability of the laser system in a scientific environment as well. In first characterizing experiments the pulse duration of PETRA III X-ray pulses has been measured to be 90 ps FWHM. In particular, there have been time resolved X-ray absorption spectroscopy experiments on Gaq3 and Znq2 conducted at beamline P11. First results show dynamics of the electronic excitation on the timescale of a few hundred pico seconds up to a few nano seconds and provide a basic understanding for further research on those molecules. For Gaq3 this data is analyzed in detail and compared with visible fluorescence measurements suggesting at least

Direct observation of superconducting gaps in MgB 2 by angle-resolved photoemission spectroscopy

Science.gov (United States)

Souma, S.; Machida, Y.; Sato, T.; Takahashi, T.; Matsui, H.; Wang, S.-C.; Ding, H.; Kaminski, A.; Campuzano, J. C.; Sasaki, S.; Kadowaki, K.

2004-08-01

High-resolution angle-resolved photoemission spectroscopy has been carried out to clarify the anomalous superconductivity of MgB 2. We observed three bands crossing the Fermi level, which are ascribed to B2p-σ, π and surface bands. We have succeeded for the first time in directly observing the superconducting gaps of these bands separately. We have found that the superconducting-gap sizes of σ and surface bands are 6.5 ± 0.5 and 6.0 ± 0.5 meV, respectively, while that of the π band is much smaller (1.5 ± 0.5 meV). The present experimental result unambiguously demonstrates the validity of the two-band superconductivity in MgB 2.

Direct observation of superconducting gaps in MgB2 by angle-resolved photoemission spectroscopy

International Nuclear Information System (INIS)

Souma, S.; Machida, Y.; Sato, T.; Takahashi, T.; Matsui, H.; Wang, S.-C.; Ding, H.; Kaminski, A.; Campuzano, J.C.; Sasaki, S.; Kadowaki, K.

2004-01-01

High-resolution angle-resolved photoemission spectroscopy has been carried out to clarify the anomalous superconductivity of MgB 2 . We observed three bands crossing the Fermi level, which are ascribed to B2p-σ, π and surface bands. We have succeeded for the first time in directly observing the superconducting gaps of these bands separately. We have found that the superconducting-gap sizes of σ and surface bands are 6.5 ± 0.5 and 6.0 ± 0.5 meV, respectively, while that of the π band is much smaller (1.5 ± 0.5 meV). The present experimental result unambiguously demonstrates the validity of the two-band superconductivity in MgB 2

On-chip dual-comb source for spectroscopy.

Science.gov (United States)

Dutt, Avik; Joshi, Chaitanya; Ji, Xingchen; Cardenas, Jaime; Okawachi, Yoshitomo; Luke, Kevin; Gaeta, Alexander L; Lipson, Michal

2018-03-01

Dual-comb spectroscopy is a powerful technique for real-time, broadband optical sampling of molecular spectra, which requires no moving components. Recent developments with microresonator-based platforms have enabled frequency combs at the chip scale. However, the need to precisely match the resonance wavelengths of distinct high quality-factor microcavities has hindered the development of on-chip dual combs. We report the simultaneous generation of two microresonator combs on the same chip from a single laser, drastically reducing experimental complexity. We demonstrate broadband optical spectra spanning 51 THz and low-noise operation of both combs by deterministically tuning into soliton mode-locked states using integrated microheaters, resulting in narrow (lasers or microwave oscillators. We demonstrate high signal-to-noise ratio absorption spectroscopy spanning 170 nm using the dual-comb source over a 20-μs acquisition time. Our device paves the way for compact and robust spectrometers at nanosecond time scales enabled by large beat-note spacings (>1 GHz).

Time-resolved X-ray absorption spectroscopy for laser-ablated silicon particles in xenon gas

International Nuclear Information System (INIS)

Makimura, Tetsuya; Sakuramoto, Tamaki; Murakami, Kouichi

1996-01-01

We developed a laboratory-scale in situ apparatus for soft X-ray absorption spectroscopy with a time resolution of 10 ns and a space resolution of 100 μm. Utilizing this spectrometer, we have investigated the dynamics of silicon atoms formed by laser ablation in xenon gas. It was found that 4d-electrons in the xenon atoms are excited through collision with electrons in the laser-generated silicon plasma. (author)

STROBE-X: X-ray Timing & Spectroscopy on Dynamical Timescales from Microseconds to Years

Science.gov (United States)

Wilson-Hodge, Colleen A.; Ray, Paul S.; Maccarone, Thomas J.; Chakrabarty, Deepto; Gendreau, Keith C.; Arzoumanian, Zaven; Jenke, Peter; Ballantyne, David; Bozzo, Enrico; Brandt, Soren; Brenneman, Laura; Christophersen, Marc; DeRosa, Alessandra; Feroci, Marco; Goldstein, Adam; Hartmann, Dieter; Hernanz, Margarita; McDonald, Michael; Phlips, Bernard; Remillard, Ronald; Stevens, Abigail; Tomsick, John; Watts, Anna; Wood, Kent S.; Zane, Silvia; STROBE-X Collaboration

2018-01-01

We describe a probe-class mission concept that provides an unprecedented view of the X-ray sky, performing timing and 0.2-30 keV spectroscopy over timescales from microseconds to years. The Spectroscopic Time-Resolving Observatory for Broadband Energy X-rays (STROBE-X) comprises three primary instruments. The first uses an array of lightweight optics (3-m focal length) that concentrate incident photons onto solid state detectors with CCD-level (85-130 eV) energy resolution, 100 ns time resolution, and low background rates to cover the 0.2-12 keV band. This technology is scaled up from NICER, with enhanced optics to take advantage of the longer focal length of STROBE-X. The second uses large-area collimated silicon drift detectors, developed for ESA's LOFT, to cover the 2-30 keV band. These two instruments each provide an order of magnitude improvement in effective area compared with its predecessor (NICER and RXTE, respectively). Finally, a sensitive sky monitor triggers pointed observations, provides high duty cycle, high time resolution, high spectral resolution monitoring of the X-ray sky with ~20 times the sensitivity of the RXTE ASM, and enables multi-wavelength and multi-messenger studies on a continuous, rather than scanning basis. We include updated instrument designs resulting from the GSFC IDL run in November 2017.For the first time, the broad coverage provides simultaneous study of thermal components, non-thermal components, iron lines, and reflection features from a single platform for accreting black holes at all scales. The enormous collecting area allows detailed studies of the dense matter equation of state using both thermal emission from rotation-powered pulsars and harder emission from X-ray burst oscillations. The combination of the wide-field monitor and the sensitive pointed instruments enables observations of potential electromagnetic counterparts to LIGO/Virgo and neutrino events. Extragalactic science, such as constraining bulk metalicity

Time-resolved photoluminescence of Ga(NAsP) multiple quantum wells grown on Si substrate: Effects of rapid thermal annealing

Energy Technology Data Exchange (ETDEWEB)

Woscholski, R., E-mail: ronja.woscholski@physik.uni-marburg.de; Shakfa, M.K.; Gies, S.; Wiemer, M.; Rahimi-Iman, A.; Zimprich, M.; Reinhard, S.; Jandieri, K.; Baranovskii, S.D.; Heimbrodt, W.; Volz, K.; Stolz, W.; Koch, M.

2016-08-31

Time-resolved photoluminescence (TR-PL) spectroscopy has been used to study the impact of rapid thermal annealing (RTA) on the optical properties and carrier dynamics in Ga(NAsP) multiple quantum well heterostructures (MQWHs) grown on silicon substrates. TR-PL measurements reveal an enhancement in the PL efficiency when the RTA temperature is increased up to 925 °C. Then, the PL intensity dramatically decreases with the annealing temperature. This behavior is explained by the variation of the disorder degree in the studied structures. The analysis of the low-temperature emission-energy-dependent PL decay time enables us to characterize the disorder in the Ga(NAsP) MQWHs. The theoretically extracted energy-scales of disorder confirm the experimental observations. - Highlights: • Ga(NAsP) multiple quantum well heterostructures (MQWHs) grown on silicon substrates • Impact of rapid thermal annealing on the optical properties and carrier dynamics • Time resolved photoluminescence spectroscopy was applied. • PL transients became continuously faster with increasing annealing temperature. • Enhancement in the PL efficiency with increasing annealing temperature up to 925 °C.

Time-resolved photoluminescence of Ga(NAsP) multiple quantum wells grown on Si substrate: Effects of rapid thermal annealing

International Nuclear Information System (INIS)

Woscholski, R.; Shakfa, M.K.; Gies, S.; Wiemer, M.; Rahimi-Iman, A.; Zimprich, M.; Reinhard, S.; Jandieri, K.; Baranovskii, S.D.; Heimbrodt, W.; Volz, K.; Stolz, W.; Koch, M.

2016-01-01

Time-resolved photoluminescence (TR-PL) spectroscopy has been used to study the impact of rapid thermal annealing (RTA) on the optical properties and carrier dynamics in Ga(NAsP) multiple quantum well heterostructures (MQWHs) grown on silicon substrates. TR-PL measurements reveal an enhancement in the PL efficiency when the RTA temperature is increased up to 925 °C. Then, the PL intensity dramatically decreases with the annealing temperature. This behavior is explained by the variation of the disorder degree in the studied structures. The analysis of the low-temperature emission-energy-dependent PL decay time enables us to characterize the disorder in the Ga(NAsP) MQWHs. The theoretically extracted energy-scales of disorder confirm the experimental observations. - Highlights: • Ga(NAsP) multiple quantum well heterostructures (MQWHs) grown on silicon substrates • Impact of rapid thermal annealing on the optical properties and carrier dynamics • Time resolved photoluminescence spectroscopy was applied. • PL transients became continuously faster with increasing annealing temperature. • Enhancement in the PL efficiency with increasing annealing temperature up to 925 °C

Capturing Structural Snapshots during Photochemical Reactions with Ultrafast Raman Spectroscopy: From Materials Transformation to Biosensor Responses.

Science.gov (United States)

Fang, Chong; Tang, Longteng; Oscar, Breland G; Chen, Cheng

2018-06-21

Chemistry studies the composition, structure, properties, and transformation of matter. A mechanistic understanding of the pertinent processes is required to translate fundamental knowledge into practical applications. The current development of ultrafast Raman as a powerful time-resolved vibrational technique, particularly femtosecond stimulated Raman spectroscopy (FSRS), has shed light on the structure-energy-function relationships of various photosensitive systems. This Perspective reviews recent work incorporating optical innovations, including the broad-band up-converted multicolor array (BUMA) into a tunable FSRS setup, and demonstrates its resolving power to watch metal speciation and photolysis, leading to high-quality thin films, and fluorescence modulation of chimeric protein biosensors for calcium ion imaging. We discuss advantages of performing FSRS in the mixed time-frequency domain and present strategies to delineate mechanisms by tracking low-frequency modes and systematically modifying chemical structures with specific functional groups. These unique insights at the chemical-bond level have started to enable the rational design and precise control of functional molecular machines in optical, materials, energy, and life sciences.

Time-resolved emission from laser-ablated uranium

International Nuclear Information System (INIS)

Stoffels, E.; Mullen, J. van der; Weijer, P. van de

1991-01-01

Time-resolved emission spectra from the plasma, induced by laser ablation of uranium samples have been studied. The dependence of the emission intensity on time is strongly affected by the nature and pressure of the buffer gas. Air and argon have been used in the pressure range 0.002 to 5 mbar. The emission intensity as a function of time displays three maxima, indicating that three different processes within the expanding plasma plume are involved. On basis of the time-resolved spectra we propose a model that explains qualitatively the phenomena that are responsible for this time behaviour. (author)

An x-ray detector for time-resolved studies

International Nuclear Information System (INIS)

Rodricks, B.; Brizard, C.; Clarke, R.; Lowe, W.

1992-01-01

The development of ultrahigh-brightness x-ray sources makes time-resolved x-ray studies more and more feasible. Improvements in x-ray optics components are also critical for obtaining the appropriate beam for a particular type of experiment. Moreover, fast parallel detectors will be essential in order to exploit the combination of high intensity x-ray sources and novel optics for time-resolved experiments. A CCD detector with a time resolution of microseconds has been developed at the Advanced Photon Source (APS). This detector is fully programmable using CAMAC electronics and a Micro Vax computer. The techniques of time-resolved x-ray studies, which include scattering, microradiography, microtomography, stroboscopy, etc., can be applied to a range of phenomena (including rapid thermal annealing, surface ordering, crystallization, and the kinetics of phase transition) in order to understand these time-dependent microscopic processes. Some of these applications will be illustrated by recent results performed at synchrotrons. New powerful x-ray sources now under construction offer the opportunity to apply innovative approaches in time-resolved work

Tunable All Reflective Spatial Heterodyne Spectroscopy, A Technique For High Resolving Power Observation OI Defused Emission Line Sources

Science.gov (United States)

Hosseini, Seyedeh Sona

The solar system presents a challenge to spectroscopic observers, because it is an astrophysically low energy environment populated with often angularly extended targets (e.g, interplanetary medium, comets, planetary upper atmospheres, and planet and satellite near space environments). Spectroscopy is a proven tool for determining compositional and other properties of remote objects. Narrow band imaging and low resolving spectroscopic measurements provide information about composition, photochemical evolution, energy distribution and density. The extension to high resolving power provides further access to temperature, velocity, isotopic ratios, separation of blended sources, and opacity effects. The drawback of high-resolution spectroscopy comes from the instrumental limitations of lower throughput, the necessity of small entrance apertures, sensitivity, field of view, and large physical instrumental size. These limitations quickly become definitive for faint and/or extended targets and for spacecraft encounters. An emerging technique with promise for the study of faint, extended sources at high resolving power is the all-reflective form of the Spatial Heterodyne Spectrometer (SHS). SHS instruments are compact and naturally possess both high etendue and high resolving power. To achieve similar spectral grasp, grating spectrometers require big telescopes. SHS is a common-path beam Fourier transform interferometer that produces Fizeau fringe pattern for all other wavelengths except the tuned wavelength. Compared to similar Fourier transform Spectrometers (FTS), SHS has considerably relaxed optical tolerances that make it easier to use in the visible and UV spectral ranges. The large etendue of SHS instruments makes them ideal for observations of extended, low surface brightness, isolated emission line sources, while their intrinsically high spectral resolution enables the study of the dynamical and spectral characteristics described above. SHS also combines very

Interaction of europium and nickel with calcite studied by Rutherford Backscattering Spectrometry and Time-Resolved Laser Fluorescence Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Sabau, A. [Agence Nationale pour la gestion des Déchets RAdioactifs, 1-7 rue J. Monnet, Parc de la Croix Blanche, 92298 Châtenay-Malabry Cedex (France); Université de Nice Sophia Antipolis, Ecosystèmes Côtiers Marins et Réponses aux Stress (ECOMERS), 28 avenue Valrose, 06108 Nice Cedex 2 (France); Pipon, Y., E-mail: pipon@ipnl.in2p3.fr [Institut de Physique Nucléaire de Lyon (IPNL), Université Lyon 1, CNRS/IN2P3, 4 rue Enrico Fermi, 69 622 Villeurbanne Cedex (France); Institut Universitaire de Technologie (IUT) Lyon-1, Université Claude Bernard Lyon 1, 69 622 Villeurbanne Cedex (France); Toulhoat, N. [Institut de Physique Nucléaire de Lyon (IPNL), Université Lyon 1, CNRS/IN2P3, 4 rue Enrico Fermi, 69 622 Villeurbanne Cedex (France); CEA/DEN, Saclay, 91191 Gif sur Yvette (France); Lomenech, C. [Université de Nice Sophia Antipolis, Ecosystèmes Côtiers Marins et Réponses aux Stress (ECOMERS), 28 avenue Valrose, 06108 Nice Cedex 2 (France); Jordan, N. [Helmholtz Zentrum Dresden Rossendorf (HZDR), Institute of Resource Ecology (IRE) (Germany); Moncoffre, N. [Institut de Physique Nucléaire de Lyon (IPNL), Université Lyon 1, CNRS/IN2P3, 4 rue Enrico Fermi, 69 622 Villeurbanne Cedex (France); Barkleit, A. [Helmholtz Zentrum Dresden Rossendorf (HZDR), Institute of Resource Ecology (IRE) (Germany); and others

2014-08-01

This study aims at elucidating the mechanisms regulating the interaction of Eu and Ni with calcite (CaCO{sub 3}). Calcite powders or single crystals (some mm sized) were put into contact with Eu or Ni solutions at concentrations ranging from 10{sup −3} to 10{sup −5} mol L{sup −1} for Eu and 10{sup −3} mol L{sup −1} for Ni. The sorption durations ranged from 1 week to 1 month. Rutherford Backscattering Spectrometry (RBS) well adapted to discriminate incorporation processes such as: (i) adsorption or co precipitation at the mineral surfaces or, (ii) incorporation into the mineral structure (through diffusion for instance), has been carried out. Moreover, using the fluorescence properties of europium, the results have been compared to those obtained by Time-Resolved Laser Fluorescence Spectroscopy (TRLFS) on calcite powders. For the single crystals, complementary SEM observations of the mineral surfaces at low voltage were also performed. Results showed that Ni accumulates at the calcite surface whereas Eu is also incorporated at a greater depth. Eu seems therefore to be incorporated into two different states in calcite: (i) heterogeneous surface accumulation and (ii) incorporation at depth greater than 160 nm after 1 month of sorption. Ni was found to accumulate at the surface of calcite without incorporation.

Site-Specific Measurement of Water Dynamics in the Substrate Pocket of Ketosteroid Isomerase Using Time-Resolved Vibrational Spectroscopy

Science.gov (United States)

Jha, Santosh Kumar; Ji, Minbiao; Gaffney, Kelly J.; Boxer, Steven G.

2012-01-01

Little is known about the reorganization capacity of water molecules at the active sites of enzymes and how this couples to the catalytic reaction. Here, we study the dynamics of water molecules at the active site of a highly proficient enzyme, Δ5-3-ketosteroid isomerase (KSI), during a light-activated mimic of its catalytic cycle. Photo-excitation of a nitrile containing photo-acid, coumarin183 (C183), mimics the change in charge density that occurs at the active site of KSI during the first step of the catalytic reaction. The nitrile of C183 is exposed to water when bound to the KSI active site, and we used time-resolved vibrational spectroscopy as a site-specific probe to study the solvation dynamics of water molecules in the vicinity of the nitrile. We observed that water molecules at the active site of KSI are highly rigid, during the light-activated catalytic cycle, compared to the solvation dynamics observed in bulk water. Based upon this result we hypothesize that rigid water dipoles at the active site might help in the maintenance of the pre-organized electrostatic environment required for efficient catalysis. The results also demonstrate the utility of nitrile probes in measuring the dynamics of local (H-bonded) water molecules in contrast to the commonly used fluorescence methods which measure the average behavior of primary and subsequent spheres of solvation. PMID:22931297

Super-Eddington accretion on to the neutron star NGC 7793 P13: Broad-band X-ray spectroscopy and ultraluminous X-ray sources

Science.gov (United States)

Walton, D. J.; Fürst, F.; Harrison, F. A.; Stern, D.; Bachetti, M.; Barret, D.; Brightman, M.; Fabian, A. C.; Middleton, M. J.; Ptak, A.; Tao, L.

2018-02-01

We present a detailed, broad-band X-ray spectral analysis of the ultraluminous X-ray source (ULX) pulsar NGC 7793 P13, a known super-Eddington source, utilizing data from the XMM-Newton, NuSTAR and Chandra observatories. The broad-band XMM-Newton+NuSTAR spectrum of P13 is qualitatively similar to the rest of the ULX sample with broad-band coverage, suggesting that additional ULXs in the known population may host neutron star accretors. Through time-averaged, phase-resolved and multi-epoch studies, we find that two non-pulsed thermal blackbody components with temperatures ∼0.5 and 1.5 keV are required to fit the data below 10 keV, in addition to a third continuum component which extends to higher energies and is associated with the pulsed emission from the accretion column. The characteristic radii of the thermal components appear to be comparable, and are too large to be associated with the neutron star itself, so the need for two components likely indicates the accretion flow outside the magnetosphere is complex. We suggest a scenario in which the thick inner disc expected for super-Eddington accretion begins to form, but is terminated by the neutron star's magnetic field soon after its onset, implying a limit of B ≲ 6 × 1012 G for the dipolar component of the central neutron star's magnetic field. Evidence of similar termination of the disc in other sources may offer a further means of identifying additional neutron star ULXs. Finally, we examine the spectrum exhibited by P13 during one of its unusual 'off' states. These data require both a hard power-law component, suggesting residual accretion on to the neutron star, and emission from a thermal plasma, which we argue is likely associated with the P13 system.

Photodissociation of gaseous CH3COSH at 248 nm by time-resolved Fourier-transform infrared emission spectroscopy: Observation of three dissociation channels

International Nuclear Information System (INIS)

Hu, En-Lan; Tsai, Po-Yu; Fan, He; Lin, King-Chuen

2013-01-01

Upon one-photon excitation at 248 nm, gaseous CH 3 C(O)SH is dissociated following three pathways with the products of (1) OCS + CH 4 , (2) CH 3 SH + CO, and (3) CH 2 CO + H 2 S that are detected using time-resolved Fourier-transform infrared emission spectroscopy. The excited state 1 (n O , π * CO ) has a radiative lifetime of 249 ± 11 ns long enough to allow for Ar collisions that induce internal conversion and enhance the fragment yields. The rate constant of collision-induced internal conversion is estimated to be 1.1 × 10 −10 cm 3 molecule −1 s −1 . Among the primary dissociation products, a fraction of the CH 2 CO moiety may undergo further decomposition to CH 2 + CO, of which CH 2 is confirmed by reaction with O 2 producing CO 2 , CO, OH, and H 2 CO. Such a secondary decomposition was not observed previously in the Ar matrix-isolated experiments. The high-resolution spectra of CO are analyzed to determine the ro-vibrational energy deposition of 8.7 ± 0.7 kcal/mol, while the remaining primary products with smaller rotational constants are recognized but cannot be spectrally resolved. The CO fragment detected is mainly ascribed to the primary production. A prior distribution method is applied to predict the vibrational distribution of CO that is consistent with the experimental findings.

