Time-Resolved In Situ Measurements During Rapid Alloy Solidification: Experimental Insight for Additive Manufacturing

DOE PAGES

McKeown, Joseph T.; Zweiacker, Kai; Liu, Can; ...

2016-01-27

In research and industrial environments, additive manufacturing (AM) of metals and alloys is becoming a pervasive technology, though significant challenges remain before widespread implementation of AM can be realized. In situ investigations of rapid alloy solidification with high spatial and temporal resolutions can provide unique experimental insight into microstructure evolution and kinetics that are relevant for AM processing. Hypoeutectic thin-film Al–Cu and Al–Si alloys were investigated using dynamic transmission electron microscopy to monitor pulsed-laser-induced rapid solidification across microsecond timescales. Solid–liquid interface velocities measured from time-resolved images revealed accelerating solidification fronts in both alloys. We observed microstructure evolution, solidification product, andmore » presence of a morphological instability at the solid–liquid interface in the Al–4 at.%Cu alloy are related to the measured interface velocities and small differences in composition that affect the thermophysical properties of the alloys. These time-resolved in situ measurements can inform and validate predictive modeling efforts for AM.« less

rf streak camera based ultrafast relativistic electron diffraction.

PubMed

Musumeci, P; Moody, J T; Scoby, C M; Gutierrez, M S; Tran, T

2009-01-01

We theoretically and experimentally investigate the possibility of using a rf streak camera to time resolve in a single shot structural changes at the sub-100 fs time scale via relativistic electron diffraction. We experimentally tested this novel concept at the UCLA Pegasus rf photoinjector. Time-resolved diffraction patterns from thin Al foil are recorded. Averaging over 50 shots is required in order to get statistics sufficient to uncover a variation in time of the diffraction patterns. In the absence of an external pump laser, this is explained as due to the energy chirp on the beam out of the electron gun. With further improvements to the electron source, rf streak camera based ultrafast electron diffraction has the potential to yield truly single shot measurements of ultrafast processes.

Improved Understanding of Implosion Symmetry through New Experimental Techniques Connecting Hohlraum Dynamics with Laser Beam Deposition

NASA Astrophysics Data System (ADS)

Ralph, Joseph; Salmonson, Jay; Dewald, Eduard; Bachmann, Benjamin; Edwards, John; Graziani, Frank; Hurricane, Omar; Landen, Otto; Ma, Tammy; Masse, Laurent; MacLaren, Stephen; Meezan, Nathan; Moody, John; Parrilla, Nicholas; Pino, Jesse; Sacks, Ryan; Tipton, Robert

2017-10-01

Understanding what affects implosion symmetry has been a challenge for scientists designing indirect drive inertial confinement fusion experiments on the National Ignition Facility (NIF). New experimental techniques and data analysis have been employed aimed at improving our understanding of the relationship between hohlraum dynamics and implosion symmetry. Thin wall imaging data allows for time-resolved imaging of 10 keV Au l-band x-rays providing for the first time on the NIF, a spatially resolved measurement of laser deposition with time. In the work described here, we combine measurements from the thin wall imaging with time resolved views of the interior of the hohlraum. The measurements presented are compared to hydrodynamic simulations as well as simplified physics models. The goal of this work is to form a physical picture that better explains the relationship of the hohlraum dynamics and capsule ablator on laser beam propagation and implosion symmetry. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344.

SVD-aided pseudo principal-component analysis: A new method to speed up and improve determination of the optimum kinetic model from time-resolved data

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

Oang, Key Young; Yang, Cheolhee; Muniyappan, Srinivasan

Determination of the optimum kinetic model is an essential prerequisite for characterizing dynamics and mechanism of a reaction. Here, we propose a simple method, termed as singular value decomposition-aided pseudo principal-component analysis (SAPPA), to facilitate determination of the optimum kinetic model from time-resolved data by bypassing any need to examine candidate kinetic models. We demonstrate the wide applicability of SAPPA by examining three different sets of experimental time-resolved data and show that SAPPA can efficiently determine the optimum kinetic model. In addition, the results of SAPPA for both time-resolved X-ray solution scattering (TRXSS) and transient absorption (TA) data of themore » same protein reveal that global structural changes of protein, which is probed by TRXSS, may occur more slowly than local structural changes around the chromophore, which is probed by TA spectroscopy.« less

Molecular orbital imaging of the acetone S2 excited state using time-resolved (e, 2e) electron momentum spectroscopy.

PubMed

Yamazaki, Masakazu; Oishi, Keiya; Nakazawa, Hiroyuki; Zhu, Chaoyuan; Takahashi, Masahiko

2015-03-13

We report a time-resolved (e, 2e) experiment on the deuterated acetone molecule in the S2 Rydberg state with a lifetime of 13.5 ps. The acetone S2 state was prepared by a 195 nm pump laser and probed with electron momentum spectroscopy using a 1.2 keV incident electron beam of 1 ps temporal width. In spite of the low data statistics as well as of the limited time resolution (±35  ps) due to velocity mismatch, the experimental results clearly demonstrate that electron momentum spectroscopy measurements of short-lived transient species are feasible, opening the door to time-resolved orbital imaging in momentum space.

An electron energy loss spectrometer based streak camera for time resolved TEM measurements.

PubMed

Ali, Hasan; Eriksson, Johan; Li, Hu; Jafri, S Hassan M; Kumar, M S Sharath; Ögren, Jim; Ziemann, Volker; Leifer, Klaus

2017-05-01

We propose an experimental setup based on a streak camera approach inside an energy filter to measure time resolved properties of materials in the transmission electron microscope (TEM). In order to put in place the streak camera, a beam sweeper was built inside an energy filter. After exciting the TEM sample, the beam is swept across the CCD camera of the filter. We describe different parts of the setup at the example of a magnetic measurement. This setup is capable to acquire time resolved diffraction patterns, electron energy loss spectra (EELS) and images with total streaking times in the range between 100ns and 10μs. Copyright © 2016 Elsevier B.V. All rights reserved.

Time-domain reflectance diffuse optical tomography with Mellin-Laplace transform for experimental detection and depth localization of a single absorbing inclusion

PubMed Central

Puszka, Agathe; Hervé, Lionel; Planat-Chrétien, Anne; Koenig, Anne; Derouard, Jacques; Dinten, Jean-Marc

2013-01-01

We show how to apply the Mellin-Laplace transform to process time-resolved reflectance measurements for diffuse optical tomography. We illustrate this method on simulated signals incorporating the main sources of experimental noise and suggest how to fine-tune the method in order to detect the deepest absorbing inclusions and optimize their localization in depth, depending on the dynamic range of the measurement. To finish, we apply this method to measurements acquired with a setup including a femtosecond laser, photomultipliers and a time-correlated single photon counting board. Simulations and experiments are illustrated for a probe featuring the interfiber distance of 1.5 cm and show the potential of time-resolved techniques for imaging absorption contrast in depth with this geometry. PMID:23577292

An implementation of the maximum-caliber principle by replica-averaged time-resolved restrained simulations

NASA Astrophysics Data System (ADS)

Capelli, Riccardo; Tiana, Guido; Camilloni, Carlo

2018-05-01

Inferential methods can be used to integrate experimental informations and molecular simulations. The maximum entropy principle provides a framework for using equilibrium experimental data, and it has been shown that replica-averaged simulations, restrained using a static potential, are a practical and powerful implementation of such a principle. Here we show that replica-averaged simulations restrained using a time-dependent potential are equivalent to the principle of maximum caliber, the dynamic version of the principle of maximum entropy, and thus may allow us to integrate time-resolved data in molecular dynamics simulations. We provide an analytical proof of the equivalence as well as a computational validation making use of simple models and synthetic data. Some limitations and possible solutions are also discussed.

An implementation of the maximum-caliber principle by replica-averaged time-resolved restrained simulations.

PubMed

Capelli, Riccardo; Tiana, Guido; Camilloni, Carlo

2018-05-14

Inferential methods can be used to integrate experimental informations and molecular simulations. The maximum entropy principle provides a framework for using equilibrium experimental data, and it has been shown that replica-averaged simulations, restrained using a static potential, are a practical and powerful implementation of such a principle. Here we show that replica-averaged simulations restrained using a time-dependent potential are equivalent to the principle of maximum caliber, the dynamic version of the principle of maximum entropy, and thus may allow us to integrate time-resolved data in molecular dynamics simulations. We provide an analytical proof of the equivalence as well as a computational validation making use of simple models and synthetic data. Some limitations and possible solutions are also discussed.

Time-resolved absorption and hemoglobin concentration difference maps: a method to retrieve depth-related information on cerebral hemodynamics.

NASA Astrophysics Data System (ADS)

Montcel, Bruno; Chabrier, Renée; Poulet, Patrick

2006-12-01

Time-resolved diffuse optical methods have been applied to detect hemodynamic changes induced by cerebral activity. We describe a near infrared spectroscopic (NIRS) reconstruction free method which allows retrieving depth-related information on absorption variations. Variations in the absorption coefficient of tissues have been computed over the duration of the whole experiment, but also over each temporal step of the time-resolved optical signal, using the microscopic Beer-Lambert law.Finite element simulations show that time-resolved computation of the absorption difference as a function of the propagation time of detected photons is sensitive to the depth profile of optical absorption variations. Differences in deoxyhemoglobin and oxyhemoglobin concentrations can also be calculated from multi-wavelength measurements. Experimental validations of the simulated results have been obtained for resin phantoms. They confirm that time-resolved computation of the absorption differences exhibited completely different behaviours, depending on whether these variations occurred deeply or superficially. The hemodynamic response to a short finger tapping stimulus was measured over the motor cortex and compared to experiments involving Valsalva manoeuvres. Functional maps were also calculated for the hemodynamic response induced by finger tapping movements.

Time-resolved absorption and hemoglobin concentration difference maps: a method to retrieve depth-related information on cerebral hemodynamics.

PubMed

Montcel, Bruno; Chabrier, Renée; Poulet, Patrick

2006-12-11

Time-resolved diffuse optical methods have been applied to detect hemodynamic changes induced by cerebral activity. We describe a near infrared spectroscopic (NIRS) reconstruction free method which allows retrieving depth-related information on absorption variations. Variations in the absorption coefficient of tissues have been computed over the duration of the whole experiment, but also over each temporal step of the time-resolved optical signal, using the microscopic Beer-Lambert law.Finite element simulations show that time-resolved computation of the absorption difference as a function of the propagation time of detected photons is sensitive to the depth profile of optical absorption variations. Differences in deoxyhemoglobin and oxyhemoglobin concentrations can also be calculated from multi-wavelength measurements. Experimental validations of the simulated results have been obtained for resin phantoms. They confirm that time-resolved computation of the absorption differences exhibited completely different behaviours, depending on whether these variations occurred deeply or superficially. The hemodynamic response to a short finger tapping stimulus was measured over the motor cortex and compared to experiments involving Valsalva manoeuvres. Functional maps were also calculated for the hemodynamic response induced by finger tapping movements.

High-power laser interaction with low-density C–Cu foams

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

Pérez, F.; Colvin, J. D.; May, M. J.

2015-11-15

We study the propagation of high-power laser beams in micro-structured carbon foams by monitoring the x-ray output from deliberately introduced Cu content. In particular, we characterize this phenomenon measuring absolute time-resolved x-ray yields, time-resolved x-ray imaging, and x-ray spectroscopy. New experimental results for C–Cu foams show a faster heat front velocity than simulation that assumed homogeneous plasma. We suggest the foam micro-structure may explain this trend.

High-power laser interaction with low-density C–Cu foams

DOE PAGES

Pérez, F.; Colvin, J. D.; May, M. J.; ...

2015-11-19

Here, we study the propagation of high-power laser beams in micro-structured carbon foams by monitoring the x-ray output from deliberately introduced Cu content. In particular, we characterize this phenomenon measuring absolute time-resolved x-ray yields, time-resolved x-ray imaging, and x-ray spectroscopy. New experimental results for C–Cu foams show a faster heat front velocity than simulation that assumed homogeneous plasma. We suggest the foam micro-structure may explain this trend.

Time-dependent first-principles study of angle-resolved secondary electron emission from atomic sheets

NASA Astrophysics Data System (ADS)

Ueda, Yoshihiro; Suzuki, Yasumitsu; Watanabe, Kazuyuki

2018-02-01

Angle-resolved secondary electron emission (ARSEE) spectra were analyzed for two-dimensional atomic sheets using a time-dependent first-principles simulation of electron scattering. We demonstrate that the calculated ARSEE spectra capture the unoccupied band structure of the atomic sheets. The excitation dynamics that lead to SEE have also been revealed by the time-dependent Kohn-Sham decomposition scheme. In the present study, the mechanism for the experimentally observed ARSEE from atomic sheets is elucidated with respect to both energetics and the dynamical aspects of SEE.

Ultrafast magnetodynamics with free-electron lasers

NASA Astrophysics Data System (ADS)

Malvestuto, Marco; Ciprian, Roberta; Caretta, Antonio; Casarin, Barbara; Parmigiani, Fulvio

2018-02-01

The study of ultrafast magnetodynamics has entered a new era thanks to the groundbreaking technological advances in free-electron laser (FEL) light sources. The advent of these light sources has made possible unprecedented experimental schemes for time-resolved x-ray magneto-optic spectroscopies, which are now paving the road for exploring the ultimate limits of out-of-equilibrium magnetic phenomena. In particular, these studies will provide insights into elementary mechanisms governing spin and orbital dynamics, therefore contributing to the development of ultrafast devices for relevant magnetic technologies. This topical review focuses on recent advancement in the study of non-equilibrium magnetic phenomena from the perspective of time-resolved extreme ultra violet (EUV) and soft x-ray spectroscopies at FELs with highlights of some important experimental results.

Time-resolved broadband cavity-enhanced absorption spectroscopy for chemical kinetics.

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

Sheps, Leonid; Chandler, David W.

Experimental measurements of elementary reaction rate coefficients and product branching ratios are essential to our understanding of many fundamentally important processes in Combustion Chemistry. However, such measurements are often impossible because of a lack of adequate detection techniques. Some of the largest gaps in our knowledge concern some of the most important radical species, because their short lifetimes and low steady-state concentrations make them particularly difficult to detect. To address this challenge, we propose a novel general detection method for gas-phase chemical kinetics: time-resolved broadband cavity-enhanced absorption spectroscopy (TR-BB-CEAS). This all-optical, non-intrusive, multiplexed method enables sensitive direct probing of transientmore » reaction intermediates in a simple, inexpensive, and robust experimental package.« less

Time-resolved vibrational spectroscopy

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

Tokmakoff, Andrei; Champion, Paul; Heilweil, Edwin J.

2009-05-14

This document contains the Proceedings from the 14th International Conference on Time-Resolved Vibrational Spectroscopy, which was held in Meredith, NH from May 9-14, 2009. The study of molecular dynamics in chemical reaction and biological processes using time-resolved spectroscopy plays an important role in our understanding of energy conversion, storage, and utilization problems. Fundamental studies of chemical reactivity, molecular rearrangements, and charge transport are broadly supported by the DOE's Office of Science because of their role in the development of alternative energy sources, the understanding of biological energy conversion processes, the efficient utilization of existing energy resources, and the mitigation ofmore » reactive intermediates in radiation chemistry. In addition, time-resolved spectroscopy is central to all fiveof DOE's grand challenges for fundamental energy science. The Time-Resolved Vibrational Spectroscopy conference is organized biennially to bring the leaders in this field from around the globe together with young scientists to discuss the most recent scientific and technological advances. The latest technology in ultrafast infrared, Raman, and terahertz spectroscopy and the scientific advances that these methods enable were covered. Particular emphasis was placed on new experimental methods used to probe molecular dynamics in liquids, solids, interfaces, nanostructured materials, and biomolecules.« less

Experimental and Theoretical Aspects of Excited State Electron Transfer and Related Phenomena: Conference Held in Honour of Zbigniew R. Grabowski in Pultusk, Poland on September 27-October 2, 1992

DTIC Science & Technology

1992-10-01

DBMBF2 ) undergoes photoreaction with olefins through a partial electron transfer that leads to cycloaddition or sensitized Diels - Alder reactions. We...8217 Fluorescence. 10:00 J.M. WARMAN: Photon-induced Intramolecular Charge Sepaiation Studied byTime-Resolved Microwave Conductivity. 10:30 Coffee 11:)) W...26 Photon-Induced Intramolecular Charge Separation Studied by Time-Resolved Microwave Conductivity John M. Warman IRI, Delft University of Technology

Light-induced radical formation and isomerization of an aromatic thiol in solution followed by time-resolved x-ray absorption spectroscopy at the sulfur K-edge

DOE PAGES

Ochmann, Miguel; von Ahnen, Inga; Cordones, Amy A.; ...

2017-02-20

Here, we applied time-resolved sulfur-1s absorption spectroscopy to a model aromatic thiol system as a promising method for tracking chemical reactions in solution. Sulfur-1s absorption spectroscopy allows tracking multiple sulfur species with a time resolution of ~70 ps at synchrotron radiation facilities. Experimental transient spectra combined with high-level electronic structure theory allow identification of a radical and two thione isomers, which are generated upon illumination with 267 nm radiation. Moreover, the regioselectivity of the thione isomerization is explained by the resulting radical frontier orbitals. This work demonstrates the usefulness and potential of time-resolved sulfur-1s absorption spectroscopy for tracking multiple chemicalmore » reaction pathways and transient products of sulfur-containing molecules in solution.« less

Light-induced radical formation and isomerization of an aromatic thiol in solution followed by time-resolved x-ray absorption spectroscopy at the sulfur K-edge

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

Ochmann, Miguel; von Ahnen, Inga; Cordones, Amy A.

Here, we applied time-resolved sulfur-1s absorption spectroscopy to a model aromatic thiol system as a promising method for tracking chemical reactions in solution. Sulfur-1s absorption spectroscopy allows tracking multiple sulfur species with a time resolution of ~70 ps at synchrotron radiation facilities. Experimental transient spectra combined with high-level electronic structure theory allow identification of a radical and two thione isomers, which are generated upon illumination with 267 nm radiation. Moreover, the regioselectivity of the thione isomerization is explained by the resulting radical frontier orbitals. This work demonstrates the usefulness and potential of time-resolved sulfur-1s absorption spectroscopy for tracking multiple chemicalmore » reaction pathways and transient products of sulfur-containing molecules in solution.« less

Coherent optical effect on time-resolved vibrational SFG spectrum of adsorbates

NASA Astrophysics Data System (ADS)

Ueba, H.; Sawabu, T.; Mii, T.

2002-04-01

We present a theory to study the influence of the coherent mixing between pump-infrared and probe-visible pulse on a time-resolved sum-frequency generation (TR-SFG) spectrum for vibrations at surfaces. The general formula of the time-dependent and its Fourier transform of the SFG polarization and its Fourier transform allows us to calculate the time-resolved vibrational SFG spectrum and the transient characteristics of the SFG intensity as a function of the delay time td between the pump-infrared and probe-visible pulse. It is found the coherent optical effect manifests itself in the broadening and narrowing of the SFG spectrum with the intrinsic width of T2 at negative and positive td, respectively, being in qualitative agreement with recent experimental results. The influence of the coherent mixing on the transient behavior of the SFG intensity is also discussed in conjunction to the T2 determination.

Evaluating scintillator performance in time-resolved hard X-ray studies at synchrotron light sources.

PubMed

Rutherford, Michael E; Chapman, David J; White, Thomas G; Drakopoulos, Michael; Rack, Alexander; Eakins, Daniel E

2016-05-01

The short pulse duration, small effective source size and high flux of synchrotron radiation is ideally suited for probing a wide range of transient deformation processes in materials under extreme conditions. In this paper, the challenges of high-resolution time-resolved indirect X-ray detection are reviewed in the context of dynamic synchrotron experiments. In particular, the discussion is targeted at two-dimensional integrating detector methods, such as those focused on dynamic radiography and diffraction experiments. The response of a scintillator to periodic synchrotron X-ray excitation is modelled and validated against experimental data collected at the Diamond Light Source (DLS) and European Synchrotron Radiation Facility (ESRF). An upper bound on the dynamic range accessible in a time-resolved experiment for a given bunch separation is calculated for a range of scintillators. New bunch structures are suggested for DLS and ESRF using the highest-performing commercially available crystal LYSO:Ce, allowing time-resolved experiments with an interframe time of 189 ns and a maximum dynamic range of 98 (6.6 bits).

Evaluating scintillator performance in time-resolved hard X-ray studies at synchrotron light sources

PubMed Central

Rutherford, Michael E.; Chapman, David J.; White, Thomas G.; Drakopoulos, Michael; Rack, Alexander; Eakins, Daniel E.

2016-01-01

The short pulse duration, small effective source size and high flux of synchrotron radiation is ideally suited for probing a wide range of transient deformation processes in materials under extreme conditions. In this paper, the challenges of high-resolution time-resolved indirect X-ray detection are reviewed in the context of dynamic synchrotron experiments. In particular, the discussion is targeted at two-dimensional integrating detector methods, such as those focused on dynamic radiography and diffraction experiments. The response of a scintillator to periodic synchrotron X-ray excitation is modelled and validated against experimental data collected at the Diamond Light Source (DLS) and European Synchrotron Radiation Facility (ESRF). An upper bound on the dynamic range accessible in a time-resolved experiment for a given bunch separation is calculated for a range of scintillators. New bunch structures are suggested for DLS and ESRF using the highest-performing commercially available crystal LYSO:Ce, allowing time-resolved experiments with an interframe time of 189 ns and a maximum dynamic range of 98 (6.6 bits). PMID:27140147

Predicting the heat of vaporization of iron at high temperatures using time-resolved laser-induced incandescence and Bayesian model selection

NASA Astrophysics Data System (ADS)

Sipkens, Timothy A.; Hadwin, Paul J.; Grauer, Samuel J.; Daun, Kyle J.

2018-03-01

Competing theories have been proposed to account for how the latent heat of vaporization of liquid iron varies with temperature, but experimental confirmation remains elusive, particularly at high temperatures. We propose time-resolved laser-induced incandescence measurements on iron nanoparticles combined with Bayesian model plausibility, as a novel method for evaluating these relationships. Our approach scores the explanatory power of candidate models, accounting for parameter uncertainty, model complexity, measurement noise, and goodness-of-fit. The approach is first validated with simulated data and then applied to experimental data for iron nanoparticles in argon. Our results justify the use of Román's equation to account for the temperature dependence of the latent heat of vaporization of liquid iron.

Reconstructing the regulatory network controlling commitment and sporulation in Physarum polycephalum based on hierarchical Petri Net modelling and simulation.

PubMed

Marwan, Wolfgang; Sujatha, Arumugam; Starostzik, Christine

2005-10-21

We reconstruct the regulatory network controlling commitment and sporulation of Physarum polycephalum from experimental results using a hierarchical Petri Net-based modelling and simulation framework. The stochastic Petri Net consistently describes the structure and simulates the dynamics of the molecular network as analysed by genetic, biochemical and physiological experiments within a single coherent model. The Petri Net then is extended to simulate time-resolved somatic complementation experiments performed by mixing the cytoplasms of mutants altered in the sporulation response, to systematically explore the network structure and to probe its dynamics. This reverse engineering approach presumably can be employed to explore other molecular or genetic signalling systems where the activity of genes or their products can be experimentally controlled in a time-resolved manner.

Using time-frequency analysis to determine time-resolved detonation velocity with microwave interferometry.

PubMed

Kittell, David E; Mares, Jesus O; Son, Steven F

2015-04-01

Two time-frequency analysis methods based on the short-time Fourier transform (STFT) and continuous wavelet transform (CWT) were used to determine time-resolved detonation velocities with microwave interferometry (MI). The results were directly compared to well-established analysis techniques consisting of a peak-picking routine as well as a phase unwrapping method (i.e., quadrature analysis). The comparison is conducted on experimental data consisting of transient detonation phenomena observed in triaminotrinitrobenzene and ammonium nitrate-urea explosives, representing high and low quality MI signals, respectively. Time-frequency analysis proved much more capable of extracting useful and highly resolved velocity information from low quality signals than the phase unwrapping and peak-picking methods. Additionally, control of the time-frequency methods is mainly constrained to a single parameter which allows for a highly unbiased analysis method to extract velocity information. In contrast, the phase unwrapping technique introduces user based variability while the peak-picking technique does not achieve a highly resolved velocity result. Both STFT and CWT methods are proposed as improved additions to the analysis methods applied to MI detonation experiments, and may be useful in similar applications.

Time-resolved scattering of a single photon by a single atom

PubMed Central

Leong, Victor; Seidler, Mathias Alexander; Steiner, Matthias; Cerè, Alessandro; Kurtsiefer, Christian

2016-01-01

Scattering of light by matter has been studied extensively in the past. Yet, the most fundamental process, the scattering of a single photon by a single atom, is largely unexplored. One prominent prediction of quantum optics is the deterministic absorption of a travelling photon by a single atom, provided the photon waveform matches spatially and temporally the time-reversed version of a spontaneously emitted photon. Here we experimentally address this prediction and investigate the influence of the photon's temporal profile on the scattering dynamics using a single trapped atom and heralded single photons. In a time-resolved measurement of atomic excitation we find a 56(11)% increase of the peak excitation by photons with an exponentially rising profile compared with a decaying one. However, the overall scattering probability remains unchanged within the experimental uncertainties. Our results demonstrate that envelope tailoring of single photons enables precise control of the photon–atom interaction. PMID:27897173

Ultrafast inter- and intramolecular vibrational energy transfer between molecules at interfaces studied by time- and polarization-resolved SFG spectroscopy.

PubMed

Yamamoto, Susumu; Ghosh, Avishek; Nienhuys, Han-Kwang; Bonn, Mischa

2010-10-28

We present experimental results on femtosecond time-resolved surface vibrational spectroscopy aimed at elucidating the sub-picosecond reorientational dynamics of surface molecules. The approach, which relies on polarization- and time-resolved surface sum frequency generation (SFG), provides a general means to monitor interfacial reorientational dynamics through vibrations inherent in surface molecules in their electronic ground state. The technique requires an anisotropic vibrational excitation of surface molecules using orthogonally polarized infrared excitation light. The decay of the resulting anisotropy is followed in real-time. We employ the technique to reveal the reorientational dynamics of vibrational transition dipoles of long-chain primary alcohols on the water surface, and of water molecules at the water-air interface. The results demonstrate that, in addition to reorientational motion of specific molecules or molecular groups at the interface, inter- and intramolecular energy transfer processes can serve to scramble the initial anisotropy very efficiently. In the two exemplary cases demonstrated here, energy transfer occurs much faster than reorientational motion of interfacial molecules. This has important implications for the interpretation of static SFG spectra. Finally, we suggest experimental schemes and strategies to decouple effects resulting from energy transfer from those associated with surface molecular motion.

Wake losses from averaged and time-resolved power measurements at full scale wind turbines

NASA Astrophysics Data System (ADS)

Castellani, Francesco; Astolfi, Davide; Mana, Matteo; Becchetti, Matteo; Segalini, Antonio

2017-05-01

This work deals with the experimental analysis of wake losses fluctuations at full-scale wind turbines. The test case is a wind farm sited on a moderately complex terrain: 4 turbines are installed, having 2 MW of rated power each. The sources of information are the time-resolved data, as collected from the OPC server, and the 10-minutes averaged SCADA data. The objective is to compare the statistical distributions of wake losses for far and middle wakes, as can be observed through the “fast” lens of time-resolved data, for certain selected test-case time series, and through the “slow” lens of SCADA data, on a much longer time basis that allow to set the standards of the mean wake losses along the wind farm. Further, time-resolved data are used for an insight into the spectral properties of wake fluctuations, highlighting the role of the wind turbine as low-pass filter. Summarizing, the wind rose, the layout of the site and the structure of the data sets at disposal allow to study middle and far wake behavior, with a “slow” and “fast” perspective.

Improved test time evaluation in an expansion tube

NASA Astrophysics Data System (ADS)

James, Christopher M.; Cullen, Timothy G.; Wei, Han; Lewis, Steven W.; Gu, Sangdi; Morgan, Richard G.; McIntyre, Timothy J.

2018-05-01

Traditionally, expansion tube test times have been experimentally evaluated using test section mounted impact pressure probes. This paper proposes two new methods which can be performed using a high-speed camera and a simple circular cylinder test model. The first is the use of a narrow bandpass optical filter to allow time-resolved radiative emission from an important species to be captured, and the second is using edge detection to track how the model shock standoff changes with time. Experimental results are presented for two test conditions using an air test gas and an optical filter aimed at capturing emission from the 777 nm atomic oxygen triplet. It is found that the oxygen emission is the most reliable experimental method, because it is shown to exhibit significant changes at the end of the test time. It is also proposed that, because the camera footage is spatially resolved, the radiative emission method can be used to examine the `effective' test time in multiple regions of the flow. For one of the test conditions, it is found that the effective test time away from the stagnation region for the cylindrical test model is at most 45% of the total test time. For the other test condition, it is found that the effective test time of a 54° wedge test model is at most a third of the total test time.

Experimental radiative lifetimes, branching fractions, and oscillator strengths of some levels in Tm III

NASA Astrophysics Data System (ADS)

Yu, Qi; Wang, Xinghao; Li, Qiu; Gong, Yimin; Dai, Zhenwen

2018-06-01

Natural radiative lifetimes for five even-parity levels of Tm III were measured by time-resolved laser-induced fluorescence method. The branching fraction measurements were performed based on the emission spectra of a hollow cathode lamp. By combining the measured branching fractions and the lifetime values reported in this work and in literature, experimental transition probabilities and oscillator strengths for 11 transitions were derived for the first time.

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

NASA Technical Reports Server (NTRS)

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 to <1 s, in principle), but also higher optical throughput, thus resulting in a substantial increase in measurement SNR.

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

NASA Astrophysics Data System (ADS)

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

PubMed

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

2017-07-07

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

Exploring Nuclear Photorelaxation of Pyranine in Aqueous Solution: an Integrated Ab-Initio Molecular Dynamics and Time Resolved Vibrational Analysis Approach.

PubMed

Chiariello, Maria Gabriella; Rega, Nadia

2018-03-22

Advances in time-resolved vibrational spectroscopy techniques provided a new stimulus for understanding the transient molecular dynamics triggered by the electronic excitation. The detailed interpretation of such time-dependent spectroscopic signals is a challenging task from both experimental and theoretical points of view. We simulated and analyzed the transient photorelaxation of the pyranine photoacid in aqueous solution, with special focus on structural parameters and low frequency skeleton modes that are possibly preparatory for the photoreaction occurring at later time, as suggested by experimental spectroscopic studies. To this aim, we adopted an accurate computational protocol that combines excited state ab initio molecular dynamics within an hybrid quantum mechanical/molecular mechanics framework and a time-resolved vibrational analysis based on the Wavelet transform. According to our results, the main nuclear relaxation on the excited potential energy surface is completed in about 500 fs, in agreement with experimental data. The rearrangement of C-C bonds occurs according to a complex vibrational dynamics, showing oscillatory patterns that are out of phase and modulated by modes below 200 cm -1 . We also analyzed in both the ground and the excited state the evolution of some structural parameters involved in excited state proton transfer reaction, namely, those involving the pyranine and the water molecule hydrogen bonded to the phenolic O-H group. Both the hydrogen bond distance and the intermolecular orientation are optimized in the excited state, resulting in a tighter proton donor-acceptor couple. Indeed, we found evidence that collective low frequency skeleton modes, such as the out of plane wagging at 108 cm -1 and the deformation at 280 cm -1 , are photoactivated by the ultrafast part of the relaxation and modulate the pyranine-water molecule rearrangement, favoring the preparatory step for the photoreactivity.

Comparison of Numerical and Experimental Time-Resolved Near-Field Hall Thruster Plasma Properties

DTIC Science & Technology

2014-03-06

Near-Field Hall Thruster Plasma Properties 5a. CONTRACT NUMBER In-House 5b. GRANT NUMBER 5c. PROGRAM ELEMENT NUMBER 6. AUTHOR(S) 5d...Resolved Near-Field Hall Thruster Plasma Properties Ashley E. Gonzales, Justin W. Koo, and William A. Hargus, Jr. Abstract— Breathing mode oscillations... thruster , HPHall, plume emission. I. INTRODUCTION HALL thrusters are a plasma propulsion technologywidely used due to their low thrust, high specific impulse

Time-resolved optical spectroscopic quantification of red blood cell damage caused by cardiovascular devices

NASA Astrophysics Data System (ADS)

Sakota, D.; Sakamoto, R.; Sobajima, H.; Yokoyama, N.; Yokoyama, Y.; Waguri, S.; Ohuchi, K.; Takatani, S.

2008-02-01

Cardiovascular devices such as heart-lung machine generate un-physiological level of shear stress to damage red blood cells, leading to hemolysis. The diagnostic techniques of cell damages, however, have not yet been established. In this study, the time-resolved optical spectroscopy was applied to quantify red blood cell (RBC) damages caused by the extracorporeal circulation system. Experimentally, the fresh porcine blood was subjected to varying degrees of shear stress in the rotary blood pump, followed with measurement of the time-resolved transmission characteristics using the pico-second pulses at 651 nm. The propagated optical energy through the blood specimen was detected using a streak camera. The data were analyzed in terms of the mean cell volume (MCV) and mean cell hemoglobin concentration (MCHC) measured separately versus the energy and propagation time of the light pulses. The results showed that as the circulation time increased, the MCV increased with decrease in MCHC. It was speculated that the older RBCs with smaller size and fragile membrane properties had been selectively destroyed by the shear stress. The time-resolved optical spectroscopy is a useful technique in quantifying the RBCs' damages by measuring the energy and propagation time of the ultra-short light pulses through the blood.

Theoretical and experimental analysis of laser altimeters for barometric measurements over the ocean

NASA Technical Reports Server (NTRS)

Tsai, B. M.; Gardner, C. S.

1984-01-01

The statistical characteristics and the waveforms of ocean-reflected laser pulses are studied. The received signal is found to be corrupted by shot noise and time-resolved speckle. The statistics of time-resolved speckle and its effects on the timing accuracy of the receiver are studied in the general context of laser altimetry. For estimating the differential propagation time, various receiver timing algorithms are proposed and their performances evaluated. The results indicate that, with the parameters of a realistic altimeter, a pressure measurement accuracy of a few millibars is feasible. The data obtained from the first airborne two-color laser altimeter experiment are processed and analyzed. The results are used to verify the pressure measurement concept.

Dynamic evolution of light-induced orientation of dye-doped liquid crystals in liquid phase studied by time-resolved optically heterodyned optical Kerr effect technique.

PubMed

Yang, Pei; Liu, Liying; Xu, Lei

2008-02-28

Transient evolution of light-induced molecular reorientation both in 1-amino-anthraquinone (1AAQ) dye and azobenzene doped isotropic liquid crystals (LCs) were studied by time-resolved optically heterodyned optical Kerr effect method. The results give clear direct experimental proof that under short pulse (30 ps) excitation, LC molecules orientate toward the excitation light polarization direction in the 1AAQ/LC system. However, LC molecular orientation becomes orthogonal to the light polarization in azobenzene/LC system. Time-resolved excited-state absorption of 1AAQ and wavelength dependent excited-state absorption of azobenzene were also observed and their contributions to the early dynamics of the third order optical responses of the two systems were confirmed. A simplified two-level mean-field theory was derived to reveal the intensity dependence of orientation enhancement factor in azobenzene/LC system considering the photoisomerization process.

Asymmetrical Capacitors for Propulsion and the ISR Asymmetrical Capacitator Thruster, Experimental Results and Improved Designs

NASA Technical Reports Server (NTRS)

Canning, Francis; Winet, Ed; Ice, Bob; Melcher, Cory; Pesavento, Phil; Holmes, Alan; Butler, Carey; Cole, John; Campbell, Jonathan

2004-01-01

The outline of this viewgraph presentation on asymmetrical capacitor thruster development includes: 1) Test apparatus; 2) Devices tested; 3) Circuits used; 4) Data collected (Time averaged, Time resolved); 5) Patterns observed; 6) Force calculation; 7) Electrostatic modeling; 8) Understand it all.

Theoretical analysis of the time-resolved binary (e, 2e) binding energy spectra on three-body photodissociation of acetone at 195 nm

NASA Astrophysics Data System (ADS)

Yamazaki, M.; Nakayama, S.; Zhu, C. Y.; Takahashi, M.

2017-11-01

We report on theoretical progress in time-resolved (e, 2e) electron momentum spectroscopy of photodissociation dynamics of the deuterated acetone molecule at 195 nm. We have examined the predicted minimum energy reaction path to investigate whether associated (e, 2e) calculations meet the experimental results. A noticeable difference between the experiment and calculations has been found at around binding energy of 10 eV, suggesting that the observed difference may originate, at least partly, in ever-unconsidered non-minimum energy paths.

Time Resolved Digital PIV Measurements of Flow Field Cyclic Variation in an Optical IC Engine

NASA Astrophysics Data System (ADS)

Jarvis, S.; Justham, T.; Clarke, A.; Garner, C. P.; Hargrave, G. K.; Halliwell, N. A.

2006-07-01

Time resolved digital particle image velocimetry (DPIV) experimental data is presented for the in-cylinder flow field development of a motored four stroke spark ignition (SI) optical internal combustion (IC) engine. A high speed DPIV system was employed to quantify the velocity field development during the intake and compression stroke at an engine speed of 1500 rpm. The results map the spatial and temporal development of the in-cylinder flow field structure allowing comparison between traditional ensemble average and cycle average flow field structures. Conclusions are drawn with respect to engine flow field cyclic variations.

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

PubMed

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.

Elasticity and Anelasticity of Materials from Time-Resolved X-ray Diffraction

NASA Astrophysics Data System (ADS)

Sinogeikin, S. V.; Smith, J.; Lin, C.; Bai, L.; Rod, E.; Shen, G.

2014-12-01

Recent advances in synchrotron sources, x-ray optics, area detectors, and sample environment control have enabled many time-resolved experimental techniques for studying materials at extreme pressure and temperature conditions. The High Pressure Collaborative Access Team (HPCAT) at the Advanced Photon Source has made a sustained effort to develop and assemble a powerful collection of high-pressure apparatus for time-resolved research, and considerable time has been invested in developing techniques for collecting high-quality time-resolved x-ray scattering data. In this talk we will outline recently developed capabilities at HPCAT for studying elasticity and anelasticity of minerals using fast compression and cyclic compression-decompression. A few recent studies will be highlighted. For example, with fast x-ray area detectors having millisecond time resolution, accurate thermal equations of state of materials at temperatures up to 1000K and megabar pressures can be collected in a matter of seconds using membrane-driven diamond anvil cells (DAC), yielding unprecedented time and pressure resolution of true isotherms. Short duration of the experiments eliminates temperature variation during the experiments and in general allows volume measurements at higher pressures and temperatures. Alternatively, high-frequency (kilohertz range) radial diffraction measurements in a panoramic DAC combined with fast, precise cyclic loading/unloading by piezo drive could provide the short time scale necessary for studying rheology of minerals from the elastic response and lattice relaxation as a function of pressure, temperature and strain rate. Finally, we consider some possible future applications for time-resolved high-pressure, high-temperature research of mantle minerals.

Modeling and validation of heat and mass transfer in individual coffee beans during the coffee roasting process using computational fluid dynamics (CFD).

PubMed

Alonso-Torres, Beatriz; Hernández-Pérez, José Alfredo; Sierra-Espinoza, Fernando; Schenker, Stefan; Yeretzian, Chahan

2013-01-01

Heat and mass transfer in individual coffee beans during roasting were simulated using computational fluid dynamics (CFD). Numerical equations for heat and mass transfer inside the coffee bean were solved using the finite volume technique in the commercial CFD code Fluent; the software was complemented with specific user-defined functions (UDFs). To experimentally validate the numerical model, a single coffee bean was placed in a cylindrical glass tube and roasted by a hot air flow, using the identical geometrical 3D configuration and hot air flow conditions as the ones used for numerical simulations. Temperature and humidity calculations obtained with the model were compared with experimental data. The model predicts the actual process quite accurately and represents a useful approach to monitor the coffee roasting process in real time. It provides valuable information on time-resolved process variables that are otherwise difficult to obtain experimentally, but critical to a better understanding of the coffee roasting process at the individual bean level. This includes variables such as time-resolved 3D profiles of bean temperature and moisture content, and temperature profiles of the roasting air in the vicinity of the coffee bean.

Dynamics of the time-resolved stimulated Raman scattering spectrum in presence of transient vibronic inversion of population on the example of optically excited trans-β-apo-8{sup ′}-carotenal

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

Kardaś, T. M., E-mail: kardas@chem.uw.edu.pl; Ratajska-Gadomska, B.; Gadomski, W.

2014-05-28

We have studied the effect of transient vibrational inversion of population in trans-β-apo-8{sup ′}-carotenal on the time-resolved femtosecond stimulated Raman scattering (TR-FSRS) signal. The experimental data are interpreted by applying a quantum mechanical approach, using the formalism of projection operators for constructing the theoretical model of TR-FSRS. Within this theoretical frame we explain the presence of transient Raman losses on the Stokes side of the TR-FSRS spectrum as the effect of vibrational inversion of population. In view of the obtained experimental and theoretical results, we conclude that the excited S{sub 2} electronic level of trans-β-apo-8{sup ′}-carotenal relaxes towards the S{submore » 0} ground state through a set of four vibrational sublevels of S{sub 1} state.« less

A CTRW-based model of time-resolved fluorescence lifetime imaging in a turbid medium

NASA Astrophysics Data System (ADS)

Chernomordik, Victor; Gandjbakhche, Amir H.; Hassan, Moinuddin; Pajevic, Sinisa; Weiss, George H.

2010-12-01

We develop an analytic model of time-resolved fluorescent imaging of photons migrating through a semi-infinite turbid medium bounded by an infinite plane in the presence of a single stationary point fluorophore embedded in the medium. In contrast to earlier models of fluorescent imaging in which photon motion is assumed to be some form of continuous diffusion process, the present analysis is based on a continuous-time random walk (CTRW) on a simple cubic lattice, the objective being to estimate the position and lifetime of the fluorophore. This can provide information related to local variations in pH and temperature with potential medical significance. Aspects of the theory were tested using time-resolved measurements of the fluorescence from small inclusions inside tissue-like phantoms. The experimental results were found to be in good agreement with theoretical predictions provided that the fluorophore was not located too close to the planar boundary, a common problem in many diffusive systems.

Time-dependent photon migration imaging

NASA Astrophysics Data System (ADS)

Sevick, Eva M.; Wang, NaiGuang; Chance, Britton

1992-02-01

Recently, the application of both time- and frequency-resolved fluorescence techniques for the determination of photon migration characteristics in strongly scattering media has been used to characterize the optical properties in strongly scattering media. Specifically, Chance and coworkers have utilized measurement of photon migration characteristics to determine tissue hemoglobin absorbance and ultimately oxygenation status in homogeneous tissues. In this study, we present simulation results and experimental measurements for both techniques to show the capacity of time-dependent photon migration characteristics to image optically obscure absorbers located in strongly scattering media. The applications of time-dependent photon imaging in the biomedical community include imaging of light absorbing hematomas, tumors, hypoxic tissue volumes, and other tissue abnormalities. Herein, we show that the time-resolved parameter of mean photon path length, , and the frequency- resolved parameter of phase-shift, (theta) , can be used similarly to obtain three dimensional information of absorber position from two-dimensional measurements. Finally, we show that unlike imaging techniques that monitor the intensity of light without regard to the migration characteristics, the resolution of time-dependent photon migration measurements is enhanced by tissue scattering, further potentiating their use for biomedical imaging.

On the formation of anions: frequency-, angle-, and time-resolved photoelectron imaging of the menadione radical anion† †Electronic supplementary information (ESI) available: A summary of the ground-state geometries and molecular orbitals from the ab initio calculations; fitted residuals from the FA-PI simulation; plots of all spectra included in the frequency-resolved two-dimensional figure; and example time-resolved PE spectra from the 3.10 + 1.55 eV pump-probe experiments. See DOI: 10.1039/c4sc03491k Click here for additional data file.

PubMed Central

Bull, James N.; West, Christopher W.

2015-01-01

Frequency-, angle-, and time-resolved photoelectron imaging of gas-phase menadione (vitamin K3) radical anions was used to show that quasi-bound resonances of the anion can act as efficient doorway states to produce metastable ground electronic state anions on a sub-picosecond timescale. Several anion resonances have been experimentally observed and identified with the assistance of ab initio calculations, and ground state anion recovery was observed across the first 3 eV above threshold. Time-resolved measurements revealed the mechanism of electronic ground state anion formation, which first involves a cascade of very fast internal conversion processes to a bound electronic state that, in turn, decays by slower internal conversion to the ground state. Autodetachment processes from populated resonances are inefficient compared with electronic relaxation through internal conversion. The mechanistic understanding gained provides insight into the formation of radical anions in biological and astrochemical systems. PMID:29560245

Optical characterization of chemistry in shocked nitromethane with time-dependent density functional theory.

PubMed

Pellouchoud, Lenson A; Reed, Evan J

2013-11-27

We compute the optical properties of the liquid-phase energetic material nitromethane (CH3NO2) for the first 100 ps behind the front of a simulated shock at 6.5 km/s, close to the experimentally observed detonation shock speed of the material. We utilize molecular dynamics trajectories computed using the multiscale shock technique (MSST) for time-resolved optical spectrum calculations based on both linear response time-dependent DFT (TDDFT) and the Kubo-Greenwood formula with Kohn-Sham DFT wave functions. We find that the TDDFT method predicts an optical conductivity 25-35% lower than the Kubo-Greenwood calculation and provides better agreement with the experimentally measured index of refraction of unreacted nitromethane. We investigate the influence of electronic temperature on the Kubo-Greenwood spectra and find no significant effect at optical wavelengths. In both Kubo-Greenwood and TDDFT, the spectra evolve nonmonotonically in time as shock-induced chemistry takes place. We attribute the time-resolved absorption at optical wavelengths to time-dependent populations of molecular decomposition products, including NO, CNO, CNOH, H2O, and larger molecules. These calculations offer direction for guiding and interpreting ultrafast optical measurements on reactive materials.

Picosecond time-resolved measurements of dense plasma line shifts

DOE PAGES

Stillman, C. R.; Nilson, P. M.; Ivancic, S. T.; ...

2017-06-13

Picosecond time-resolved x-ray spectroscopy is used to measure the spectral line shift of the 1s2p–1s 2 transition in He-like Al ions as a function of the instantaneous plasma conditions. The plasma temperature and density are inferred from the Al He α complex using a nonlocal-thermodynamic-equilibrium atomic physics model. The experimental spectra show a linearly increasing red shift for electron densities of 1 to 5 × 10 23 cm –3. Furthermore, the measured line shifts are broadly consistent with a generalized analytic line-shift model based on calculations of a self-consistent field ion sphere model.

Picosecond time-resolved measurements of dense plasma line shifts

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

Stillman, C. R.; Nilson, P. M.; Ivancic, S. T.

Picosecond time-resolved x-ray spectroscopy is used to measure the spectral line shift of the 1s2p–1s 2 transition in He-like Al ions as a function of the instantaneous plasma conditions. The plasma temperature and density are inferred from the Al He α complex using a nonlocal-thermodynamic-equilibrium atomic physics model. The experimental spectra show a linearly increasing red shift for electron densities of 1 to 5 × 10 23 cm –3. Furthermore, the measured line shifts are broadly consistent with a generalized analytic line-shift model based on calculations of a self-consistent field ion sphere model.

Information hidden in the velocity distribution of ions and the exact kinetic Bohm criterion

NASA Astrophysics Data System (ADS)

Tsankov, Tsanko V.; Czarnetzki, Uwe

2017-05-01

Non-equilibrium distribution functions of electrons and ions play an important role in plasma physics. A prominent example is the kinetic Bohm criterion. Since its first introduction it has been controversial for theoretical reasons and due to the lack of experimental data, in particular on the ion distribution function. Here we resolve the theoretical as well as the experimental difficulties by an exact solution of the kinetic Boltzmann equation including charge exchange collisions and ionization. This also allows for the first time non-invasive measurement of spatially resolved ion velocity distributions, absolute values of the ion and electron densities, temperatures, and mean energies as well as the electric field and the plasma potential in the entire plasma. The non-invasive access to the spatially resolved distribution functions of electrons and ions is applied to the problem of the kinetic Bohm criterion. Theoretically a so far missing term in the criterion is derived and shown to be of key importance. With the new term the validity of the kinetic criterion at high collisionality and its agreement with the fluid picture are restored. All findings are supported by experimental data, theory and a numerical model with excellent agreement throughout.

Reaction-time-resolved measurements of laser-induced fluorescence in a shock tube with a single laser pulse

NASA Astrophysics Data System (ADS)

Zabeti, S.; Fikri, M.; Schulz, C.

2017-11-01

Shock tubes allow for the study of ultra-fast gas-phase reactions on the microsecond time scale. Because the repetition rate of the experiments is low, it is crucial to gain as much information as possible from each individual measurement. While reaction-time-resolved species concentration and temperature measurements with fast absorption methods are established, conventional laser-induced fluorescence (LIF) measurements with pulsed lasers provide data only at a single reaction time. Therefore, fluorescence methods have rarely been used in shock-tube diagnostics. In this paper, a novel experimental concept is presented that allows reaction-time-resolved LIF measurements with one single laser pulse using a test section that is equipped with several optical ports. After the passage of the shock wave, the reactive mixture is excited along the center of the tube with a 266-nm laser beam directed through a window in the end wall of the shock tube. The emitted LIF signal is collected through elongated sidewall windows and focused onto the entrance slit of an imaging spectrometer coupled to an intensified CCD camera. The one-dimensional spatial resolution of the measurement translates into a reaction-time-resolved measurement while the species information can be gained from the spectral axis of the detected two-dimensional image. Anisole pyrolysis was selected as the benchmark reaction to demonstrate the new apparatus.

Experimental set-up for time resolved small angle X-ray scattering studies of nanoparticles formation using a free-jet micromixer

NASA Astrophysics Data System (ADS)

Marmiroli, Benedetta; Grenci, Gianluca; Cacho-Nerin, Fernando; Sartori, Barbara; Laggner, Peter; Businaro, Luca; Amenitsch, Heinz

2010-02-01

Recently, we have designed, fabricated and tested a free-jet micromixer for time resolved small angle X-ray scattering (SAXS) studies of nanoparticles formation in the <100 μs time range. The microjet has a diameter of 25 μm and a time of first accessible measurement of 75 μs has been obtained. This result can still be improved. In this communication, we present a method to estimate whether a given chemical or biological reaction can be investigated with the micromixer, and to optimize the beam size for the measurement at the chosen SAXS beamline. Moreover, we describe a system based on stereoscopic imaging which allows the alignment of the jet with the X-ray beam with a precision of 20 μm. The proposed experimental procedures have been successfully employed to observe the formation of calcium carbonate (CaCO 3) nanoparticles from the reaction of sodium carbonate (Na 2CO 3) and calcium chloride (CaCl 2). The induction time has been estimated in the order of 200 μs and the determined radius of the particles is about 14 nm.

Automatic Gain Control in Compact Spectrometers.

PubMed

Protopopov, Vladimir

2016-03-01

An image intensifier installed in the optical path of a compact spectrometer may act not only as a fast gating unit, which is widely used for time-resolved measurements, but also as a variable attenuator-amplifier in a continuous wave mode. This opens the possibility of an automatic gain control, a new feature in spectroscopy. With it, the user is relieved from the necessity to manually adjust signal level at a certain value that it is done automatically by means of an electronic feedback loop. It is even more important that automatic gain control is done without changing exposure time, which is an additional benefit in time-resolved experiments. The concept, algorithm, design considerations, and experimental results are presented. © The Author(s) 2016.

Time-resolved measurements in diffuse reflectance: effects of the instrument response function of different detection systems on the depth sensitivity

NASA Astrophysics Data System (ADS)

Puszka, Agathe; Planat-Chrétien, Anne; Berger, Michel; Hervé, Lionel; Dinten, Jean-Marc

2014-02-01

We demonstrate the loss of depth sensitivity induced by the instrument response function on reflectance time-resolved diffuse optical tomography through the comparison of 3 detection systems: on one hand a photomultiplier tube (PMT) and a hybrid PMT coupled with a time-correlated single-photon counting card and on the other hand a high rate intensified camera. We experimentally evaluate the depth sensitivity achieved for each detection module with an absorbing inclusion embedded in a turbid medium. The different interfiber distances of 5, 10 and 15 mm are considered. Finally, we determine a maximal depth reached for each detection system by using 3D tomographic reconstructions based on the Mellin-Laplace transform.

Determination of blood oxygenation in the brain by time-resolved reflectance spectroscopy: influence of the skin, skull, and meninges

NASA Astrophysics Data System (ADS)

Hielscher, Andreas H.; Liu, Hanli; Wang, Lihong V.; 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.

Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop

NASA Astrophysics Data System (ADS)

Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young I.; Alpert, Bradley K.; Damrauer, Niels H.; Doriese, William B.; Fatur, Steven M.; Fowler, Joseph W.; Hilton, Gene C.; Jimenez, Ralph; Reintsema, Carl D.; Schmidt, Daniel R.; Silverman, Kevin L.; Swetz, Daniel S.; Tatsuno, Hideyuki; Ullom, Joel N.

2016-07-01

Experimental tools capable of monitoring both atomic and electronic structure on ultrafast (femtosecond to picosecond) time scales are needed for investigating photophysical processes fundamental to light harvesting, photocatalysis, energy and data storage, and optical display technologies. Time-resolved hard x-ray (>3 keV ) spectroscopies have proven valuable for these measurements due to their elemental specificity and sensitivity to geometric and electronic structures. Here, we present the first tabletop apparatus capable of performing time-resolved x-ray emission spectroscopy. The time resolution of the apparatus is better than 6 ps. By combining a compact laser-driven plasma source with a highly efficient array of microcalorimeter x-ray detectors, we are able to observe photoinduced spin changes in an archetypal polypyridyl iron complex [Fe (2 ,2'-bipyridine)3]2 + and accurately measure the lifetime of the quintet spin state. Our results demonstrate that ultrafast hard x-ray emission spectroscopy is no longer confined to large facilities and now can be performed in conventional laboratories with 10 times better time resolution than at synchrotrons. Our results are enabled, in part, by a 100- to 1000-fold increase in x-ray collection efficiency compared to current techniques.

Short-period cyclic loading system for in situ X-ray observation of anelastic properties at high pressure.

PubMed

Yoshino, Takashi; Yamazaki, Daisuke; Tange, Yoshinori; Higo, Yuji

2016-10-01

To determine the anelastic properties of materials of the Earth's interior, a short-period cyclic loading system was installed for in situ X-ray radiographic observation under high pressure to the multi-anvil deformation DIA press at the bending magnet beam line BL04B1 at SPring-8. The hydraulic system equipped with a piston controlled by a solenoid was designed so as to enable producing smooth sinusoidal stress in a wide range of oscillation period from 0.2 to 100 s and generating variable amplitudes. Time resolved X-ray radiography imaging of the sample and reference material provides their strain as a function of time during cyclic loading. A synchrotron X-ray radiation source allows us to resolve their strain variation with time even at the short period (<1 s). The minimum resolved strain is as small as 10 -4 , and the shortest oscillation period to detect small strain is 0.5 s. Preliminary experimental results exhibited that the new system can resolve attenuation factor Q -1 at upper mantle conditions. These results are in quantitative agreement with previously reported data obtained at lower pressures.

Chemistry resolved kinetic flow modeling of TATB based explosives

NASA Astrophysics Data System (ADS)

Vitello, Peter; Fried, Laurence E.; William, Howard; Levesque, George; Souers, P. Clark

2012-03-01

Detonation waves in insensitive, TATB-based explosives are believed to have multiple time scale regimes. The initial burn rate of such explosives has a sub-microsecond time scale. However, significant late-time slow release in energy is believed to occur due to diffusion limited growth of carbon. In the intermediate time scale concentrations of product species likely change from being in equilibrium to being kinetic rate controlled. We use the thermo-chemical code CHEETAH linked to an ALE hydrodynamics code to model detonations. We term our model chemistry resolved kinetic flow, since CHEETAH tracks the time dependent concentrations of individual species in the detonation wave and calculates EOS values based on the concentrations. We present here two variants of our new rate model and comparison with hot, ambient, and cold experimental data for PBX 9502.

Real-time absorption and scattering characterization of slab-shaped turbid samples obtained by a combination of angular and spatially resolved measurements.

PubMed

Dam, Jan S; Yavari, Nazila; Sørensen, Søren; Andersson-Engels, Stefan

2005-07-10

We present a fast and accurate method for real-time determination of the absorption coefficient, the scattering coefficient, and the anisotropy factor of thin turbid samples by using simple continuous-wave noncoherent light sources. The three optical properties are extracted from recordings of angularly resolved transmittance in addition to spatially resolved diffuse reflectance and transmittance. The applied multivariate calibration and prediction techniques are based on multiple polynomial regression in combination with a Newton--Raphson algorithm. The numerical test results based on Monte Carlo simulations showed mean prediction errors of approximately 0.5% for all three optical properties within ranges typical for biological media. Preliminary experimental results are also presented yielding errors of approximately 5%. Thus the presented methods show a substantial potential for simultaneous absorption and scattering characterization of turbid media.

Measurements of population densities of metastable and resonant levels of argon using laser induced fluorescence

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

Nikolić, M.; Newton, J.; Sukenik, C. I.

2015-01-14

We present a new approach to measure population densities of Ar I metastable and resonant excited states in low temperature Ar plasmas at pressures higher than 1 Torr. This approach combines the time resolved laser induced fluorescence technique with the kinetic model of Ar. The kinetic model of Ar is based on calculating the population rates of metastable and resonant levels by including contributions from the processes that affect population densities of Ar I excited states. In particular, we included collisional quenching processes between atoms in the ground state and excited states, since we are investigating plasma at higher pressures. Wemore » also determined time resolved population densities of Ar I 2 p excited states by employing optical emission spectroscopy technique. Time resolved Ar I excited state populations are presented for the case of the post-discharge of the supersonic flowing microwave discharge at pressures of 1.7 and 2.3 Torr. The experimental set-up consists of a pulsed tunable dye laser operating in the near infrared region and a cylindrical resonance cavity operating in TE{sub 111} mode at 2.45 GHz. Results show that time resolved population densities of Ar I metastable and resonant states oscillate with twice the frequency of the discharge.« less

Experimental Performance of a Genetic Algorithm for Airborne Strategic Conflict Resolution

NASA Technical Reports Server (NTRS)

Karr, David A.; Vivona, Robert A.; Roscoe, David A.; DePascale, Stephen M.; Consiglio, Maria

2009-01-01

The Autonomous Operations Planner, a research prototype flight-deck decision support tool to enable airborne self-separation, uses a pattern-based genetic algorithm to resolve predicted conflicts between the ownship and traffic aircraft. Conflicts are resolved by modifying the active route within the ownship s flight management system according to a predefined set of maneuver pattern templates. The performance of this pattern-based genetic algorithm was evaluated in the context of batch-mode Monte Carlo simulations running over 3600 flight hours of autonomous aircraft in en-route airspace under conditions ranging from typical current traffic densities to several times that level. Encountering over 8900 conflicts during two simulation experiments, the genetic algorithm was able to resolve all but three conflicts, while maintaining a required time of arrival constraint for most aircraft. Actual elapsed running time for the algorithm was consistent with conflict resolution in real time. The paper presents details of the genetic algorithm s design, along with mathematical models of the algorithm s performance and observations regarding the effectiveness of using complimentary maneuver patterns when multiple resolutions by the same aircraft were required.

Experimental Performance of a Genetic Algorithm for Airborne Strategic Conflict Resolution

NASA Technical Reports Server (NTRS)

Karr, David A.; Vivona, Robert A.; Roscoe, David A.; DePascale, Stephen M.; Consiglio, Maria

2009-01-01

The Autonomous Operations Planner, a research prototype flight-deck decision support tool to enable airborne self-separation, uses a pattern-based genetic algorithm to resolve predicted conflicts between the ownship and traffic aircraft. Conflicts are resolved by modifying the active route within the ownship's flight management system according to a predefined set of maneuver pattern templates. The performance of this pattern-based genetic algorithm was evaluated in the context of batch-mode Monte Carlo simulations running over 3600 flight hours of autonomous aircraft in en-route airspace under conditions ranging from typical current traffic densities to several times that level. Encountering over 8900 conflicts during two simulation experiments, the genetic algorithm was able to resolve all but three conflicts, while maintaining a required time of arrival constraint for most aircraft. Actual elapsed running time for the algorithm was consistent with conflict resolution in real time. The paper presents details of the genetic algorithm's design, along with mathematical models of the algorithm's performance and observations regarding the effectiveness of using complimentary maneuver patterns when multiple resolutions by the same aircraft were required.

Time-resolved observation of thermally activated rupture of a capillary-condensed water nanobridge

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

Bak, Wan; Sung, Baekman; Kim, Jongwoo

2015-01-05

The capillary-condensed liquid bridge is one of the most ubiquitous forms of liquid in nature and contributes significantly to adhesion and friction of biological molecules as well as microscopic objects. Despite its important role in nanoscience and technology, the rupture process of the bridge is not well understood and needs more experimental works. Here, we report real-time observation of rupture of a capillary-condensed water nanobridge in ambient condition. During slow and stepwise stretch of the nanobridge, we measured the activation time for rupture, or the latency time required for the bridge breakup. By statistical analysis of the time-resolved distribution ofmore » activation time, we show that rupture is a thermally activated stochastic process and follows the Poisson statistics. In particular, from the Arrhenius law that the rupture rate satisfies, we estimate the position-dependent activation energies for the capillary-bridge rupture.« less

Efficient use of single molecule time traces to resolve kinetic rates, models and uncertainties

NASA Astrophysics Data System (ADS)

Schmid, Sonja; Hugel, Thorsten

2018-03-01

Single molecule time traces reveal the time evolution of unsynchronized kinetic systems. Especially single molecule Förster resonance energy transfer (smFRET) provides access to enzymatically important time scales, combined with molecular distance resolution and minimal interference with the sample. Yet the kinetic analysis of smFRET time traces is complicated by experimental shortcomings—such as photo-bleaching and noise. Here we recapitulate the fundamental limits of single molecule fluorescence that render the classic, dwell-time based kinetic analysis unsuitable. In contrast, our Single Molecule Analysis of Complex Kinetic Sequences (SMACKS) considers every data point and combines the information of many short traces in one global kinetic rate model. We demonstrate the potential of SMACKS by resolving the small kinetic effects caused by different ionic strengths in the chaperone protein Hsp90. These results show an unexpected interrelation between conformational dynamics and ATPase activity in Hsp90.

