Resolving Confined 7Li Dynamics of Uranyl Peroxide Capsule U 24

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

Xie, Jing; Neal, Harrison A.; Szymanowski, Jennifer

Here, we obtained a kerosene-soluble form of the lithium salt [UO 2(O 2)(OH) 2] 24 phase (Li-U 24), by adding cetyltrimethylammonium bromide surfactant to aqueous Li-U 24. Interestingly, its variable-temperature solution 7Li NMR spectroscopy resolves two narrowly spaced resonances down to –10 °C, which shift upfield with increasing temperature, and finally coalesce at temperatures > 85 °C. Comparison with solid-state NMR demonstrates that the Li dynamics in the Li-U 24-CTA phase involves only exchange between different local encapsulated environments. This behavior is distinct from the rapid Li exchange dynamics observed between encapsulated and external Li environments for Li-U 24 inmore » both the aqueous and the solid-state phases. Density functional theory calculations suggest that the two experimental 7Li NMR chemical shifts are due to Li cations coordinated within the square and hexagonal faces of the U 24 cage, and they can undergo exchange within the confined environment, as the solution is heated. Very different than U 24 in aqueous media, there is no evidence that the Li cations exit the cage, and therefore, this represents a truly confined space.« less

Energetics and dynamics of simple impulsive solar flares

NASA Technical Reports Server (NTRS)

Starr, R.; Heindl, W. A.; Crannell, C. J.; Thomas, R. J.; Batchelor, D. A.; Magun, A.

1987-01-01

Flare energetics and dynamics were studied using observations of simple impulsive spike bursts. A large, homogeneous set of events was selected to enable the most definite tests possible of competing flare models, in the absence of spatially resolved observations. The emission mechanisms and specific flare models that were considered in this investigation are described, and the derivations of the parameters that were tested are presented. Results of the correlation analysis between soft and hard X-ray energetics are also presented. The ion conduction front model and tests of that model with the well-observed spike bursts are described. Finally, conclusions drawn from this investigation and suggestions for future studies are discussed.

Final Technical Report for DE-SC0008149

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

Buchanan, Kristen

The major goal of this project is to study spin waves in magnetic thin films, especially how spin waves respond to external stimuli. This is expected to lead to new insight into dynamic processes and new ideas for methods to control spin waves. Experimental studies are being done primarily using time- and spatially-resolved Brillouin light scattering (BLS) measurements on extended and patterned magnetic thin films. BLS is a versatile tool that provides a non-invasive probe of spin dynamics with frequencies of ~1 GHz to well over 100 GHz, diffraction-limited spatial resolution, 250-ps temporal resolution, and it is sensitive enough tomore » detect thermal magnons.« less

Improving predictions of large scale soil carbon dynamics: Integration of fine-scale hydrological and biogeochemical processes, scaling, and benchmarking

NASA Astrophysics Data System (ADS)

Riley, W. J.; Dwivedi, D.; Ghimire, B.; Hoffman, F. M.; Pau, G. S. H.; Randerson, J. T.; Shen, C.; Tang, J.; Zhu, Q.

2015-12-01

Numerical model representations of decadal- to centennial-scale soil-carbon dynamics are a dominant cause of uncertainty in climate change predictions. Recent attempts by some Earth System Model (ESM) teams to integrate previously unrepresented soil processes (e.g., explicit microbial processes, abiotic interactions with mineral surfaces, vertical transport), poor performance of many ESM land models against large-scale and experimental manipulation observations, and complexities associated with spatial heterogeneity highlight the nascent nature of our community's ability to accurately predict future soil carbon dynamics. I will present recent work from our group to develop a modeling framework to integrate pore-, column-, watershed-, and global-scale soil process representations into an ESM (ACME), and apply the International Land Model Benchmarking (ILAMB) package for evaluation. At the column scale and across a wide range of sites, observed depth-resolved carbon stocks and their 14C derived turnover times can be explained by a model with explicit representation of two microbial populations, a simple representation of mineralogy, and vertical transport. Integrating soil and plant dynamics requires a 'process-scaling' approach, since all aspects of the multi-nutrient system cannot be explicitly resolved at ESM scales. I will show that one approach, the Equilibrium Chemistry Approximation, improves predictions of forest nitrogen and phosphorus experimental manipulations and leads to very different global soil carbon predictions. Translating model representations from the site- to ESM-scale requires a spatial scaling approach that either explicitly resolves the relevant processes, or more practically, accounts for fine-resolution dynamics at coarser scales. To that end, I will present recent watershed-scale modeling work that applies reduced order model methods to accurately scale fine-resolution soil carbon dynamics to coarse-resolution simulations. Finally, we contend that creating believable soil carbon predictions requires a robust, transparent, and community-available benchmarking framework. I will present an ILAMB evaluation of several of the above-mentioned approaches in ACME, and attempt to motivate community adoption of this evaluation approach.