Real-time reflectance-difference spectroscopy of GaAs molecular beam epitaxy homoepitaxial growth

Directory of Open Access Journals (Sweden)

A. Lastras-Martínez

2014-03-01

Full Text Available We report on real time-resolved Reflectance-difference (RD spectroscopy of GaAs(001 grown by molecular beam epitaxy, with a time-resolution of 500 ms per spectrum within the 2.3–4.0 eV photon energy range. Through the analysis of transient RD spectra we demonstrated that RD line shapes are comprised of two components with different physical origins and determined their evolution during growth. Such components were ascribed to the subsurface strain induced by surface reconstruction and to surface stoichiometry. Results reported in this paper render RD spectroscopy as a powerful tool for the study of fundamental processes during the epitaxial growth of zincblende semiconductors.

Time-resolved laser-excited Shpol'skii spectrometry with a fiber-optic probe and ICCD camera

International Nuclear Information System (INIS)

Bystol, Adam J.; Campiglia, Andres D.; Gillispie, Gregory D.

2000-01-01

Improved methodology for chemical analysis via laser-excited Shpol'skii spectrometry is reported. The complications of traditional methodology for measurements at liquid nitrogen temperature are avoided by freezing the distal end of a bifurcated fiber-optic probe directly into the sample matrix. Emission wavelength-time matrices were rapidly collected by automatically incrementing the gate delay of an intensified charge-coupled device (ICCD) camera relative to the laser excitation pulse. The excitation source is a compact frequency-doubled tunable dye laser whose bandwidth (<0.03 nm) is well matched for Shpol'skii spectroscopy. Data reproducibility for quantitative analysis purposes and analytical figures of merit are demonstrated for several polycyclic aromatic hydrocarbons at 77 K. Although not attempted in this study, time-resolved excitation-emission matrices could easily be collected with this instrumental system. (c) 2000 Society for Applied Spectroscopy

A variable-tune spatial heterodyne spectrometer for broadband spectral line studies in the visible and near-UV

Science.gov (United States)

Dawson, Olivia R.; Harris, Walter M.

2017-11-01

Reflective Spatial Heterodyne Spectroscopy (SHS) is an interferometric technique that combines high resolving power and a large input acceptance angle in a format that is compact enough for use at small telescope focal planes and in spacecraft observations of targets in the visible to far ultra-violet (FUV) spectral range. SHS instruments are well suited to the study of faint, extended emission line sources, particularly in the UV where stellar background continuum becomes weak. Their primary limitation comes from the limited spatial sampling of the output interference pattern generated by the incoming spectral source, which limits their use to narrow bandpass near the central tuning wavelength. We describe a the first light results from a broadband SHS that can be used to scan the tuning wavelength across a bandpass extending from 300 to 700 nm. The limitations on the bandpass are arbitrary and can easily be extended into the UV or near infrared. We discuss the results of these validation program and the potential improvements that could be used to expand and/or improve the broadband spectral response of the instrument.

Nanosecond retinal structure changes in K-590 during the room-temperature bacteriorhodopsin photocycle: picosecond time-resolved coherent anti-stokes Raman spectroscopy

OpenAIRE

Weidlich, O.; Ujj, L.; Jäger, F.; Atkinson, G.H.

1997-01-01

Time-resolved vibrational spectra are used to elucidate the structural changes in the retinal chromophore within the K-590 intermediate that precedes the formation of the L-550 intermediate in the room-temperature (RT) bacteriorhodopsin (BR) photocycle. Measured by picosecond time-resolved coherent anti-Stokes Raman scattering (PTR/CARS), these vibrational data are recorded within the 750 cm-1 to 1720 cm-1 spectral region and with time delays of 50-260 ns after the RT/BR photocycle is optical...

Multicomponent gas analysis using broadband quantum cascade laser spectroscopy

NARCIS (Netherlands)

Reyes Reyes, A.; Hou, Z.; Van Mastrigt, E.; Horsten, R.C.; De Jongste, J.C.; Pijnenburg, M.W.; Urbach, H.P.; Bhattacharya, N.

2014-01-01

We present a broadband quantum cascade laser-based spectroscopic system covering the region between 850 and 1250 cm?1. Its robust multipass cavity ensures a constant interaction length over the entire spectral region. The device enables the detection and identification of numerous molecules present

A Polarization-Adjustable Picosecond Deep-Ultraviolet Laser for Spin- and Angle-Resolved Photoemission Spectroscopy

International Nuclear Information System (INIS)

Zhang Feng-Feng; Yang Feng; Zhang Shen-Jin; Wang Zhi-Min; Xu Feng-Liang; Peng Qin-Jun; Zhang Jing-Yuan; Xu Zu-Yan; Wang Xiao-Yang; Chen Chuang-Tian

2012-01-01

We report on a polarization-adjustable picosecond deep-ultraviolet (DUV) laser at 177.3 nm. The DUV laser was produced by second harmonic generation from a mode-locked laser at 355 nm in nonlinear optical crystal KBBF. The laser delivered a maximum average output power of 1.1 mW at 177.3 nm. The polarization of the 177.3 nm beam was adjusted with linear and circular polarization by means of λ/4 and λ/2 wave plates. To the best of our knowledge, the laser has been employed as the circularly polarized and linearly polarized DUV light source for a spin- and angle-resolved photoemission spectroscopy with high resolution for the first time. (fundamental areas of phenomenology(including applications))

Spatially resolved positron annihilation spectroscopy on friction stir weld induced defects.

Science.gov (United States)

Hain, Karin; Hugenschmidt, Christoph; Pikart, Philip; Böni, Peter

2010-04-01

A friction stir welded (FSW) Al alloy sample was investigated by Doppler broadening spectroscopy (DBS) of the positron annihilation line. The spatially resolved defect distribution showed that the material in the joint zone becomes completely annealed during the welding process at the shoulder of the FSW tool, whereas at the tip, annealing is prevailed by the deterioration of the material due to the tool movement. This might be responsible for the increased probability of cracking in the heat affected zone of friction stir welds. Examination of a material pairing of steel S235 and the Al alloy Silafont36 by coincident Doppler broadening spectroscopy (CDBS) indicates the formation of annealed steel clusters in the Al alloy component of the sample. The clear visibility of Fe in the CDB spectra is explained by the very efficient trapping at the interface between steel cluster and bulk.

Effective temporal resolution in pump-probe spectroscopy with strongly chirped pulses

International Nuclear Information System (INIS)

Polli, D.; Lanzani, G.; Brida, D.; Cerullo, G.; Mukamel, S.

2010-01-01

This paper introduces a general theoretical description of femtosecond pump-probe spectroscopy with chirped pulses whose joint spectral and temporal profile is expressed by Wigner spectrograms. We demonstrate that the actual experimental time resolution intimately depends on the pulse-sample interaction and that the commonly used instrumental response function needs to be replaced by a sample-dependent effective response function. We also show that, using the proper configurations in excitation and/or detection, it is possible to overcome the temporal smearing of the measured dynamics due to chirp-induced pulse broadening and recover the temporal resolution that would be afforded by the transform-limited pulses. We verify these predictions with experiments using broadband chirped pump and probe pulses. Our results allow optimization of the temporal resolution in the common case when the chirp of the pump and/or probe pulse is not corrected and may be extended to a broad range of time-resolved experiments.

Metalation of positively charged water soluble mesoporphyrins studied via time-resolved SERRS spectroscopy

Science.gov (United States)

Procházka, Marek; Hanzliková, Jana; Štěpánek, Josef; Baumruk, Vladimir

1997-06-01

Time-resolved SERRS spectra of 5,10,15,20-tetrakis[4-(trimethylammonio)phenyl]21 H,23 H-porphine (TMAP) were recorded (using a multichannel Raman spectrometer) in various SERS-active Ag colloid/porphyrin systems. Data treatment based on a factor analysis was used to decompose all the SERRS spectra into two main components: SERRS spectrum of the free base TMAP and that of its Ag metalated form. The metalation kinetics obtained in this way was found to be highly dependent on the presence of phosphate anions, citrate and/or Triton X-100 in the colloidal system. The results are analogous to those previously obtained for 5,10,15,20-tetrakis(1-methyl-4-pyridyl)21 H,23 H-porphine, a porphyrin with a substantially stronger tendency towards metalation.

Direct observation of superconducting gaps in MgB{sub 2} by angle-resolved photoemission spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Souma, S.; Machida, Y.; Sato, T.; Takahashi, T.; Matsui, H.; Wang, S.-C.; Ding, H.; Kaminski, A.; Campuzano, J.C.; Sasaki, S.; Kadowaki, K

2004-08-01

High-resolution angle-resolved photoemission spectroscopy has been carried out to clarify the anomalous superconductivity of MgB{sub 2}. We observed three bands crossing the Fermi level, which are ascribed to B2p-{sigma}, {pi} and surface bands. We have succeeded for the first time in directly observing the superconducting gaps of these bands separately. We have found that the superconducting-gap sizes of {sigma} and surface bands are 6.5 {+-} 0.5 and 6.0 {+-} 0.5 meV, respectively, while that of the {pi} band is much smaller (1.5 {+-} 0.5 meV). The present experimental result unambiguously demonstrates the validity of the two-band superconductivity in MgB{sub 2}.

Multidimensional high harmonic spectroscopy

International Nuclear Information System (INIS)

Bruner, Barry D; Soifer, Hadas; Shafir, Dror; Dudovich, Nirit; Serbinenko, Valeria; Smirnova, Olga

2015-01-01

High harmonic generation (HHG) has opened up a new frontier in ultrafast science where attosecond time resolution and Angstrom spatial resolution are accessible in a single measurement. However, reconstructing the dynamics under study is limited by the multiple degrees of freedom involved in strong field interactions. In this paper we describe a new class of measurement schemes for resolving attosecond dynamics, integrating perturbative nonlinear optics with strong-field physics. These approaches serve as a basis for multidimensional high harmonic spectroscopy. Specifically, we show that multidimensional high harmonic spectroscopy can measure tunnel ionization dynamics with high precision, and resolves the interference between multiple ionization channels. In addition, we show how multidimensional HHG can function as a type of lock-in amplifier measurement. Similar to multi-dimensional approaches in nonlinear optical spectroscopy that have resolved correlated femtosecond dynamics, multi-dimensional high harmonic spectroscopy reveals the underlying complex dynamics behind attosecond scale phenomena. (paper)

Femtosecond time-resolved two-photon photoemission study of organic semiconductor copper phthalocyanine film

International Nuclear Information System (INIS)

Tanaka, A.; Tohoku University; University of Rochester, NY; Yan, L.; Watkins, N.J.; Gao, Y.

2004-01-01

Full text: Organic semiconductors are recently attracting much interest from the viewpoints of both device and fundamental physics. These organic semiconductors are considered to be important constituents of the future devices, such as organic light-emitting diode, organic field effect transistor, and organic solid-state injection laser. In order to elucidate their detailed physical properties and to develop the future devices, it is indispensable to understand their excited-state dynamics as well as their electronic structures. The femtosecond time-resolved two-photon photoemission (TR-2PPE) spectroscopy is attracting much interest because of its capability to observe the energy-resolved excited electron dynamics. In this work, we have carried out a TR-2PPE study of the organic semiconductor copper phthalocyanine (CuPc) film. Furthermore, we have investigated the detailed electronic structure of CuPc film using the photoemission (PES) and inverse photoemission (IPES) spectroscopies. From the simultaneous PES and IPES measurements for CuPc film with a thickness of 100 nm, the lowest unoccupied molecular orbital (LUMO), highest occupied molecular orbital, and ionization potential of CuPc film have been directly determined. The observed two-photon photoemission (2PPE) spectrum of the present CuPc film, measured with photon energy of about hv=3.3 eV, exhibits a broad feature. From the energy diagram of CuPc film determined by the PES and IPES measurements, the intermediate state observed in the present 2PPE spectrum of CuPc film corresponds to the energy region between about 0.4 and 1.7 eV above the LUMO energy. From the time-resolved pump-probe measurements, it is found that the relaxation lifetimes of excited states in the present CuPc films are very short (all below 50 fs) and monotonously become faster with increasing excitation energy. We attribute this extremely fast relaxation process of photoexcitation to a rapid internal conversion process. From these results

Time-resolved photoion imaging spectroscopy: Determining energy distribution in multiphoton absorption experiments

Science.gov (United States)

Qian, D. B.; Shi, F. D.; Chen, L.; Martin, S.; Bernard, J.; Yang, J.; Zhang, S. F.; Chen, Z. Q.; Zhu, X. L.; Ma, X.

2018-04-01

We propose an approach to determine the excitation energy distribution due to multiphoton absorption in the case of excited systems following decays to produce different ion species. This approach is based on the measurement of the time-resolved photoion position spectrum by using velocity map imaging spectrometry and an unfocused laser beam with a low fluence and homogeneous profile. Such a measurement allows us to identify the species and the origin of each ion detected and to depict the energy distribution using a pure Poisson's equation involving only one variable which is proportional to the absolute photon absorption cross section. A cascade decay model is used to build direct connections between the energy distribution and the probability to detect each ionic species. Comparison between experiments and simulations permits the energy distribution and accordingly the absolute photon absorption cross section to be determined. This approach is illustrated using C60 as an example. It may therefore be extended to a wide variety of molecules and clusters having decay mechanisms similar to those of fullerene molecules.

Guest–Host Interactions Investigated by Time-Resolved X-ray Spectroscopies and Scattering at MHz Rates

DEFF Research Database (Denmark)

Haldrup, Martin Kristoffer; Vanko, G.; Gawelda, W.

2012-01-01

We have studied the photoinduced low spin (LS) to high spin (HS) conversion of [Fe(bipy)3]2+ in aqueous solution. In a laser pump/X-ray probe synchrotron setup permitting simultaneous, time-resolved X-ray diffuse scattering (XDS) and X-ray spectroscopic measurements at a 3.26 MHz repetition rate...... lifetime, allowing the detection of an ultrafast change in bulk solvent density. An analysis approach directly utilizing the spectroscopic data in the XDS analysis effectively reduces the number of free parameters, and both combined permit extraction of information about the ultrafast structural dynamics...

Kinetically controlled glass transition measurement of organic aerosol thin films using broadband dielectric spectroscopy

Directory of Open Access Journals (Sweden)

Y. Zhang

2018-06-01

Full Text Available Glass transitions from liquid to semi-solid and solid phase states have important implications for reactivity, growth, and cloud-forming (cloud condensation nuclei and ice nucleation capabilities of secondary organic aerosols (SOAs. The small size and relatively low mass concentration of SOAs in the atmosphere make it difficult to measure atmospheric SOA glass transitions using conventional methods. To circumvent these difficulties, we have adapted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols. Aerosol particles to be studied are deposited in the form of a thin film onto an interdigitated electrode (IDE using electrostatic precipitation. Dielectric spectroscopy provides dipole relaxation rates for organic aerosols as a function of temperature (373 to 233 K that are used to calculate the glass transition temperatures for several cooling or heating rates. IDE-enabled broadband dielectric spectroscopy (BDS was successfully used to measure the kinetically controlled glass transition temperatures of aerosols consisting of glycerol and four other compounds with selected cooling and heating rates. The glass transition results agree well with available literature data for these five compounds. The results indicate that the IDE-BDS method can provide accurate glass transition data for organic aerosols under atmospheric conditions. The BDS data obtained with the IDE-BDS technique can be used to characterize glass transitions for both simulated and ambient organic aerosols and to model their climate effects.

Efficient calculation of open quantum system dynamics and time-resolved spectroscopy with distributed memory HEOM (DM-HEOM).

Science.gov (United States)

Kramer, Tobias; Noack, Matthias; Reinefeld, Alexander; Rodríguez, Mirta; Zelinskyy, Yaroslav

2018-06-11

Time- and frequency-resolved optical signals provide insights into the properties of light-harvesting molecular complexes, including excitation energies, dipole strengths and orientations, as well as in the exciton energy flow through the complex. The hierarchical equations of motion (HEOM) provide a unifying theory, which allows one to study the combined effects of system-environment dissipation and non-Markovian memory without making restrictive assumptions about weak or strong couplings or separability of vibrational and electronic degrees of freedom. With increasing system size the exact solution of the open quantum system dynamics requires memory and compute resources beyond a single compute node. To overcome this barrier, we developed a scalable variant of HEOM. Our distributed memory HEOM, DM-HEOM, is a universal tool for open quantum system dynamics. It is used to accurately compute all experimentally accessible time- and frequency-resolved processes in light-harvesting molecular complexes with arbitrary system-environment couplings for a wide range of temperatures and complex sizes. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.

Low pressure-induced secondary structure transitions of regenerated silk fibroin in its wet film studied by time-resolved infrared spectroscopy.

Science.gov (United States)

He, Zhipeng; Liu, Zhao; Zhou, Xiaofeng; Huang, He

2018-06-01

The secondary structure transitions of regenerated silk fibroin (RSF) under different external perturbations have been studied extensively, except for pressure. In this work, time-resolved infrared spectroscopy with the attenuated total reflectance (ATR) accessory was employed to follow the secondary structure transitions of RSF in its wet film under low pressure. It has been found that pressure alone is favorable only to the formation of β-sheet structure. Under constant pressure there is an optimum amount of D 2 O in the wet film (D 2 O : film = 2:1) so as to provide the optimal condition for the reorganization of the secondary structure and to have the largest formation of β-sheet structure. Under constant amount of D 2 O and constant pressure, the secondary structure transitions of RSF in its wet film can be divided into three stages along with time. In the first stage, random coil, α-helix, and β-turn were quickly transformed into β-sheet. In the second stage, random coil and β-turn were relatively slowly transformed into β-sheet and α-helix, and the content of α-helix was recovered to the value prior to the application of pressure. In the third and final stage, no measurable changes can be found for each secondary structure. This study may be helpful to understand the secondary structure changes of silk fibroin in silkworm's glands under hydrostatic pressure. © 2018 Wiley Periodicals, Inc.

Electronic structure of Sr2RuO4 studied by angle-resolved photoemission spectroscopy

International Nuclear Information System (INIS)

Iwasawa, H.; Aiura, Y.; Saitoh, T.; Yoshida, Y.; Hase, I.; Ikeda, S.I.; Bando, H.; Kubota, M.; Ono, K.

2007-01-01

Electronic structure of the monolayer strontium ruthenate Sr 2 RuO 4 was investigated by high-resolution angle-resolved photoemission spectroscopy. We present photon-energy (hν) dependence of the electronic structure near the Fermi level along the ΓM line. The hν dependence has shown a strong spectral weight modulation of the Ru 4d xy and 4d zx bands

A versatile optical microscope for time-dependent single-molecule and single-particle spectroscopy

Science.gov (United States)

Li, Hao; Yang, Haw

2018-03-01

This work reports the design and implementation of a multi-function optical microscope for time-dependent spectroscopy on single molecules and single nanoparticles. It integrates the now-routine single-object measurements into one standalone platform so that no reconfiguration is needed when switching between different types of sample or spectroscopy modes. The illumination modes include evanescent field through total internal reflection, dark-field illumination, and epi-excitation onto a diffraction-limited spot suitable for confocal detection. The detection modes include spectrally resolved line imaging, wide-field imaging with dual-color capability, and two-color single-element photon-counting detection. The switch between different spectroscopy and data acquisition modes is fully automated and executed through computer programming. The capability of this microscope is demonstrated through selected proof-of-principle experiments.

A versatile optical microscope for time-dependent single-molecule and single-particle spectroscopy.

Science.gov (United States)

Li, Hao; Yang, Haw

2018-03-28

This work reports the design and implementation of a multi-function optical microscope for time-dependent spectroscopy on single molecules and single nanoparticles. It integrates the now-routine single-object measurements into one standalone platform so that no reconfiguration is needed when switching between different types of sample or spectroscopy modes. The illumination modes include evanescent field through total internal reflection, dark-field illumination, and epi-excitation onto a diffraction-limited spot suitable for confocal detection. The detection modes include spectrally resolved line imaging, wide-field imaging with dual-color capability, and two-color single-element photon-counting detection. The switch between different spectroscopy and data acquisition modes is fully automated and executed through computer programming. The capability of this microscope is demonstrated through selected proof-of-principle experiments.

Bogoliubov Angle, Particle-Hole Mixture and Angular Resolved Photoemission Spectroscopy in Superconductors

Energy Technology Data Exchange (ETDEWEB)

Balatsky, A.

2010-05-04

Superconducting excitations - Bogoliubov quasiparticles - are the quantum mechanical mixture of negatively charged electron (-e) and positively charged hole (+e). We propose a new observable for Angular Resolved Photoemission Spectroscopy (ARPES) studies that is the manifestation of the particle-hole entanglement of the superconducting quasiparticles. We call this observable a Bogoliubov angle. This angle measures the relative weight of particle and hole amplitude in the superconducting (Bogoliubov) quasiparticle. We show how this quantity can be measured by comparing the ratio of spectral intensities at positive and negative energies.

Broadband time domain acoustic holography based on the discrete orthonormal S-transform

NARCIS (Netherlands)

Zhou, H.; Lopez Arteaga, I.; Nijmeijer, H.; Lim, Kian Meng

2015-01-01

The purpose of this paper is to deal with the problem of nonstationary broadband sound fields more efficiently. A basis function of the discrete orthonormal S-transform (DOST) is used to analyze the measured signal. With respect to the time domain signal in a certain band, DOST leads to a

Improvements in brain activation detection using time-resolved diffuse optical means

Science.gov (United States)

Montcel, Bruno; Chabrier, Renee; Poulet, Patrick

2005-08-01

An experimental method based on time-resolved absorbance difference is described. The absorbance difference is calculated over each temporal step of the optical signal with the time-resolved Beer-Lambert law. Finite element simulations show that each step corresponds to a different scanned zone and that cerebral contribution increases with the arrival time of photons. Experiments are conducted at 690 and 830 nm with a time-resolved system consisting of picosecond laser diodes, micro-channel plate photo-multiplier tube and photon counting modules. The hemodynamic response to a short finger tapping stimulus is measured over the motor cortex. Time-resolved absorbance difference maps show that variations in the optical signals are not localized in superficial regions of the head, which testify for their cerebral origin. Furthermore improvements in the detection of cerebral activation is achieved through the increase of variations in absorbance by a factor of almost 5 for time-resolved measurements as compared to non-time-resolved measurements.

The electronically excited states of LH2 complexes from Rhodopseudomonas acidophila strain 10050 studied by time-resolved spectroscopy and dynamic Monte Carlo simulations. I. Isolated, non-interacting LH2 complexes.