Ejecta from Targets Strong and Weak: Experimental Measurements of Strength Controlled and Strengthless Craters

NASA Astrophysics Data System (ADS)

Hermalyn, B.

2014-09-01

This study presents novel time-resolved 3D measurements of the impact ejecta through crater formation and the arresting process that ceases growth into a variety of targets exhibiting a spectrum of different strengths of interest on planetary bodies.

Using Separable Nonnegative Matrix Factorization Techniques for the Analysis of Time-Resolved Raman Spectra

NASA Astrophysics Data System (ADS)

Luce, R.; Hildebrandt, P.; Kuhlmann, U.; Liesen, J.

2016-09-01

The key challenge of time-resolved Raman spectroscopy is the identification of the constituent species and the analysis of the kinetics of the underlying reaction network. In this work we present an integral approach that allows for determining both the component spectra and the rate constants simultaneously from a series of vibrational spectra. It is based on an algorithm for non-negative matrix factorization which is applied to the experimental data set following a few pre-processing steps. As a prerequisite for physically unambiguous solutions, each component spectrum must include one vibrational band that does not significantly interfere with vibrational bands of other species. The approach is applied to synthetic "experimental" spectra derived from model systems comprising a set of species with component spectra differing with respect to their degree of spectral interferences and signal-to-noise ratios. In each case, the species involved are connected via monomolecular reaction pathways. The potential and limitations of the approach for recovering the respective rate constants and component spectra are discussed.

Luminescence lifetime enhanced by exciton-plasmon couple in hybrid CsPbBr3 perovskite/Pt nanostructure

NASA Astrophysics Data System (ADS)

Liu, Chunxu; Zhang, Jisen; Chen, Yongyi; Jing, Pengtao; Zhang, Ligong; Zhao, Haifeng; Fu, Xihong; Wang, Lijun

2018-02-01

Photoluminescence (PL) and time-resolved spectroscopic studies on plasmonically coupled semiconductor nanoparticles (SNPs) have demonstrated the PL quenched and lifetime enhanced of SNPs in the presence of metal nanoparticles (MNPs). The hybrid colloidal CsPbBr3 perovskite SNPs/Pt MNPs (S-M) structures exhibit novel optical properties due to the synergetic interaction between the individual components. In hybrid S-M nanostructures colloidal chemistry incorporates SNP and MNP into a single unit resulting in the formation of plexciton (or excimon) which has now been established in a series of hybrid structures. The experimental results of femtosecond transient absorption (TA) spectroscopy based on the time-resolved pump-probe confirm the transformation from excitons to plexcitons. It was found that the experimental data can’t be well described by the theory based on conventional Fӧster resonance energy transfer (FRET). The differences between theory and experiment may be due to the missing some PbBr2 PL peaks, the reason will be revealed further.

A transmission-grating-modulated pump-probe absorption spectroscopy and demonstration of diffusion dynamics of photoexcited carriers in bulk intrinsic GaAs film.

PubMed

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

2012-02-13

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

Temporally resolved diagnosis of an atmospheric-pressure pulse-modulated argon surface wave plasma by optical emission spectroscopy

NASA Astrophysics Data System (ADS)

Chen, Chuan-Jie; Li, Shou-Zhe; Zhang, Jialiang; Liu, Dongping

2018-01-01

A pulse-modulated argon surface wave plasma generated at atmospheric pressure is characterized by means of temporally resolved optical emission spectroscopy (OES). The temporal evolution of the gas temperature, the electron temperature and density, the radiative species of atomic Ar, and the molecular band of OH(A) and N2(C) are investigated experimentally by altering the instantaneous power, pulse repetitive frequency, and duty ratio. We focused on the physical phenomena occurring at the onset of the time-on period and after the power interruption at the start of the time-off period. Meanwhile, the results are discussed qualitatively for an in-depth insight of its dynamic evolution.

Experimental validation of a numerical model predicting the charging characteristics of Teflon and Kapton under electron beam irradiation

NASA Technical Reports Server (NTRS)

Hazelton, R. C.; Yadlowsky, E. J.; Churchill, R. J.; Parker, L. W.; Sellers, B.

1981-01-01

The effect differential charging of spacecraft thermal control surfaces is assessed by studying the dynamics of the charging process. A program to experimentally validate a computer model of the charging process was established. Time resolved measurements of the surface potential were obtained for samples of Kapton and Teflon irradiated with a monoenergetic electron beam. Results indicate that the computer model and experimental measurements agree well and that for Teflon, secondary emission is the governing factor. Experimental data indicate that bulk conductivities play a significant role in the charging of Kapton.

Femtosecond timing measurement and control using ultrafast organic thin films

NASA Astrophysics Data System (ADS)

Naruse, Makoto; Mitsu, Hiroyuki; Furuki, Makoto; Iwasa, Izumi; Sato, Yasuhiro; Tatsuura, Satoshi; Tian, Minquan

2003-12-01

We show a femtosecond timing measurement and control technique using a squarylium dye J-aggregate film, which is an organic thin film that acts as an ultrafast two-dimensional optical switch. Optical pulse timing is directly mapped to space-domain position on the film, and the large area and ultrafast response offer a femtosecond-resolved, large dynamic range, real-time, multichannel timing measurement capability. A timing fluctuation (jitter, wander, and skew) reduction architecture is presented and experimentally demonstrated.

Time-resolved photoacoustic measurement for evaluation of viscoelastic properties of biological tissues

NASA Astrophysics Data System (ADS)

Zhao, Yue; Chen, Conggui; Liu, Hongwei; Yang, Sihua; Xing, Da

2016-11-01

In this letter, we proposed a method for viscoelastic characterization of biological tissues based on time-resolved photoacoustic measurement. The theoretical and experimental study was performed on the influence of viscoelasticity effects on photoacoustic generation. Taking the time delay between the photoacoustic signal and the exciting laser, the viscoelasticity distribution of biological tissues can be mapped. To validate our method, gelatin phantoms with different densities were measured. We also applied this method in discrimination between fat and liver to confirm the usefulness of the viscoelastic evaluation. Furthermore, pilot experiments were performed on atherosclerosis artery from an apolipoprotein E-knockout mouse to show the viscoelastic characterization of atherosclerotic plaque. Our results demonstrate that this technique has the potential for visualizing the biomechanical properties and lesions of biological tissues.

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

NASA Astrophysics Data System (ADS)

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.

Chemistry Resolved Kinetic Flow Modeling of TATB Based Explosives

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

Vitello, P A; Fried, L E; Howard, W M

2011-07-21

Detonation waves in insensitive, TATB based explosives are believed to have multi-time scale regimes. The initial burn rate of such explosives has a sub-microsecond time scale. However, significant late-time slow release in energy is believed to occur due to diffusion limited growth of carbon. In the intermediate time scale concentrations of product species likely change from being in equilibrium to being kinetic rate controlled. They use the thermo-chemical code CHEETAH linked to an ALE hydrodynamics code to model detonations. They term their model chemistry resolved kinetic flow as CHEETAH tracks the time dependent concentrations of individual species in the detonationmore » wave and calculates EOS values based on the concentrations. A HE-validation suite of model simulations compared to experiments at ambient, hot, and cold temperatures has been developed. They present here a new rate model and comparison with experimental data.« less

Direct Observation of the Surface Segregation of Cu in Pd by Time-Resolved Positron-Annihilation-Induced Auger Electron Spectroscopy

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

Mayer, J.; Hugenschmidt, C.; Schreckenbach, K.

2010-11-12

Density functional theory calculations predict the surface segregation of Cu in the second atomic layer of Pd which has not been unambiguously confirmed by experiment so far. We report measurements on Pd surfaces covered with three and six monolayers of Cu using element selective positron-annihilation-induced Auger electron spectroscopy (PAES) which is sensitive to the topmost atomic layer. Moreover, time-resolved PAES, which was applied for the first time, enables the investigation of the dynamics of surface atoms and hence the observation of the segregation process. The time constant for segregation was experimentally determined to {tau}=1.38(0.21) h, and the final segregated configurationmore » was found to be consistent with calculations. Time-dependent PAES is demonstrated to be a novel element selective technique applicable for the investigation of, e.g., heterogeneous catalysis, corrosion, or surface alloying.« less

Direct Observation of the Surface Segregation of Cu in Pd by Time-Resolved Positron-Annihilation-Induced Auger Electron Spectroscopy

NASA Astrophysics Data System (ADS)

Mayer, J.; Hugenschmidt, C.; Schreckenbach, K.

2010-11-01

Density functional theory calculations predict the surface segregation of Cu in the second atomic layer of Pd which has not been unambiguously confirmed by experiment so far. We report measurements on Pd surfaces covered with three and six monolayers of Cu using element selective positron-annihilation-induced Auger electron spectroscopy (PAES) which is sensitive to the topmost atomic layer. Moreover, time-resolved PAES, which was applied for the first time, enables the investigation of the dynamics of surface atoms and hence the observation of the segregation process. The time constant for segregation was experimentally determined to τ=1.38(0.21)h, and the final segregated configuration was found to be consistent with calculations. Time-dependent PAES is demonstrated to be a novel element selective technique applicable for the investigation of, e.g., heterogeneous catalysis, corrosion, or surface alloying.

Shock compression response of cold-rolled Ni/Al multilayer composites

DOE PAGES

Specht, Paul E.; Weihs, Timothy P.; Thadhani, Naresh N.

2017-01-06

Uniaxial strain, plate-on-plate impact experiments were performed on cold-rolled Ni/Al multilayer composites and the resulting Hugoniot was determined through time-resolved measurements combined with impedance matching. The experimental Hugoniot agreed with that previously predicted by two dimensional (2D) meso-scale calculations. Additional 2D meso-scale simulations were performed using the same computational method as the prior study to reproduce the experimentally measured free surface velocities and stress profiles. Finally, these simulations accurately replicated the experimental profiles, providing additional validation for the previous computational work.

Pressure spectra from single-snapshot tomographic PIV

NASA Astrophysics Data System (ADS)

Schneiders, Jan F. G.; Avallone, Francesco; Pröbsting, Stefan; Ragni, Daniele; Scarano, Fulvio

2018-03-01

The power spectral density and coherence of temporal pressure fluctuations are obtained from low-repetition-rate tomographic PIV measurements. This is achieved by extension of recent single-snapshot pressure evaluation techniques based upon the Taylor's hypothesis (TH) of frozen turbulence and vortex-in-cell (VIC) simulation. Finite time marching of the measured instantaneous velocity fields is performed using TH and VIC. Pressure is calculated from the resulting velocity time series. Because of the theoretical limitations, the finite time marching can be performed until the measured flow structures are convected out of the measurement volume. This provides a lower limit of resolvable frequency range. An upper limit is given by the spatial resolution of the measurements. Finite time-marching approaches are applied to low-repetition-rate tomographic PIV data of the flow past a straight trailing edge at 10 m/s. Reference results of the power spectral density and coherence are obtained from surface pressure transducers. In addition, the results are compared to state-of-the-art experimental data obtained from time-resolved tomographic PIV performed at 10 kHz. The time-resolved approach suffers from low spatial resolution and limited maximum acquisition frequency because of hardware limitations. Additionally, these approaches strongly depend upon the time kernel length chosen for pressure evaluation. On the other hand, the finite time-marching approaches make use of low-repetition-rate tomographic PIV measurements that offer higher spatial resolution. Consequently, increased accuracy of the power spectral density and coherence of pressure fluctuations are obtained in the high-frequency range, in comparison to the time-resolved measurements. The approaches based on TH and VIC are found to perform similarly in the high-frequency range. At lower frequencies, TH is found to underestimate coherence and intensity of the pressure fluctuations in comparison to time-resolved PIV and the microphone reference data. The VIC-based approach, on the other hand, returns results on the order of the reference.

Photoelectron Angular Distributions of Transition Metal Dioxide Anions - a joint experimental and theoretical study

NASA Astrophysics Data System (ADS)

Iordanov, Ivan; Gunaratne, Dasitha; Harmon, Christopher; Sofo, Jorge; Castleman, A. W., Jr.

2012-02-01

Angular-resolved photoelectron spectroscopy (PES) studies of the MO2- (M=Ti, Zr, Hf, Co, Rh) clusters are presented for the first time along with theoretical calculations of their properties. We confirm previously reported non-angular PES results for the vertical detachment energies (VDE), vibrational energies and geometric structures of these clusters and further explore the effect of the 'lanthanide contraction' on the MO2- clusters by comparing the electronic spectra of 4d and 5d transition metal dioxides. Angular-resolved PES provides the angular momentum contributions to the HOMO of these clusters and we use theoretical calculations to examine the HOMO and compare to our experimental results. First-principles calculations are done using both density functional theory (DFT) and the coupled-cluster, singles, doubles and triples (CCSD(T)) methods.

An efficient and accurate approach to MTE-MART for time-resolved tomographic PIV

NASA Astrophysics Data System (ADS)

Lynch, K. P.; Scarano, F.

2015-03-01

The motion-tracking-enhanced MART (MTE-MART; Novara et al. in Meas Sci Technol 21:035401, 2010) has demonstrated the potential to increase the accuracy of tomographic PIV by the combined use of a short sequence of non-simultaneous recordings. A clear bottleneck of the MTE-MART technique has been its computational cost. For large datasets comprising time-resolved sequences, MTE-MART becomes unaffordable and has been barely applied even for the analysis of densely seeded tomographic PIV datasets. A novel implementation is proposed for tomographic PIV image sequences, which strongly reduces the computational burden of MTE-MART, possibly below that of regular MART. The method is a sequential algorithm that produces a time-marching estimation of the object intensity field based on an enhanced guess, which is built upon the object reconstructed at the previous time instant. As the method becomes effective after a number of snapshots (typically 5-10), the sequential MTE-MART (SMTE) is most suited for time-resolved sequences. The computational cost reduction due to SMTE simply stems from the fewer MART iterations required for each time instant. Moreover, the method yields superior reconstruction quality and higher velocity field measurement precision when compared with both MART and MTE-MART. The working principle is assessed in terms of computational effort, reconstruction quality and velocity field accuracy with both synthetic time-resolved tomographic images of a turbulent boundary layer and two experimental databases documented in the literature. The first is the time-resolved data of flow past an airfoil trailing edge used in the study of Novara and Scarano (Exp Fluids 52:1027-1041, 2012); the second is a swirling jet in a water flow. In both cases, the effective elimination of ghost particles is demonstrated in number and intensity within a short temporal transient of 5-10 frames, depending on the seeding density. The increased value of the velocity space-time correlation coefficient demonstrates the increased velocity field accuracy of SMTE compared with MART.

In-situ straining and time-resolved electron tomography data acquisition in a transmission electron microscope.

PubMed

Hata, S; Miyazaki, S; Gondo, T; Kawamoto, K; Horii, N; Sato, K; Furukawa, H; Kudo, H; Miyazaki, H; Murayama, M

2017-04-01

This paper reports the preliminary results of a new in-situ three-dimensional (3D) imaging system for observing plastic deformation behavior in a transmission electron microscope (TEM) as a directly relevant development of the recently reported straining-and-tomography holder [Sato K et al. (2015) Development of a novel straining holder for transmission electron microscopy compatible with single tilt-axis electron tomography. Microsc. 64: 369-375]. We designed an integrated system using the holder and newly developed straining and image-acquisition software and then developed an experimental procedure for in-situ straining and time-resolved electron tomography (ET) data acquisition. The software for image acquisition and 3D visualization was developed based on the commercially available ET software TEMographyTM. We achieved time-resolved 3D visualization of nanometer-scale plastic deformation behavior in a Pb-Sn alloy sample, thus demonstrating the capability of this system for potential applications in materials science. © The Author 2016. Published by Oxford University Press on behalf of The Japanese Society of Microscopy. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

Efficient calculation of open quantum system dynamics and time-resolved spectroscopy with distributed memory HEOM (DM-HEOM).

PubMed

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.

Assessment of swirl spray interaction in lab scale combustor using time-resolved measurements

NASA Astrophysics Data System (ADS)

Rajamanickam, Kuppuraj; Jain, Manish; Basu, Saptarshi

2017-11-01

Liquid fuel injection in highly turbulent swirling flows becomes common practice in gas turbine combustors to improve the flame stabilization. It is well known that the vortex bubble breakdown (VBB) phenomenon in strong swirling jets exhibits complicated flow structures in the spatial domain. In this study, the interaction of hollow cone liquid sheet with such coaxial swirling flow field has been studied experimentally using time-resolved measurements. In particular, much attention is focused towards the near field breakup mechanism (i.e. primary atomization) of liquid sheet. The detailed swirling gas flow field characterization is carried out using time-resolved PIV ( 3.5 kHz). Furthermore, the complicated breakup mechanisms and interaction of the liquid sheet are imaged with the help of high-speed shadow imaging system. Subsequently, proper orthogonal decomposition (POD) and dynamic mode decomposition (DMD) is implemented over the instantaneous data sets to retrieve the modal information associated with the interaction dynamics. This helps to delineate more quantitative nature of interaction process between the liquid sheet and swirling gas phase flow field.

Spectroscopic Diagnosis of Excited-State Aromaticity: Capturing Electronic Structures and Conformations upon Aromaticity Reversal.

PubMed

Oh, Juwon; Sung, Young Mo; Hong, Yongseok; Kim, Dongho

2018-03-06

Aromaticity, the special energetic stability derived from cyclic [4 n + 2]π-conjugated electronic structures, has been the topic of intense interest in chemistry because it plays a critical role in rationalizing molecular stability, reactivity, and physical/chemical properties. Recently, the pioneering work by Colin Baird on aromaticity reversal, postulating that aromatic (antiaromatic) character in the ground state reverses to antiaromatic (aromatic) character in the lowest excited triplet state, has attracted much scientific attention. The completely reversed aromaticity in the excited state provides direct insight into understanding the photophysical/chemical properties of photoactive materials. In turn, the application of aromatic molecules to photoactive materials has led to numerous studies revealing this aromaticity reversal. However, most studies of excited-state aromaticity have been based on the theoretical point of view. The experimental evaluation of aromaticity in the excited state is still challenging and strenuous because the assessment of (anti)aromaticity with conventional magnetic, energetic, and geometric indices is difficult in the excited state, which practically restricts the extension and application of the concept of excited-state aromaticity. Time-resolved optical spectroscopies can provide a new and alternative avenue to evaluate excited-state aromaticity experimentally while observing changes in the molecular features in the excited states. Time-resolved optical spectroscopies take advantage of ultrafast laser pulses to achieve high time resolution, making them suitable for monitoring ultrafast changes in the excited states of molecular systems. This can provide valuable information for understanding the aromaticity reversal. This Account presents recent breakthroughs in the experimental assessment of excited-state aromaticity and the verification of aromaticity reversal with time-resolved optical spectroscopic measurements. To scrutinize this intriguing and challenging scientific issue, expanded porphyrins have been utilized as the ideal testing platform for investigating aromaticity because they show distinct aromatic and antiaromatic characters with aromaticity-specific spectroscopic features. Expanded porphyrins exhibit perfect aromatic and antiaromatic congener pairs having the same molecular framework but different numbers of π electrons, which facilitates the study of the pure effect of aromaticity by comparative analyses. On the basis of the characteristics of expanded porphyrins, time-resolved electronic and vibrational absorption spectroscopies capture the changes in electronic structure and molecular conformations driven by the change in aromaticity and provide clear evidence for aromaticity reversal in the excited states. The approaches described in this Account pave the way for the development of new and alternative experimental indices for the evaluation of excited-state aromaticity, which will enable overarching and fundamental comprehension of the role of (anti)aromaticity in the stability, dynamics, and reactivity in the excited states with possible implications for practical applications.

Novel physical chemistry approaches in biophysical researches with advanced application of lasers: Detection and manipulation.

PubMed

Iwata, Koichi; Terazima, Masahide; Masuhara, Hiroshi

2018-02-01

Novel methodologies utilizing pulsed or intense CW irradiation obtained from lasers have a major impact on biological sciences. In this article, recent development in biophysical researches fully utilizing the laser irradiation is described for three topics, time-resolved fluorescence spectroscopy, time-resolved thermodynamics, and manipulation of the biological assemblies by intense laser irradiation. First, experimental techniques for time-resolved fluorescence spectroscopy are concisely explained in Section 2. As an example of the recent application of time-resolved fluorescence spectroscopy to biological systems, evaluation of the viscosity of lipid bilayer membranes is described. The results of the spectroscopic experiments strongly suggest the presence of heterogeneous membrane structure with two different viscosity values in liposomes formed by a single phospholipid. Section 3 covers the time-resolved thermodynamics. Thermodynamical properties are important to characterize biomolecules. However, measurement of these quantities for short-lived intermediate species has been impossible by traditional thermodynamical techniques. Recently, development of a spectroscopic method based on the transient grating method enables us to measure these quantities and also to elucidate reaction kinetics which cannot be detected by other spectroscopic methods. The principle of the measurements and applications to some protein reactions are reviewed. Manipulation and fabrication of supramolecues, amino acids, proteins, and living cells by intense laser irradiation are described in Section 4. Unconventional assembly, crystallization and growth, amyloid fibril formation, and living cell manipulation are achieved by CW laser trapping and femtosecond laser-induced cavitation bubbling. Their spatio-temporal controllability is opening a new avenue in the relevant molecular and bioscience research fields. This article is part of a Special Issue entitled "Biophysical Exploration of Dynamical Ordering of Biomolecular Systems" edited by Dr. Koichi Kato. Copyright © 2017. Published by Elsevier B.V.

Observation and modeling of interspecies ion separation in inertial confinement fusion implosions via imaging x-ray spectroscopy

DOE PAGES

Joshi, Tirtha Raj; Hakel, Peter; Hsu, Scott C.; ...

2017-03-22

In this article, we report the first direct experimental evidence of interspecies ion separation in direct-drive inertial confinement fusion experiments performed at the OMEGA laser facility via spectrally, temporally, and spatially resolved imaging x-ray-spectroscopy data [S. C. Hsu et al., Europhys. Lett. 115, 65001 (2016)]. These experiments were designed based on the expectation that interspecies ion thermo-diffusion would be the strongest for species with a large mass and charge difference. The targets were spherical plastic shells filled with D2 and a trace amount of Ar (0.1% or 1% by atom). Ar K-shell spectral features were observed primarily between the timemore » of first-shock convergence and slightly before the neutron bang time, using a time- and space-integrated spectrometer, a streaked crystal spectrometer, and two gated multi-monochromatic x-ray imagers fielded along quasi-orthogonal lines of sight. Detailed spectroscopic analyses of spatially resolved Ar K-shell lines reveal the deviation from the initial 1% Ar gas fill and show both Ar-concentration enhancement and depletion at different times and radial positions of the implosion. The experimental results are interpreted using radiation-hydrodynamic simulations that include recently implemented, first-principles models of interspecies ion diffusion. Lastly, the experimentally inferred Ar-atom fraction profiles agree reasonably with calculated profiles associated with the incoming and rebounding first shock.« less

Rapid detection of trace amounts of surfactants using nanoparticles in fluorometric assays

NASA Astrophysics Data System (ADS)

Härmä, Harri; Laakso, Susana; Pihlasalo, Sari; Hänninen, Pekka; Faure, Bertrand; Rana, Subhasis; Bergström, Lennart

2010-01-01

Rapid microtiter assays that utilize the time-resolved fluorescence resonance energy transfer or quenching of dye-labeled proteins adsorbed onto the surfaces of polystyrene or maghemite nanoparticles have been developed for the detection and quantification of trace amounts of surfactants at concentrations down to 10 nM.Rapid microtiter assays that utilize the time-resolved fluorescence resonance energy transfer or quenching of dye-labeled proteins adsorbed onto the surfaces of polystyrene or maghemite nanoparticles have been developed for the detection and quantification of trace amounts of surfactants at concentrations down to 10 nM. Electronic supplementary information (ESI) available: Experimental details and Fig. S1 and S2. See DOI: 10.1039/b9nr00172g

Time resolved photo-luminescent decay characterization of mercury cadmium telluride focal plane arrays

DOE PAGES

Soehnel, Grant

2015-01-20

The minority carrier lifetime is a measurable material property that is an indication of infrared detector device performance. To study the utility of measuring the carrier lifetime, an experiment has been constructed that can time resolve the photo-luminescent decay of a detector or wafer sample housed inside a liquid nitrogen cooled Dewar. Motorized stages allow the measurement to be scanned over the sample surface, and spatial resolutions as low as 50µm have been demonstrated. A carrier recombination simulation was developed to analyze the experimental data. Results from measurements performed on 4 mercury cadmium telluride focal plane arrays show strong correlationmore » between spatial maps of the lifetime, dark current, and relative response.« less

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

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

Weber, S. J., E-mail: sebastien.weber@cea.fr; Manschwetus, B.; Billon, M.

2015-03-15

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

Electron heating and thermal relaxation of gold nanorods revealed by two-dimensional electronic spectroscopy.

PubMed

Lietard, Aude; Hsieh, Cho-Shuen; Rhee, Hanju; Cho, Minhaeng

2018-03-01

To elucidate the complex interplay between the size and shape of gold nanorods and their electronic, photothermal, and optical properties for molecular imaging, photothermal therapy, and optoelectronic devices, it is a prerequisite to characterize ultrafast electron dynamics in gold nanorods. Time-resolved transient absorption (TA) studies of plasmonic electrons in various nanostructures have revealed the time scales for electron heating, lattice vibrational excitation, and phonon relaxation processes in condensed phases. However, because linear spectroscopic and time-resolved TA signals are vulnerable to inhomogeneous line-broadening, pure dephasing and direct electron heating effects are difficult to observe. Here we show that femtosecond two-dimensional electronic spectroscopy, with its unprecedented time resolution and phase sensitivity, can be used to collect direct experimental evidence for ultrafast electron heating, anomalously strong coherent and transient electronic plasmonic responses, and homogenous dephasing processes resulting from electron-vibration couplings even for polydisperse gold nanorods.

Quantum control via a genetic algorithm of the field ionization pathway of a Rydberg electron

NASA Astrophysics Data System (ADS)

Gregoric, Vincent C.; Kang, Xinyue; Liu, Zhimin Cheryl; Rowley, Zoe A.; Carroll, Thomas J.; Noel, Michael W.

2017-08-01

Quantum control of the pathway along which a Rydberg electron field ionizes is experimentally and computationally demonstrated. Selective field ionization is typically done with a slowly rising electric field pulse. The (1/n*)4 scaling of the classical ionization threshold leads to a rough mapping between arrival time of the electron signal and principal quantum number of the Rydberg electron. This is complicated by the many avoided level crossings that the electron must traverse on the way to ionization, which in general leads to broadening of the time-resolved field ionization signal. In order to control the ionization pathway, thus directing the signal to the desired arrival time, a perturbing electric field produced by an arbitrary wave-form generator is added to a slowly rising electric field. A genetic algorithm evolves the perturbing field in an effort to achieve the target time-resolved field ionization signal.

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

Rameau, J. D.; Freutel, S.; Kemper, A. F.

We report that in complex materials various interactions have important roles in determining electronic properties. Angle-resolved photoelectron spectroscopy (ARPES) is used to study these processes by resolving the complex single-particle self-energy and quantifying how quantum interactions modify bare electronic states. However, ambiguities in the measurement of the real part of the self-energy and an intrinsic inability to disentangle various contributions to the imaginary part of the self-energy can leave the implications of such measurements open to debate. Here we employ a combined theoretical and experimental treatment of femtosecond time-resolved ARPES (tr-ARPES) show how population dynamics measured using tr-ARPES can bemore » used to separate electron–boson interactions from electron–electron interactions. In conclusion, we demonstrate a quantitative analysis of a well-defined electron–boson interaction in the unoccupied spectrum of the cuprate Bi 2Sr 2CaCu 2O 8+x characterized by an excited population decay time that maps directly to a discrete component of the equilibrium self-energy not readily isolated by static ARPES experiments.« less

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

NASA Astrophysics Data System (ADS)

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.

Real-time spectral interferometry probes the internal dynamics of femtosecond soliton molecules

NASA Astrophysics Data System (ADS)

Herink, G.; Kurtz, F.; Jalali, B.; Solli, D. R.; Ropers, C.

2017-04-01

Solitons, particle-like excitations ubiquitous in many fields of physics, have been shown to exhibit bound states akin to molecules. The formation of such temporal soliton bound states and their internal dynamics have escaped direct experimental observation. By means of an emerging time-stretch technique, we resolve the evolution of femtosecond soliton molecules in the cavity of a few-cycle mode-locked laser. We track two- and three-soliton bound states over hundreds of thousands of consecutive cavity roundtrips, identifying fixed points and periodic and aperiodic molecular orbits. A class of trajectories acquires a path-dependent geometrical phase, implying that its dynamics may be topologically protected. These findings highlight the importance of real-time detection in resolving interactions in complex nonlinear systems, including the dynamics of soliton bound states, breathers, and rogue waves.

Determining the nature of excitonic dephasing in high-quality GaN/AlGaN quantum wells through time-resolved and spectrally resolved four-wave mixing spectroscopy

NASA Astrophysics Data System (ADS)

Gallart, M.; Ziegler, M.; Crégut, O.; Feltin, E.; Carlin, J.-F.; Butté, R.; Grandjean, N.; Hönerlage, B.; Gilliot, P.

2017-07-01

Applying four-wave mixing spectroscopy to a high-quality GaN/AlGaN single quantum well, we report on the experimental determination of excitonic dephasing times at different temperatures and exciton densities in III-nitride heterostructures. By comparing the evolution with the temperature of the dephasing and the spin-relaxation rate, we conclude that both processes are related to the rate of excitonic collisions. When spin relaxation occurs in the motional-narrowing regime, it remains constant over a large temperature range as the spin-precession frequency increases linearly with temperature, hence compensating for the observed decrease in the dephasing time. From those measurements, a value of the electron-hole exchange interaction strength of 0.45 meV at T =10 K is inferred.

Time-resolved structural dynamics of thin metal films heated with femtosecond optical pulses.

PubMed

Chen, Jie; Chen, Wei-Kan; Tang, Jau; Rentzepis, Peter M

2011-11-22

We utilize 100 fs optical pulses to induce ultrafast disorder of 35- to 150-nm thick single Au(111) crystals and observe the subsequent structural evolution using 0.6-ps, 8.04-keV X-ray pulses. Monitoring the picosecond time-dependent modulation of the X-ray diffraction intensity, width, and shift, we have measured directly electron/phonon coupling, phonon/lattice interaction, and a histogram of the lattice disorder evolution, such as lattice breath due to a pressure wave propagating at sonic velocity, lattice melting, and recrystallization, including mosaic formation. Results of theoretical simulations agree and support the experimental data of the lattice/liquid phase transition process. These time-resolved X-ray diffraction data provide a detailed description of all the significant processes induced by ultrafast laser pulses impinging on thin metallic single crystals.

Concept of proton radiography using energy resolved dose measurement.

PubMed

Bentefour, El H; Schnuerer, Roland; Lu, Hsiao-Ming

2016-08-21

Energy resolved dosimetry offers a potential path to single detector based proton imaging using scanned proton beams. This is because energy resolved dose functions encrypt the radiological depth at which the measurements are made. When a set of predetermined proton beams 'proton imaging field' are used to deliver a well determined dose distribution in a specific volume, then, at any given depth x of this volume, the behavior of the dose against the energies of the proton imaging field is unique and characterizes the depth x. This concept applies directly to proton therapy scanning delivery methods (pencil beam scanning and uniform scanning) and it can be extended to the proton therapy passive delivery methods (single and double scattering) if the delivery of the irradiation is time-controlled with a known time-energy relationship. To derive the water equivalent path length (WEPL) from the energy resolved dose measurement, one may proceed in two different ways. A first method is by matching the measured energy resolved dose function to a pre-established calibration database of the behavior of the energy resolved dose in water, measured over the entire range of radiological depths with at least 1 mm spatial resolution. This calibration database can also be made specific to the patient if computed using the patient x-CT data. A second method to determine the WEPL is by using the empirical relationships between the WEPL and the integral dose or the depth at 80% of the proximal fall off of the energy resolved dose functions in water. In this note, we establish the evidence of the fundamental relationship between the energy resolved dose and the WEPL at the depth of the measurement. Then, we illustrate this relationship with experimental data and discuss its imaging dynamic range for 230 MeV protons.

Optical characterization of shock-induced chemistry in the explosive nitromethane using DFT and time-dependent DFT

NASA Astrophysics Data System (ADS)

Pellouchoud, Lenson; Reed, Evan

2014-03-01

With continual improvements in ultrafast optical spectroscopy and new multi-scale methods for simulating chemistry for hundreds of picoseconds, the opportunity is beginning to exist to connect experiments with simulations on the same timescale. We compute the optical properties of the liquid phase energetic material nitromethane (CH3NO2) for the first 100 picoseconds behind the front of a simulated shock at 6.5km/s, close to the experimentally observed detonation shock speed. We utilize molecular dynamics trajectories computed using the multi-scale shock technique (MSST) for time-resolved optical spectrum calculations based on both linear response time-dependent DFT (TDDFT) and the Kubo-Greenwood (KG) formula within Kohn-Sham DFT. We find that TDDFT predicts optical conductivities 25-35% lower than KG-based values and provides better agreement with the experimentally measured index of refraction of unreacted nitromethane. We investigate the influence of electronic temperature on the KG spectra and find no significant effect at optical wavelengths. With all methods, the spectra evolve non-monotonically in time as shock-induced chemistry takes place. We attribute the time-resolved absorption at optical wavelengths to time-dependent populations of molecular decomposition products, including NO, CNO, CNOH, H2O, and larger molecules. Supported by NASA Space Technology Research Fellowship (NSTRF) #NNX12AM48H.

Time resolved optical system for an early detection of prostate tumor

NASA Astrophysics Data System (ADS)

Hervé, Lionel; Laidevant, Aurélie; Debourdeau, Mathieu; Boutet, Jérôme; Dinten, Jean-Marc

2011-02-01

We developed an endorectal time-resolved optical probe aiming at an early detection of prostate tumors targeted by fluorescent markers. Optical fibers are embedded inside a clinical available ultrasound endorectal probe. Excitation light is driven sequentially from a femtosecond laser (775 nm) into 6 source fibers. 4 detection fibers collect the medium responses at the excitation and fluorescence wavelength (850 nm) by the mean of 4 photomultipliers associated with a 4 channel time-correlated single photon counting card. We also developed the method to process the experimental data. This involves the numerical computation of the forward model, the creation of robust features which are automatically correctly from numerous experimental possible biases and the reconstruction of the inclusion by using the intensity and mean time of these features. To evaluate our system performance, we acquired measurements of a 40 μL ICG inclusion (10 μmol.L-1) at various lateral and depth locations in a phantom. Analysis of results showed we correctly reconstructed the fluorophore for the lateral positions (16 mm range) and for a distance to the probe going up to 1.5 cm. Precision of localization was found to be around 1 mm which complies well with precision specifications needed for the clinical application.

Experimental studies on coherent synchrotron radiation at an emittance exchange beam line

NASA Astrophysics Data System (ADS)

Thangaraj, J. C. T.; Thurman-Keup, R.; Ruan, J.; Johnson, A. S.; Lumpkin, A. H.; Santucci, J.

2012-11-01

One of the goals of the Fermilab A0 photoinjector is to investigate experimentally the transverse to longitudinal emittance exchange (EEX) principle. Coherent synchrotron radiation in the emittance exchange line could limit the performance of the emittance exchanger at short bunch lengths. In this paper, we present experimental and simulation studies of the coherent synchrotron radiation (CSR) in the emittance exchange line at the A0 photoinjector. We report on time-resolved CSR studies using a skew-quadrupole technique. We also demonstrate the advantages of running the EEX with an energy-chirped beam.

Shock compression response of cold-rolled Ni/Al multilayer composites

NASA Astrophysics Data System (ADS)

Specht, Paul E.; Weihs, Timothy P.; Thadhani, Naresh N.

2017-01-01

Uniaxial strain, plate-on-plate impact experiments were performed on cold-rolled Ni/Al multilayer composites and the resulting Hugoniot was determined through time-resolved measurements combined with impedance matching. The experimental Hugoniot agreed with that previously predicted by two dimensional (2D) meso-scale calculations [Specht et al., J. Appl. Phys. 111, 073527 (2012)]. Additional 2D meso-scale simulations were performed using the same computational method as the prior study to reproduce the experimentally measured free surface velocities and stress profiles. These simulations accurately replicated the experimental profiles, providing additional validation for the previous computational work.

Design of a Hole Trapping Ligand

DOE PAGES

La Croix, Andrew D.; O’Hara, Andrew; Reid, Kemar R.; ...

2017-01-18

A new ligand that covalently attaches to the surface of colloidal CdSe/ CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate$-$bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic$-$organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer frommore » the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV$-$vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Lastly, theoretically predicted red shifts in absorbance were observed experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence« less

Design of a Hole Trapping Ligand

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

La Croix, Andrew D.; O’Hara, Andrew; Reid, Kemar R.

A new ligand that covalently attaches to the surface of colloidal CdSe/ CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate$-$bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic$-$organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer frommore » the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV$-$vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Lastly, theoretically predicted red shifts in absorbance were observed experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence« less

Using Separable Nonnegative Matrix Factorization Techniques for the Analysis of Time-Resolved Raman Spectra.

PubMed

Luce, Robert; Hildebrandt, Peter; Kuhlmann, Uwe; Liesen, Jörg

2016-09-01

The key challenge of time-resolved Raman spectroscopy is the identification of the constituent species and the analysis of the kinetics of the underlying reaction network. In this work we present an integral approach that allows for determining both the component spectra and the rate constants simultaneously from a series of vibrational spectra. It is based on an algorithm for nonnegative matrix factorization that is applied to the experimental data set following a few pre-processing steps. As a prerequisite for physically unambiguous solutions, each component spectrum must include one vibrational band that does not significantly interfere with the vibrational bands of other species. The approach is applied to synthetic "experimental" spectra derived from model systems comprising a set of species with component spectra differing with respect to their degree of spectral interferences and signal-to-noise ratios. In each case, the species involved are connected via monomolecular reaction pathways. The potential and limitations of the approach for recovering the respective rate constants and component spectra are discussed. © The Author(s) 2016.

Large eddy simulation of forced ignition of an annular bluff-body burner

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

Subramanian, V.; Domingo, P.; Vervisch, L.

2010-03-15

The optimization of the ignition process is a crucial issue in the design of many combustion systems. Large eddy simulation (LES) of a conical shaped bluff-body turbulent nonpremixed burner has been performed to study the impact of spark location on ignition success. This burner was experimentally investigated by Ahmed et al. [Combust. Flame 151 (2007) 366-385]. The present work focuses on the case without swirl, for which detailed measurements are available. First, cold-flow measurements of velocities and mixture fractions are compared with their LES counterparts, to assess the prediction capabilities of simulations in terms of flow and turbulent mixing. Timemore » histories of velocities and mixture fractions are recorded at selected spots, to probe the resolved probability density function (pdf) of flow variables, in an attempt to reproduce, from the knowledge of LES-resolved instantaneous flow conditions, the experimentally observed reasons for success or failure of spark ignition. A flammability map is also constructed from the resolved mixture fraction pdf and compared with its experimental counterpart. LES of forced ignition is then performed using flamelet fully detailed tabulated chemistry combined with presumed pdfs. Various scenarios of flame kernel development are analyzed and correlated with typical flow conditions observed in this burner. The correlations between, velocities and mixture fraction values at the sparking time and the success or failure of ignition, are then further discussed and analyzed. (author)« less

Time resolved flow-field measurements of a turbulent mixing layer over a rectangular cavity

NASA Astrophysics Data System (ADS)

Bian, Shiyao; Driscoll, James F.; Elbing, Brian R.; Ceccio, Steven L.

2011-07-01

High Reynolds number, low Mach number, turbulent shear flow past a rectangular, shallow cavity has been experimentally investigated with the use of dual-camera cinematographic particle image velocimetry (CPIV). The CPIV had a 3 kHz sampling rate, which was sufficient to monitor the time evolution of large-scale vortices as they formed, evolved downstream and impinged on the downstream cavity wall. The time-averaged flow properties (velocity and vorticity fields, streamwise velocity profiles and momentum and vorticity thickness) were in agreement with previous cavity flow studies under similar operating conditions. The time-resolved results show that the separated shear layer quickly rolled-up and formed eddies immediately downstream of the separation point. The vortices convect downstream at approximately half the free-stream speed. Vorticity strength intermittency as the structures approach the downstream edge suggests an increase in the three-dimensionality of the flow. Time-resolved correlations reveal that the in-plane coherence of the vortices decays within 2-3 structure diameters, and quasi-periodic flow features are present with a vortex passage frequency of ~1 kHz. The power spectra of the vertical velocity fluctuations within the shear layer revealed a peak at a non-dimensional frequency corresponding to that predicted using linear, inviscid instability theory.

Nanomechanical effects of light unveil photons momentum in medium

PubMed Central

Verma, Gopal; Chaudhary, Komal; Singh, Kamal P.

2017-01-01

Precision measurement on momentum transfer between light and fluid interface has many implications including resolving the intriguing nature of photons momentum in a medium. For example, the existence of Abraham pressure of light under specific experimental configuration and the predictions of Chau-Amperian formalism of optical momentum for TE and TM polarizations remain untested. Here, we quantitatively and cleanly measure nanomehanical dynamics of water surface excited by radiation pressure of a laser beam. We systematically scanned wide range of experimental parameters including long exposure times, angle of incidence, spot size and laser polarization, and used two independent pump-probe techniques to validate a nano- bump on the water surface under all the tested conditions, in quantitative agreement with the Minkowski’s momentum of light. With careful experiments, we demonstrate advantages and limitations of nanometer resolved optical probing techniques and narrow down actual manifestation of optical momentum in a medium. PMID:28198468

Room-temperature ultrafast nonlinear spectroscopy of a single molecule

NASA Astrophysics Data System (ADS)

Liebel, Matz; Toninelli, Costanza; van Hulst, Niek F.

2018-01-01

Single-molecule spectroscopy aims to unveil often hidden but potentially very important contributions of single entities to a system's ensemble response. Albeit contributing tremendously to our ever growing understanding of molecular processes, the fundamental question of temporal evolution, or change, has thus far been inaccessible, thus painting a static picture of a dynamic world. Here, we finally resolve this dilemma by performing ultrafast time-resolved transient spectroscopy on a single molecule. By tracing the femtosecond evolution of excited electronic state spectra of single molecules over hundreds of nanometres of bandwidth at room temperature, we reveal their nonlinear ultrafast response in an effective three-pulse scheme with fluorescence detection. A first excitation pulse is followed by a phase-locked de-excitation pulse pair, providing spectral encoding with 25 fs temporal resolution. This experimental realization of true single-molecule transient spectroscopy demonstrates that two-dimensional electronic spectroscopy of single molecules is experimentally within reach.

Heating Rate of Light Absorbing Aerosols: Time-Resolved Measurements, the Role of Clouds, and Source Identification.

PubMed

Ferrero, Luca; Močnik, Griša; Cogliati, Sergio; Gregorič, Asta; Colombo, Roberto; Bolzacchini, Ezio

2018-03-20

Light absorbing aerosols (LAA) absorb sunlight and heat the atmosphere. This work presents a novel methodology to experimentally quantify the heating rate (HR) induced by LAA into an atmospheric layer. Multiwavelength aerosol absorption measurements were coupled with spectral measurements of the direct, diffuse and surface reflected radiation to obtain highly time-resolved measurements of HR apportioned in the context of LAA species (black carbon, BC; brown carbon, BrC; dust), sources (fossil fuel, FF; biomass burning, BB), and as a function of cloudiness. One year of continuous and time-resolved measurements (5 min) of HR were performed in the Po Valley. We experimentally determined (1) the seasonal behavior of HR (winter 1.83 ± 0.02 K day -1 ; summer 1.04 ± 0.01 K day -1 ); (2) the daily cycle of HR (asymmetric, with higher values in the morning than in the afternoon); (3) the HR in different sky conditions (from 1.75 ± 0.03 K day -1 in clear sky to 0.43 ± 0.01 K day -1 in complete overcast); (4) the apportionment to different sources: HR FF (0.74 ± 0.01 K day -1 ) and HR BB (0.46 ± 0.01 K day -1 ); and (4) the HR of BrC (HR BrC : 0.15 ± 0.01 K day -1 , 12.5 ± 0.6% of the total) and that of BC (HR BC : 1.05 ± 0.02 K day -1 ; 87.5 ± 0.6% of the total).

Fast time-resolved electrostatic force microscopy: Achieving sub-cycle time resolution

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

Karatay, Durmus U.; Harrison, Jeffrey S.; Glaz, Micah S.

The ability to measure microsecond- and nanosecond-scale local dynamics below the diffraction limit with widely available atomic force microscopy hardware would enable new scientific studies in fields ranging from biology to semiconductor physics. However, commercially available scanning-probe instruments typically offer the ability to measure dynamics only on time scales of milliseconds to seconds. Here, we describe in detail the implementation of fast time-resolved electrostatic force microscopy using an oscillating cantilever as a means to measure fast local dynamics following a perturbation to a sample. We show how the phase of the oscillating cantilever relative to the perturbation event is criticalmore » to achieving reliable sub-cycle time resolution. We explore how noise affects the achievable time resolution and present empirical guidelines for reducing noise and optimizing experimental parameters. Specifically, we show that reducing the noise on the cantilever by using photothermal excitation instead of piezoacoustic excitation further improves time resolution. We demonstrate the discrimination of signal rise times with time constants as fast as 10 ns, and simultaneous data acquisition and analysis for dramatically improved image acquisition times.« less

Time-Resolved and Spatio-Temporal Analysis of Complex Cognitive Processes and their Role in Disorders like Developmental Dyscalculia

PubMed Central

Mórocz, István Akos; Janoos, Firdaus; van Gelderen, Peter; Manor, David; Karni, Avi; Breznitz, Zvia; von Aster, Michael; Kushnir, Tammar; Shalev, Ruth

2012-01-01

The aim of this article is to report on the importance and challenges of a time-resolved and spatio-temporal analysis of fMRI data from complex cognitive processes and associated disorders using a study on developmental dyscalculia (DD). Participants underwent fMRI while judging the incorrectness of multiplication results, and the data were analyzed using a sequence of methods, each of which progressively provided more a detailed picture of the spatio-temporal aspect of this disease. Healthy subjects and subjects with DD performed alike behaviorally though they exhibited parietal disparities using traditional voxel-based group analyses. Further and more detailed differences, however, surfaced with a time-resolved examination of the neural responses during the experiment. While performing inter-group comparisons, a third group of subjects with dyslexia (DL) but with no arithmetic difficulties was included to test the specificity of the analysis and strengthen the statistical base with overall fifty-eight subjects. Surprisingly, the analysis showed a functional dissimilarity during an initial reading phase for the group of dyslexic but otherwise normal subjects, with respect to controls, even though only numerical digits and no alphabetic characters were presented. Thus our results suggest that time-resolved multi-variate analysis of complex experimental paradigms has the ability to yield powerful new clinical insights about abnormal brain function. Similarly, a detailed compilation of aberrations in the functional cascade may have much greater potential to delineate the core processing problems in mental disorders. PMID:22368322

Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy

DOE PAGES

Hassan, Asra; Zhang, Xiaoyi; Liu, Xiaohan; ...

2017-08-28

Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report the results of time-resolved X-ray absorption studies on copper-doped cadmium sulfide nanoparticles that provide an explicit description of the electronic dynamics of the dopants. The interaction of a dopant ion and an excess charge carrier is unambiguously observed via monitoring the oxidation state. The experimental data combined with DFT calculations demonstrate that dopant bonding to the host matrix is modulated by its interaction with charge carriers. Additionally, the transient photoluminescence and the kinetics of dopantmore » oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.« less

Time-resolved laser spectroscopy of multiply ionized atoms: natural radiative lifetimes in Ce IV.

PubMed

Zhang, Z G; Svanberg, S; Quinet, P; Palmeri, P; Biémont, E

2001-12-31

Radiative lifetimes have been measured for two excited levels of Ce IV using the time-resolved laser-induced fluorescence technique. Ce3+ ions were produced in a laser-induced plasma. In the measurements, a suitable magnetic field was applied to reduce the recombination between electrons and the ions and thus the background light from the recombination, and special care was exercised to avoid flight-out-of-view effects on the lifetime measurements for the high-velocity ions. The experimental lifetime results, tau = 30(2) ns for the level 49 737 cm(-1) and tau = 30(3) ns for the level 52 226 cm(-1), were compared with relativistic Hartree-Fock calculations (tau = 30.5 and 30.0 ns) indicating a particularly excellent agreement.

Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy

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

Hassan, Asra; Zhang, Xiaoyi; Liu, Xiaohan

Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report the results of time-resolved X-ray absorption studies on copper-doped cadmium sulfide nanoparticles that provide an explicit description of the electronic dynamics of the dopants. The interaction of a dopant ion and an excess charge carrier is unambiguously observed via monitoring the oxidation state. The experimental data combined with DFT calculations demonstrate that dopant bonding to the host matrix is modulated by its interaction with charge carriers. Additionally, the transient photoluminescence and the kinetics of dopantmore » oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.« less

X-rays only when you want them: optimized pump–probe experiments using pseudo-single-bunch operation

PubMed Central

Hertlein, M. P.; Scholl, A.; Cordones, A. A.; Lee, J. H.; Engelhorn, K.; Glover, T. E.; Barbrel, B.; Sun, C.; Steier, C.; Portmann, G.; Robin, D. S.

2015-01-01

Laser pump–X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500 kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shot X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated. PMID:25931090

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.

PubMed

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.

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

NASA Astrophysics Data System (ADS)

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.

X-rays only when you want them: Optimized pump–probe experiments using pseudo-single-bunch operation

DOE PAGES

Hertlein, M. P.; Scholl, A.; Cordones, A. A.; ...

2015-04-02

Laser pump–X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500 kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shotmore » X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated.« less

Phase Reconstruction from FROG Using Genetic Algorithms[Frequency-Resolved Optical Gating

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

Omenetto, F.G.; Nicholson, J.W.; Funk, D.J.

1999-04-12

The authors describe a new technique for obtaining the phase and electric field from FROG measurements using genetic algorithms. Frequency-Resolved Optical Gating (FROG) has gained prominence as a technique for characterizing ultrashort pulses. FROG consists of a spectrally resolved autocorrelation of the pulse to be measured. Typically a combination of iterative algorithms is used, applying constraints from experimental data, and alternating between the time and frequency domain, in order to retrieve an optical pulse. The authors have developed a new approach to retrieving the intensity and phase from FROG data using a genetic algorithm (GA). A GA is a generalmore » parallel search technique that operates on a population of potential solutions simultaneously. Operators in a genetic algorithm, such as crossover, selection, and mutation are based on ideas taken from evolution.« less

Photon-Induced Thermal Desorption of CO from Small Metal-Carbonyl Clusters

NASA Astrophysics Data System (ADS)

Lüttgens, G.; Pontius, N.; Bechthold, P. S.; Neeb, M.; Eberhardt, W.

2002-02-01

Thermal CO desorption from photoexcited free metal-carbonyl clusters has been resolved in real time using two-color pump-probe photoelectron spectroscopy. Sequential energy dissipation steps between the initial photoexcitation and the final desorption event, e.g., electron relaxation and thermalization, have been resolved for Au2(CO)- and Pt2(CO)-5. The desorption rates for the two clusters differ considerably due to the different numbers of vibrational degrees of freedom. The unimolecular CO-desorption thresholds of Au2(CO)- and Pt2(CO)-5 have been approximated by means of a statistical Rice-Ramsperger-Kassel calculation using the experimentally derived desorption rate constants.

Integrated microfluidic chip for rapid DNA digestion and time-resolved capillary electrophoresis analysis

PubMed Central

Lin, Che-Hsin; Wang, Yao-Nan; Fu, Lung-Ming

2012-01-01

An integrated microfluidic chip is proposed for rapid DNA digestion and time-resolved capillary electrophoresis (CE) analysis. The chip comprises two gel-filled chambers for DNA enrichment and purification, respectively, a T-form micromixer for DNA/restriction enzyme mixing, a serpentine channel for DNA digestion reaction, and a CE channel for on-line capillary electrophoresis analysis. The DNA and restriction enzyme are mixed electroomostically using a pinched-switching DC field. The experimental and numerical results show that a mixing performance of 97% is achieved within a distance of 1 mm from the T-junction when a driving voltage of 90 V/cm and a switching frequency of 4 Hz are applied. Successive mixing digestion and capillary electrophoresis operation clearly present the changes on digesting φx-174 DNA in different CE runs. The time-resolved electropherograms show that the proposed device enables a φx-174 DNA sample comprising 11 fragments to be concentrated and analyzed within 24 min. Overall, the results presented in this study show that the proposed microfluidic chip provides a rapid and effective tool for DNA digestion and CE analysis applications. PMID:22662085

Time-resolved fluorescence of thioredoxin single-tryptophan mutants: modeling experimental results with minimum perturbation mapping

NASA Astrophysics Data System (ADS)

Silva, Norberto D., Jr.; Haydock, Christopher; Prendergast, Franklyn G.

1994-08-01

The time-resolved fluorescence decay of single tryptophan (Trp) proteins is typically described using either a distribution of lifetimes or a sum of two or more exponential terms. A possible interpretation for this fluorescence decay heterogeneity is the existence of different isomeric conformations of Trp about its (chi) +1) and (chi) +2) dihedral angles. Are multiple Trp conformations compatible with the remainder of the protein in its crystallographic configuration or do they require repacking of neighbor side chains? It is conceivable that isomers of the neighbor side chains interconvert slowly on the fluorescence timescale and contribute additional lifetime components to the fluorescence intensity. We have explored this possibility by performing minimum perturbation mapping simulations of Trp 28 and Trp 31 in thioredoxin (TRX) using CHARMm 22. Mappings of Trp 29 and Trp 31 give the TRX Trp residue energy landscape as a function of (chi) +1) and (chi) +2) dihedral angles. Time-resolved fluorescence intensity and anisotropy decay of mutant TRX (W28F and W31F) are measured and interpreted in light of the above simulations. Relevant observables, like order parameters and isomerization rates, can be derived from the minimum perturbation maps and compared with experiment.

TIME EVOLUTION OF KELVIN–HELMHOLTZ VORTICES ASSOCIATED WITH COLLISIONLESS SHOCKS IN LASER-PRODUCED PLASMAS

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

Kuramitsu, Y.; Moritaka, T.; Mizuta, A.

2016-09-10

We report experimental results on Kelvin–Helmholtz (KH) instability and resultant vortices in laser-produced plasmas. By irradiating a double plane target with a laser beam, asymmetric counterstreaming plasmas are created. The interaction of the plasmas with different velocities and densities results in the formation of asymmetric shocks, where the shear flow exists along the contact surface and the KH instability is excited. We observe the spatial and temporal evolution of plasmas and shocks with time-resolved diagnostics over several shots. Our results clearly show the evolution of transverse fluctuations, wavelike structures, and circular features, which are interpreted as the KH instability andmore » resultant vortices. The relevant numerical simulations demonstrate the time evolution of KH vortices and show qualitative agreement with experimental results. Shocks, and thus the contact surfaces, are ubiquitous in the universe; our experimental results show general consequences where two plasmas interact.« less

Environment effect on the acoustic vibration of metal nanoparticles

NASA Astrophysics Data System (ADS)

Voisin, C.; Christofilos, D.; Del Fatti, N.; Vallée, F.

2002-05-01

The impact of the environment on the frequency and damping of the breathing acoustic mode of noble metal nanoparticle is discussed using the model of isotropic homogeneous elastic spheres embedded in an elastic medium. The results are compared to the experimental investigations performed in glass embedded silver nanoparticles and gold colloids using a time-resolved pump-probe technique.

Fluid Flow Characterization of High Turbulent Intensity Compressible Flow Using Particle Image Velocimetry

DTIC Science & Technology

2015-08-01

completed in order to begin further experimentation. A 10 kHz Time Resolved Particle Image Velocimetry (TR-PIV) system and a 3 kHz Planer Laser ...9 2.3.2 Planar Laser Induced Fluorescence (PLIF...35 Figure 4.4: Solenoid valve (a), proportional control valve (b) and flowmeter (c) ...................................... 36 Figure 4.5

Using the Bifocal Modeling Framework to Resolve "Discrepant Events" between Physical Experiments and Virtual Models in Biology

ERIC Educational Resources Information Center

Blikstein, Paulo; Fuhrmann, Tamar; Salehi, Shima

2016-01-01

In this paper, we investigate an approach to supporting students' learning in science through a combination of physical experimentation and virtual modeling. We present a study that utilizes a scientific inquiry framework, which we call "bifocal modeling," to link student-designed experiments and computer models in real time. In this…

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

DTIC Science & Technology

2016-01-12

15. SUBJECT TERMS Materials Characterization, Materials Chemistry, Nonlinear Optical Materials, Spectroscopy 16. SECURITY CLASSIFICATION...nanostructures will translate into new ground-breaking developments that not only allow the structure-property relationships to be probed in greater detail... spectroscopy . I. Experimental method 1. Steady-state Spectroscopy - UV-Vis-NIR Absorption & Emission Steady-state Spectroscopy - NIR

New approaches for the reliable in vitro assessment of binding affinity based on high-resolution real-time data acquisition of radioligand-receptor binding kinetics.

PubMed

Zeilinger, Markus; Pichler, Florian; Nics, Lukas; Wadsak, Wolfgang; Spreitzer, Helmut; Hacker, Marcus; Mitterhauser, Markus

2017-12-01

Resolving the kinetic mechanisms of biomolecular interactions have become increasingly important in early-phase drug development. Since traditional in vitro methods belong to dose-dependent assessments, binding kinetics is usually overlooked. The present study aimed at the establishment of two novel experimental approaches for the assessment of binding affinity of both, radiolabelled and non-labelled compounds targeting the A 3 R, based on high-resolution real-time data acquisition of radioligand-receptor binding kinetics. A novel time-resolved competition assay was developed and applied to determine the K i of eight different A 3 R antagonists, using CHO-K1 cells stably expressing the hA 3 R. In addition, a new kinetic real-time cell-binding approach was established to quantify the rate constants k on and k off , as well as the dedicated K d of the A 3 R agonist [ 125 I]-AB-MECA. Furthermore, lipophilicity measurements were conducted to control influences due to physicochemical properties of the used compounds. Two novel real-time cell-binding approaches were successfully developed and established. Both experimental procedures were found to visualize the kinetic binding characteristics with high spatial and temporal resolution, resulting in reliable affinity values, which are in good agreement with values previously reported with traditional methods. Taking into account the lipophilicity of the A 3 R antagonists, no influences on the experimental performance and the resulting affinity were investigated. Both kinetic binding approaches comprise tracer administration and subsequent binding to living cells, expressing the dedicated target protein. Therefore, the experiments resemble better the true in vivo physiological conditions and provide important markers of cellular feedback and biological response.

Development of a Rayleigh Scattering Diagnostic for Time-Resolved Gas Flow Velocity, Temperature, and Density Measurements in Aerodynamic Test Facilities

NASA Technical Reports Server (NTRS)

Mielke, Amy F.; Elam, Kristie A.; Sung, Chih-Jen

2007-01-01

A molecular Rayleigh scattering technique is developed to measure time-resolved gas velocity, temperature, and density in unseeded turbulent flows at sampling rates up to 32 kHz. A high power continuous-wave laser beam is focused at a point in an air flow field and Rayleigh scattered light is collected and fiber-optically transmitted to the spectral analysis and detection equipment. The spectrum of the light, which contains information about the temperature and velocity of the flow, is analyzed using a Fabry-Perot interferometer. Photomultiplier tubes operated in the photon counting mode allow high frequency sampling of the circular interference pattern to provide time-resolved flow property measurements. An acoustically driven nozzle flow is studied to validate velocity fluctuation measurements, and an asymmetric oscillating counterflow with unequal enthalpies is studied to validate the measurement of temperature fluctuations. Velocity fluctuations are compared with constant temperature anemometry measurements and temperature fluctuations are compared with constant current anemometry measurements at the same locations. Time-series and power spectra of the temperature and velocity measurements are presented. A numerical simulation of the light scattering and detection process was developed and compared with experimental data for future use as an experiment design tool.

Energy dissipation from a correlated system driven out of equilibrium

DOE PAGES

Rameau, J. D.; Freutel, S.; Kemper, A. F.; ...

2016-12-20

We report that in complex materials various interactions have important roles in determining electronic properties. Angle-resolved photoelectron spectroscopy (ARPES) is used to study these processes by resolving the complex single-particle self-energy and quantifying how quantum interactions modify bare electronic states. However, ambiguities in the measurement of the real part of the self-energy and an intrinsic inability to disentangle various contributions to the imaginary part of the self-energy can leave the implications of such measurements open to debate. Here we employ a combined theoretical and experimental treatment of femtosecond time-resolved ARPES (tr-ARPES) show how population dynamics measured using tr-ARPES can bemore » used to separate electron–boson interactions from electron–electron interactions. In conclusion, we demonstrate a quantitative analysis of a well-defined electron–boson interaction in the unoccupied spectrum of the cuprate Bi 2Sr 2CaCu 2O 8+x characterized by an excited population decay time that maps directly to a discrete component of the equilibrium self-energy not readily isolated by static ARPES experiments.« less

Development of a Nomarski-type multi-frame interferometer as a time and space resolving diagnostics for the free electron density of laser-generated plasma

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

Boerner, M.; Frank, A.; Pelka, A.