Science.gov (United States)

Pflock, Tobias J; Oellerich, Silke; Southall, June; Cogdell, Richard J; Ullmann, G Matthias; Köhler, Jürgen

2011-07-21

We have employed time-resolved spectroscopy on the picosecond time scale in combination with dynamic Monte Carlo simulations to investigate the photophysical properties of light-harvesting 2 (LH2) complexes from the purple photosynthetic bacterium Rhodopseudomonas acidophila. The variations of the fluorescence transients were studied as a function of the excitation fluence, the repetition rate of the excitation and the sample preparation conditions. Here we present the results obtained on detergent solubilized LH2 complexes, i.e., avoiding intercomplex interactions, and show that a simple four-state model is sufficient to grasp the experimental observations quantitatively without the need for any free parameters. This approach allows us to obtain a quantitative measure for the singlet-triplet annihilation rate in isolated, noninteracting LH2 complexes.

Time resolved infrared spectroscopy of femtosecond proton dynamics in the liquid phase; Spectroscopie infrarouge resolue en temps pour l'etude de la dynamique femtoseconde du proton en phase liquide

Energy Technology Data Exchange (ETDEWEB)

Amir, W

2003-12-15

This work of thesis aims to understand the strong mobility of protons in water. Water is fundamental to life and mediates many chemical and biological processes. However this liquid is poorly understood at the molecular level. The richness of interdisciplinary sciences allows us to study the properties which make it so unique. The technique used for this study was the femtosecond time resolved vibrational spectroscopy. Several experiments were carried out to characterize the femtosecond proton dynamics in water. The visualization of the rotation of water molecules obtained by anisotropy measurements will be presented. This experiment is carried out in isotopic water HDO/D{sub 2}O for reasons of experimental and theoretical suitability. However this is not water. Pure water H{sub 2}O was also studied without thermal effects across vibrations modes. An intermolecular energy resonant transfer was observed. Finally the localized structure of the proton in water (called Eigen form) was clearly experimentally observed. This molecule is implicated in the abnormal mobility of the proton in water (Grotthuss mechanism). (author)

Ghost Spectroscopy with Classical Thermal Light Emitted by a Superluminescent Diode

Science.gov (United States)

Janassek, Patrick; Blumenstein, Sébastien; Elsäßer, Wolfgang

2018-02-01

We propose and realize the first classical ghost-imaging (GI) experiment in the frequency or wavelength domain, thus performing ghost spectroscopy using thermal light exhibiting photon bunching. The required wavelength correlations are provided by light emitted by spectrally broadband near-infrared amplified spontaneous emission of a semiconductor-based superluminescent diode. They are characterized by wavelength-resolved intensity cross-correlation measurements utilizing two-photon-absorption interferometry. Finally, a real-world spectroscopic application of this ghost spectroscopy with a classical light scheme is demonstrated in which an absorption band of trichloromethane (chloroform) at 1214 nm is reconstructed with a spectral resolution of 10 nm as a proof-of-principle experiment. This ghost-spectroscopy work fills the gap of a hitherto missing analogy between the spatial and the spectral domain in classical GI modalities, with the expectation of contributing towards a broader dissemination of correlated photon ghost modalities, hence paving the way towards more applications which exploit the favorable advantages.

Angle-resolved photoemission spectroscopy of liquid water at 29.5 eV.

Science.gov (United States)

Nishitani, Junichi; West, Christopher W; Suzuki, Toshinori

2017-07-01

Angle-resolved photoemission spectroscopy of liquid water was performed using extreme ultraviolet radiation at 29.5 eV and a time-of-flight photoelectron spectrometer. SiC/Mg coated mirrors were employed to select the single-order 19th harmonic from laser high harmonics, which provided a constant photon flux for different laser polarizations. The instrument was tested by measuring photoemission anisotropy for rare gases and water molecules and applied to a microjet of an aqueous NaI solution. The solute concentration was adjusted to eliminate an electric field gradient around the microjet. The observed photoelectron spectra were analyzed considering contributions from liquid water, water vapor, and an isotropic background. The anisotropy parameters of the valence bands (1 b 1 , 3 a 1 , and 1 b 2 ) of liquid water are considerably smaller than those of gaseous water, which is primarily attributed to electron scattering in liquid water.

Time-resolved X-ray transmission microscopy on magnetic microstructures; Zeitaufloesende Roentgentransmissionsmikroskopie an magnetischen Mikrostrukturen

Energy Technology Data Exchange (ETDEWEB)

Puzic, Aleksandar

2007-10-23

Three excitation schemes were designed for stroboscopic imaging of magnetization dynamics with time-resolved magnetic transmission X-ray microscopy (TR-MTXM). These techniques were implemented into two types of X-ray microscopes, namely the imaging transmission X-ray microscope (ITXM) and the scanning transmission X-ray microscope (STXM), both installed at the electron storage ring of the Advanced Light Source in Berkeley, USA. Circular diffraction gratings (Fresnel zone plates) used in both microscopes as focusing and imaging elements presently allow for lateral resolution down to 30 nm. Magnetic imaging is performed by using the X-ray magnetic circular dichroism (XMCD) as element specific contrast mechanism. The developed methods have been successfully applied to the experimental investigation of magnetization dynamics in ferromagnetic microstructures. A temporal resolution well below 100 ps was achieved. A conventional pump-probe technique was implemented first. The dynamic response of the magnetization excited by a broadband pulsed magnetic field was imaged spatially resolved using focused X-ray flashes. As a complementary method, the spatially resolved ferromagnetic resonance (SR-FMR) technique was developed for experimental study of magnetization dynamics in the frequency domain. As a third excitation mode, the burst excitation was implemented. The performance and efficiency of the developed methods have been demonstrated by imaging the local magnetization dynamics in laterally patterned ferromagnetic thin-film elements and three-layer stacks. The existence of multiple eigenmodes in the excitation spectra of ferromagnetic microstructures has been verified by using the pump-probe technique. Magnetostatic spin waves were selectively excited and detected with a time resolution of 50 ps using the SR-FMR technique. Thorough analysis of 20 in most cases independently prepared samples has verified that vortices which exhibit a low-amplitude switching of their core

Identifying Broadband Rotational Spectra with Neural Networks

Science.gov (United States)

Zaleski, Daniel P.; Prozument, Kirill

2017-06-01

A typical broadband rotational spectrum may contain several thousand observable transitions, spanning many species. Identifying the individual spectra, particularly when the dynamic range reaches 1,000:1 or even 10,000:1, can be challenging. One approach is to apply automated fitting routines. In this approach, combinations of 3 transitions can be created to form a "triple", which allows fitting of the A, B, and C rotational constants in a Watson-type Hamiltonian. On a standard desktop computer, with a target molecule of interest, a typical AUTOFIT routine takes 2-12 hours depending on the spectral density. A new approach is to utilize machine learning to train a computer to recognize the patterns (frequency spacing and relative intensities) inherit in rotational spectra and to identify the individual spectra in a raw broadband rotational spectrum. Here, recurrent neural networks have been trained to identify different types of rotational spectra and classify them accordingly. Furthermore, early results in applying convolutional neural networks for spectral object recognition in broadband rotational spectra appear promising. Perez et al. "Broadband Fourier transform rotational spectroscopy for structure determination: The water heptamer." Chem. Phys. Lett., 2013, 571, 1-15. Seifert et al. "AUTOFIT, an Automated Fitting Tool for Broadband Rotational Spectra, and Applications to 1-Hexanal." J. Mol. Spectrosc., 2015, 312, 13-21. Bishop. "Neural networks for pattern recognition." Oxford university press, 1995.

Subpicosecond oxygen trapping in the heme pocket of the oxygen sensor FixL observed by time-resolved resonance Raman spectroscopy.

Science.gov (United States)

Kruglik, Sergei G; Jasaitis, Audrius; Hola, Klara; Yamashita, Taku; Liebl, Ursula; Martin, Jean-Louis; Vos, Marten H

2007-05-01

Dissociation of oxygen from the heme domain of the bacterial oxygen sensor protein FixL constitutes the first step in hypoxia-induced signaling. In the present study, the photodissociation of the heme-O2 bond was used to synchronize this event, and time-resolved resonance Raman (TR(3)) spectroscopy with subpicosecond time resolution was implemented to characterize the heme configuration of the primary photoproduct. TR(3) measurements on heme-oxycomplexes are highly challenging and have not yet been reported. Whereas in all other known six-coordinated heme protein complexes with diatomic ligands, including the oxymyoglobin reported here, heme iron out-of-plane motion (doming) occurs faster than 1 ps after iron-ligand bond breaking; surprisingly, no sizeable doming is observed in the oxycomplex of the Bradyrhizobium japonicum FixL sensor domain (FixLH). This assessment is deduced from the absence of the iron-histidine band around 217 cm(-1) as early as 0.5 ps. We suggest that efficient ultrafast oxygen rebinding to the heme occurs on the femtosecond time scale, thus hindering heme doming. Comparing WT oxy-FixLH, mutant proteins FixLH-R220H and FixLH-R220Q, the respective carbonmonoxy-complexes, and oxymyoglobin, we show that a hydrogen bond of the terminal oxygen atom with the residue in position 220 is responsible for the observed behavior; in WT FixL this residue is arginine, crucially implicated in signal transmission. We propose that the rigid O2 configuration imposed by this residue, in combination with the hydrophobic and constrained properties of the distal cavity, keep dissociated oxygen in place. These results uncover the origin of the "oxygen cage" properties of this oxygen sensor protein.

Broadband Access

Indian Academy of Sciences (India)

First page Back Continue Last page Overview Graphics. Broadband Access. Worldwide market for broadband access $30 Billion! Over 200 million broadband subscribers worldwide! Various Competing Broadband access. Digital Subscriber line; Wireless; Optical Fiber.

Pricing by timing: innovating broadband data plans

Science.gov (United States)

Ha, Sangtae; Joe-Wong, Carlee; Sen, Soumya; Chiang, Mung

2012-01-01

Wireless Internet usage is doubling every year. Users are using more of high bandwidth data applications, and the heavy usage concentrates on several peak hours in a day, forcing ISPs to overprovision their networks accordingly. In order to remain profitable, ISPs have been using pricing as a congestion management tool. We review many of such pricing schemes in practice today and argue that they do not solve ISPs' problem of growing data traffic. We believe that dynamic, time-dependent usage pricing, which charges users based on when they access the Internet, can incentivize users to spread out their bandwidth consumption more evenly across different times of the day, thus helping ISPs to overcome the problem of peak congestion. Congestion pricing is not a new idea in itself, but the time for its implementation in data networks has finally arrived. Our key contribution lies in developing new analysis and a fully integrated system architecture, called TUBE (Time-dependent Usage-based Broadband price Engineering) that enables ISPs to implement the proposed TDP plan. The theory, simulation, and system implementation of TUBE system is further complemented with consumer surveys conducted in India and the US, along with preparations for a field trial that is currently underway.

Molecular dynamics of amorphous pharmaceutical fenofibrate studied by broadband dielectric spectroscopy

Directory of Open Access Journals (Sweden)

U. Sailaja

2016-06-01

Full Text Available Fenofibrate is mainly used to reduce cholesterol level in patients at risk of cardiovascular disease. Thermal transition study with the help of differential scanning calorimetry (DSC shows that the aforesaid active pharmaceutical ingredient (API is a good glass former. Based on our DSC study, the molecular dynamics of this API has been carried out by broadband dielectric spectroscopy (BDS covering wide temperature and frequency ranges. Dielectric measurements of amorphous fenofibrate were performed after its vitrification by fast cooling from a few degrees above the melting point (Tm=354.11 K to deep glassy state. The sample does not show any crystallization tendency during cooling and reaches the glassy state. The temperature dependence of the structural relaxation has been fitted by single Vogel–Fulcher–Tamman (VFT equation. From VFT fit, glass transition temperature (Tg was estimated as 250.56 K and fragility (m was determined as 94.02. This drug is classified as a fragile glass former. Deviations of experimental data from Kohlrausch–Williams–Watts (KWW fits on high-frequency flank of α-peak indicate the presence of an excess wing in fenofibrate. Based on Ngai׳s coupling model, we identified the excess wing as true Johari–Goldstein (JG process. Below the glass transition temperature one can clearly see a secondary relaxation (γ with an activation energy of 32.67 kJ/mol.

Time-resolved Femtosecond Photon Echo Probes Bimodal Solvent Dynamics

NARCIS (Netherlands)

Pshenichnikov, M.S; Duppen, K.; Wiersma, D. A.

1995-01-01

We report on time-resolved femtosecond photon echo experiments of a dye molecule in a polar solution. The photon echo is time resolved by mixing the echo with a femtosecond gate pulse in a nonlinear crystal. It is shown that the temporal profile of the photon echo allows separation of the

A tunable low-energy photon source for high-resolution angle-resolved photoemission spectroscopy

International Nuclear Information System (INIS)

Harter, John W.; Monkman, Eric J.; Shai, Daniel E.; Nie Yuefeng; Uchida, Masaki; Burganov, Bulat; Chatterjee, Shouvik; King, Philip D. C.; Shen, Kyle M.

2012-01-01

We describe a tunable low-energy photon source consisting of a laser-driven xenon plasma lamp coupled to a Czerny-Turner monochromator. The combined tunability, brightness, and narrow spectral bandwidth make this light source useful in laboratory-based high-resolution photoemission spectroscopy experiments. The source supplies photons with energies up to ∼7 eV, delivering under typical conditions >10 12 ph/s within a 10 meV spectral bandwidth, which is comparable to helium plasma lamps and many synchrotron beamlines. We first describe the lamp and monochromator system and then characterize its output, with attention to those parameters which are of interest for photoemission experiments. Finally, we present angle-resolved photoemission spectroscopy data using the light source and compare its performance to a conventional helium plasma lamp.

Spatially resolved Raman spectroscopy study of transformed zones in magnesia-partially-stabilized zirconia

International Nuclear Information System (INIS)

Davskardt, R.H.; Veirs, D.K.; Ritchie, R.O.

1989-01-01

Raman vibrational spectroscopy provides an effective phase characterization technique in materials systems containing particle dispersions of the tetragonal and monoclinic polymorphs of zirconia, each of which yields a unique Raman spectrum. An investigation is reported to assess a novel, spatially resolved Raman spectroscopy system in the study of transformed zones surrounding cracks in partially stabilized MgO-ZrO 2 (PSZ). The experimental arrangement uses an imaging (two-dimensional) photomultiplier tube to produce a one-dimensional Raman profile of phase compositions along a slitlike laser beam without translation of either the sample or the laser beam and without scanning the spectrometer. Results from phase characterization studies of the size, frontal morphology, and extent of transformation of transformation zones surrounding cracks produced under monotonic and cyclic loading conditions are presented

The analysis of time-resolved optically stimulated luminescence: I. Theoretical considerations

International Nuclear Information System (INIS)

Chithambo, M L

2007-01-01

This is the first of two linked papers on the analysis of time-resolved optically stimulated luminescence. This paper focusses on a theoretical basis of analytical methods and on methods for interpretation of time-resolved luminescence spectra and calculation of luminescence throughput. Using a comparative analysis of the principal features of time-resolved luminescence and relevant analogues from steady state optical stimulation, formulae for configuring a measurement system for optimum performance are presented. We also examine the possible use of stretched-exponential functions for analysis of time-resolved optically stimulated luminescence spectra

Kinetics and branching ratios of the reactions NH2+NO2->N2O+H2O and NH2+NO2->H2NO+NO studied by pulse radiolysis combined with time-resolved infrared diode laser spectroscopy

DEFF Research Database (Denmark)

Meunier, H.; Pagsberg, Palle Bjørn; Sillesen, A.

1996-01-01

studied by monitoring the decay of NH2 and the simultaneous formation of N2O and NO by time-resolved infrared diode laser spectroscopy. The decay rate of NH2 was studied as a function of NO2 concentration to obtain an overall rate constant k(NH2 + NO2) = (1.35 +/- 0.15) X 10(-11) molecule(-1) cm(3) s(-1...

Spatially resolved NEXAFS spectroscopy of siderophores in biological matrices

International Nuclear Information System (INIS)

Thieme, J; Kilcoyne, D; Tyliszczak, T; Haselwandter, K

2013-01-01

Iron is an essential nutrient for almost all forms of life. In the presence of oxygen iron is present in its ferric form which precipitates under formation of rather insoluble oxide-hydroxide polymers. Hence the bioavailability of iron is extremely low ( −17 M at pH 7 for Fe 3+ ). Under such conditions almost all microorganisms synthesize siderophores as iron chelating agents, thus solubilizing ferric iron from rather insoluble iron sources. Siderophores form soluble complexes with Fe 3+ . The present study aims at developing a methodology that would allow for the specific detection and localization of such iron chelators in their natural environment. The applicability of spatially resolved NEXAFS spectroscopy in the soft X-ray energy (E < 1 keV) range was evaluated for localization of typical fungal hydroxamate siderophores like ferrichrome or coprogen, which can be present in various biological materials. Results obtained with the scanning transmission X-ray microscopes at beamlines 11.0.2 and 5.3.2 of the ALS have shown characteristic signatures for siderophores. Thus NEXAFS spectroscopy at the carbon K-edge, nitrogen K-edge and iron L-edge with high spatial resolution has proven to be extremely useful for their identification in their natural environment. Spectra of different siderophores as well as spectra and images of biological material containing siderophores are presented

Study of the Bulk Charge Carrier Dynamics in Anatase and Rutile TiO2 Single Crystals by Femtosecond Time Resolved Spectroscopy

KAUST Repository

Maity, Partha

2018-04-02

Understanding of the fundamentals behind charge carriers of photo-catalytic materials are still illusive hindering progress in our quest for renewable energy. TiO2 anatase and rutile are the most understood phases in photo-catalysis and serve as the best model for fundamental studies. Their ultrafast charge carrier dynamics especially on TiO2 anatase single crystal (the most active phase) are unresolved. Here femtosecond time resolved spectroscopy (TRS) was carried out to explore the dynamics of photo-excited charge carriers’ recombination in anatase single crystal, for the first time using pump fluence effects, and compares it to that of the rutile single crystal. A significant difference in charge carrier recombination rates between both crystals is observed. We found that the time constants for carrier recombination are two orders of magnitude slower for anatase (101) when compared to those of rutile (110). Moreover, bulk defects introduced by reduction of the samples via annealing in ultra-high vacuum resulted in faster recombination rates for both polymorphs. Both states (fresh and reduced) probed by pump fluence dependence measurements revealed that the major recombination channel in fresh and reduced anatase and reduced rutile is the first-order Shockley–Reed mediated. However, for fresh rutile, third-body Auger recombination was observed, attributed to the presence of higher density of intrinsic charge carriers. At all excitation wavelengths and fluence investigated, anatase (101) single crystal show longer charge carrier lifetime when compared to rutile (110) single. This may explain the superiority of the anatase phase for the electron transfer H+ reduction to molecular hydrogen.

Angle-resolved photoemission spectroscopy with 9-eV photon-energy pulses generated in a gas-filled hollow-core photonic crystal fiber

Science.gov (United States)

Bromberger, H.; Ermolov, A.; Belli, F.; Liu, H.; Calegari, F.; Chávez-Cervantes, M.; Li, M. T.; Lin, C. T.; Abdolvand, A.; Russell, P. St. J.; Cavalleri, A.; Travers, J. C.; Gierz, I.

2015-08-01

A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few μJ energy generate vacuum ultraviolet radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi2Se3 with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promises time-resolved ARPES measurements at repetition rates of hundreds of kHz or even MHz, with photon energies that cover the first Brillouin zone of most materials.

Time-resolved CT angiography in aortic dissection

International Nuclear Information System (INIS)

Meinel, Felix G.; Nikolaou, Konstantin; Weidenhagen, Rolf; Hellbach, Katharina; Helck, Andreas; Bamberg, Fabian; Reiser, Maximilian F.; Sommer, Wieland H.

2012-01-01

Objectives: We performed this study to assess feasibility and additional diagnostic value of time-resolved CT angiography of the entire aorta in patients with aortic dissection. Materials and methods: 14 consecutive patients with known or suspected aortic dissection (aged 60 ± 9 years) referred for aortic CT angiography were scanned on a dual-source CT scanner (Somatom Definition Flash; Siemens, Forchheim, Germany) using a shuttle mode for multiphasic image acquisition (range 48 cm, time resolution 6 s, 6 phases, 100 kV, 110 mAs/rot). Effective radiation doses were calculated from recorded dose length products. For all phases, CT densities were measured in the aortic lumen and renal parenchyma. From the multiphasic data, 3 phases corresponding to a triphasic standard CT protocol, served as a reference and were compared against findings from the time-resolved datasets. Results: Mean effective radiation dose was 27.7 ± 3.5 mSv. CT density of the true lumen peaked at 355 ± 53 HU. Compared to the simulated triphasic protocol, time-resolved CT angiography added diagnostic information regarding a number of important findings: the enhancement delay between true and false lumen (n = 14); the degree of membrane oscillation (n = 14); the perfusion delay in arteries originating from the false lumen (n = 9). Other additional information included true lumen collapse (n = 4), quantitative assessment of renal perfusion asymmetry (n = 2), and dynamic occlusion of aortic branches (n = 2). In 3/14 patients (21%), these additional findings of the multiphasic protocol altered patient management. Conclusions: Multiphasic, time-resolved CT angiography covering the entire aorta is feasible at a reasonable effective radiation dose and adds significant diagnostic information with therapeutic consequences in patients with aortic dissection.

Detection in shallow water using broadband-DORT

Science.gov (United States)

Fromm, David M.; Gaumond, Charles F.; Lingevitch, Joseph F.; Gauss, Roger C.; Menis, Richard

2003-10-01

The decomposition of the time-reversal operator (DORT) [Prada et al., J. Acoust. Soc. Am. 99, 2067-2076 (1996)] has been extended into a coherent, broadband method. Broadband DORT has also been shown to isolate resolvable scatterers at various depths and ranges in a bistatic, active sonar in shallow water. Results are shown from the application of DORT to sea data taken in an area south of Hudson Canyon off the New Jersey coast during Geoclutter II. The vertical source/receiver array with 56 hydrophones spanning the water column was operated between 3.0 and 3.5 kHz. The elements were divided into four groups, with each group acting as a coherent, broadside source. Two methods were used for exciting the separate channels. One method was the use of subsequent LFMs and the other was the use of simultaneous transmission of four pseudorandom-noise signals. The target was a midwater column echo-repeater. Results are compared with modeling based on in situ environmental measurements during the experiment. [The authors acknowledge signal-processing expertise from Dr. Ning Xiang, University of Mississippi, and ENS Alan Meyer, LLNL, support from Dr. Jeff Simmen, ONR, and assistance from Dr. Charles Holland, ARL/PSU. Work supported by ONR.

Ultrafast stimulated Raman spectroscopy in the near-infrared region

International Nuclear Information System (INIS)

Takaya, Tomohisa

2016-01-01

A number of electronic transitions in the near-infrared wavelength region are associated with migration or delocalization of electrons in large molecules or molecular systems. Time-resolved near-infrared Raman spectroscopy will be a powerful tool for investigating the structural dynamic of samples with delocalized electrons. However, the sensitivity of near-infrared spontaneous Raman spectrometers is significantly low due to an extremely small probability of Raman scattering and a low sensitivity of near-infrared detectors. Nonlinear Raman spectroscopy is one of the techniques that can overcome the sensitivity problems and enable us to obtain time-resolved Raman spectra in resonance with near-IR transitions. In this article, the author introduces recent progress of ultrafast time-resolved near-infrared stimulated Raman spectroscopy. Optical setup, spectral and temporal resolution, and applications of the spectrometer are described. (author)

Angle-resolved photoemission spectroscopy of liquid water at 29.5 eV

Directory of Open Access Journals (Sweden)

Junichi Nishitani

2017-07-01

Full Text Available Angle-resolved photoemission spectroscopy of liquid water was performed using extreme ultraviolet radiation at 29.5 eV and a time-of-flight photoelectron spectrometer. SiC/Mg coated mirrors were employed to select the single-order 19th harmonic from laser high harmonics, which provided a constant photon flux for different laser polarizations. The instrument was tested by measuring photoemission anisotropy for rare gases and water molecules and applied to a microjet of an aqueous NaI solution. The solute concentration was adjusted to eliminate an electric field gradient around the microjet. The observed photoelectron spectra were analyzed considering contributions from liquid water, water vapor, and an isotropic background. The anisotropy parameters of the valence bands (1b1, 3a1, and 1b2 of liquid water are considerably smaller than those of gaseous water, which is primarily attributed to electron scattering in liquid water.

Element-resolved x-ray ferrimagnetic and ferromagnetic resonance spectroscopy

International Nuclear Information System (INIS)

Boero, G; Mouaziz, S; Rusponi, S; Bencok, P; Nolting, F; Stepanow, S; Gambardella, P

2008-01-01

We report on the measurement of element-specific magnetic resonance spectra at gigahertz frequencies using x-ray magnetic circular dichroism (XMCD). We investigate the ferrimagnetic precession of Gd and Fe ions in Gd-substituted yttrium iron garnet, showing that the resonant field and linewidth of Gd precisely coincide with Fe up to the nonlinear regime of parametric excitations. The opposite sign of the Gd x-ray magnetic resonance signal with respect to Fe is consistent with dynamic antiferromagnetic alignment of the two ionic species. Further, we investigate a bilayer metal film, Ni 80 Fe 20 (5 nm)/Ni(50 nm), where the coupled resonance modes of Ni and Ni 80 Fe 20 are separately resolved, revealing shifts in the resonance fields of individual layers but no mutual driving effects. Energy-dependent dynamic XMCD measurements are introduced, combining x-ray absorption and magnetic resonance spectroscopies

New methods and applications in time-resolved X-ray absorption spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Stoetzel, Jan Eric

2012-07-01

Recent experimental advances and developments in the QEXAFS technique were presented along with new applications in the disciplines of catalysis and surface science. Both performance and user-friendliness of the QEXAFS method were significantly improved, while the applicability of QEXAFS was extended by newly designed mechanics. The application of a fast angular encoder proved to be capable to sample the continuously changing Bragg angle of the monochromator crystal synchronized to the acquired absorption data. A new data acquisition system was designed, based on a multifunctional ADC board, which provides high acquisition frequencies, while low noise acquisition could be achieved due to the provided differential acquisition mode. Additionally, control of all experimental devices as current amplifiers, monochromator motors and sample stages were implemented to further increase the efficiency of the experimental setup for QEFAS measurements. In order to simplify the processing of the huge generated QEXAFS raw data files, a completely new software tool for data analysis was designed, which provides not only the basic procedures of QEXAFS data analysis, but also many approaches customized for time-resolved data. Apart from technical advances, various experiments were performed with QEXAFS to gain new insights into the complex processes of several catalytic reactions, the thermal decomposition of metal oxalates, as well as layer growth processes and reactions on rough surfaces. Supported Pd catalysts were investigated during catalytic partial oxidation of methane, whereby oscillations in the conversion were linked to structural changes of the catalyst. Kinetic oscillations were also investigated on a supported Pt catalyst during the extinction of CO oxidation induced by decreasing temperature. Modulated experiments were investigated (i) on supported Pt-Rh/Al{sub 2}O{sub 3} catalysts during active catalytic partial oxidation in switching gas atmospheres of methane and

Broadband for all: Connecting people from the ground up – one last mile at a time

CSIR Research Space (South Africa)

Matthee, K

2012-10-01

Full Text Available that are currently not connected utilising low-cost, locally-owned and locally-supported infrastructure to create socio-economic and commercial opportunities. ? Objectives of the project ? Establish a large scale demonstrator of the wireless mesh networks R...: Connecting people from the ground up ? one last mile at a time 4th Biennial Conference Presented by: Karel Matthee Date: 9 October 2012 Overview ? South African broadband context ? The need for broadband in rural areas ? ICT as an enabler (of socio...

Time-Resolved Spectroscopy Diagnostic of Laser-Induced Optical Breakdown

Directory of Open Access Journals (Sweden)

Christian G. Parigger

2010-01-01

Full Text Available Transient laser plasma is generated in laser-induced optical breakdown (LIOB. Here we report experiments conducted with 10.6-micron CO2 laser radiation, and with 1.064-micron fundamental, 0.532-micron frequency-doubled, 0.355-micron frequency-tripled Nd:YAG laser radiation. Characterization of laser induced plasma utilizes laser-induced breakdown spectroscopy (LIBS techniques. Atomic hydrogen Balmer series emissions show electron number density of 1017 cm−3 measured approximately 10 μs and 1 μs after optical breakdown for CO2 and Nd:YAG laser radiation, respectively. Recorded molecular recombination emission spectra of CN and C2 Swan bands indicate an equilibrium temperature in excess of 7000 Kelvin, inferred for these diatomic molecules. Reported are also graphite ablation experiments where we use unfocused laser radiation that is favorable for observation of neutral C3 emission due to reduced C3 cation formation. Our analysis is based on computation of diatomic molecular spectra that includes accurate determination of rotational line strengths, or Hönl-London factors.

Broadband luminescence in liquid-solid transition

CERN Document Server

Achilov, M F; Trunilina, O V

2002-01-01

Broadband luminescence (BBL) intensity behavior in liquid-solid transition in polyethyleneglycol-600 has been established. Oscillation of BBL intensity observed in liquid-polycrystal transition are not found to observed in liquid-amorphous solid transition. It is shown that application of the theory of electron state tails to interpretation of BBL spectral properties in liquids demands restriction. BBL spectroscopy may be applied for optimization of preparation of polymers with determined properties. (author)

Time-resolved UV spectroscopy on ammonia excited by a pulsed CO2 laser

International Nuclear Information System (INIS)

Holbach, H.

1980-07-01

This work investigates the excitation of ammonia by a pulsed CO 2 laser, in particular the processes associated with collisions with argon. It was prompted by two previous observations: the previously reported infrared multiphoton dissociation of NH 3 under nearly collisionless conditions, and the ill understood excitation mechanism of apparently nonresonant low vibrational levels in the presence of Ar. Based on recent spectroscopic data, all vibrational-rotational levels were determined which are simultaneously excited by different CO 2 laser lines. Transitions between the 1 + and 2 - vibrational levels were also taken into account. The linewidth in these calculations was dominated by power broadening, which generates a half width at half maximum of 0.36 cm -1 at the typical power density of 10 MW/cm 2 . In order to reproduce published experimental absorption data, it proved necessary to take account all transitions within a distance of 20 cm -1 from the laser line. This fact implies in most cases the simultaneous population of a large number of vibrational-rotational levels. The population of levels by absorption or by subsequent collisional processes was probed by time-resolved absorption measurement of vibrational bands and their rotational envelope in the near UV. Time resolution (5...10) was sufficient to observe rotational relaxation within individual vibrational levels. Characteristic differences were found for the various excitation lines. (orig.) [de

Time-resolved soft x-ray spectra from laser-produced Cu plasma

International Nuclear Information System (INIS)

Cone, K.V.; Dunn, J.; Baldis, H.A.; May, M.J.; Purvis, M.A.; Scott, H.A.; Schneider, M.B.

2012-01-01

The volumetric heating of a thin copper target has been studied with time resolved x-ray spectroscopy. The copper target was heated from a plasma produced using the Lawrence Livermore National Laboratory's Compact Multipulse Terrawatt (COMET) laser. A variable spaced grating spectrometer coupled to an x-ray streak camera measured soft x-ray emission (800-1550 eV) from the back of the copper target to characterize the bulk heating of the target. Radiation hydrodynamic simulations were modeled in 2-dimensions using the HYDRA code. The target conditions calculated by HYDRA were post-processed with the atomic kinetics code CRETIN to generate synthetic emission spectra. A comparison between the experimental and simulated spectra indicates the presence of specific ionization states of copper and the corresponding electron temperatures and ion densities throughout the laser-heated copper target.

Femtosecond Time-resolved Optical Polarigraphy (FTOP)

International Nuclear Information System (INIS)

Aoshima, S.; Fujimoto, M.; Hosoda, M.; Tsuchiya, Y.

2000-01-01

A novel time-resolved imaging technique named FTOP (Femtosecond Time-resolved Optical Polarigraphy) for visualizing the ultrafast propagation dynamics of intense light pulses in a medium has been proposed and demonstrated. Femtosecond snapshot images can be created with a high spatial resolution by imaging only the polarization components of the probe pulse; these polarization components change due to the instantaneous birefringence induced by the pump pulse in the medium. Ultrafast temporal changes in the two-dimensional spatial distribution of the optical pulse intensity were clearly visualized in consecutive images by changing the delay between the pump and probe. We observe that several filaments appear and then come together before the vacuum focus due to nonlinear effects in air. We also prove that filamentation dynamics such as the formation position and the propagation behavior are complex and are strongly affected by the pump energy. The results collected clearly show that this method FTOP succeeds for the first time in directly visualizing the ultrafast dynamics of the self-modulated nonlinear propagation of light. (author)

Effects of aging on working memory performance and prefrontal cortex activity:A time-resolved spectroscopy study

Institute of Scientific and Technical Information of China (English)

Jie Shi; Wenjing Zhou; Tongchao Geng; Huancong Zuo; Masahiro Tanida; Kaoru Sakatani

2016-01-01

Objective:This study aimed to employ time‐resolved spectroscopy (TRS) to explore age‐related differences in prefrontal cortex (PFC) activity while subjects performed a working memory task. Methods:We employed TRS to measure PFC activity in ten healthy younger and ten healthy older subjects while they performed a working memory (WM) task. All subjects performed the Sternberg test (ST) in which the memory‐set size varied between one and six digits. Using TRS, we recorded changes in cerebral blood oxygenation as a measure of changes in PFC activity during the task. In order to identify left/right asymmetry of PFC activity during the working memory task, we calculated the laterality score, i.e.,Δoxy‐Hb (rightΔoxy‐Hb—leftΔoxy‐Hb);positive values indicate greater activity in the right PFC, while negative values indicate greater activity in the left PFC. Results:During the ST, statistical analyses showed no significant differences between the younger and older groups in accuracy for low memory‐load and high memory‐load. In high memory‐load tasks, however, older subjects were slower than younger subjects (P Conclusions: The present results are consistent with the hemispheric asymmetry reduction in older adults (HAROLD) model;working memory tasks cause asymmetrical PFC activation in younger adults, while older adults tend to show reduced hemispheric lateralization.

Observation of Broadband Time-Dependent Rabi Shifting in Microplasmas

International Nuclear Information System (INIS)

Compton, Ryan; Filin, Alex; Romanov, Dmitri A.; Levis, Robert J.

2009-01-01

Coherent broadband radiation in the form of Rabi sidebands is observed when a ps probe laser propagates through a weakly ionized, electronically excited microplasma generated in the focus of an intense pump beam. The sidebands arise from the interaction of the probe beam with pairs of excited states of a constituent neutral atom via the probe-induced Rabi oscillation. Sideband shifting of >90 meV from the probe carrier frequency results in an effective bandwidth of 200 meV. The sidebands are controlled by the intensity and temporal profile of the probe pulse; with amplitude and shift in agreement with the predictions of a time-dependent generalized Rabi cycling model.

Nonlinear Optical Spectroscopy in the Time Domain: Studies of Ultrafast Molecular Processes in the Condensed Phase.

Science.gov (United States)

Joo, Taiha

Ultrafast molecular processes in the condensed phase at room temperature are studied in the time domain by four wave mixing spectroscopy. The structure/dynamics of various quantum states can be studied by varying the time ordering of the incident fields, their polarization, their colors, etc. In one, time-resolved coherent Stokes Raman spectroscopy of benzene is investigated at room temperature. The reorientational correlation time of benzene as well as the T_2 time of the nu _1 ring-breathing mode have been measured by using two different polarization geometries. Bohr frequency difference beats have also been resolved between the nu_1 modes of ^ {12}C_6H_6 and ^{12}C_5^{13 }CH_6.. The dephasing dynamics of the nu _1 ring-breathing mode of neat benzene is studied by time-resolved coherent anti-Stokes Raman scattering. Ultrafast time resolution reveals deviation from the conventional exponential decay. The correlation time, tau _{rm c}, and the rms magnitude, Delta, of the Bohr frequency modulation are determined for the process responsible for the vibrational dephasing by Kubo dephasing function analysis. The electronic dephasing of two oxazine dyes in ethylene glycol at room temperature is investigated by photon echo experiments. It was found that at least two stochastic processes are responsible for the observed electronic dephasing. Both fast (homogeneous) and slow (inhomogeneous) dynamics are recovered using Kubo line shape analysis. Moreover, the slow dynamics is found to spectrally diffuse over the inhomogeneous distribution on the time scale around a picosecond. Time-resolved degenerate four wave mixing signal of dyes in a population measurement geometry is reported. The vibrational coherences both in the ground and excited electronic states produced strong oscillations in the signal together with the usual population decay from the excited electronic state. Absolute frequencies and their dephasing times of the vibrational modes at ~590 cm^{-1} are obtained

Angle-resolved photoemission spectroscopy with 9-eV photon-energy pulses generated in a gas-filled hollow-core photonic crystal fiber

Energy Technology Data Exchange (ETDEWEB)

Bromberger, H., E-mail: Hubertus.Bromberger@mpsd.mpg.de; Liu, H.; Chávez-Cervantes, M.; Gierz, I. [Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg (Germany); Ermolov, A.; Belli, F.; Abdolvand, A.; Russell, P. St. J.; Travers, J. C. [Max Planck Institute for the Science of Light, Günther-Scharowsky-Str. 1, 91058 Erlangen (Germany); Calegari, F. [Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg (Germany); Institute for Photonics and Nanotechnologies, IFN-CNR, Piazza Leonardo da Vinci 32, I-20133 Milano (Italy); Li, M. T.; Lin, C. T. [Max Planck Institute for Solid State Research, Heisenbergstr. 1, 70569 Stuttgart (Germany); Cavalleri, A. [Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg (Germany); Clarendon Laboratory, Department of Physics, University of Oxford, Parks Rd. Oxford OX1 3PU (United Kingdom)

2015-08-31

A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few μJ energy generate vacuum ultraviolet radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi{sub 2}Se{sub 3} with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promises time-resolved ARPES measurements at repetition rates of hundreds of kHz or even MHz, with photon energies that cover the first Brillouin zone of most materials.

Angle-resolved photoemission spectroscopy with 9-eV photon-energy pulses generated in a gas-filled hollow-core photonic crystal fiber

International Nuclear Information System (INIS)

Bromberger, H.; Liu, H.; Chávez-Cervantes, M.; Gierz, I.; Ermolov, A.; Belli, F.; Abdolvand, A.; Russell, P. St. J.; Travers, J. C.; Calegari, F.; Li, M. T.; Lin, C. T.; Cavalleri, A.

2015-01-01

A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few μJ energy generate vacuum ultraviolet radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi 2 Se 3 with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promises time-resolved ARPES measurements at repetition rates of hundreds of kHz or even MHz, with photon energies that cover the first Brillouin zone of most materials

Determination of blood oxygenation in the brain by time-resolved reflectance spectroscopy: influence of the skin, skull, and meninges

Science.gov (United States)

Hielscher, Andreas H.; Liu, Hanli; Wang, Lihong; Tittel, Frank K.; Chance, Britton; Jacques, Steven L.

1994-07-01

Near infrared light has been used for the determination of blood oxygenation in the brain but little attention has been paid to the fact that the states of blood oxygenation in arteries, veins, and capillaries differ substantially. In this study, Monte Carlo simulations for a heterogeneous system were conducted, and near infrared time-resolved reflectance measurements were performed on a heterogeneous tissue phantom model. The model was made of a solid polyester resin, which simulates the tissue background. A network of tubes was distributed uniformly through the resin to simulate the blood vessels. The time-resolved reflectance spectra were taken with different absorbing solutions filled in the network. Based on the simulation and experimental results, we investigated the dependence of the absorption coefficient obtained from the heterogeneous system on the absorption of the actual absorbing solution filled in the tubes. We show that light absorption by the brain should result from the combination of blood and blood-free tissue background.

Investigation of verbal and visual working memory by multi-channel time-resolved functional near-infrared spectroscopy

Science.gov (United States)

Contini, D.; Caffini, M.; Re, R.; Zucchelli, L.; Spinelli, L.; Basso Moro, S.; Bisconti, S.; Ferrari, M.; Quaresima, V.; Cutini, S.; Torricelli, A.

2013-03-01

Working memory (WM) is fundamental for a number of cognitive processes, such as comprehension, reasoning and learning. WM allows the short-term maintenance and manipulation of the information selected by attentional processes. The goal of this study was to examine by time-resolved fNIRS neural correlates of the verbal and visual WM during forward and backward digit span (DF and DB, respectively) tasks, and symbol span (SS) task. A neural dissociation was hypothesised between the maintenance and manipulation processes. In particular, a dorsolateral/ventrolateral prefrontal cortex (DLPFC/VLPFC) recruitment was expected during the DB task, whilst a lateralised involvement of Brodmann Area (BA) 10 was expected during the execution of the DF task. Thirteen subjects were monitored by a multi-channel, dual-wavelength (690 and 829 nm) time-resolved fNIRS system during 3 minutes long DF and DB tasks and 4 minutes long SS task. The participants' mean memory span was calculated for each task: DF: 6.46+/-1.05 digits; DB: 5.62+/-1.26 digits; SS: 4.69+/-1.32 symbols. No correlation was found between the span level and the heart rate data (measured by pulse oximeter). As expected, DB elicited a broad activated area, in the bilateral VLPFC and the right DLPFC, whereas a more localised activation was observed over the right hemisphere during either DF (BA 10) or SS (BA 10 and 44). The robust involvement of the DLPFC during DB, compared to DF, is compatible with previous findings and with the key role of the central executive subserving in manipulating processes.

Time-domain SFG spectroscopy using mid-IR pulse shaping: practical and intrinsic advantages.

Science.gov (United States)

Laaser, Jennifer E; Xiong, Wei; Zanni, Martin T

2011-03-24

Sum-frequency generation (SFG) spectroscopy is a ubiquitous tool in the surface sciences. It provides infrared transition frequencies and line shapes that probe the structure and environment of molecules at interfaces. In this article, we apply techniques learned from the multidimensional spectroscopy community to SFG spectroscopy. We implement balanced heterodyne detection to remove scatter and the local oscillator background. Heterodyning also separates the resonant and nonresonant signals by acquiring both the real and imaginary parts of the spectrum. We utilize mid-IR pulse shaping to control the phase and delay of the mid-IR pump pulse. Pulse shaping allows phase cycling for data collection in the rotating frame and additional background subtraction. We also demonstrate time-domain data collection, which is a Fourier transform technique, and has many advantages in signal throughput, frequency resolution, and line shape accuracy over existing frequency domain methods. To demonstrate time-domain SFG spectroscopy, we study an aryl isocyanide on gold, and find that the system has an inhomogeneous structural distribution, in agreement with computational results, but which was not resolved by previous frequency-domain SFG studies. The ability to rapidly and actively manipulate the mid-IR pulse in an SFG pules sequence makes possible new experiments and more accurate spectra. © 2011 American Chemical Society

Angle-resolved reflection spectroscopy of high-quality PMMA opal crystal

Science.gov (United States)

Nemtsev, Ivan V.; Tambasov, Igor A.; Ivanenko, Alexander A.; Zyryanov, Victor Ya.

2018-02-01

PMMA opal crystal was prepared by a simple hybrid method, which includes sedimentation, meniscus formation and evaporation. We investigated three surfaces of this crystal by angle-resolved reflective light spectroscopy and SEM study. The angle-resolved reflective measurements were carried out in the 400-1100 nm range. We have determined the high-quality ordered surface of the crystal region. Narrow particle size distribution of the surface has been revealed. The average particle diameter obtained with SEM was nearly 361 nm. The most interesting result was that reflectivity of the surface turned out up to 98% at normal light incidence. Using a fit of dependences of the maximum reflectivity wavelength from an angle based on the Bragg-Snell law, the wavelength of maximum 0° reflectivity, the particle diameter and the fill factor have been determined. For the best surface maximum reflectivity wavelength of a 0° angle was estimated to be 869 nm. The particle diameter and fill factor were calculated as 372 nm and 0.8715, respectively. The diameter obtained by fitting is in excellent agreement with the particle diameter obtained with SEM. The reflectivity maximum is assumed to increase significantly when increasing the fill factor. We believe that using our simple approach to manufacture PMMA opal crystals will significantly increase the fabrication of high-quality photonic crystal templates and thin films.