2012-04-15

This article reports on the development and set-up of a Nomarski-type multi-frame interferometer as a time and space resolving diagnostics of the free electron density in laser-generated plasma. The interferometer allows the recording of a series of 4 images within 6 ns of a single laser-plasma interaction. For the setup presented here, the minimal accessible free electron density is 5 x 10{sup 18} cm{sup -3}, the maximal one is 2 x 10{sup 20} cm{sup -3}. Furthermore, it provides a resolution of the electron density in space of 50 {mu}m and in time of 0.5 ns for one image with amore » customizable magnification in space for each of the 4 images. The electron density was evaluated from the interferograms using an Abel inversion algorithm. The functionality of the system was proven during first experiments and the experimental results are presented and discussed. A ray tracing procedure was realized to verify the interferometry pictures taken. In particular, the experimental results are compared to simulations and show excellent agreement, providing a conclusive picture of the evolution of the electron density distribution.« less

Tracking the photodissociation dynamics of liquid nitromethane at 266 nm by femtosecond time-resolved broadband transient grating spectroscopy

NASA Astrophysics Data System (ADS)

Wu, Honglin; Song, Yunfei; Yu, Guoyang; Wang, Yang; Wang, Chang; Yang, Yanqiang

2016-05-01

Femtosecond time-resolved transient grating (TG) technique was employed to get insight into the photodissociation mechanism of liquid nitromethane (NM). Broadband white-light continuum was introduced as the probe to observe the evolution of electronic excited states of NM molecules and the formation of photodissociation products simultaneously. The reaction channel of liquid NM under 266 nm excitation was obtained that NM molecules in excited state S2 relax through two channels: about 73% relax to low lying S1 state through S2/S1 internal conversion with a time constant of 0.24 ps and then go back to the ground state through S1/S0 internal conversion; the other 27% will dissociate with a time constant of 2.56 ps. NO2 was found to be one of the products from the experimental TG spectra, which confirmed that C-N bond rupture was the primary dissociation channel of liquid NM.

Electron phonon couplings in 2D perovskite probed by ultrafast photoinduced absorption spectroscopy

NASA Astrophysics Data System (ADS)

Huynh, Uyen; Ni, Limeng; Rao, Akshay

We use the time-resolved photoinduced absorption (PIA) spectroscopy with 20fs time resolution to investigate the electron phonon coupling in the self-assembled hybrid organic layered perovskite, the hexyl ammonium lead iodide compound (C6H13NH3)2 (PbI4) . The coupling results in the broadening and asymmetry of its temperature-dependence photoluminescence spectra. The exact time scale of this coupling, however, wasn't reported experimentally. Here we show that using an ultrashort excitation pulse allows us to resolve from PIA kinetics the oscillation of coherent longitudinal optical phonons that relaxes and self-traps electrons to lower energy states within 200 fs. The 200fs relaxation time is equivalent to a coupling strength of 40meV. Two coupled phonon modes are also identified as about 100 cm-1 and 300 cm-1 from the FFT spectrum of the PIA kinetics. The lower energy mode is consistent with previous reports and Raman spectrum but the higher energy one hasn't been observed before.

Fiber optic sensing technology for detecting gas hydrate formation and decomposition.

PubMed

Rawn, C J; Leeman, J R; Ulrich, S M; Alford, J E; Phelps, T J; Madden, M E

2011-02-01

A fiber optic-based distributed sensing system (DSS) has been integrated with a large volume (72 l) pressure vessel providing high spatial resolution, time-resolved, 3D measurement of hybrid temperature-strain (TS) values within experimental sediment-gas hydrate systems. Areas of gas hydrate formation (exothermic) and decomposition (endothermic) can be characterized through this proxy by time series analysis of discrete data points collected along the length of optical fibers placed within a sediment system. Data are visualized as an animation of TS values along the length of each fiber over time. Experiments conducted in the Seafloor Process Simulator at Oak Ridge National Laboratory clearly indicate hydrate formation and dissociation events at expected pressure-temperature conditions given the thermodynamics of the CH(4)-H(2)O system. The high spatial resolution achieved with fiber optic technology makes the DSS a useful tool for visualizing time-resolved formation and dissociation of gas hydrates in large-scale sediment experiments.

Fiber optic sensing technology for detecting gas hydrate formation and decomposition

NASA Astrophysics Data System (ADS)

Rawn, C. J.; Leeman, J. R.; Ulrich, S. M.; Alford, J. E.; Phelps, T. J.; Madden, M. E.

2011-02-01

A fiber optic-based distributed sensing system (DSS) has been integrated with a large volume (72 l) pressure vessel providing high spatial resolution, time-resolved, 3D measurement of hybrid temperature-strain (TS) values within experimental sediment-gas hydrate systems. Areas of gas hydrate formation (exothermic) and decomposition (endothermic) can be characterized through this proxy by time series analysis of discrete data points collected along the length of optical fibers placed within a sediment system. Data are visualized as an animation of TS values along the length of each fiber over time. Experiments conducted in the Seafloor Process Simulator at Oak Ridge National Laboratory clearly indicate hydrate formation and dissociation events at expected pressure-temperature conditions given the thermodynamics of the CH4-H2O system. The high spatial resolution achieved with fiber optic technology makes the DSS a useful tool for visualizing time-resolved formation and dissociation of gas hydrates in large-scale sediment experiments.

Terahertz-Radiation-Enhanced Emission of Fluorescence from Gas Plasma

NASA Astrophysics Data System (ADS)

Liu, Jingle; Zhang, X.-C.

2009-12-01

We report the study of femtosecond laser-induced air plasma fluorescence under the illumination of terahertz (THz) pulses. Semiclassical modeling and experimental verification indicate that time-resolved THz radiation-enhanced emission of fluorescence is dominated by the electron kinetics and the electron-impact excitation of gas molecules or ions. We demonstrate that the temporal waveform of the THz field could be retrieved from the transient enhanced fluorescence, making omnidirectional, coherent detection available for THz time-domain spectroscopy.

Observation of Transonic Ionization Fronts in Low-Density Foam Targets

NASA Astrophysics Data System (ADS)

Hoarty, D.; Barringer, L.; Vickers, C.; Willi, O.; Nazarov, W.

1999-04-01

Transonic ionization fronts have been observed in low-density chlorinated foam targets using time-resolved K-shell absorption spectroscopy. The front was driven by an intense pulse of soft x rays produced by high-power laser irradiation of a thin foil. The density and temperature profiles inferred from the radiographs provided detailed measurement of the conditions at a number of times. The experimental data were compared to radiation hydrodynamics simulations and reasonable agreement was obtained.

The electronically excited states of LH2 complexes from Rhodopseudomonas acidophila strain 10050 studied by time-resolved spectroscopy and dynamic Monte Carlo simulations. II. Homo-arrays of LH2 complexes reconstituted into phospholipid model membranes.

PubMed

Pflock, Tobias J; Oellerich, Silke; Krapf, Lisa; Southall, June; Cogdell, Richard J; Ullmann, G Matthias; Köhler, Jürgen

2011-07-21

We performed time-resolved spectroscopy on homoarrays of LH2 complexes from the photosynthetic purple bacterium Rhodopseudomonas acidophila. Variations of the fluorescence transients were monitored as a function of the excitation fluence and the repetition rate of the excitation. These parameters are directly related to the excitation density within the array and to the number of LH2 complexes that still carry a triplet state prior to the next excitation. Comparison of the experimental observations with results from dynamic Monte Carlo simulations for a model cluster of LH2 complexes yields qualitative agreement without the need for any free parameter and reveals the mutual relationship between energy transfer and annihilation processes.

Space- and time-resolved resistive measurements of liquid metal wall thickness

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

Mirhoseini, S. M. H.; Volpe, F. A., E-mail: fvolpe@columbia.edu

In a fusion reactor internally coated with liquid metal, it will be important to diagnose the thickness of the liquid at various locations in the vessel, as a function of time, and possibly respond to counteract undesired bulging or depletion. The electrical conductance between electrodes immersed in the liquid metal can be used as a simple proxy for the local thickness. Here a matrix of electrodes is shown to provide spatially and temporally resolved measurements of liquid metal thickness in the absence of plasma. First a theory is developed for m × n electrodes, and then it is experimentally demonstratedmore » for 3 × 1 electrodes, as the liquid stands still or is agitated by means of a shaker. The experiments were carried out with Galinstan, but are easily extended to lithium or other liquid metals.« less

Space- and time-resolved resistive measurements of liquid metal wall thickness.

PubMed

Mirhoseini, S M H; Volpe, F A

2016-11-01

In a fusion reactor internally coated with liquid metal, it will be important to diagnose the thickness of the liquid at various locations in the vessel, as a function of time, and possibly respond to counteract undesired bulging or depletion. The electrical conductance between electrodes immersed in the liquid metal can be used as a simple proxy for the local thickness. Here a matrix of electrodes is shown to provide spatially and temporally resolved measurements of liquid metal thickness in the absence of plasma. First a theory is developed for m × n electrodes, and then it is experimentally demonstrated for 3 × 1 electrodes, as the liquid stands still or is agitated by means of a shaker. The experiments were carried out with Galinstan, but are easily extended to lithium or other liquid metals.

Two-dimensional electronic spectra of the photosynthetic apparatus of green sulfur bacteria

NASA Astrophysics Data System (ADS)

Kramer, Tobias; Rodriguez, Mirta

2017-03-01

Advances in time resolved spectroscopy have provided new insight into the energy transmission in natural photosynthetic complexes. Novel theoretical tools and models are being developed in order to explain the experimental results. We provide a model calculation for the two-dimensional electronic spectra of Cholorobaculum tepidum which correctly describes the main features and transfer time scales found in recent experiments. From our calculation one can infer the coupling of the antenna chlorosome with the environment and the coupling between the chlorosome and the Fenna-Matthews-Olson complex. We show that environment assisted transport between the subunits is the required mechanism to reproduce the experimental two-dimensional electronic spectra.

Current Sheet Formation in a Conical Theta Pinch Faraday Accelerator with Radio-frequency Assisted Discharge

NASA Technical Reports Server (NTRS)

Polzin, Kurt A.; Hallock, Ashley K.; Choueiri, Edgar Y.

2008-01-01

Data from an inductive conical theta pinch accelerator are presented to gain insight into the process of inductive current sheet formation in the presence of a preionized background gas produced by a steady-state RF-discharge. The presence of a preionized plasma has been previously shown to allow for current sheet formation at lower discharge voltages and energies than those found in other pulsed inductive accelerator concepts, leading to greater accelerator efficiencies at lower power levels. Time-resolved magnetic probe measurements are obtained for different background pressures and pulse energies to characterize the effects of these parameters on current sheet formation. Indices are defined that describe time-resolved current sheet characteristics, such as the total current owing in the current sheet, the time-integrated total current ('strength'), and current sheet velocity. It is found that for a given electric field strength, maximums in total current, strength, and velocity occur for one particular background pressure. At other pressures, these current sheet indices are considerably smaller. The trends observed in these indices are explained in terms of the principles behind Townsend breakdown that lead to a dependence on the ratio of the electric field to the background pressure. Time-integrated photographic data are also obtained at the same experimental conditions, and qualitatively they compare quite favorably with the time-resolved magnetic field data.

Resolving Cognitive Conflict in a Realistic Situation with Modeling Characteristics: Coping with a Changing Reference in Fractions

ERIC Educational Resources Information Center

Shahbari, Juhaina Awawdeh; Peled, Irit

2015-01-01

This study investigates the effect of using a realistic situation with modeling characteristics in creating and resolving a cognitive conflict to promote understanding of a changing reference in fraction calculations. The study was conducted among 96 seventh graders divided into 2 experimental groups and 1 control group. The experimental groups…

Graphene-enhanced infrared near-field microscopy.

PubMed

Li, Peining; Wang, Tao; Böckmann, Hannes; Taubner, Thomas

2014-08-13

Graphene is a promising two-dimensional platform for widespread nanophotonic applications. Recent theories have predicted that graphene can also enhance evanescent fields for subdiffraction-limited imaging. Here, for the first time we experimentally demonstrate that monolayer graphene offers a 7-fold enhancement of evanescent information, improving conventional infrared near-field microscopy to resolve buried structures at a 500 nm depth with λ/11-resolution.

The quest for four-dimensional imaging in plant cell biology: it's just a matter of time

PubMed Central

Domozych, David S.

2012-01-01

Background Analysis of plant cell dynamics over time, or four-dimensional imaging (4-DI), represents a major goal of plant science. The ability to resolve structures in the third dimension within the cell or tissue during developmental events or in response to environmental or experimental stresses (i.e. 4-DI) is critical to our understanding of gene expression, post-expression modulations of macromolecules and sub-cellular system interactions. Scope Microscopy-based technologies have been profoundly integral to this type of investigation, and new and refined microscopy technologies now allow for the visualization of cell dynamics with unprecedented resolution, contrast and experimental versatility. However, certain realities of light and electron microscopy, choice of specimen and specimen preparation techniques limit the scope of readily attaining 4-DI. Today, the plant microscopist must use a combinatorial strategy whereby multiple microscopy-based investigations are used. Modern fluorescence, confocal laser scanning, transmission electron and scanning electron microscopy provide effective conduits for synthesizing data detailing live cell dynamics and highly resolved snapshots of specific cell structures that will ultimately lead to 4-DI. This review provides a synopsis of such technologies available. PMID:22628381

In Situ 3D Coherent X-ray Diffraction Imaging of Shock Experiments: Possible?

NASA Astrophysics Data System (ADS)

Barber, John

2011-03-01

In traditional coherent X-ray diffraction imaging (CXDI), a 2D or quasi-2D object is illuminated by a beam of coherent X-rays to produce a diffraction pattern, which is then manipulated via a process known as iterative phase retrieval to reconstruct an image of the original 2D sample. Recently, there have been dramatic advances in methods for performing fully 3D CXDI of a sample from a single diffraction pattern [Raines et al, Nature 463 214-7 (2010)], and these methods have been used to image samples tens of microns in size using soft X-rays. In this work, I explore the theoretical possibility of applying 3D CXDI techniques to the in situ imaging of the interaction between a shock front and a polycrystal, a far more stringent problem. A delicate trade-off is required between photon energy, spot size, imaging resolution, and the dimensions of the experimental setup. In this talk, I will outline the experimental and computational requirements for performing such an experiment, and I will present images and movies from simulations of one such hypothetical experiment, including both the time-resolved X-ray diffraction patterns and the time-resolved sample imagery.

Turbomachinery

NASA Technical Reports Server (NTRS)

Simoneau, Robert J.; Strazisar, Anthony J.; Sockol, Peter M.; Reid, Lonnie; Adamczyk, John J.

1987-01-01

The discipline research in turbomachinery, which is directed toward building the tools needed to understand such a complex flow phenomenon, is based on the fact that flow in turbomachinery is fundamentally unsteady or time dependent. Success in building a reliable inventory of analytic and experimental tools will depend on how the time and time-averages are treated, as well as on who the space and space-averages are treated. The raw tools at disposal (both experimentally and computational) are truly powerful and their numbers are growing at a staggering pace. As a result of this power, a case can be made that a situation exists where information is outstripping understanding. The challenge is to develop a set of computational and experimental tools which genuinely increase understanding of the fluid flow and heat transfer in a turbomachine. Viewgraphs outline a philosophy based on working on a stairstep hierarchy of mathematical and experimental complexity to build a system of tools, which enable one to aggressively design the turbomachinery of the next century. Examples of the types of computational and experimental tools under current development at Lewis, with progress to date, are examined. The examples include work in both the time-resolved and time-averaged domains. Finally, an attempt is made to identify the proper place for Lewis in this continuum of research.

Volume versus surface-mediated recombination in anatase TiO2 nanoparticles

NASA Astrophysics Data System (ADS)

Cavigli, Lucia; Bogani, Franco; Vinattieri, Anna; Faso, Valentina; Baldi, Giovanni

2009-09-01

We present an experimental study of the radiative recombination dynamics in size-controlled anatase TiO2 nanoparticles in the range 20-130 nm. From time-integrated photoluminescence spectra and picosecond time-resolved experiments as a function of the nanoparticle size, excitation density, and temperature, we show that photoluminescence comes out from a bulk and a surface radiative recombination. The spectral shift and the different time dynamics provide a clear distinction between them. Moreover, the intrinsic nature of the emission is also proven, providing a quantitative evaluation of volume and surface contributions.

Lattice-Assisted Spectroscopy: A Generalized Scanning Tunneling Microscope for Ultracold Atoms.

PubMed

Kantian, A; Schollwöck, U; Giamarchi, T

2015-10-16

We propose a scheme to measure the frequency-resolved local particle and hole spectra of any optical lattice-confined system of correlated ultracold atoms that offers single-site addressing and imaging, which is now an experimental reality. Combining perturbation theory and time-dependent density matrix renormalization group simulations, we quantitatively test and validate this approach of lattice-assisted spectroscopy on several one-dimensional example systems, such as the superfluid and Mott insulator, with and without a parabolic trap, and finally on edge states of the bosonic Su-Schrieffer-Heeger model. We highlight extensions of our basic scheme to obtain an even wider variety of interesting and important frequency resolved spectra.

Tunneling Flight Time, Chemistry, and Special Relativity.

PubMed

Petersen, Jakob; Pollak, Eli

2017-09-07

Attosecond ionization experiments have not resolved the question "What is the tunneling time?". Different definitions of tunneling time lead to different results. Second, a zero tunneling time for a material particle suggests that the nonrelativistic theory includes speeds greater than the speed of light. Chemical reactions, occurring via tunneling, should then not be considered in terms of a nonrelativistic quantum theory calling into question quantum dynamics computations on tunneling reactions. To answer these questions, we define a new experimentally measurable paradigm, the tunneling flight time, and show that it vanishes for scattering through an Eckart or a square barrier, irrespective of barrier length or height, generalizing the Hartman effect. We explain why this result does not lead to experimental measurement of speeds greater than the speed of light. We show that this tunneling is an incoherent process by comparing a classical Wigner theory with exact quantum mechanical computations.

Assessment of electron propagator methods for the simulation of vibrationally-resolved valence and core photoionization spectra

PubMed Central

Baiardi, A.; Paoloni, L.; Barone, V.; Zakrzewski, V.G.; Ortiz, J.V.

2017-01-01

The analysis of photoelectron spectra is usually facilitated by quantum mechanical simulations. Due to the recent improvement of experimental techniques, the resolution of experimental spectra is rapidly increasing, and the inclusion of vibrational effects is usually mandatory to obtain a reliable reproduction of the spectra. With the aim of defining a robust computational protocol, a general time-independent formulation to compute different kinds of vibrationally-resolved electronic spectra has been generalized to support also photoelectron spectroscopy. The electronic structure data underlying the simulation are computed using different electron propagator approaches. In addition to the more standard approaches, a new and robust implementation of the second-order self-energy approximation of the electron propagator based on a transition operator reference (TOEP2) is presented. To validate our implementation, a series of molecules has been used as test cases. The result of the simulations shows that, for ultraviolet photoionization spectra, the more accurate non-diagonal approaches are needed to obtain a reliable reproduction of vertical ionization energies, but diagonal approaches are sufficient for energy gradients and pole strengths. For X-ray photoelectron spectroscopy, the TOEP2 approach, besides being more efficient, is also the most accurate in the reproduction of both vertical ionization energies and vibrationally-resolved bandshapes. PMID:28521087

Role of phase instabilities in the early response of bulk fused silica during laser-induced breakdown

NASA Astrophysics Data System (ADS)

Demange, P.; Negres, R. A.; Raman, R. N.; Colvin, J. D.; Demos, S. G.

2011-08-01

We report on the experimental and hydrocode modeling investigation of the early material response to localized energy deposition via nanosecond laser pulses in bulk fused silica. A time-resolved microscope system was used to acquire transient images with adequate spatial and temporal resolution to resolve the material behavior from the onset of the process. These images revealed a high-pressure shock front propagating at twice the speed of sound at ambient conditions and bounding a region of modified material at delays up to one nanosecond. Hydrocode simulations matching the experimental conditions were also performed and indicated initial pressures of ˜40 GPa and temperatures of ˜1 eV at the absorption region. Both the simulations and the image data show a clear boundary between distinct material phases, a hot plasma and solid silica, with a suggestion that growth of perturbations at the Rayleigh-Taylor unstable interface between the two phases is the seed mechanism for the growth of cracks into the stressed solid.

Stimulated backward Raman scattering driven collectively by two picosecond laser pulses in a bi- or multi-speckle configuration

NASA Astrophysics Data System (ADS)

Glize, K.; Rousseaux, C.; Bénisti, D.; Dervieux, V.; Gremillet, L.; Baton, S. D.; Lancia, L.

2017-03-01

In this paper, we investigate, both experimentally and numerically, the backward stimulated Raman scattering (SRS) excited collectively by two laser pulses. The experiments have been carried out at the LULI facility using two co-propagating 1- μ m wavelength, 1.5- ps duration laser pulses focused in a preformed underdense plasma. A particular emphasis is laid on the configuration where the pulses are focused side-by-side, with a lateral distance of 80 - 90 μ m , but not simultaneously. It is experimentally demonstrated that a weak-intensity speckle, ineffective when fired alone in a preformed plasma, yields a significant SRS-induced reflectivity if launched a few picoseconds after a strong one. The data have been obtained by using both highly space-time resolved Thomson diagnostics and space-resolved SRS reflectivity measurements. By choosing either parallel or orthogonal polarizations for the two laser pulses, our experiments shed light on the role of either electrostatic or electromagnetic seeding in enhancing SRS from weak-intensity speckles. A major finding is that seeding operates over unexpectedly long times ( 15 - 20 ps under our experimental conditions). Similar results are obtained in lower-density plasmas, or when the weak pulse is smoothed by a random phase plate, thus leading to multiple speckle interaction, while the strong pulse is focused within the speckle pattern. The data are discussed with the help of particle-in-cell numerical simulations, which confirm the destabilizing effect of the strong pulse over the weak one after a short transient time.

Detonation Reaction Zones in Condensed Explosives

NASA Astrophysics Data System (ADS)

Tarver, Craig M.

2006-07-01

Experimental measurements using nanosecond time resolved embedded gauges and laser interferometric techniques, combined with Non-Equilibrium Zeldovich - von Neumann - Doling (NEZND) theory and Ignition and Growth reactive flow hydrodynamic modeling, have revealed the average pressure/particle velocity states attained in reaction zones of self-sustaining detonation waves in several solid and liquid explosives. The time durations of these reaction zone processes are discussed for explosives based on pentaerythritol tetranitrate (PETN), nitromethane, octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX), triaminitrinitrobenzene(TATB) and trinitrotoluene (TNT).

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

PubMed

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

2016-08-10

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

Experimental optimization of directed field ionization

NASA Astrophysics Data System (ADS)

Liu, Zhimin Cheryl; Gregoric, Vincent C.; Carroll, Thomas J.; Noel, Michael W.

2017-04-01

The state distribution of an ensemble of Rydberg atoms is commonly measured using selective field ionization. The resulting time resolved ionization signal from a single energy eigenstate tends to spread out due to the multiple avoided Stark level crossings atoms must traverse on the way to ionization. The shape of the ionization signal can be modified by adding a perturbation field to the main field ramp. Here, we present experimental results of the manipulation of the ionization signal using a genetic algorithm. We address how both the genetic algorithm and the experimental parameters were adjusted to achieve an optimized result. This work was supported by the National Science Foundation under Grants No. 1607335 and No. 1607377.

Effects of mother-infant skin-to-skin contact on severe latch-on problems in older infants: a randomized trial.

PubMed

Svensson, Kristin E; Velandia, Marianne I; Matthiesen, Ann-Sofi T; Welles-Nyström, Barbara L; Widström, Ann-Marie E

2013-03-11

Infants with latch-on problems cause stress for parents and staff, often resulting in early termination of breastfeeding. Healthy newborns experiencing skin-to-skin contact at birth are pre-programmed to find the mother's breast. This study investigates if skin-to-skin contact between mothers with older infants having severe latching on problems would resolve the problem. Mother-infant pairs with severe latch-on problems, that were not resolved during screening procedures at two maternity hospitals in Stockholm 1998-2004, were randomly assigned to skin-to-skin contact (experimental group) or not (control group) during breastfeeding. Breastfeeding counseling was given to both groups according to a standard model. Participants were unaware of their treatment group. Objectives were to compare treatment groups concerning the proportion of infants regularly latching on, the time from intervention to regular latching on and maternal emotions and pain before and during breastfeeding. On hundred and three mother-infant pairs with severe latch-on problems 1-16 weeks postpartum were randomly assigned and analyzed. There was no significant difference between the groups in the proportion of infants starting regular latching-on (75% experimental group, vs. 86% control group). Experimental group infants, who latched on, had a significantly shorter median time from start of intervention to regular latching on than control infants, 2.0 weeks (Q1 = 1.0, Q3 = 3.7) vs. 4.7 weeks (Q1 = 2.0, Q3 = 8.0), (p-value = 0.020). However, more infants in the experimental group (94%), with a history of "strong reaction" during "hands-on latch intervention", latched-on within 3 weeks compared to 33% in the control infants (Fisher Exact test p-value = 0.0001). Mothers in the experimental group (n = 53) had a more positive breastfeeding experience according to the Breastfeeding Emotional Scale during the intervention than mothers in the control group (n = 50) (p-value = 0.022). Skin-to-skin contact during breastfeeding seems to immediately enhance maternal positive feelings and shorten the time it takes to resolve severe latch-on problems in the infants who started to latch. An underlying mechanism may be that skin-to-skin contact with the mother during breastfeeding may calm infants with earlier strong reaction to "hands on latch intervention" and relieve the stress which may have blocked the infant's inborn biological program to find the breast and latch on. Karolinska Clinical Trial Registration number CT20100055.

Flow topologies and turbulence scales in a jet-in-cross-flow

DOE PAGES

Oefelein, Joseph C.; Ruiz, Anthony M.; Lacaze, Guilhem

2015-04-03

This study presents a detailed analysis of the flow topologies and turbulence scales in the jet-in-cross-flow experiment of [Su and Mungal JFM 2004]. The analysis is performed using the Large Eddy Simulation (LES) technique with a highly resolved grid and time-step and well controlled boundary conditions. This enables quantitative agreement with the first and second moments of turbulence statistics measured in the experiment. LES is used to perform the analysis since experimental measurements of time-resolved 3D fields are still in their infancy and because sampling periods are generally limited with direct numerical simulation. A major focal point is the comprehensivemore » characterization of the turbulence scales and their evolution. Time-resolved probes are used with long sampling periods to obtain maps of the integral scales, Taylor microscales, and turbulent kinetic energy spectra. Scalar-fluctuation scales are also quantified. In the near-field, coherent structures are clearly identified, both in physical and spectral space. Along the jet centerline, turbulence scales grow according to a classical one-third power law. However, the derived maps of turbulence scales reveal strong inhomogeneities in the flow. From the modeling perspective, these insights are useful to design optimized grids and improve numerical predictions in similar configurations.« less

Experimental technique for measuring the isentrope of hydrogen to several megabars

NASA Astrophysics Data System (ADS)

Barker, L. M.; Truncano, T. G.; Wise, J. I.; Asay, J. R.

The experimental measurement of the Equations of State (EOS) of hydrogen has been of interest for some time because of the theoretical expectation of a transition to the metallic state in the multi-megabar pressure regime. Previous experiments have reported results which are consistent with a metallic transition, but experimental uncertainties have precluded positive identification of the metallic phase. In this paper we describe a new experimental approach to the measurement of the high-pressure EOS of hydrogen. A cryogenic hydrogen specimen, either liquid or solid, is located in the muzzle of a gun barrel between a tungsten anvil and another tungsten disk called a shim. Helium gas in the gun barrel cushions the impact and allows nearly isentropic compression of the hydrogen. The time-resolved pressure in the specimen is calculated from a laser interferometer (VISAR) measurement of the acceleration history of the anvil's free surface, and volume measurements at specific times are made by combining VISAR data, which define the position of the anvil, with flash X-ray photographs which define the shim position.

Time- and frequency-dependent model of time-resolved coherent anti-Stokes Raman scattering (CARS) with a picosecond-duration probe pulse

NASA Astrophysics Data System (ADS)

Stauffer, Hans U.; Miller, Joseph D.; Slipchenko, Mikhail N.; Meyer, Terrence R.; Prince, Benjamin D.; Roy, Sukesh; Gord, James R.

2014-01-01

The hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) technique presents a promising alternative to either fs time-resolved or ps frequency-resolved CARS in both gas-phase thermometry and condensed-phase excited-state dynamics applications. A theoretical description of time-dependent CARS is used to examine this recently developed probe technique, and quantitative comparisons of the full time-frequency evolution show excellent accuracy in predicting the experimental vibrational CARS spectra obtained for two model systems. The interrelated time- and frequency-domain spectral signatures of gas-phase species produced by hybrid fs/ps CARS are explored with a focus on gas-phase N2 vibrational CARS, which is commonly used as a thermometric diagnostic of combusting flows. In particular, we discuss the merits of the simple top-hat spectral filter typically used to generate the ps-duration hybrid fs/ps CARS probe pulse, including strong discrimination against non-resonant background that often contaminates CARS signal. It is further demonstrated, via comparison with vibrational CARS results on a time-evolving solvated organic chromophore, that this top-hat probe-pulse configuration can provide improved spectral resolution, although the degree of improvement depends on the dephasing timescales of the observed molecular modes and the duration and timing of the narrowband final pulse. Additionally, we discuss the virtues of a frequency-domain Lorentzian probe-pulse lineshape and its potential for improving the hybrid fs/ps CARS technique as a diagnostic in high-pressure gas-phase thermometry applications.

Time- and frequency-dependent model of time-resolved coherent anti-Stokes Raman scattering (CARS) with a picosecond-duration probe pulse.

PubMed

Stauffer, Hans U; Miller, Joseph D; Slipchenko, Mikhail N; Meyer, Terrence R; Prince, Benjamin D; Roy, Sukesh; Gord, James R

2014-01-14

The hybrid femtosecond∕picosecond coherent anti-Stokes Raman scattering (fs∕ps CARS) technique presents a promising alternative to either fs time-resolved or ps frequency-resolved CARS in both gas-phase thermometry and condensed-phase excited-state dynamics applications. A theoretical description of time-dependent CARS is used to examine this recently developed probe technique, and quantitative comparisons of the full time-frequency evolution show excellent accuracy in predicting the experimental vibrational CARS spectra obtained for two model systems. The interrelated time- and frequency-domain spectral signatures of gas-phase species produced by hybrid fs∕ps CARS are explored with a focus on gas-phase N2 vibrational CARS, which is commonly used as a thermometric diagnostic of combusting flows. In particular, we discuss the merits of the simple top-hat spectral filter typically used to generate the ps-duration hybrid fs∕ps CARS probe pulse, including strong discrimination against non-resonant background that often contaminates CARS signal. It is further demonstrated, via comparison with vibrational CARS results on a time-evolving solvated organic chromophore, that this top-hat probe-pulse configuration can provide improved spectral resolution, although the degree of improvement depends on the dephasing timescales of the observed molecular modes and the duration and timing of the narrowband final pulse. Additionally, we discuss the virtues of a frequency-domain Lorentzian probe-pulse lineshape and its potential for improving the hybrid fs∕ps CARS technique as a diagnostic in high-pressure gas-phase thermometry applications.

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

PubMed

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.

Two-dimensional time-resolved X-ray diffraction study of liquid/solid fraction and solid particle size in Fe-C binary system with an electrostatic levitator furnace

NASA Astrophysics Data System (ADS)

Yonemura, M.; Okada, J.; Watanabe, Y.; Ishikawa, T.; Nanao, S.; Shobu, T.; Toyokawa, H.

2013-03-01

Liquid state provides functions such as matter transport or a reaction field and plays an important role in manufacturing processes such as refining, forging or welding. However, experimental procedures are significantly difficult for an observation of solidification process of iron and iron-based alloys in order to identify rapid transformations subjected to fast temperature evolution. Therefore, in order to study the solidification in iron and iron-based alloys, we considered a combination of high energy X-ray diffraction measurements and an electrostatic levitation method (ESL). In order to analyze the liquid/solid fraction, the solidification of melted spherical specimens was measured at a time resolution of 0.1 seconds during rapid cooling using the two-dimensional time-resolved X-ray diffraction. Furthermore, the observation of particle sizes and phase identification was performed on a trial basis using X-ray small angle scattering with X-ray diffraction.

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

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

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Time-Resolved Kinetic Chirped-Pulse Rotational Spectroscopy in a Room-Temperature Flow Reactor

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

Zaleski, Daniel P.; Harding, Lawrence B.; Klippenstein, Stephen J.

Chirped-pulse Fourier transform millimeter-wave spectroscopy is a potentially powerful tool for studying chemical reaction dynamics and kinetics. Branching ratios of multiple reaction products and intermediates can be measured with unprecedented chemical specificity; molecular isomers, conformers, and vibrational states have distinct rotational spectra. Here we demonstrate chirped-pulse spectroscopy of vinyl cyanide photoproducts in a flow tube reactor at ambient temperature of 295 K and pressures of 1-10 mu bar. This in situ and time-resolved experiment illustrates the utility of this novel approach to investigating chemical reaction dynamics and kinetics. Following 193 nm photodissociation of CH2CHCN, we observe rotational relaxation of energizedmore » HCN, HNC, and HCCCN photoproducts with 10 mu s time resolution and sample the vibrational population distribution of HCCCN. The experimental branching ratio HCN/HCCCN is compared with a model based on RRKM theory using high-level ab initio calculations, which were in turn validated by comparisons to Active Thermochemical Tables enthalpies.« less

Time-Resolved Kinetic Chirped-Pulse Rotational Spectroscopy in a Room-Temperature Flow Reactor

DOE PAGES

Zaleski, Daniel P.; Harding, Lawrence B.; Klippenstein, Stephen J.; ...

2017-12-01

Chirped-pulse Fourier transform millimeter-wave spectroscopy is a potentially powerful tool for studying chemical reaction dynamics and kinetics. Branching ratios of multiple reaction products and intermediates can be measured with unprecedented chemical specificity; molecular isomers, conformers, and vibrational states have distinct rotational spectra. Here we demonstrate chirped-pulse spectroscopy of vinyl cyanide photoproducts in a flow tube reactor at ambient temperature of 295 K and pressures of 1-10 mu bar. This in situ and time-resolved experiment illustrates the utility of this novel approach to investigating chemical reaction dynamics and kinetics. Following 193 nm photodissociation of CH2CHCN, we observe rotational relaxation of energizedmore » HCN, HNC, and HCCCN photoproducts with 10 mu s time resolution and sample the vibrational population distribution of HCCCN. The experimental branching ratio HCN/HCCCN is compared with a model based on RRKM theory using high-level ab initio calculations, which were in turn validated by comparisons to Active Thermochemical Tables enthalpies.« less

Ultrafast Imaging of Surface Plasmons Propagating on a Gold Surface

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

Gong, Yu; Joly, Alan G.; Hu, Dehong

2015-05-13

We record time-resolved nonlinear photoemission electron microscopy (tr-PEEM) images of propagating surface plasmons (PSPs) launched from a lithographically patterned rectangular trench on a flat gold surface. Our tr-PEEM scheme involves a pair of identical, spatially separated, and interferometrically-locked femtosecond laser pulses. Power dependent PEEM images provide experimental evidence for a sequential coherent nonlinear photoemission process, in which one laser source creates a PSP polarization state through a linear interaction, and the second subsequently probes the prepared state via two photon photoemission. The recorded time-resolved movies of a PSP allow us to directly measure various properties of the surface-bound wave packet,more » including its carrier wavelength (785 nm) and group velocity (0.95c). In addition, tr-PEEM in concert with finite-difference time domain simulations together allow us to set a lower limit of 75 μm for the decay length of the PSP on a 100 nm thick gold film.« less

Influence of hydrostatic pressure on dynamics and spatial distribution of protein partial molar volume: time-resolved surficial Kirkwood-Buff approach.

PubMed

Yu, Isseki; Tasaki, Tomohiro; Nakada, Kyoko; Nagaoka, Masataka

2010-09-30

The influence of hydrostatic pressure on the partial molar volume (PMV) of the protein apomyoglobin (AMb) was investigated by all-atom molecular dynamics (MD) simulations. Using the time-resolved Kirkwood-Buff (KB) approach, the dynamic behavior of the PMV was identified. The simulated time average value of the PMV and its reduction by 3000 bar pressurization correlated with experimental data. In addition, with the aid of the surficial KB integral method, we obtained the spatial distributions of the components of PMV to elucidate the detailed mechanism of the PMV reduction. New R-dependent PMV profiles identified the regions that increase or decrease the PMV under the high pressure condition. The results indicate that besides the hydration in the vicinity of the protein surface, the outer space of the first hydration layer also significantly influences the total PMV change. These results provide a direct and detailed picture of pressure induced PMV reduction.

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

NASA Astrophysics Data System (ADS)

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.

Time-resolved x-ray diffraction and electrical resistance measurements of structural phase transitions in zirconium

DOE PAGES

Velisavljevic, N.; Sinogeikin, S.; Saavedra, R.; ...

2014-05-07

Here, we have designed a portable pressure controller module to tune compression rates and maximum pressures attainable in a standard gas-membrane diamond anvil cell (DAC). During preliminary experiments, performed on zirconium (Zr) metal sample, pressure jumps of up to 80 GPa were systematically obtained in less than 0.2s (resulting in compression rate of few GPa/s up to more than 400 GPa/s). In-situ x-ray diffraction and electrical resistance measurements were performed simultaneously during this rapid pressure increase to provide the first time resolved data on α → ω → β structural evolution in Zr at high pressures. Direct control of compressionmore » rates and peak pressures, which can be held for prolonged time, allows for investigation of structural evolution and kinetics of structural phase transitions of materials under previously unexplored compression rate-pressure conditions that bridge traditional static and shock/dynamic experimental platforms.« less

Evaluating the accuracy of recent electron transport models at predicting Hall thruster plasma dynamics

NASA Astrophysics Data System (ADS)

Cappelli, Mark; Young, Christopher

2016-10-01

We present continued efforts towards introducing physical models for cross-magnetic field electron transport into Hall thruster discharge simulations. In particular, we seek to evaluate whether such models accurately capture ion dynamics, both averaged and resolved in time, through comparisons with measured ion velocity distributions which are now becoming available for several devices. Here, we describe a turbulent electron transport model that is integrated into 2-D hybrid fluid/PIC simulations of a 72 mm diameter laboratory thruster operating at 400 W. We also compare this model's predictions with one recently proposed by Lafluer et al.. Introducing these models into 2-D hybrid simulations is relatively straightforward and leverages the existing framework for solving the electron fluid equations. The models are tested for their ability to capture the time-averaged experimental discharge current and its fluctuations due to ionization instabilities. Model predictions are also more rigorously evaluated against recent laser-induced fluorescence measurements of time-resolved ion velocity distributions.

Nanosecond step-scan FT-infrared absorption spectroscopy in photochemistry and catalysis

NASA Astrophysics Data System (ADS)

Frei, H.

1998-06-01

Time-resolved step-scan FT-IR absorption spectroscopy has been expanded to a resolution of 20 nanosecond. Following a description of the experimental set-up, applications in four research areas are presented. In the first project, we discuss a reversible isomerization, namely the bacteriorhodopsin photocycle. Main results are the discovery of 2 processes with distinct kinetics on the nanosecond time scale not detected by previous spectroscopic techniques, and observation of an instantaneous response of the protein environment to chromophore dynamics within the nanosecond laser pulse duration. In a second project, alkane C-H bond activation by a transition metal complex in room temperature solution is investigated and the first measurement of the formation of a C-H insertion product reported (alkyl hydride). Then, a nanosecond study of a pericyclic reaction, the ring-opening of cyclohexadiene, is discussed. The fourth example describes the first observation of a transient molecule in a zeolite matrix, a triplet excited quinone, by time-resolved infrared spectroscopy.

Large-k exciton dynamics in GaN epilayers: Nonthermal and thermal regimes

NASA Astrophysics Data System (ADS)

Vinattieri, Anna; Bogani, Franco; Cavigli, Lucia; Manzi, Donatella; Gurioli, Massimo; Feltin, Eric; Carlin, Jean-François; Martin, Denis; Butté, Raphaël; Grandjean, Nicolas

2013-02-01

We present a detailed investigation performed at low temperature (T<50 K) concerning the exciton dynamics in GaN epilayers grown on c-plane sapphire substrates, focusing on the exciton formation and the transition from the nonthermal to the thermal regime. The time-resolved kinetics of longitudinal-optical-phonon replicas is used to address the energy relaxation in the excitonic band. From picosecond time-resolved spectra, we bring evidence for a long lasting nonthermal excitonic distribution, which accounts for the first 50 ps. Such a behavior is confirmed in different experimental conditions when both nonresonant and resonant excitations are used. At low excitation power density, the exciton formation and their subsequent thermalization are dominated by impurity scattering rather than by acoustic phonon scattering. The estimate of the average energy of the excitons as a function of delay after the excitation pulse provides information on the relaxation time, which describes the evolution of the exciton population to the thermal regime.

Time-Resolved Luminescence Nanothermometry with Nitrogen-Vacancy Centers in Nanodiamonds

NASA Astrophysics Data System (ADS)

Tsai, Pei-Chang; Chen, Oliver Y.; Tzeng, Yan-Kai; Liu, Hsiou-Yuan; Hsu, Hsiang; Huang, Shaio-Chih; Chen, Jeson; Yee, Fu-Ghoul; Chang, Huan-Cheng; Chang, Ming-Shien

2016-05-01

Measuring thermal properties with nanoscale spatial resolution either at or far from equilibrium is gaining importance in many scientific and engineering applications. Although negatively charged nitrogen-vacancy (NV-) centers in diamond have recently emerged as promising nanometric temperature sensors, most previous measurements were performed under steady state conditions. Here we employ a three-point sampling method which not only enables real-time detection of temperature changes over +/-100 K with a sensitivity of 2 K/(Hz)1/2, but also allows the study of nanometer scale heat transfer with a temporal resolution of better than 1 μs with the use of a pump-probe-type experiment. In addition to temperature sensing, we further show that nanodiamonds conjugated with gold nanorods, as optically-activated dual-functional nanoheaters and nanothermometers, are useful for highly localized hyperthermia treatment. We experimentally demonstrated time-resolved fluorescence nanothermometry, and the validity of the measurements was verified with finite-element numerical simulations. The approaches provided here will be useful for probing dynamical thermal properties on nanodevices in operation.

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE PAGES

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung; ...

2017-05-24

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Hugoniot measurements of double-shocked precompressed dense xenon plasmas

NASA Astrophysics Data System (ADS)

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

2012-12-01

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

Characterization of Ultrafast Laser Pulses using a Low-dispersion Frequency Resolved Optical Grating Spectrometer

NASA Astrophysics Data System (ADS)

Whitelock, Hope; Bishop, Michael; Khosravi, Soroush; Obaid, Razib; Berrah, Nora

2016-05-01

A low dispersion frequency-resolved optical gating (FROG) spectrometer was designed to characterize ultrashort (<50 femtosecond) laser pulses from a commercial regenerative amplifier, optical parametric amplifier, and a home-built non-colinear optical parametric amplifier. This instrument splits a laser pulse into two replicas with a 90:10 intensity ratio using a thin pellicle beam-splitter and then recombines the pulses in a birefringent medium. The instrument detects a wavelength-sensitive change in polarization of the weak probe pulse in the presence of the stronger pump pulse inside the birefringent medium. Scanning the time delay between the two pulses and acquiring spectra allows for characterization of the frequency and time content of ultrafast laser pulses, that is needed for interpretation of experimental results obtained from these ultrafast laser systems. Funded by the DoE-BES, Grant No. DE-SC0012376.

Denoising time-resolved microscopy image sequences with singular value thresholding.

PubMed

Furnival, Tom; Leary, Rowan K; Midgley, Paul A

2017-07-01

Time-resolved imaging in microscopy is important for the direct observation of a range of dynamic processes in both the physical and life sciences. However, the image sequences are often corrupted by noise, either as a result of high frame rates or a need to limit the radiation dose received by the sample. Here we exploit both spatial and temporal correlations using low-rank matrix recovery methods to denoise microscopy image sequences. We also make use of an unbiased risk estimator to address the issue of how much thresholding to apply in a robust and automated manner. The performance of the technique is demonstrated using simulated image sequences, as well as experimental scanning transmission electron microscopy data, where surface adatom motion and nanoparticle structural dynamics are recovered at rates of up to 32 frames per second. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

Electronic and Vibrational Coherence in Charge-Transfer Reactions

NASA Astrophysics Data System (ADS)

Scherer, Norbert

1996-03-01

The ultrafast dynamics associated with optically-induced intervalence charge-transfer reactions in solution and protein environments are reported. These studies include the Fe^(II)-Fe^(III) MMCT complex Prussian blue and the mixed valence dimer (CN)_5Ru^(II)CNRuRu^(III)(NH_3)_5. The protein systems include blue copper proteins and the bacterial photosynthetic reaction center. The experimental approaches include photon echo, wavelength-resolved pump-probe and anisotropy measurements performed with 12-16fs duration optical pulses. Complicated time-domain waveforms reflect the several different p[rocesses and time scales for relaxation of coherences (both electronic and vibrational) and populations within these systems. The photon echo and anisotropy results probe electronic coherence and dephasing prior to back electron transfer. Wavelength-resolved pump-probe results reveal vibrational modes coupled to the CT-coordinate as well as formation of new product states or vibrational cooling in the ground state following back electron transfer.

Effects of inlet boundary conditions, on the computed flow in the Turbine-99 draft tube, using OpenFOAM and CFX

NASA Astrophysics Data System (ADS)

Nilsson, H.; Cervantes, M. J.

2012-11-01

The flow in the Turbine-99 Kaplan draft tube was thoroughly investigated at three workshops (1999, 2001, 2005), which aimed at determining the state of the art of draft tube simulations. The flow is challenging due to the different flow phenomena appearing simultaneously such as unsteadiness, separation, swirl, turbulence, and a strong adverse pressure gradient. The geometry and the experimentally determined inlet boundary conditions were provided to the Turbine-99 workshop participants. At the final workshop, angular resolved inlet velocity boundary conditions were provided. The rotating non-axi-symmetry of the inlet flow due to the runner blades was thus included. The effect of the rotating angular resolution was however not fully investigated at that workshop. The first purpose of this work is to further investigate this effect. Several different inlet boundary conditions are applied - the angular resolved experimental data distributed at the Turbine-99 workshop, the angular resolved results of a runner simulation with interpolated values using different resolution in the tangential and radial directions, and an axi-symmetric variant of the same numerical data. The second purpose of this work is to compare the results from the OpenFOAM and CFX CFD codes, using as similar settings as possible. The present results suggest that the experimental angular inlet boundary conditions proposed to the workshop are not adequate to simulate accurately the flow in the T-99 draft tube. The reason for this is that the experimental phase-averaged data has some important differences compared to the previously measured time-averaged data. Using the interpolated data from the runner simulation as inlet boundary condition however gives good results as long as the resolution of that data is sufficient. It is shown that the difference between the results using the angular-resolved and the corresponding symmetric inlet data is very small, suggesting that the importance of the angular resolution is small. The results from OpenFOAM and CFX are very similar as long as the inlet data resolution is fine enough. CFX seems to be more sensitive to that resolution.

Spatially resolved X-ray emission measurements of the residual velocity during the stagnation phase of inertial confinement fusion implosion experiments

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

Ruby, J. J.; Pak, A., E-mail: pak5@llnl.gov; Field, J. E.

2016-07-15

A technique for measuring residual motion during the stagnation phase of an indirectly driven inertial confinement experiment has been implemented. This method infers a velocity from spatially and temporally resolved images of the X-ray emission from two orthogonal lines of sight. This work investigates the accuracy of recovering spatially resolved velocities from the X-ray emission data. A detailed analytical and numerical modeling of the X-ray emission measurement shows that the accuracy of this method increases as the displacement that results from a residual velocity increase. For the typical experimental configuration, signal-to-noise ratios, and duration of X-ray emission, it is estimatedmore » that the fractional error in the inferred velocity rises above 50% as the velocity of emission falls below 24 μm/ns. By inputting measured parameters into this model, error estimates of the residual velocity as inferred from the X-ray emission measurements are now able to be generated for experimental data. Details of this analysis are presented for an implosion experiment conducted with an unintentional radiation flux asymmetry. The analysis shows a bright localized region of emission that moves through the larger emitting volume at a relatively higher velocity towards the location of the imposed flux deficit. This technique allows for the possibility of spatially resolving velocity flows within the so-called central hot spot of an implosion. This information would help to refine our interpretation of the thermal temperature inferred from the neutron time of flight detectors and the effect of localized hydrodynamic instabilities during the stagnation phase. Across several experiments, along a single line of sight, the average difference in magnitude and direction of the measured residual velocity as inferred from the X-ray and neutron time of flight detectors was found to be ∼13 μm/ns and ∼14°, respectively.« less

Spatially resolved X-ray emission measurements of the residual velocity during the stagnation phase of inertial confinement fusion implosion experiments

DOE PAGES

Ruby, J. J.; Pak, A.; Field, J. E.; ...

2016-07-01

A technique for measuring residual motion during the stagnation phase of an indirectly driven inertial confinement experiment has been implemented. Our method infers a velocity from spatially and temporally resolved images of the X-ray emission from two orthogonal lines of sight. This work investigates the accuracy of recovering spatially resolved velocities from the X-ray emission data. A detailed analytical and numerical modeling of the X-ray emission measurement shows that the accuracy of this method increases as the displacement that results from a residual velocity increase. For the typical experimental configuration, signal-to-noise ratios, and duration of X-ray emission, it is estimatedmore » that the fractional error in the inferred velocity rises above 50% as the velocity of emission falls below 24 μm/ns. Furthermore, by inputting measured parameters into this model, error estimates of the residual velocity as inferred from the X-ray emission measurements are now able to be generated for experimental data. Details of this analysis are presented for an implosion experiment conducted with an unintentional radiation flux asymmetry. The analysis shows a bright localized region of emission that moves through the larger emitting volume at a relatively higher velocity towards the location of the imposed flux deficit. Our technique allows for the possibility of spatially resolving velocity flows within the so-called central hot spot of an implosion. This information would help to refine our interpretation of the thermal temperature inferred from the neutron time of flight detectors and the effect of localized hydrodynamic instabilities during the stagnation phase. Across several experiments, along a single line of sight, the average difference in magnitude and direction of the measured residual velocity as inferred from the X-ray and neutron time of flight detectors was found to be ~13 μm/ns and ~14°, respectively.« less

Effetto black drop e istanti dei contatti nel transito di Venere sul Sole

NASA Astrophysics Data System (ADS)

di Giovanni, Giovanni

2005-04-01

Digital measurements of the chords common to the Sun and Venus during the transit of 8 June 2004 are reported. The time of the four contacts of the planet with the solar limb are calculated resolving the relative equations for entry and exit phases. The solutions were obtained with least square methods applied to experimental data with analytical functions used by different Authors during the Sun's eclipses. The well-known black drop effect was observed during the third contact. Atmospheric turbulence and optical effects interfere making timings uncertain by at least one second. There is also a comment about the numerical values and the estimate of the experimental errors. The observations were made by four high school students.

Experimental joint weak measurement on a photon pair as a probe of Hardy's paradox.

PubMed

Lundeen, J S; Steinberg, A M

2009-01-16

It has been proposed that the ability to perform joint weak measurements on postselected systems would allow us to study quantum paradoxes. These measurements can investigate the history of those particles that contribute to the paradoxical outcome. Here we experimentally perform weak measurements of joint (i.e., nonlocal) observables. In an implementation of Hardy's paradox, we weakly measure the locations of two photons, the subject of the conflicting statements behind the paradox. Remarkably, the resulting weak probabilities verify all of these statements but, at the same time, resolve the paradox.

Experimental search for Exact Coherent Structures in turbulent small aspect ratio Taylor-Couette flow

NASA Astrophysics Data System (ADS)

Crowley, Christopher J.; Krygier, Michael; Grigoriev, Roman O.; Schatz, Michael F.

2017-11-01

Recent theoretical and experimental work suggests that the dynamics of turbulent flows are guided by unstable nonchaotic solutions to the Navier-Stokes equations. These solutions, known as exact coherent structures (ECS), play a key role in a fundamentally deterministic description of turbulence. In order to quantitatively demonstrate that actual turbulence in 3D flows is guided by ECS, high resolution, 3D-3C experimental measurements of the velocity need to be compared to solutions from direct numerical simulation of the Navier-Stokes equations. In this talk, we will present experimental measurements of fully time resolved, velocity measurements in a volume of turbulence in a counter-rotating, small aspect ratio Taylor-Couette flow. This work is supported by the Army Research Office (Contract # W911NF-16-1-0281).

Experimental evidence of hourglass fermion in the candidate nonsymmorphic topological insulator KHgSb

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

Ma, Junzhang; Yi, Changjiang; Lv, Baiqing

Topological insulators (TIs) host novel states of quantum matter characterized by nontrivial conducting boundary states connecting valence and conduction bulk bands. All TIs discovered experimentally so far rely on either time-reversal or mirror crystal symmorphic symmetry to protect massless Dirac-like boundary states. Several materials were recently proposed to be TIs with nonsymmorphic symmetry, where a glide mirror protects exotic surface fermions with hourglass-shaped dispersion. However, an experimental confirmation of this new fermion is missing. Using angle-resolved photoemission spectroscopy, we provide experimental evidence of hourglass fermions on the (010) surface of crystalline KHgSb, whereas the (001) surface has no boundary state,more » in agreement with first-principles calculations. Our study will stimulate further research activities of topological properties of nonsymmorphic materials.« less

Experimental evidence of hourglass fermion in the candidate nonsymmorphic topological insulator KHgSb

DOE PAGES

Ma, Junzhang; Yi, Changjiang; Lv, Baiqing; ...

2017-05-05

Topological insulators (TIs) host novel states of quantum matter characterized by nontrivial conducting boundary states connecting valence and conduction bulk bands. All TIs discovered experimentally so far rely on either time-reversal or mirror crystal symmorphic symmetry to protect massless Dirac-like boundary states. Several materials were recently proposed to be TIs with nonsymmorphic symmetry, where a glide mirror protects exotic surface fermions with hourglass-shaped dispersion. However, an experimental confirmation of this new fermion is missing. Using angle-resolved photoemission spectroscopy, we provide experimental evidence of hourglass fermions on the (010) surface of crystalline KHgSb, whereas the (001) surface has no boundary state,more » in agreement with first-principles calculations. Our study will stimulate further research activities of topological properties of nonsymmorphic materials.« less

Excited-state dissociation dynamics of phenol studied by a new time-resolved technique

NASA Astrophysics Data System (ADS)

Lin, Yen-Cheng; Lee, Chin; Lee, Shih-Huang; Lee, Yin-Yu; Lee, Yuan T.; Tseng, Chien-Ming; Ni, Chi-Kung

2018-02-01

Phenol is an important model molecule for the theoretical and experimental investigation of dissociation in the multistate potential energy surfaces. Recent theoretical calculations [X. Xu et al., J. Am. Chem. Soc. 136, 16378 (2014)] suggest that the phenoxyl radical produced in both the X and A states from the O-H bond fission in phenol can contribute substantially to the slow component of photofragment translational energy distribution. However, current experimental techniques struggle to separate the contributions from different dissociation pathways. A new type of time-resolved pump-probe experiment is described that enables the selection of the products generated from a specific time window after molecules are excited by a pump laser pulse and can quantitatively characterize the translational energy distribution and branching ratio of each dissociation pathway. This method modifies conventional photofragment translational spectroscopy by reducing the acceptance angles of the detection region and changing the interaction region of the pump laser beam and the molecular beam along the molecular beam axis. The translational energy distributions and branching ratios of the phenoxyl radicals produced in the X, A, and B states from the photodissociation of phenol at 213 and 193 nm are reported. Unlike other techniques, this method has no interference from the undissociated hot molecules. It can ultimately become a standard pump-probe technique for the study of large molecule photodissociation in multistates.

Single-shot Monitoring of Ultrafast Processes via X-ray Streaking at a Free Electron Laser.

PubMed

Buzzi, Michele; Makita, Mikako; Howald, Ludovic; Kleibert, Armin; Vodungbo, Boris; Maldonado, Pablo; Raabe, Jörg; Jaouen, Nicolas; Redlin, Harald; Tiedtke, Kai; Oppeneer, Peter M; David, Christian; Nolting, Frithjof; Lüning, Jan

2017-08-03

The advent of x-ray free electron lasers has extended the unique capabilities of resonant x-ray spectroscopy techniques to ultrafast time scales. Here, we report on a novel experimental method that allows retrieving with a single x-ray pulse the time evolution of an ultrafast process, not only at a few discrete time delays, but continuously over an extended time window. We used a single x-ray pulse to resolve the laser-induced ultrafast demagnetisation dynamics in a thin cobalt film over a time window of about 1.6 ps with an excellent signal to noise ratio. From one representative single shot measurement we extract a spin relaxation time of (130 ± 30) fs with an average value, based on 193 single shot events of (113 ± 20) fs. These results are limited by the achieved experimental time resolution of 120 fs, and both values are in excellent agreement with previous results and theoretical modelling. More generally, this new experimental approach to ultrafast x-ray spectroscopy paves the way to the study of non-repetitive processes that cannot be investigated using traditional repetitive pump-probe schemes.

Ultrafast measurements of chlorine dioxide photochemistry

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

Ludowise, P.D.

Time-resolved mass spectrometry and time-resolved photoelectron spectroscopy are used to study the ultrafast photodissociation dynamics of chlorine dioxide, an important constituent in stratospheric ozone depletion. Chapter 1 introduces these pump/probe techniques, in which a femtosecond pump pulse excites a molecule to a dissociative state. At a later time, a second femtosecond probe pulse ionizes the molecule. The resulting mass and photoelectron spectra are acquired as a function of the delay between the pump and probe pulses, which follows the evolution of the molecule on the excited state. A comparison to other techniques used to study reaction dynamics is discussed. Chaptermore » 2 includes a detailed description of the design and construction of the experimental apparatus, which consists of a femtosecond laser system, a molecular beam time-of-flight spectrometer, and a data acquisition system. The time-of-flight spectrometer is specifically designed to have a short flight distance to maximize the photoelectron collection efficiency without degrading the resolution, which is limited by the bandwidth of the femtosecond laser system. Typical performance of the apparatus is demonstrated in a study of the time-resolved photoelectron spectroscopy of nitric oxide. The results of the time-resolved mass spectrometry experiments of chlorine dioxide are presented in Chapter 3. Upon excitation to the A {sup 2}A{sub 2} state near 3.2 eV, the molecule dissociates through an indirect two-step mechanism. The direct dissociation channel has been predicted to be open, but is not observed. A quantum beat is observed in the OClO{sup +} species, which is described as a vibrational coherence of the optically prepared A {sup 2}A{sub 2} state. Chapter 4 presents the results of the time-resolved photoelectron experiments of chlorine dioxide. At short delay time, the quantum beat of the OClO{sup +} species is observed in the X {sup 1}A{sub 1} state of the ion. At infinite delay, the signal is dominated by the ClO{sup +} ion, observed in a variety of electronic states. The photoelectron data is shown to support the indirect two-step dissociation mechanism derived from the mass results. Conclusions of the mass and photoelectron results are discussed in context of the stratospheric ozone depletion problem.« less

Nonlinear Optical Spectroscopy in the Time Domain: Studies of Ultrafast Molecular Processes in the Condensed Phase.

NASA Astrophysics Data System (ADS)

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. Finally, a new inverse transform procedure is presented that calculates the absorption band (ABS) from an experimental Raman excitation profile (REP). An iterative solution is sought for an integral Hilbert transform relation. An exact ABS is recovered regardless of the starting ABS when sufficient iterations are performed.

Femtosecond mega-electron-volt electron microdiffraction

DOE PAGES

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

2017-09-01

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

Femtosecond mega-electron-volt electron microdiffraction

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

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

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

Time-resolved spectral analysis of Radachlorin luminescence in water

NASA Astrophysics Data System (ADS)

Belik, V. P.; Gadzhiev, I. M.; Semenova, I. V.; Vasyutinskii, O. S.

2017-05-01

We report results of spectral- and time-resolved study of Radachlorin photosensitizer luminescence in water in the spectral range of 950-1350nm and for determination of the photosensitizer triplet state and the singlet oxygen lifetimes responsible for singlet oxygen generation and degradation. At any wavelength within the explored spectral range the luminescence decay contained two major contributions: a fast decay at the ns time scale and a slow evolution at the μs time scale. The fast decay was attributed to electric dipole fluorescence transitions in photosensitizer molecules and the slow evolution to intercombination phosphorescence transitions in singlet oxygen and photosensitizer molecules. Relatively high-amplitude ns peak observed at all wavelengths suggests that singlet oxygen monitoring with spectral isolation methods alone, without additional temporal resolution can be controversial. In the applied experimental conditions the total phosphorescence signal at any wavelength contained a contribution from the photosensitizer triplet state decay, while at 1274nm the singlet oxygen phosphorescence dominated. The results obtained can be used for optimization of the methods of singlet oxygen monitoring and imaging.

Simulations of the temporal and spatial resolution for a compact time-resolved electron diffractometer

NASA Astrophysics Data System (ADS)

Robinson, Matthew S.; Lane, Paul D.; Wann, Derek A.

2016-02-01

A novel compact electron gun for use in time-resolved gas electron diffraction experiments has recently been designed and commissioned. In this paper we present and discuss the extensive simulations that were performed to underpin the design in terms of the spatial and temporal qualities of the pulsed electron beam created by the ionisation of a gold photocathode using a femtosecond laser. The response of the electron pulses to a solenoid lens used to focus the electron beam has also been studied. The simulated results show that focussing the electron beam affects the overall spatial and temporal resolution of the experiment in a variety of ways, and that factors that improve the resolution of one parameter can often have a negative effect on the other. A balance must, therefore, be achieved between spatial and temporal resolution. The optimal experimental time resolution for the apparatus is predicted to be 416 fs for studies of gas-phase species, while the predicted spatial resolution of better than 2 nm-1 compares well with traditional time-averaged electron diffraction set-ups.