A time-resolved image sensor for tubeless streak cameras

Science.gov (United States)

Yasutomi, Keita; Han, SangMan; Seo, Min-Woong; Takasawa, Taishi; Kagawa, Keiichiro; Kawahito, Shoji

2014-03-01

This paper presents a time-resolved CMOS image sensor with draining-only modulation (DOM) pixels for tube-less streak cameras. Although the conventional streak camera has high time resolution, the device requires high voltage and bulky system due to the structure with a vacuum tube. The proposed time-resolved imager with a simple optics realize a streak camera without any vacuum tubes. The proposed image sensor has DOM pixels, a delay-based pulse generator, and a readout circuitry. The delay-based pulse generator in combination with an in-pixel logic allows us to create and to provide a short gating clock to the pixel array. A prototype time-resolved CMOS image sensor with the proposed pixel is designed and implemented using 0.11um CMOS image sensor technology. The image array has 30(Vertical) x 128(Memory length) pixels with the pixel pitch of 22.4um. .

Decomposition of time-resolved tomographic PIV

NARCIS (Netherlands)

Schmid, P.J.; Violato, D.; Scarano, F.

2012-01-01

An experimental study has been conducted on a transitional water jet at a Reynolds number of Re = 5,000. Flow fields have been obtained by means of time-resolved tomographic particle image velocimetry capturing all relevant spatial and temporal scales. The measured threedimensional flow fields have

The laser spectroscopy for the quality and safety food of vegetables

International Nuclear Information System (INIS)

Falconieri, Mauro; Sighicelli, Maria

2015-01-01

ENEA has long been engaged in research in order to the development of instrumentation and application of spectroscopic methods for monitoring and diagnostics early and non-destructive state of health of plants and the quality of food products. In addition to the most common spectroscopic techniques (such as the Fourier transform infrared spectroscopy, the spectroscopy transmittance and reflectance in the visible and near infrared spectroscopy and photoluminescence), the use of which in the agro-industry is well documented in the scientific literature, particular attention has recently been paid to the Raman spectroscopy and reflectance spectroscopy Time resolved (time-resolved reflectivity spectroscopy, TRRS) with ultrashort laser pulses (in the domain of hundreds of femto seconds, 10 -15 s). [it

Nonequilibrium Molecular Energy Coupling and Conversion Mechanisms

Science.gov (United States)

2016-08-28

resolved temperature measurements, by pure rotational picosecond broadband Coherent Anti-Stokes Raman Spectroscopy ( CARS ), and kinetic modeling...rotational ps CARS for thermometry measurements in highly transient nonequilibrium plasmas. Rotational-translational temperatures are measured for time...primarily on localized flow heating on sub-acoustic time scale, and for assessing feasibility of high-speed aerodynamic flow control by vibrational

Voxel-based measurement sensitivity of spatially resolved near-infrared spectroscopy in layered tissues.

Science.gov (United States)

Niwayama, Masatsugu

2018-03-01

We quantitatively investigated the measurement sensitivity of spatially resolved spectroscopy (SRS) across six tissue models: cerebral tissue, a small animal brain, the forehead of a fetus, an adult brain, forearm muscle, and thigh muscle. The optical path length in the voxel of the model was analyzed using Monte Carlo simulations. It was found that the measurement sensitivity can be represented as the product of the change in the absorption coefficient and the difference in optical path length in two states with different source-detector distances. The results clarified the sensitivity ratio between the surface layer and the deep layer at each source-detector distance for each model and identified changes in the deep measurement area when one of the detectors was close to the light source. A comparison was made with the results from continuous-wave spectroscopy. The study also identified measurement challenges that arise when the surface layer is inhomogeneous. Findings on the measurement sensitivity of SRS at each voxel and in each layer can support the correct interpretation of measured values when near-infrared oximetry or functional near-infrared spectroscopy is used to investigate different tissue structures. (2018) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).

Portable double-sided pulsed laser heating system for time-resolved geoscience and materials science applications.

Science.gov (United States)

Aprilis, G; Strohm, C; Kupenko, I; Linhardt, S; Laskin, A; Vasiukov, D M; Cerantola, V; Koemets, E G; McCammon, C; Kurnosov, A; Chumakov, A I; Rüffer, R; Dubrovinskaia, N; Dubrovinsky, L

2017-08-01

A portable double-sided pulsed laser heating system for diamond anvil cells has been developed that is able to stably produce laser pulses as short as a few microseconds with repetition frequencies up to 100 kHz. In situ temperature determination is possible by collecting and fitting the thermal radiation spectrum for a specific wavelength range (particularly, between 650 nm and 850 nm) to the Planck radiation function. Surface temperature information can also be time-resolved by using a gated detector that is synchronized with the laser pulse modulation and space-resolved with the implementation of a multi-point thermal radiation collection technique. The system can be easily coupled with equipment at synchrotron facilities, particularly for nuclear resonance spectroscopy experiments. Examples of applications include investigations of high-pressure high-temperature behavior of iron oxides, both in house and at the European Synchrotron Radiation Facility using the synchrotron Mössbauer source and nuclear inelastic scattering.

Size effects in van der Waals clusters studied by spin and angle-resolved electron spectroscopy and multi-coincidence ion imaging

International Nuclear Information System (INIS)

Rolles, D; Pesic, Z D; Zhang, H; Bilodeau, R C; Bozek, J D; Berrah, N

2007-01-01

We have studied the valence and inner-shell photoionization of free rare-gas clusters by means of angle and spin resolved photoelectron spectroscopy and momentum resolving electron-multi-ion coincidence spectroscopy. The electron measurements probe the evolution of the photoelectron angular distribution and spin polarization parameters as a function of photon energy and cluster size, and reveal a strong cluster size dependence of the photoelectron angular distributions in certain photon energy regions. In contrast, the spin polarization parameter of the cluster photoelectrons is found to be very close to the atomic value for all covered photon energies and cluster sizes. The ion imaging measurements, which probe the fragmentation dynamics of multiply charged van der Waals clusters, also exhibit a pronounced cluster size dependence

Time-resolved studies

International Nuclear Information System (INIS)

Mills, D.M.

1992-01-01

When new or more powerful probes become available that offer both shorter data-collection times and the opportunity to apply innovative approaches to established techniques, it is natural that investigators consider the feasibility of exploring the kinetics of time-evolving systems. This stimulating area of research not only can lead to insights into the metastable or excited states that a system may populate on its way to a ground state, but can also lead to a better understanding of that final state. Synchrotron radiation, with its unique properties, offers just such a tool to extend X-ray measurements from the static to the time-resolved regime. The most straight-forward application of synchrotron radiation to the study of transient phenomena is directly through the possibility of decreased data-collection times via the enormous increase in flux over that of a laboratory X-ray system. Even further increases in intensity can be obtained through the use of novel X-ray optical devices. Widebandpass monochromators, e.g., that utilize the continuous spectral distribution of synchrotron radiation, can increase flux on the sample several orders of magnitude over conventional X-ray optical systems thereby allowing a further shortening of the data-collection time. Another approach that uses the continuous spectral nature of synchrotron radiation to decrease data-collection times is the open-quote parallel data collectionclose quotes method. Using this technique, intensities as a function of X-ray energy are recorded simultaneously for all energies rather than sequentially recording data at each energy, allowing for a dramatic decrease in the data-collection time

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

Science.gov (United States)

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-05-08

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification

Alignment of time-resolved data from high throughput experiments.

Science.gov (United States)

Abidi, Nada; Franke, Raimo; Findeisen, Peter; Klawonn, Frank

2016-12-01

To better understand the dynamics of the underlying processes in cells, it is necessary to take measurements over a time course. Modern high-throughput technologies are often used for this purpose to measure the behavior of cell products like metabolites, peptides, proteins, [Formula: see text]RNA or mRNA at different points in time. Compared to classical time series, the number of time points is usually very limited and the measurements are taken at irregular time intervals. The main reasons for this are the costs of the experiments and the fact that the dynamic behavior usually shows a strong reaction and fast changes shortly after a stimulus and then slowly converges to a certain stable state. Another reason might simply be missing values. It is common to repeat the experiments and to have replicates in order to carry out a more reliable analysis. The ideal assumptions that the initial stimulus really started exactly at the same time for all replicates and that the replicates are perfectly synchronized are seldom satisfied. Therefore, there is a need to first adjust or align the time-resolved data before further analysis is carried out. Dynamic time warping (DTW) is considered as one of the common alignment techniques for time series data with equidistant time points. In this paper, we modified the DTW algorithm so that it can align sequences with measurements at different, non-equidistant time points with large gaps in between. This type of data is usually known as time-resolved data characterized by irregular time intervals between measurements as well as non-identical time points for different replicates. This new algorithm can be easily used to align time-resolved data from high-throughput experiments and to come across existing problems such as time scarcity and existing noise in the measurements. We propose a modified method of DTW to adapt requirements imposed by time-resolved data by use of monotone cubic interpolation splines. Our presented approach

Two dimensional numerical simulations of carrier dynamics during time-resolved photoluminescence decays in two-photon microscopy measurements in semiconductors

International Nuclear Information System (INIS)

Kanevce, Ana; Kuciauskas, Darius; Levi, Dean H.; Johnston, Steven W.; Allende Motz, Alyssa M.

2015-01-01

We use two-dimensional numerical simulations to analyze high spatial resolution time-resolved spectroscopy data. This analysis is applied to two-photon excitation time-resolved photoluminescence (2PE-TRPL) but is broadly applicable to all microscopic time-resolved techniques. By solving time-dependent drift-diffusion equations, we gain insight into carrier dynamics and transport characteristics. Accurate understanding of measurement results establishes the limits and potential of the measurement and enhances its value as a characterization method. Diffusion of carriers outside of the collection volume can have a significant impact on the measured decay but can also provide an estimate of carrier mobility as well as lifetime. In addition to material parameters, the experimental conditions, such as spot size and injection level, can impact the measurement results. Although small spot size provides better resolution, it also increases the impact of diffusion on the decay; if the spot size is much smaller than the diffusion length, it impacts the entire decay. By reproducing experimental 2PE-TRPL decays, the simulations determine the bulk carrier lifetime from the data. The analysis is applied to single-crystal and heteroepitaxial CdTe, material important for solar cells, but it is also applicable to other semiconductors where carrier diffusion from the excitation volume could affect experimental measurements

Highly doped semiconductor plasmonic nanoantenna arrays for polarization selective broadband surface-enhanced infrared absorption spectroscopy of vanillin

Science.gov (United States)

Barho, Franziska B.; Gonzalez-Posada, Fernando; Milla, Maria-Jose; Bomers, Mario; Cerutti, Laurent; Tournié, Eric; Taliercio, Thierry

2017-11-01

Tailored plasmonic nanoantennas are needed for diverse applications, among those sensing. Surface-enhanced infrared absorption (SEIRA) spectroscopy using adapted nanoantenna substrates is an efficient technique for the selective detection of molecules by their vibrational spectra, even in small quantity. Highly doped semiconductors have been proposed as innovative materials for plasmonics, especially for more flexibility concerning the targeted spectral range. Here, we report on rectangular-shaped, highly Si-doped InAsSb nanoantennas sustaining polarization switchable longitudinal and transverse plasmonic resonances in the mid-infrared. For small array periodicities, the highest reflectance intensity is obtained. Large periodicities can be used to combine localized surface plasmon resonances (SPR) with array resonances, as shown in electromagnetic calculations. The nanoantenna arrays can be efficiently used for broadband SEIRA spectroscopy, exploiting the spectral overlap between the large longitudinal or transverse plasmonic resonances and narrow infrared active absorption features of an analyte molecule. We demonstrate an increase of the vibrational line intensity up to a factor of 5.7 of infrared-active absorption features of vanillin in the fingerprint spectral region, yielding enhancement factors of three to four orders of magnitude. Moreover, an optimized readout for SPR sensing is proposed based on slightly overlapping longitudinal and transverse localized SPR.

Highly doped semiconductor plasmonic nanoantenna arrays for polarization selective broadband surface-enhanced infrared absorption spectroscopy of vanillin

Directory of Open Access Journals (Sweden)

Barho Franziska B.

2017-11-01

Full Text Available Tailored plasmonic nanoantennas are needed for diverse applications, among those sensing. Surface-enhanced infrared absorption (SEIRA spectroscopy using adapted nanoantenna substrates is an efficient technique for the selective detection of molecules by their vibrational spectra, even in small quantity. Highly doped semiconductors have been proposed as innovative materials for plasmonics, especially for more flexibility concerning the targeted spectral range. Here, we report on rectangular-shaped, highly Si-doped InAsSb nanoantennas sustaining polarization switchable longitudinal and transverse plasmonic resonances in the mid-infrared. For small array periodicities, the highest reflectance intensity is obtained. Large periodicities can be used to combine localized surface plasmon resonances (SPR with array resonances, as shown in electromagnetic calculations. The nanoantenna arrays can be efficiently used for broadband SEIRA spectroscopy, exploiting the spectral overlap between the large longitudinal or transverse plasmonic resonances and narrow infrared active absorption features of an analyte molecule. We demonstrate an increase of the vibrational line intensity up to a factor of 5.7 of infrared-active absorption features of vanillin in the fingerprint spectral region, yielding enhancement factors of three to four orders of magnitude. Moreover, an optimized readout for SPR sensing is proposed based on slightly overlapping longitudinal and transverse localized SPR.

Ultra-Broadband Two-Dimensional Electronic Spectroscopy and Pump-Probe Microscopy of Molecular Systems

Science.gov (United States)

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

Spectroscopy and reactions of vibrationally excited transient molecules

Energy Technology Data Exchange (ETDEWEB)

Dai, H.L. [Univ. of Pennsylvania, Philadelphia (United States)

1993-12-01

Spectroscopy, energy transfer and reactions of vibrationally excited transient molecules are studied through a combination of laser-based excitation techniques and efficient detection of emission from the energized molecules with frequency and time resolution. Specifically, a Time-resolved Fourier Transform Emission Spectroscopy technique has been developed for detecting dispersed laser-induced fluorescence in the IR, visible and UV regions. The structure and spectroscopy of the excited vibrational levels in the electronic ground state, as well as energy relaxation and reactions induced by specific vibronic excitations of a transient molecule can be characterized from time-resolved dispersed fluorescence in the visible and UV region. IR emissions from highly vibrational excited levels, on the other hand, reveal the pathways and rates of collision induced vibrational energy transfer.

Structure and function of proteins investigated by crystallographic and spectroscopic time-resolved methods

Science.gov (United States)

Purwar, Namrta

crystal. Time-resolved X-ray data collected at pH's of 4, 7 and 9 demonstrate that pH alters the kinetics of the PYP photocycle dramatically. At pH 4 the photocycle lasts almost one order of magnitude longer in time compared to pH 7. The final intermediate that accumulates at both pH 7 and pH 4 is absent at pH 9. Results from the dose- and the pH-dependent time-resolved crystallographic experiments show that it is imperative to carefully control the conditions under which time-resolved data are collected. With these considerations we collected a comprehensive time-series from nanoseconds to seconds at 14 different temperature settings from -40 °C to 70 °C. Results from time-resolved crystallography are corroborated by employing time-resolved absorption spectroscopy. For this, absorption spectra on crystals and solution are collected by a fast micro-spectrophotometer custom-designed in our lab. We identify kinetic phases of the PYP photocycle at all 14 temperature settings. Relaxation times associated with these phases are temperature-dependent and can be fit by the Van't Hoff-Arrhenius equation. Kinetic modeling yields entropy and enthalpy values at the barriers of the activation solely from the time-resolved crystallographic data. With this, we advance crystallography to a new frontier: the determination of free energy surfaces. Investigating enzymatic reactions can be challenging, because they are non-cyclic. After one turnover product must be washed away and substrate must be reloaded. A promising approach for routine application can be envisioned at the new 4th generation X-ray sources, such as X-ray free electron lasers (XFELs). With our results we set the scene to comprehensively investigate all kinds of enzymatic reactions with these instruments.

Time-resolved brightness measurements by streaking

Science.gov (United States)

Torrance, Joshua S.; Speirs, Rory W.; McCulloch, Andrew J.; Scholten, Robert E.

2018-03-01

Brightness is a key figure of merit for charged particle beams, and time-resolved brightness measurements can elucidate the processes involved in beam creation and manipulation. Here we report on a simple, robust, and widely applicable method for the measurement of beam brightness with temporal resolution by streaking one-dimensional pepperpots, and demonstrate the technique to characterize electron bunches produced from a cold-atom electron source. We demonstrate brightness measurements with 145 ps temporal resolution and a minimum resolvable emittance of 40 nm rad. This technique provides an efficient method of exploring source parameters and will prove useful for examining the efficacy of techniques to counter space-charge expansion, a critical hurdle to achieving single-shot imaging of atomic scale targets.

Multichannel, time-resolved picosecond laser ultrasound imaging and spectroscopy with custom complementary metal-oxide-semiconductor detector

International Nuclear Information System (INIS)

Smith, Richard J.; Light, Roger A.; Johnston, Nicholas S.; Pitter, Mark C.; Somekh, Mike G.; Sharples, Steve D.

2010-01-01

This paper presents a multichannel, time-resolved picosecond laser ultrasound system that uses a custom complementary metal-oxide-semiconductor linear array detector. This novel sensor allows parallel phase-sensitive detection of very low contrast modulated signals with performance in each channel comparable to that of a discrete photodiode and a lock-in amplifier. Application of the instrument is demonstrated by parallelizing spatial measurements to produce two-dimensional thickness maps on a layered sample, and spectroscopic parallelization is demonstrated by presenting the measured Brillouin oscillations from a gallium arsenide wafer. This paper demonstrates the significant advantages of our approach to pump probe systems, especially picosecond ultrasonics.

Multichannel, time-resolved picosecond laser ultrasound imaging and spectroscopy with custom complementary metal-oxide-semiconductor detector

Energy Technology Data Exchange (ETDEWEB)

Smith, Richard J.; Light, Roger A.; Johnston, Nicholas S.; Pitter, Mark C.; Somekh, Mike G. [Institute of Biophysics, Imaging and Optical Science, University of Nottingham, Nottinghamshire NG7 2RD (United Kingdom); Sharples, Steve D. [Applied Optics Group, Electrical Systems and Optics Research Division, University of Nottingham, Nottinghamshire NG7 2RD (United Kingdom)

2010-02-15

This paper presents a multichannel, time-resolved picosecond laser ultrasound system that uses a custom complementary metal-oxide-semiconductor linear array detector. This novel sensor allows parallel phase-sensitive detection of very low contrast modulated signals with performance in each channel comparable to that of a discrete photodiode and a lock-in amplifier. Application of the instrument is demonstrated by parallelizing spatial measurements to produce two-dimensional thickness maps on a layered sample, and spectroscopic parallelization is demonstrated by presenting the measured Brillouin oscillations from a gallium arsenide wafer. This paper demonstrates the significant advantages of our approach to pump probe systems, especially picosecond ultrasonics.

A split imaging spectrometer for temporally and spatially resolved titanium absorption spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Hager, J. D., E-mail: hager@lanl.gov; Lanier, N. E.; Kline, J. L.; Flippo, K. A. [Los Alamos National Laboratory, Los Alamos, New Mexico 87545 (United States); Bruns, H. C.; Schneider, M.; Saculla, M.; McCarville, T. [Lawrence Livermore National Laboratory, Livermore, California 94550 (United States)

2014-11-15

We present a temporally and a spatially resolved spectrometer for titanium x-ray absorption spectroscopy along 2 axial symmetric lines-of-sight. Each line-of-sight of the instrument uses an elliptical crystal to acquire both the 2p and 3p Ti absorption lines on a single, time gated channel of the instrument. The 2 axial symmetric lines-of-sight allow the 2p and 3p absorption features to be measured through the same point in space using both channels of the instrument. The spatially dependent material temperature can be inferred by observing the 2p and the 3p Ti absorption features. The data are recorded on a two strip framing camera with each strip collecting data from a single line-of-sight. The design is compatible for use at both the OMEGA laser and the National Ignition Facility. The spectrometer is intended to measure the material temperature behind a Marshak wave in a radiatively driven SiO{sub 2} foam with a Ti foam tracer. In this configuration, a broad band CsI backlighter will be used for a source and the Ti absorption spectrum measured.

Self-biased broadband magnet-free linear isolator based on one-way space-time coherency

Science.gov (United States)

Taravati, Sajjad

2017-12-01

This paper introduces a self-biased broadband magnet-free and linear isolator based on one-way space-time coherency. The incident wave and the space-time-modulated medium share the same temporal frequency and are hence temporally coherent. However, thanks to the unidirectionally of the space-time modulation, the space-time-modulated medium and the incident wave are spatially coherent only in the forward direction and not in the opposite direction. As a consequence, the energy of the medium strongly couples to the propagating wave in the forward direction, while it conflicts with the propagating wave in the opposite direction, yielding strong isolation. We first derive a closed-form solution for the wave scattering from a spatiotemporally coherent medium and then show that a perfectly coherent space-time-modulated medium provides a moderate isolation level which is also subject to one-way transmission gain. To overcome this issue, we next investigate the effect of space-coherency imperfection between the medium and the wave, while they are still perfectly temporally coherent. Leveraging the spatial-coherency imperfection, the medium exhibits a quasiarbitrary and strong nonreciprocal transmission. Finally, we present the experimental demonstration of the self-biased version of the proposed broadband isolator, exhibiting more than 122 % fractional operation bandwidth.

Towards atomically resolved EELS elemental and fine structure mapping via multi-frame and energy-offset correction spectroscopy.

Science.gov (United States)

Wang, Yi; Huang, Michael R S; Salzberger, Ute; Hahn, Kersten; Sigle, Wilfried; van Aken, Peter A

2018-01-01

Electron energy-loss spectroscopy and energy-dispersive X-ray spectroscopy are two of the most common means for chemical analysis in the scanning transmission electron microscope. The marked progress of the instrumentation hardware has made chemical analysis at atomic resolution readily possible nowadays. However, the acquisition and interpretation of atomically resolved spectra can still be problematic due to image distortions and poor signal-to-noise ratio of the spectra, especially for investigation of energy-loss near-edge fine structures. By combining multi-frame spectrum imaging and automatic energy-offset correction, we developed a spectrum imaging technique implemented into customized DigitalMicrograph scripts for suppressing image distortions and improving the signal-to-noise ratio. With practical examples, i.e. SrTiO 3 bulk material and Sr-doped La 2 CuO 4 superlattices, we demonstrate the improvement of elemental mapping and the EELS spectrum quality, which opens up new possibilities for atomically resolved EELS fine structure mapping. Copyright © 2017 The Authors. Published by Elsevier B.V. All rights reserved.