Study on ultra-fast single photon counting spectrometer based on PCI

NASA Astrophysics Data System (ADS)

Zhang, Xi-feng

2010-10-01

The time-correlated single photon counting spectrometer developed uses PCI bus technology. We developed the ultrafast data acquisition card based on PCI, replace multi-channel analyzer primary. The system theory and design of the spectrometer are presented in detail, and the process of operation is introduced with the integration of the system. Many standard samples have been measured and the data have been analyzed and contrasted. Experimental results show that the spectrometer, s sensitive is single photon counting, and fluorescence life-span and time resolution is picosecond level. And the instrument could measure time-resolved spectroscopy.

Artifacts in time-resolved Kelvin probe force microscopy

DOE PAGES

Sadewasser, Sascha; Nicoara, Nicoleta; Solares, Santiago D.

2018-04-24

Kelvin probe force microscopy (KPFM) has been used for the characterization of metals, insulators, and semiconducting materials on the nanometer scale. Especially in semiconductors, the charge dynamics are of high interest. Recently, several techniques for time-resolved measurements with time resolution down to picoseconds have been developed, many times using a modulated excitation signal, e.g. light modulation or bias modulation that induces changes in the charge carrier distribution. For fast modulation frequencies, the KPFM controller measures an average surface potential, which contains information about the involved charge carrier dynamics. Here, we show that such measurements are prone to artifacts due tomore » frequency mixing, by performing numerical dynamics simulations of the cantilever oscillation in KPFM subjected to a bias-modulated signal. For square bias pulses, the resulting time-dependent electrostatic forces are very complex and result in intricate mixing of frequencies that may, in some cases, have a component at the detection frequency, leading to falsified KPFM measurements. Additionally, we performed fast Fourier transform (FFT) analyses that match the results of the numerical dynamics simulations. Small differences are observed that can be attributed to transients and higher-order Fourier components, as a consequence of the intricate nature of the cantilever driving forces. These results are corroborated by experimental measurements on a model system. In the experimental case, additional artifacts are observed due to constructive or destructive interference of the bias modulation with the cantilever oscillation. Also, in the case of light modulation, we demonstrate artifacts due to unwanted illumination of the photodetector of the beam deflection detection system. Lastly, guidelines for avoiding such artifacts are given.« less

Artifacts in time-resolved Kelvin probe force microscopy

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

Sadewasser, Sascha; Nicoara, Nicoleta; Solares, Santiago D.

Kelvin probe force microscopy (KPFM) has been used for the characterization of metals, insulators, and semiconducting materials on the nanometer scale. Especially in semiconductors, the charge dynamics are of high interest. Recently, several techniques for time-resolved measurements with time resolution down to picoseconds have been developed, many times using a modulated excitation signal, e.g. light modulation or bias modulation that induces changes in the charge carrier distribution. For fast modulation frequencies, the KPFM controller measures an average surface potential, which contains information about the involved charge carrier dynamics. Here, we show that such measurements are prone to artifacts due tomore » frequency mixing, by performing numerical dynamics simulations of the cantilever oscillation in KPFM subjected to a bias-modulated signal. For square bias pulses, the resulting time-dependent electrostatic forces are very complex and result in intricate mixing of frequencies that may, in some cases, have a component at the detection frequency, leading to falsified KPFM measurements. Additionally, we performed fast Fourier transform (FFT) analyses that match the results of the numerical dynamics simulations. Small differences are observed that can be attributed to transients and higher-order Fourier components, as a consequence of the intricate nature of the cantilever driving forces. These results are corroborated by experimental measurements on a model system. In the experimental case, additional artifacts are observed due to constructive or destructive interference of the bias modulation with the cantilever oscillation. Also, in the case of light modulation, we demonstrate artifacts due to unwanted illumination of the photodetector of the beam deflection detection system. Lastly, guidelines for avoiding such artifacts are given.« less

Darius Kuciauskas | NREL

Science.gov Websites

, low-temperature and time-resolved photoluminescence spectrometers, and a microscope for time-resolved Diploma Physics, Vilnius University Featured Publications Kuciauskas et al., "Time-resolved ;Dependence of the minority-carrier lifetime on the stoichiometry of CdTe using time-resolved

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

Shayduk, Roman; Vonk, Vedran; Strempfer, Jörg

We report on the quantitative determination of the transient surface temperature of Pt(110) upon nanosecond laser pulse heating. We find excellent agreement between heat transport theory and the experimentally determined transient surface temperature as obtained from time-resolved X-ray diffraction on timescales from hundred nanoseconds to milliseconds. Exact knowledge of the surface temperature's temporal evolution after laser excitation is crucial for future pump-probe experiments at synchrotron storage rings and X-ray free electron lasers.

Assessment of the pseudo-tracking approach for the calculation of material acceleration and pressure fields from time-resolved PIV: part II. Spatio-temporal filtering

NASA Astrophysics Data System (ADS)

van Gent, P. L.; Schrijer, F. F. J.; van Oudheusden, B. W.

2018-04-01

The present study characterises the spatio-temporal filtering associated with pseudo-tracking. A combined theoretical and numerical assessment is performed that uses the relatively simple flow case of a two-dimensional Taylor vortex as analytical test case. An additional experimental assessment considers the more complex flow of a low-speed axisymmetric base flow, for which time-resolved tomographic PIV measurements and microphone measurements were obtained. The results of these assessments show how filtering along Lagrangian tracks leads to amplitude modulation of flow structures. A cut-off track length and spatial resolution are specified to support future applications of the pseudo-tracking approach. The experimental results show a fair agreement between PIV and microphone pressure data in terms of fluctuation levels and pressure frequency spectra. The coherence and correlation between microphone and PIV pressure measurements were found to be substantial and almost independent of the track length, indicating that the low-frequency behaviour of the flow could be reproduced regardless of the track length. It is suggested that a spectral analysis can be used inform the selection of a suitable track length and to estimate the local error margin of reconstructed pressure values.

In situ distributed diagnostics of flowable electrode systems: resolving spatial and temporal limitations.

PubMed

Dennison, C R; Gogotsi, Y; Kumbur, E C

2014-09-14

In this study, we have developed an in situ distributed diagnostics tool to investigate spatial and temporal effects in electrochemical systems based on flowable electrodes. Specifically, an experimental approach was developed that enables spatially-resolved voltage measurements to be obtained in situ, in real-time. To extract additional data from these distributed measurements, an experimentally-parameterized equivalent circuit model with a new 'flow capacitor' circuit element was developed to predict the distributions of various system parameters during operation. As a case study, this approach was applied to investigate the behavior of the suspension electrodes used in an electrochemical flow capacitor under flowing and static conditions. The volumetric capacitance is reduced from 15.6 F ml(-1) to 1.1 F ml(-1) under flowing conditions. Results indicate that the majority of the charging in suspension electrodes occurs within ∼750 μm of the current collectors during flow, which gives rise to significant state-of-charge gradients across the cell, as well as underutilization of the available active material. The underlying cause of this observation is attributed to the relatively high electrical resistance of the slurry coupled with a stratified charging regime and insufficient residence time. The observations highlight the need to develop more conductive slurries and to design cells with reduced charge transport lengths.

Depth resolved lattice-charge coupling in epitaxial BiFeO3 thin film

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

Lee, Hyeon Jun; Lee, Sung Su; Kwak, Jeong Hun

2016-12-01

For epitaxial films, a critical thickness (t c) can create a phenomenological interface between a strained bottom layer and a relaxed top layer. Here, we present an experimental report of how the tc in BiFeO 3 thin films acts as a boundary to determine the crystalline phase, ferroelectricity, and piezoelectricity in 60 nm thick BiFeO 3/SrRuO 3/SrTiO 3 substrate. We found larger Fe cation displacement of the relaxed layer than that of strained layer. In the time-resolved X-ray microdiffraction analyses, the piezoelectric response of the BiFeO 3 film was resolved into a strained layer with an extremely low piezoelectric coefficientmore » of 2.4 pm/V and a relaxed layer with a piezoelectric coefficient of 32 pm/V. The difference in the Fe displacements between the strained and relaxed layers is in good agreement with the differences in the piezoelectric coefficient due to the electromechanical coupling.« less

Depth resolved lattice-charge coupling in epitaxial BiFeO3 thin film

PubMed Central

Lee, Hyeon Jun; Lee, Sung Su; Kwak, Jeong Hun; Kim, Young-Min; Jeong, Hu Young; Borisevich, Albina Y.; Lee, Su Yong; Noh, Do Young; Kwon, Owoong; Kim, Yunseok; Jo, Ji Young

2016-01-01

For epitaxial films, a critical thickness (tc) can create a phenomenological interface between a strained bottom layer and a relaxed top layer. Here, we present an experimental report of how the tc in BiFeO3 thin films acts as a boundary to determine the crystalline phase, ferroelectricity, and piezoelectricity in 60 nm thick BiFeO3/SrRuO3/SrTiO3 substrate. We found larger Fe cation displacement of the relaxed layer than that of strained layer. In the time-resolved X-ray microdiffraction analyses, the piezoelectric response of the BiFeO3 film was resolved into a strained layer with an extremely low piezoelectric coefficient of 2.4 pm/V and a relaxed layer with a piezoelectric coefficient of 32 pm/V. The difference in the Fe displacements between the strained and relaxed layers is in good agreement with the differences in the piezoelectric coefficient due to the electromechanical coupling. PMID:27929103

Time-resolved infrared and resonance Raman studies of benzil. Vibrational analysis and structures of the excited states

NASA Astrophysics Data System (ADS)

Mizuno, Misao; Iwata, Koichi; Takahashi, Hiroaki

2003-12-01

Structures of the S 1 and T 1 states of benzil are examined based on the experimental results from nanosecond time-resolved infrared spectroscopy and picosecond time-resolved Raman spectroscopy. Nanosecond time-resolved infrared spectra of the T 1 state of benzil as well as its three isotopically substituted analogues were measured in carbon tetrachloride. The observed infrared bands of T 1 benzil were assigned based on the frequency shifts on isotopic ( 18O, and deuteration) substitutions. The infrared band at 1312 cm -1 is assigned to the CO anti-symmetric stretch vibration. An infrared band that has large contribution from the central C-C stretch is not observed. Picosecond time-resolved resonance Raman spectra of the S 1 state of benzil were also measured. It has been reported that after the photoexcitation, the benzil molecule shows an ultrafast conformational change in the S 1 state. The observed resonance Raman bands are attributable to the vibrations of the relaxed form of the S 1 state. By comparing the Raman and infrared spectra of the S 0, S 1, and T 1 states of benzil, the structures of benzil in the excited states are discussed. Upon going from the S 0 state to the S 1 or T 1 state, the bond order of the CO bond decreases while that of the central C-C bond increases. Although several ground-state bands appear in both the infrared and Raman spectra, there is no band observed simultaneously in the infrared and Raman spectra of the T 1 state, except for bands attributable to the phenyl ring vibrations. We conclude that T 1 benzil has the inversion center that arises from the trans-planar structure. The spectral pattern of the resonance Raman scattering of the relaxed S 1 state is very similar to that of the T 1 state. This implies that the molecular structure of the relaxed S 1 state is similar to that of the T 1 state. The structure of the relaxed form of the S 1 state is also considered to be trans-planar.

Individuals with clinically significant insomnia symptoms are characterised by a negative sleep-related expectancy bias: Results from a cognitive-experimental assessment.

PubMed

Courtauld, Hannah; Notebaert, Lies; Milkins, Bronwyn; Kyle, Simon D; Clarke, Patrick J F

2017-08-01

Cognitive models of insomnia consistently suggest that negative expectations regarding the consequences of poor sleep contribute to the maintenance of insomnia. To date, however, no research has sought to determine whether insomnia is indeed characterised by such a negative sleep-related expectancy bias, using objective cognitive assessment tasks which are more immune to response biases than questionnaire assessments. Therefore, the current study employed a reaction-time task assessing biased expectations among a group with clinically significant insomnia symptoms (n = 30) and a low insomnia symptoms group (n = 40). The task involved the presentation of scenarios describing the consequences of poor sleep, and non-sleep related activities, which could be resolved in a benign or a negative manner. The results demonstrated that the high insomnia symptoms group were disproportionately fast to resolve sleep-related scenarios in line with negative outcomes, as compared to benign outcomes, relative to the low insomnia symptoms group. The two groups did not differ in their pattern of resolving non-sleep related scenarios. This pattern of findings is entirely consistent with a sleep-specific expectancy bias operating in individuals with clinically significant insomnia symptoms, and highlights the potential of cognitive-experimental assessment tasks to objectively index patterns of biased cognition in insomnia. Copyright © 2017 Elsevier Ltd. All rights reserved.

High pressure and time resolved studies of optical properties of n-type doped GaN/AlN multi-quantum wells: Experimental and theoretical analysis

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

Kaminska, A.; Cardinal Stefan Wyszynski University, College of Science, Department of Mathematics and Natural Sciences, Dewajtis 5, 01-815 Warsaw; Jankowski, D.

High-pressure and time-resolved studies of the optical emission from n-type doped GaN/AlN multi-quantum-wells (MQWs) with various well thicknesses are analysed in comparison with ab initio calculations of the electronic (band structure, density of states) and optical (emission energies and their pressure derivatives, oscillator strength) properties. The optical properties of GaN/AlN MQWs are strongly affected by quantum confinement and polarization-induced electric fields. Thus, the photoluminescence (PL) peak energy decreases by over 1 eV with quantum well (QW) thicknesses increasing from 1 to 6 nm. Furthermore, the respective PL decay times increased from about 1 ns up to 10 μs, due to the strong built-in electricmore » field. It was also shown that the band gap pressure coefficients are significantly reduced in MQWs as compared to bulk AlN and GaN crystals. Such coefficients are strongly dependent on the geometric factors such as the thickness of the wells and barriers. The transition energies, their oscillator strength, and pressure dependence are modeled for tetragonally strained structures of the same geometry using a full tensorial representation of the strain in the MQWs under external pressure. These MQWs were simulated directly using density functional theory calculations, taking into account two different systems: the semi-insulating QWs and the n-doped QWs with the same charge density as in the experimental samples. Such an approach allowed an assessment of the impact of n-type doping on optical properties of GaN/AlN MQWs. We find a good agreement between these two approaches and between theory and experimental results. We can therefore confirm that the nonlinear effects induced by the tetragonal strain related to the lattice mismatch between the substrates and the polar MQWs are responsible for the drastic decrease of the pressure coefficients observed experimentally.« less

Time-resolved fluorescence spectroscopy of human brain tumors

NASA Astrophysics Data System (ADS)

Marcu, Laura; Thompson, Reid C.; Garde, Smita; Sedrak, Mark; Black, Keith L.; Yong, William H.

2002-05-01

Fluorescence spectroscopy of the endogenous emission of brain tumors has been researched as a potentially important method for the intraoperative localization of brain tumor margins. In this study, we investigate the use of time-resolved laser-induced fluorescence spectroscopy (TR-LIFS) for demarcation of primary brain tumors by studying the time-resolved spectra of gliomas of different histologic grades. Time-resolved fluorescence (3 ns, 337 nm excitation) from excised human brain tumor show differences between the time-resolved emission of malignant glioma and normal brain tissue (gray and white matter). Our findings suggest that brain tumors can be differentiated from normal brain tissue based upon unique time-resolved fluorescence signature.

Temporal-resolved characterization of laser-induced plasma for spectrochemical analysis of gas shales

NASA Astrophysics Data System (ADS)

Xu, Tao; Zhang, Yong; Zhang, Ming; He, Yi; Yu, Qiaoling; Duan, Yixiang

2016-07-01

Optical emission of laser ablation plasma on a shale target surface provides sensitive laser-induced breakdown spectrometry (LIBS) detection of major, minor or trace elements. An exploratory study for the characterization of the plasma induced on shale materials was carried out with the aim to trigger a crucial step towards the quantitative LIBS measurement. In this work, the experimental strategies that optimize the plasma generation on a pressed shale pellet surface are presented. The temporal evolution properties of the plasma induced by ns Nd:YAG laser pulse at the fundamental wavelength in air were investigated using time-resolved space-integrated optical emission spectroscopy. The electron density as well as the temperatures of the plasma were diagnosed as functions of the decay time for the bulk plasma analysis. In particular, the values of time-resolved atomic and ionic temperatures of shale elements, such as Fe, Mg, Ca, and Ti, were extracted from the well-known Boltzmann or Saha-Boltzmann plot method. Further comparison of these temperatures validated the local thermodynamic equilibrium (LTE) within specific interval of the delay time. In addition, the temporal behaviors of the signal-to-noise ratio of shale elements, including Si, Al, Fe, Ca, Mg, Ba, Li, Ti, K, Na, Sr, V, Cr, and Ni, revealed the coincidence of their maximum values with LIBS LTE condition in the time frame, providing practical implications for an optimized LIBS detection of shale elements. Analytical performance of LIBS was further evaluated with the linear calibration procedure for the most concerned trace elements of Sr, V, Cr, and Ni present in different shales. Their limits of detection obtained are elementally dependent and can be lower than tens of parts per million with the present LIBS experimental configurations. However, the occurrence of saturation effect for the calibration curve is still observable with the increasing trace element content, indicating that, due to the complex composition of shale materials, the omnipresent "matrix effect" is still a great challenging for the performance of quantitative LIBS measurement even in the framework of the LTE approach.

From Supercomputer Modeling to Highest Mass Resolution in FT-ICR.

PubMed

N Nikolaev, Evgene; N Vladimirov, Gleb; Jertz, Roland; Baykut, Gökhan

2013-01-01

Understanding of behavior of ion ensembles inside FT-ICR cell based on the computer simulation of ion motion gives rise to the new ideas of cell designs. The recently introduced novel FT-ICR cell based on a Penning ion trap with specially shaped excitation and detection electrodes prevents distortion of ion cyclotron motion phases (normally caused by non-ideal electric trapping fields) by averaging the trapping DC electric field during the ion motion in the ICR cell. Detection times of 5 min resulting in resolving power close to 40,000,000 have been reached for reserpine at m/z 609 at a magnetic field of only 7 Tesla. Fine structures of resolved 13Cn isotopic cluster groups could be measured for molecular masses up to 5.7 kDa (insulin) with resolving power of 4,000,000 at 7 Tesla. Based on resolved fine structure patterns atomic compositions can be directly determined using a new developed algorithm for fine structure processing. Mass spectra of proteins and multimers of proteins reaching masses up to 186 kDa (enolase tetramer) could be measured with isotopic resolution. For instance, at 7 Tesla resolving power of 800,000 was achieved for enolase dimer (96 kDa) and 500,000 for molecular masses above 100 kDa. Experimental data indicate that there is practically no limit for the resolving power of this ICR cell except by collisional damping in the ultrahigh vacuum chamber.

Modelling Time-Resolved Two-Dimensional Electronic Spectroscopy of the Primary Photoisomerization Event in Rhodopsin

PubMed Central

2015-01-01

Time-resolved two-dimensional (2D) electronic spectra (ES) tracking the evolution of the excited state manifolds of the retinal chromophore have been simulated along the photoisomerization pathway in bovine rhodopsin, using a state-of-the-art hybrid QM/MM approach based on multiconfigurational methods. Simulations of broadband 2D spectra provide a useful picture of the overall detectable 2D signals from the near-infrared (NIR) to the near-ultraviolet (UV). Evolution of the stimulated emission (SE) and excited state absorption (ESA) 2D signals indicates that the S1 → SN (with N ≥ 2) ESAs feature a substantial blue-shift only after bond inversion and partial rotation along the cis → trans isomerization angle, while the SE rapidly red-shifts during the photoinduced skeletal relaxation of the polyene chain. Different combinations of pulse frequencies are proposed in order to follow the evolution of specific ESA signals. These include a two-color 2DVis/NIR setup especially suited for tracking the evolution of the S1 → S2 transitions that can be used to discriminate between different photochemical mechanisms of retinal photoisomerization as a function of the environment. The reported results are consistent with the available time-resolved pump–probe experimental data, and may be used for the design of more elaborate transient 2D electronic spectroscopy techniques. PMID:24794143

Nonradiative inter- and intramolecular energy transfer from the aromatic donor anisole to a synthesized photoswitchable acceptor system.

PubMed

Bardhan, Munmun; Bhattacharya, Sudeshna; Misra, Tapas; Mukhopadhyay, Rupa; De, Asish; Chowdhury, Joydeep; Ganguly, Tapan

2010-02-01

We report steady state and time resolved fluorescence measurements on acetonitrile (ACN) solutions of the model compounds, energy donor anisole (A) and a photoswitchable acceptor N,N'-1,2-phenylene di-p-tosylamide (B) and the multichromophore (M) where A and B are connected by a spacer containing both rigid triple (acetylenic) and flexible methylene bonds. Both steady state and time correlated single photon counting measurements demonstrate that though intermolecular energy transfer, of Forster type, between the donor and acceptor moieties occurs with rate 10(8)s(-1) but when these two reacting components are linked by a spacer (multichromophore, M) the observed transfer rate ( approximately 10(11)s(-1)) enhances. This seemingly indicates that the imposition of the spacer by inserting a triple bond may facilitate in the propagation of electronic excitation energy through bond. The time resolved fluorescence measurements along with the theoretical predictions using Configuration interaction singles (CIS) method by using 6-31G (d,p) basis set, implemented in the Gaussian package indicate the formations of the two excited conformers of B. The experimental findings made from the steady state and time resolved fluorescence measurements demonstrate that, though two different isomeric species of the acceptor B are formed in the excited singlet states, the prevailing singlet-singlet nonradiative energy transfer route was found from the donor A to the relatively longer-lived isomeric species of B. Copyright (c) 2009 Elsevier B.V. All rights reserved.

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

PubMed

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

2014-07-28

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

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

NASA Astrophysics Data System (ADS)

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.

Spatially and momentum resolved energy electron loss spectra from an ultra-thin PrNiO{sub 3} layer

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

Kinyanjui, M. K., E-mail: michael.kinyanjui@uni-ulm.de; Kaiser, U.; Benner, G.

2015-05-18

We present an experimental approach which allows for the acquisition of spectra from ultra-thin films at high spatial, momentum, and energy resolutions. Spatially and momentum (q) resolved electron energy loss spectra have been obtained from a 12 nm ultra-thin PrNiO{sub 3} layer using a nano-beam electron diffraction based approach which enabled the acquisition of momentum resolved spectra from individual, differently oriented nano-domains and at different positions of the PrNiO{sub 3} thin layer. The spatial and wavelength dependence of the spectral excitations are obtained and characterized after the analysis of the experimental spectra using calculated dielectric and energy loss functions. The presentedmore » approach makes a contribution towards obtaining momentum-resolved spectra from nanostructures, thin film, heterostructures, surfaces, and interfaces.« less

Pulse retrieval algorithm for interferometric frequency-resolved optical gating based on differential evolution.

PubMed

Hyyti, Janne; Escoto, Esmerando; Steinmeyer, Günter

2017-10-01

A novel algorithm for the ultrashort laser pulse characterization method of interferometric frequency-resolved optical gating (iFROG) is presented. Based on a genetic method, namely, differential evolution, the algorithm can exploit all available information of an iFROG measurement to retrieve the complex electric field of a pulse. The retrieval is subjected to a series of numerical tests to prove the robustness of the algorithm against experimental artifacts and noise. These tests show that the integrated error-correction mechanisms of the iFROG method can be successfully used to remove the effect from timing errors and spectrally varying efficiency in the detection. Moreover, the accuracy and noise resilience of the new algorithm are shown to outperform retrieval based on the generalized projections algorithm, which is widely used as the standard method in FROG retrieval. The differential evolution algorithm is further validated with experimental data, measured with unamplified three-cycle pulses from a mode-locked Ti:sapphire laser. Additionally introducing group delay dispersion in the beam path, the retrieval results show excellent agreement with independent measurements with a commercial pulse measurement device based on spectral phase interferometry for direct electric-field retrieval. Further experimental tests with strongly attenuated pulses indicate resilience of differential-evolution-based retrieval against massive measurement noise.

Practical issues in ultrashort-laser-pulse measurement using frequency-resolved optical gating

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

DeLong, K.W.; Fittinghoff, D.N.; Trebino, R.

1996-07-01

The authors explore several practical experimental issues in measuring ultrashort laser pulses using the technique of frequency-resolved optical gating (FROG). They present a simple method for checking the consistency of experimentally measured FROG data with the independently measured spectrum and autocorrelation of the pulse. This method is a powerful way of discovering systematic errors in FROG experiments. They show how to determine the optimum sampling rate for FROG and show that this satisfies the Nyquist criterion for the laser pulse. They explore the low- and high-power limits to FROG and determine that femtojoule operation should be possible, while the effectsmore » of self-phase modulation limit the highest signal efficiency in FROG to 1%. They also show quantitatively that the temporal blurring due to a finite-thickness medium in single-shot geometries does not strongly limit the FROG technique. They explore the limiting time-bandwidth values that can be represented on a FROG trace of a given size. Finally, they report on a new measure of the FROG error that improves convergence in the presence of noise.« less

Resolving the detailed structure of cortical and thalamic neurons in the adult rat brain with refined biotinylated dextran amine labeling.

PubMed

Ling, Changying; Hendrickson, Michael L; Kalil, Ronald E

2012-01-01

Biotinylated dextran amine (BDA) has been used frequently for both anterograde and retrograde pathway tracing in the central nervous system. Typically, BDA labels axons and cell somas in sufficient detail to identify their topographical location accurately. However, BDA labeling often has proved to be inadequate to resolve the fine structural details of axon arbors or the dendrites of neurons at a distance from the site of BDA injection. To overcome this limitation, we varied several experimental parameters associated with the BDA labeling of neurons in the adult rat brain in order to improve the sensitivity of the method. Specifically, we compared the effect on labeling sensitivity of: (a) using 3,000 or 10,000 MW BDA; (b) injecting different volumes of BDA; (c) co-injecting BDA with NMDA; and (d) employing various post-injection survival times. Following the extracellular injection of BDA into the visual cortex, labeled cells and axons were observed in both cortical and thalamic areas of all animals studied. However, the detailed morphology of axon arbors and distal dendrites was evident only under optimal conditions for BDA labeling that take into account the: molecular weight of the BDA used, concentration and volume of BDA injected, post-injection survival time, and toning of the resolved BDA with gold and silver. In these instances, anterogradely labeled axons and retrogradely labeled dendrites were resolved in fine detail, approximating that which can be achieved with intracellularly injected compounds such as biocytin or fluorescent dyes.

Comparison of femtosecond laser ablation of aluminum in water and in air by time-resolved optical diagnosis.

PubMed

Hu, Haofeng; Liu, Tiegen; Zhai, Hongchen

2015-01-26

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

- and Frequency-Domain Signatures of Velocity Changing Collisions in Sub-Doppler Saturation Spectra and Pressure Broadening

NASA Astrophysics Data System (ADS)

Hall, Gregory; Xu, Hong; Forthomme, Damien; Dagdigian, Paul; Sears, Trevor

2017-06-01

We have combined experimental and theoretical approaches to the competition between elastic and inelastic collisions of CN radicals with Ar, and how this competition influences time-resolved saturation spectra. Experimentally, we have measured transient, two-color sub-Doppler saturation spectra of CN radicals with an amplitude chopped saturation laser tuned to selected Doppler offsets within rotational lines of the A-X (2-0) band, while scanning a frequency modulated probe laser across the hyperfine-resolved saturation features of corresponding rotational lines of the A-X (1-0) band. A steady-state depletion spectrum includes off-resonant contributions ascribed to velocity diffusion, and the saturation recovery rates depend on the sub-Doppler detuning. The experimental results are compared with Monte Carlo solutions to the Boltzmann equation for the collisional evolution of the velocity distributions of CN radicals, combined with a pressure-dependent and speed-dependent lifetime broadening. Velocity changing collisions are included by appropriately sampling the energy resolved differential cross sections for elastic scattering of selected rotational states of CN (X). The velocity space diffusion of Doppler tagged molecules proceeds through a series of small-angle scattering events, eventually terminating in an inelastic collision that removes the molecule from the coherently driven ensemble of interest. Collision energy-dependent total cross sections and differential cross sections for elastic scattering of selected CN rotational states with Ar were computed with Hibridon quantum scattering calculations, and used for sampling in the Monte Carlo modeling. Acknowledgments: Work at Brookhaven National Laboratory was carried out under Contract No. DE-SC0012704 with the U.S. Department of Energy, Office of Science, and supported by its Division of Chemical Sciences, Geosciences and Biosciences within the Office of Basic Energy Sciences.

Flow temporal reconstruction from non-time-resolved data part I: mathematic fundamentals

NASA Astrophysics Data System (ADS)

Legrand, Mathieu; Nogueira, José; Lecuona, Antonio

2011-10-01

At least two circumstances point to the need of postprocessing techniques to recover lost time information from non-time-resolved data: the increasing interest in identifying and tracking coherent structures in flows of industrial interest and the high data throughput of global measuring techniques, such as PIV, for the validation of computational fluid dynamics (CFD) codes. This paper offers the mathematic fundamentals of a space--time reconstruction technique from non-time-resolved, statistically independent data. An algorithm has been developed to identify and track traveling coherent structures in periodic flows. Phase-averaged flow fields are reconstructed with a correlation-based method, which uses information from the Proper Orthogonal Decomposition (POD). The theoretical background shows that the snapshot POD coefficients can be used to recover flow phase information. Once this information is recovered, the real snapshots are used to reconstruct the flow history and characteristics, avoiding neither the use of POD modes nor any associated artifact. The proposed time reconstruction algorithm is in agreement with the experimental evidence given by the practical implementation proposed in the second part of this work (Legrand et al. in Exp Fluids, 2011), using the coefficients corresponding to the first three POD modes. It also agrees with the results on similar issues by other authors (Ben Chiekh et al. in 9 Congrès Francophone de Vélocimétrie Laser, Bruxelles, Belgium, 2004; Van Oudheusden et al. in Exp Fluids 39-1:86-98, 2005; Meyer et al. in 7th International Symposium on Particle Image Velocimetry, Rome, Italy, 2007a; in J Fluid Mech 583:199-227, 2007b; Perrin et al. in Exp Fluids 43-2:341-355, 2007). Computer time to perform the reconstruction is relatively short, of the order of minutes with current PC technology.

Impact of clocking on the aero-thermodynamics of a second stator tested in a one and a half stage HP turbine

NASA Astrophysics Data System (ADS)

Billiard, N.; Paniagua, Guillermo; Dénos, R.

2008-06-01

This paper focuses on the experimental investigation of the time-averaged and time-accurate aero-thermodynamics of a second stator tested in a 1.5 stage high-pressure turbine. The effect of clocking on aerodynamic and heat transfer are investigated. Tests are performed under engine representative conditions in the VKI compression tube CT3. The test program includes four different clocking positions, i.e. relative pitch-wise positions between the first and the second stator. Probes located upstream and downstream of the second stator provide the thermodynamic conditions of the flow field. On the second stator airfoil, measurements are taken around the blade profile at 15, 50 and 85% span with pressure sensors and thin-film gauges. Both time-averaged and time-resolved aspects of the flow field are addressed. Regarding the time-averaged results, clocking effects are mainly observed within the leading edge region of the second stator, the largest effects being observed at 15% span. The surface static pressure distribution is changed locally, hence affecting the overall airfoil performance. For one clocking position, the thermal load of the airfoil is noticeably reduced. Pressure fluctuations are attributed to the passage of the upstream transonic rotor and its associated pressure gradients. The pattern of these fluctuations changes noticeably as a function of clocking. The time-resolved variations of heat flux and static pressure are analyzed together showing that the major effect is due to a potential interaction. The time-resolved pressure distribution integrated along the second stator surface yields the unsteady forces on the vane. The magnitude of the unsteady force is very dependent on the clocking position.

Femtosecond characterization of vibrational optical activity of chiral molecules.

PubMed

Rhee, Hanju; June, Young-Gun; Lee, Jang-Soo; Lee, Kyung-Koo; Ha, Jeong-Hyon; Kim, Zee Hwan; Jeon, Seung-Joon; Cho, Minhaeng

2009-03-19

Optical activity is the result of chiral molecules interacting differently with left versus right circularly polarized light. Because of this intrinsic link to molecular structure, the determination of optical activity through circular dichroism (CD) spectroscopy has long served as a routine method for obtaining structural information about chemical and biological systems in condensed phases. A recent development is time-resolved CD spectroscopy, which can in principle map the structural changes associated with biomolecular function and thus lead to mechanistic insights into fundamental biological processes. But implementing time-resolved CD measurements is experimentally challenging because CD is a notoriously weak effect (a factor of 10(-4)-10(-6) smaller than absorption). In fact, this problem has so far prevented time-resolved vibrational CD experiments. Here we show that vibrational CD spectroscopy with femtosecond time resolution can be realized when using heterodyned spectral interferometry to detect the phase and amplitude of the infrared optical activity free-induction-decay field in time (much like in a pulsed NMR experiment). We show that we can detect extremely weak signals in the presence of large achiral background contributions, by simultaneously measuring with a femtosecond laser pulse the vibrational CD and optical rotatory dispersion spectra of dissolved chiral limonene molecules. We have so far only targeted molecules in equilibrium, but it would be straightforward to extend the method for the observation of ultrafast structural changes such as those occurring during protein folding or asymmetric chemical reactions. That is, we should now be in a position to produce 'molecular motion pictures' of fundamental molecular processes from a chiral perspective.

Observation of ionization fronts in low density foam targets

NASA Astrophysics Data System (ADS)

Hoarty, D.; Willi, O.; Barringer, L.; Vickers, C.; Watt, R.; Nazarov, W.

1999-05-01

Ionization fronts have been observed in low density chlorinated foam targets and low density foams confined in gold tubes using time resolved K-shell absorption spectroscopy. The front was driven by an intense pulse of soft x-rays produced by high power laser irradiation. The density and temperature profiles inferred from the radiographs provided detailed measurement of the conditions. The experimental data were compared to radiation hydrodynamics simulations and reasonable agreement was obtained.

Experimental Investigation of the Interaction of Electrothermal Plasmas with Solid Propellants

DTIC Science & Technology

2007-09-14

formation increases propellant burning rate (Koleczko, et al . 2001). The experiments described here were designed to create time and spatially resolved...Pesce-Rodriguez 2004, Koleczko, et al . 2001). Most tests involving plasma propellant interactions involve higher plasma energies than the 3.1 kJ of...product that scatters light. The large jump in pressurization seen in closed bomb plasma ignition tests (Lieb, et al . 2001) during the plasma discharge

Determination of the spin orbit coupling and crystal field splitting in wurtzite InP by polarization resolved photoluminescence

NASA Astrophysics Data System (ADS)

Chauvin, Nicolas; Mavel, Amaury; Jaffal, Ali; Patriarche, Gilles; Gendry, Michel

2018-02-01

Excitation photoluminescence spectroscopy is usually used to extract the crystal field splitting (ΔCR) and spin orbit coupling (ΔSO) parameters of wurtzite (Wz) InP nanowires (NWs). However, the equations expressing the valence band splitting are symmetric with respect to these two parameters, and a choice ΔCR > ΔSO or ΔCR < ΔSO has to be taken into account in order to assign the numerical values. To solve this issue, polarization resolved micro-photoluminescence was performed on vertically aligned and untapered Wz InP NWs grown on silicon. The experimental results combined with a theoretical model and finite difference time domain calculations allow us to conclude that ΔCR > ΔSO in Wz InP.

Ultrafast Physics Behind the Nonradiative Relaxation Process of Chromium Ions in Forsterite Crystals.

NASA Astrophysics Data System (ADS)

Demos, Stavros Gregorios

The nonradiative relaxation following photoexcitation has been studied in Cr^{4+} -doped forsterite (Mg_2SiO _4) using picosecond laser excitation and ultrasensitive photon counting detection. The experimental techniques utilized were time resolved antiStokes Raman scattering and up-converted hot and ordinary luminescence. The up-converted hot luminescence technique allowed the investigation of the upper state nonradiative relaxation of the excited state manifold of Cr^{4+ }-doped forsterite. The excitation involves the absorption of two photons per photoexcited ion in a two-step absorption. Discrete peaks are observed in the hot up-converted luminescence spectrum and are attributed to the population of nonequilibrium vibronic levels during the deexcitation of the ions by phonon emission. This work reveals that the phonon modes participating in the initial steps of the nonradiative relaxation of the photoexcited ions have energies 218 +/- 20, 325 +/- 20, 365 +/- 20 and 513 +/- 12 cm^ {-1}. The shape of the luminescence spectral envelope suggests two electronic bottlenecks at ~2.1 and ~2.45 eV associated with slower rates of vibrational relaxation at different parts of the excited state manifold. Time resolved measurements indicated that the average time for phonon emission is of the order of hundreds of fs. Information on the nonequilibrium phonon dynamics of the 225, 335 and 370 cm^{-1} modes of forsterite has been obtained using time resolved Raman scattering. Laser pulses of 450 fs in duration and 590 nm in wavelength were used to excite the Cr ions 2.1 eV above the ground state. The probe pulses (obtained from the same laser) are monitoring the nonequilibrium phonon population through the intensity of the antiStokes Raman lines at various pump-probe delay times. Experiments were performed at room and liquid nitrogen temperatures. The observed nonequilibrium phonon populations are associated with the overall complex nonradiative decay following the excitation of the impurity Cr^{4+} ions. Using rate equations to describe the electron -lattice system, the nonradiative relaxation time and the phonon lifetimes were estimated by fitting to the experimental data. The nonradiative relaxation time is estimated to be in the order of few ps while the phonon lifetimes are of the order of 10 ps. Best fit suggests the presence of an electronic bottleneck immediately after photoexcitation with an estimated lifetime of 3 ps at room temperature.

Remote sensing of methane with OSAS-lidar on the 2ν3 band Q-branch: Experimental proof

NASA Astrophysics Data System (ADS)

Galtier, Sandrine; Anselmo, Christophe; Welschinger, Jean-Yves; Sivignon, J. F.; Cariou, Jean-Pierre; Miffre, Alain; Rairoux, Patrick

2018-06-01

Optical sensors based on absorption spectroscopy play a central role in the detection and monitoring of atmospheric trace gases. We here present for the first time the experimental demonstration of OSAS-Lidar on the remote sensing of CH4 in the atmosphere. This new methodology, the OSAS-Lidar, couples the Optical Similitude Absorption Spectroscopy (OSAS) methodology with a light detection and ranging device. It is based on the differential absorption of spectrally integrated signals following Beer Lambert-Bouguer law, which are range-resolved. Its novelty originates from the use of broadband laser spectroscopy and from the mathematical approach used to retrieve the trace gas concentration. We previously applied the OSAS methodology in laboratory on the 2ν3 methane absorption band, centered at the 1665 nm wavelength and demonstrated that the OSAS-methodology is almost independent from atmospheric temperature and pressure. In this paper, we achieve an OSAS-Lidar device capable of observing large concentrations of CH4 released from a methane source directly into the atmosphere. Comparison with a standard in-situ measurement device shows that the path-integrated concentrations retrieved from OSAS-Lidar methodology exhibit sufficient sensitivity (2 000 ppm m) and observational time resolution (1 s) to remotely sense methane leaks in the atmosphere. The coupling of OSAS-lidar with a wind measurement device opens the way to monitor time-resolved methane flux emissions, which is important in regards to future climate mitigation involving regional reduction of CH4 flux emissions.

Dielectric barrier discharge-based plasma actuator operation in artificial atmospheres for validation of modeling and simulation

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

Mangina, R. S.; Enloe, C. L.; Font, G. I.

2015-11-15

We present an experimental case study of time-resolved force production by an aerodynamic plasma actuator immersed in various mixtures of electropositive (N{sub 2}) and electronegative gases (O{sub 2} and SF{sub 6}) at atmospheric pressure using a fixed AC high-voltage input of 16 kV peak amplitude at 200 Hz frequency. We have observed distinct changes in the discharge structures during both negative- and positive-going voltage half-cycles, with corresponding variations in the actuator's force production: a ratio of 4:1 in the impulse produced by the negative-going half-cycle of the discharge among the various gas mixtures we explored, 2:1 in the impulse produced by themore » positive-going half-cycle, and cases in which the negative-going half-cycle dominates force production (by a ratio of 1.5:1), where the half-cycles produce identical force levels, and where the positive-going half cycle dominates (by a ratio of 1:5). We also present time-resolved experimental evidence for the first time that shows electrons do play a significant role in the momentum coupling to surrounding neutrals during the negative going voltage half-cycle of the N{sub 2} discharge. We show that there is sufficient macroscopic variation in the plasma that the predictions of numerical models at the microscopic level can be validated even though the plasma itself cannot be measured directly on those spatial and temporal scales.« less

Preliminary investigation of flow dynamics during the start-up of a bulb turbine model

NASA Astrophysics Data System (ADS)

Coulaud, M.; Fraser, R.; Lemay, J.; Duquesne, P.; Aeschlimann, V.; Deschênes, C.

2016-11-01

Nowadays, the electricity network undergoes more perturbations due to the market demand. Additionally, an increase of the production from alternative resources such as wind or solar also induces important variations on the grid. Hydraulic power plants are used to respond quickly to these variations to stabilize the network. Hydraulic turbines have to face more frequent start-up and stop sequences that might shorten significantly their life time. In this context, an experimental analysis of start-up sequences has been conducted on the bulb turbine model of the BulbT project at the Hydraulic Machines Laboratory (LAMH) of Laval University. Maintaining a constant head, guide vanes are opened from 0 ° to 30 °. Three guide vanes opening speed have been chosen from 5 °/s to 20 °/s. Several repetitions were done for each guide vanes opening speed. During these sequences, synchronous time resolved measurements have been performed. Pressure signals were recorded at the runner inlet and outlet and along the draft tube. Also, 25 pressure measurements and strain measurements were obtained on the runner blades. Time resolved particle image velocimetry were used to evaluate flowrate during start-up for some repetitions. Torque fluctuations at shaft were also monitored. This paper presents the experimental set-up and start-up conditions chosen to simulate a prototype start-up. Transient flowrate methodology is explained and validation measurements are detailed. The preliminary results of global performances and runner pressure measurements are presented.

Time-resolved non-sequential ray-tracing modelling of non-line-of-sight picosecond pulse LIDAR

NASA Astrophysics Data System (ADS)

Sroka, Adam; Chan, Susan; Warburton, Ryan; Gariepy, Genevieve; Henderson, Robert; Leach, Jonathan; Faccio, Daniele; Lee, Stephen T.

2016-05-01

The ability to detect motion and to track a moving object that is hidden around a corner or behind a wall provides a crucial advantage when physically going around the obstacle is impossible or dangerous. One recently demonstrated approach to achieving this goal makes use of non-line-of-sight picosecond pulse laser ranging. This approach has recently become interesting due to the availability of single-photon avalanche diode (SPAD) receivers with picosecond time resolution. We present a time-resolved non-sequential ray-tracing model and its application to indirect line-of-sight detection of moving targets. The model makes use of the Zemax optical design programme's capabilities in stray light analysis where it traces large numbers of rays through multiple random scattering events in a 3D non-sequential environment. Our model then reconstructs the generated multi-segment ray paths and adds temporal analysis. Validation of this model against experimental results is shown. We then exercise the model to explore the limits placed on system design by available laser sources and detectors. In particular we detail the requirements on the laser's pulse energy, duration and repetition rate, and on the receiver's temporal response and sensitivity. These are discussed in terms of the resulting implications for achievable range, resolution and measurement time while retaining eye-safety with this technique. Finally, the model is used to examine potential extensions to the experimental system that may allow for increased localisation of the position of the detected moving object, such as the inclusion of multiple detectors and/or multiple emitters.

Femtosecond time-resolved MeV electron diffraction

DOE PAGES

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

2015-06-02

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

Time-Resolved Small-Angle X-ray Scattering Reveals Millisecond Transitions of a DNA Origami Switch.

PubMed

Bruetzel, Linda K; Walker, Philipp U; Gerling, Thomas; Dietz, Hendrik; Lipfert, Jan

2018-04-11

Self-assembled DNA structures enable creation of specific shapes at the nanometer-micrometer scale with molecular resolution. The construction of functional DNA assemblies will likely require dynamic structures that can undergo controllable conformational changes. DNA devices based on shape complementary stacking interactions have been demonstrated to undergo reversible conformational changes triggered by changes in ionic environment or temperature. An experimentally unexplored aspect is how quickly conformational transitions of large synthetic DNA origami structures can actually occur. Here, we use time-resolved small-angle X-ray scattering to monitor large-scale conformational transitions of a two-state DNA origami switch in free solution. We show that the DNA device switches from its open to its closed conformation upon addition of MgCl 2 in milliseconds, which is close to the theoretical diffusive speed limit. In contrast, measurements of the dimerization of DNA origami bricks reveal much slower and concentration-dependent assembly kinetics. DNA brick dimerization occurs on a time scale of minutes to hours suggesting that the kinetics depend on local concentration and molecular alignment.

DCS - A high flux beamline for time resolved dynamic compression science – Design highlights

DOE PAGES

Capatina, D.; D’Amico, K.; Nudell, J.; ...

2016-07-27

The Dynamic Compression Sector (DCS) beamline, a national user facility for time resolved dynamic compression science supported by the National Nuclear Security Administration (NNSA) of the Department of Energy (DOE), has recently completed construction and is being commissioned at Sector 35 of the Advanced Photon Source (APS) at Argonne National Laboratory (ANL). The beamline consists of a First Optics Enclosure (FOE) and four experimental enclosures. A Kirkpatrick–Baez focusing mirror system with 2.2 mrad incident angles in the FOE delivers pink beam to the experimental stations. A refocusing Kirkpatrick–Baez mirror system is situated in each of the two most downstream enclosures.more » Experiments can be conducted in either white, monochromatic, pink or monochromatic-reflected beam mode in any of the experimental stations by changing the position of two interlocked components in the FOE. The beamline Radiation Safety System (RSS) components have been designed to handle the continuous beam provided by two in-line revolver undulators with periods of 27 and 30 mm, at closed gap, 150 mA beam current, and passing through a power limiting aperture of 1.5 x 1.0 mm 2. A novel pink beam end station stop [1] is used to stop the continuous and focused pink beam which can achieve a peak heat flux of 105 kW/mm 2. Finally, a new millisecond shutter design [2] is used to deliver a quick pulse of beam to the sample, synchronized with the dynamic event, the microsecond shutter, and the storage ring clock.« less

DCS - A high flux beamline for time resolved dynamic compression science – Design highlights

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

Capatina, D., E-mail: capatina@aps.anl.gov; D’Amico, K., E-mail: kdamico@aps.anl.gov; Nudell, J., E-mail: jnudell@aps.anl.gov

2016-07-27

The Dynamic Compression Sector (DCS) beamline, a national user facility for time resolved dynamic compression science supported by the National Nuclear Security Administration (NNSA) of the Department of Energy (DOE), has recently completed construction and is being commissioned at Sector 35 of the Advanced Photon Source (APS) at Argonne National Laboratory (ANL). The beamline consists of a First Optics Enclosure (FOE) and four experimental enclosures. A Kirkpatrick–Baez focusing mirror system with 2.2 mrad incident angles in the FOE delivers pink beam to the experimental stations. A refocusing Kirkpatrick–Baez mirror system is situated in each of the two most downstream enclosures.more » Experiments can be conducted in either white, monochromatic, pink or monochromatic-reflected beam mode in any of the experimental stations by changing the position of two interlocked components in the FOE. The beamline Radiation Safety System (RSS) components have been designed to handle the continuous beam provided by two in-line revolver undulators with periods of 27 and 30 mm, at closed gap, 150 mA beam current, and passing through a power limiting aperture of 1.5 x 1.0 mm{sup 2}. A novel pink beam end station stop [1] is used to stop the continuous and focused pink beam which can achieve a peak heat flux of 105 kW/mm{sup 2}. A new millisecond shutter design [2] is used to deliver a quick pulse of beam to the sample, synchronized with the dynamic event, the microsecond shutter, and the storage ring clock.« less

DCS - A High Flux Beamline for Time Resolved Dynamic Compression Science – Design Highlights

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

Capatina, D.; D'Amico, Kevin L.; Nudell, J.

2016-07-27

The Dynamic Compression Sector (DCS) beamline, a national user facility for time resolved dynamic compression science supported by the National Nuclear Security Administration (NNSA) of the Department of Energy (DOE), has recently completed construction and is being commissioned at Sector 35 of the Advanced Photon Source (APS) at Argonne National Laboratory (ANL). The beamline consists of a First Optics Enclosure (FOE) and four experimental enclosures. A Kirkpatrick–Baez focusing mirror system with 2.2 mrad incident angles in the FOE delivers pink beam to the experimental stations. A refocusing Kirkpatrick–Baez mirror system is situated in each of the two most downstream enclosures.more » Experiments can be conducted in either white, monochromatic, pink or monochromatic-reflected beam mode in any of the experimental stations by changing the position of two interlocked components in the FOE. The beamline Radiation Safety System (RSS) components have been designed to handle the continuous beam provided by two in-line revolver undulators with periods of 27 and 30 mm, at closed gap, 150 mA beam current, and passing through a power limiting aperture of 1.5 x 1.0 mm2. A novel pink beam end station stop [1] is used to stop the continuous and focused pink beam which can achieve a peak heat flux of 105 kW/mm2. A new millisecond shutter design [2] is used to deliver a quick pulse of beam to the sample, synchronized with the dynamic event, the microsecond shutter, and the storage ring clock.« less

Electron Correlation in the Ionization Continuum of Molecules: Photoionization of N2 in the Vicinity of the Hopfield Series of Autoionizing States.

PubMed

Klinker, Markus; Marante, Carlos; Argenti, Luca; González-Vázquez, Jesús; Martín, Fernando

2018-02-15

Direct measurement of autoionization lifetimes by using time-resolved experimental techniques is a promising approach when energy-resolved spectroscopic methods do not work. Attosecond time-resolved experiments have recently provided the first quantitative determination of autoionization lifetimes of the lowest members of the well-known Hopfield series of resonances in N 2 . In this work, we have used the recently developed XCHEM approach to study photoionization of the N 2 molecule in the vicinity of these resonances. The XCHEM approach allows us to describe electron correlation in the molecular electronic continuum at a level similar to that provided by multireference configuration interaction methods in bound state calculations, a necessary condition to accurately describe autoionization, shakeup, and interchannel couplings occurring in this range of photon energies. Our results show that electron correlation leading to interchannel mixing is the main factor that determines the magnitude and shape of the N 2 photoionization cross sections, as well as the lifetimes of the Hopfield resonances. At variance with recent speculations, nonadiabatic effects do not seem to play a significant role. These conclusions are supported by the very good agreement between the calculated cross sections and those determined in synchrotron radiation and attosecond experiments.

Simultaneous temporally resolved DPIV and pressure measurements of symmetric oscillations in a scaled-up vocal fold model

NASA Astrophysics Data System (ADS)

Ringenberg, Hunter; Rogers, Dylan; Wei, Nathaniel; Krane, Michael; Wei, Timothy

2017-11-01

The objective of this study is to apply experimental data to theoretical framework of Krane (2013) in which the principal aeroacoustic source is expressed in terms of vocal fold drag, glottal jet dynamic head, and glottal exit volume flow, reconciling formal theoretical aeroacoustic descriptions of phonation with more traditional lumped-element descriptions. These quantities appear in the integral equations of motion for phonatory flow. In this way time resolved velocity field measurements can be used to compute time-resolved estimates of the relevant terms in the integral equations of motion, including phonation aeroacoustic source strength. A simplified 10x scale vocal fold model from Krane, et al. (2007) was used to examine symmetric, i.e. `healthy', oscillatory motion of the vocal folds. By using water as the working fluid, very high spatial and temporal resolution was achieved. Temporal variation of transglottal pressure was simultaneously measured with flow on the vocal fold model mid-height. Experiments were dynamically scaled to examine a range of frequencies corresponding to male and female voice. The simultaneity of the pressure and flow provides new insights into the aeroacoustics associated with vocal fold oscillations. Supported by NIH Grant No. 2R01 DC005642-11.

Experimental research on time-resolved evolution of cathode plasma expansion velocity in a long pulsed magnetically insulated coaxial diode

NASA Astrophysics Data System (ADS)

Zhu, Danni; Zhang, Jun; Zhong, Huihuang; Ge, Xingjun; Gao, Jingming

2018-02-01

Unlike planar diodes, separate research of the axial and radial plasma expansion velocities is difficult for magnetically insulated coaxial diodes. Time-resolved electrical diagnostic which is based on the voltage-ampere characteristics has been employed to study the temporal evolution of the axial and radial cathode plasma expansion velocities in a long pulsed magnetically insulated coaxial diode. Different from a planar diode with a "U" shaped profile of temporal velocity evolution, the temporal evolution trend of the axial expansion velocity is proved to be a "V" shaped profile. Apart from the suppression on the radial expansion velocity, the strong magnetic field is also conducive to slowing down the axial expansion velocity. Compared with the ordinary graphite cathode, the carbon velvet and graphite composite cathode showed superior characteristics as judged by the low plasma expansion velocity and long-term electrical stability as a promising result for applications where long-pulsed and reliable operation at high power is required.

Vibrationally resolved photoelectron spectra of lower diamondoids: A time-dependent approach

NASA Astrophysics Data System (ADS)

Xiong, Tao; Włodarczyk, Radosław; Gallandi, Lukas; Körzdörfer, Thomas; Saalfrank, Peter

2018-01-01

Vibrationally resolved lowest-energy bands of the photoelectron spectra (PES) of adamantane, diamantane, and urotropine were simulated by a time-dependent correlation function approach within the harmonic approximation. Geometries and normal modes for neutral and cationic molecules were obtained from B3LYP hybrid density functional theory (DFT). It is shown that the simulated spectra reproduce the experimentally observed vibrational finestructure (or its absence) quite well. Origins of the finestructure are discussed and related to recurrences of autocorrelation functions and dominant vibrations. Remaining quantitative and qualitative errors of the DFT-derived PES spectra refer to (i) an overall redshift by ˜0.5 eV and (ii) the absence of satellites in the high-energy region of the spectra. The former error is shown to be due to the neglect of many-body corrections to ordinary Kohn-Sham methods, while the latter has been argued to be due to electron-nuclear couplings beyond the Born-Oppenheimer approximation [Gali et al., Nat. Commun. 7, 11327 (2016)].

Time-Resolved Investigations of Heterobimetallic Cofactor Assembly in R2lox Reveal Distinct Mn/Fe Intermediates.

PubMed

Miller, Effie K; Trivelas, Nicholas E; Maugeri, Pearson T; Blaesi, Elizabeth J; Shafaat, Hannah S

2017-07-05

The assembly mechanism of the Mn/Fe ligand-binding oxidases (R2lox), a family of proteins that are homologous to the nonheme diiron carboxylate enzymes, has been investigated using time-resolved techniques. Multiple heterobimetallic intermediates that exhibit unique spectral features, including visible absorption bands and exceptionally broad electron paramagnetic resonance signatures, are observed through optical and magnetic resonance spectroscopies. On the basis of comparison to known diiron species and model compounds, the spectra have been attributed to (μ-peroxo)-Mn III /Fe III and high-valent Mn/Fe species. Global spectral analysis coupled with isotopic substitution and kinetic modeling reveals elementary rate constants for the assembly of Mn/Fe R2lox under aerobic conditions. A complete reaction mechanism for cofactor maturation that is consistent with experimental data has been developed. These results suggest that the Mn/Fe cofactor can perform direct C-H bond abstraction, demonstrating the potential for potent chemical reactivity that remains unexplored.

Can CO2 Turbulent Flux Be Measured by Lidar? A Preliminary Study

NASA Technical Reports Server (NTRS)

Gilbert, Fabien; Koch, Grady; Beyon, Jeffrey Y.; Hilton, Timothy W.; Davis, Kenneth J.; Andrews, Arlyn; Flamant, Pierre H.; Singh, Upendra N.

2011-01-01

The vertical profiling ofCO2 turbulent fluxes in the atmospheric boundary layer (ABL) is investigated using a coherent differential absorption lidar (CDIAL) operated nearby a tall tower in Wisconsin during June 2007. A CDIAL can perform simultaneous range-resolved CO2 DIAL and velocity measurements. The lidar eddy covariance technique is presented. The aims of the study are (i) an assessment of performance and current limitation of available CDIAL for CO2 turbulent fluxes and (ii) the derivation of instrument specifications to build a future CDIAL to perform accurate range-resolved CO2 fluxes. Experimental lidar CO2 mixing ratio and vertical velocity profiles are successfully compared with in situ sensors measurements. Time and space integral scales of turbulence in the ABL are addressed that result in limitation for time averaging and range accumulation. A first attempt to infer CO2 fluxes using an eddy covariance technique with currently available 2-mm CDIAL dataset is reported.

Estimation of the absorption coefficients of two-layered media by a simple method using spatially and time-resolved reflectances

NASA Astrophysics Data System (ADS)

Shimada, M.; Sato, C.; Hoshi, Y.; Yamada, Y.

2009-08-01

Our newly developed method using spatially and time-resolved reflectances can easily estimate the absorption coefficients of each layer in a two-layered medium if the thickness of the upper layer and the reduced scattering coefficients of the two layers are known a priori. We experimentally validated this method using phantoms and examined its possibility of estimating the absorption coefficients of the tissues in human heads. In the case of a homogeneous plastic phantom (polyacetal block), the absorption coefficient estimated by our method agreed well with that obtained by a conventional method. Also, in the case of two-layered phantoms, our method successfully estimated the absorption coefficients of the two layers. Furthermore, the absorption coefficients of the extracerebral and cerebral tissue inside human foreheads were estimated under the assumption that the human heads were two-layered media. It was found that the absorption coefficients of the cerebral tissues were larger than those of the extracerebral tissues.

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

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

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born–Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersionmore » of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.« less

Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5.

PubMed

Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G

2015-08-28

Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization.

Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5

PubMed Central

Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G.

2015-01-01

Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization. PMID:26314613

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

PubMed

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.

Fluid mechanics and heat transfer spirally fluted tubing

NASA Astrophysics Data System (ADS)

Yampolsky, J. S.; Libby, P. A.; Launder, B. E.; Larue, J. C.

1984-12-01

The objective of this program is to develop an understanding of the fluid mechanics and heat transfer mechanisms that result in the demonstrated performance of the spiral fluted tubing under development at GA Technologies Inc. Particularly emphasized are the processes that result in the augmentation of the heat transfer coefficient without an increase in friction coefficient in the single-phase flow. Quantitative delineation of these processes would allow for their application to the optimal solution of heat transfer problems in general was well as to tubular heat exchanges using spiral fluted tubes. The experimental phase of the program consisted of the following: (1) Flow visualization studies using high-speed photography of dye injected into water flowing in a cast acrylic spiral fluted tube. (2) Time-resolved axial velocity measurements as a function of radius at the exit plane of a spiral fluted tube with water flowing through the tube. (3) Simultaneous time-resolved measurements of the axial and radial velocity components and temperature with heated air flowing through the tube cooled by a water jacket.

Transition mechanism of sH to filled-ice Ih structure of methane hydrate under fixed pressure condition

NASA Astrophysics Data System (ADS)

Kadobayashi, H.; Hirai, H.; Ohfuji, H.; Kojima, Y.; Ohishi, Y.; Hirao, N.; Ohtake, M.; Yamamoto, Y.

2017-10-01

The phase transition mechanism of methane hydrate from sH to filled-ice Ih structure was examined using a combination of time-resolved X-ray diffractometry (XRD) and Raman spectroscopy in conjunction with charge-coupled device (CCD) camera observation under fixed pressure conditions. Prior to time-resolved Raman experiments, the typical C-H vibration modes and their pressure dependence of three methane hydrate structures, fluid methane and solid methane were measured using Raman spectroscopy to distinguish the phase transitions of methane hydrates from decomposition to solid methane and ice VI or VII. Experimental results by XRD, Raman spectroscopy and CCD camera observation revealed that the structural transition of sH to filled-ice Ih occurs through a collapse of the sH framework followed by the release of fluid methane that is then gradually incorporated into the filled-ice Ih to reconstruct its structure. These observations suggest that the phase transition of sH to filled-ice Ih takes place by a typical reconstructive mechanism.

Mediation of donor–acceptor distance in an enzymatic methyl transfer reaction

PubMed Central

Zhang, Jianyu; Kulik, Heather J.; Martinez, Todd J.; Klinman, Judith P.

2015-01-01

Enzymatic methyl transfer, catalyzed by catechol-O-methyltransferase (COMT), is investigated using binding isotope effects (BIEs), time-resolved fluorescence lifetimes, Stokes shifts, and extended graphics processing unit (GPU)-based quantum mechanics/molecular mechanics (QM/MM) approaches. The WT enzyme is compared with mutants at Tyr68, a conserved residue that is located behind the reactive sulfur of cofactor. Small (>1) BIEs are observed for an S-adenosylmethionine (AdoMet)-binary and abortive ternary complex containing 8-hydroxyquinoline, and contrast with previously reported inverse (<1) kinetic isotope effects (KIEs). Extended GPU-based computational studies of a ternary complex containing catecholate show a clear trend in ground state structures, from noncanonical bond lengths for WT toward solution values with mutants. Structural and dynamical differences that are sensitive to Tyr68 have also been detected using time-resolved Stokes shift measurements and molecular dynamics. These experimental and computational results are discussed in the context of active site compaction that requires an ionization of substrate within the enzyme ternary complex. PMID:26080432

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

DOE PAGES

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert; ...

2017-05-24

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born–Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersionmore » of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.« less

Theoretical and experimental study on near infrared time-resolved optical diffuse tomography

NASA Astrophysics Data System (ADS)

Zhao, Huijuan; Gao, Feng; Tanikawa, Yukari; Yamada, Yukio

2006-08-01

Parts of the works of our group in the past five years on near infrared time-resolved (TR) optical tomography are summarized in this paper. The image reconstruction algorithm is based on Newton Raphson scheme with a datatype R generated from modified Generalized Pulse Spectrum Technique. Firstly, the algorithm is evaluated with simulated data from a 2-D model and the datatype R is compared with other popularly used datatypes. In this second part of the paper, the in vitro and in vivo NIR DOT imaging on a chicken leg and a human forearm, respectively are presented for evaluating both the image reconstruction algorithm and the TR measurement system. The third part of this paper is about the differential pathlength factor of human head while monitoring head activity with NIRS and applying the modified Lambert-Beer law. Benefiting from the TR system, the measured DPF maps of the three import areas of human head are presented in this paper.

A radially resolved kinetic model for nonlocal electron ripple diffusion losses in tokamaks

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

Robertson, Scott

A relatively simple radially resolved kinetic model is applied to the ripple diffusion problem for electrons in tokamaks. The distribution function f(r,v) is defined on a two-dimensional grid, where r is the radial coordinate and v is the velocity coordinate. Particle transport in the radial direction is from ripple and banana diffusion and transport in the velocity direction is described by the Fokker-Planck equation. Particles and energy are replaced by source functions that are adjusted to maintain a constant central density and temperature. The relaxed profiles of f(r,v) show that the electron distribution function at the wall contains suprathermal electronsmore » that have diffused from the interior that enhance ripple transport. The transport at the periphery is therefore nonlocal. The energy replacement times from the computational model are near to the experimental replacement times for tokamak discharges in the compilation by Pfeiffer and Waltz [Nucl. Fusion 19, 51 (1979)].« less

Homogeneous time-resolved G protein-coupled receptor-ligand binding assay based on fluorescence cross-correlation spectroscopy.

PubMed

Antoine, Thomas; Ott, David; Ebell, Katharina; Hansen, Kerrin; Henry, Luc; Becker, Frank; Hannus, Stefan

2016-06-01

G protein-coupled receptors (GPCRs) mediate many important physiological functions and are considered as one of the most successful therapeutic target classes for a wide spectrum of diseases. Drug discovery projects generally benefit from a broad range of experimental approaches for screening compound libraries and for the characterization of binding modes of drug candidates. Owing to the difficulties in solubilizing and purifying GPCRs, assay formats have been so far mainly limited to cell-based functional assays and radioligand binding assays. In this study, we used fluorescence cross-correlation spectroscopy (FCCS) to analyze the interaction of detergent-solubilized receptors to various types of GPCR ligands: endogenous peptides, small molecules, and a large surrogate antagonist represented by a blocking monoclonal antibody. Our work demonstrates the suitability of the homogeneous and time-resolved FCCS assay format for a robust, high-throughput determination of receptor-ligand binding affinities and kinetic rate constants for various therapeutically relevant GPCRs. Copyright © 2016 The Authors. Published by Elsevier Inc. All rights reserved.

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

NASA Astrophysics Data System (ADS)

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert; van Driel, Tim B.; Chollet, Matthieu; Glownia, James M.; Song, Sanghoon; Zhu, Diling; Pace, Elisabetta; Matar, Samir F.; Nielsen, Martin M.; Benfatto, Maurizio; Gaffney, Kelly J.; Collet, Eric; Cammarata, Marco

2017-05-01

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.

Distance distributions of short polypeptides recovered by fluorescence resonance energy transfer in the 10 A domain.

PubMed

Sahoo, Harekrushna; Roccatano, Danilo; Zacharias, Martin; Nau, Werner M

2006-06-28

Fluorescence resonance energy transfer (FRET) between tryptophan (Trp) as donor and 2,3-diazabicyclo[2.2.2]oct-2-ene (Dbo) as acceptor was studied by steady-state and time-resolved fluorescence spectroscopy. The unique feature of this FRET pair is its exceptionally short Förster radius (10 A), which allows one to recover distance distributions in very short structureless peptides. The technique was applied to Trp-(GlySer)n-Dbo-NH2 peptides with n = 0-10, for which the average probe/quencher distance ranged between 8.7 and 13.7 A experimentally (in propylene glycol, analysis according to wormlike chain model) and 8.6-10.2 A theoretically (for n = 0-6, GROMOS96 molecular dynamics simulations). The larger FRET efficiency in steady-state compared to time-resolved fluorescence experiments was attributed to a static quenching component, suggesting that a small but significant part (ca. 10%) of the conformations are already in van der Waals contact when excitation occurs.

Computational and experimental study of laminar flames

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

Smooke, Mitchell

During the past three years, our research has centered on an investigation of the effects of complex chemistry and detailed transport on the structure and extinction of hydrocarbon flames in coflowing axisymmetric configurations. We have pursued both computational and experimental aspects of the research in parallel on both steady-state and time-dependent systems. The computational work has focused on the application of accurate and efficient numerical methods for the solution of the steady-state and time-dependent boundary value problems describing the various reacting systems. Detailed experimental measurements were performed on axisymmetric coflow flames using two-dimensional imaging techniques. Previously, spontaneous Raman scattering, chemiluminescence,more » and laser-induced fluorescence were used to measure the temperature, major and minor species profiles. Particle image velocimetry (PIV) has been used to investigate velocity distributions and for calibration of time-varying flames. Laser-induced incandescence (LII) with an extinction calibration was used to determine soot volume fractions, while soot surface temperatures were measured with three-color optical pyrometry using a color digital camera. A blackbody calibration of the camera allows for determination of soot volume fraction as well, which can be compared with the LII measurements. More recently, we have concentrated on a detailed characterization of soot using a variety of techniques including time-resolved LII (TiRe-LII) for soot primary particles sizes, multi-angle light scattering (MALS) for soot radius of gyration, and spectrally-resolved line of sight attenuation (spec-LOSA). Combining the information from all of these soot measurements can be used to determine the soot optical properties, which are observed to vary significantly depending on spatial location and fuel dilution. Our goal has been to obtain a more fundamental understanding of the important fluid dynamic and chemical interactions in these flames so that this information can be used effectively in combustion modeling.« less

Evaluation of a fast single-photon avalanche photodiode for measurement of early transmitted photons through diffusive media.

PubMed

Mu, Ying; Valim, Niksa; Niedre, Mark

2013-06-15

We tested the performance of a fast single-photon avalanche photodiode (SPAD) in measurement of early transmitted photons through diffusive media. In combination with a femtosecond titanium:sapphire laser, the overall instrument temporal response time was 59 ps. Using two experimental models, we showed that the SPAD allowed measurement of photon-density sensitivity functions that were approximately 65% narrower than the ungated continuous wave case at very early times. This exceeds the performance that we have previously achieved with photomultiplier-tube-based systems and approaches the theoretical maximum predicted by time-resolved Monte Carlo simulations.

Experimental Investigation of Superradiance in a Tapered Free-Electron Laser Amplifier

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

Hidaka, Y.; She, Y.; Murphy, J.B.

2011-03-28

We report experimental studies of the effect of undulator tapering on superradiance in a single-pass high-gain free-electron laser (FEL) amplifier. The experiments were performed at the Source Development Laboratory (SDL) of National Synchrotron Light Source (NSLS). Efficiency was nearly tripled with tapering. Both the temporal and spectral properties of the superradiant FEL along the uniform and tapered undulator were experimentally characterized using frequency-resolved optical gating (FROG) images. Numerical studies predicted pulse broadening and spectral cleaning by undulator tapering Pulse broadening was experimentally verified. However, spectral cleanliness degraded with tapering. We have performed first experiments with a tapered undulator and amore » short seed laser pulse. Pulse broadening with tapering expected from simulations was experimentally confirmed. However, the experimentally obtained spectra degraded with tapering, whereas the simulations predicted improvement. A further numerical study is under way to resolve this issue.« less

Light scattering microscopy measurements of single nuclei compared with GPU-accelerated FDTD simulations

NASA Astrophysics Data System (ADS)

Stark, Julian; Rothe, Thomas; Kieß, Steffen; Simon, Sven; Kienle, Alwin

2016-04-01

Single cell nuclei were investigated using two-dimensional angularly and spectrally resolved scattering microscopy. We show that even for a qualitative comparison of experimental and theoretical data, the standard Mie model of a homogeneous sphere proves to be insufficient. Hence, an accelerated finite-difference time-domain method using a graphics processor unit and domain decomposition was implemented to analyze the experimental scattering patterns. The measured cell nuclei were modeled as single spheres with randomly distributed spherical inclusions of different size and refractive index representing the nucleoli and clumps of chromatin. Taking into account the nuclear heterogeneity of a large number of inclusions yields a qualitative agreement between experimental and theoretical spectra and illustrates the impact of the nuclear micro- and nanostructure on the scattering patterns.

Experimental triple-slit interference in a strongly driven V-type artificial atom

NASA Astrophysics Data System (ADS)

Dada, Adetunmise C.; Santana, Ted S.; Koutroumanis, Antonios; Ma, Yong; Park, Suk-In; Song, Jindong; Gerardot, Brian D.

2017-08-01

Rabi oscillations of a two-level atom appear as a quantum interference effect between the amplitudes associated with atomic superpositions, in analogy with the classic double-slit experiment which manifests a sinusoidal interference pattern. By extension, through direct detection of time-resolved resonance fluorescence from a quantum-dot neutral exciton driven in the Rabi regime, we experimentally demonstrate triple-slit-type quantum interference via quantum erasure in a V-type three-level artificial atom. This result is of fundamental interest in the experimental studies of the properties of V-type three-level systems and may pave the way for further insight into their coherence properties as well as applications for quantum information schemes. It also suggests quantum dots as candidates for multipath-interference experiments for probing foundational concepts in quantum physics.

Light scattering microscopy measurements of single nuclei compared with GPU-accelerated FDTD simulations.

PubMed

Stark, Julian; Rothe, Thomas; Kieß, Steffen; Simon, Sven; Kienle, Alwin

2016-04-07

Single cell nuclei were investigated using two-dimensional angularly and spectrally resolved scattering microscopy. We show that even for a qualitative comparison of experimental and theoretical data, the standard Mie model of a homogeneous sphere proves to be insufficient. Hence, an accelerated finite-difference time-domain method using a graphics processor unit and domain decomposition was implemented to analyze the experimental scattering patterns. The measured cell nuclei were modeled as single spheres with randomly distributed spherical inclusions of different size and refractive index representing the nucleoli and clumps of chromatin. Taking into account the nuclear heterogeneity of a large number of inclusions yields a qualitative agreement between experimental and theoretical spectra and illustrates the impact of the nuclear micro- and nanostructure on the scattering patterns.

Control of experimental uncertainties in filtered Rayleigh scattering measurements

NASA Technical Reports Server (NTRS)

Forkey, Joseph N.; Finkelstein, N. D.; Lempert, Walter R.; Miles, Richard B.

1995-01-01

Filtered Rayleigh Scattering is a technique which allows for measurement of velocity, temperature, and pressure in unseeded flows, spatially resolved in 2-dimensions. We present an overview of the major components of a Filtered Rayleigh Scattering system. In particular, we develop and discuss a detailed theoretical model along with associated model parameters and related uncertainties. Based on this model, we then present experimental results for ambient room air and for a Mach 2 free jet, including spatially resolved measurements of velocity, temperature, and pressure.

Experimental investigation of the dynamics of pellet ablation on the Texas Experimental Tokamak

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

Durst, R.D.

1988-01-01

Rapid fluctuations in the ablation of hydrogen pellets in the Texas Experimental Tokamak were studied using fast photographic techniques. It is proposed that the fluctuations are a type of relaxation oscillation driven by the motion of the particle across the magnetic field. This is shown to be consistent with a time-dependent model of plasma shielding due to Kaufmann et al. A technique to include this effect in calculations of pellet ablation is discussed. Spatially resolved measurements of the temperature and density in the pellet-ablation cloud were obtained by line-to-continuum ratios and Stark broadening, respectively. Typical parameters in the pellet-ablation cloudmore » are 5-6 eV and 1.0-1.5 {times} 10{sup 17} cm{sup {minus}3}. The flow along the magnetic field is found to be isobaric. The heating of the expanding ablatant is strongly asymmetric, being stronger on the side facing the electron-drift direction. This may be due to suprathermal electrons.« less

Simulation of FRET dyes allows quantitative comparison against experimental data

NASA Astrophysics Data System (ADS)

Reinartz, Ines; Sinner, Claude; Nettels, Daniel; Stucki-Buchli, Brigitte; Stockmar, Florian; Panek, Pawel T.; Jacob, Christoph R.; Nienhaus, Gerd Ulrich; Schuler, Benjamin; Schug, Alexander

2018-03-01

Fully understanding biomolecular function requires detailed insight into the systems' structural dynamics. Powerful experimental techniques such as single molecule Förster Resonance Energy Transfer (FRET) provide access to such dynamic information yet have to be carefully interpreted. Molecular simulations can complement these experiments but typically face limits in accessing slow time scales and large or unstructured systems. Here, we introduce a coarse-grained simulation technique that tackles these challenges. While requiring only few parameters, we maintain full protein flexibility and include all heavy atoms of proteins, linkers, and dyes. We are able to sufficiently reduce computational demands to simulate large or heterogeneous structural dynamics and ensembles on slow time scales found in, e.g., protein folding. The simulations allow for calculating FRET efficiencies which quantitatively agree with experimentally determined values. By providing atomically resolved trajectories, this work supports the planning and microscopic interpretation of experiments. Overall, these results highlight how simulations and experiments can complement each other leading to new insights into biomolecular dynamics and function.

Ultrafast Time-Resolved Photoluminescence Studies of Gallium-Arsenide

NASA Astrophysics Data System (ADS)

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-alloyed GaAs. It is found that the PL intensity contrast between bright and dark areas correlates with the ratio of the lifetimes measured using PECS in these areas. Thus, the PL intensity contrast is due to the difference in the carrier lifetimes in the different regions. The carrier lifetimes in the bright and dark regions have different temperature dependences. (Abstract shortened with permission of author.).

Study of particle evolution from Composition B-3 detonation by time-resolved small angle x-ray scattering

NASA Astrophysics Data System (ADS)

Huber, R.; Podlesak, D.; Dattelbaum, D.; Firestone, M.; Gustavsen, R.; Jensen, B.; Ringstrand, B.; Watkins, E.; Bagge-Hansen, M.; Hodgin, R.; Lauderbach, L.; Willey, T.; van Buuren, T.; Graber, T.; Rigg, P.; Sinclair, N.; Seifert, S.

2017-06-01

High explosive (HE) detonations produce an assortment of gases (CO, CO2, N2) and solid carbon products (nanodiamond, graphite). The evolution of solid carbon particles, within the chemical reaction zone, help to propel the detonation wave forward. Due to the violent nature and short reaction times during HE detonations, experimental observation are limited. Through time-resolved small angle x-ray scattering (TRSAXS) we are able to observed nanocarbon formation on nanosecond time scales. This TRSAXS setup is the first of its kind in the United States at Argonne National Laboratory at the Advanced Photon Source in the Dynamic Compression Sector. From the empirical and analytical analysis of the x-ray scattering of an in-line detonation we are able to temporally follow morphology and size. Two detonation geometries were studied for the HE Comp B-3 (40% TNT/60% RDX), producing steady and overdriven conditions. Steady wave particle evolution plateaued by 2 microseconds, where overdriven condition particle size decreases at the collision of the two shock fronts then plateaus. Post detonation soot is also analyzed to confirm size and shape of nanocarbon formation from Comp B-3 detonations. LA-UR-17-21443.

Time-dependent, x-ray spectral unfolds and brightness temperatures for intense Li{sup +} ion beam-driven hohlraums

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

Fehl, D.L.; Chandler, G.A.; Biggs, F.

X-ray-producing hohlraums are being studied as indirect drives for Inertial Confinement Fusion targets. In a 1994 target series on the PBFAII accelerator, cylindrical hohlraum targets were heated by an intense Li{sup +} ion beam and viewed by an array of 13 time-resolved, filtered x-ray detectors (XRDs). The UFO unfold code and its suite of auxiliary functions were used extensively in obtaining time- resolved x-ray spectra and radiation temperatures from this diagnostic. UFO was also used to obtain fitted response functions from calibration data, to simulate data from blackbody x-ray spectra of interest, to determine the suitability of various unfolding parametersmore » (e.g., energy domain, energy partition, smoothing conditions, and basis functions), to interpolate the XRD signal traces, and to unfold experimental data. The simulation capabilities of the code were useful in understanding an anomalous feature in the unfolded spectra at low photon energies ({le} 100 eV). Uncertainties in the differential and energy-integrated unfolded spectra were estimated from uncertainties in the data. The time-history of the radiation temperature agreed well with independent calculations of the wall temperature in the hohlraum.« less

Unraveling the electronic relaxation dynamics in photoexcited 2,4-difluoroaniline via femtosecond time-resolved photoelectron imaging

NASA Astrophysics Data System (ADS)

Ling, Fengzi; Li, Shuai; Wei, Jie; Liu, Kai; Wang, Yanmei; Zhang, Bing

2018-04-01

Time-resolved photoelectron imaging is employed to investigate the relaxation dynamics of the lowest two excited electronic states S1(ππ*) and S2(π3s/πσ*) in 2,4-difluoroaniline (24DFA). As the S1(ππ*) state is populated directly following 289 nm excitation, the population undergoes ultrafast intramolecular vibrational redistribution on a 540 fs time scale, followed by efficient intersystem crossing from S1(ππ*) to the triplet state within 379 ps, and the subsequent slower deactivation process of the triplet state. For excitation to the S2(π3s/πσ*) state at 238 nm, the population probably bifurcates into two decay channels. The dominant channel with 84 fs involves ultrafast internal conversion to the S1(ππ*) state, from which it relaxes to the electronic ground state on a 116 ps time scale. The other appears to involve motion along the S2(π3s/πσ*) potential energy surface. Our data also determine experimentally the electronic energies of S2(π3s/πσ*), S3(ππ*), and several Rydberg states in 24DFA.

A wavelength dependent investigation of the indole photophysics via ionization and fragmentation pump-probe spectroscopies.

PubMed

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

2015-10-14

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

Communication: Electron ionization of DNA bases.

PubMed

Rahman, M A; Krishnakumar, E

2016-04-28

No reliable experimental data exist for the partial and total electron ionization cross sections for DNA bases, which are very crucial for modeling radiation damage in genetic material of living cell. We have measured a complete set of absolute partial electron ionization cross sections up to 500 eV for DNA bases for the first time by using the relative flow technique. These partial cross sections are summed to obtain total ion cross sections for all the four bases and are compared with the existing theoretical calculations and the only set of measured absolute cross sections. Our measurements clearly resolve the existing discrepancy between the theoretical and experimental results, thereby providing for the first time reliable numbers for partial and total ion cross sections for these molecules. The results on fragmentation analysis of adenine supports the theory of its formation in space.

Resolved simulations of a granular-fluid flow through a check dam with a SPH-DCDEM model

NASA Astrophysics Data System (ADS)

Birjukovs Canelas, Ricardo; Domínguez, Jose; Crespo, Alejandro; Gómez-Gesteira, Moncho; Ferreira, Rui M. L.

2017-04-01

Debris flows represent some of the most relevant phenomena in geomorphological events. Due to the potential destructiveness of such flows, they are the target of a vast amount of research. Experimental research in laboratory facilities or in the field is fundamental to characterize the fundamental rheological properties of these flows and to provide insights on its structure. However, characterizing interparticle contacts and the structure of the motion of the granular phase is difficult, even in controlled laboratory conditions, and possible only for simple geometries. This work addresses the need for a numerical simulation tool applicable to granular-fluid mixtures featuring high spatial and temporal resolution, thus capable of resolving the motion of individual particles, including all interparticle contacts and susceptible to complement laboratory research. The DualSPHysics meshless numerical implementation based on Smoothed Particle Hydrodynamics (SPH) is expanded with a Distributed Contact Discrete Element Method (DCDEM) in order to explicitly solve the fluid and the solid phase. The specific objective is to test the SPH-DCDEM approach by comparing its results with experimental data. An experimental set-up for stony debris flows in a slit check dam is reproduced numerically, where solid material is introduced through a hopper assuring a constant solid discharge for the considered time interval. With each sediment particle possibly undergoing several simultaneous contacts, thousands of time-evolving interactions are efficiently treated due to the model's algorithmic structure and the HPC implementation of DualSPHysics. The results, comprising mainly of retention curves, are in good agreement with the measurements, correctly reproducing the changes in efficiency with slit spacing and density. The encouraging results, coupled with the prospect of so far unique insights into the internal dynamics of a debris flow show the potential of high-performance resolved approaches to the description of the flow and the study of its mitigation strategies. This research as partially supported by Portuguese and European funds, within programs COMPETE2020 and PORL-FEDER, through project PTDC/ECM-HID/6387/2014 granted by the National Foundation for Science and Technology (FCT).

Quantum theoretical study of electron solvation dynamics in ice layers on a Cu(111) surface.

PubMed

Andrianov, I; Klamroth, T; Saalfrank, P; Bovensiepen, U; Gahl, C; Wolf, M

2005-06-15

Recent experiments using time- and angle-resolved two-photon photoemission (2PPE) spectroscopy at metal/polar adsorbate interfaces succeeded in time-dependent analysis of the process of electron solvation. A fully quantum mechanical, two-dimensional simulation of this process, which explicitly includes laser excitation, is presented here, confirming the origin of characteristic features, such as the experimental observation of an apparently negative dispersion. The inference of the spatial extent of the localized electron states from the angular dependence of the 2PPE spectra has been found to be non-trivial and system-dependent.

The SPORT-NMR Software: A Tool for Determining Relaxation Times in Unresolved NMR Spectra

NASA Astrophysics Data System (ADS)

Geppi, Marco; Forte, Claudia

1999-03-01

A software package which allows the correct determination of individual relaxation times for all the nonequivalent nuclei in poorly resolved NMR spectra is described. The procedure used, based on the fitting of each spectrum in the series recorded in the relaxation experiment, should improve the analysis of relaxation data in terms of quantitative dynamic information, especially in anisotropic phases. Tests on simulated data and experimental examples concerning1H and13CT1ρmeasurement in a solid copolymer and2HT1ZandT1Qmeasurement in a liquid crystal are shown and discussed.

Continuous distribution of emission states from single CdSe/ZnS quantum dots.

PubMed

Zhang, Kai; Chang, Hauyee; Fu, Aihua; Alivisatos, A Paul; Yang, Haw

2006-04-01

The photoluminescence dynamics of colloidal CdSe/ZnS/streptavidin quantum dots were studied using time-resolved single-molecule spectroscopy. Statistical tests of the photon-counting data suggested that the simple "on/off" discrete state model is inconsistent with experimental results. Instead, a continuous emission state distribution model was found to be more appropriate. Autocorrelation analysis of lifetime and intensity fluctuations showed a nonlinear correlation between them. These results were consistent with the model that charged quantum dots were also emissive, and that time-dependent charge migration gave rise to the observed photoluminescence dynamics.

Carrier recombination dynamics in anatase TiO 2 nanoparticles

NASA Astrophysics Data System (ADS)

Cavigli, Lucia; Bogani, Franco; Vinattieri, Anna; Cortese, Lorenzo; Colocci, Marcello; Faso, Valentina; Baldi, Giovanni

2010-11-01

We present an experimental study of the radiative recombination dynamics in size-controlled TiO 2 nanoparticles in the range 20-130 nm. Time-integrated photoluminescence spectra clearly show a dominance of self-trapped exciton (STE) emission, with main features not dependent on the nanoparticle size and on its environment. From picosecond time-resolved experiments as a function of the excitation density and the nanoparticle size we address the STE recombination dynamics as the result of two main processes related to the direct STE formation and to the indirect STE formation mediated by non-radiative surface states.

Measurement of electron-ion relaxation in warm dense copper

DOE PAGES

Cho, B. I.; Ogitsu, T.; Engelhorn, K.; ...

2016-01-06

Experimental investigation of electron-ion coupling and electron heat capacity of copper in warm and dense states are presented. From time-resolved x-ray absorption spectroscopy, the temporal evolution of electron temperature is obtained for non-equilibrium warm dense copper heated by an intense femtosecond laser pulse. Electron heat capacity and electron-ion coupling are inferred from the initial electron temperature and its decrease over 10 ps. As a result, data are compared with various theoretical models.

Impact of time-resolved MRA on diagnostic accuracy in patients with symptomatic peripheral artery disease of the calf station.

PubMed

Hansmann, Jan; Michaely, Henrik J; Morelli, John N; Diehl, Steffen J; Meyer, Mathias; Schoenberg, Stefan O; Attenberger, Ulrike I

2013-12-01

The purpose of this article is to evaluate the added diagnostic accuracy of time-resolved MR angiography (MRA) of the calves compared with continuous-table-movement MRA in patients with symptomatic lower extremity peripheral artery disease (PAD) using digital subtraction angiography (DSA) correlation. Eighty-four consecutive patients with symptomatic PAD underwent a low-dose 3-T MRA protocol, consisting of continuous-table-movement MRA, acquired from the diaphragm to the calves, and an additional time-resolved MRA of the calves; 0.1 mmol/kg body weight (bw) of contrast material was used (0.07 mmol/kg bw for continuous-table-movement MRA and 0.03 mmol/kg bw for time-resolved MRA). Two radiologists rated image quality on a 4-point scale and stenosis degree on a 3-point scale. An additional assessment determined the degree of venous contamination and whether time-resolved MRA improved diagnostic confidence. The accuracy of stenosis gradation with continuous-table-movement and time-resolved MRA was compared with that of DSA as a correlation. Overall diagnostic accuracy was calculated for continuous-table-movement and time-resolved MRA. Median image quality was rated as good for 578 vessel segments with continuous-table-movement MRA and as excellent for 565 vessel segments with time-resolved MRA. Interreader agreement was excellent (κ = 0.80-0.84). Venous contamination interfered with diagnosis in more than 60% of continuous-table-movement MRA examinations. The degree of stenosis was assessed for 340 vessel segments. The diagnostic accuracies (continuous-table-movement MRA/time-resolved MRA) combined for the readers were obtained for the tibioperoneal trunk (84%/93%), anterior tibial (69%/87%), posterior tibial (85%/91%), and peroneal (67%/81%) arteries. The addition of time-resolved MRA improved diagnostic confidence in 69% of examinations. The addition of time-resolved MRA at the calf station improves diagnostic accuracy over continuous-table-movement MRA alone in symptomatic patients with PAD.

Gamma Knife surgery for arteriovenous malformations in the brain: integration of time-resolved contrast-enhanced magnetic resonance angiography into dosimetry planning. Technical note.

PubMed

Taschner, Christian A; Le Thuc, Vianney; Reyns, Nicolas; Gieseke, Juergen; Gauvrit, Jean-Yves; Pruvo, Jean-Pierre; Leclerc, Xavier

2007-10-01

The aim of this study was to develop an algorithm for the integration of time-resolved contrast-enhanced magnetic resonance (MR) angiography into dosimetry planning for Gamma Knife surgery (GKS) of arteriovenous malformations (AVMs) in the brain. Twelve patients harboring brain AVMs referred for GKS underwent intraarterial digital subtraction (DS) angiography and time-resolved MR angiography while wearing an externally applied cranial stereotactic frame. Time-resolved MR angiography was performed on a 1.5-tesla MR unit (Achieva, Philips Medical Systems) using contrast-enhanced 3D fast field echo sequencing with stochastic central k-space ordering. Postprocessing with interactive data language (Research Systems, Inc.) produced hybrid data sets containing dynamic angiographic information and the MR markers necessary for stereotactic transformation. Image files were sent to the Leksell GammaPlan system (Elekta) for dosimetry planning. Stereotactic transformation of the hybrid data sets containing the time-resolved MR angiography information with automatic detection of the MR markers was possible in all 12 cases. The stereotactic coordinates of vascular structures predefined from time-resolved MR angiography matched with DS angiography data in all cases. In 10 patients dosimetry planning could be performed based on time-resolved MR angiography data. In two patients, time-resolved MR angiography data alone were considered insufficient. The target volumes showed a notable shift of centers between modalities. Integration of time-resolved MR angiography data into the Leksell GammaPlan system for patients with brain AVMs is feasible. The proposed algorithm seems concise and sufficiently robust for clinical application. The quality of the time-resolved MR angiography sequencing needs further improvement.

Polarization resolved angular optical scattering of aerosol particles

NASA Astrophysics Data System (ADS)

Redding, B.; Pan, Y.; Wang, C.; Videen, G.; Cao, Hui

2014-05-01

Real-time detection and identification of bio-aerosol particles are crucial for the protection against chemical and biological agents. The strong elastic light scattering properties of airborne particles provides a natural means for rapid, non-invasive aerosol characterization. Recent theoretical predictions suggested that variations in the polarization dependent angular scattering cross section could provide an efficient means of classifying different airborne particles. In particular, the polarization dependent scattering cross section of aggregate particles is expected to depend on the shape of the primary particles. In order to experimentally validate this prediction, we built a high throughput, sampling system, capable of measuring the polarization resolved angular scattering cross section of individual aerosol particles flowing through an interrogating volume with a single shot of laser pulse. We calibrated the system by comparing the polarization dependent scattering cross section of individual polystyrene spheres with that predicted by Mie theory. We then used the system to study different particles types: Polystyrene aggregates composed 500 nm spheres and Bacillus subtilis (BG, Anthrax simulant) spores composed of elongated 500 nm × 1000 nm cylinder-line particles. We found that the polarization resolved scattering cross section depends on the shape of the constituent elements of the aggregates. This work indicates that the polarization resolved scattering cross section could be used for rapid discrimination between different bio-aerosol particles.

Dynamics of dipole- and valence bound anions in iodide-adenine binary complexes: A time-resolved photoelectron imaging and quantum mechanical investigation

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

Stephansen, Anne B.; King, Sarah B.; Li, Wei-Li

2015-09-14

Dipole bound (DB) and valence bound (VB) anions of binary iodide-adenine complexes have been studied using one-color and time-resolved photoelectron imaging at excitation energies near the vertical detachment energy. The experiments are complemented by quantum chemical calculations. One-color spectra show evidence for two adenine tautomers, the canonical, biologically relevant A9 tautomer and the A3 tautomer. In the UV-pump/IR-probe time-resolved experiments, transient adenine anions can be formed by electron transfer from the iodide. These experiments show signals from both DB and VB states of adenine anions formed on femto- and picosecond time scales, respectively. Analysis of the spectra and comparison withmore » calculations suggest that while both the A9 and A3 tautomers contribute to the DB signal, only the DB state of the A3 tautomer undergoes a transition to the VB anion. The VB anion of A9 is higher in energy than both the DB anion and the neutral, and the VB anion is therefore not accessible through the DB state. Experimental evidence of the metastable A9 VB anion is instead observed as a shape resonance in the one-color photoelectron spectra, as a result of UV absorption by A9 and subsequent electron transfer from iodide into the empty π-orbital. In contrast, the iodide-A3 complex constitutes an excellent example of how DB states can act as doorway state for VB anion formation when the VB state is energetically available.« less

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

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

Wu, Guorong; State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023; Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026

The dynamics of pyrrole excited at wavelengths in the range 242-217 nm are studied using a combination of time-resolved photoelectron spectroscopy and wavepacket propagations performed using the multi-configurational time-dependent Hartree method. Excitation close to the origin of pyrrole’s electronic spectrum, at 242 and 236 nm, is found to result in an ultrafast decay of the system from the ionization window on a single timescale of less than 20 fs. This behaviour is explained fully by assuming the system to be excited to the A{sub 2}(πσ{sup ∗}) state, in accord with previous experimental and theoretical studies. Excitation at shorter wavelengths hasmore » previously been assumed to result predominantly in population of the bright A{sub 1}(ππ{sup ∗}) and B{sub 2}(ππ{sup ∗}) states. We here present time-resolved photoelectron spectra at a pump wavelength of 217 nm alongside detailed quantum dynamics calculations that, together with a recent reinterpretation of pyrrole’s electronic spectrum [S. P. Neville and G. A. Worth, J. Chem. Phys. 140, 034317 (2014)], suggest that population of the B{sub 1}(πσ{sup ∗}) state (hitherto assumed to be optically dark) may occur directly when pyrrole is excited at energies in the near UV part of its electronic spectrum. The B{sub 1}(πσ{sup ∗}) state is found to decay on a timescale of less than 20 fs by both N-H dissociation and internal conversion to the A{sub 2}(πσ{sup ∗}) state.« less

Application of the space-resolving flux detector for radiation measurements from an octahedral-aperture spherical hohlraum

NASA Astrophysics Data System (ADS)

Xie, Xufei; Du, Huabing; Chen, Jinwen; Liu, Shenye; Li, Zhichao; Yang, Dong; Huang, Yunbao; Ren, Kuan; Hou, Lifei; Li, Sanwei; Guo, Liang; Jiang, Xiaohua; Huo, Wenyi; Chen, Yaohua; Ren, Guoli; Lan, Ke; Wang, Feng; Jiang, Shaoen; Ding, Yongkun

2018-06-01

Space-resolving flux detection is an important technique for the diagnostic of the radiation field within the hohlraum in inertial confinement fusion, especially for the radiation field diagnostic in the novel spherical hohlraum with octahedral six laser entrance holes (LEHs), where localized measurements are necessary for the discrimination of the radiation flux from different LEHs. A novel space-resolving flux detector (SRFD) is developed at the SG-III laser facility for the radiation flux measurement in the first campaign of the octahedral spherical hohlraum energetics experiment. The principle and configuration of the SRFD system is introduced. The radiation flux from the wall of a gas-filled octahedral spherical hohlraum is measured for the first time by placing the SRFD system at the equatorial position of the SG-III laser facility, aiming at the hohlraum wall through one of the six LEHs. The absolute radiation flux from the re-emission area on the hohlraum wall is measured, and good consistency is found between the experimental data and the calculated data from a three-dimensional view factor analysis.

Time-Resolved Magnetic Field Effects Distinguish Loose Ion Pairs from Exciplexes

PubMed Central

2013-01-01

We describe the experimental investigation of time-resolved magnetic field effects in exciplex-forming organic donor–acceptor systems. In these systems, the photoexcited acceptor state is predominantly deactivated by bimolecular electron transfer reactions (yielding radical ion pairs) or by direct exciplex formation. The delayed fluorescence emitted by the exciplex is magnetosensitive if the reaction pathway involves loose radical ion pair states. This magnetic field effect results from the coherent interconversion between the electronic singlet and triplet radical ion pair states as described by the radical pair mechanism. By monitoring the changes in the exciplex luminescence intensity when applying external magnetic fields, details of the reaction mechanism can be elucidated. In this work we present results obtained with the fluorophore-quencher pair 9,10-dimethylanthracene/N,N-dimethylaniline (DMA) in solvents of systematically varied permittivity. A simple theoretical model is introduced that allows discriminating the initial state of quenching, viz., the loose ion pair and the exciplex, based on the time-resolved magnetic field effect. The approach is validated by applying it to the isotopologous fluorophore-quencher pairs pyrene/DMA and pyrene-d10/DMA. We detect that both the exciplex and the radical ion pair are formed during the initial quenching stage. Upon increasing the solvent polarity, the relative importance of the distant electron transfer quenching increases. However, even in comparably polar media, the exciplex pathway remains remarkably significant. We discuss our results in relation to recent findings on the involvement of exciplexes in photoinduced electron transfer reactions. PMID:24041160

Time-resolved perfusion imaging at the angiography suite: preclinical comparison of a new flat-detector application to computed tomography perfusion.

PubMed

Jürgens, Julian H W; Schulz, Nadine; Wybranski, Christian; Seidensticker, Max; Streit, Sebastian; Brauner, Jan; Wohlgemuth, Walter A; Deuerling-Zheng, Yu; Ricke, Jens; Dudeck, Oliver

2015-02-01

The objective of this study was to compare the parameter maps of a new flat-panel detector application for time-resolved perfusion imaging in the angiography room (FD-CTP) with computed tomography perfusion (CTP) in an experimental tumor model. Twenty-four VX2 tumors were implanted into the hind legs of 12 rabbits. Three weeks later, FD-CTP (Artis zeego; Siemens) and CTP (SOMATOM Definition AS +; Siemens) were performed. The parameter maps for the FD-CTP were calculated using a prototype software, and those for the CTP were calculated with VPCT-body software on a dedicated syngo MultiModality Workplace. The parameters were compared using Pearson product-moment correlation coefficient and linear regression analysis. The Pearson product-moment correlation coefficient showed good correlation values for both the intratumoral blood volume of 0.848 (P < 0.01) and the blood flow of 0.698 (P < 0.01). The linear regression analysis of the perfusion between FD-CTP and CTP showed for the blood volume a regression equation y = 4.44x + 36.72 (P < 0.01) and for the blood flow y = 0.75x + 14.61 (P < 0.01). This preclinical study provides evidence that FD-CTP allows a time-resolved (dynamic) perfusion imaging of tumors similar to CTP, which provides the basis for clinical applications such as the assessment of tumor response to locoregional therapies directly in the angiography suite.

Experimental Approaches for Solution X-Ray Scattering and Fiber Diffraction

PubMed Central

Irving, T. C.

2008-01-01

X-ray scattering and diffraction from non-crystalline systems have gained renewed interest in recent years, as focus shifts from the structural chemistry information gained by high-resolution studies to the context of structural physiology at larger length scales. Such techniques permit the study of isolated macromolecules as well as highly organized macromolecular assemblies as a whole under near-physiological conditions. Time-resolved approaches, made possible by advanced synchrotron instrumentation, add a critical dimension to many of these investigations. This article reviews experimental approaches in non-crystalline x-ray scattering and diffraction that may be used to illuminate important scientific questions such as protein/nucleic acid folding and structure-function relationships in large macromolecular assemblies. PMID:18801437

Phenomena induced by charged particle beams. [experimental design for Spacelab

NASA Technical Reports Server (NTRS)

Beghin, C.

1981-01-01

The injection of energetic particles along the Earth's magnetic field lines is a possible remote sensing method for measuring the electric fields parallel to the magnetic field with good time resolution over the entire magnetic field. Neutralization processes, return-current effects, dynamics of the beams, triggered instabilities, and waves must be investigated before the fundamental question about proper experimental conditions, such as energy, intensity and divergence of the beams, pitch-angle injection, ion species, proper probes and detectors and their location, and rendezvous conditions, can be resolved. An experiment designed to provide a better understanding of these special physical processes and to provide some answers to questions concerning beam injection techniques is described.

Resolving the Detailed Structure of Cortical and Thalamic Neurons in the Adult Rat Brain with Refined Biotinylated Dextran Amine Labeling

PubMed Central

Ling, Changying; Hendrickson, Michael L.; Kalil, Ronald E.

2012-01-01

Biotinylated dextran amine (BDA) has been used frequently for both anterograde and retrograde pathway tracing in the central nervous system. Typically, BDA labels axons and cell somas in sufficient detail to identify their topographical location accurately. However, BDA labeling often has proved to be inadequate to resolve the fine structural details of axon arbors or the dendrites of neurons at a distance from the site of BDA injection. To overcome this limitation, we varied several experimental parameters associated with the BDA labeling of neurons in the adult rat brain in order to improve the sensitivity of the method. Specifically, we compared the effect on labeling sensitivity of: (a) using 3,000 or 10,000 MW BDA; (b) injecting different volumes of BDA; (c) co-injecting BDA with NMDA; and (d) employing various post-injection survival times. Following the extracellular injection of BDA into the visual cortex, labeled cells and axons were observed in both cortical and thalamic areas of all animals studied. However, the detailed morphology of axon arbors and distal dendrites was evident only under optimal conditions for BDA labeling that take into account the: molecular weight of the BDA used, concentration and volume of BDA injected, post-injection survival time, and toning of the resolved BDA with gold and silver. In these instances, anterogradely labeled axons and retrogradely labeled dendrites were resolved in fine detail, approximating that which can be achieved with intracellularly injected compounds such as biocytin or fluorescent dyes. PMID:23144777

Microlensed dual-fiber probe for depth-resolved fluorescence measurements

NASA Astrophysics Data System (ADS)

Choi, Hae Young; Ryu, Seon Young; Kim, Jae Young; Kim, Geon Hee; Park, Seong Jun; Lee, Byeong Ha; Chang, Ki Soo

2011-07-01

We propose and demonstrate a compact microlensed dual-fiber probe that has a good collection efficiency and a high depth-resolution ability for fluorescence measurements. The probe is formed with a conventional fusion splicer creating a common focusing lens on two fibers placed side by side. The collection efficiency of the fabricated probe was evaluated by measuring the fluorescence signal of a fresh ginkgo leaf. It was shown experimentally that the proposed probe could effectively collect the fluorescence signal with a six-fold increase compared to that of a general flat-tipped probe. The beam propagation method was used to design a probe with an optimized working distance and an improved resolving depth. It was found that the working distance depends mainly on the radius of curvature of the lens, whereas the resolving depth is determined by the core diameters of the illumination and collection fibers. The depth-resolved ability of probes with working distances of ~100 μm and 300 μm was validated by using a two-layer tissue phantom. The experimental results demonstrate that the microlensed dual-fiber probe has the potential to facilitate depth-resolved fluorescence detection of epithelial tissue.

An inexpensive technique for the time resolved laser induced plasma spectroscopy

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

Ahmed, Rizwan, E-mail: rizwan.ahmed@ncp.edu.pk; Ahmed, Nasar; Iqbal, J.

We present an efficient and inexpensive method for calculating the time resolved emission spectrum from the time integrated spectrum by monitoring the time evolution of neutral and singly ionized species in the laser produced plasma. To validate our assertion of extracting time resolved information from the time integrated spectrum, the time evolution data of the Cu II line at 481.29 nm and the molecular bands of AlO in the wavelength region (450–550 nm) have been studied. The plasma parameters were also estimated from the time resolved and time integrated spectra. A comparison of the results clearly reveals that the time resolved informationmore » about the plasma parameters can be extracted from the spectra registered with a time integrated spectrograph. Our proposed method will make the laser induced plasma spectroscopy robust and a low cost technique which is attractive for industry and environmental monitoring.« less

Garry Rumbles | NREL

Science.gov Websites

, colloidal quantum dots, and single-walled carbon nanotubes. Laser-based experiments (time-resolved fluorescence spectroscopy; time-resolved resonance Raman spectroscopy; laser-induced fluorescence spectroscopy ; time-resolved evanescent wave-induced fluorescence spectroscopy; picosecond coherent anti-Stokes Raman

An Experimental Study of a Low-Jitter Pulsed Electromagnetic Plasma Accelerator

NASA Technical Reports Server (NTRS)

Thio, Y. C. Francis; Lee, Michael; Eskridge, Richard; Smith, James; Martin, Adam; Rodgers, Stephen L. (Technical Monitor)

2001-01-01

An experimental plasma accelerator for a variety of applications under development at the NASA Marshall Space Flight Center is described. The accelerator is a pulsed plasma thruster and has been tested experimentally and plasma jet velocities of approximately 50 kilometers per second have been obtained. The plasma jet structure has been photographed with 10 ns exposure times to reveal a stable and repeatable plasma structure. Data for velocity profile information has been obtained using light pipes embedded in the gun walls to record the plasma transit at various barrel locations. Preliminary spatially resolved spectral data and magnetic field probe data are also presented. A high speed triggering system has been developed and tested as a means of reducing the gun "jitter". This jitter has been characterized and future work for second generation "ultra-low jitter" gun development is identified.

Modeling of coherent ultrafast magneto-optical experiments: Light-induced molecular mean-field model

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

Hinschberger, Y.; Hervieux, P.-A.

2015-12-28

We present calculations which aim to describe coherent ultrafast magneto-optical effects observed in time-resolved pump-probe experiments. Our approach is based on a nonlinear semi-classical Drude-Voigt model and is used to interpret experiments performed on nickel ferromagnetic thin film. Within this framework, a phenomenological light-induced coherent molecular mean-field depending on the polarizations of the pump and probe pulses is proposed whose microscopic origin is related to a spin-orbit coupling involving the electron spins of the material sample and the electric field of the laser pulses. Theoretical predictions are compared to available experimental data. The model successfully reproduces the observed experimental trendsmore » and gives meaningful insight into the understanding of magneto-optical rotation behavior in the ultrafast regime. Theoretical predictions for further experimental studies are also proposed.« less

High-resolution Imaging of Deuterium-Tritium Capsule Implosions on the National Ignition Facility

NASA Astrophysics Data System (ADS)

Bachmann, Benjamin; Rygg, Ryan; Collins, Gilbert; Patel, Pravesh

2017-10-01

Highly-resolved 3-D simulations of inertial confinement fusion (ICF) implosions predict a hot spot plasma that exhibits complex micron-scale structure originating from a variety of 3-D perturbations. Experimental diagnosis of these conditions requires high spatial resolution imaging techniques. X-ray penumbral imaging can improve the spatial resolution over pinhole imaging while simultaneously increasing the detected photon yield at x-ray energies where the ablator opacity becomes negligible. Here we report on the first time-integrated x-ray penumbral imaging experiments of ICF capsule implosions at the National Ignition Facility that achieved spatial resolution as high as 4 micrometer. 6 to 30 keV hot spot images from layered DT implosions will be presented from a variety of experimental ICF campaigns, revealing previously unseen detail. It will be discussed how these and future results can be used to improve our physics understanding of inertially confined fusion plasmas by enabling spatially resolved measurements of hot spot properties, such as radiation energy, temperature or derived quantities. This work performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344.

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

Lechman, Jeremy B.; Battaile, Corbett Chandler.; Bolintineanu, Dan

This report summarizes a project in which the authors sought to develop and deploy: (i) experimental techniques to elucidate the complex, multiscale nature of thermal transport in particle-based materials; and (ii) modeling approaches to address current challenges in predicting performance variability of materials (e.g., identifying and characterizing physical- chemical processes and their couplings across multiple length and time scales, modeling information transfer between scales, and statically and dynamically resolving material structure and its evolution during manufacturing and device performance). Experimentally, several capabilities were successfully advanced. As discussed in Chapter 2 a flash diffusivity capability for measuring homogeneous thermal conductivity ofmore » pyrotechnic powders (and beyond) was advanced; leading to enhanced characterization of pyrotechnic materials and properties impacting component development. Chapter 4 describes success for the first time, although preliminary, in resolving thermal fields at speeds and spatial scales relevant to energetic components. Chapter 7 summarizes the first ever (as far as the authors know) application of TDTR to actual pyrotechnic materials. This is the first attempt to actually characterize these materials at the interfacial scale. On the modeling side, new capabilities in image processing of experimental microstructures and direct numerical simulation on complicated structures were advanced (see Chapters 3 and 5). In addition, modeling work described in Chapter 8 led to improved prediction of interface thermal conductance from first principles calculations. Toward the second point, for a model system of packed particles, significant headway was made in implementing numerical algorithms and collecting data to justify the approach in terms of highlighting the phenomena at play and pointing the way forward in developing and informing the kind of modeling approach originally envisioned (see Chapter 6). In both cases much more remains to be accomplished.« less

Is Photolytic Production a Viable Source of HCN and HNC in Astrophysical Environments? A Laboratory-based Feasibility Study of Methyl Cyanoformate

NASA Astrophysics Data System (ADS)

Wilhelm, Michael J.; Martínez-Núñez, Emilio; González-Vázquez, Jesús; Vázquez, Saulo A.; Smith, Jonathan M.; Dai, Hai-Lung

2017-11-01

Motivated by the possibility that cyano-containing hydrocarbons may act as photolytic sources for HCN and HNC in astrophysical environments, we conducted a combined experimental and theoretical investigation of the 193 nm photolysis of the cyano-ester, methyl cyanoformate (MCF). Experimentally, nanosecond time-resolved infrared emission spectroscopy was used to detect the emission from nascent products generated in the photolysis reaction. The time-resolved spectra were analyzed using a recently developed spectral reconstruction analysis, which revealed spectral bands assignable to HCN and HNC. Fitting of the emission band shape and intensity allowed determination of the photolysis quantum yields of HCN, HNC, and {CN}({A}2{{{\\Pi }}}1) and an HNC/HCN ratio of ˜0.076 ± 0.059. Additionally, multiconfiguration self-consistent field calculations were used to characterize photoexcitation-induced reactions in the ground and four lowest singlet excited states of MCF. At 193 nm excitation, dissociation is predicted to occur predominantly on the repulsive S 2 state, with minor pathways via internal conversion from S 2 to highly excited ground state. An automated transition-state search algorithm was employed to identify the corresponding ground-state dissociation channels, and Rice-Ramsperger-Kassel-Marcus and Kinetic Monte Carlo simulations were used to calculate the associated branching ratios. The proposed mechanisms were validated using the experimentally measured and quasi-classical trajectory-deduced nascent internal energy distributions of HCN and HNC. This work, along with previous studies, illustrates the propensity for cyano-containing hydrocarbons to act as photolytic sources for astrophysical HCN and HNC and may help explain the observed overabundance of HNC in astrophysical environments.

Ultrafast Spectroscopic Studies of Two-Photon States in Third Order Optical Processes of Dye Chromophores.

NASA Astrophysics Data System (ADS)

Yu, Yi-Zhong

1995-01-01

Conjugated organic and polymeric materials usually have large, nonresonant third order optical nonlinearity due to correlations of their delocalized pi -electrons. Most materials studied so far show positive values of third order nonlinear susceptibility when all frequencies that generate the third order effect are below any optical transition. A new class of organic molecules, namely indole squarylium (ISQ) and anilinium squarylium (BSQ), exhibit negative < gamma(-omega_4;omega_1, omega_2,omega_3)> when all three frequencies, omega_1, omega_2 and omega_3, lie below the first electronic transition. Although quantum many-electron calculations based on multiple-excitation configuration interaction have shown that the negative third order coefficient is essentially due to the contribution from high-lying two-photon states, the field of experimental studies exploring the microscopic origins of the negative squaraines remains uncultivated. The work presented in this thesis involves extensive experimental investigation of squaraines using techniques such as time-resolved transit absorption spectroscopy and saturable absorption. Theoretical simulations studying nonlinear absorption behavior of a simplified two-level system with ultrashort pulses are also presented. Part of the thesis is dedicated to the development, fabrication and characterization of our ultrafast laser system which offers tunable femtosecond pulses at wavelengths from UV to IR and served as a major tool in the experimental measurements. The dynamics of the population inversion between the ground state and the first excited state was also investigated through time-resolved experiments. The experiment results agree well with the theoretical predictions. Strong couplings between the gateway state and high-lying two-photon states were observed in BSQ squarylium molecules, which suggested a complete quantum calculation with multiple energy levels is required to correctly describe the negative third order effect.

Micro-Optical Distributed Sensors for Aero Propulsion Applications

NASA Astrophysics Data System (ADS)

Arnold, S.; Otugen, V.

2003-01-01

The objective of this research is to develop micro-opto-mechanical system (MOMS)-based sensors for time- and space-resolved measurements of flow properties in aerodynamics applications. The measurement technique we propose uses optical resonances in dielectric micro-spheres that can be excited by radiation tunneling from optical fibers. It exploits the tunneling-induced and morphology-dependent shifts in the resonant frequencies. The shift in the resonant frequency is dependent on the size, shape, and index of refraction of the micro-sphere. A physical change in the environment surrounding a micro-bead can change one or more of these properties of the sphere thereby causing a shift in frequency of resonance. The change of the resonance frequency can be detected with high resolution by scanning a frequency-tunable laser that is coupled into the fiber and observing the transmission spectrum at the output of the fiber. It is expected that, in the future, the measurement concept will lead to a system of distributed micro-sensors providing spatial data resolved in time and space. The present project focuses on the development and demonstration of temperature sensors using the morphology-dependent optical resonances although in the latter part of the work, we will also develop a pressure sensor. During the period covered in this report, the optical and electronic equipment necessary for the experimental work was assembled and the experimental setup was designed for the single sensor temperature measurements. Software was developed for real-time tracking of the optical resonance shifts. Some preliminary experiments were also carried out to detect temperature using a single bead in a water bath.

Micro-optical Distributed Sensors for Aero Propulsion Applications

NASA Technical Reports Server (NTRS)

Arnold, S.; Otugen, V.; Seasholtz, Richard G. (Technical Monitor)

2003-01-01

The objective of this research is to develop micro-opto-mechanical system (MOMS)-based sensors for time- and space-resolved measurements of flow properties in aerodynamics applications. The measurement technique we propose uses optical resonances in dielectric micro-spheres that can be excited by radiation tunneling from optical fibers. It exploits the tunneling-induced and morphology-dependent shifts in the resonant frequencies. The shift in the resonant frequency is dependent on the size, shape, and index of refraction of the micro-sphere. A physical change in the environment surrounding a micro-bead can change one or more of these properties of the sphere thereby causing a shift in frequency of resonance. The change of the resonance frequency can be detected with high resolution by scanning a frequency-tunable laser that is coupled into the fiber and observing the transmission spectrum at the output of the fiber. It is expected that, in the future, the measurement concept will lead to a system of distributed micro-sensors providing spatial data resolved in time and space. The present project focuses on the development and demonstration of temperature sensors using the morphology-dependent optical resonances although in the latter part of the work, we will also develop a pressure sensor. During the period covered in this report, the optical and electronic equipment necessary for the experimental work was assembled and the experimental setup was designed for the single sensor temperature measurements. Software was developed for real-time tracking of the optical resonance shifts. Some preliminary experiments were also carried out to detect temperature using a single bead in a water bath.

Tight-binding model of the photosystem II reaction center: application to two-dimensional electronic spectroscopy

NASA Astrophysics Data System (ADS)

Gelzinis, Andrius; Valkunas, Leonas; Fuller, Franklin D.; Ogilvie, Jennifer P.; Mukamel, Shaul; Abramavicius, Darius

2013-07-01

We propose an optimized tight-binding electron-hole model of the photosystem II (PSII) reaction center (RC). Our model incorporates two charge separation pathways and spatial correlations of both static disorder and fast fluctuations of energy levels. It captures the main experimental features observed in time-resolved two-dimensional (2D) optical spectra at 77 K: peak pattern, lineshapes and time traces. Analysis of 2D spectra kinetics reveals that specific regions of the 2D spectra of the PSII RC are sensitive to the charge transfer states. We find that the energy disorder of two peripheral chlorophylls is four times larger than the other RC pigments.

NMR relaxometry study of cement hydration in the presence of different oxidic fine fraction materials.

PubMed

Nestle, Nikolaus

2004-01-01

NMR relaxometry has been applied to study hydrating cements for about 25 years now. The most important advantage over other experimental approaches is the possibility to conduct non-destructive measurements with a time resolution of minutes. NMR relaxometry data thus can help to identify details in the time course of cement hydration that possibly would be overlooked in other experiments with lower temporal resolution. Time-resolved information on cement hydration kinetics can provide interesting insights into the impact of oxidic additive materials on cement hydration. For PbO, a very strong delay was observed which then was systematically studied. An explanation for this delay is suggested.

Observation of Rayleigh-Taylor-instability evolution in a plasma with magnetic and viscous effects

DOE PAGES

Adams, Colin S.; Moser, Auna L.; Hsu, Scott C.

2015-11-06

We present time-resolved observations of Rayleigh-Taylor-instability (RTI) evolution at the interface between an unmagnetized plasma jet colliding with a stagnated, magnetized plasma. The observed instability growth time (~10μs) is consistent with the estimated linear RTI growth rate calculated using experimentally inferred values of density (~10 14cm–3) and deceleration (~10 9 m/s 2). The observed mode wavelength (≳1 cm) nearly doubles within a linear growth time. Furthermore, theoretical estimates of magnetic and viscous stabilization and idealized magnetohydrodynamic simulations including a physical viscosity model both suggest that the observed instability evolution is subject to magnetic and/or viscous effects.

Assessing the Potential Consequences of Subsurface Bioremediation: Fe-oxide Bioreductive Processes and the Propensity for Contaminant-colloid Co-transport and Media Structural Breakdown

DTIC Science & Technology

2017-05-12

were resolved by a technical approach that included three well-integrated experimental tasks follows: Task A: Quantify the impact of time- dependent ...aggregate breakdown and colloid dispersion depending on the extent of Fe(III) reduction and altered the pore structure and chemical reactivity of the porous...have significant effect on the transport of molecular and colloidal tracers (but not on the ionic tracer Br-) and colloid generation depending on

Joint Aircraft Survivability Program Final Test Report for the Acoustic Fire Suppression Project JASP-TR-14-05

DTIC Science & Technology

2016-09-01

focus of early research was the effects of acoustics on droplet burning in turbine engines and combustion chambers.5,21–23 The results of this... Wire Anemometer. Time-resolved mass readings were made using a model MS4002S Mettler Toledo Precision Balance. 5. Acoustic Extinction This section...nanotube sound projectors. Nanotechnology. 2013;24(23):235501. 40. Hu L, Liu S, Xu Y, Li D. A wind tunnel experimental study on burning rate

Novel portable press for synchrotron time-resolved 3-D micro-imagining under extreme conditions

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

Philippe, J.; Le Godec, Y., E-mail: yann.legodec@impmc.upmc.fr; Bergame, F.

Here we present the instrumental development to extend the synchrotron X-ray microtomography techniques to in situ studies under static compression (HP) or shear stress or the both conditions at high temperatures (HT). To achieve this, a new rotating tomography Paris-Edinburgh cell (rotoPEc) has been developed. This ultra-compact portable device, easily and successfully adapted to various multi-modal synchrotron experimental set-up at ESRF, SOLEIL and DIAMOND is explained in detail.

Super-resolution with an SLM and two intensity images

NASA Astrophysics Data System (ADS)

Alcalá Ochoa, Noé; de León, Y. Ponce

2018-06-01

It is reported a method which may simplify the optical setups used to achieve super-resolution through the amplitude multiplication of two waves. For this end we decompose a super-resolving pupil into two complex masks and with the aid of a Spatial Light Modulator (LCoS) we obtain two intensity images that are subtracted. With this proposal, the traditional experimental optical setups are considerably simplified, with the additional benefit that different masks can be utilized without needing to perform the setup alignment each time.

Computational Aeroacoustic Analysis of Slat Trailing-Edge Flow

NASA Technical Reports Server (NTRS)

Singer, Bart A.; Lockard, David P.; Brentner, Kenneth S.; Khorrami, Mehdi R.; Berkman, Mert E.; Choudhari, Meelan

2000-01-01

An acoustic analysis based on the Ffowcs Williams and Hawkings equation was performed for a high-lift system. As input, the acoustic analysis used un- steady flow data obtained from a highly resolved, time-dependent, Reynolds-averaged Navier-Stokes calculation. The analysis strongly suggests that vor- tex shedding from the trailing edge of the slat results in a high-amplitude, high-frequency acoustic signal, similar to that which was observed in a correspond- ing experimental study of the high-lift system.

Time-resolved confocal fluorescence microscopy: novel technical features and applications for FLIM, FRET and FCS using a sophisticated data acquisition concept in TCSPC

NASA Astrophysics Data System (ADS)

Koberling, Felix; Krämer, Benedikt; Kapusta, Peter; Patting, Matthias; Wahl, Michael; Erdmann, Rainer

2007-05-01

In recent years time-resolved fluorescence measurement and analysis techniques became a standard in single molecule microscopy. However, considering the equipment and experimental implementation they are typically still an add-on and offer only limited possibilities to study the mutual dependencies with common intensity and spectral information. In contrast, we are using a specially designed instrument with an unrestricted photon data acquisition approach which allows to store spatial, temporal, spectral and intensity information in a generalized format preserving the full experimental information. This format allows us not only to easily study dependencies between various fluorescence parameters but also to use, for example, the photon arrival time for sorting and weighting the detected photons to improve the significance in common FCS and FRET analysis schemes. The power of this approach will be demonstrated for different techniques: In FCS experiments the concentration determination accuracy can be easily improved by a simple time-gated photon analysis to suppress the fast decaying background signal. A more detailed analysis of the arrival times allows even to separate FCS curves for species which differ in their fluorescence lifetime but, for example, cannot be distinguished spectrally. In multichromophoric systems like a photonic wire which undergoes unidirectional multistep FRET the lifetime information complements significantly the intensity based analysis and helps to assign the respective FRET partners. Moreover, together with pulsed excitation the time-correlated analysis enables directly to take advantage of alternating multi-colour laser excitation. This pulsed interleaved excitation (PIE) can be used to identify and rule out inactive FRET molecules which cause interfering artefacts in standard FRET efficiency analysis. We used a piezo scanner based confocal microscope with compact picosecond diode lasers as excitation sources. The timing performance can be significantly increased by using new SPAD detectors which enable, in conjunction with new TCSPC electronics, an overall IRF width of less than 120 ps maintaining single molecule sensitivity.

Matter-Radiation Interactions in Extremes

Science.gov Websites

to resolve this capability gap. An experimental explosive is shown igniting during small-scale impact testing. An experimental explosive is shown igniting during small-scale impact testing. Accelerating in to

Adaptive Decomposition of Highly Resolved Time Series into Local and Non‐local Components

EPA Science Inventory

Highly time-resolved air monitoring data are widely being collected over long time horizons in order to characterizeambient and near-source air quality trends. In many applications, it is desirable to split the time-resolved data into two ormore components (e.g., local and region...

Theoretical and experimental analyses of the performance of two-color laser ranging systems

NASA Technical Reports Server (NTRS)

Im, K. E.; Gardner, C. S.

1985-01-01

The statistical properties of the signals reflected from the retroreflector equipped satellites were studied. It is found that coherence interference between pulse reflections from retroreflectors of different ranges on the array platform is the primary cause of signal fluctuations. The performance of a cross-correlation technique to estimate the differential propagation time is analyzed by considering both shot noise and speckle. For the retroreflector arrays, timing performance is dominated by interference induced speckle, and the differential propagation time cannot be resolved to better than the pulse widths of the received signals. The differential timing measurements obtained over a horizontal path are analyzed. The ocean-reflected pulse measurements obtained from the airborne two-color laser altimeter experiment are presented.

Measurement of the Resolution of the Optical Microscope.

ERIC Educational Resources Information Center

Bowlt, C.

1983-01-01

Outlines procedures demonstrating that the aperture of a microscope objective limits resolving power and then, by using ancillary measurements made with a calibrated graticule in the microscope eyepiece, that the experimentally determined value for the maximum resolving power of a given objective is close to the value predicted by theory. (JN)

Unmixing the Materials and Mechanics Contributions in Non-resolved Object Signatures

DTIC Science & Technology

2008-09-01

abundances from hyperspectral or multi-spectral time - resolved signatures. A Fourier analysis of temporal variation of material abundance provides...factorization technique to extract the temporal variation of material abundances from hyperspectral or multi-spectral time - resolved signatures. A Fourier...approximately one hundred wavelengths in the visible spectrum. The frame rate for the instrument was not large enough to collect time resolved data. However

A hierarchy of models for simulating experimental results from a 3D heterogeneous porous medium

NASA Astrophysics Data System (ADS)

Vogler, Daniel; Ostvar, Sassan; Paustian, Rebecca; Wood, Brian D.