Binding and relaxation behavior of Coumarin-153 in lecithin-taurocholate mixed micelles: A time resolved fluorescence spectroscopic study

Science.gov (United States)

Chakrabarty, Debdeep; Chakraborty, Anjan; Seth, Debabrata; Hazra, Partha; Sarkar, Nilmoni

2005-09-01

The microenvironment of the bile salt-lecithin mixed aggregates has been investigated using steady state and picosecond time resolved fluorescence spectroscopy. The steady state spectra show that the polarity of the bile salt is higher compared to lecithin vesicles or the mixed aggregates. We have observed slow solvent relaxation in bile salt micelles and lecithin vesicles. The solvation time is gradually slowed down due to gradual addition of the bile salt in lecithin vesicles. Addition of bile salt leads to the tighter head group packing in lecithin. Thus, mobility of the water molecules becomes slower and consequently the solvation time is also retarded. We have observed bimodal slow rotational relaxation time in all these systems.

Time Resolved Deposition Measurements in NSTX

International Nuclear Information System (INIS)

Skinner, C.H.; Kugel, H.; Roquemore, A.L.; Hogan, J.; Wampler, W.R.

2004-01-01

Time-resolved measurements of deposition in current tokamaks are crucial to gain a predictive understanding of deposition with a view to mitigating tritium retention and deposition on diagnostic mirrors expected in next-step devices. Two quartz crystal microbalances have been installed on NSTX at a location 0.77m outside the last closed flux surface. This configuration mimics a typical diagnostic window or mirror. The deposits were analyzed ex-situ and found to be dominantly carbon, oxygen, and deuterium. A rear facing quartz crystal recorded deposition of lower sticking probability molecules at 10% of the rate of the front facing one. Time resolved measurements over a 4-week period with 497 discharges, recorded 29.2 (micro)g/cm 2 of deposition, however surprisingly, 15.9 (micro)g/cm 2 of material loss occurred at 7 discharges. The net deposited mass of 13.3 (micro)g/cm 2 matched the mass of 13.5 (micro)g/cm 2 measured independently by ion beam analysis. Monte Carlo modeling suggests that transient processes are likely to dominate the deposition

Femtosecond time-resolved hot carrier energy distributions of photoexcited semiconductor quantum dots

International Nuclear Information System (INIS)

Chuang, Chi-Hung; Burda, Clemens; Chen, Xiaobo

2013-01-01

Using femtosecond transient absorption spectroscopy, we investigated hot carrier distributions in semiconductor cadmium selenide quantum dots. The relaxation processes represent the behavior of an ensemble of QDs. This concept is applied for analysis with the Fermi-Dirac distribution and relaxation processes among different electron-hole pair states. By extracting the experimental hot carrier distribution and fitting with the Fermi-Dirac function, we resolved the rapid thermalization processes, such as carrier-carrier and carrier-phonon interactions was resolved within one picosecond upon photoexcitation. The analysis, using the Fermi-Dirac distribution modulated by the density of states, provides a general route to understanding the carrier cooling and heat dissipation processes in quantum dot-based systems. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Time-resolved biophysical approaches to nucleocytoplasmic transport

Directory of Open Access Journals (Sweden)

Francesco Cardarelli

Full Text Available Molecules are continuously shuttling across the nuclear envelope barrier that separates the nucleus from the cytoplasm. Instead of being just a barrier to diffusion, the nuclear envelope is rather a complex filter that provides eukaryotes with an elaborate spatiotemporal regulation of fundamental molecular processes, such as gene expression and protein translation. Given the highly dynamic nature of nucleocytoplasmic transport, during the past few decades large efforts were devoted to the development and application of time resolved, fluorescence-based, biophysical methods to capture the details of molecular motion across the nuclear envelope. These methods are here divided into three major classes, according to the differences in the way they report on the molecular process of nucleocytoplasmic transport. In detail, the first class encompasses those methods based on the perturbation of the fluorescence signal, also known as ensemble-averaging methods, which average the behavior of many molecules (across many pores. The second class comprises those methods based on the localization of single fluorescently-labelled molecules and tracking of their position in space and time, potentially across single pores. Finally, the third class encompasses methods based on the statistical analysis of spontaneous fluorescence fluctuations out of the equilibrium or stationary state of the system. In this case, the behavior of single molecules is probed in presence of many similarly-labelled molecules, without dwelling on any of them. Here these three classes, with their respective pros and cons as well as their main applications to nucleocytoplasmic shuttling will be briefly reviewed and discussed. Keywords: Fluorescence recovery after photobleaching, Single particle tracking, Fluorescence correlation spectroscopy, Diffusion, Transport, GFP, Nuclear pore complex, Live cell, Confocal microscopy

Direct UV-written broadband directional broadband planar waveguide couplers

DEFF Research Database (Denmark)

Olivero, Massimo; Svalgaard, Mikael

2005-01-01

We report the fabrication of broadband directional couplers by direct UV-writing. The fabrication process is shown to be beneficial, robust and flexible. The components are compact and show superior performance in terms of loss and broadband operation.......We report the fabrication of broadband directional couplers by direct UV-writing. The fabrication process is shown to be beneficial, robust and flexible. The components are compact and show superior performance in terms of loss and broadband operation....

Characterization of Microsolvated Crown Ethers from Broadband Rotational Spectroscopy

Science.gov (United States)

Perez, Cristobal; Schnell, Melanie; Blanco, Susana; Lopez, Juan Carlos

2016-06-01

Since they were first synthetized, crown ethers have been extensively used in organometallic chemistry due to their unparalleled binding selectivity with alkali metal cations. From a structural point of view, crown ethers are heterocycles containing oxygen and/or other heteroatoms, although the most common ones are formed from ethylene oxide unit. Crown ethers are conventionally seen as being hydrophilic inside and hydrophobic outside when the structures found for the metal cation complexes are considered. However, crown ethers are extremely flexible and in isolation may present a variety of stable conformations so that their structure may be easily adapted in presence of a strong ligand as an alkali metal cation minimize the energy of the resulting complex. Water can be considered a soft ligand which interacts with crown ethers through moderate hydrogen bonds. It is thus interesting to investigate which conformers are selected by water to form complexes, the preferred interaction sites and the possible conformational changes due to the presence of one or more water molecules. Previous studies identified microsolvated crown ethers but in all cases with a chromophore group attached to the structure. Here we present a broadband rotational spectroscopy study of microsolvated crown ethers produced in a pulsed molecular jet expansion. Several 1:1 and 1:2 crown ether:water aggregates are presented for 12-crown-4, 15-crown-5 and 18-crown-6. Unambiguous identification of the structures has been achieved using isotopic substitution within the water unit. The subtle changes induced in the structures of the crown ether monomer upon complexation and the hydrogen-bonding network that hold them together will be also discussed. F. Gámez, B. Martínez-Haya, S. Blanco,J. C. López and J. L. Alonso, Phys. Chem. Chem. Phys. 2014, 14 12912-12918 V. A. Shubert, C.W. Müller and T. Zwier, J. Phys. Chem. A 2009, 113 8067-8079

Time-resolved plasma spectroscopy of thin foils heated by a relativistic-intensity short-pulse laser

International Nuclear Information System (INIS)

Audebert, P.; Gauthier, J.-C.; Shepherd, R.; Fournier, K.B.; Price, D.; Lee, R.W.; Springer, P.; Peyrusse, O.; Klein, L.

2002-01-01

Time-resolved K-shell x-ray spectra are recorded from sub-100 nm aluminum foils irradiated by 150-fs laser pulses at relativistic intensities of Iλ 2 =2x10 18 W μm 2 /cm 2 . The thermal penetration depth is greater than the foil thickness in these targets so that uniform heating takes place at constant density before hydrodynamic motion occurs. The high-contrast, high-intensity laser pulse, broad spectral band, and short time resolution utilized in this experiment permit a simplified interpretation of the dynamical evolution of the radiating matter. The observed spectrum displays two distinct phases. At early time, ≤500 fs after detecting target emission, a broad quasicontinuous spectral feature with strong satellite emission from multiply excited levels is seen. At a later time, the He-like resonance line emission is dominant. The time-integrated data is in accord with previous studies with time resolution greater than 1 ps. The early time satellite emission is shown to be a signature of an initial large area, high density, low-temperature plasma created in the foil by fast electrons accelerated by the intense radiation field in the laser spot. We conclude that, because of this early time phenomenon and contrary to previous predictions, a short, high-intensity laser pulse incident on a thin foil does not create a uniform hot and dense plasma. The heating mechanism has been studied as a function of foil thickness, laser pulse length, and intensity. In addition, the spectra are found to be in broad agreement with a hydrodynamic expansion code postprocessed by a collisional-radiative model based on superconfiguration average rates and on the unresolved transition array formalism

The dependence of the ultrafast relaxation kinetics of the S2 and S1 states in β-carotene homologs and lycopene on conjugation length studied by femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies

Science.gov (United States)

Kosumi, Daisuke; Fujiwara, Masazumi; Fujii, Ritsuko; Cogdell, Richard J.; Hashimoto, Hideki; Yoshizawa, Masayuki

2009-06-01

The ultrafast relaxation kinetics of all-trans-β-carotene homologs with varying numbers of conjugated double bonds n(n =7-15) and lycopene (n =11) has been investigated using femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies, both carried out under identical excitation conditions. The nonradiative relaxation rates of the optically allowed S2(1Bu+1) state were precisely determined by the time-resolved fluorescence. The kinetics of the optically forbidden S1(2Ag-1) state were observed by the time-resolved absorption measurements. The dependence of the S1 relaxation rates upon the conjugation length is adequately described by application of the energy gap law. In contrast to this, the nonradiative relaxation rates of S2 have a minimum at n =9 and show a reverse energy gap law dependence for values of n above 11. This anomalous behavior of the S2 relaxation rates can be explained by the presence of an intermediate state (here called the Sx state) located between the S2 and S1 states at large values of n (such as n =11). The presence of such an intermediate state would then result in the following sequential relaxation pathway S2→Sx→S1→S0. A model based on conical intersections between the potential energy curves of these excited singlet states can readily explain the measured relationships between the decay rates and the energy gaps.

Structural differences in the two agonist binding sites of the Torpedo nicotinic acetylcholine receptor revealed by time-resolved fluorescence spectroscopy

DEFF Research Database (Denmark)

Martinez, K. L.; Corringer, P. J.; Edelstein, S. J.

2000-01-01

The nicotinic acetylcholine receptor (nAChR) from Torpedo marmorata carries two nonequivalent agonist binding sites at the αδ and αγ subunit interfaces. These sites have been characterized by time-resolved fluorescence with the partial nicotinic agonist dansyl-C6-choline (Dnscho). When bound...

X-ray Crystal Structure and Time-resolved Spectroscopy of the Blue Carotenoid Violerythrin

Czech Academy of Sciences Publication Activity Database

Polívka, Tomáš; Frank, H.A.; Enriquez, M.M.; Niedzwiedzki, D.M.; Liaaen-Jensen, S.; Hemming, J.; Helliwell, J.R.; Helliwell, M.

2010-01-01

Roč. 114, č. 26 (2010), s. 8760-8769 ISSN 1520-6106 Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoids * excited states * spectroscopy Subject RIV: BO - Biophysics Impact factor: 3.603, year: 2010

The development of angle-resolved photoelectron spectroscopy; 1900-1960

International Nuclear Information System (INIS)

Jenkin, J.G.; La Trobe Univ., Bundoora

1981-01-01

Angle-resolved photoelectron spectroscopy (ARPES) is now a sophisticated and particularly powerful technique for studying the electronic structure of matter, in addition the photoelectric effect has been of great significance in the history of 20th-century physics. This article seeks to uncover the origins and chart the development of the ARPES field, and focusses on the first half of this century; that is, up to the beginnings of the modern phase in the late 1960's. It is suggested that present workers will find interest in, and indeed profit from a knowledge of, the enormous experimental effort that was made to acquire quality data, the frustrating attempts that were initially made to understand them theoretically, and the contribution of early wave-mechanics, which brought order to a troubled field and thereby provided the necessary foundation for current studies. In addition, it is noted that the physicists involved often obtained inspiration and important insights which led them into studies of other significant problems of 20th-century physics. (orig.)

Laser ablation of an indium target: time-resolved Fourier-transform infrared spectra of In I in the 700–7700 cm−1 range

Czech Academy of Sciences Publication Activity Database

Civiš, Svatopluk; Kubelík, Petr; Ferus, Martin; Chernov, Vladislav E.; Zanozina, Ekaterina M.; Juha, Libor

2014-01-01

Roč. 29, č. 12 (2014), s. 2275-2283 ISSN 0267-9477 R&D Projects: GA MŠk LD14115; GA MŠk(CZ) LG13029 Institutional support: RVO:61388955 ; RVO:68378271 Keywords : time-resolved fluorescence * Fourier transform infra reds * Laser-induced breakdown spectroscopy Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.466, year: 2014

Time- and space-resolved spectroscopic characterization of laser-induced swine muscle tissue plasma

Energy Technology Data Exchange (ETDEWEB)

Camacho, J.J. [Departamento de Química-Física Aplicada, Facultad de Ciencias, Universidad Autónoma de Madrid, Cantoblanco, 28049 Madrid (Spain); Diaz, L., E-mail: luis.diaz@csic.es [Instituto de Estructura de la Materia, CFMAC, CSIC, Serrano 121, 28006 Madrid (Spain); Martinez-Ramirez, S. [Instituto de Estructura de la Materia, CFMAC, CSIC, Serrano 121, 28006 Madrid (Spain); Caceres, J.O. [Departamento de Química Analítica, Facultad de Ciencias Químicas, Universidad Complutense, Cuidad Universitaria, 28040 Madrid (Spain)

2015-09-01

The spatial-temporal evolution of muscle tissue sample plasma induced by a high-power transversely excited atmospheric (TEA) CO{sub 2} pulsed laser at vacuum conditions (0.1–0.01 Pa) has been investigated using high-resolution optical emission spectroscopy (OES) and imaging methods. The induced plasma shows mainly electronically excited neutral Na, K, C, Mg, H, Ca, N and O atoms, ionized C{sup +}, C{sup 2+}, C{sup 3+}, Mg{sup +}, Mg{sup 2+}, N{sup +}, N{sup 2+}, Ca{sup +}, O{sup +} and O{sup 2+} species and molecular band systems of CN(B{sup 2}Σ{sup +}–X{sup 2}Σ{sup +}), C{sub 2}(d{sup 3}Π{sub g}–a{sup 3}Π{sub u}), CH(B{sup 2}Σ{sup −}–X{sup 2}Π; A{sup 2}Δ–X{sup 2}Π), NH(A{sup 3}Π–X{sup 3}Σ{sup −}), OH(A{sup 2}Σ{sup +}–X{sup 2} Σ{sup +}), and CaOH(B{sup 2}Σ{sup +}–X{sup 2}Σ{sup +}; A{sup 2}Π–X{sup 2}Σ{sup +}). Time-resolved two-dimensional emission spectroscopy is used to study the expanded distribution of different species ejected during ablation. Spatial and temporal variations of different atoms and ionic excited species are reported. Plasma parameters such as electron density and temperature were measured from the spatio-temporal analysis of different species. Average velocities of some plasma species were estimated. - Highlights: • LIBS of swine muscle tissue sample generated by CO{sub 2} laser pulses has been done for the first time. • Average velocities of some plasma species have been calculated from spatial and temporally resolved 2D OES images. • Electron density (~ 9 × 10{sup 17} cm{sup -3}) has been studied with spatial and temporal resolution. • Temporal evolution of the plasma temperature has been calculated by means of Boltzmann plots.

Imaging buried organic islands by spatially resolved ballistic electron emission spectroscopy

International Nuclear Information System (INIS)

Goh, Kuan Eng J; Bannani, A; Troadec, C

2008-01-01

The well-known Au/n-Si(111) Schottky interface is modified by a discontinuous pentacene film (∼1.5 nm thick) and studied using spatially resolved ballistic electron emission spectroscopy (BEES). The pentacene film introduced subtle changes to the interface which cannot be definitively detected by current-voltage measurements or a standard BEES analysis of the barrier height. In contrast, analyzing the BEES results in a dual-parameter (transmission attenuation and barrier height) space allows the effect of the pentacene film on the Au/n-Si(111) interface to be clearly demonstrated. We found that the pentacene film behaves like a tunneling barrier and increases the distribution of local barrier heights with a tendency toward lower values. Our results highlight the potential of the dual-parameter BEES analysis for understanding local interface modification by molecules.

Timepix3 as X-ray detector for time resolved synchrotron experiments

Energy Technology Data Exchange (ETDEWEB)

Yousef, Hazem, E-mail: hazem.yousef@diamond.ac.uk; Crevatin, Giulio; Gimenez, Eva N.; Horswell, Ian; Omar, David; Tartoni, Nicola

2017-02-11

The Timepix3 ASIC can be used very effectively for time resolved experiments at synchrotron facilities. We have carried out characterizations with the synchrotron beam in order to determine the time resolution and other characteristics such as the energy resolution, charge sharing and signals overlapping. The best time resolution achieved is 19 ns FWHM for 12 keV photons and 350 V bias voltage. The time resolution shows dependency on the photon energy as well as on the chip and acquisition parameters. - Highlights: • An estimate time resolution of the Timepix3 is produced based on the arrival time. • At high resolution, the time structure of the DLS synchrotron beam is resolved. • The arrival time information improves combining the charge split events. • The results enable performing a wide range of time resolved experiments.

Timepix3 as X-ray detector for time resolved synchrotron experiments

International Nuclear Information System (INIS)

Yousef, Hazem; Crevatin, Giulio; Gimenez, Eva N.; Horswell, Ian; Omar, David; Tartoni, Nicola

2017-01-01

The Timepix3 ASIC can be used very effectively for time resolved experiments at synchrotron facilities. We have carried out characterizations with the synchrotron beam in order to determine the time resolution and other characteristics such as the energy resolution, charge sharing and signals overlapping. The best time resolution achieved is 19 ns FWHM for 12 keV photons and 350 V bias voltage. The time resolution shows dependency on the photon energy as well as on the chip and acquisition parameters. - Highlights: • An estimate time resolution of the Timepix3 is produced based on the arrival time. • At high resolution, the time structure of the DLS synchrotron beam is resolved. • The arrival time information improves combining the charge split events. • The results enable performing a wide range of time resolved experiments.

Ultrafast time-resolved absorption spectroscopy of geometric isomers of xanthophylls

Science.gov (United States)

Niedzwiedzki, Dariusz M.; Enriquez, Miriam M.; LaFountain, Amy M.; Frank, Harry A.

2010-07-01

This paper presents an ultrafast optical spectroscopic investigation of the excited state energies, lifetimes and spectra of specific geometric isomers of neoxanthin, violaxanthin, lutein, and zeaxanthin. All- trans- and 15,15'- cis-β-carotene were also examined. The spectroscopy was done on molecules purified by HPLC frozen immediately to inhibit isomerization. The spectra were taken at 77 K to maintain the configurations and to provide better spectral resolution than seen at room temperature. The kinetics reveal that for all of the molecules except neoxanthin, the S 1 state lifetime of the cis isomers is shorter than that of the all- trans isomers. The S 1 excited state energies of all the isomers were determined by recording S 1 → S 2 transient absorption spectra. The results obtained in this manner at cryogenic temperatures provide an unprecedented level of precision in the measurement of the S 1 energies of these xanthophylls, which are critical components in light-harvesting pigment-protein complexes of green plants.

Time-resolved photoluminescence study of CdSe/CdMnS/CdS core/multi-shell nanoplatelets

International Nuclear Information System (INIS)

Murphy, J. R.; Delikanli, S.; Demir, H. V.; Scrace, T.; Zhang, P.; Norden, T.; Petrou, A.; Thomay, T.; Cartwright, A. N.

2016-01-01

We used photoluminescence spectroscopy to resolve two emission features in CdSe/CdMnS/CdS and CdSe/CdS core/multi-shell nanoplatelet heterostructures. The photoluminescence from the magnetic sample has a positive circular polarization with a maximum centered at the position of the lower energy feature. The higher energy feature has a corresponding signature in the absorption spectrum; this is not the case for the low-energy feature. We have also studied the temporal evolution of these features using a pulsed-excitation/time-resolved photoluminescence technique to investigate their corresponding recombination channels. A model was used to analyze the temporal dynamics of the photoluminescence which yielded two distinct timescales associated with these recombination channels. The above results indicate that the low-energy feature is associated with recombination of electrons with holes localized at the core/shell interfaces; the high-energy feature, on the other hand, is excitonic in nature with the holes confined within the CdSe cores.

Time-resolved photoluminescence study of CdSe/CdMnS/CdS core/multi-shell nanoplatelets

Energy Technology Data Exchange (ETDEWEB)

Murphy, J. R. [Department of Electrical Engineering, State University of New York, University at Buffalo, Buffalo, New York 14260 (United States); Department of Physics, State University of New York, University at Buffalo, Buffalo, New York 14260 (United States); Delikanli, S.; Demir, H. V., E-mail: volkan@bilkent.edu.tr [LUMINOUS Center of Excellence for Semiconductor Lighting and Displays, School of Electrical and Electronic Engineering, School of Physical and Materials Sciences, Nanyang Technological University, Singapore 639798 (Singapore); Department of Electrical and Electronics Engineering, Department of Physics, UNAM−Institute of Materials Science and Nanotechnology, Bilkent University, Ankara 06800 (Turkey); Scrace, T.; Zhang, P.; Norden, T.; Petrou, A., E-mail: petrou@buffalo.edu [Department of Physics, State University of New York, University at Buffalo, Buffalo, New York 14260 (United States); Thomay, T.; Cartwright, A. N. [Department of Electrical Engineering, State University of New York, University at Buffalo, Buffalo, New York 14260 (United States)

2016-06-13

We used photoluminescence spectroscopy to resolve two emission features in CdSe/CdMnS/CdS and CdSe/CdS core/multi-shell nanoplatelet heterostructures. The photoluminescence from the magnetic sample has a positive circular polarization with a maximum centered at the position of the lower energy feature. The higher energy feature has a corresponding signature in the absorption spectrum; this is not the case for the low-energy feature. We have also studied the temporal evolution of these features using a pulsed-excitation/time-resolved photoluminescence technique to investigate their corresponding recombination channels. A model was used to analyze the temporal dynamics of the photoluminescence which yielded two distinct timescales associated with these recombination channels. The above results indicate that the low-energy feature is associated with recombination of electrons with holes localized at the core/shell interfaces; the high-energy feature, on the other hand, is excitonic in nature with the holes confined within the CdSe cores.