2018-04-01

In this work we examine the dispersion of conservative tracers (bromide and fluorescein) in an experimentally-constructed three-dimensional dual-porosity porous medium. The medium is highly heterogeneous (σY2 = 5.7), and consists of spherical, low-hydraulic-conductivity inclusions embedded in a high-hydraulic-conductivity matrix. The bimodal medium was saturated with tracers, and then flushed with tracer-free fluid while the effluent breakthrough curves were measured. The focus for this work is to examine a hierarchy of four models (in the absence of adjustable parameters) with decreasing complexity to assess their ability to accurately represent the measured breakthrough curves. The most information-rich model was (1) a direct numerical simulation of the system in which the geometry, boundary and initial conditions, and medium properties were fully independently characterized experimentally with high fidelity. The reduced-information models included; (2) a simplified numerical model identical to the fully-resolved direct numerical simulation (DNS) model, but using a domain that was one-tenth the size; (3) an upscaled mobile-immobile model that allowed for a time-dependent mass-transfer coefficient; and, (4) an upscaled mobile-immobile model that assumed a space-time constant mass-transfer coefficient. The results illustrated that all four models provided accurate representations of the experimental breakthrough curves as measured by global RMS error. The primary component of error induced in the upscaled models appeared to arise from the neglect of convection within the inclusions. We discuss the necessity to assign value (via a utility function or other similar method) to outcomes if one is to further select from among model options. Interestingly, these results suggested that the conventional convection-dispersion equation, when applied in a way that resolves the heterogeneities, yields models with high fidelity without requiring the imposition of a more complex non-Fickian model.

Thermal Diffusivity Measurements in Edible Oils using Transient Thermal Lens

NASA Astrophysics Data System (ADS)

Valdez, R. Carbajal.; Pérez, J. L. Jiménez.; Cruz-Orea, A.; Martín-Martínez, E. San.

2006-11-01

Time resolved thermal lens (TL) spectrometry is applied to the study of the thermal diffusivity of edible oils such as olive, and refined and thermally treated avocado oils. A two laser mismatched-mode experimental configuration was used, with a He Ne laser as a probe beam and an Ar+ laser as the excitation one. The characteristic time constant of the transient thermal lens was obtained by fitting the experimental data to the theoretical expression for a transient thermal lens. The results showed that virgin olive oil has a higher thermal diffusivity than for refined and thermally treated avocado oils. This measured thermal property may contribute to a better understanding of the quality of edible oils, which is very important in the food industry. The thermal diffusivity results for virgin olive oil, obtained from this technique, agree with those reported in the literature.

On turbulence decay of a shear-thinning fluid

NASA Astrophysics Data System (ADS)

Rahgozar, S.; Rival, D. E.

2017-12-01

An experimental investigation of turbulent flow in a shear-thinning fluid is presented. The experimental flow is a boundary-free, uniformly sheared flow at a relatively high Reynolds number (i.e., Re λmax=275 ), which decays in time. As just one example of decaying turbulence, the experiment can be thought of as a simple model of bulk turbulence in large arteries. The dimensionless parameters used are Reynolds, Strouhal, and Womersley numbers, which have been adapted according to the characteristics of the present experiment. The working fluid is a solution of aqueous 35 ppm xanthan gum, a well-known shear-thinning fluid. The velocity fields are acquired via time-resolved particle image velocimetry in the streamwise/cross-stream and streamwise/spanwise planes. The results show that the presence of xanthan gum not only modifies the turbulent kinetic energy and the dissipation rate but also significantly alters the characteristics of the large-scale eddies.

Generation and Evolution of High-Mach-Number Laser-Driven Magnetized Collisionless Shocks in the Laboratory.

PubMed

Schaeffer, D B; Fox, W; Haberberger, D; Fiksel, G; Bhattacharjee, A; Barnak, D H; Hu, S X; Germaschewski, K

2017-07-14

We present the first laboratory generation of high-Mach-number magnetized collisionless shocks created through the interaction of an expanding laser-driven plasma with a magnetized ambient plasma. Time-resolved, two-dimensional imaging of plasma density and magnetic fields shows the formation and evolution of a supercritical shock propagating at magnetosonic Mach number M_{ms}≈12. Particle-in-cell simulations constrained by experimental data further detail the shock formation and separate dynamics of the multi-ion-species ambient plasma. The results show that the shocks form on time scales as fast as one gyroperiod, aided by the efficient coupling of energy, and the generation of a magnetic barrier between the piston and ambient ions. The development of this experimental platform complements present remote sensing and spacecraft observations, and opens the way for controlled laboratory investigations of high-Mach number collisionless shocks, including the mechanisms and efficiency of particle acceleration.

Angular distribution of ions and extreme ultraviolet emission in laser-produced tin droplet plasma

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

Chen, Hong; Duan, Lian; Lan, Hui

Angular-resolved ion time-of-flight spectra as well as extreme ultraviolet radiation in laser-produced tin droplet plasma are investigated experimentally and theoretically. Tin droplets with a diameter of 150 μm are irradiated by a pulsed Nd:YAG laser. The ion time-of-flight spectra measured from the plasma formed by laser irradiation of the tin droplets are interpreted in terms of a theoretical elliptical Druyvesteyn distribution to deduce ion density distributions including kinetic temperatures of the plasma. The opacity of the plasma for extreme ultraviolet radiation is calculated based on the deduced ion densities and temperatures, and the angular distribution of extreme ultraviolet radiation is expressedmore » as a function of the opacity using the Beer–Lambert law. Our results show that the calculated angular distribution of extreme ultraviolet radiation is in satisfactory agreement with the experimental data.« less

Communication: Electron ionization of DNA bases

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

Rahman, M. A.; Krishnakumar, E., E-mail: ekkumar@tifr.res.in

2016-04-28

No reliable experimental data exist for the partial and total electron ionization cross sections for DNA bases, which are very crucial for modeling radiation damage in genetic material of living cell. We have measured a complete set of absolute partial electron ionization cross sections up to 500 eV for DNA bases for the first time by using the relative flow technique. These partial cross sections are summed to obtain total ion cross sections for all the four bases and are compared with the existing theoretical calculations and the only set of measured absolute cross sections. Our measurements clearly resolve themore » existing discrepancy between the theoretical and experimental results, thereby providing for the first time reliable numbers for partial and total ion cross sections for these molecules. The results on fragmentation analysis of adenine supports the theory of its formation in space.« less

Angular distribution of ions and extreme ultraviolet emission in laser-produced tin droplet plasma

NASA Astrophysics Data System (ADS)

Chen, Hong; Wang, Xinbing; Duan, Lian; Lan, Hui; Chen, Ziqi; Zuo, Duluo; Lu, Peixiang

2015-05-01

Angular-resolved ion time-of-flight spectra as well as extreme ultraviolet radiation in laser-produced tin droplet plasma are investigated experimentally and theoretically. Tin droplets with a diameter of 150 μm are irradiated by a pulsed Nd:YAG laser. The ion time-of-flight spectra measured from the plasma formed by laser irradiation of the tin droplets are interpreted in terms of a theoretical elliptical Druyvesteyn distribution to deduce ion density distributions including kinetic temperatures of the plasma. The opacity of the plasma for extreme ultraviolet radiation is calculated based on the deduced ion densities and temperatures, and the angular distribution of extreme ultraviolet radiation is expressed as a function of the opacity using the Beer-Lambert law. Our results show that the calculated angular distribution of extreme ultraviolet radiation is in satisfactory agreement with the experimental data.

In-situ material-motion diagnostics and fuel radiography in experimental reactors

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

DeVolpi, A.

1982-01-01

Material-motion monitoring has become a routine part of in-pile transient reactor-safety experiments. Diagnostic systems, such as the fast-neutron hodoscope, were developed for the purpose of providing direct time-resolved data on pre-failure fuel motion, cladding-breach time and location, and post-failure fuel relocation. Hodoscopes for this purpose have been installed at TREAT and CABRI; other types of imaging systems that have been tested are a coded-aperture at ACRR and a pinhole at TREAT. Diagnostic systems that use penetrating radiation emitted from the test section can non-invasively monitor fuel without damage to the measuring instrument during the radiographic images of test sections installedmore » in the reator. Studies have been made of applications of hodoscopes to other experimental reactors, including PBF, FARET, STF, ETR, EBR-II, SAREF-STF, and DMT.« less

Laser Blow-Off Impurity Injection Experiments at the HSX Stellarator

NASA Astrophysics Data System (ADS)

Castillo, J. F.; Bader, A.; Likin, K. M.; Anderson, D. T.; Anderson, F. S. B.; Kumar, S. T. A.; Talmadge, J. N.

2017-10-01

Results from the HSX laser blow-off experiment are presented and compared to a synthetic diagnostic implemented in the STRAHL impurity transport modeling code in order to measure the impurity transport diffusivity and convective velocity. A laser blow-off impurity injection system is used to rapidly deposit a small, controlled quantity of aluminum into the confinement volume. Five AXUV photodiode arrays are used to take time-resolved measurements of the impurity radiation. The spatially one-dimensional impurity transport code STRAHL is used to calculate a time-dependent plasma emissivity profile. Modeled intensity signals calculated from a synthetic diagnostic code provide direct comparison between plasma simulation and experimental results. An optimization algorithm with impurity transport coefficients acting as free parameters is used to fit the model to experimental data. This work is supported by US DOE Grant DE-FG02-93ER54222.

Watching ultrafast responses of structure and magnetism in condensed matter with momentum-resolved probes

PubMed Central

Johnson, S. L.; Savoini, M.; Beaud, P.; Ingold, G.; Staub, U.; Carbone, F.; Castiglioni, L.; Hengsberger, M.; Osterwalder, J.

2017-01-01

We present a non-comprehensive review of some representative experimental studies in crystalline condensed matter systems where the effects of intense ultrashort light pulses are probed using x-ray diffraction and photoelectron spectroscopy. On an ultrafast (sub-picosecond) time scale, conventional concepts derived from the assumption of thermodynamic equilibrium must often be modified in order to adequately describe the time-dependent changes in material properties. There are several commonly adopted approaches to this modification, appropriate in different experimental circumstances. One approach is to treat the material as a collection of quasi-thermal subsystems in thermal contact with each other in the so-called “N-temperature” models. On the other extreme, one can also treat the time-dependent changes as fully coherent dynamics of a sometimes complex network of excitations. Here, we present examples of experiments that fall into each of these categories, as well as experiments that partake of both models. We conclude with a discussion of the limitations and future potential of these concepts. PMID:29308418

An experimental study of high-pressure droplet combustion

NASA Technical Reports Server (NTRS)

Norton, Chris M.; Litchford, Ron J.; Jeng, San-Mou

1990-01-01

The results are presented of an experimental study on suspended n-heptane droplet combustion in air for reduced pressures up to P(r) = 2.305. Transition to fully transient heat-up through the critical state is demonstrated above a threshold pressure corresponding to P(r) of roughly 1.4. A silhouette imaging technique resolves the droplet surface for reduced pressures up to about P(r) roughly 0.63, but soot formation conceals the surface at higher pressures. Images of the soot plumes do not show any sudden change in behavior indicative of critical transition. Mean burning rate constants are computed from the d-squared variation law using measured effective droplet diameters at ignition and measured burn times, and corrected burning times are computed for an effective initial droplet diameter. The results show that the burning rates increase as the fuel critical pressure is approached and decrease as the pressure exceeds the fuel critical pressure. Corrected burning times show inverse behavior.

Experimental and theoretical investigation of radiation and dynamics properties in laser-produced carbon plasmas

NASA Astrophysics Data System (ADS)

Min, Qi; Su, Maogen; Wang, Bo; Cao, Shiquan; Sun, Duixiong; Dong, Chenzhong

2018-05-01

The radiation and dynamics properties of laser-produced carbon plasma in vacuum were studied experimentally with aid of a spatio-temporally resolved emission spectroscopy technique. In addition, a radiation hydrodynamics model based on the fluid dynamic equations and the radiative transfer equation was presented, and calculation of the charge states was performed within the time-dependent collisional radiative model. Detailed temporal and spatial evolution behavior about plasma parameters have been analyzed, such as velocity, electron temperature, charge state distribution, energy level population, and various atomic processes. At the same time, the effects of different atomic processes on the charge state distribution were examined. Finally, the validity of assuming a local thermodynamic equilibrium in the carbon plasma expansion was checked, and the results clearly indicate that the assumption was valid only at the initial (<80 ns) stage of plasma expansion. At longer delay times, it was not applicable near the plasma boundary because of a sharp drop of plasma temperature and electron density.

Spectroscopic characterization of III-V semiconductor nanomaterials

NASA Astrophysics Data System (ADS)

Crankshaw, Shanna Marie

III-V semiconductor materials form a broad basis for optoelectronic applications, including the broad basis of the telecom industry as well as smaller markets for high-mobility transistors. In a somewhat analogous manner as the traditional silicon logic industry has so heavily depended upon process manufacturing development, optoelectronics often relies instead on materials innovations. This thesis focuses particularly on III-V semiconductor nanomaterials, detailed characterization of which is invaluable for translating the exhibited behavior into useful applications. Specifically, the original research described in these thesis chapters is an investigation of semiconductors at a fundamental materials level, because the nanostructures in which they appear crystallize in quite atypical forms for the given semiconductors. Rather than restricting the experimental approaches to any one particular technique, many different types of optical spectroscopies are developed and applied where relevant to elucidate the connection between the crystalline structure and exhibited properties. In the first chapters, for example, a wurtzite crystalline form of the prototypical zincblende III-V binary semiconductor, GaAs, is explored through polarization-dependent Raman spectroscopy and temperature-dependent photoluminescence, as well as second-harmonic generation (SHG). The altered symmetry properties of the wurtzite crystalline structure are particularly evident in the Raman and SHG polarization dependences, all within a bulk material realm. A rather different but deeply elegant aspect of crystalline symmetry in GaAs is explored in a separate study on zincblende GaAs samples quantum-confined in one direction, i.e. quantum well structures, whose quantization direction corresponds to the (110) direction. The (110) orientation modifies the low-temperature electron spin relaxation mechanisms available compared to the usual (001) samples, leading to altered spin coherence times explored through a novel spectroscopic technique first formulated for the rather different purpose of dispersion engineering for slow-light schemes. The frequency-resolved technique combined with the unusual (110) quantum wells in a furthermore atypical waveguide experimental geometry has revealed fascinating behavior of electron spin splitting which points to the possibility of optically orienting electron spins with linearly polarized light---an experimental result supporting a theoretical description of the phenomenon itself only a few years old. Lastly, to explore a space of further-restricted dimensionality, the final chapters describe InP semiconductor nanowires with dimensions small enough to be considered truly one-dimensional. Like the bulk GaAs of the first few chapters, the InP nanowires here crystallize in a wurtzite structure. In the InP nanowire case, though, the experimental techniques explored for characterization are temperature-dependent time-integrated photoluminescence at the single-wire level (including samples with InAsP insertions) and time-resolved photoluminescence at the ensemble level. The carrier dynamics revealed through these time-resolved studies are the first of their kind for wurtzite InP nanowires. The chapters are thus ordered as a progression from three (bulk), to two (quantum well), to one (nanowire), to zero dimensions (axially-structured nanowire), with the uniting theme the emphasis on connecting the semiconductor nanomaterials' crystallinity to its exhibited properties by relevant experimental spectroscopic techniques, whether these are standard methods or effectively invented for the case at hand.

Time-resolved contrast-enhanced MRA (TWIST) with gadofosveset trisodium in the classification of soft-tissue vascular anomalies in the head and neck in children following updated 2014 ISSVA classification: first report on systematic evaluation of MRI and TWIST in a cohort of 47 children.

PubMed

Higgins, L J; Koshy, J; Mitchell, S E; Weiss, C R; Carson, K A; Huisman, T A G M; Tekes, A

2016-01-01

To evaluate the relative accuracy of contrast-enhanced time-resolved angiography with interleaved stochastic trajectories versus conventional contrast-enhanced magnetic resonance imaging (MRI) following International Society for the Study of Vascular Anomalies updated 2014-based classification of soft-tissue vascular anomalies in the head and neck in children. Time-resolved angiography with interleaved stochastic trajectories versus conventional contrast-enhanced MRI of children with diagnosis of soft-tissue vascular anomalies in the head and neck referred for MRI between 2008 and 2014 were retrospectively reviewed. Forty-seven children (0-18 years) were evaluated. Two paediatric neuroradiologists evaluated time-resolved MRA and conventional MRI in two different sessions (30 days apart). Blood-pool endovascular MRI contrast agent gadofosveset trisodium was used. The present cohort had the following diagnoses: infantile haemangioma (n=6), venous malformation (VM; n=23), lymphatic malformation (LM; n=16), arteriovenous malformation (AVM; n=2). Time-resolved MRA alone accurately classified 38/47 (81%) and conventional MRI 42/47 (89%), respectively. Although time-resolved MRA alone is slightly superior to conventional MRI alone for diagnosis of infantile haemangioma, conventional MRI is slightly better for diagnosis of venous and LMs. Neither time-resolved MRA nor conventional MRI was sufficient for accurate diagnosis of AVM in this cohort. Conventional MRI combined with time-resolved MRA accurately classified 44/47 cases (94%). Time-resolved MRA using gadofosveset trisodium can accurately classify soft-tissue vascular anomalies in the head and neck in children. The addition of time-resolved MRA to existing conventional MRI protocols provides haemodynamic information, assisting the diagnosis of vascular anomalies in the paediatric population at one-third of the dose of other MRI contrast agents. Copyright © 2015 The Royal College of Radiologists. Published by Elsevier Ltd. All rights reserved.

The time-resolved photoelectron spectrum of toluene using a perturbation theory approach

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

Richings, Gareth W.; Worth, Graham A., E-mail: g.a.worth@bham.ac.uk

A theoretical study of the intra-molecular vibrational-energy redistribution of toluene using time-resolved photo-electron spectra calculated using nuclear quantum dynamics and a simple, two-mode model is presented. Calculations have been carried out using the multi-configuration time-dependent Hartree method, using three levels of approximation for the calculation of the spectra. The first is a full quantum dynamics simulation with a discretisation of the continuum wavefunction of the ejected electron, whilst the second uses first-order perturbation theory to calculate the wavefunction of the ion. Both methods rely on the explicit inclusion of both the pump and probe laser pulses. The third method includesmore » only the pump pulse and generates the photo-electron spectrum by projection of the pumped wavepacket onto the ion potential energy surface, followed by evaluation of the Fourier transform of the autocorrelation function of the subsequently propagated wavepacket. The calculations performed have been used to study the periodic population flow between the 6a and 10b16b modes in the S{sub 1} excited state, and compared to recent experimental data. We obtain results in excellent agreement with the experiment and note the efficiency of the perturbation method.« less

Fast, deep record length, time-resolved visible spectroscopy of plasmas using fiber grids

NASA Astrophysics Data System (ADS)

Brockington, Samuel; Case, Andrew; Cruz, Edward; Witherspoon, F. Douglas; Horton, Robert; Klauser, Ruth; Hwang, D. Q.

2016-10-01

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. New solid-state Silicon Photo-Multiplier (SiPM) chips are capable of single photon event detection and high speed data acquisition. By coupling the output of a spectrometer to an imaging fiber bundle connected to a bank of amplified SiPMs, time-resolved spectroscopic imagers of 100 to 1,000 pixels can be constructed. Target pixel performance is 10 Megaframes/sec with record lengths of up to 256,000 frames yielding 25.6 milliseconds of record at10 Megasamples/sec resolution. Pixel resolutions of 8 to 12 bits are pos- sible. Pixel pitch can be refined by using grids of 100 μm to 1000 μm diameter fibers. A 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) as a full demonstration of the concept. Experimental results will be dis-cussed, along with future plans for the Phase 2 project, and potential applications to plasma experiments . Work supported by USDOE SBIR Grant DE-SC0013801.

Silicon drift detectors as a tool for time-resolved fluorescence XAFS on low-concentrated samples in catalysis.

PubMed

Kappen, Peter; Tröger, Larc; Materlik, Gerhard; Reckleben, Christian; Hansen, Karsten; Grunwaldt, Jan-Dierk; Clausen, Bjerne S

2002-07-01

A silicon drift detector (SDD) was used for ex situ and time-resolved in situ fluorescence X-ray absorption fine structure (XAFS) on low-concentrated catalyst samples. For a single-element and a seven-element SDD the energy resolution and the peak-to-background ratio were verified at high count rates, sufficient for fluorescence XAFS. An experimental set-up including the seven-element SDD without any cooling and an in situ cell with gas supply and on-line gas analysis was developed. With this set-up the reduction and oxidation of a zeolite supported catalyst containing 0.3 wt% platinum was followed by fluorescence near-edge scans with a time resolution of 10 min each. From ex situ experiments on low-concentrated platinum- and gold-based catalysts fluorescence XAFS scans could be obtained with sufficient statistical quality for a quantitative analysis. Structural information on the gold and platinum particles could be extracted by both the Fourier transforms and the near-edge region of the XAFS spectra. Moreover, it was found that with the seven-element SDD concentrations of the element of interest as low as 100 ppm can be examined by fluorescence XAFS.

Time-resolved imaging of flyer dynamics for femtosecond laser-induced backward transfer of solid polymer thin films

NASA Astrophysics Data System (ADS)

Feinaeugle, M.; Gregorčič, P.; Heath, D. J.; Mills, B.; Eason, R. W.

2017-02-01

We have studied the transfer regimes and dynamics of polymer flyers from laser-induced backward transfer (LIBT) via time-resolved shadowgraphy. Imaging of the flyer ejection phase of LIBT of 3.8 μm and 6.4 μm thick SU-8 polymer films on germanium and silicon carrier substrates was performed over a time delay range of 1.4-16.4 μs after arrival of the laser pulse. The experiments were carried out with 150 fs, 800 nm pulses spatially shaped using a digital micromirror device, and laser fluences of up to 3.5 J/cm2 while images were recorded via a CCD camera and a spark discharge lamp. Velocities of flyers found in the range of 6-20 m/s, and the intact and fragmented ejection regimes, were a function of donor thickness, carrier and laser fluence. The crater profile of the donor after transfer and the resulting flyer profile indicated different flyer ejection modes for Si carriers and high fluences. The results contribute to better understanding of the LIBT process, and help to determine experimental parameters for successful LIBT of intact deposits.

Time-resolved X-ray Absorption Spectroscopy for Electron Transport Study in Warm Dense Gold

NASA Astrophysics Data System (ADS)

Lee, Jong-Won; Bae, Leejin; Engelhorn, Kyle; Heimann, Philip; Ping, Yuan; Barbrel, Ben; Fernandez, Amalia; Beckwith, Martha Anne; Cho, Byoung-Ick; GIST Team; IBS Team; LBNL Collaboration; SLAC Collaboration; LLNL Collaboration

2015-11-01

The warm dense Matter represents states of which the temperature is comparable to Fermi energy and ions are strongly coupled. One of the experimental techniques to create such state in the laboratory condition is the isochoric heating of thin metal foil with femtosecond laser pulses. This concept largely relies on the ballistic transport of electrons near the Fermi-level, which were mainly studied for the metals in ambient conditions. However, they were barely investigated in warm dense conditions. We present a time-resolved x-ray absorption spectroscopy measured for the Au/Cu dual layered sample. The front Au layer was isochorically heated with a femtosecond laser pulse, and the x-ray absorption changes around L-edge of Cu, which was attached on the backside of Au, was measured with a picosecond resolution. Time delays between the heating of the `front surface' of Au layer and the alternation of x-ray spectrum of Cu attached on the `rear surface' of Au indicate the energetic electron transport mechanism through Au in the warm dense conditions. IBS (IBS-R012-D1) and the NRF (No. 2013R1A1A1007084) of Korea.

Frequency-resolved optical gating with the use of second-harmonic generation

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

DeLong, K.W.; Trebino, R.; Hunter, J.

1994-11-01

We discuss the use of second-harmonic generation (SHG) as the nonlinearity in the technique of frequency-resolved optical gating (FROG) for measuring the full intensity and phase evolution of an arbitrary ultrashort pulse. FROG that uses a third-order nonlinearity in the polarization-gate geometry has proved extremely successful, and the algorithm required for extraction of the intensity and the phase from the experimental data is quite robust. However, for pulse intensities less than [similar to] 1 MW, third-order nonlinearities generate insufficient signal strength, and therefore SHG FROG appears necessary. We discuss the theoretical, algorithmic, and experimental considerations of SHG FROG in detail.more » SHG FROG has an ambiguity in the direction of time, and its traces are somewhat unintuitive. Also, previously published algorithms are generally ineffective at extracting the intensity and the phase of an arbitrary laser pulse from the SHG FROG trace. We present an improved pulse-retrieval algorithm, based on the method of generalized projections, that is far superior to the previously published algorithms, although it is still not so robust as the polarization-gate algorithm. We discuss experimental sources of error such as pump depletion and group-velocity mismatch. We also present several experimental examples of pulses measured with SHG FROG and show that the derived intensities and phases are in agreement with more conventional diagnostic techniques, and we demonstrate the high-dynamic-range capability of SHG FROG. We conclude that, despite the above drawbacks, SHG FROG should be useful in measuring low-energy pulses.« less

Effect of the surface heterogeneity of the stationary phase on the range of concentration for linear chromatography

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

Gritti, Fabrice; Guiochon, Georges A

2005-02-01

The range of sample sizes within which linear chromatographic behavior is achieved in a column depends on the surface heterogeneity of the RPLC adsorbents. Two widely different commercial adsorbents were tested, the end-capped XTerra-C{sub 18} and the non-end-capped Resolve-C{sub 18}. Adsorption isotherm data of caffeine were acquired by frontal analysis. These data were modeled and used to calculate the adsorption energy distribution (AED). This double analysis informs on the degree of surface heterogeneity. The best adsorption isotherm models are the bi-Langmuir and the tetra-Langmuir isotherms for XTerra and Resolve, respectively. Their respective AEDs are bimodal and quadrimodal distributions. This interpretationmore » of the results and the actual presence of a low density of high-energy adsorption sites on Resolve-C{sub 18} were validated by measuring the dependence of the peak retention times on the size of caffeine samples (20-{micro}L volume, concentrations 10, 1, 0.1, 1 x 10{sup -2}, 1 x 10{sup -3}, 1 x 10{sup -4}, and 1 x 10{sup -5} g/L). The experimental chromatograms agree closely with the band profiles calculated from the best isotherms. On Resolve-C{sub 18}, the retention time decreases by 40% when the sample concentration is increased from 1 x 10{sup -5} to 10 g/L. The decrease is only 10% for Xterra-C{sub 18} under the same conditions. The upper limit for linear behavior is 1 x 10{sup -4} g/L for the former adsorbent and 0.01 g/L for the latter. The presence of a few high-energy adsorption sites on Resolve-C{sub 18}, with an adsorption energy 20 kJ/mol larger than that of the low-energy sites while the same difference on Xterra is only 5 kJ/mol, explains this difference. The existence of adsorption sites with a very high energy for certain compounds affects the reproducibility of their retention times and a rapid loss of efficiency in a sample size range within which linear behavior is incorrectly anticipated.« less

Critical evaluation of measured line positions of 14N16O in X2П state

NASA Astrophysics Data System (ADS)

Sulakshina, O. N.; Borkov, Yu. G.

2018-04-01

All available line positions for unresolved and resolved Λ-doublets of the 14N16O molecule in the X2 П state were collected from the literature and tested using the RITZ computer code. These data have been critically analysed and used to obtain the most complete set of 1789 experimental energy levels of unresolved Λ-doublets covering the 0-35,866 cm-1 interval. A set of 425 experimental energy levels of resolved Λ-doublets covering the 0-5957 cm-1 interval for two states 2П1/2 and 2П3/2 also have been obtained. These levels together with calculated correlation matrix can be used to generate the precise list of transitions with confidence intervals. Comparisons with the HITRAN as well as with Amiot calculations are discussed. The systematic shift between experimental energy levels of unresolved Λ-doublets and those calculated by Amiot for 2П3/2 state was found. The same systematic shift for transitions frequencies of unresolved Λ-doublets in forbidden subbands 2П1/2↔2П3/2 is also established in the HITRAN database. Comparison of the RITZ energy levels with calculated energy levels by Wong at al. was also done. It was found, that experimental RITZ energy levels for resolved Λ-doublets of 14N16O coincide with those calculated by Wong at al. within experimental uncertainties.

Experimental measurement of spatially resolved electron density in a filament of a pulsed positive streamer discharge in water

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

Wen, Xiao Qiong; Niu, Zhi Wen; Ren, Chun-Sheng

2015-06-29

By combining a high-speed frame camera with a monochromator, the spatially resolved optical emission spectrum of hydrogen α line in a single filament of a pulsed positive streamer discharge in water has been experimentally measured. The spatially resolved electron densities in a single filament of a pulsed positive streamer discharge in water with a conductivity of 200 μS/cm were investigated. During the experiment, the average energy per pulse of discharge was 90.6 ± 13.6 mJ. The results show that the electron density in the streamer filament is 10{sup 17–18}/cm{sup 3}, and present a decreasing tendency along the axial direction of the streamer filamentmore » with increasing distance from the tip of the anode.« less

First spatial separation of a heavy ion isomeric beam with a multiple-reflection time-of-flight mass spectrometer

NASA Astrophysics Data System (ADS)

Dickel, T.; Plaß, W. R.; Ayet San Andres, S.; Ebert, J.; Geissel, H.; Haettner, E.; Hornung, C.; Miskun, I.; Pietri, S.; Purushothaman, S.; Reiter, M. P.; Rink, A.-K.; Scheidenberger, C.; Weick, H.; Dendooven, P.; Diwisch, M.; Greiner, F.; Heiße, F.; Knöbel, R.; Lippert, W.; Moore, I. D.; Pohjalainen, I.; Prochazka, A.; Ranjan, M.; Takechi, M.; Winfield, J. S.; Xu, X.

2015-05-01

211Po ions in the ground and isomeric states were produced via 238U projectile fragmentation at 1000 MeV/u. The 211Po ions were spatially separated in flight from the primary beam and other reaction products by the fragment separator FRS. The ions were energy-bunched, slowed-down and thermalized in a gas-filled cryogenic stopping cell (CSC). They were then extracted from the CSC and injected into a high-resolution multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). The excitation energy of the isomer and, for the first time, the isomeric-to-ground state ratio were determined from the measured mass spectrum. In the subsequent experimental step, the isomers were spatially separated from the ions in the ground state by an ion deflector and finally collected with a silicon detector for decay spectroscopy. This pioneering experimental result opens up unique perspectives for isomer-resolved studies. With this versatile experimental method new isomers with half-lives longer than a few milliseconds can be discovered and their decay properties can be measured with highest sensitivity and selectivity. These experiments can be extended to studies with isomeric beams in nuclear reactions.

Contrast-enhanced time-resolved MRA for follow-up of intracranial aneurysms treated with the pipeline embolization device.

PubMed

Boddu, S R; Tong, F C; Dehkharghani, S; Dion, J E; Saindane, A M

2014-01-01

Endovascular reconstruction and flow diversion by using the Pipeline Embolization Device is an effective treatment for complex cerebral aneurysms. Accurate noninvasive alternatives to DSA for follow-up after Pipeline Embolization Device treatment are desirable. This study evaluated the accuracy of contrast-enhanced time-resolved MRA for this purpose, hypothesizing that contrast-enhanced time-resolved MRA will be comparable with DSA and superior to 3D-TOF MRA. During a 24-month period, 37 Pipeline Embolization Device-treated intracranial aneurysms in 26 patients underwent initial follow-up by using 3D-TOF MRA, contrast-enhanced time-resolved MRA, and DSA. MRA was performed on a 1.5T unit by using 3D-TOF and time-resolved imaging of contrast kinetics. All patients underwent DSA a median of 0 days (range, 0-68) after MRA. Studies were evaluated for aneurysm occlusion, quality of visualization of the reconstructed artery, and measurable luminal diameter of the Pipeline Embolization Device, with DSA used as the reference standard. The sensitivity, specificity, and positive and negative predictive values of contrast-enhanced time-resolved MRA relative to DSA for posttreatment aneurysm occlusion were 96%, 85%, 92%, and 92%. Contrast-enhanced time-resolved MRA demonstrated superior quality of visualization (P = .0001) and a higher measurable luminal diameter (P = .0001) of the reconstructed artery compared with 3D-TOF MRA but no significant difference compared with DSA. Contrast-enhanced time-resolved MRA underestimated the luminal diameter of the reconstructed artery by 0.965 ± 0.497 mm (27% ± 13%) relative to DSA. Contrast-enhanced time-resolved MRA is a reliable noninvasive method for monitoring intracranial aneurysms following flow diversion and vessel reconstruction by using the Pipeline Embolization Device. © 2014 by American Journal of Neuroradiology.

Detection of bacterial endospores by means of ultrafast coherent Raman spectroscopy

NASA Astrophysics Data System (ADS)

Pestov, Dmitry Sergeyevich

This work is devoted to formulation and development of a laser spectroscopic technique for rapid detection of biohazards, such as Bacillus anthracis spores. Coherent anti-Stokes Raman scattering (CARS) is used as an underlying process for active retrieval of species-specific characteristics of an analyte. Vibrational modes of constituent molecules are Raman-excited by a pair of ultrashort, femtosecond laser pulses, and then probed through inelastic scattering of a third, time-delayed laser field. We first employ the already known time-resolved CARS technique. We apply it to the spectroscopy of easy-to-handle methanol-water mixtures, and then continue building our expertise on solutions of dipicolinic acid (DPA) and its salts, which happen to be marker molecules for bacterial spores. Various acquisition schemes are evaluated, and the preference is given to multi-channel frequency-resolved detection, when the whole CARS spectrum is recorded as a function of the probe pulse delay. We demonstrate a simple detection algorithm that manages to differentiate DPA solution from common interferents. We investigate experimentally the advantages and disadvantages of near-resonant probing of the excited molecular coherence, and finally observe the indicative backscattered CARS signal from DPA and NaDPA powders. The possibility of selective Raman excitation via pulse shaping of the preparation pulses is also demonstrated. The analysis of time-resolved CARS experiments on powders and B. subtilis spores, a harmless surrogate for B. anthracis, facilitates the formulation of a new approach, where we take full advantage of the multi-channel frequency-resolved acquisition and spectrally discriminate the Raman-resonant CARS signal from the background due to other instantaneous four-wave mixing (FWM) processes. Using narrowband probing, we decrease the magnitude of the nonresonant FWM, which is further suppressed by the timing of the laser pulses. The devised technique, referred to as hybrid CARS, leads to a single-shot detection of as few as 104 bacterial spores, bringing CARS spectroscopy to the forefront of potential candidates for real-time biohazard detection. It also gives promise to many other applications of CARS, hindered so far by the presence of the overwhelming nonresonant FWM background, mentioned above.

Spectrally resolved single-molecule electrometry

NASA Astrophysics Data System (ADS)

Ruggeri, F.; Krishnan, M.

2018-03-01

Escape-time electrometry is a recently developed experimental technique that offers the ability to measure the effective electrical charge of a single biomolecule in solution with sub-elementary charge precision. The approach relies on measuring the average escape-time of a single charged macromolecule or molecular species transiently confined in an electrostatic fluidic trap. Comparing the experiments with the predictions of a mean-field model of molecular electrostatics, we have found that the measured effective charge even reports on molecular conformation, e.g., folded or disordered state, and non-uniform charge distribution in disordered proteins or polyelectrolytes. Here we demonstrate the ability to use the spectral dimension to distinguish minute differences in electrical charge between individual molecules or molecular species in a single simultaneous measurement, under identical experimental conditions. Using one spectral channel for referenced measurement, this kind of photophysical distinguishability essentially eliminates the need for accurate knowledge of key experimental parameters, otherwise obtained through intensive characterization of the experimental setup. As examples, we demonstrate the ability to detect small differences (˜5%) in the length of double-stranded DNA fragments as well as single amino acid exchange in an intrinsically disordered protein, prothymosin α.

Spectral measurements of asymmetrically irradiated capsule backlighters

DOE PAGES

Keiter, P. A.; Drake, R. P.

2016-09-09

Capsule backlighters provide a quasi-continuum x-ray spectrum over a wide range of photon energies. Ideally one irradiates the capsule backlighter symmetrically, however, in complex experimental geometries, this is not always possible. In recent experiments we irradiated capsule backlighters asymmetrically and measured the x-ray spectrum from multiple directions. We will present time-integrated spectra over the photon energy range of ~2-13 keV and time-resolved spectra over the photon energy range of ~2-3 keV. Lastly, we will compare the spectra from different lines of sight to determine if the laser asymmetry results in an angular dependence in the x-ray emission.

Experimental radiative lifetimes, branching fractions, and oscillator strengths of some levels in Co I

NASA Astrophysics Data System (ADS)

Wang, Xinghao; Yu, Qi; Li, Qiu; Gao, Yang; Dai, Zhenwen

2018-04-01

The radiative lifetime measurements by the time-resolved laser-induced fluorescence technique are reported for 24 levels of Co I with the energy range of 283 45.86-55 922.3 cm-1, amongst which the lifetimes of 20 levels are reported for the first time. The branching fraction measurements by the emission spectrum of a hollow cathode lamp were performed for 11 levels of them together with other two levels reported in the literature, and branching fractions of 39 transitions were obtained. By combining them with lifetime values, the transition probabilities and absolute oscillator strengths of these lines were determined.

First spin-resolved electron distributions in crystals from combined polarized neutron and X-ray diffraction experiments.

PubMed

Deutsch, Maxime; Gillon, Béatrice; Claiser, Nicolas; Gillet, Jean-Michel; Lecomte, Claude; Souhassou, Mohamed

2014-05-01

Since the 1980s it has been possible to probe crystallized matter, thanks to X-ray or neutron scattering techniques, to obtain an accurate charge density or spin distribution at the atomic scale. Despite the description of the same physical quantity (electron density) and tremendous development of sources, detectors, data treatment software etc., these different techniques evolved separately with one model per experiment. However, a breakthrough was recently made by the development of a common model in order to combine information coming from all these different experiments. Here we report the first experimental determination of spin-resolved electron density obtained by a combined treatment of X-ray, neutron and polarized neutron diffraction data. These experimental spin up and spin down densities compare very well with density functional theory (DFT) calculations and also confirm a theoretical prediction made in 1985 which claims that majority spin electrons should have a more contracted distribution around the nucleus than minority spin electrons. Topological analysis of the resulting experimental spin-resolved electron density is also briefly discussed.

Experimental Constraints of the Exotic Shearing of Space-Time

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

Richardson, Jonathan William

2016-08-01

The Holometer program is a search for rst experimental evidence that space-time has quantum structure. The detector consists of a pair of co-located 40-m power-recycled interferometers whose outputs are read out synchronously at 50 MHz, achieving sensitivity to spatiallycorrelated uctuations in dierential position on time scales shorter than the light-crossing time of the instruments. Unlike gravitational wave interferometers, which time-resolve transient geometrical disturbances in the spatial background, the Holometer is searching for a universal, stationary quantization noise of the background itself. This dissertation presents the nal results of the Holometer Phase I search, an experiment congured for sensitivity to exoticmore » coherent shearing uctuations of space-time. Measurements of high-frequency cross-spectra of the interferometer signals obtain sensitivity to spatially-correlated eects far exceeding any previous measurement, in a broad frequency band extending to 7.6 MHz, twice the inverse light-crossing time of the apparatus. This measurement is the statistical aggregation of 2.1 petabytes of 2-byte dierential position measurements obtained over a month-long exposure time. At 3 signicance, it places an upper limit on the coherence scale of spatial shear two orders of magnitude below the Planck length. The result demonstrates the viability of this novel spatially-correlated interferometric detection technique to reach unprecedented sensitivity to coherent deviations of space-time from classicality, opening the door for direct experimental tests of theories of relational quantum gravity.« less

Anisotropy enhanced X-ray scattering from solvated transition metal complexes

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

Biasin, Elisa; van Driel, Tim B.; Levi, Gianluca

Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolvedmore » X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. Here it is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute,i.e.the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.« less

Time-dependent, x-ray spectral unfolds and brightness temperatures for intense Li{sup +} ion beam-driven hohlraums

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

Fehl, D.L.; Chandler, G.A.; Biggs, F.

X-ray-producing hohlraums are being studied as indirect drives for inertial confinement fusion targets. In a 1994 target series on the PBFAII accelerator, cylindrical hohlraum targets were heated by an intense Li{sup +} ion beam and viewed by an array of 13 time-resolved, filtered x-ray detectors (XRDs). The unfold operator (UFO) code and its suite of auxiliary functions were used extensively in obtaining time-resolved x-ray spectra and radiation temperatures from this diagnostic. The UFO was also used to obtain fitted response functions from calibration data, to simulate data from blackbody x-ray spectra of interest, to determine the suitability of various unfoldingmore » parameters (e.g., energy domain, energy partition, smoothing conditions, and basis functions), to interpolate the XRD signal traces, and to unfold experimental data. The simulation capabilities of the code were useful in understanding an anomalous feature in the unfolded spectra at low photon energies ({le}100 eV). Uncertainties in the differential and energy-integrated unfolded spectra were estimated from uncertainties in the data. The time{endash}history of the radiation temperature agreed well with independent calculations of the wall temperature in the hohlraum. {copyright} {ital 1997 American Institute of Physics.}« less

Acoustically regulated optical emission dynamics from quantum dot-like emission centers in GaN/InGaN nanowire heterostructures

NASA Astrophysics Data System (ADS)

Lazić, S.; Chernysheva, E.; Hernández-Mínguez, A.; Santos, P. V.; van der Meulen, H. P.

2018-03-01

We report on experimental studies of the effects induced by surface acoustic waves on the optical emission dynamics of GaN/InGaN nanowire quantum dots. We employ stroboscopic optical excitation with either time-integrated or time-resolved photoluminescence detection. In the absence of the acoustic wave, the emission spectra reveal signatures originated from the recombination of neutral exciton and biexciton confined in the probed nanowire quantum dot. When the nanowire is perturbed by the propagating acoustic wave, the embedded quantum dot is periodically strained and its excitonic transitions are modulated by the acousto-mechanical coupling. Depending on the recombination lifetime of the involved optical transitions, we can resolve acoustically driven radiative processes over time scales defined by the acoustic cycle. At high acoustic amplitudes, we also observe distortions in the transmitted acoustic waveform, which are reflected in the time-dependent spectral response of our sensor quantum dot. In addition, the correlated intensity oscillations observed during temporal decay of the exciton and biexciton emission suggest an effect of the acoustic piezoelectric fields on the quantum dot charge population. The present results are relevant for the dynamic spectral and temporal control of photon emission in III-nitride semiconductor heterostructures.

Anisotropy enhanced X-ray scattering from solvated transition metal complexes

DOE PAGES

Biasin, Elisa; van Driel, Tim B.; Levi, Gianluca; ...

2018-02-13

Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolvedmore » X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. Here it is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute,i.e.the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.« less

Vibrational population relaxation of carbon monoxide in the heme pocket of photolyzed carbonmonoxy myoglobin: Comparison of time-resolved mid-IR absorbance experiments and molecular dynamics simulations

PubMed Central

Sagnella, Diane E.; Straub, John E.; Jackson, Timothy A.; Lim, Manho; Anfinrud, Philip A.

1999-01-01

The vibrational energy relaxation of carbon monoxide in the heme pocket of sperm whale myoglobin was studied by using molecular dynamics simulation and normal mode analysis methods. Molecular dynamics trajectories of solvated myoglobin were run at 300 K for both the δ- and ɛ-tautomers of the distal His-64. Vibrational population relaxation times of 335 ± 115 ps for the δ-tautomer and 640 ± 185 ps for the ɛ-tautomer were estimated by using the Landau–Teller model. Normal mode analysis was used to identify those protein residues that act as the primary “doorway” modes in the vibrational relaxation of the oscillator. Although the CO relaxation rates in both the ɛ- and δ-tautomers are similar in magnitude, the simulations predict that the vibrational relaxation of the CO is faster in the δ-tautomer with the distal His playing an important role in the energy relaxation mechanism. Time-resolved mid-IR absorbance measurements were performed on photolyzed carbonmonoxy hemoglobin (Hb13CO). From these measurements, a T1 time of 600 ± 150 ps was determined. The simulation and experimental estimates are compared and discussed. PMID:10588704

The 700-1500 cm{sup −1} region of the S{sub 1} (A{sup ~1}B{sub 2}) state of toluene studied with resonance-enhanced multiphoton ionization (REMPI), zero-kinetic-energy (ZEKE) spectroscopy, and time-resolved slow-electron velocity-map imaging (tr-SEVI) spectroscopy

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

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

We report (nanosecond) resonance-enhanced multiphoton ionization (REMPI), (nanosecond) zero-kinetic-energy (ZEKE) and (picosecond) time-resolved slow-electron velocity map imaging (tr-SEVI) spectra of fully hydrogenated toluene (Tol-h{sub 8}) and the deuterated-methyl group isotopologue (α{sub 3}-Tol-d{sub 3}). Vibrational assignments are made making use of the activity observed in the ZEKE and tr-SEVI spectra, together with the results from quantum chemical and previous experimental results. Here, we examine the 700–1500 cm{sup −1} region of the REMPI spectrum, extending our previous work on the region ≤700 cm{sup −1}. We provide assignments for the majority of the S{sub 1} and cation bands observed, and in particular wemore » gain insight regarding a number of regions where vibrations are coupled via Fermi resonance. We also gain insight into intramolecular vibrational redistribution in this molecule.« less

Time resolved interferometric study of the plasma plume induced shock wave in confined geometry: Two-dimensional mapping of the ambient and plasma density

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

Choudhury, Kaushik; Singh, R. K.; Kumar, Ajai, E-mail: ajai@ipr.res.in

2016-04-15

An experimental investigation of the laser produced plasma induced shock wave in the presence of confining walls placed along the axial as well as the lateral direction has been performed. A time resolved Mach Zehnder interferometer is set up to track the primary as well as the reflected shock waves and its effect on the evolving plasma plume has been studied. An attempt has been made to discriminate the electronic and medium density contributions towards the changes in the refractive index of the medium. Two dimensional spatial distributions for both ambient medium density and plasma density (electron density) have beenmore » obtained by employing customised inversion technique and algorithm on the recorded interferograms. The observed density pattern of the surrounding medium in the presence of confining walls is correlated with the reflected shock wave propagation in the medium. Further, the shock wave plasma interaction and the subsequent changes in the shape and density of the plasma plume in confined geometry are briefly described.« less

Time- and space-resolved light emission and spectroscopic research of the flashover plasma

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

Gleizer, J. Z.; Krasik, Ya. E.; Leopold, J.

2015-02-21

The results of an experimental study of the evolution of surface flashover across the surface of an insulator in vacuum subject to a high-voltage pulse and the parameters of the flashover plasma are reported. For the system studied, flashover is always initiated at the cathode triple junctions. Using time-resolved framing photography of the plasma light emission the velocity of the light emission propagation along the surface of the insulator was found to be ∼2.5·10{sup 8} cm/s. Spectroscopic measurements show that the flashover is characterized by a plasma density of 2–4 × 10{sup 14} cm{sup −3} and neutral and electron temperatures of 2–4 eV and 1–3 eV,more » respectively, corresponding to a plasma conductivity of ∼0.2 Ω{sup −1} cm{sup −1} and a discharge current density of up to ∼10 kA/cm{sup 2}.« less

Increasing the intensity of an induction accelerator and reduction of the beam breakup instability

NASA Astrophysics Data System (ADS)

Coleman, J. E.; Moir, D. C.; Ekdahl, C. A.; Johnson, J. B.; McCuistian, B. T.; Sullivan, G. W.; Crawford, M. T.

2014-03-01

A 7 cm cathode has been deployed for use on a 3.8 MV, 80 ns (FWHM) Blumlein, to increase the extracted electron current from the nominal 1.7 to 2.9 kA. The intense relativistic electron bunch is accelerated and transported through a nested solenoid and ferrite induction core lattice consisting of 64 elements, exiting the accelerator with a nominal energy of 19.8 MeV. The principal objective of these experiments is to quantify the space-charge limitations on the beam quality, its coupling with the beam breakup (BBU) instability, and provide an independent validation of the BBU theory in a higher current regime, I >2 kA. Time resolved centroid measurements indicate a reduction in BBU >10× with simply a 50% increase in the average B-field used to transport the beam through the accelerator. A qualitative comparison of experimental and calculated results are presented, which include time resolved current density distributions, radial BBU amplitude relative to the calculated beam envelope, and frequency analyzed BBU amplitude with different accelerator lattice tunes.

Computation of turbulent boundary layers employing the defect wall-function method. M.S. Thesis

NASA Technical Reports Server (NTRS)

Brown, Douglas L.

1994-01-01

In order to decrease overall computational time requirements of spatially-marching parabolized Navier-Stokes finite-difference computer code when applied to turbulent fluid flow, a wall-function methodology, originally proposed by R. Barnwell, was implemented. This numerical effort increases computational speed and calculates reasonably accurate wall shear stress spatial distributions and boundary-layer profiles. Since the wall shear stress is analytically determined from the wall-function model, the computational grid near the wall is not required to spatially resolve the laminar-viscous sublayer. Consequently, a substantially increased computational integration step size is achieved resulting in a considerable decrease in net computational time. This wall-function technique is demonstrated for adiabatic flat plate test cases from Mach 2 to Mach 8. These test cases are analytically verified employing: (1) Eckert reference method solutions, (2) experimental turbulent boundary-layer data of Mabey, and (3) finite-difference computational code solutions with fully resolved laminar-viscous sublayers. Additionally, results have been obtained for two pressure-gradient cases: (1) an adiabatic expansion corner and (2) an adiabatic compression corner.

Time-resolved Small Angle X-ray Scattering During the Formation of Detonation Nano-Carbon Condensates

NASA Astrophysics Data System (ADS)

Bagge-Hansen, Michael; Hammons, Josh; Nielsen, Mike; Lauderbach, Lisa; Hodgin, Ralph; Bastea, Sorin; van Buuren, Tony; Pagoria, Phil; May, Chadd; Jensen, Brian; Gustavsen, Rick; Watkins, Erik; Firestone, Millie; Dattelbaum, Dana; Fried, Larry; Cowan, Matt; Willey, Trevor

2017-06-01

Carbon nanomaterials are spontaneously generated under high pressure and temperature conditions present during the detonation of many high explosive (HE) materials. Thermochemical modeling suggests that the phase, size, and morphology of carbon condensates are strongly dependent on the type of HE used and associated evolution of temperature and pressure during the very early stages of detonation. Experimental validation of carbon condensation under these extreme conditions has been technically challenging. Here, we present synchrotron-based, time-resolved small-angle x-ray scattering (TR-SAXS) measurements collected during HE detonations, acquired from discrete sub-100 ps x-ray pulses, every 153.4 ns. We select from various HE materials and geometries to explore a range of achievable pressures and temperatures that span detonation conditions and, correspondingly, generate an array of nano-carbon products, including nano-diamonds and nano-onions. The TR-SAXS patterns evolve rapidly over the first few hundred nanoseconds. Comparing the results with modeling offers significant progress towards a general carbon equation of state. Prepared by LLNL under Contract DE-AC52-07NA27344.

Electron and ion dynamics study of iron in warm dense matter regime by time-resolved XAS measurements and from first-principles

NASA Astrophysics Data System (ADS)

Ogitsu, T.; Fernandez-Paãella, A.; Correa, A.; Engelhorn, K.; Barbrel, B.; Prendergast, D. G.; Pemmaraju, D.; Beckwith, M.; Kraus, D.; Hamel, S.; Cho, B. I.; Jin, L.; Wong, J.; Heinman, P.; Collins, G. W.; Falcone, R.; Ping, Y.

2016-10-01

We present a study of the electron-phonon coupling of warm dense iron upon femtosecond laser excitation by time-resolved x-ray absorption near edge spectroscopy (XANES). The dynamics of iron in electron-ion non-equilibrium conditions was studied using ab-initio density-functional-theory (DFT) simulations combined with the Two Temperature Model (TTM) where spatial inhomogeneity of electron (and ion) temperature(s) due to short ballistic electron transport length in iron was explicitly taken into consideration. Detailed comparison between our simulation results and experiments indicates that the ion temperature dependence on specific heat and on electron-phonon coupling also plays a relevant role in modeling the relaxation dynamics of electrons and ions. These results are the first experimental evidence of the suppression of the electron-phonon coupling factor of a transition metal at electron temperatures ranging 5000- 10000 K. This work was performed under DOE contract DE-AC52-07NA27344 with support from OFES Early Career program and LLNL LDRD program.

Grain Boundaries Act as Solid Walls for Charge Carrier Diffusion in Large Crystal MAPI Thin Films.

PubMed

Ciesielski, Richard; Schäfer, Frank; Hartmann, Nicolai F; Giesbrecht, Nadja; Bein, Thomas; Docampo, Pablo; Hartschuh, Achim

2018-03-07

Micro- and nanocrystalline methylammonium lead iodide (MAPI)-based thin-film solar cells today reach power conversion efficiencies of over 20%. We investigate the impact of grain boundaries on charge carrier transport in large crystal MAPI thin films using time-resolved photoluminescence (PL) microscopy and numerical model calculations. Crystal sizes in the range of several tens of micrometers allow for the spatially and time resolved study of boundary effects. Whereas long-ranged diffusive charge carrier transport is observed within single crystals, no detectable diffusive transport occurs across grain boundaries. The observed PL transients are found to crucially depend on the microscopic geometry of the crystal and the point of observation. In particular, spatially restricted diffusion of charge carriers leads to slower PL decay near crystal edges as compared to the crystal center. In contrast to many reports in the literature, our experimental results show no quenching or additional loss channels due to grain boundaries for the studied material, which thus do not negatively affect the performance of the derived thin-film devices.

Tempo-spatially resolved dynamics of elec- trons and holes in bilayer MoS2 -WS2

NASA Astrophysics Data System (ADS)

Galicia-Hernandez, J. M.; Turkowski, V.; Hernandez-Cocoletzi, G.; Rahman, T. S.

We have performed a Density-Matrix Time-Dependent Density-Functional Theory analysis of the response of bilayer MoS2-WS2 to external laser-pulse perturbations. Time-resolved study of the dynamics of electrons and holes, including formation and dissociation of strongly-bound intra- and inter-layer excitonic states, shows that the experimentally observed ultrafast inter-layer MoS2 to WS2 migration of holes may be attributed to unusually large delocalization of the hole state which extends far into the inter-layer region. We also argue that the velocity of the hole transfer may be further enhanced by its interaction with transfer phonon modes. We analyze other possible consequences of the hole delocalization in the system, including reduction of the effects of the electron-electron and hole-hole repulsion in the trions and biexcitons as compared to that in the monolayers Work supported in part by DOE Grant No. DOE-DE-FG02-07ER46354 and by CONACYT Scholarship No. 23210 (J.M.G.H.).

Time-resolved optical emission spectroscopic studies of picosecond laser produced Cr plasma

NASA Astrophysics Data System (ADS)

Rao, Kavya H.; Smijesh, N.; Klemke, N.; Philip, R.; Litvinyuk, I. V.; Sang, R. T.

2018-06-01

Time-resolved optical emission spectroscopic measurements of a plasma generated by irradiating a Cr target using 60 picosecond (ps) and 300 ps laser pulses are carried out to investigate the variation in the line width (δλ) of emission from neutrals and ions for increasing ambient pressures. Measurements ranging from 10-6 Torr to 102 Torr show a distinctly different variation in the δλ of neutrals (Cr I) compared to that of singly ionized Cr (Cr II), for both irradiations. δλ increases monotonously with pressure for Cr II, but an oscillation is evident at intermediate pressures for Cr I. This oscillation does not depend on the laser pulse widths used. In spite of the differences in the plasma formation mechanisms, it is experimentally found that there is an optimum intermediate background pressure for which δλ of neutrals drops to a minimum. Importantly, these results underline the fact that for intermediate pressures, the usual practice of calculating the plasma number density from the δλ of neutrals needs to be judiciously done, to avoid reaching inaccurate conclusions.

Quantitative study of energy-transfer mechanism in Eu,O-codoped GaN by time-resolved photoluminescence spectroscopy

NASA Astrophysics Data System (ADS)

Inaba, Tomohiro; Kojima, Takanori; Yamashita, Genki; Matsubara, Eiichi; Mitchell, Brandon; Miyagawa, Reina; Eryu, Osamu; Tatebayashi, Jun; Ashida, Masaaki; Fujiwara, Yasufumi

2018-04-01

In order to investigate the excitation processes in Eu,O-codoped GaN (GaN:Eu,O), the time-resolved photoluminescence signal including the rising part is analyzed. A rate equation is developed based upon a model for the excitation processes in GaN:Eu to fit the experimental data. The non-radiative recombination rate of the trap state in the GaN host, the energy transfer rate between the Eu3+ ions and the GaN host, the radiative transition probability of Eu3+ ion, as well as the ratio of the number of luminescent sites (OMVPE 4α and OMVPE 4β), are simultaneously determined. It is revealed and quantified that radiative transition probability of the Eu ion is the bottleneck for the enhancement of light output from GaN:Eu. We also evaluate the effect of the growth conditions on the luminescent efficiency of GaN:Eu quantitatively, and find the correlation between emission intensity of GaN:Eu and the fitting parameters introduced in our model.

Time-resolved EPR study on the photoexcited triplet state of the electron-donor-acceptor complex formed in the system of fac-tris[2-(4-octyl-phenyl) pyridine] iridium(III) and tetracene.

PubMed

Zhebin, Fu; Shuhei, Yoshioka; Hisao, Murai

2014-01-09

The physical properties of the phosphorescent organic light-emitting diode material fac-tris(phenylpyridine) iridium(III), Ir(ppy)3, have been reported with experimental and theoretical studies. Here, the photochemical properties of the excited triplet state of partially modified fac-tris[2-(4-octyl-phenyl) pyridine] iridium(III), Ir(C8ppy)3, were investigated using time-resolved electron paramagnetic resonance (tr-EPR) and optical methods by adding tetracene in the toluene solution. The tr-EPR observation at 77 K revealed the following two species: the excited triplet state of tetracene and another triplet species with zero field splitting parameters of |D| = 0.088 cm(-1) and |E| = 0.018 cm(-1) with characteristic spin polarization. The latter species was assigned to the electron-donor-acceptor (EDA) complex formed between Ir(C8ppy)3 and tetracene. The mechanism of formation and the properties of this EDA complex, including the information on the principal axes of (3)Ir(C8ppy)3*, are discussed.

Artifacts in time-resolved NUS: A case study of NOE build-up curves from 2D NOESY.

PubMed

Dass, Rupashree; Kasprzak, Paweł; Koźmiński, Wiktor; Kazimierczuk, Krzysztof

2016-04-01

Multidimensional NMR spectroscopy requires time-consuming sampling of indirect dimensions and so is usually used to study stable samples. However, dynamically changing compounds or their mixtures commonly occur in problems of natural science. Monitoring them requires the use multidimensional NMR in a time-resolved manner - in other words, a series of quick spectra must be acquired at different points in time. Among the many solutions that have been proposed to achieve this goal, time-resolved non-uniform sampling (TR-NUS) is one of the simplest. In a TR-NUS experiment, the signal is sampled using a shuffled random schedule and then divided into overlapping subsets. These subsets are then processed using one of the NUS reconstruction methods, for example compressed sensing (CS). The resulting stack of spectra forms a temporal "pseudo-dimension" that shows the changes caused by the process occurring in the sample. CS enables the use of small subsets of data, which minimizes the averaging of the effects studied. Yet, even within these limited timeframes, the sample undergoes certain changes. In this paper we discuss the effect of varying signal amplitude in a TR-NUS experiment. Our theoretical calculations show that the variations within the subsets lead to t1-noise, which is dependent on the rate of change of the signal amplitude. We verify these predictions experimentally. As a model case we choose a novel 2D TR-NOESY experiment in which mixing time is varied in parallel with shuffled NUS in the indirect dimension. The experiment, performed on a sample of strychnine, provides a near-continuous NOE build-up curve, whose shape closely reflects the t1-noise level. 2D TR-NOESY reduces the measurement time compared to the conventional approach and makes it possible to verify the theoretical predictions about signal variations during TR-NUS. Copyright © 2016 Elsevier Inc. All rights reserved.

Extreme ultraviolet resonant inelastic X-ray scattering (RIXS) at a seeded free-electron laser

DOE PAGES

Dell’Angela, M.; Hieke, F.; Malvestuto, M.; ...

2016-12-12

In the past few years, we have been witnessing an increased interest for studying materials properties under non-equilibrium conditions. Several well established spectroscopies for experiments in the energy domain have been successfully adapted to the time domain with sub-picosecond time resolution. Here we show the realization of high resolution resonant inelastic X-ray scattering (RIXS) with a stable ultrashort X-ray source such as an externally seeded free electron laser (FEL). We have designed and constructed a RIXS experimental endstation that allowed us to successfully measure the d-d excitations in KCoF 3 single crystals at the cobalt M 2,3-edge at FERMI FELmore » (Elettra-Sincrotrone Trieste, Italy). The FEL-RIXS spectra show an excellent agreement with the ones obtained from the same samples at the MERIXS endstation of the MERLIN beamline at the Advanced Light Source storage ring (Berkeley, USA). We established experimental protocols for performing time resolved RIXS experiments at a FEL source to avoid X ray-induced sample damage, while retaining comparable acquisition time to the synchrotron based measurements. Finally, we measured and modelled the influence of the FEL mixed electromagnetic modes, also present in externally seeded FELs, and the beam transport with ~120 meV experimental resolution achieved in the presented RIXS setup.« less

Correlated, precision measurements of θ 23 and δ using only the electron neutrino appearance experiments

DOE PAGES

Minakata, Hisakazu; Parke, Stephen J.