Quantum state-resolved gas/surface reaction dynamics probed by reflection absorption infrared spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Chen Li [Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, Goettingen (Germany); Ueta, Hirokazu; Beck, Rainer D. [Laboratoire de Chimie Physique Moleculaire, Ecole Polytechnique Federale de Lausanne (Switzerland); Bisson, Regis [Aix-Marseille Universite, PIIM, CNRS, UMR 7345, 13397 Marseille (France)

2013-05-15

We report the design and characterization of a new molecular-beam/surface-science apparatus for quantum state-resolved studies of gas/surface reaction dynamics combining optical state-specific reactant preparation in a molecular beam by rapid adiabatic passage with detection of surface-bound reaction products by reflection absorption infrared spectroscopy (RAIRS). RAIRS is a non-invasive infrared spectroscopic detection technique that enables online monitoring of the buildup of reaction products on the target surface during reactant deposition by a molecular beam. The product uptake rate obtained by calibrated RAIRS detection yields the coverage dependent state-resolved reaction probability S({theta}). Furthermore, the infrared absorption spectra of the adsorbed products obtained by the RAIRS technique provide structural information, which help to identify nascent reaction products, investigate reaction pathways, and determine branching ratios for different pathways of a chemisorption reaction. Measurements of the dissociative chemisorption of methane on Pt(111) with this new apparatus are presented to illustrate the utility of RAIRS detection for highly detailed studies of chemical reactions at the gas/surface interface.

Fast time-resolved aerosol collector: proof of concept

Science.gov (United States)

Yu, X.-Y.; Cowin, J. P.; Iedema, M. J.; Ali, H.

2010-10-01

Atmospheric particles can be collected in the field on substrates for subsequent laboratory analysis via chemically sensitive single particle methods such as scanning electron microscopy with energy dispersive x-ray analysis. With moving substrates time resolution of seconds to minutes can be achieved. In this paper, we demonstrate how to increase the time resolution when collecting particles on a substrate to a few milliseconds to provide real-time information. Our fast time-resolved aerosol collector ("Fast-TRAC") microscopically observes the particle collection on a substrate and records an on-line video. Particle arrivals are resolved to within a single frame (4-17 ms in this setup), and the spatial locations are matched to the subsequent single particle analysis. This approach also provides in-situ information on particle size and number concentration. Applications are expected in airborne studies of cloud microstructure, pollution plumes, and surface long-term monitoring.

Time-resolved measurements of luminescence

Energy Technology Data Exchange (ETDEWEB)

Collier, Bradley B. [Department of Biomedical Engineering, 408 Mechanical Engineering Office Building, Spence Street, Texas A and M University, College Station, TX 77843 (United States); McShane, Michael J., E-mail: mcshane@tamu.edu [Department of Biomedical Engineering, 408 Mechanical Engineering Office Building, Spence Street, Texas A and M University, College Station, TX 77843 (United States); Materials Science and Engineering Program, 408 Mechanical Engineering Office Building, Spence Street, Texas A and M University, College Station, TX 77843 (United States)

2013-12-15

Luminescence sensing and imaging has become more widespread in recent years in a variety of industries including the biomedical and environmental fields. Measurements of luminescence lifetime hold inherent advantages over intensity-based response measurements, and advances in both technology and methods have enabled their use in a broader spectrum of applications including real-time medical diagnostics. This review will focus on recent advances in analytical methods, particularly calculation techniques, including time- and frequency-domain lifetime approaches as well as other time-resolved measurements of luminescence. -- Highlights: • Developments in technology have led to widespread use of luminescence lifetime. • Growing interest for sensing and imaging applications. • Recent advances in approaches to lifetime calculations are reviewed. • Advantages and disadvantages of various methods are weighed. • Other methods for measurement of luminescence lifetime also described.

Time-resolved measurements of luminescence

International Nuclear Information System (INIS)

Collier, Bradley B.; McShane, Michael J.

2013-01-01

Luminescence sensing and imaging has become more widespread in recent years in a variety of industries including the biomedical and environmental fields. Measurements of luminescence lifetime hold inherent advantages over intensity-based response measurements, and advances in both technology and methods have enabled their use in a broader spectrum of applications including real-time medical diagnostics. This review will focus on recent advances in analytical methods, particularly calculation techniques, including time- and frequency-domain lifetime approaches as well as other time-resolved measurements of luminescence. -- Highlights: • Developments in technology have led to widespread use of luminescence lifetime. • Growing interest for sensing and imaging applications. • Recent advances in approaches to lifetime calculations are reviewed. • Advantages and disadvantages of various methods are weighed. • Other methods for measurement of luminescence lifetime also described

GHz Yb:KYW oscillators in time-resolved spectroscopy

Science.gov (United States)

Li, Changxiu; Krauß, Nico; Schäfer, Gerhard; Ebner, Lukas; Kliebisch, Oliver; Schmidt, Johannes; Winnerl, Stephan; Hettich, Mike; Dekorsy, Thomas

2018-02-01

A high-speed asynchronous optical sampling system (ASOPS) based on Yb:KYW oscillators with 1-GHz repetition rate is reported. Two frequency-offset-stabilized diode-pumped Yb:KYW oscillators are employed as pump and probe source, respectively. The temporal resolution of this system within 1-ns time window is limited to 500 fs and the noise floor around 10-6 (ΔR/R) close to the shot-noise level is obtained within an acquisition time of a few seconds. Coherent acoustic phonons are investigated by measuring multilayer semiconductor structures with multiple quantum wells and aluminum/silicon membranes in this ASOPS system. A wavepacket-like phonon sequence at 360 GHz range is detected in the semiconductor structures and a decaying sequence of acoustic oscillations up to 200 GHz is obtained in the aluminum/silicon membranes. Coherent acoustic phonons generated from semiconductor structures are further manipulated by a double pump scheme through pump time delay control.

Effects of aging on working memory performance and prefrontal cortex activity: A time-resolved spectroscopy study

Institute of Scientific and Technical Information of China (English)

Jie Shi; Wenjing Zhou; Tongchao Geng; Huancong Zuo; Masahiro Tanida; Kaoru Sakatani

2016-01-01

Objective:This study aimed to employ time‐resolved spectroscopy(TRS)to explore age‐related differences in prefrontal cortex(PFC)activity while subjects performed a working memory task.Methods:We employed TRS to measure PFC activity in ten healthy younger and ten healthy older subjects while they performed a working memory(WM)task.All subjects performed the Sternberg test(ST)in which the memory‐set size varied between one and six digits.Using TRS,we recorded changes in cerebral blood oxygenation as a measure of changes in PFC activity during the task.In order to identify left/right asymmetry of PFC activity during the working memory task,we calculated the laterality score,i.e.,Δoxy‐Hb(rightΔoxy‐Hb—leftΔoxy‐Hb);positive values indicate greater activity in the right PFC,while negative values indicate greater activity in the left PFC.Results:During the ST,statistical analyses showed no significant differences between the younger and older groups in accuracy for low memory‐load and high memory‐load.In high memory‐load tasks,however,older subjects were slower than younger subjects(P<0.05).We found that the younger group showed right lateral responses with a stronger right than left activation in the frontal pole,whereas the older group showed bilateral responses(P<0.05).Conclusions:The present results are consistent with the hemispheric asymmetry reduction in older adults(HAROLD)model;working memory tasks cause asymmetrical PFC activation in younger adults,while older adults tend to show reduced hemispheric lateralization.

Time-Resolved Small-Angle X-Ray Scattering

NARCIS (Netherlands)

ten Elshof, Johan E.; Besselink, R.; Stawski, Tomasz; Castricum, H.L.; Levy, D.; Zayat, M.

2015-01-01

This chapter focuses on time-resolved studies of nanostructure development in sol-gel liquids, that is, diluted sols, wet gels, and drying thin fffilms. The most commonly investigated classes of sol-gel materials are silica, organically modified silica, template-directed mesostructured silica,

Multi-frame pyramid correlation for time-resolved PIV

NARCIS (Netherlands)

Sciacchitano, A.; Scarano, F.; Wieneke, B.

2012-01-01

A novel technique is introduced to increase the precision and robustness of time-resolved particle image velocimetry (TR-PIV) measurements. The innovative element of the technique is the linear combination of the correlation signal computed at different separation time intervals. The domain of the

Spatially Resolved Imaging and Spectroscopy of Candidate Dual Active Galactic Nuclei

Science.gov (United States)

McGurk, R. C.; Max, C. E.; Medling, A. M.; Shields, G. A.; Comerford, J. M.

2015-09-01

When galaxies merge, both central supermassive black holes are immersed in a dense and chaotic environment. If there is sufficient gas in the nuclear regions, one expects to see close pairs of active galactic nuclei (AGNs), or dual AGNs, in a fraction of galaxy mergers. However, finding them remains a challenge. The presence of double-peaked [O iii] emission lines has been proposed as a technique to select dual AGNs efficiently. We studied a sample of double-peaked narrow [O iii] emitting AGNs from Sloan Digital Sky Survey (SDSS) DR7. By obtaining new and archival high spatial resolution images taken with the Keck II Laser Guide Star Adaptive Optics system and the near-infrared camera NIRC2, we show that 30% of 140 double-peaked [O iii] emission line SDSS AGNs have two spatial components within a 3″ radius. However, spatially resolved spectroscopy or X-ray observations are needed to confirm these galaxy pairs as systems containing two AGNs. We followed up three spatially double candidate dual AGNs with integral field spectroscopy from Keck OSIRIS and 10 candidates with long-slit spectroscopy from the Shane Kast Double Spectrograph at Lick Observatory. We find that the double-peaked emission lines in our sample of 12 candidates are caused by: one dual AGN (SDSS J114642.47+511029.6), one confirmed outflow and four likely outflows, two pairs of star-forming galaxies, one candidate indeterminate due to sky line interference, and three AGNs with spatially coincident double [O iii] peaks, likely due to unresolved complex narrow line kinematics, outflows, binary AGN, or small-scale jets.

SPATIALLY RESOLVED IMAGING AND SPECTROSCOPY OF CANDIDATE DUAL ACTIVE GALACTIC NUCLEI

Energy Technology Data Exchange (ETDEWEB)

McGurk, R. C.; Max, C. E. [Astronomy Department and UCO-Lick Observatory, University of California, Santa Cruz, CA 95064 (United States); Medling, A. M. [Research School of Astronomy and Astrophysics, Australian National University, Mount Stromlo Observatory, Cotter Road, Weston Creek, ACT 2611 (Australia); Shields, G. A. [Laguna Falls Institute for Astrophysics, Austin, TX 78746 (United States); Comerford, J. M., E-mail: rosalie.mcgurk@gmail.com, E-mail: max@ucolick.org, E-mail: anne.medling@anu.edu.au, E-mail: shields@lfastro.org, E-mail: julie.comerford@colorado.edu [Department of Astrophysical and Planetary Sciences, University of Colorado, Boulder, CO 80309 (United States)

2015-09-20

When galaxies merge, both central supermassive black holes are immersed in a dense and chaotic environment. If there is sufficient gas in the nuclear regions, one expects to see close pairs of active galactic nuclei (AGNs), or dual AGNs, in a fraction of galaxy mergers. However, finding them remains a challenge. The presence of double-peaked [O iii] emission lines has been proposed as a technique to select dual AGNs efficiently. We studied a sample of double-peaked narrow [O iii] emitting AGNs from Sloan Digital Sky Survey (SDSS) DR7. By obtaining new and archival high spatial resolution images taken with the Keck II Laser Guide Star Adaptive Optics system and the near-infrared camera NIRC2, we show that 30% of 140 double-peaked [O iii] emission line SDSS AGNs have two spatial components within a 3″ radius. However, spatially resolved spectroscopy or X-ray observations are needed to confirm these galaxy pairs as systems containing two AGNs. We followed up three spatially double candidate dual AGNs with integral field spectroscopy from Keck OSIRIS and 10 candidates with long-slit spectroscopy from the Shane Kast Double Spectrograph at Lick Observatory. We find that the double-peaked emission lines in our sample of 12 candidates are caused by: one dual AGN (SDSS J114642.47+511029.6), one confirmed outflow and four likely outflows, two pairs of star-forming galaxies, one candidate indeterminate due to sky line interference, and three AGNs with spatially coincident double [O iii] peaks, likely due to unresolved complex narrow line kinematics, outflows, binary AGN, or small-scale jets.

SPATIALLY RESOLVED IMAGING AND SPECTROSCOPY OF CANDIDATE DUAL ACTIVE GALACTIC NUCLEI

International Nuclear Information System (INIS)

McGurk, R. C.; Max, C. E.; Medling, A. M.; Shields, G. A.; Comerford, J. M.

2015-01-01

When galaxies merge, both central supermassive black holes are immersed in a dense and chaotic environment. If there is sufficient gas in the nuclear regions, one expects to see close pairs of active galactic nuclei (AGNs), or dual AGNs, in a fraction of galaxy mergers. However, finding them remains a challenge. The presence of double-peaked [O iii] emission lines has been proposed as a technique to select dual AGNs efficiently. We studied a sample of double-peaked narrow [O iii] emitting AGNs from Sloan Digital Sky Survey (SDSS) DR7. By obtaining new and archival high spatial resolution images taken with the Keck II Laser Guide Star Adaptive Optics system and the near-infrared camera NIRC2, we show that 30% of 140 double-peaked [O iii] emission line SDSS AGNs have two spatial components within a 3″ radius. However, spatially resolved spectroscopy or X-ray observations are needed to confirm these galaxy pairs as systems containing two AGNs. We followed up three spatially double candidate dual AGNs with integral field spectroscopy from Keck OSIRIS and 10 candidates with long-slit spectroscopy from the Shane Kast Double Spectrograph at Lick Observatory. We find that the double-peaked emission lines in our sample of 12 candidates are caused by: one dual AGN (SDSS J114642.47+511029.6), one confirmed outflow and four likely outflows, two pairs of star-forming galaxies, one candidate indeterminate due to sky line interference, and three AGNs with spatially coincident double [O iii] peaks, likely due to unresolved complex narrow line kinematics, outflows, binary AGN, or small-scale jets

Time-Resolved Hard X-Ray Spectrometer

International Nuclear Information System (INIS)

Kenneth Moya; Ian McKennaa; Thomas Keenana; Michael Cuneob

2007-01-01

Wired array studies are being conducted at the SNL Z accelerator to maximize the x-ray generation for inertial confinement fusion targets and high energy density physics experiments. An integral component of these studies is the characterization of the time-resolved spectral content of the x-rays. Due to potential spatial anisotropy in the emitted radiation, it is also critical to diagnose the time-evolved spectral content in a space-resolved manner. To accomplish these two measurement goals, we developed an x-ray spectrometer using a set of high-speed detectors (silicon PIN diodes) with a collimated field-of-view that converged on a 1-cm-diameter spot at the pinch axis. Spectral discrimination is achieved by placing high Z absorbers in front of these detectors. We built two spectrometers to permit simultaneous different angular views of the emitted radiation. Spectral data have been acquired from recent Z shots for the radial and polar views. UNSPEC1 has been adapted to analyze and unfold the measured data to reconstruct the x-ray spectrum. The unfold operator code, UFO2, is being adapted for a more comprehensive spectral unfolding treatment

Resonance Raman Spectroscopy of Free Radicals Produced by Ionizing Radiation

DEFF Research Database (Denmark)

Wilbrandt, Robert Walter

1984-01-01

Applications of time-resolved resonance Raman spectroscopy to the study of short-lived free radicals produced by ionizing radiation are briefly reviewed. Potential advantages and limitations of this technique are discussed in the light of given examples. The reduction of p-nitrobenzylchloride and......Applications of time-resolved resonance Raman spectroscopy to the study of short-lived free radicals produced by ionizing radiation are briefly reviewed. Potential advantages and limitations of this technique are discussed in the light of given examples. The reduction of p......-nitrobenzylchloride and subsequent formation of the p-nitrobenzyl radical and the reaction of p-nitrotoluene with O– are studied by resonance Raman and optical absorption spectroscopy....

Time-resolved pump-probe experiments at the LCLS

Energy Technology Data Exchange (ETDEWEB)

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

2011-08-12

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

Tunable Reflective Spatial Heterodyne Spectrometer: A Technique for High Resolving Power, Wide Field Of View Observation Of Diffuse Emission Line Sources

Science.gov (United States)

Hosseini, Seyedeh Sona

The purpose of this dissertation is to discuss the need for new technology in broadband high-resolution spectroscopy based on the emerging technique of Spatial Heterodyne Spectroscopy (SHS) and to propose new solutions that should enhance and generalize this technology to other fields. Spectroscopy is a proven tool for determining compositional and other properties of remote objects. Narrow band imaging and low resolving spectroscopic measurements provide information about composition, photochemical evolution, energy distribution and density. The extension to high resolving power provides further access to temperature, velocity, isotopic ratios, separation of blended sources, and opacity effects. In current high resolving power devices, the drawback of high-resolution spectroscopy is bound to the instrumental limitations of lower throughput, the necessity of small entrance apertures, sensitivity, field of view, and large physical instrumental size. These limitations quickly become handicapping for observation of faint and/or extended targets and for spacecraft encounters. A technique with promise for the study of faint and extended sources at high resolving power is the reflective format of the Spatial Heterodyne Spectrometer (SHS). SHS instruments are compact and naturally tailored for both high etendue (defined in section 2.2.5) and high resolving power. In contrast, to achieve similar spectral grasp, grating spectrometers require large telescopes. For reference, SHS is a cyclical interferometer that produces Fizeau fringe pattern for all other wavelengths except the tuned wavelength. The large etendue obtained by SHS instruments makes them ideal for observations of extended, low surface brightness, isolated emission line sources, while their intrinsically high spectral resolution enables one to study the dynamical and physical properties described above. This document contains four chapters. Chapter 1, introduces a class of scientific targets that formerly have

Lifetime measurements of odd-parity high-excitation levels of Sn I by time-resolved laser spectroscopy

International Nuclear Information System (INIS)

Zhang, Wei; Feng, Yanyan; Xu, Jiaxin; Dai, Zhenwen; Palmeri, Patrick; Quinet, Pascal; Biemont, Emile

2010-01-01

Natural radiative lifetimes of 38 odd-parity highly excited levels in neutral tin in the energy range from 43 682.737 to 56 838.68 cm -1 have been measured by a time-resolved laser-induced fluorescence technique in an atomic beam produced by laser ablation on a solid tin sample. All the levels were excited from the metastable 3 P 1, 2 and 1 D 2 levels in the ground configuration. The second and third harmonics of a dye laser were adopted as the tunable exciting source (207-250 nm). The lifetime results obtained in this paper are in the range from 4.6 to 292 ns and will be useful in extending the set of oscillator strengths available in Sn I.

Spatially-resolved measurement of optically stimulated luminescence and time-resolved luminescence

International Nuclear Information System (INIS)

Bailiff, I.K.; Mikhailik, V.B.

2003-01-01

Spatially-resolved measurements of optically stimulated luminescence (OSL) were performed using a two-dimensional scanning system designed for use with planar samples. The scanning system employs a focused laser beam to stimulate a selected area of the sample, which is moved under the beam by a motorised stage. Exposure of the sample is controlled by an electronic shutter. Mapping of the distribution of OSL using a continuous wave laser source was obtained with sub-millimeter resolution for samples of sliced brick, synthetic single crystal quartz, concrete and dental ceramic. These revealed sporadic emission in the case of brick or concrete and significant spatial variation of emission for quartz and dental ceramic slices. Determinations of absorbed dose were performed for quartz grains within a slice of modern brick. Reconfiguration of the scanner with a pulsed laser source enabled quartz and feldspathic minerals within a ceramic sample to be thinner region. about 6 nm from the extrapolation of themeasuring the time-resolved luminescence spectrum

Spatially resolved acoustic spectroscopy for rapid imaging of material microstructure and grain orientation

International Nuclear Information System (INIS)

Smith, Richard J; Li, Wenqi; Coulson, Jethro; Clark, Matt; Somekh, Michael G; Sharples, Steve D

2014-01-01

Measuring the grain structure of aerospace materials is very important to understand their mechanical properties and in-service performance. Spatially resolved acoustic spectroscopy is an acoustic technique utilizing surface acoustic waves to map the grain structure of a material. When combined with measurements in multiple acoustic propagation directions, the grain orientation can be obtained by fitting the velocity surface to a model. The new instrument presented here can take thousands of acoustic velocity measurements per second. The spatial and velocity resolution can be adjusted by simple modification to the system; this is discussed in detail by comparison of theoretical expectations with experimental data. (paper)

Applications of Cr:ZnSe and Cr:ZnS lasers to ultrabroadband high-resolution spectroscopy

International Nuclear Information System (INIS)

Sorokin, E.; Sorokina, I.; Picque, N.; Guelachvili, G.

2006-01-01

Full text: Cr 2+ :ZnSe laser, and since recently also the Cr 2+ :ZnS laser proved to be versatile laser sources for trace gas measurements in the whole range between 2 and 3.1 μm. Among the existing methods of sensitive gas detection, intracavity laser absorption spectroscopy (ICLAS) offers some distinct advantages such as the simultaneous coverage of a broad spectral domain and large dynamic range. Under ICLAS the absorbing medium is put inside a laser cavity with broadband gain. As a result, the laser cavity acts as a multipass cell. Equivalent absorption path length of tens of kilometers can be achieved, corresponding to high detection sensitivities of the order of 10 -8 cm -1 and better. Only few examples of ICLAS spectrometers were demonstrated beyond 2 μm. Among them are: KCl:Li Fa(II) color center laser with coverage up to 4 nm at 2638 nm, Co:MgF 2 , covering up to 30 nm around 2040 and 2245 nm, Tm:YAG with coverage up to 35 nm at 2030 nm, and pulsed Cr:ZnSe, with coverage up to 50 nmat 2500 nm. In this talk we discuss application of a Cr 2+ :ZnSe laser to high-resolution and high-sensitivity intracavity absorption spectroscopy (ICLAS) analyzed by time-resolved Fourier transform spectroscopy. This represents the extreme limit presently reached in the infrared by ICLAS with Doppler limited resolution. Our most recent works concern application of a Cr 2+ :ZnS laser for broadband ultrasensitive intracavity laser spectroscopy (ICLAS), with effective absorption path up to about 50 km in the 2.4 μm range. The spectrometer operates with both Er-fiber and direct diode pumping in the very interesting water-free window between ∼ 2.1 and 2.5 μm. The sensitivity of 2 x 10 -9 cm -1 at Doppler-limited resolution allows obtaining spectral information that was previously unreachable in laboratory conditions. Summarizing, intracavity laser spectroscopy technique has been successfully used for measuring and detecting gas constituents with extreme sensitivity and

Magnetization pinning in conducting films demonstrated using broadband ferromagnetic resonance

Science.gov (United States)

Kostylev, M.; Stashkevich, A. A.; Adeyeye, A. O.; Shakespeare, C.; Kostylev, N.; Ross, N.; Kennewell, K.; Magaraggia, R.; Roussigné, Y.; Stamps, R. L.

2010-11-01

The broadband microstrip ferromagnetic resonance (FMR), cavity FMR, and Brillouin light scattering spectroscopy techniques have been applied for detection and characterization of a magnetic inhomogeneity in a film sample. In the case of a 100 nm thick permalloy film, an additional magnetically depleted top sublayer has been detected due to pinning effect it produces on the magnetization in the bulk of the film. The pinning results in appearance of an exchange standing spin wave mode in the broadband FMR absorption spectrum, whose amplitudes are different depending on whether the film or the film substrate faces the microstrip transducer. Comparison of the experimental amplitudes for this mode with results of our theory for both film placements revealed that the depleted layer is located at the film surface facing away from the film substrate. Subsequent broadband FMR characterization of a large number of other presumably single-layer films with thicknesses in the range 30-100 nm showed the same result.

Adoption of Broadband Services

DEFF Research Database (Denmark)

Falch, Morten

2008-01-01

Broadband is seen as a key infrastructure for developing the information society. For this reason many Governments are actively engaged in stimulating investments in broadband infrastructures and use of broadband services. This chapter compares a wide range of broadband strategies in the most suc....... Many countries have provided active support for stimulating diffusion of broadband and national variants of this type of policies in different countries are important for an explanation of national differences in adoption of broadband....

TIME-RESOLVED SPECTROSCOPY OF THE POLAR EU CANCRI IN THE OPEN CLUSTER MESSIER 67

International Nuclear Information System (INIS)

Williams, Kurtis A.; Howell, Steve B.; Liebert, James; Smith, Paul S.; Bellini, Andrea; Rubin, Kate H. R.; Bolte, Michael

2013-01-01

We present time-resolved spectroscopic and polarimetric observations of the AM Her system EU Cnc. EU Cnc is located near the core of the old open cluster Messier 67; new proper motion measurements indicate that EU Cnc is indeed a member of the star cluster, and this system therefore is useful to constrain the formation and evolution of magnetic cataclysmic variables. The spectra exhibit two-component emission features with independent radial velocity variations as well as time-variable cyclotron emission indicating a magnetic field strength of 41 MG. The period of the radial velocity and cyclotron hump variations are consistent with the previously known photometric period, and the spectroscopic flux variations are consistent in amplitude with previous photometric amplitude measurements. The secondary star is also detected in the spectrum. We also present polarimetric imaging measurements of EU Cnc that show a clear detection of polarization, and the degree of polarization drops below our detection threshold at phases when the cyclotron emission features are fading or not evident. The combined data are all consistent with the interpretation that EU Cnc is a low-state polar in the cluster Messier 67. The mass function of the system gives an estimate of the accretor mass of M WD ≥ 0.68 M ☉ with M WD ≈ 0.83 M ☉ for an average inclination. We are thus able to place a lower limit on the progenitor mass of the accreting white dwarf of ≥1.43 M ☉ .

Soft X-ray angle-resolved photoemission spectroscopy of heavily boron-doped superconducting diamond films

Directory of Open Access Journals (Sweden)

T. Yokoya, T. Nakamura, T. Matushita, T. Muro, H. Okazaki, M. Arita, K. Shimada, H. Namatame, M. Taniguchi, Y. Takano, M. Nagao, T. Takenouchi, H. Kawarada and T. Oguchi

2006-01-01

Full Text Available We have performed soft X-ray angle-resolved photoemission spectroscopy (SXARPES of microwave plasma-assisted chemical vapor deposition diamond films with different B concentrations in order to study the origin of the metallic behavior of superconducting diamond. SXARPES results clearly show valence band dispersions with a bandwidth of ~23 eV and with a top of the valence band at gamma point in the Brillouin zone, which are consistent with the calculated valence band dispersions of pure diamond. Boron concentration-dependent band dispersions near the Fermi level (EF exhibit a systematic shift of EF, indicating depopulation of electrons due to hole doping. These SXARPES results indicate that diamond bands retain for heavy boron doping and holes in the diamond band are responsible for the metallic states leading to superconductivity at low temperature. A high-resolution photoemission spectroscopy spectrum near EF of a heavily boron-doped diamond superconductor is also presented.

Ultrafast Carrier Trapping of a Metal-Doped Titanium Dioxide Semiconductor Revealed by Femtosecond Transient Absorption Spectroscopy

KAUST Repository

Sun, Jingya; Yang, Yang; Khan, Jafar I.; Alarousu, Erkki; Guo, Zaibing; Zhang, Xixiang; Zhang, Qiang; Mohammed, Omar F.

2014-01-01

We explored for the first time the ultrafast carrier trapping of a metal-doped titanium dioxide (TiO2) semiconductor using broad-band transient absorption (TA) spectroscopy with 120 fs temporal resolution. Titanium dioxide was successfully doped layer-by-layer with two metal ions, namely tungsten and cobalt. The time-resolved data demonstrate clearly that the carrier trapping time decreases progressively as the doping concentration increases. A global-fitting procedure for the carrier trapping suggests the appearance of two time components: a fast one that is directly associated with carrier trapping to the defect state in the vicinity of the conduction band and a slow one that is attributed to carrier trapping to the deep-level state from the conduction band. With a relatively long doping deposition time on the order of 30 s, a carrier lifetime of about 1 ps is obtained. To confirm that the measured ultrafast carrier dynamics are associated with electron trapping by metal doping, we explored the carrier dynamics of undoped TiO2. The findings reported here may be useful for the implementation of high-speed optoelectronic applications and fast switching devices.

Ultrafast Carrier Trapping of a Metal-Doped Titanium Dioxide Semiconductor Revealed by Femtosecond Transient Absorption Spectroscopy

KAUST Repository

Sun, Jingya

2014-06-11

We explored for the first time the ultrafast carrier trapping of a metal-doped titanium dioxide (TiO2) semiconductor using broad-band transient absorption (TA) spectroscopy with 120 fs temporal resolution. Titanium dioxide was successfully doped layer-by-layer with two metal ions, namely tungsten and cobalt. The time-resolved data demonstrate clearly that the carrier trapping time decreases progressively as the doping concentration increases. A global-fitting procedure for the carrier trapping suggests the appearance of two time components: a fast one that is directly associated with carrier trapping to the defect state in the vicinity of the conduction band and a slow one that is attributed to carrier trapping to the deep-level state from the conduction band. With a relatively long doping deposition time on the order of 30 s, a carrier lifetime of about 1 ps is obtained. To confirm that the measured ultrafast carrier dynamics are associated with electron trapping by metal doping, we explored the carrier dynamics of undoped TiO2. The findings reported here may be useful for the implementation of high-speed optoelectronic applications and fast switching devices.

Programming for time resolved spectrum in pulse radiolysis experiments

International Nuclear Information System (INIS)

Betty, C.A.; Panajkar, M.S.; Shirke, N.D.

1993-01-01

A user friendly program in Pascal has been developed for data acquisition and subsequent processing of time resolved spectra of transient species produced in pulse radiolysis experiments. The salient features of the program are (i) thiocyanate dosimetry and (ii) spectrum acquisition. The thiocyanate dosimetry is carried out to normalize experimental conditions to a standard value as determined by computing absorbance of the transient signal CNS -2 that is produced from thiocyanate solution by a 7 MeV electron pulse. Spectrum acquisition allows the acquisition of the time resolved data at 20 different times points and subsequent display of the plots of absorbance vs. wavelength for the desired time points during the experiment. It is also possible to plot single time point spectrum as well as superimposed spectra for different time points. Printing, editing and merging facilities are also provided. (author). 2 refs., 7 figs

Near-infrared incoherent broadband cavity enhanced absorption spectroscopy (NIR-IBBCEAS) for detection and quantification of natural gas components.

Science.gov (United States)

Prakash, Neeraj; Ramachandran, Arun; Varma, Ravi; Chen, Jun; Mazzoleni, Claudio; Du, Ke

2018-06-28

The principle of near-infrared incoherent broadband cavity enhanced absorption spectroscopy was employed to develop a novel instrument for detecting natural gas leaks as well as for testing the quality of natural gas mixtures. The instrument utilizes the absorption features of methane, butane, ethane, and propane in the wavelength region of 1100 nm to 1250 nm. The absorption cross-section spectrum in this region for methane was adopted from the HITRAN database, and those for the other three gases were measured in the laboratory. A singular-value decomposition (SVD) based analysis scheme was employed for quantifying methane, butane, ethane, and propane by performing a linear least-square fit. The developed instrument achieved a detection limit of 460 ppm, 141 ppm, 175 ppm and 173 ppm for methane, butane, ethane, and propane, respectively, with a measurement time of 1 second and a cavity length of 0.59 m. These detection limits are less than 1% of the Lower Explosive Limit (LEL) for each gas. The sensitivity can be further enhanced by changing the experimental parameters (such as cavity length, lamp power etc.) and using longer averaging intervals. The detection system is a low-cost and portable instrument suitable for performing field monitorings. The results obtained on the gas mixture emphasize the instrument's potential for deployment at industrial facilities dealing with natural gas, where potential leaks pose a threat to public safety.

System and method for detection of dispersed broadband signals

Science.gov (United States)

Qian, S.; Dunham, M.E.

1999-06-08

A system and method for detecting the presence of dispersed broadband signals in real time are disclosed. The present invention utilizes a bank of matched filters for detecting the received dispersed broadband signals. Each matched filter uses a respective robust time template that has been designed to approximate the dispersed broadband signals of interest, and each time template varies across a spectrum of possible dispersed broadband signal time templates. The received dispersed broadband signal x(t) is received by each of the matched filters, and if one or more matches occurs, then the received data is determined to have signal data of interest. This signal data can then be analyzed and/or transmitted to Earth for analysis, as desired. The system and method of the present invention will prove extremely useful in many fields, including satellite communications, plasma physics, and interstellar research. The varying time templates used in the bank of matched filters are determined as follows. The robust time domain template is assumed to take the form w(t)=A(t)cos[l brace]2[phi](t)[r brace]. Since the instantaneous frequency f(t) is known to be equal to the derivative of the phase [phi](t), the trajectory of a joint time-frequency representation of x(t) is used as an approximation of [phi][prime](t). 10 figs.

Application of spectroscopy and super-resolution microscopy: Excited state

Energy Technology Data Exchange (ETDEWEB)

Bhattacharjee, Ujjal [Iowa State Univ., Ames, IA (United States)

2016-02-19

Photophysics of inorganic materials and organic molecules in complex systems have been extensively studied with absorption and emission spectroscopy.1-4 Steady-state and time-resolved fluorescence studies are commonly carried out to characterize excited-state properties of fluorophores. Although steady-state fluorescence measurements are widely used for analytical applications, time-resolved fluorescence measurements provide more detailed information about excited-state properties and the environment in the vicinity of the fluorophore. Many photophysical processes, such as photoinduced electron transfer (PET), rotational reorientation, solvent relaxation, and energy transfer, occur on a nanosecond (10^-9 s) timescale, thus affecting the lifetime of the fluorophores. Moreover, time-resolved microscopy methods, such as lifetimeimaging, combine the benefits of the microscopic measurement and information-rich, timeresolved data. Thus, time-resolved fluorescence spectroscopy combined with microscopy can be used to quantify these processes and to obtain a deeper understanding of the chemical surroundings of the fluorophore in a small area under investigation. This thesis discusses various photophysical and super-resolution microscopic studies of organic and inorganic materials, which have been outlined below.

Temperature-induced band shift in bulk γ-InSe by angle-resolved photoemission spectroscopy

Science.gov (United States)

Xu, Huanfeng; Wang, Wei; Zhao, Yafei; Zhang, Xiaoqian; Feng, Yue; Tu, Jian; Gu, Chenyi; Sun, Yizhe; Liu, Chang; Nie, Yuefeng; Edmond Turcu, Ion C.; Xu, Yongbing; He, Liang

2018-05-01

Indium selenide (InSe) has recently become popular research topics because of its unique layered crystal structure, direct band gap and high electron mobilities. In this work, we have acquired the electronic structure of bulk γ-InSe at various temperatures using angle-resolved photoemission spectroscopy (ARPES). We have also found that as the temperature decreases, the valence bands of γ-InSe exhibit a monotonic shift to lower binding energies. This band shift is attributed to the change of lattice parameters and has been validated by variable temperature X-ray diffraction measurements and theoretical calculations.

Lifetime measurements of odd-parity high-excitation levels of Sn I by time-resolved laser spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Zhang, Wei; Feng, Yanyan; Xu, Jiaxin; Dai, Zhenwen [College of Physics, Jilin University and Key Lab of Coherent Light, Atomic and Molecular Spectroscopy, Ministry of Education, Changchun 130021 (China); Palmeri, Patrick; Quinet, Pascal; Biemont, Emile, E-mail: dai@jlu.edu.c [Astrophysique et Spectroscopie, Universite de Mons-UMONS, B-7000 Mons (Belgium)

2010-10-28

Natural radiative lifetimes of 38 odd-parity highly excited levels in neutral tin in the energy range from 43 682.737 to 56 838.68 cm{sup -1} have been measured by a time-resolved laser-induced fluorescence technique in an atomic beam produced by laser ablation on a solid tin sample. All the levels were excited from the metastable {sup 3}P{sub 1,} {sub 2} and {sup 1}D{sub 2} levels in the ground configuration. The second and third harmonics of a dye laser were adopted as the tunable exciting source (207-250 nm). The lifetime results obtained in this paper are in the range from 4.6 to 292 ns and will be useful in extending the set of oscillator strengths available in Sn I.

Time-resolved crystallography using the Hadamard Transform

Science.gov (United States)

Yorke, Briony A.; Beddard, Godfrey S.; Owen, Robin L.; Pearson, Arwen R.

2014-01-01

A new method for performing time-resolved X-ray crystallographic experiments based on the Hadamard Transform is proposed and demonstrated. The time-resolution is defined by the underlying periodicity of the probe pulse sequence and the signal to noise is greatly improved compared to the fastest experiments depending on a single pulse. This approach is general and equally applicable to any spectroscopic or imaging measurement where the probe can be encoded. PMID:25282611

Aerofoil broadband and tonal noise modelling using stochastic sound sources and incorporated large scale fluctuations

Science.gov (United States)

Proskurov, S.; Darbyshire, O. R.; Karabasov, S. A.

2017-12-01

The present work discusses modifications to the stochastic Fast Random Particle Mesh (FRPM) method featuring both tonal and broadband noise sources. The technique relies on the combination of incorporated vortex-shedding resolved flow available from Unsteady Reynolds-Averaged Navier-Stokes (URANS) simulation with the fine-scale turbulence FRPM solution generated via the stochastic velocity fluctuations in the context of vortex sound theory. In contrast to the existing literature, our method encompasses a unified treatment for broadband and tonal acoustic noise sources at the source level, thus, accounting for linear source interference as well as possible non-linear source interaction effects. When sound sources are determined, for the sound propagation, Acoustic Perturbation Equations (APE-4) are solved in the time-domain. Results of the method's application for two aerofoil benchmark cases, with both sharp and blunt trailing edges are presented. In each case, the importance of individual linear and non-linear noise sources was investigated. Several new key features related to the unsteady implementation of the method were tested and brought into the equation. Encouraging results have been obtained for benchmark test cases using the new technique which is believed to be potentially applicable to other airframe noise problems where both tonal and broadband parts are important.

On-chip dual comb source for spectroscopy

OpenAIRE

Dutt, Avik; Joshi, Chaitanya; Ji, Xingchen; Cardenas, Jaime; Okawachi, Yoshitomo; Luke, Kevin; Gaeta, Alexander L.; Lipson, Michal

2016-01-01

Dual-comb spectroscopy is a powerful technique for real-time, broadband optical sampling of molecular spectra which requires no moving components. Recent developments with microresonator-based platforms have enabled frequency combs at the chip scale. However, the need to precisely match the resonance wavelengths of distinct high-quality-factor microcavities has hindered the development of an on-chip dual comb source. Here, we report the first simultaneous generation of two microresonator comb...

Watching proteins function with time-resolved x-ray crystallography

Science.gov (United States)

Šrajer, Vukica; Schmidt, Marius

2017-09-01

Macromolecular crystallography was immensely successful in the last two decades. To a large degree this success resulted from use of powerful third generation synchrotron x-ray sources. An expansive database of more than 100 000 protein structures, of which many were determined at resolution better than 2 Å, is available today. With this achievement, the spotlight in structural biology is shifting from determination of static structures to elucidating dynamic aspects of protein function. A powerful tool for addressing these aspects is time-resolved crystallography, where a genuine biological function is triggered in the crystal with a goal of capturing molecules in action and determining protein kinetics and structures of intermediates (Schmidt et al 2005a Methods Mol. Biol. 305 115-54, Schmidt 2008 Ultrashort Laser Pulses in Biology and Medicine (Berlin: Springer) pp 201-41, Neutze and Moffat 2012 Curr. Opin. Struct. Biol. 22 651-9, Šrajer 2014 The Future of Dynamic Structural Science (Berlin: Springer) pp 237-51). In this approach, short and intense x-ray pulses are used to probe intermediates in real time and at room temperature, in an ongoing reaction that is initiated synchronously and rapidly in the crystal. Time-resolved macromolecular crystallography with 100 ps time resolution at synchrotron x-ray sources is in its mature phase today, particularly for studies of reversible, light-initiated reactions. The advent of the new free electron lasers for hard x-rays (XFELs; 5-20 keV), which provide exceptionally intense, femtosecond x-ray pulses, marks a new frontier for time-resolved crystallography. The exploration of ultra-fast events becomes possible in high-resolution structural detail, on sub-picosecond time scales (Tenboer et al 2014 Science 346 1242-6, Barends et al 2015 Science 350 445-50, Pande et al 2016 Science 352 725-9). We review here state-of-the-art time-resolved crystallographic experiments both at synchrotrons and XFELs. We also outline

Anomalous Temporal Behaviour of Broadband Ly Alpha Observations During Solar Flares from SDO/EVE

Science.gov (United States)

Milligan, Ryan O.; Chamberlin, Phillip C.

2016-01-01

Although it is the most prominent emission line in the solar spectrum, there has been a notable lack of studies devoted to variations in Lyman-alpha (Ly-alpha) emission during solar flares in recent years. However, the few examples that do exist have shown Ly-alpha emission to be a substantial radiator of the total energy budget of solar flares (of the order of 10 percent). It is also a known driver of fluctuations in the Earth's ionosphere. The EUV (Extreme Ultra-Violet) Variability Experiment (EVE) on board the Solar Dynamics Observatory (SDO) now provides broadband, photometric Ly-alpha data at 10-second cadence with its Multiple EUV Grating Spectrograph-Photometer (MEGS-P) component, and has observed scores of solar flares in the 5 years since it was launched. However, the MEGS-P time profiles appear to display a rise time of tens of minutes around the time of the flare onset. This is in stark contrast to the rapid, impulsive increase observed in other intrinsically chromospheric features (H-alpha, Ly-beta, LyC, C III, etc.). Furthermore, the emission detected by MEGS-P peaks around the time of the peak of thermal soft X-ray emission and not during the impulsive phase when energy deposition in the chromosphere (often assumed to be in the form of non-thermal electrons) is greatest. The time derivative of Ly-alpha lightcurves also appears to resemble that of the time derivative of soft X-rays, reminiscent of the Neupert effect. Given that spectrally-resolved Ly-alpha observations during flares from SORCE / SOLSTICE (Solar Radiation and Climate Experiment / Solar Stellar Irradiance Comparison Experiment) peak during the impulsive phase as expected, this suggests that the atypical behaviour of MEGS-P data is a manifestation of the broadband nature of the observations. This could imply that other lines andor continuum emission that becomes enhanced during flares could be contributing to the passband. Users are hereby urged to exercise caution when interpreting

Ultrafast Time-Resolved Photoluminescence Studies of Gallium-Arsenide

Science.gov (United States)

Johnson, Matthew Bruce

This thesis concerns the study of ultrafast phenomena in GaAs using time-resolved photoluminescence (PL). The thesis consists of five chapters. Chapter one is an introduction, which discusses the study of ultrafast phenomena in semiconductors. Chapter two is a description of the colliding-pulse mode-locked (CPM) ring dye laser, which is at the heart of the experimental apparatus used in this thesis. Chapter three presents a detailed experimental and theoretical investigation of photoluminescence excitation correlation spectroscopy (PECS), the novel technique which is used to time-resolve ultrafast PL phenomena. Chapters 4 and 5 discuss two applications of the PECS technique. In Chapter 4 the variation of PL intensity in In-alloyed GaAs substrate material is studied, while Chapter 5 discusses the variation of carrier lifetimes in ion-damaged GaAs used in photo-conductive circuit elements (PCEs). PECS is a pulse-probe technique that measures the cross correlation of photo-excited carrier populations. The theoretical model employed in this thesis is based upon the rate equation for a simple three-level system consisting of valence and conduction bands and a single trap level. In the limit of radiative band-to-band dominated recombination, no PECS signal should be observed; while in the capture -dominated recombination limit, the PECS signal from the band-to-band PL measures the cross correlation of the excited electron and hole populations and thus, the electron and hole lifetimes. PECS is experimentally investigated using a case study of PL in semi-insulating (SI) GaAs and In -alloyed GaAs. At 77 K, the PECS signal is characteristic of a capture-dominated system, yielding an electron-hole lifetime of about 200 ps. However, at 5 K the behavior is more complicated and shows saturation effects due to the C acceptor level, which is un-ionized at 5 K. As a first application, PECS is used to investigate the large band-to-band PL contrast observed near dislocations in In

Toward noninvasive detection and monitoring of malaria with broadband diffuse optical spectroscopy

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