2013-06-04

Precision measurement of the leptonic CP violating phase δ will suffer from the, then surviving, large uncertainty of sin 2θ 23 of 10–20% in the experimentally interesting region near maximal mixing of θ 23. We advocate a new method for determination of both θ 23 and δ at the same time using only the ν e and ν̄ e appearance channels and show that sin 2θ 23 can be determined automatically with much higher accuracy, approximately a factor of six, than sinδ. In this method, we identify a new degeneracy for the simultaneous determination of θ 23 and δ, themore » θ 23 intrinsic degeneracy, which must be resolved in order to achieve precision measurement of these two parameters. Spectral information around the vacuum oscillation maxima is shown to be the best way to resolve this degeneracy.« less

Autonomous Operations Planner: A Flexible Platform for Research in Flight-Deck Support for Airborne Self-Separation

NASA Technical Reports Server (NTRS)

Karr, David A.; Vivona, Robert A.; DePascale, Stephen M.; Wing, David J.

2012-01-01

The Autonomous Operations Planner (AOP), developed by NASA, is a flexible and powerful prototype of a flight-deck automation system to support self-separation of aircraft. The AOP incorporates a variety of algorithms to detect and resolve conflicts between the trajectories of its own aircraft and traffic aircraft while meeting route constraints such as required times of arrival and avoiding airspace hazards such as convective weather and restricted airspace. This integrated suite of algorithms provides flight crew support for strategic and tactical conflict resolutions and conflict-free trajectory planning while en route. The AOP has supported an extensive set of experiments covering various conditions and variations on the self-separation concept, yielding insight into the system s design and resolving various challenges encountered in the exploration of the concept. The design of the AOP will enable it to continue to evolve and support experimentation as the self-separation concept is refined.

Plasma diagnostics of low pressure high power impulse magnetron sputtering assisted by electron cyclotron wave resonance plasma

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

Stranak, Vitezslav; University of South Bohemia, Institute of Physics and Biophysics, Branisovska 31, 370 05 Ceske Budejovice; Herrendorf, Ann-Pierra

2012-11-01

This paper reports on an investigation of the hybrid pulsed sputtering source based on the combination of electron cyclotron wave resonance (ECWR) inductively coupled plasma and high power impulse magnetron sputtering (HiPIMS) of a Ti target. The plasma source, operated in an Ar atmosphere at a very low pressure of 0.03 Pa, provides plasma where the major fraction of sputtered particles is ionized. It was found that ECWR assistance increases the electron temperature during the HiPIMS pulse. The discharge current and electron density can achieve their stable maximum 10 {mu}s after the onset of the HiPIMS pulse. Further, a highmore » concentration of double charged Ti{sup ++} with energies of up to 160 eV was detected. All of these facts were verified experimentally by time-resolved emission spectroscopy, retarding field analyzer measurement, Langmuir probe, and energy-resolved mass spectrometry.« less

Colloidal suspensions in external rotating electric field: experimental studies and prospective applications in physics, material science, and biomedicine

NASA Astrophysics Data System (ADS)

Yakovlev, Egor V.; Troshina, Anna V.; Korsakova, Sofia A.; Andronik, Mikhail; Rodionov, Ilya A.; Aliev, Ismail N.; Zaytsev, Kirill I.; Cherkasova, Olga P.; Tuchin, Valery V.; Yurchenko, Stanislav O.

2018-04-01

Colloidal suspensions and tunable self-assembly of colloidal particles attract a great interest in recent years. In this paper, we propose a new setup and technology for studies of self-assembly of colloidal particles, interection of which between themselves is tuned by external rotating electric fields. We reveal wide prospectives of electric field employment for tunable self-assembly, from suspensions of inorganic particles to ensembles of biological cells. These results make enable particle-resolved studies of various collective phenomena and fundamental processes in many-particle systems in equilibrium state and far from it, while the dynamics can be resolved at the level of individual particles using video microscopy. For the first time, we demonstrate that, apart from ability to prepare photonic crystalline films of inorganic silica particles, the tunable self-assembly provides a novel technological way for manipulation with ensembles of biological cells by control of interactions between them.

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

Godfrey, T. J.; Yu, Hui; Ullrich, Susanne, E-mail: ullrich@physast.uga.edu

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

Ejection of spalled layers from laser shock-loaded metals

NASA Astrophysics Data System (ADS)

Lescoute, E.; De Rességuier, T.; Chevalier, J.-M.; Loison, D.; Cuq-Lelandais, J.-P.; Boustie, M.; Breil, J.; Maire, P.-H.; Schurtz, G.

2010-11-01

Dynamic fragmentation of shock-loaded metals is an issue of considerable importance for both basic science and a variety of technological applications, such as inertial confinement fusion, which involves high energy laser irradiation of thin metallic shells. In this context, we present an experimental and numerical study of debris ejection in laser shock-loaded metallic targets (aluminum, gold, and iron) where fragmentation is mainly governed by spall fracture occurring upon tensile loading due to wave interactions inside the sample. Experimental results consist of time-resolved velocity measurements, transverse optical shadowgraphy of ejected debris, and postshock observations of targets and fragments recovered within a transparent gel of low density. They are compared to numerical computations performed with a hydrodynamic code. A correct overall consistency is obtained.

Overview of Fuel Rod Simulator Usage at ORNL

NASA Astrophysics Data System (ADS)

Ott, Larry J.; McCulloch, Reg

2004-02-01

During the 1970s and early 1980s, the Oak Ridge National Laboratory (ORNL) operated large out-of-reactor experimental facilities to resolve thermal-hydraulic safety issues in nuclear reactors. The fundamental research ranged from material mechanical behavior of fuel cladding during the depressurization phase of a loss-of-coolant accident (LOCA) to basic heat transfer research in gas- or sodium-cooled cores. The largest facility simulated the initial phase (less than 1 min. of transient time) of a LOCA in a commercial pressurized-water reactor. The nonnuclear reactor cores of these facilities were mimicked via advanced, highly instrumented electric fuel rod simulators locally manufactured at ORNL. This paper provides an overview of these experimental facilities with an emphasis on the fuel rod simulators.

Introduction to Time-Resolved Spectroscopy: Nanosecond Transient Absorption and Time-Resolved Fluorescence of Eosin B

ERIC Educational Resources Information Center

Farr, Erik P.; Quintana, Jason C.; Reynoso, Vanessa; Ruberry, Josiah D.; Shin, Wook R.; Swartz, Kevin R.

2018-01-01

Here we present a new undergraduate laboratory that will introduce the concepts of time-resolved spectroscopy and provide insight into the natural time scales on which chemical dynamics occur through direct measurement. A quantitative treatment of the acquired data will provide a deeper understanding of the role of quantum mechanics and various…

Ultrafast magneto-optical spectroscopy of GaMnAs (Invited Paper)

NASA Astrophysics Data System (ADS)

Heroux, Jean Benoit; Kojima, Eiji; Ino, Y.; Hashimoto, Y.; Katsumoto, Shingo; Iye, Yasushiro; Kuwata-Gonokami, Makoto

2005-04-01

Spin dynamics in the III-V dilute magnetic semiconductor GaMnAs is investigated by photo-induced demagnetization. Experimental results obtained from two different time-dependent characterization techniques - "two color-probe" magneto-optical Kerr effect (TR-MOKE) and mid-infrared differential transmittance -- are compared. Upon photo-excitation with a 100 fs, 3.1 eV light pulse, a long demagnetization time in the hundreds of picoseconds timescale is found by TR-MOKE, indicating a spin-dependent band structure in this material. In mid-infrared measurements, a positive increase of the differential transmittance is observed in the same time interval when the sample is cooled below its Currie temperature. It is shown that this mid-infrared absorption feature is directly related to ferromagnetism in this material. The magnetism-related component of the broad DC mid-infrared absorption peak characteristic of this p-type material could be observed with this time-resolved measurement. Experimental results were simulated with a model describing the interaction between three thermal reservoirs (hole, spin and lattice) and taking thermal diffusion into account.

A remote laboratory for USRP-based software defined radio

NASA Astrophysics Data System (ADS)

Gandhinagar Ekanthappa, Rudresh; Escobar, Rodrigo; Matevossian, Achot; Akopian, David

2014-02-01

Electrical and computer engineering graduates need practical working skills with real-world electronic devices, which are addressed to some extent by hands-on laboratories. Deployment capacity of hands-on laboratories is typically constrained due to insufficient equipment availability, facility shortages, and lack of human resources for in-class support and maintenance. At the same time, at many sites, existing experimental systems are usually underutilized due to class scheduling bottlenecks. Nowadays, online education gains popularity and remote laboratories have been suggested to broaden access to experimentation resources. Remote laboratories resolve many problems as various costs can be shared, and student access to instrumentation is facilitated in terms of access time and locations. Labs are converted to homeworks that can be done without physical presence in laboratories. Even though they are not providing full sense of hands-on experimentation, remote labs are a viable alternatives for underserved educational sites. This paper studies remote modality of USRP-based radio-communication labs offered by National Instruments (NI). The labs are offered to graduate and undergraduate students and tentative assessments support feasibility of remote deployments.

Physical Justification for Negative Remanent Magnetization in Homogeneous Nanoparticles

PubMed Central

Gu, Shuo; He, Weidong; Zhang, Ming; Zhuang, Taisen; Jin, Yi; ElBidweihy, Hatem; Mao, Yiwu; Dickerson, James H.; Wagner, Michael J.; Torre, Edward Della; Bennett, Lawrence H.

2014-01-01

The phenomenon of negative remanent magnetization (NRM) has been observed experimentally in a number of heterogeneous magnetic systems and has been considered anomalous. The existence of NRM in homogenous magnetic materials is still in debate, mainly due to the lack of compelling support from experimental data and a convincing theoretical explanation for its thermodynamic validation. Here we resolve the long-existing controversy by presenting experimental evidence and physical justification that NRM is real in a prototype homogeneous ferromagnetic nanoparticle, an europium sulfide nanoparticle. We provide novel insights into major and minor hysteresis behavior that illuminate the true nature of the observed inverted hysteresis and validate its thermodynamic permissibility and, for the first time, present counterintuitive magnetic aftereffect behavior that is consistent with the mechanism of magnetization reversal, possessing unique capability to identify NRM. The origin and conditions of NRM are explained quantitatively via a wasp-waist model, in combination of energy calculations. PMID:25183061

Extinction ratio enhancement of SOA-based delayed-interference signal converter using detuned filtering

NASA Astrophysics Data System (ADS)

Zhang, B.; Kumar, S.; Yan, L.-S.; Willner, A. E.

2007-12-01

We demonstrate experimentally >3 dB extinction ratio improvement at the output of SOA-based delayed-interference signal converter (DISC) using optical off-centered filtering. Through careful modeling of the carrier and the phase dynamics, we explain in detail the origin of sub-pulses in the wavelength converted output, with an emphasis on the time-resolved frequency chirping of the output signal. Through our simulations we conclude that the sub-pulses and the main-pulses are oppositely chirped, which is also verified experimentally by analyzing the output with a chirp form analyzer. We propose and demonstrate an optical off-center filtering technique which effectively suppresses these sub-pulses. The effects of filter detuning and phase bias adjustment in the delayed-interferometer are experimentally characterized and optimized, leading to a >3 dB extinction ratio enhancement of the output signal.

An experimental application of the Periodic Tracer Hierarchy (PERTH) method to quantify time-variable water and solute transport in a sloping soil lysimeter

NASA Astrophysics Data System (ADS)

Pangle, L. A.; Cardoso, C.; Kim, M.; Lora, M.; Wang, Y.; Troch, P. A. A.; Harman, C. J.

2014-12-01

Water molecules traverse myriad flow paths and spend different lengths of time on or within the landscape before they are discharged into a stream channel. The transit-time distribution (TTD) is a probability distribution that represents the range and likelihood of transit times for water and conservative solutes within soils and catchments, and is useful for comparative analysis and prediction of solute transport into streams. The TTD has customarily been assumed to be time-invariant in practical applications, but is understood to vary due to unsteady flow rates, changes in water-balance partitioning, and shifting flow pathways. Recent theoretical advances have clarified how the distribution of transit times experienced by water and solutes within a stream channel at any moment in time is conditional on the specific series of precipitation events preceding that time. Observations resolving how TTDs vary during a specific sequence of precipitation events could be obtained by introducing unique and conservative tracers during each event and quantifying their distinct breakthrough curves in the stream. At present, the number of distinct and conservative tracers available for this purpose is insufficient. Harman and Kim [Harman, C.J. and Kim, M., 2014, Geophysical Research Letters, 41, 1567-1575] proposed a new experimental method—based on the establishment of periodic steady-state conditions—that allows multiple overlapping breakthrough curves of non-unique tracers to be decomposed, thus enabling analysis of the distinct TTDs associated with their specific times of introduction through precipitation. We present results from one of the first physical experiments to test this methodology. Our experiment involves a sloping lysimeter (10° slope) that contains one cubic meter of crushed basalt rock (loamy sand texture), an irrigation system adaptable to controlled tracer introductions, and instruments that enable total water balance monitoring. We imposed a repeated sequence of rainfall pulses and achieved periodic-steady-state conditions over 24 days. Using systematic introductions of deuterium- and chloride-enriched water, and the PERTH method, we resolve the time-conditional TTDs associated with tracer injections that occurred during specific intervals of the overall rainfall sequence.

The Fresnel Zone Light Field Spectral Imager

DTIC Science & Technology

2017-03-23

Marciniak Member AFIT-ENP-MS-17-M-095 Abstract This thesis provides a computational model and the first experimental demonstration of a Fresnel zone...Fresnel propagation. It was validated experimentally and provides excellent demonstration of system capabilities. The experimentally demonstrated system...in the measured light fields, they did not degrade the system’s performance. Experimental demonstration also showed the capability to resolve between

Difference structures from time-resolved small-angle and wide-angle x-ray scattering

NASA Astrophysics Data System (ADS)

Nepal, Prakash; Saldin, D. K.

2018-05-01

Time-resolved small-angle x-ray scattering/wide-angle x-ray scattering (SAXS/WAXS) is capable of recovering difference structures directly from difference SAXS/WAXS curves. It does so by means of the theory described here because the structural changes in pump-probe detection in a typical time-resolved experiment are generally small enough to be confined to a single residue or group in close proximity which is identified by a method akin to the difference Fourier method of time-resolved crystallography. If it is assumed, as is usual with time-resolved structures, that the moved atoms lie within the residue, the 100-fold reduction in the search space (assuming a typical protein has about 100 residues) allows the exaction of the structure by a simulated annealing algorithm with a huge reduction in computing time and leads to a greater resolution by varying the positions of atoms only within that residue. This reduction in the number of potential moved atoms allows us to identify the actual motions of the individual atoms. In the case of a crystal, time-resolved calculations are normally performed using the difference Fourier method, which is, of course, not directly applicable to SAXS/WAXS. The method developed in this paper may be thought of as a substitute for that method which allows SAXS/WAXS (and hence disordered molecules) to also be used for time-resolved structural work.

Discrimination of binary coherent states using a homodyne detector and a photon number resolving detector

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

Wittmann, Christoffer; Sych, Denis; Leuchs, Gerd

2010-06-15

We investigate quantum measurement strategies capable of discriminating two coherent states probabilistically with significantly smaller error probabilities than can be obtained using nonprobabilistic state discrimination. We apply a postselection strategy to the measurement data of a homodyne detector as well as a photon number resolving detector in order to lower the error probability. We compare the two different receivers with an optimal intermediate measurement scheme where the error rate is minimized for a fixed rate of inconclusive results. The photon number resolving (PNR) receiver is experimentally demonstrated and compared to an experimental realization of a homodyne receiver with postselection. Inmore » the comparison, it becomes clear that the performance of the PNR receiver surpasses the performance of the homodyne receiver, which we prove to be optimal within any Gaussian operations and conditional dynamics.« less

Overtone Mobility Spectrometry (Part 2): Theoretical Considerations of Resolving Power

PubMed Central

Valentine, Stephen J.; Stokes, Sarah T.; Kurulugama, Ruwan T.; Nachtigall, Fabiane M.; Clemmer, David E.

2009-01-01

The transport of ions through multiple drift regions is modeled in order to develop an equation that is useful for an understanding of the resolving power of an overtone mobility spectrometry (OMS) technique. It is found that resolving power is influenced by a number of experimental variables, including those that define ion mobility spectrometry (IMS) resolving power: drift field (E), drift region length (L), and buffer gas temperature (T). However, unlike IMS, the resolving power of OMS is also influenced by the number of drift regions (n), harmonic frequency value (m), and the phase number (ϕ) of the applied drift field. The OMS resolving power dependence upon the new OMS variables (n, m, and ϕ) scales differently than the square root dependence of the E, L, and T variables in IMS. The results provide insight about optimal instrumental design and operation. PMID:19230705

Gas-liquid Phase Distribution and Void Fraction Measurements Using the MRI

NASA Technical Reports Server (NTRS)

Daidzic, N. E.; Schmidt, E.; Hasan, M. M.; Altobelli, S.

2004-01-01

We used a permanent-magnet MRI system to estimate the integral and spatially- and/or temporally-resolved void-fraction distributions and flow patterns in gas-liquid two-phase flows. Air was introduced at the bottom of the stagnant liquid column using an accurate and programmable syringe pump. Air flow rates were varied between 1 and 200 ml/min. The cylindrical non-conducting test tube in which two-phase flow was measured was placed in a 2.67 kGauss MRI with MRT spectrometer/imager. Roughly linear relationship has been obtained for the integral void-fraction, obtained by volume-averaging of the spatially-resolved signals, and the air flow rate in upward direction. The time-averaged spatially-resolved void fraction has also been obtained for the quasi-steady flow of air in a stagnant liquid column. No great accuracy is claimed as this was an exploratory proof-of-concept type of experiment. Preliminary results show that MRI a non-invasive and non-intrusive experimental technique can indeed provide a wealth of different qualitative and quantitative data and is especially well suited for averaged transport processes in adiabatic and diabatic multi-phase and/or multi-component flows.

State resolved vibrational relaxation modeling for strongly nonequilibrium flows

NASA Astrophysics Data System (ADS)

Boyd, Iain D.; Josyula, Eswar

2011-05-01

Vibrational relaxation is an important physical process in hypersonic flows. Activation of the vibrational mode affects the fundamental thermodynamic properties and finite rate relaxation can reduce the degree of dissociation of a gas. Low fidelity models of vibrational activation employ a relaxation time to capture the process at a macroscopic level. High fidelity, state-resolved models have been developed for use in continuum gas dynamics simulations based on computational fluid dynamics (CFD). By comparison, such models are not as common for use with the direct simulation Monte Carlo (DSMC) method. In this study, a high fidelity, state-resolved vibrational relaxation model is developed for the DSMC technique. The model is based on the forced harmonic oscillator approach in which multi-quantum transitions may become dominant at high temperature. Results obtained for integrated rate coefficients from the DSMC model are consistent with the corresponding CFD model. Comparison of relaxation results obtained with the high-fidelity DSMC model shows significantly less excitation of upper vibrational levels in comparison to the standard, lower fidelity DSMC vibrational relaxation model. Application of the new DSMC model to a Mach 7 normal shock wave in carbon monoxide provides better agreement with experimental measurements than the standard DSMC relaxation model.

X-ray absorption spectroscopy with time-tagged photon counting: application to study the structure of a Co(i) intermediate of H2 evolving photo-catalyst.

PubMed

Smolentsev, Grigory; Guda, Alexander A; Janousch, Markus; Frieh, Cristophe; Jud, Gaudenz; Zamponi, Flavio; Chavarot-Kerlidou, Murielle; Artero, Vincent; van Bokhoven, Jeroen A; Nachtegaal, Maarten

2014-01-01

In order to probe the structure of reaction intermediates of photochemical reactions a new setup for laser-initiated time-resolved X-ray absorption (XAS) measurements has been developed. With this approach the arrival time of each photon in respect to the laser pulse is measured and therefore full kinetic information is obtained. All X-rays that reach the detector are used to measure this kinetic information and therefore the detection efficiency of this method is high. The newly developed setup is optimized for time-resolved experiments in the microsecond range for samples with relatively low metal concentration (∼1mM). This setup has been applied to study a multicomponent photocatalytic system with a Co(dmgBF(2))(2) catalyst (dmg(2-) = dimethylglyoximato dianion), [Ru(bpy)(3)](2+) chromophore (bpy = 2,2'-bipyridine) and methyl viologen as the electron relay. On the basis of the analysis of hundreds of Co K-edge XAS spectra corresponding to different delay times after the laser excitation of the chromophore, the presence of a Co(i) intermediate is confirmed. The calculated X-ray transient signal for a model of Co(i) state with a 0.14 Å displacement of Co out of the dmg ligand plane and with the closest solvent molecule at a distance of 2.06 Å gives reasonable agreement with the experimental data.

LES/RANS Simulation of a Supersonic Reacting Wall Jet

NASA Technical Reports Server (NTRS)

Edwards, Jack R.; Boles, John A.; Baurle, Robert A.

2010-01-01

This work presents results from large-eddy / Reynolds-averaged Navier-Stokes (LES/RANS) simulations of the well-known Burrows-Kurkov supersonic reacting wall-jet experiment. Generally good agreement with experimental mole fraction, stagnation temperature, and Pitot pressure profiles is obtained for non-reactive mixing of the hydrogen jet with a non-vitiated air stream. A lifted flame, stabilized between 10 and 22 cm downstream of the hydrogen jet, is formed for hydrogen injected into a vitiated air stream. Flame stabilization occurs closer to the hydrogen injection location when a three-dimensional combustor geometry (with boundary layer development resolved on all walls) is considered. Volumetric expansion of the reactive shear layer is accompanied by the formation of large eddies which interact strongly with the reaction zone. Time averaged predictions of the reaction zone structure show an under-prediction of the peak water concentration and stagnation temperature, relative to experimental data and to results from a Reynolds-averaged Navier-Stokes calculation. If the experimental data can be considered as being accurate, this result indicates that the present LES/RANS method does not correctly capture the cascade of turbulence scales that should be resolvable on the present mesh. Instead, energy is concentrated in the very largest scales, which provide an over-mixing effect that excessively cools and strains the flame. Predictions improve with the use of a low-dissipation version of the baseline piecewise parabolic advection scheme, which captures the formation of smaller-scale structures superimposed on larger structures of the order of the shear-layer width.

Weakly-Correlated Nature of Ferromagnetism in Nonsymmorphic CrO2 Revealed by Bulk-Sensitive Soft-X-Ray ARPES

NASA Astrophysics Data System (ADS)

Bisti, F.; Rogalev, V. A.; Karolak, M.; Paul, S.; Gupta, A.; Schmitt, T.; Güntherodt, G.; Eyert, V.; Sangiovanni, G.; Profeta, G.; Strocov, V. N.

2017-10-01

Chromium dioxide CrO2 belongs to a class of materials called ferromagnetic half-metals, whose peculiar aspect is that they act as a metal in one spin orientation and as a semiconductor or insulator in the opposite one. Despite numerous experimental and theoretical studies motivated by technologically important applications of this material in spintronics, its fundamental properties such as momentum-resolved electron dispersions and the Fermi surface have so far remained experimentally inaccessible because of metastability of its surface, which instantly reduces to amorphous Cr2O3 . In this work, we demonstrate that direct access to the native electronic structure of CrO2 can be achieved with soft-x-ray angle-resolved photoemission spectroscopy whose large probing depth penetrates through the Cr2O3 layer. For the first time, the electronic dispersions and Fermi surface of CrO2 are measured, which are fundamental prerequisites to solve the long debate on the nature of electronic correlations in this material. Since density functional theory augmented by a relatively weak local Coulomb repulsion gives an exhaustive description of our spectroscopic data, we rule out strong-coupling theories of CrO2 . Crucial for the correct interpretation of our experimental data in terms of the valence-band dispersions is the understanding of a nontrivial spectral response of CrO2 caused by interference effects in the photoemission process originating from the nonsymmorphic space group of the rutile crystal structure of CrO2 .

Development and Experimental Verification of a High Resolution, Tunable LIDAR Computer Simulation Model for Atmospheric Laser Remote Sensing

NASA Astrophysics Data System (ADS)

Wilcox, William Edward, Jr.

1995-01-01

A computer program (LIDAR-PC) and associated atmospheric spectral databases have been developed which accurately simulate the laser remote sensing of the atmosphere and the system performance of a direct-detection Lidar or tunable Differential Absorption Lidar (DIAL) system. This simulation program allows, for the first time, the use of several different large atmospheric spectral databases to be coupled with Lidar parameter simulations on the same computer platform to provide a real-time, interactive, and easy to use design tool for atmospheric Lidar simulation and modeling. LIDAR -PC has been used for a range of different Lidar simulations and compared to experimental Lidar data. In general, the simulations agreed very well with the experimental measurements. In addition, the simulation offered, for the first time, the analysis and comparison of experimental Lidar data to easily determine the range-resolved attenuation coefficient of the atmosphere and the effect of telescope overlap factor. The software and databases operate on an IBM-PC or compatible computer platform, and thus are very useful to the research community for Lidar analysis. The complete Lidar and atmospheric spectral transmission modeling program uses the HITRAN database for high-resolution molecular absorption lines of the atmosphere, the BACKSCAT/LOWTRAN computer databases and models for the effects of aerosol and cloud backscatter and attenuation, and the range-resolved Lidar equation. The program can calculate the Lidar backscattered signal-to-noise for a slant path geometry from space and simulate the effect of high resolution, tunable, single frequency, and moderate line width lasers on the Lidar/DIAL signal. The program was used to model and analyze the experimental Lidar data obtained from several measurements. A fixed wavelength, Ho:YSGG aerosol Lidar (Sugimoto, 1990) developed at USF and a tunable Ho:YSGG DIAL system (Cha, 1991) for measuring atmospheric water vapor at 2.1 μm were analyzed. The simulations agreed very well with the measurements, and also yielded, for the first time, the ability to easily deduce the atmospheric attentuation coefficient, alpha, from the Lidar data. Simulations and analysis of other Lidar measurements included that of a 1.57 mu m OPO aerosol Lidar system developed at USF (Harrell, 1995) and of the NASA LITE (Laser-in-Space Technology Experiment) Lidar recently flown in the Space shuttle. Finally, an extensive series of laboratory experiments were made with the 1.57 μm OPO Lidar system to test calculations of the telescope/laser overlap and the effect of different telescope sizes and designs. The simulations agreed well with the experimental data for the telescope diameter and central obscuration test cases. The LIDAR-PC programs are available on the Internet from the USAF Lidar Home Page Web site, http://www.cas.usf.edu/physics/lidar.html/.

Experimental and Numerical Investigation of Combined Sensible/Latent Thermal Energy Storage for High-Temperature Applications.

PubMed

Geissbühler, Lukas; Zavattoni, Simone; Barbato, Maurizio; Zanganeh, Giw; Haselbacher, Andreas; Steinfeld, Aldo

2015-01-01

Combined sensible/latent heat storage allows the heat-transfer fluid outflow temperature during discharging to be stabilized. A lab-scale combined storage consisting of a packed bed of rocks and steel-encapsulated AlSi(12) was investigated experimentally and numerically. Due to the small tank-to-particle diameter ratio of the lab-scale storage, void-fraction variations were not negligible, leading to channeling effects that cannot be resolved in 1D heat-transfer models. The void-fraction variations and channeling effects can be resolved in 2D models of the flow and heat transfer in the storage. The resulting so-called bypass fraction extracted from the 2D model was used in the 1D model and led to good agreement with experimental measurements.

Children's Use of Gesture to Resolve Lexical Ambiguity

ERIC Educational Resources Information Center

Kidd, Evan; Holler, Judith

2009-01-01

We report on a study investigating 3-5-year-old children's use of gesture to resolve lexical ambiguity. Children were told three short stories that contained two homonym senses; for example, "bat" (flying mammal) and "bat" (sports equipment). They were then asked to re-tell these stories to a second experimenter. The data were coded for the means…

Electronic structure of the dilute magnetic semiconductor G a1 -xM nxP from hard x-ray photoelectron spectroscopy and angle-resolved photoemission

NASA Astrophysics Data System (ADS)

Keqi, A.; Gehlmann, M.; Conti, G.; Nemšák, S.; Rattanachata, A.; Minár, J.; Plucinski, L.; Rault, J. E.; Rueff, J. P.; Scarpulla, M.; Hategan, M.; Pálsson, G. K.; Conlon, C.; Eiteneer, D.; Saw, A. Y.; Gray, A. X.; Kobayashi, K.; Ueda, S.; Dubon, O. D.; Schneider, C. M.; Fadley, C. S.

2018-04-01

We have investigated the electronic structure of the dilute magnetic semiconductor (DMS) G a0.98M n0.02P and compared it to that of an undoped GaP reference sample, using hard x-ray photoelectron spectroscopy (HXPS) and hard x-ray angle-resolved photoemission spectroscopy (HARPES) at energies of about 3 keV. We present experimental data, as well as theoretical calculations, to understand the role of the Mn dopant in the emergence of ferromagnetism in this material. Both core-level spectra and angle-resolved or angle-integrated valence spectra are discussed. In particular, the HARPES experimental data are compared to free-electron final-state model calculations and to more accurate one-step photoemission theory. The experimental results show differences between G a0.98M n0.02P and GaP in both angle-resolved and angle-integrated valence spectra. The G a0.98M n0.02P bands are broadened due to the presence of Mn impurities that disturb the long-range translational order of the host GaP crystal. Mn-induced changes of the electronic structure are observed over the entire valence band range, including the presence of a distinct impurity band close to the valence-band maximum of the DMS. These experimental results are in good agreement with the one-step photoemission calculations and a prior HARPES study of G a0.97M n0.03As and GaAs [Gray et al., Nat. Mater. 11, 957 (2012), 10.1038/nmat3450], demonstrating the strong similarity between these two materials. The Mn 2 p and 3 s core-level spectra also reveal an essentially identical state in doping both GaAs and GaP.

Time-resolved EPR spectroscopy in a Unix environment.

PubMed

Lacoff, N M; Franke, J E; Warden, J T

1990-02-01

A computer-aided time-resolved electron paramagnetic resonance (EPR) spectrometer implemented under version 2.9 BSD Unix was developed by interfacing a Varian E-9 EPR spectrometer and a Biomation 805 waveform recorder to a PDP-11/23A minicomputer having MINC A/D and D/A capabilities. Special problems with real-time data acquisition in a multiuser, multitasking Unix environment, addressing of computer main memory for the control of hardware devices, and limitation of computer main memory were resolved, and their solutions are presented. The time-resolved EPR system and the data acquisition and analysis programs, written entirely in C, are described. Furthermore, the benefits of utilizing the Unix operating system and the C language are discussed, and system performance is illustrated with time-resolved EPR spectra of the reaction center cation in photosystem 1 of green plant photosynthesis.

Flow characteristics in a canine aneurysm model: A comparison of 4D accelerated phase-contrast MR measurements and computational fluid dynamics simulations

PubMed Central

Jiang, Jingfeng; Johnson, Kevin; Valen-Sendstad, Kristian; Mardal, Kent-Andre; Wieben, Oliver; Strother, Charles

2011-01-01

Purpose: Our purpose was to compare quantitatively velocity fields in and around experimental canine aneurysms as measured using an accelerated 4D PC-MR angiography (MRA) method and calculated based on animal-specific CFD simulations. Methods: Two animals with a surgically created bifurcation aneurysm were imaged using an accelerated 4D PC-MRA method. Meshes were created based on the geometries obtained from the PC-MRA and simulations using “subject-specific” pulsatile velocity waveforms and geometries were then solved using a commercial CFD solver. Qualitative visual assessments and quantitative comparisons of the time-resolved velocity fields obtained from the PC-MRA measurements and the CFD simulations were performed using a defined similarity metric combining both angular and magnitude differences of vector fields. Results: PC-MRA and image-based CFD not only yielded visually consistent representations of 3D streamlines in and around both aneurysms, but also showed good agreement with regard to the spatial velocity distributions. The estimated similarity between time-resolved velocity fields from both techniques was reasonably high (mean value >0.60; one being the highest and zero being the lowest). Relative differences in inflow and outflow zones among selected planes were also reasonable (on the order of 10%–20%). The correlation between CFD-calculated and PC-MRA-measured time-averaged wall shear stresses was low (0.22 and 0.31, p < 0.001). Conclusions: In two experimental canine aneurysms, PC-MRA and image-based CFD showed favorable agreement in intra-aneurismal velocity fields. Combining these two complementary techniques likely will further improve the ability to characterize and interpret the complex flow that occurs in human intracranial aneurysms. PMID:22047395

Influence of shallow traps on time-resolved optically stimulated luminescence measurements of Al2O3:C,Mg

NASA Astrophysics Data System (ADS)

Denis, G.; Akselrod, M. S.; Yukihara, E. G.

2011-05-01

The objective of this paper is to investigate the influence of shallow traps on the signals from Al2O3:C,Mg obtained using time-resolved optically stimulated luminescence (TR-OSL) measurements through experiments and numerical simulations. TR-OSL measurements of Al2O3:C,Mg were carried out and the resulting optically stimulated luminescence (OSL) curves were investigated as a function of the temperature. The numerical simulations were carried out using the rate-equations for a simplified model of Al2O3:C,Mg containing two types of luminescence centers with different luminescence lifetimes and three types of electron traps (a shallow trap, a main dosimetric trap, and a thermally disconnected deep trap). Both experimental results and simulations show that the OSL signals during and between the stimulation pulses are affected by the presence of shallow traps. However, with an appropriate choice of timing parameters, the influence of shallow traps can be reduced by calculating the difference between the signals during and between stimulation pulses. Therefore, TR-OSL can be useful in dosimetry using materials having a large concentration of shallow traps and OSL components with short luminescence lifetimes, for example Al2O3:C,Mg and BeO. Our results also show that the presence of shallow traps has to be taken into account when using the TR-OSL for discrimination between luminescence centers with different luminescence lifetimes, or separation between the OSL from different materials based on their characteristic luminescence lifetimes. The experimental results also show evidence of thermal assistance in the OSL process of Al2O3:C,Mg.

Appropriate Minimal Dose of Gadobutrol for 3D Time-Resolved MRA of the Supra-Aortic Arteries: Comparison with Conventional Single-Phase High-Resolution 3D Contrast-Enhanced MRA.

PubMed

Bak, S H; Roh, H G; Moon, W-J; Choi, J W; An, H S

2017-07-01

The development of nephrogenic systemic fibrosis and neural tissue deposition is gadolinium dose-dependent. The purpose of this study was to determine the appropriate minimal dose of gadobutrol with time-resolved MRA to assess supra-aortic arterial stenosis with contrast-enhanced MRA as a reference standard. Four hundred sixty-two consecutive patients underwent both standard-dose contrast-enhanced MRA and low-dose time-resolved MRA and were classified into 3 groups; group A (a constant dose of 1 mL for time-resolved MRA), group B (2 mL), or group C (3 mL). All studies were independently evaluated by 2 radiologists for image quality by using a 5-point scale (from 0 = failure to 4 = excellent), grading of arterial stenosis (0 = normal, 1 = mild [<30%], 2 = moderate [30%-69%], 3 = severe to occlusion [≥70%]), and signal-to-noise ratio. The image quality of time-resolved MRA was similar to that of contrast-enhanced MRA in groups B and C, but it was inferior to contrast-enhanced MRA in group A. For the grading of arterial stenosis, there was an excellent correlation between contrast-enhanced MRA and time-resolved MRA ( R = 0.957 for group A, R = 0.988 for group B, R = 0.991 for group C). The SNR of time-resolved MRA tended to be lower than that of contrast-enhanced MRA in groups A and B. However, SNR was higher for time-resolved MRA compared with contrast-enhanced MRA in group C. Low-dose time-resolved MRA is feasible in the evaluation of supra-aortic stenosis and could be used as an alternative to contrast-enhanced MRA for a diagnostic technique in high-risk populations. © 2017 by American Journal of Neuroradiology.

Mapping atomic motions with ultrabright electrons: towards fundamental limits in space-time resolution.

PubMed

Manz, Stephanie; Casandruc, Albert; Zhang, Dongfang; Zhong, Yinpeng; Loch, Rolf A; Marx, Alexander; Hasegawa, Taisuke; Liu, Lai Chung; Bayesteh, Shima; Delsim-Hashemi, Hossein; Hoffmann, Matthias; Felber, Matthias; Hachmann, Max; Mayet, Frank; Hirscht, Julian; Keskin, Sercan; Hada, Masaki; Epp, Sascha W; Flöttmann, Klaus; Miller, R J Dwayne

2015-01-01

The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or "film" for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics.

An experimental investigation of clocking effects on turbine aerodynamics using a modern 3-D one and one-half stage high pressure turbine for code verification and flow model development

NASA Astrophysics Data System (ADS)

Haldeman, Charles Waldo, IV

2003-10-01

This research uses a modern 1 and 1/2 stage high-pressure (HP) turbine operating at the proper design corrected speed, pressure ratio, and gas to metal temperature ratio to generate a detailed data set containing aerodynamic, heat-transfer and aero-performance information. The data was generated using the Ohio State University Gas Turbine Laboratory Turbine Test Facility (TTF), which is a short-duration shock tunnel facility. The research program utilizes an uncooled turbine stage for which all three airfoils are heavily instrumented at multiple spans and on the HPV and LPV endwalls and HPB platform and tips. Heat-flux and pressure data are obtained using the traditional shock-tube and blowdown facility operational modes. Detailed examination show that the aerodynamic (pressure) data obtained in the blowdown mode is the same as obtained in the shock-tube mode when the corrected conditions are matched. Various experimental conditions and configurations were performed, including LPV clocking positions, off-design corrected speed conditions, pressure ratio changes, and Reynolds number changes. The main research for this dissertation is concentrated on the LPV clocking experiments, where the LPV was clocked relative to the HPV at several different passage locations and at different Reynolds numbers. Various methods were used to evaluate the effect of clocking on both the aeroperformance (efficiency) and aerodynamics (pressure loading) on the LPV, including time-resolved measurements, time-averaged measurements and stage performance measurements. A general improvement in overall efficiency of approximately 2% is demonstrated and could be observed using a variety of independent methods. Maximum efficiency is obtained when the time-average pressures are highest on the LPV, and the time-resolved data both in the time domain and frequency domain show the least amount of variation. The gain in aeroperformance is obtained by integrating over the entire airfoil as the three-dimensional effects on the LPV surface are significant.

International Conference on Vacuum Ultraviolet Radiation Physics, 8th, Lunds Universitet, Sweden, Aug. 4-8, 1986, Proceedings

NASA Technical Reports Server (NTRS)

Nilsson, Per-Olof (Editor); Nordgren, Joseph (Editor)

1987-01-01

The interactions of VUV radiation with solids are explored in reviews and reports of recent theoretical and experimental investigations from the fields of atomic and molecular physics, solid-state physics, and VUV instrumentation. Topics examined include photoabsorption and photoionization, multiphoton processes, plasma physics, VUV lasers, time-resolved spectroscopy, synchrotron radiation centers, solid-state spectroscopy, and dynamical processes involving localized levels. Consideration is given to the fundamental principles of photoemission, spin-polarized photoemission, inverse photoemission, semiconductors, organic materials, and adsorbates.

The atmosphere of heaven: the 1799 nitrous oxide researches reconsidered.

PubMed

Jay, Mike

2009-09-20

Thomas Beddoes's and Humphry Davy's accounts of the nitrous oxide experiments carried out at the Pneumatic Institution in 1799 include extravagant descriptions of its mind-altering effects. Many people, both at the time and subsequently, have considered these descriptions to be the product not of the gas but of its subjects' overheated imaginations. To what extent were these effects 'all in the mind' of the experimenters? Modern understandings of nitrous oxide throw new light on this question; but it was also considered, and resolved in different ways, by Beddoes and Davy themselves.

Chemical bond activation observed with an x-ray laser

DOE PAGES

Beye, Martin; Öberg, Henrik; Xin, Hongliang; ...

2016-09-01

The concept of bonding and anti-bonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Lastly, we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding–anti-bonding splitting following bond-activation using an ultra short optical laser pulse.

FESTR: Finite-Element Spectral Transfer of Radiation spectroscopic modeling and analysis code

DOE PAGES

Hakel, Peter

2016-10-01

Here we report on the development of a new spectral postprocessor of hydrodynamic simulations of hot, dense plasmas. Based on given time histories of one-, two-, and three-dimensional spatial distributions of materials, and their local temperature and density conditions, spectroscopically-resolved signals are computed. The effects of radiation emission and absorption by the plasma on the emergent spectra are simultaneously taken into account. This program can also be used independently of hydrodynamic calculations to analyze available experimental data with the goal of inferring plasma conditions.

Local Sampling of the Wigner Function at Telecom Wavelength with Loss-Tolerant Detection of Photon Statistics.

PubMed

Harder, G; Silberhorn, Ch; Rehacek, J; Hradil, Z; Motka, L; Stoklasa, B; Sánchez-Soto, L L

2016-04-01

We report the experimental point-by-point sampling of the Wigner function for nonclassical states created in an ultrafast pulsed type-II parametric down-conversion source. We use a loss-tolerant time-multiplexed detector based on a fiber-optical setup and a pair of photon-number-resolving avalanche photodiodes. By capitalizing on an expedient data-pattern tomography, we assess the properties of the light states with outstanding accuracy. The method allows us to reliably infer the squeezing of genuine two-mode states without any phase reference.

FESTR: Finite-Element Spectral Transfer of Radiation spectroscopic modeling and analysis code

NASA Astrophysics Data System (ADS)

Hakel, Peter

2016-10-01

We report on the development of a new spectral postprocessor of hydrodynamic simulations of hot, dense plasmas. Based on given time histories of one-, two-, and three-dimensional spatial distributions of materials, and their local temperature and density conditions, spectroscopically-resolved signals are computed. The effects of radiation emission and absorption by the plasma on the emergent spectra are simultaneously taken into account. This program can also be used independently of hydrodynamic calculations to analyze available experimental data with the goal of inferring plasma conditions.

Opportunities and challenges for time-resolved studies of protein structural dynamics at X-ray free-electron lasers.

PubMed

Neutze, Richard

2014-07-17

X-ray free-electron lasers (XFELs) are revolutionary X-ray sources. Their time structure, providing X-ray pulses of a few tens of femtoseconds in duration; and their extreme peak brilliance, delivering approximately 10(12) X-ray photons per pulse and facilitating sub-micrometre focusing, distinguish XFEL sources from synchrotron radiation. In this opinion piece, I argue that these properties of XFEL radiation will facilitate new discoveries in life science. I reason that time-resolved serial femtosecond crystallography and time-resolved wide angle X-ray scattering are promising areas of scientific investigation that will be advanced by XFEL capabilities, allowing new scientific questions to be addressed that are not accessible using established methods at storage ring facilities. These questions include visualizing ultrafast protein structural dynamics on the femtosecond to picosecond time-scale, as well as time-resolved diffraction studies of non-cyclic reactions. I argue that these emerging opportunities will stimulate a renaissance of interest in time-resolved structural biochemistry.

A Low-Cost Time-Resolved Spectrometer for the Study of Ruby Emission

ERIC Educational Resources Information Center

McBane, George C.; Cannella, Christian; Schaertel, Stephanie

2018-01-01

A low-cost time-resolved emission spectrometer optimized for ruby emission is presented. The use of a Class II diode laser module as the excitation source reduces costs and hazards. The design presented here can facilitate the inclusion of time-resolved emission spectroscopy with laser excitation sources in the undergraduate laboratory curriculum.…

Cluster Analysis of Time-Dependent Crystallographic Data: Direct Identification of Time-Independent Structural Intermediates

PubMed Central

Kostov, Konstantin S.; Moffat, Keith

2011-01-01

The initial output of a time-resolved macromolecular crystallography experiment is a time-dependent series of difference electron density maps that displays the time-dependent changes in underlying structure as a reaction progresses. The goal is to interpret such data in terms of a small number of crystallographically refinable, time-independent structures, each associated with a reaction intermediate; to establish the pathways and rate coefficients by which these intermediates interconvert; and thereby to elucidate a chemical kinetic mechanism. One strategy toward achieving this goal is to use cluster analysis, a statistical method that groups objects based on their similarity. If the difference electron density at a particular voxel in the time-dependent difference electron density (TDED) maps is sensitive to the presence of one and only one intermediate, then its temporal evolution will exactly parallel the concentration profile of that intermediate with time. The rationale is therefore to cluster voxels with respect to the shapes of their TDEDs, so that each group or cluster of voxels corresponds to one structural intermediate. Clusters of voxels whose TDEDs reflect the presence of two or more specific intermediates can also be identified. From such groupings one can then infer the number of intermediates, obtain their time-independent difference density characteristics, and refine the structure of each intermediate. We review the principles of cluster analysis and clustering algorithms in a crystallographic context, and describe the application of the method to simulated and experimental time-resolved crystallographic data for the photocycle of photoactive yellow protein. PMID:21244840

Shockwave compression of Ar gas at several initial densities

NASA Astrophysics Data System (ADS)

Dattelbaum, Dana M.; Goodwin, Peter M.; Garcia, Daniel B.; Gustavsen, Richard L.; Lang, John M.; Aslam, Tariq D.; Sheffield, Stephen A.; Gibson, Lloyd L.; Morris, John S.

2017-01-01

Experimental data of the principal Hugoniot locus of variable density gas-phase noble and molecular gases are rare. The majority of shock Hugoniot data is either from shock tube experiments on low-pressure gases or from plate impact experiments on cryogenic, liquefied gases. In both cases, physics regarding shock compressibility, thresholds for the on-set of shock-driven ionization, and even dissociation chemistry are difficult to infer for gases at intermediate densities. We have developed an experimental target design for gas gun-driven plate impact experiments on noble gases at initial pressures between 200-1000 psi. Using optical velocimetry, we are able to directly determine both the shock and particle velocities of the gas on the principal Hugoniot locus, as well as clearly differentiate ionization thresholds. The target design also results in multiply shocking the gas in a quasi-isentropic fashion yielding off-Hugoniot compression data. We describe the results of a series of plate impact experiments on Ar with starting densities between 0.02-0.05 g/cm3 at room temperature. Furthermore, by coupling optical fibers to the targets, we have measured the time-resolved optical emission from the shocked gas using a spectrometer coupled to an optical streak camera to spectrally-resolve the emission, and with a 5-color optical pyrometer for temperature determination.

Feasibility demonstration of a massively parallelizable optical near-field sensor for sub-wavelength defect detection and imaging

PubMed Central

Mostafavi, Mahkamehossadat; Diaz, Rodolfo E.

2016-01-01

To detect and resolve sub-wavelength features at optical frequencies, beyond the diffraction limit, requires sensors that interact with the electromagnetic near-field of those features. Most instruments operating in this modality scan a single detector element across the surface under inspection because the scattered signals from a multiplicity of such elements would end up interfering with each other. However, an alternative massively parallelized configuration, capable of interrogating multiple adjacent areas of the surface at the same time, was proposed in 2002. Full physics simulations of the photonic antenna detector element that enables this instrument, show that using conventional red laser light (in the 600 nm range) the detector magnifies the signal from an 8 nm particle by up to 1.5 orders of magnitude. The antenna is a shaped slot element in a 60 nm silver film. The ability of this detector element to resolve λ/78 objects is confirmed experimentally at radio frequencies by fabricating an artificial material structure that mimics the optical permittivity of silver scaled to 2 GHz, and “cutting” into it the slot antenna. The experimental set-up is also used to demonstrate the imaging of a patterned surface in which the critical dimensions of the pattern are λ/22 in size. PMID:27185385

High resolution photoelectron imaging of UO(-) and UO2(-) and the low-lying electronic states and vibrational frequencies of UO and UO2.

PubMed

Czekner, Joseph; Lopez, Gary V; Wang, Lai-Sheng

2014-12-28

We report a study of the electronic and vibrational structures of the gaseous uranium monoxide and dioxide molecules using high-resolution photoelectron imaging. Vibrationally resolved photoelectron spectra are obtained for both UO(-) and UO2(-). The spectra for UO2(-) are consistent with, but much better resolved than a recent study using a magnetic-bottle photoelectron analyzer [W. L. Li et al., J. Chem. Phys. 140, 094306 (2014)]. The electron affinity (EA) of UO is reported for the first time as 1.1407(7) eV, whereas a much more accurate EA is obtained for UO2 as 1.1688(6) eV. The symmetric stretching modes for the neutral and anionic ground states, and two neutral excited states for UO2 are observed, as well as the bending mode for the neutral ground state. These vibrational frequencies are consistent with previous experimental and theoretical results. The stretching vibrational modes for the ground state and one excited state are observed for UO. The current results for UO and UO2 are compared with previous theoretical calculations including relativistic effects and spin-orbit coupling. The accurate experimental data reported here provide more stringent tests for future theoretical methods for actinide-containing species.

Time-resolved computed tomography of the liver: retrospective, multi-phase image reconstruction derived from volumetric perfusion imaging.

PubMed

Fischer, Michael A; Leidner, Bertil; Kartalis, Nikolaos; Svensson, Anders; Aspelin, Peter; Albiin, Nils; Brismar, Torkel B

2014-01-01

To assess feasibility and image quality (IQ) of a new post-processing algorithm for retrospective extraction of an optimised multi-phase CT (time-resolved CT) of the liver from volumetric perfusion imaging. Sixteen patients underwent clinically indicated perfusion CT using 4D spiral mode of dual-source 128-slice CT. Three image sets were reconstructed: motion-corrected and noise-reduced (MCNR) images derived from 4D raw data; maximum and average intensity projections (time MIP/AVG) of the arterial/portal/portal-venous phases and all phases (total MIP/ AVG) derived from retrospective fusion of dedicated MCNR split series. Two readers assessed the IQ, detection rate and evaluation time; one reader assessed image noise and lesion-to-liver contrast. Time-resolved CT was feasible in all patients. Each post-processing step yielded a significant reduction of image noise and evaluation time, maintaining lesion-to-liver contrast. Time MIPs/AVGs showed the highest overall IQ without relevant motion artefacts and best depiction of arterial and portal/portal-venous phases respectively. Time MIPs demonstrated a significantly higher detection rate for arterialised liver lesions than total MIPs/AVGs and the raw data series. Time-resolved CT allows data from volumetric perfusion imaging to be condensed into an optimised multi-phase liver CT, yielding a superior IQ and higher detection rate for arterialised liver lesions than the raw data series. • Four-dimensional computed tomography is limited by motion artefacts and poor image quality. • Time-resolved-CT facilitates 4D-CT data visualisation, segmentation and analysis by condensing raw data. • Time-resolved CT demonstrates better image quality than raw data images. • Time-resolved CT improves detection of arterialised liver lesions in cirrhotic patients.

Theory of time-resolved photoelectron imaging. Comparison of a density functional with a time-dependent density functional approach

NASA Astrophysics Data System (ADS)

Suzuki, Yoshi-ichi; Seideman, Tamar; Stener, Mauro

2004-01-01

Time-resolved photoelectron differential cross sections are computed within a quantum dynamical theory that combines a formally exact solution of the nuclear dynamics with density functional theory (DFT)-based approximations of the electronic dynamics. Various observables of time-resolved photoelectron imaging techniques are computed at the Kohn-Sham and at the time-dependent DFT levels. Comparison of the results serves to assess the reliability of the former method and hence its usefulness as an economic approach for time-domain photoelectron cross section calculations, that is applicable to complex polyatomic systems. Analysis of the matrix elements that contain the electronic dynamics provides insight into a previously unexplored aspect of femtosecond-resolved photoelectron imaging.

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging.

PubMed

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui; Savelyev, Evgeny; Obaid, Razib; Kaderiya, Balram; Augustin, Sven; Schnorr, Kirsten; Dumitriu, Ileana; Osipov, Timur; Bilodeau, René; Kilcoyne, David; Kumarappan, Vinod; Rudenko, Artem; Berrah, Nora; Rolles, Daniel

2016-12-02

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C 2 H 2 Br 2 ). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. The experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model.

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

PubMed Central

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui; Savelyev, Evgeny; Obaid, Razib; Kaderiya, Balram; Augustin, Sven; Schnorr, Kirsten; Dumitriu, Ileana; Osipov, Timur; Bilodeau, René; Kilcoyne, David; Kumarappan, Vinod; Rudenko, Artem; Berrah, Nora; Rolles, Daniel

2016-01-01

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C2H2Br2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. The experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model. PMID:27910943

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

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

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C 2H 2Br 2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. Lastly, the experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model.

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

DOE PAGES

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui; ...

2016-12-02

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C 2H 2Br 2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. Lastly, the experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model.

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

NASA Astrophysics Data System (ADS)

Ogawa, Manami; Yamamoto, Susumu; Kousa, Yuka; Nakamura, Fumitaka; Yukawa, Ryu; Fukushima, Akiko; Harasawa, Ayumi; Kondoh, Hiroshi; Tanaka, Yoshihito; Kakizaki, Akito; Matsuda, Iwao

2012-02-01

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.

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

PubMed

Ogawa, Manami; Yamamoto, Susumu; Kousa, Yuka; Nakamura, Fumitaka; Yukawa, Ryu; Fukushima, Akiko; Harasawa, Ayumi; Kondoh, Hiroshi; Tanaka, Yoshihito; Kakizaki, Akito; Matsuda, Iwao

2012-02-01

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.

Dynamics of nonspherical microbubble oscillations above instability threshold

NASA Astrophysics Data System (ADS)

Guédra, Matthieu; Cleve, Sarah; Mauger, Cyril; Blanc-Benon, Philippe; Inserra, Claude

2017-12-01

Time-resolved dynamics of nonspherical oscillations of micrometer-sized bubbles are captured and analyzed using high-speed imaging. The axisymmetry of the bubble shape is ensured with certainty for the first time from the recordings of two synchronous high-speed cameras located at 90∘. The temporal dynamics of finite-amplitude nonspherical oscillations are then analyzed for various acoustic pressures above the instability threshold. The experimental results are compared with recent theories accounting for nonlinearities and mode coupling, highlighting particular effects inherent to these mechanisms (saturation of the instability, triggering of nonparametric shape modes). Finally, the amplitude of the nonspherical oscillations is given as function of the driving pressure both for quadrupolar and octupolar bubbles.

Rapid 3D NMR using the filter diagonalization method: application to oligosaccharides derivatized with 13C-labeled acetyl groups

NASA Astrophysics Data System (ADS)

Armstrong, Geoffrey S.; Cano, Kristin E.; Mandelshtam, Vladimir A.; Shaka, A. J.; Bendiak, Brad

2004-09-01

Rapid 3D NMR spectroscopy of oligosaccharides having isotopically labeled acetyl "isotags" was made possible with high resolution in the indirect dimensions using the filter diagonalization method (FDM). A pulse sequence was designed for the optimal correlation of acetyl methyl protons, methyl carbons, and carbonyl carbons. The multi-dimensional nature of the FDM, coupled with the advantages of constant-time evolution periods, resulted in marked improvements over Fourier transform (FT) and mirror-image linear prediction (MI-LP) processing methods. The three methods were directly compared using identical data sets. A highly resolved 3D spectrum was achieved with the FDM using a very short experimental time (28 min).

Rapid 3D NMR using the filter diagonalization method: application to oligosaccharides derivatized with 13C-labeled acetyl groups.

PubMed

Armstrong, Geoffrey S; Cano, Kristin E; Mandelshtam, Vladimir A; Shaka, A J; Bendiak, Brad

2004-09-01

Rapid 3D NMR spectroscopy of oligosaccharides having isotopically labeled acetyl "isotags" was made possible with high resolution in the indirect dimensions using the filter diagonalization method (FDM). A pulse sequence was designed for the optimal correlation of acetyl methyl protons, methyl carbons, and carbonyl carbons. The multi-dimensional nature of the FDM, coupled with the advantages of constant-time evolution periods, resulted in marked improvements over Fourier transform (FT) and mirror-image linear prediction (MI-LP) processing methods. The three methods were directly compared using identical data sets. A highly resolved 3D spectrum was achieved with the FDM using a very short experimental time (28 min).

Photon diffusion coefficient in scattering and absorbing media.

PubMed

Pierrat, Romain; Greffet, Jean-Jacques; Carminati, Rémi

2006-05-01

We present a unified derivation of the photon diffusion coefficient for both steady-state and time-dependent transport in disordered absorbing media. The derivation is based on a modal analysis of the time-dependent radiative transfer equation. This approach confirms that the dynamic diffusion coefficient is given by the random-walk result D = cl(*)/3, where l(*) is the transport mean free path and c is the energy velocity, independent of the level of absorption. It also shows that the diffusion coefficient for steady-state transport, often used in biomedical optics, depends on absorption, in agreement with recent theoretical and experimental works. These two results resolve a recurrent controversy in light propagation and imaging in scattering media.

Theory of retrieving orientation-resolved molecular information using time-domain rotational coherence spectroscopy

NASA Astrophysics Data System (ADS)

Wang, Xu; Le, Anh-Thu; Zhou, Zhaoyan; Wei, Hui; Lin, C. D.

2017-08-01

We provide a unified theoretical framework for recently emerging experiments that retrieve fixed-in-space molecular information through time-domain rotational coherence spectroscopy. Unlike a previous approach by Makhija et al. (V. Makhija et al., arXiv:1611.06476), our method can be applied to the retrieval of both real-valued (e.g., ionization yield) and complex-valued (e.g., induced dipole moment) molecular response information. It is also a direct retrieval method without using iterations. We also demonstrate that experimental parameters, such as the fluence of the aligning laser pulse and the rotational temperature of the molecular ensemble, can be quite accurately determined using a statistical method.

Floquet Engineering of Correlated Tunneling in the Bose-Hubbard Model with Ultracold Atoms.

PubMed

Meinert, F; Mark, M J; Lauber, K; Daley, A J; Nägerl, H-C

2016-05-20

We report on the experimental implementation of tunable occupation-dependent tunneling in a Bose-Hubbard system of ultracold atoms via time-periodic modulation of the on-site interaction energy. The tunneling rate is inferred from a time-resolved measurement of the lattice site occupation after a quantum quench. We demonstrate coherent control of the tunneling dynamics in the correlated many-body system, including full suppression of tunneling as predicted within the framework of Floquet theory. We find that the tunneling rate explicitly depends on the atom number difference in neighboring lattice sites. Our results may open up ways to realize artificial gauge fields that feature density dependence with ultracold atoms.

Experimental framework to study tip vortex interactions in multirotor wakes

NASA Astrophysics Data System (ADS)

Yao, Rongnan; Araya, Daniel

2017-11-01

We present an experimental study to compare the dynamic characteristics of tip vortices shed from a propeller in a crossflow to similar characteristics of an isolated vortex column generated in a closed system. Our aim is to evaluate the feasibility of using this simple isolated system to study the more complicated three-dimensional vortex interactions inherent to multirotor wakes, where the local unsteadiness generated by one rotor can strongly impact the performance of nearby rotors. Time-resolved particle image velocimetry is used to measure the velocity field of the propeller wake flow in a wind tunnel and the vortex column in a water tank. Specific attention is placed on analyzing the observed vortex core precession in the isolated system and comparing this to characteristic tip-vortex wandering phenomenon.

Photoinduced random molecular reorientation by nonradiative energy relaxation: An experimental test

NASA Astrophysics Data System (ADS)

Manzo, C.; Paparo, D.; Marrucci, L.

2004-11-01

By measuring the time-resolved fluorescence depolarization as a function of light excitation wavelength we address the question of a possible photoinduced orientational randomization of amino-anthraquinone dyes in liquid solutions. We find no significant dependence within the experimental uncertainties of both the initial molecule anisotropy and of the subsequent rotational diffusion dynamics on the photon energy. This indicates that this effect, if present, must be very small. A simple model of photoinduced local heating and corresponding enhanced rotational diffusion is in accordance with this result. This null result rules out some recent proposals that photoinduced local heating may contribute significantly to molecular reorientation effects in different materials. A small but statistically significant effect of photon energy is instead found in the excited-state lifetime of the dye.

A technique for measurement of instantaneous heat transfer in steady-flow ambient-temperature facilities

NASA Technical Reports Server (NTRS)

O'Brien, James E.

1990-01-01

An experimental technique is described for obtaining time-resolved heat flux measurements with high-frequency response (up to 100 kHz) in a steady-flow ambient-temperature facility. The heat transfer test object is preheated and suddenly injected into an established steady flow. Thin-film gages deposited on the test surface detect the unsteady substrate surface temperature. Analog circuitry designed for use in short-duration facilities and based on one-dimensional semiinfinite heat conduction is used to perform the temperature/heat flux transformation. A detailed description of substrate properties, instrumentation, experimental procedure, and data reduction is given, along with representative results obtained in the stagnation region of a circular cylinder subjected to a wake-dominated unsteady flow. An in-depth discussion of related work is also provided.

Plume splitting and oscillatory behavior in transient plasmas generated by high-fluence laser ablation in vacuum

NASA Astrophysics Data System (ADS)

Focsa, C.; Gurlui, S.; Nica, P.; Agop, M.; Ziskind, M.

2017-12-01

We present a short overview of studies performed in our research groups over the last decade on the characterization of transient plasma plumes generated by laser ablation in various temporal regimes, from nanosecond to femtosecond. New results are also presented along with this overview, both being placed in the context of similar studies performed by other investigators. Optical (fast gate intensified CCD camera imaging and space- and time-resolved emission spectroscopy) and electrical (mainly Langmuir probe) methods have been applied to experimentally explore the dynamics of the plasma plume and its constituents. Peculiar effects as plume splitting and sharpening or oscillations onset have been evidenced in vacuum at high laser fluence. New theoretical approaches have been developed to account for the experimental observations.

Primary separation between three aircraft using traffic displays

NASA Technical Reports Server (NTRS)

Chappell, S. L.; Palmer, E. A.

1983-01-01

The use of a sophisticated traffic and map display termed electronic flight rules (EFR) by general aviation pilots for primary seperation in low density airspace is studied. The experimental flights were made under four conditions: with and without sensor noise in the traffic information and with and without communications for traffic coordination. Pilots were required to maintain two miles horizontal and 500 ft vertical separation from other aircraft for 24 different traffic situations repeated randomly for each of the four experimental conditions. Of 1152 aircraft encounters 12.8 percent were in violation of separation minimums. In general, the effects of sensor noise were minimal, communications affected some of the measures, and the group effect was quite significant. When pilots were able to communicate and coordinate their maneuvers, the time to resolve conflict was reduced.

Sensitivity-encoded (SENSE) proton echo-planar spectroscopic imaging (PEPSI) in the human brain.

PubMed

Lin, Fa-Hsuan; Tsai, Shang-Yueh; Otazo, Ricardo; Caprihan, Arvind; Wald, Lawrence L; Belliveau, John W; Posse, Stefan

2007-02-01

Magnetic resonance spectroscopic imaging (MRSI) provides spatially resolved metabolite information that is invaluable for both neuroscience studies and clinical applications. However, lengthy data acquisition times, which are a result of time-consuming phase encoding, represent a major challenge for MRSI. Fast MRSI pulse sequences that use echo-planar readout gradients, such as proton echo-planar spectroscopic imaging (PEPSI), are capable of fast spectral-spatial encoding and thus enable acceleration of image acquisition times. Combining PEPSI with recent advances in parallel MRI utilizing RF coil arrays can further accelerate MRSI data acquisition. Here we investigate the feasibility of ultrafast spectroscopic imaging at high field (3T and 4T) by combining PEPSI with sensitivity-encoded (SENSE) MRI using eight-channel head coil arrays. We show that the acquisition of single-average SENSE-PEPSI data at a short TE (15 ms) can be accelerated to 32 s or less, depending on the field strength, to obtain metabolic images of choline (Cho), creatine (Cre), N-acetyl-aspartate (NAA), and J-coupled metabolites (e.g., glutamate (Glu) and inositol (Ino)) with acceptable spectral quality and localization. The experimentally measured reductions in signal-to-noise ratio (SNR) and Cramer-Rao lower bounds (CRLBs) of metabolite resonances were well explained by both the g-factor and reduced measurement times. Thus, this technology is a promising means of reducing the scan times of 3D acquisitions and time-resolved 2D measurements. Copyright (c) 2007 Wiley-Liss, Inc.

Twin-mediated crystal growth: an enigma resolved

PubMed Central

Shahani, Ashwin J.; Gulsoy, E. Begum; Poulsen, Stefan O.; Xiao, Xianghui; Voorhees, Peter W.

2016-01-01

During crystal growth, faceted interfaces may be perturbed by defects, leading to a rich variety of polycrystalline growth forms. One such defect is the coherent Σ3 {111} twin boundary, which is widely known to catalyze crystal growth. These defects have a profound effect on the properties of many materials: for example, electron-hole recombination rates strongly depend on the character of the twin boundaries in polycrystalline Si photovoltaic cells. However, the morphology of the twinned interface during growth has long been a mystery due to the lack of four-dimensional (i.e., space and time resolved) experiments. Many controversial mechanisms have been proposed for this process, most of which lack experimental verification. Here, we probe the real-time interfacial dynamics of polycrystalline Si particles growing from an Al-Si-Cu liquid via synchrotron-based X-ray tomography. Our novel analysis of the time evolution of the interfacial normals allows us to quantify unambiguously the habit plane and grain boundary orientations during growth. This, when combined with direct measurements of the interfacial morphology provide the first confirmation of twin-mediated growth, proposed over 50 years ago. Using the insights provided by these experiments, we have developed a unified picture of the phenomena responsible for the dynamics of faceted Si growth. PMID:27346073

Miniaturization of the Clonogenic Assay Using Confluence Measurement

PubMed Central

Mayr, Christian; Beyreis, Marlena; Dobias, Heidemarie; Gaisberger, Martin; Pichler, Martin; Ritter, Markus; Jakab, Martin; Neureiter, Daniel; Kiesslich, Tobias

2018-01-01

The clonogenic assay is a widely used method to study the ability of cells to ‘infinitely’ produce progeny and is, therefore, used as a tool in tumor biology to measure tumor-initiating capacity and stem cell status. However, the standard protocol of using 6-well plates has several disadvantages. By miniaturizing the assay to a 96-well microplate format, as well as by utilizing the confluence detection function of a multimode reader, we here describe a new and modified protocol that allows comprehensive experimental setups and a non-endpoint, label-free semi-automatic analysis. Comparison of bright field images with confluence images demonstrated robust and reproducible detection of clones by the confluence detection function. Moreover, time-resolved non-endpoint confluence measurement of the same well showed that semi-automatic analysis was suitable for determining the mean size and colony number. By treating cells with an inhibitor of clonogenic growth (PTC-209), we show that our modified protocol is suitable for comprehensive (broad concentration range, addition of technical replicates) concentration- and time-resolved analysis of the effect of substances or treatments on clonogenic growth. In summary, this protocol represents a time- and cost-effective alternative to the commonly used 6-well protocol (with endpoint staining) and also provides additional information about the kinetics of clonogenic growth. PMID:29510509

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

NASA Astrophysics Data System (ADS)

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.

Measurement of Coherence Decay in GaMnAs Using Femtosecond Four-wave Mixing

PubMed Central

Webber, Daniel; de Boer, Tristan; Yildirim, Murat; March, Sam; Mathew, Reuble; Gamouras, Angela; Liu, Xinyu; Dobrowolska, Margaret; Furdyna, Jacek; Hall, Kimberley

2013-01-01

The application of femtosecond four-wave mixing to the study of fundamental properties of diluted magnetic semiconductors ((s,p)-d hybridization, spin-flip scattering) is described, using experiments on GaMnAs as a prototype III-Mn-V system.  Spectrally-resolved and time-resolved experimental configurations are described, including the use of zero-background autocorrelation techniques for pulse optimization.  The etching process used to prepare GaMnAs samples for four-wave mixing experiments is also highlighted.  The high temporal resolution of this technique, afforded by the use of short (20 fsec) optical pulses, permits the rapid spin-flip scattering process in this system to be studied directly in the time domain, providing new insight into the strong exchange coupling responsible for carrier-mediated ferromagnetism.  We also show that spectral resolution of the four-wave mixing signal allows one to extract clear signatures of (s,p)-d hybridization in this system, unlike linear spectroscopy techniques.   This increased sensitivity is due to the nonlinearity of the technique, which suppresses defect-related contributions to the optical response. This method may be used to measure the time scale for coherence decay (tied to the fastest scattering processes) in a wide variety of semiconductor systems of interest for next generation electronics and optoelectronics. PMID:24326982

Time-Resolved Analysis of Cytosolic and Surface-Associated Proteins of Staphylococcus aureus HG001 under Planktonic and Biofilm Conditions.

PubMed

Moche, Martin; Schlüter, Rabea; Bernhardt, Jörg; Plate, Kristina; Riedel, Katharina; Hecker, Michael; Becher, Dörte

2015-09-04

Staphylococcal biofilms are associated with persistent infections due to their capacity to protect bacteria against the host's immune system and antibiotics. Cell-surface-associated proteins are of great importance during biofilm formation. In the present study, an optimized biotinylation approach for quantitative GeLC-MS-based analysis of the staphylococcal cell-surface proteome was applied and the cytoplasmic protein fraction was analyzed to elucidate proteomic differences between colony biofilms and planktonic cells. The experimental setup enabled a time-resolved monitoring of the proteome under both culture conditions and the comparison of biofilm cells to planktonic cells at several time points. This allowed discrimination of differences attributed to delayed growth phases from responses provoked by biofilm conditions. Biofilm cells expressed CcpA-dependent catabolic proteins earlier than planktonic cells and strongly accumulated proteins that belong to the SigB stress regulon. The amount of the cell-surface protein and virulence gene regulator Rot decreased within biofilms and MgrA-dependent regulations appeared more pronounced. Biofilm cells simultaneously up-regulated activators (e.g., SarZ) as well as repressors (e.g., SarX) of RNAIII. A decreased amount of high-affinity iron uptake systems and an increased amount of the iron-storage protein FtnA possibly indicated a lower demand of iron in biofilms.

Dynamic organization of myristoylated Src in the live cell plasma membrane

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

Smith, Adam W.; Huang, Hector H.; Endres, Nicholas F.

The spatial organization of lipid-anchored proteins in the plasma membrane directly influences cell signaling, but measuring such organization in situ is experimentally challenging. The canonical oncogene, c-Src, is a lipid anchored protein that plays a key role in integrin-mediated signal transduction within focal adhesions and cell–cell junctions. Because of its activity in specific plasma membrane regions, structural motifs within the protein have been hypothesized to play an important role in its subcellular localization. This study used a combination of time-resolved fluorescence fluctuation spectroscopy and super-resolution microscopy to quantify the dynamic organization of c-Src in live cell membranes. Pulsed-interleaved excitation fluorescencemore » cross-correlation spectroscopy (PIE–FCCS) showed that a small fraction of c-Src transiently sorts into membrane clusters that are several times larger than the monomers. Photoactivated localization microscopy (PALM) confirmed that c-Src partitions into clusters with low probability and showed that the characteristic size of the clusters is 10–80 nm. Finally, time-resolved fluorescence anisotropy measurements were used to quantify the rotational mobility of c-Src to determine how it interacts with its local environment. Altogether, these results build a quantitative description of the mobility and clustering behavior of the c-Src nonreceptor tyrosine kinase in the live cell plasma membrane.« less

Dynamic organization of myristoylated Src in the live cell plasma membrane

DOE PAGES

Smith, Adam W.; Huang, Hector H.; Endres, Nicholas F.; ...

2016-01-15

The spatial organization of lipid-anchored proteins in the plasma membrane directly influences cell signaling, but measuring such organization in situ is experimentally challenging. The canonical oncogene, c-Src, is a lipid anchored protein that plays a key role in integrin-mediated signal transduction within focal adhesions and cell–cell junctions. Because of its activity in specific plasma membrane regions, structural motifs within the protein have been hypothesized to play an important role in its subcellular localization. This study used a combination of time-resolved fluorescence fluctuation spectroscopy and super-resolution microscopy to quantify the dynamic organization of c-Src in live cell membranes. Pulsed-interleaved excitation fluorescencemore » cross-correlation spectroscopy (PIE–FCCS) showed that a small fraction of c-Src transiently sorts into membrane clusters that are several times larger than the monomers. Photoactivated localization microscopy (PALM) confirmed that c-Src partitions into clusters with low probability and showed that the characteristic size of the clusters is 10–80 nm. Finally, time-resolved fluorescence anisotropy measurements were used to quantify the rotational mobility of c-Src to determine how it interacts with its local environment. Altogether, these results build a quantitative description of the mobility and clustering behavior of the c-Src nonreceptor tyrosine kinase in the live cell plasma membrane.« less

Time-resolved microplasma excitation temperature in a pulsed microwave discharge

NASA Astrophysics Data System (ADS)

Hopwood, Jeffrey; Monfared, Shabnam; Hoskinson, Alan

2013-09-01

Microwave-driven microplasmas are usually operated in a steady-state mode such that the electron temperature is constant in time. Transient measurements of excitation temperature and helium emission lines, however, suggest that short microwave pulses can be used to raise the electron energy by 20-30% for approximately 100 ns. Time-resolved optical emission spectrometry reveals an initial burst of light emission from the igniting microplasma. This emission overshoot is also correlated with a measured increase in excitation temperature. Excimer emission lags atomic emission, however, and does not overshoot. A simple model demonstrates that an increase in electron temperature is responsible for the overshoot of atomic optical emission at the beginning of each microwave pulse. The formation of dimers and subsequent excimer emission requires slower three-body collisions with the excited rare gas atom; this is why excimer emission does not overshoot the steady state value. Similar experimental and modeling results are observed in argon gas. The overshoot in electron temperature may be used to manipulate the collisional production of species in microplasmas using short, low-duty cycle microwave pulses. This material is based upon work supported by the USAF and Physical Sciences Inc., under contract No. FA8650-C-12-C-2312. Additional support was provided by the DARPA MPD program under award FA9550-12-1-0006.

Energy research with neutrons (ErwiN) and installation of a fast neutron powder diffraction option at the MLZ, Germany1

PubMed Central

Mühlbauer, Martin J.

2018-01-01

The need for rapid data collection and studies of small sample volumes in the range of cubic millimetres are the main driving forces for the concept of a new high-throughput monochromatic diffraction instrument at the Heinz Maier-Leibnitz Zentrum (MLZ), Germany. A large region of reciprocal space will be accessed by a detector with sufficient dynamic range and microsecond time resolution, while allowing for a variety of complementary sample environments. The medium-resolution neutron powder diffraction option for ‘energy research with neutrons’ (ErwiN) at the high-flux FRM II neutron source at the MLZ is foreseen to meet future demand. ErwiN will address studies of energy-related systems and materials with respect to their structure and uniformity by means of bulk and spatially resolved neutron powder diffraction. A set of experimental options will be implemented, enabling time-resolved studies, rapid parametric measurements as a function of external parameters and studies of small samples using an adapted radial collimator. The proposed powder diffraction option ErwiN will bridge the gap in functionality between the high-resolution powder diffractometer SPODI and the time-of-flight diffractometers POWTEX and SAPHiR at the MLZ. PMID:29896055

Optical Manipulation and Detection of Emergent Phenomena in Topological Insulators

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

Gedik, Nuh

The three-dimensional topological insulator (TI) is a new quantum phase of matter that exhibits quantum-Hall-like properties, even in the absence of an external magnetic field. These materials are insulators in the bulk but have a topologically protected conducting state at the surface. Charge carriers on these surface states behave like a two-dimensional gas of massless helical Dirac fermions for which the spin is ideally locked perpendicular to the momentum. The purpose of this project is to probe the unique collective electronic behaviors of topological insulators by developing and using advanced time resolved spectroscopic techniques with state-of-the-art temporal and spatial resolutions.more » The nature of these materials requires development of specialized ultrafast techniques (such as time resolved ARPES that also has spin detection capability, ultrafast electron diffraction that has sub-100 fs time resolution and THz magneto-spectroscopy). The focus of this report is to detail our achievements in terms of establishing state of the art experimental facilities. Below, we will describe achievements under this award for the entire duration of five years. We will focus on detailing the development of ultrafast technqiues here. The details of the science that was done with these technqiues can be found in the publications referencing this grant.« less

Twin-mediated crystal growth: an enigma resolved

NASA Astrophysics Data System (ADS)

Shahani, Ashwin J.; Gulsoy, E. Begum; Poulsen, Stefan O.; Xiao, Xianghui; Voorhees, Peter W.

2016-06-01

During crystal growth, faceted interfaces may be perturbed by defects, leading to a rich variety of polycrystalline growth forms. One such defect is the coherent Σ3 {111} twin boundary, which is widely known to catalyze crystal growth. These defects have a profound effect on the properties of many materials: for example, electron-hole recombination rates strongly depend on the character of the twin boundaries in polycrystalline Si photovoltaic cells. However, the morphology of the twinned interface during growth has long been a mystery due to the lack of four-dimensional (i.e., space and time resolved) experiments. Many controversial mechanisms have been proposed for this process, most of which lack experimental verification. Here, we probe the real-time interfacial dynamics of polycrystalline Si particles growing from an Al-Si-Cu liquid via synchrotron-based X-ray tomography. Our novel analysis of the time evolution of the interfacial normals allows us to quantify unambiguously the habit plane and grain boundary orientations during growth. This, when combined with direct measurements of the interfacial morphology provide the first confirmation of twin-mediated growth, proposed over 50 years ago. Using the insights provided by these experiments, we have developed a unified picture of the phenomena responsible for the dynamics of faceted Si growth.

Effects of Blade Boundary Layer Transition and Daytime Atmospheric Turbulence on Wind Turbine Performance Analyzed with Blade-Resolved Simulation and Field Data

NASA Astrophysics Data System (ADS)

Nandi, Tarak Nath

Relevant to utility scale wind turbine functioning and reliability, the present work focuses on enhancing our understanding of wind turbine responses from interactions between energy-dominant daytime atmospheric turbulence eddies and rotating blades of a GE 1.5 MW wind turbine using a unique data set from a GE field experiment and computer simulations at two levels of fidelity. Previous studies have shown that the stability state of the lower troposphere has a major impact on the coherent structure of the turbulence eddies, with corresponding differences in wind turbine loading response. In this study, time-resolved aerodynamic data measured locally at the leading edge and trailing edge of three outer blade sections on a GE 1.5 MW wind turbine blade and high-frequency SCADA generator power data from a daytime field campaign are combined with computer simulations that mimic the GE wind turbine within a numerically generated atmospheric boundary layer (ABL) flow field which is a close approximation of the atmospheric turbulence experienced by the wind turbine in the field campaign. By combining the experimental and numerical data sets, this study describes the time-response characteristics of the local loadings on the blade sections in response to nonsteady nonuniform energetic atmospheric turbulence eddies within a daytime ABL which have spatial scale commensurate with that of the turbine blade length. This study is the first of its kind where actuator line and blade boundary layer resolved CFD studies of a wind turbine field campaign are performed with the motivation to validate the numerical predictions with the experimental data set, and emphasis is given on understanding the influence of the laminar to turbulent transition process on the blade loadings. The experimental and actuator line method data sets identify three important response time scales quantified at the blade location: advective passage of energy-dominant eddies (≈25 - 50 s), blade rotation (1P, ≈3 s) and sub-1P scale (< 1 s) response to internal eddy structure. Large amplitude short-time ramp-like and oscillatory load fluctuations result in response to temporal changes in velocity vector inclination in the airfoil plane, modulated by eddy passage at longer time scales. Generator power is found to respond strongly to large-eddy wind modulations. The experimental data show that internal dynamics of blade boundary layer near the trailing edge is temporally modulated by the nonsteady external ABL flow that was measured at the leading edge, as well as blade generated turbulence motions. A blade boundary layer resolved CFD study of a GE 1.5MW wind turbine blade is carried out using a hybrid URANS/LES framework to quantify the influence of transition on the blade boundary layer dynamics and subsequent loadings, and also to predict the velocity magnitude data set measured by the trailing edge rakes in the experiment. A URANS based transition model is used as the near-wall model, and its ability to predict nonsteady boundary layer dynamics is assessed for flow over an oscillating airfoil exhibiting varying extents of nonsteady behavior. The CFD study shows that, at rated conditions, the transition and separation locations on the blade surface can be quite dynamic, but the transitional flow has negligible influence on the determination of the separation location and the overall pressure distribution at various blade sections, and subsequently the power output. But this conclusion should be accepted with caution for wind turbines running in off-design conditions (e.g. with significant yaw error, off-design pitch or rapid changes in pitch), where massive separation and dynamic stall may occur. Analysis of the near-blade flow field shows strong three dimensional flow in the inboard regions, which can possibly weaken the chordwise flow in the relatively outboard regions and make them more prone to separation. The trailing edge velocity profiles show qualitative resemblance with some specific cycles observed in the field experiment. The factors leading to the observed differences from the experimental data are also mentioned.

Thermal Management Using Pulsating Jet Cooling Technology

NASA Astrophysics Data System (ADS)

Alimohammadi, S.; Dinneen, P.; Persoons, T.; Murray, D. B.

2014-07-01

The existing methods of heat removal from compact electronic devises are known to be deficient as the evolving technology demands more power density and accordingly better cooling techniques. Impinging jets can be used as a satisfactory method for thermal management of electronic devices with limited space and volume. Pulsating flows can produce an additional enhancement in heat transfer rate compared to steady flows. This article is part of a comprehensive experimental and numerical study performed on pulsating jet cooling technology. The experimental approach explores heat transfer performance of a pulsating air jet impinging onto a flat surface for nozzle-to-surface distances 1 <= H/D <= 6, Reynolds numbers 1,300 <= Re <= 2,800 pulsation frequency 2Hz <= f <= 65Hz, and Strouhal number 0.0012 <= Sr = fD/Um <= 0.084. The time-resolved velocity at the nozzle exit is measured to quantify the turbulence intensity profile. The numerical methodology is firstly validated using the experimental local Nusselt number distribution for the steady jet with the same geometry and boundary conditions. For a time-averaged Reynolds number of 6,000, the heat transfer enhancement using the pulsating jet for 9Hz <= f <= 55Hz and 0.017 <= Sr <= 0.102 and 1 <= H/D <= 6 are calculated. For the same range of Sr number, the numerical and experimental methods show consistent results.

Quantitative characterization of steady and time-varying, sooting, laminar diffusion flames using optical techniques

NASA Astrophysics Data System (ADS)

Connelly, Blair C.

In order to reduce the emission of pollutants such as soot and NO x from combustion systems, a detailed understanding of pollutant formation is required. In addition to environmental concerns, this is important for a fundamental understanding of flame behavior as significant quantities of soot lower local flame temperatures, increase overall flame length and affect the formation of such temperature-dependent species as NOx. This problem is investigated by carrying out coupled computational and experimental studies of steady and time-varying sooting, coflow diffusion flames. Optical diagnostic techniques are a powerful tool for characterizing combustion systems, as they provide a noninvasive method of probing the environment. Laser diagnostic techniques have added advantages, as systems can be probed with high spectral, temporal and spatial resolution, and with species selectivity. Experimental soot volume fractions were determined by using two-dimensional laser-induced incandescence (LII), calibrated with an on-line extinction measurement, and soot pyrometry. Measurements of soot particle size distributions are made using time-resolved LII (TR-LII). Laser-induced fluorescence measurements are made of NO and formaldehyde. These experimental measurements, and others, are compared with computational results in an effort to understand and model soot formation and to examine the coupled relationship of soot and NO x formation.

Time-resolved optical studies of wide-gap II-VI semiconductor heterostructures

NASA Astrophysics Data System (ADS)

Wang, Hong

ZnSe and ZnSe-based quantum well and superlattice structures are potential candidates for light emitting devices and other optical devices such as switches and modulators working in the blue-green wavelength range. Carrier dynamics studies of these structures are important in evaluating device performance as well as understanding the underlying physical processes. In this thesis, a carrier dynamics investigation is conducted for temperature from 77K to 295K on CdZnSSe/ZnSSe single quantum well structure (SQW) and ZnSe/ZnSTe superlattice fabricated by molecular beam epitaxy (MBE). Two experimental techniques with femtosecond time resolution are used in this work: up-conversion technique for time- resolved photoluminescence (PL) and pump-probe technique for time-resolved differential absorption studies. For both heterostructures, the radiative recombination is dominated by exciton transition due to the large exciton binding energy as a result of quantum confinement effect. The measured decay time of free exciton PL in CdZnSSe/ZnSSe SQW increases linearly with increasing temperature which agrees with the theoretical prediction by considering the conservation of momentum requirement for radiative recombination. However, the recombination of free carriers is also observed in CdZnSSe/ZnSSe SQW for the whole temperature range studied. On the other hand, in ZnSe/ZnSTe superlattice structures, the non- radiative recombination processes are non-negligible even at 77K and become more important in higher temperature range. The relaxation processes such as spectral hole burning, carrier thermalization and hot-carrier cooling are observed in ZnSe/ZnSTe superlattices at room temperature (295K) by the femtosecond pump-probe measurements. A rapid cooling of the thermalized hot- carrier from 763K to 450K within 4ps is deduced. A large optical nonlinearity (i.e., the induced absorption change) around the heavy-hole exciton energy is also obtained.

Quasi-Steady-State Analysis based on Structural Modules and Timed Petri Net Predict System's Dynamics: The Life Cycle of the Insulin Receptor.

PubMed

Scheidel, Jennifer; Lindauer, Klaus; Ackermann, Jörg; Koch, Ina

2015-12-17

The insulin-dependent activation and recycling of the insulin receptor play an essential role in the regulation of the energy metabolism, leading to a special interest for pharmaceutical applications. Thus, the recycling of the insulin receptor has been intensively investigated, experimentally as well as theoretically. We developed a time-resolved, discrete model to describe stochastic dynamics and study the approximation of non-linear dynamics in the context of timed Petri nets. Additionally, using a graph-theoretical approach, we analyzed the structure of the regulatory system and demonstrated the close interrelation of structural network properties with the kinetic behavior. The transition invariants decomposed the model into overlapping subnetworks of various sizes, which represent basic functional modules. Moreover, we computed the quasi-steady states of these subnetworks and demonstrated that they are fundamental to understand the dynamic behavior of the system. The Petri net approach confirms the experimental results of insulin-stimulated degradation of the insulin receptor, which represents a common feature of insulin-resistant, hyperinsulinaemic states.

Molten nitrate salt technology development

NASA Astrophysics Data System (ADS)

Carling, R. W.

1981-04-01

This paper presents an overview of the experimental programs underway in support of the Thermal Energy Storage for Solar Thermal Applications (TESSTA) program. The experimental programs are concentrating on molten nitrate salts which have been proposed as heat transfer and energy storage medium. The salt composition of greatest interest is drawsalt, nominally a 50-50 molar mixture of NaNO3 and KNO3 with a melting point of 220 C. Several technical uncertainties have been identified that must be resolved before nitrate based solar plants can be commercialized. Research programs at Sandia National Laboratories, universities, and industrial suppliers have been implemented to resolve these technical uncertainties. The experimental programs involve corrosion, decomposition, physical properties, and environmental cracking. Summaries of each project and how they impact central receiver applications such as the repowering/industrial retrofit and cogeneration program are presented.

Toward Femtosecond Time-Resolved Studies of Solvent-Solute Energy Transfer in Doped Helium Nanodroplets

NASA Astrophysics Data System (ADS)

Bacellar, C.; Ziemkiewicz, M. P.; Leone, S. R.; Neumark, D. M.; Gessner, O.

2015-05-01

Superfluid helium nanodroplets provide a unique cryogenic matrix for high resolution spectroscopy and ultracold chemistry applications. With increasing photon energy and, in particular, in the increasingly important Extreme Ultraviolet (EUV) regime, the droplets become optically dense and, therefore, participate in the EUV-induced dynamics. Energy- and charge-transfer mechanisms between the host droplets and dopant atoms, however, are poorly understood. Static energy domain measurements of helium droplets doped with noble gas atoms (Xe, Kr) indicate that Penning ionization due to energy transfer from the excited droplet to dopant atoms may be a significant relaxation channel. We have set up a femtosecond time-resolved photoelectron imaging experiment to probe these dynamics directly in the time-domain. Droplets containing 104 to 106 helium atoms and a small percentage (<10-4) of dopant atoms (Xe, Kr, Ne) are excited to the 1s2p Rydberg band by 21.6 eV photons produced by high harmonic generation (HHG). Transiently populated states are probed by 1.6 eV photons, generating time-dependent photoelectron kinetic energy distributions, which are monitored by velocity map imaging (VMI). The results will provide new information about the dynamic timescales and the different relaxation channels, giving access to a more complete physical picture of solvent-solute interactions in the superfluid environment. Prospects and challenges of the novel experiment as well as preliminary experimental results will be discussed.

Recent Advances in 3D Time-Resolved Contrast-Enhanced MR Angiography

PubMed Central

Riederer, Stephen J.; Haider, Clifton R.; Borisch, Eric A.; Weavers, Paul T.; Young, Phillip M.

2015-01-01

Contrast-enhanced MR angiography (CE-MRA) was first introduced for clinical studies approximately 20 years ago. Early work provided 3 to 4 mm spatial resolution with acquisition times in the 30 sec range. Since that time there has been continuing effort to provide improved spatial resolution with reduced acquisition time, allowing high resolution three-dimensional (3D) time-resolved studies. The purpose of this work is to describe how this has been accomplished. Specific technical enablers have been: improved gradients allowing reduced repetition times, improved k-space sampling and reconstruction methods, parallel acquisition particularly in two directions, and improved and higher count receiver coil arrays. These have collectively made high resolution time-resolved studies readily available for many anatomic regions. Depending on the application, approximate 1 mm isotropic resolution is now possible with frame times of several seconds. Clinical applications of time-resolved CE-MRA are briefly reviewed. PMID:26032598

Modelling Short-Term Maximum Individual Exposure from Airborne Hazardous Releases in Urban Environments. Part ΙI: Validation of a Deterministic Model with Wind Tunnel Experimental Data.

PubMed

Efthimiou, George C; Bartzis, John G; Berbekar, Eva; Hertwig, Denise; Harms, Frank; Leitl, Bernd

2015-06-26

The capability to predict short-term maximum individual exposure is very important for several applications including, for example, deliberate/accidental release of hazardous substances, odour fluctuations or material flammability level exceedance. Recently, authors have proposed a simple approach relating maximum individual exposure to parameters such as the fluctuation intensity and the concentration integral time scale. In the first part of this study (Part I), the methodology was validated against field measurements, which are governed by the natural variability of atmospheric boundary conditions. In Part II of this study, an in-depth validation of the approach is performed using reference data recorded under truly stationary and well documented flow conditions. For this reason, a boundary-layer wind-tunnel experiment was used. The experimental dataset includes 196 time-resolved concentration measurements which detect the dispersion from a continuous point source within an urban model of semi-idealized complexity. The data analysis allowed the improvement of an important model parameter. The model performed very well in predicting the maximum individual exposure, presenting a factor of two of observations equal to 95%. For large time intervals, an exponential correction term has been introduced in the model based on the experimental observations. The new model is capable of predicting all time intervals giving an overall factor of two of observations equal to 100%.

Extension of local front reconstruction method with controlled coalescence model

NASA Astrophysics Data System (ADS)

Rajkotwala, A. H.; Mirsandi, H.; Peters, E. A. J. F.; Baltussen, M. W.; van der Geld, C. W. M.; Kuerten, J. G. M.; Kuipers, J. A. M.

2018-02-01

The physics of droplet collisions involves a wide range of length scales. This poses a challenge to accurately simulate such flows with standard fixed grid methods due to their inability to resolve all relevant scales with an affordable number of computational grid cells. A solution is to couple a fixed grid method with subgrid models that account for microscale effects. In this paper, we improved and extended the Local Front Reconstruction Method (LFRM) with a film drainage model of Zang and Law [Phys. Fluids 23, 042102 (2011)]. The new framework is first validated by (near) head-on collision of two equal tetradecane droplets using experimental film drainage times. When the experimental film drainage times are used, the LFRM method is better in predicting the droplet collisions, especially at high velocity in comparison with other fixed grid methods (i.e., the front tracking method and the coupled level set and volume of fluid method). When the film drainage model is invoked, the method shows a good qualitative match with experiments, but a quantitative correspondence of the predicted film drainage time with the experimental drainage time is not obtained indicating that further development of film drainage model is required. However, it can be safely concluded that the LFRM coupled with film drainage models is much better in predicting the collision dynamics than the traditional methods.

Highly sensitive time-resolved thermography and multivariate image analysis of the cerebral cortex for intrasurgical diagnostics

NASA Astrophysics Data System (ADS)

Hollmach, Julia; Hoffmann, Nico; Schnabel, Christian; Küchler, Saskia; Sobottka, Stephan; Kirsch, Matthias; Schackert, Gabriele; Koch, Edmund; Steiner, Gerald

2013-03-01

Time-resolved thermography is a novel method to assess thermal variations and heterogeneities in tissue and blood. The recent generation of thermal cameras provides a sensitivity of less than mK. This high sensitivity in conjunction with non-invasive, label-free and radiation-free monitoring makes thermography a promising tool for intrasurgical diagnostics. In brain surgery, time-resolved thermography can be employed to distinguish between normal and anomalous tissue. In this study, we investigated and discussed the potential of time-resolved thermography in neurosurgery for the intraoperative detection and demarcation of tumor borders. Algorithms for segmentation, reduction of movement artifacts and image fusion were developed. The preprocessed image stacks were subjected to discrete wavelet transform to examine individual frequency components. K-means clustering was used for image evaluation to reveal similarities within the image sequence. The image evaluation shows significant differences for both types of tissue. Tumor and normal tissues have different time characteristics in heat production and transfer. Furthermore, tumor could be highlighted. These results demonstrate that time-resolved thermography is able to support the detection of tumors in a contactless manner without any side effects for the tissue. The intraoperative usage of time-resolved thermography improves the accuracy of tumor resections to prevent irreversible brain damage during surgery.

Time-resolved transillumination and optical tomography

NASA Astrophysics Data System (ADS)

de Haller, Emmanuel B.

1996-01-01

In response to an invitation by the editor-in-chief, I would like to present the current status of time-domain imaging. With exciting new photon diffusion techniques being developed in the frequency domain and promising optical coherence tomography, time-resolved transillumination is in constant evolution and the subject of passionate discussions during the numerous conferences dedicated to this subject. The purpose of time-resolved optical tomography is to provide noninvasive, high-resolution imaging of the interior of living bodies by the use of nonionizing radiation. Moreover, the use of visible to near-infrared wavelength yields metabolic information. Breast cancer screening is the primary potential application for time-resolved imaging. Neurology and tissue characterization are also possible fields of applications. Time- resolved transillumination and optical tomography should not only improve diagnoses, but the welfare of the patient. As no overview of this technique has yet been presented to my knowledge, this paper briefly describes the various methods enabling time-resolved transillumination and optical tomography. The advantages and disadvantages of these methods, as well as the clinical challenges they face are discussed. Although an analytic and computable model of light transport through tissues is essential for a meaningful interpretation of the transillumination process, this paper will not dwell on the mathematics of photon propagation.

Poster - 16: Time-resolved diode dosimetry for in vivo proton therapy range verification: calibration through numerical modeling

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

Toltz, Allison; Hoesl, Michaela; Schuemann, Jan

Purpose: A method to refine the implementation of an in vivo, adaptive proton therapy range verification methodology was investigated. Simulation experiments and in-phantom measurements were compared to validate the calibration procedure of a time-resolved diode dosimetry technique. Methods: A silicon diode array system has been developed and experimentally tested in phantom for passively scattered proton beam range verification by correlating properties of the detector signal to the water equivalent path length (WEPL). The implementation of this system requires a set of calibration measurements to establish a beam-specific diode response to WEPL fit for the selected ‘scout’ beam in a solidmore » water phantom. This process is both tedious, as it necessitates a separate set of measurements for every ‘scout’ beam that may be appropriate to the clinical case, as well as inconvenient due to limited access to the clinical beamline. The diode response to WEPL relationship for a given ‘scout’ beam may be determined within a simulation environment, facilitating the applicability of this dosimetry technique. Measurements for three ‘scout’ beams were compared against simulated detector response with Monte Carlo methods using the Tool for Particle Simulation (TOPAS). Results: Detector response in water equivalent plastic was successfully validated against simulation for spread out Bragg peaks of range 10 cm, 15 cm, and 21 cm (168 MeV, 177 MeV, and 210 MeV) with adjusted R{sup 2} of 0.998. Conclusion: Feasibility has been shown for performing calibration of detector response for a given ‘scout’ beam through simulation for the time resolved diode dosimetry technique.« less

Generation and Evolution of High-Mach-Number Laser-Driven Magnetized Collisionless Shocks in the Laboratory

DOE PAGES

Schaeffer, D. B.; Fox, W.; Haberberger, D.; ...

2017-07-13

Here, we present the first laboratory generation of high-Mach-number magnetized collisionless shocks created through the interaction of an expanding laser-driven plasma with a magnetized ambient plasma. Time-resolved, two-dimensional imaging of plasma density and magnetic fields shows the formation and evolution of a supercritical shock propagating at magnetosonic Mach number M ms ≈ 12. Particle-in-cell simulations constrained by experimental data further detail the shock formation and separate dynamics of the multi-ion-species ambient plasma. The results show that the shocks form on time scales as fast as one gyroperiod, aided by the efficient coupling of energy, and the generation of a magneticmore » barrier between the piston and ambient ions. The development of this experimental platform complements present remote sensing and spacecraft observations, and opens the way for controlled laboratory investigations of high-Mach number collisionless shocks, including the mechanisms and efficiency of particle acceleration.« less

Generation and Evolution of High-Mach-Number Laser-Driven Magnetized Collisionless Shocks in the Laboratory

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

Schaeffer, D. B.; Fox, W.; Haberberger, D.

Here, we present the first laboratory generation of high-Mach-number magnetized collisionless shocks created through the interaction of an expanding laser-driven plasma with a magnetized ambient plasma. Time-resolved, two-dimensional imaging of plasma density and magnetic fields shows the formation and evolution of a supercritical shock propagating at magnetosonic Mach number M ms ≈ 12. Particle-in-cell simulations constrained by experimental data further detail the shock formation and separate dynamics of the multi-ion-species ambient plasma. The results show that the shocks form on time scales as fast as one gyroperiod, aided by the efficient coupling of energy, and the generation of a magneticmore » barrier between the piston and ambient ions. The development of this experimental platform complements present remote sensing and spacecraft observations, and opens the way for controlled laboratory investigations of high-Mach number collisionless shocks, including the mechanisms and efficiency of particle acceleration.« less

Example-Based Super-Resolution Fluorescence Microscopy.

PubMed

Jia, Shu; Han, Boran; Kutz, J Nathan

2018-04-23

Capturing biological dynamics with high spatiotemporal resolution demands the advancement in imaging technologies. Super-resolution fluorescence microscopy offers spatial resolution surpassing the diffraction limit to resolve near-molecular-level details. While various strategies have been reported to improve the temporal resolution of super-resolution imaging, all super-resolution techniques are still fundamentally limited by the trade-off associated with the longer image acquisition time that is needed to achieve higher spatial information. Here, we demonstrated an example-based, computational method that aims to obtain super-resolution images using conventional imaging without increasing the imaging time. With a low-resolution image input, the method provides an estimate of its super-resolution image based on an example database that contains super- and low-resolution image pairs of biological structures of interest. The computational imaging of cellular microtubules agrees approximately with the experimental super-resolution STORM results. This new approach may offer potential improvements in temporal resolution for experimental super-resolution fluorescence microscopy and provide a new path for large-data aided biomedical imaging.

Directed Field Ionization

NASA Astrophysics Data System (ADS)

Gregoric, Vincent C.; Kang, Xinyue; Liu, Zhimin Cheryl; Rowley, Zoe A.; Carroll, Thomas J.; Noel, Michael W.

2017-04-01

Selective field ionization is an important experimental technique used to study the state distribution of Rydberg atoms. This is achieved by applying a steadily increasing electric field, which successively ionizes more tightly bound states. An atom prepared in an energy eigenstate encounters many avoided Stark level crossings on the way to ionization. As it traverses these avoided crossings, its amplitude is split among multiple different states, spreading out the time resolved electron ionization signal. By perturbing the electric field ramp, we can change how the atoms traverse the avoided crossings, and thus alter the shape of the ionization signal. We have used a genetic algorithm to evolve these perturbations in real time in order to arrive at a target ionization signal shape. This process is robust to large fluctuations in experimental conditions. This work was supported by the National Science Foundation under Grants No. 1607335 and No. 1607377 and used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation Grant Number OCI-1053575.

Low-dimensional and Data Fusion Techniques Applied to a Rectangular Supersonic Multi-stream Jet

NASA Astrophysics Data System (ADS)

Berry, Matthew; Stack, Cory; Magstadt, Andrew; Ali, Mohd; Gaitonde, Datta; Glauser, Mark

2017-11-01

Low-dimensional models of experimental and simulation data for a complex supersonic jet were fused to reconstruct time-dependent proper orthogonal decomposition (POD) coefficients. The jet consists of a multi-stream rectangular single expansion ramp nozzle, containing a core stream operating at Mj , 1 = 1.6 , and bypass stream at Mj , 3 = 1.0 with an underlying deck. POD was applied to schlieren and PIV data to acquire the spatial basis functions. These eigenfunctions were projected onto their corresponding time-dependent large eddy simulation (LES) fields to reconstruct the temporal POD coefficients. This reconstruction was able to resolve spectral peaks that were previously aliased due to the slower sampling rates of the experiments. Additionally, dynamic mode decomposition (DMD) was applied to the experimental and LES datasets, and the spatio-temporal characteristics were compared to POD. The authors would like to acknowledge AFOSR, program manager Dr. Doug Smith, for funding this research, Grant No. FA9550-15-1-0435.

Quantitative time-resolved analysis reveals intricate, differential regulation of standard- and immuno-proteasomes

PubMed Central

Liepe, Juliane; Holzhütter, Hermann-Georg; Bellavista, Elena; Kloetzel, Peter M; Stumpf, Michael PH; Mishto, Michele

2015-01-01

Proteasomal protein degradation is a key determinant of protein half-life and hence of cellular processes ranging from basic metabolism to a host of immunological processes. Despite its importance the mechanisms regulating proteasome activity are only incompletely understood. Here we use an iterative and tightly integrated experimental and modelling approach to develop, explore and validate mechanistic models of proteasomal peptide-hydrolysis dynamics. The 20S proteasome is a dynamic enzyme and its activity varies over time because of interactions between substrates and products and the proteolytic and regulatory sites; the locations of these sites and the interactions between them are predicted by the model, and experimentally supported. The analysis suggests that the rate-limiting step of hydrolysis is the transport of the substrates into the proteasome. The transport efficiency varies between human standard- and immuno-proteasomes thereby impinging upon total degradation rate and substrate cleavage-site usage. DOI: http://dx.doi.org/10.7554/eLife.07545.001 PMID:26393687

Time-resolved gas-phase kinetic, quantum chemical, and RRKM studies of reactions of silylene with alcohols.

PubMed

Becerra, Rosa; Cannady, J Pat; Walsh, Robin

2011-05-05

Time-resolved kinetic studies of silylene, SiH(2), generated by laser flash photolysis of 1-silacyclopent-3-ene and phenylsilane, have been carried out to obtain rate constants for its bimolecular reactions with methanol, ethanol, 1-propanol, 1-butanol, and 2-methyl-1-butanol. The reactions were studied in the gas phase over the pressure range 1-100 Torr in SF(6) bath gas, at room temperature. In the study with methanol several buffer gases were used. All five reactions showed pressure dependences characteristic of third body assisted association reactions. The rate constant pressure dependences were modeled using RRKM theory, based on E(0) values of the association complexes obtained by ab initio calculation (G3 level). Transition state models were adjusted to fit experimental fall-off curves and extrapolated to obtain k(∞) values in the range (1.9-4.5) × 10(-10) cm(3) molecule(-1) s(-1). These numbers, corresponding to the true bimolecular rate constants, indicate efficiencies of between 16% and 67% of the collision rates for these reactions. In the reaction of SiH(2) + MeOH there is a small kinetic component to the rate which is second order in MeOH (at low total pressures). This suggests an additional catalyzed reaction pathway, which is supported by the ab initio calculations. These calculations have been used to define specific MeOH-for-H(2)O substitution effects on this catalytic pathway. Where possible our experimental and theoretical results are compared with those of previous studies.

Raman linewidth measurements using time-resolved hybrid picosecond/nanosecond rotational CARS.

PubMed

Nordström, Emil; Hosseinnia, Ali; Brackmann, Christian; Bood, Joakim; Bengtsson, Per-Erik

2015-12-15

We report an innovative approach for time-domain measurements of S-branch Raman linewidths using hybrid picosecond/nanosecond pure-rotational coherent anti-Stokes Raman spectroscopy (RCARS). The Raman coherences are created by two picosecond excitation pulses and are probed using a narrow-band nanosecond pulse at 532 nm. The generated RCARS signal contains the entire coherence decay in a single pulse. By extracting the decay times of the individual transitions, the J-dependent Raman linewidths can be calculated. Self-broadened S-branch linewidths for nitrogen and oxygen at 293 K and ambient pressure are in good agreement with previous time-domain measurements. Experimental considerations of the approach are discussed along with its merits and limitations. The approach can be extended to a wide range of pressures and temperatures and has potential for simultaneous single-shot thermometry and linewidth determination.

Pulse pile-up in hard X-ray detector systems. [for solar X-rays

NASA Technical Reports Server (NTRS)

Datlowe, D. W.

1975-01-01

When pulse-height spectra are measured by a nuclear detection system at high counting rates, the probability that two or more pulses will arrive within the resolving time of the system is significant. This phenomenon, pulse pile-up, distorts the pulse-height spectrum and must be considered in the interpretation of spectra taken at high counting rates. A computational technique for the simulation of pile-up is developed. The model is examined in the three regimes where (1) the time between pulses is long compared to the detector-system resolving time, (2) the time between pulses is comparable to the resolving time, and (3) many pulses occur within the resolving time. The technique is used to model the solar hard X-ray experiment on the OSO-7 satellite; comparison of the model with data taken during three large flares shows excellent agreement. The paper also describes rule-of-thumb tests for pile-up and identifies the important detector design factors for minimizing pile-up, i.e., thick entrance windows and short resolving times in the system electronics.

Recognition without identification, erroneous familiarity, and déjà vu.

PubMed

O'Connor, Akira R; Moulin, Chris J A

2010-06-01

Déjà vu is characterized by the recognition of a situation concurrent with the awareness that this recognition is inappropriate. Although forms of déjà vu resolve in favor of the inappropriate recognition and therefore have behavioral consequences, typical déjà vu experiences resolve in favor of the awareness that the sensation of recognition is inappropriate. The resultant lack of behavioral modification associated with typical déjà vu means that clinicians and experimenters rely heavily on self-report when observing the experience. In this review, we focus on recent déjà vu research. We consider issues facing neuropsychological, neuroscientific, and cognitive experimental frameworks attempting to explore and experimentally generate the experience. In doing this, we suggest the need for more experimentation and a more cautious interpretation of research findings, particularly as many techniques being used to explore déjà vu are in the early stages of development.

High-Energy, High-Pulse-Rate Light Sources for Enhanced Time-Resolved Tomographic PIV of Unsteady and Turbulent Flows

DTIC Science & Technology

2017-07-31

Report: High-Energy, High-Pulse-Rate Light Sources for Enhanced Time -Resolved Tomographic PIV of Unsteady & Turbulent Flows The views, opinions and/or...reporting burden for this collection of information is estimated to average 1 hour per response, including the time for reviewing instructions, searching...High-Energy, High-Pulse-Rate Light Sources for Enhanced Time -Resolved Tomographic PIV of Unsteady & Turbulent Flows Report Term: 0-Other Email

Measurements of the principal Hugoniots of dense gaseous deuterium-helium mixtures: Combined multi-channel optical pyrometry, velocity interferometry, and streak optical pyrometry measurements

NASA Astrophysics Data System (ADS)

Li, Zhi-Guo; Chen, Qi-Feng; Gu, Yun-Jun; Zheng, Jun; Chen, Xiang-Rong

2016-10-01

The accurate hydrodynamic description of an event or system that addresses the equations of state, phase transitions, dissociations, ionizations, and compressions, determines how materials respond to a wide range of physical environments. To understand dense matter behavior in extreme conditions requires the continual development of diagnostic methods for accurate measurements of the physical parameters. Here, we present a comprehensive diagnostic technique that comprises optical pyrometry, velocity interferometry, and time-resolved spectroscopy. This technique was applied to shock compression experiments of dense gaseous deuterium-helium mixtures driven via a two-stage light gas gun. The advantage of this approach lies in providing measurements of multiple physical parameters in a single experiment, such as light radiation histories, particle velocity profiles, and time-resolved spectra, which enables simultaneous measurements of shock velocity, particle velocity, pressure, density, and temperature and expands understanding of dense high pressure shock situations. The combination of multiple diagnostics also allows different experimental observables to be measured and cross-checked. Additionally, it implements an accurate measurement of the principal Hugoniots of deuterium-helium mixtures, which provides a benchmark for the impedance matching measurement technique.

Intramolecular trap formation and Förster energy transfer in the hexapyropheophorbide- a molecular system

NASA Astrophysics Data System (ADS)

Al-Omari, S.

2006-12-01

The photophysical properties of the hexapyropheophorbide- a (P6) compound were studied using both steady-state and time-resolved spectroscopy. It was found that neighboring pyropheophorbide- a (pyroPheo) molecules covalently linked to each other through carbon chains, which could stack. This structural property is the reason for the possibility of formation of two different types of energy traps, which could be resolved experimentally. One of them is formed via face-to-face stacking of two pyroPheo molecules with a direction of the transition dipole moments parallel to each other. The second type of energy trap gives the dominant contribution to the fluorescence signal at a registration wavelength having the oblique geometry or orthogonal direction of the transition dipole moments of the interacting pyroPheo molecules. In any case, the dipole-dipole Förster energy transfer between pyroPheo molecules caused a very fast and efficient delivery of the excitation to a trap. As a result, the fluorescence as well as the singlet oxygen quantum yields of P6 were reduced by four and three times, respectively, compared to those values of the reference bispyrophephorbide- a (P2) compound.

Equatorial F region neutral winds and shears near sunset measured with chemical release techniques

NASA Astrophysics Data System (ADS)

Kiene, A.; Larsen, M. F.; Kudeki, E.

2015-10-01

The period near sunset is a dynamic and critical time for the daily development of the equatorial nighttime ionosphere and the instabilities that occur there. It is during these hours that the preconditions necessary for the later development of Equatorial Spread F (ESF) plasma instabilities occur. The neutral dynamics of the sunset ionosphere are also of critical importance to the generation of currents and electric fields; however, the behavior of the neutrals is experimentally understood primarily through very limited single-altitude measurements or measurements that provide weighted altitude means of the winds as a function of time. To date, there have been very few vertically resolved neutral wind measurements in the F region at sunset. We present two sets of sounding rocket chemical release measurements, one from a launch in the Marshall Islands on Kwajalein atoll and one from Alcantara, Brazil. Analysis of the release motions has yielded vertically resolved neutral wind profiles that show both the mean horizontal winds and the vertical shears in the winds. In both experiments, we observe significant vertical gradients in the zonal wind that are unexpected by classical assumptions about the behavior of the neutral wind at these altitudes at sunset near the geomagnetic equator.

Aeroacoustic analysis of an airfoil with Gurney flap based on time-resolved particle image velocimetry measurements

NASA Astrophysics Data System (ADS)

Zhang, Xueqing; Sciacchitano, Andrea; Pröbsting, Stefan

2018-05-01

Particle image velocimetry for the experimental assessment of trailing edge noise sources has become focus of research in recent years. The present study investigates the feasibility of the noise prediction for high-lift devices based on time-resolved particle image velocimetry (PIV). The model under investigation is a NACA 0015 airfoil with a Gurney flap with a height of 6% of the chord length. The velocity fields around and downstream of the Gurney flap were measured by PIV and used to compute the corresponding pressure fields by solving the Poisson equation for incompressible flows. The reconstructed pressure fluctuations on the airfoil surface constitute the source term for Curle's aeroacoustic analogy, which was employed in both the distributed and compact formulation to estimate the noise emission from PIV. The results of the two formulations are compared with the simultaneous far-field microphone measurements in the temporal and spectral domains. Both formulations of Curle's analogy yield acoustic sound pressure levels in good agreement with the simultaneous microphone measurements for the tonal component. The estimated far-field sound power spectra (SPL) from the PIV measurements reproduce the peak at the vortex shedding frequency, which also agrees well with the acoustic measurements.

4D Magnetic Resonance Velocimetry in a 3D printed brain aneurysm

NASA Astrophysics Data System (ADS)

Amili, Omid; Schiavazzi, Daniele; Coletti, Filippo

2016-11-01

Cerebral aneurysms are of great clinical importance. It is believed that hemodynamics play a critical role in the development, growth, and rupture of brain arteries with such condition. The flow structure in the aneurysm sac is complex, unsteady, and three-dimensional. Therefore the time-resolved measurement of the three-dimensional three-component velocity field is crucial to predict the clinical outcome. In this study magnetic resonance velocimetry is used to assess the fluid dynamics inside a 3D printed model of a giant intracranial aneurysm. We reach sub-millimeter resolution while resolving sixteen instances within the cardiac cycle. The physiological flow waveform is imposed using an in-house built pump in a flow circuit where the cardiovascular impedance is matched. The flow evolution over time is reconstructed in detail. The complex flow structure is characterized by vortical and helical motions that reside in the aneurysm for most part of the cycle. The 4D pressured distribution is also reconstructed from the velocity field. The present case study was used in a previous CFD challenge, therefore these results may provide useful experimental comparison for simulations performed by other research groups.

Development of a High Resolution X-ray Spectrometer on the National Ignition Facility

NASA Astrophysics Data System (ADS)

Gao, L.; Kraus, B.; Hill, K. W.; Bitter, M.; Efthimion, P.; Schneider, M. B.; Chen, H.; Ayers, J.; Liedahl, D.; Macphee, A. G.; Le, H. P.; Thorn, D.; Nelson, D.

2017-10-01

A high-resolution x-ray spectrometer has been designed, calibrated, and deployed on the National Ignition Facility (NIF) to measure plasma parameters for a Kr-doped surrogate capsule imploded at NIF conditions. Two conical crystals, each diffracting the He α and He β complexes respectively, focus the spectra onto a steak camera photocathode for time-resolved measurements with a temporal resolution of <20 ps. A third cylindrical crystal focuses the entire He α to He β spectrum onto an image plate for a time-integrated spectrum to correlate the two streaked signals. The instrument was absolutely calibrated by the x-ray group at the Princeton Plasma Physics Laboratory using a micro-focus x-ray source. Detailed calibration procedures, including source and spectrum alignment, energy calibration, crystal performance evaluation, and measurement of the resolving power and the integrated reflectivity will be presented. Initial NIF experimental results will also be discussed. This work was performed under the auspices of the U.S. Department of Energy by Princeton Plasma Physics Laboratory under contract DE-AC02-09CH11466 and by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344.

Simultaneous manipulation and observation of multiple ro-vibrational eigenstates in solid para-hydrogen.

PubMed

Katsuki, Hiroyuki; Ohmori, Kenji

2016-09-28

We have experimentally performed the coherent control of delocalized ro-vibrational wave packets (RVWs) of solid para-hydrogen (p-H 2 ) by the wave packet interferometry (WPI) combined with coherent anti-Stokes Raman scattering (CARS). RVWs of solid p-H 2 are delocalized in the crystal, and the wave function with wave vector k ∼ 0 is selectively excited via the stimulated Raman process. We have excited the RVW twice by a pair of femtosecond laser pulses with delay controlled by a stabilized Michelson interferometer. Using a broad-band laser pulse, multiple ro-vibrational states can be excited simultaneously. We have observed the time-dependent Ramsey fringe spectra as a function of the inter-pulse delay by a spectrally resolved CARS technique using a narrow-band probe pulse, resolving the different intermediate states. Due to the different fringe oscillation periods among those intermediate states, we can manipulate their amplitude ratio by tuning the inter-pulse delay on the sub-femtosecond time scale. The state-selective manipulation and detection of the CARS signal combined with the WPI is a general and efficient protocol for the control of the interference of multiple quantum states in various quantum systems.

Reduction of Fermi level pinning and recombination at polycrystalline CdTe surfaces by laser irradiation

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

Simonds, Brian J.; Kheraj, Vipul; Department of Applied Physics, S. V. National Institute of Technology, Surat 395 007

2015-06-14

Laser processing of polycrystalline CdTe is a promising approach that could potentially increase module manufacturing throughput while reducing capital expenditure costs. For these benefits to be realized, the basic effects of laser irradiation on CdTe must be ascertained. In this study, we utilize surface photovoltage spectroscopy (SPS) to investigate the changes to the electronic properties of the surface of polycrystalline CdTe solar cell stacks induced by continuous-wave laser annealing. The experimental data explained within a model consisting of two space charge regions, one at the CdTe/air interface and one at the CdTe/CdS junction, are used to interpret our SPS results.more » The frequency dependence and phase spectra of the SPS signal are also discussed. To support the SPS findings, low-temperature spectrally-resolved photoluminescence and time-resolved photoluminescence were also measured. The data show that a modest laser treatment of 250 W/cm{sup 2} with a dwell time of 20 s is sufficient to reduce the effects of Fermi level pinning at the surface due to surface defects.« less

Calibrated simulations of Z opacity experiments that reproduce the experimentally measured plasma conditions

DOE PAGES

Nagayama, T.; Bailey, J. E.; Loisel, G.; ...

2016-02-05

Recently, frequency-resolved iron opacity measurements at electron temperatures of 170–200 eV and electron densities of (0.7 – 4.0) × 10 22 cm –3 revealed a 30–400% disagreement with the calculated opacities [J. E. Bailey et al., Nature (London) 517, 56 (2015)]. The discrepancies have a high impact on astrophysics, atomic physics, and high-energy density physics, and it is important to verify our understanding of the experimental platform with simulations. Reliable simulations are challenging because the temporal and spatial evolution of the source radiation and of the sample plasma are both complex and incompletely diagnosed. In this article, we describe simulationsmore » that reproduce the measured temperature and density in recent iron opacity experiments performed at the Sandia National Laboratories Z facility. The time-dependent spectral irradiance at the sample is estimated using the measured time- and space-dependent source radiation distribution, in situ source-to-sample distance measurements, and a three-dimensional (3D) view-factor code. The inferred spectral irradiance is used to drive 1D sample radiation hydrodynamics simulations. The images recorded by slit-imaged space-resolved spectrometers are modeled by solving radiation transport of the source radiation through the sample. We find that the same drive radiation time history successfully reproduces the measured plasma conditions for eight different opacity experiments. These results provide a quantitative physical explanation for the observed dependence of both temperature and density on the sample configuration. Simulated spectral images for the experiments without the FeMg sample show quantitative agreement with the measured spectral images. The agreement in spectral profile, spatial profile, and brightness provides further confidence in our understanding of the backlight-radiation time history and image formation. Furthermore, these simulations bridge the static-uniform picture of the data interpretation and the dynamic-gradient reality of the experiments, and they will allow us to quantitatively assess the impact of effects neglected in the data interpretation.« less

Hydrogen and Ethene Plasma Assisted Ignition by NS discharge at Elevated Temperatures

NASA Astrophysics Data System (ADS)

Starikovskiy, Andrey

2015-09-01

The kinetics of ignition in lean H2:O2:Ar and C2H4:O2:Ar mixtures has been studied experimentally and numerically after a high-voltage nanosecond discharge. The ignition delay time behind a reflected shock wave was measured with and without the discharge. It was shown that the initiation of the discharge with a specific deposited energy of 10 - 30 mJ/cm3 leads to an order of magnitude decrease in the ignition delay time. Discharge processes and following chain chemical reactions with energy release were simulated. The generation of atoms, radicals and excited and charged particles was numerically simulated using the measured time - resolved discharge current and electric field in the discharge phase. The calculated densities of the active particles were used as input data to simulate plasma-assisted ignition. Good agreement was obtained between the calculated ignition delay times and the experimental data. It follows from the analysis of the calculated results that the main mechanism of the effect of gas discharge on the ignition of hydrocarbons is the electron impact dissociation of O2 molecules in the discharge phase. Detailed kinetic mechanism for plasma assisted ignition of hydrogen and ethene is elaborated and verified.

Experimental Investigation of Reynolds Number Effects on Test Quality in a Hypersonic Expansion Tube

NASA Astrophysics Data System (ADS)

Rossmann, Tobias; Devin, Alyssa; Shi, Wen; Verhoog, Charles

2017-11-01

Reynolds number effects on test time and the temporal and spatial flow quality in a hypersonic expansion tube are explored using high-speed pressure, infrared optical, and Schlieren imaging measurements. Boundary layer models for shock tube flows are fairly well established to assist in the determination of test time and flow dimensions at typical high enthalpy test conditions. However, the application of these models needs to be more fully explored due to the unsteady expansion of turbulent boundary layers and contact regions separating dissimilar gasses present in expansion tube flows. Additionally, expansion tubes rely on the development of a steady jet with a large enough core-flow region at the exit of the acceleration tube to create a constant velocity region inside of the test section. High-speed measurements of pressure and Mach number at several locations within the expansion tube allow for the determination of an experimental x-t diagram. The comparison of the experimentally determined x-t diagram to theoretical highlights the Reynolds number dependent effects on expansion tube. Additionally, spatially resolved measurements of the Reynolds number dependent, steady core-flow in the expansion tube viewing section are shown. NSF MRI CBET #1531475, Lafayette College, McCutcheon Foundation.

Theoretical and experimental investigations of coincidences in Poisson distributed pulse trains and spectral distortion caused by pulse pileup

NASA Astrophysics Data System (ADS)

Bristow, Quentin

1990-03-01

The occurrence rates of pulse strings, or sequences of pulses with interarrival times less than the resolving time of the pulse-height analysis system used to acquire spectra, are derived from theoretical considerations. Logic circuits were devised to make experimental measurements of multiple pulse string occurrence rates in the output from a scintillation detector over a wide range of count rates. Markov process theory was used to predict state transition rates in the logic circuits, enabling the experimental data to be checked rigorously for conformity with those predicted for a Poisson distribution. No fundamental discrepancies were observed. Monte Carlo simulations, incorporating criteria for pulse pileup inherent in the operation of modern analog to digital converters, were used to generate pileup spectra due to coincidences between two pulses (first order pileup) and three pulses (second order pileup) for different semi-Gaussian pulse shapes. Coincidences between pulses in a single channel produced a basic probability density function spectrum. The use of a flat spectrum showed the first order pileup distorted the spectrum to a linear ramp with a pileup tail. A correction algorithm was successfully applied to correct entire spectra (simulated and real) for first and second order pileups.

Knowledge Extraction from Atomically Resolved Images.

PubMed

Vlcek, Lukas; Maksov, Artem; Pan, Minghu; Vasudevan, Rama K; Kalinin, Sergei V

2017-10-24

Tremendous strides in experimental capabilities of scanning transmission electron microscopy and scanning tunneling microscopy (STM) over the past 30 years made atomically resolved imaging routine. However, consistent integration and use of atomically resolved data with generative models is unavailable, so information on local thermodynamics and other microscopic driving forces encoded in the observed atomic configurations remains hidden. Here, we present a framework based on statistical distance minimization to consistently utilize the information available from atomic configurations obtained from an atomically resolved image and extract meaningful physical interaction parameters. We illustrate the applicability of the framework on an STM image of a FeSe x Te 1-x superconductor, with the segregation of the chalcogen atoms investigated using a nonideal interacting solid solution model. This universal method makes full use of the microscopic degrees of freedom sampled in an atomically resolved image and can be extended via Bayesian inference toward unbiased model selection with uncertainty quantification.

Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd

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

Neupane, Madhab; Alidoust, Nasser; Hosen, M. Mofazzel

Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here in this paper we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of suchmore » spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.« less

Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd

DOE PAGES

Neupane, Madhab; Alidoust, Nasser; Hosen, M. Mofazzel; ...

2016-11-07

Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here in this paper we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of suchmore » spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.« less