Increasing the efficiency and accuracy of time-resolved electronic spectra calculations with on-the-fly ab initio quantum dynamics methods

NASA Astrophysics Data System (ADS)

Vanicek, Jiri

2014-03-01

Rigorous quantum-mechanical calculations of coherent ultrafast electronic spectra remain difficult. I will present several approaches developed in our group that increase the efficiency and accuracy of such calculations: First, we justified the feasibility of evaluating time-resolved spectra of large systems by proving that the number of trajectories needed for convergence of the semiclassical dephasing representation/phase averaging is independent of dimensionality. Recently, we further accelerated this approximation with a cellular scheme employing inverse Weierstrass transform and optimal scaling of the cell size. The accuracy of potential energy surfaces was increased by combining the dephasing representation with accurate on-the-fly ab initio electronic structure calculations, including nonadiabatic and spin-orbit couplings. Finally, the inherent semiclassical approximation was removed in the exact quantum Gaussian dephasing representation, in which semiclassical trajectories are replaced by communicating frozen Gaussian basis functions evolving classically with an average Hamiltonian. Among other examples I will present an on-the-fly ab initio semiclassical dynamics calculation of the dispersed time-resolved stimulated emission spectrum of the 54-dimensional azulene. This research was supported by EPFL and by the Swiss National Science Foundation NCCR MUST (Molecular Ultrafast Science and Technology) and Grant No. 200021124936/1.

Light-induced nonadiabatic dynamics in molecular assemblies and nanostructures

NASA Astrophysics Data System (ADS)

Mitric, Roland

The combination of mixed quantum-classical dynamics with efficient electronic structure methods was developed in order to simulate the light-induced processes in complex molecules, multichromophoric aggregates and metallic nanostructures. We will demonstrate how the combination of nonadiabatic dynamics with experimental pump-probe techniques such as time-resolved photoelectron imaging (TRPEI) allows to fully resolve the mechanism of excited state relaxation through conical intersections in several prototype organic- and biomolecules. Specifically, the role of the solvent in the excited state relaxation in microsolvated and fully solvated systems will be addressed. Currently there is growing evidence that nonadiabatic relaxation processes also play a fundamental role in determining the efficiency of excitonic transfer or charge injection in multichromophoric assemblies. Since such systems are currently out of the reach of the state-of-the-art quantum chemistry a development of even more efficient quantum chemical approaches is necessary in order to describe the excited state dynamics in such assemblies. For this purpose we have recently developed long-range corrected time-dependent density functional tight binding (LC-TDDFTB) nonadiabatic dynamics and combined it with the QM/MM approach in order to simulate exciton relaxation in complex systems. The applications of the method to the investigation of the optical properties and dynamics in multichromophoric assemblies including stacked pi-conjugated organic chromophores, model molecular crystals as well as self-organized dye aggregates will be presented. Finally, we will address exciton transport dynamics coupled with the light propagation in hybrid exciton-plasmon nanostructures, which represent promising materials fort the development of novel light-harvesting systems.

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.

Integration of Structural Dynamics and Molecular Evolution via Protein Interaction Networks: A New Era in Genomic Medicine

PubMed Central

Kumar, Avishek; Butler, Brandon M.; Kumar, Sudhir; Ozkan, S. Banu

2016-01-01

Summary Sequencing technologies are revealing many new non-synonymous single nucleotide variants (nsSNVs) in each personal exome. To assess their functional impacts, comparative genomics is frequently employed to predict if they are benign or not. However, evolutionary analysis alone is insufficient, because it misdiagnoses many disease-associated nsSNVs, such as those at positions involved in protein interfaces, and because evolutionary predictions do not provide mechanistic insights into functional change or loss. Structural analyses can aid in overcoming both of these problems by incorporating conformational dynamics and allostery in nSNV diagnosis. Finally, protein-protein interaction networks using systems-level methodologies shed light onto disease etiology and pathogenesis. Bridging these network approaches with structurally resolved protein interactions and dynamics will advance genomic medicine. PMID:26684487

Climate Dynamics and Hysteresis at Low and High Obliquity

NASA Astrophysics Data System (ADS)

Colose, C.; Del Genio, A. D.; Way, M.

2017-12-01

We explore the large-scale climate dynamics at low and high obliquity for an Earth-like planet using the ROCKE-3D (Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics) 3-D General Circulation model being developed at NASA GISS as part of the Nexus for Exoplanet System Science (NExSS) initiative. We highlight the role of ocean heat storage and transport in determining the seasonal cycle at high obliquity, and describe the large-scale circulation and resulting regional climate patterns using both aquaplanet and Earth topographical boundary conditions. Finally, we contrast the hysteresis structure to varying CO2 concentration for a low and high obliquity planet near the outer edge of the habitable zone. We discuss the prospects for habitability for a high obliquity planet susceptible to global glaciation.

Dynamic cellular manufacturing system considering machine failure and workload balance

NASA Astrophysics Data System (ADS)

Rabbani, Masoud; Farrokhi-Asl, Hamed; Ravanbakhsh, Mohammad

2018-02-01

Machines are a key element in the production system and their failure causes irreparable effects in terms of cost and time. In this paper, a new multi-objective mathematical model for dynamic cellular manufacturing system (DCMS) is provided with consideration of machine reliability and alternative process routes. In this dynamic model, we attempt to resolve the problem of integrated family (part/machine cell) formation as well as the operators' assignment to the cells. The first objective minimizes the costs associated with the DCMS. The second objective optimizes the labor utilization and, finally, a minimum value of the variance of workload between different cells is obtained by the third objective function. Due to the NP-hard nature of the cellular manufacturing problem, the problem is initially validated by the GAMS software in small-sized problems, and then the model is solved by two well-known meta-heuristic methods including non-dominated sorting genetic algorithm and multi-objective particle swarm optimization in large-scaled problems. Finally, the results of the two algorithms are compared with respect to five different comparison metrics.

Time-resolved light emission of a, c, and r-cut sapphires shock-compressed to 65 GPa

NASA Astrophysics Data System (ADS)

Liu, Q. C.; Zhou, X. M.

2018-04-01

To investigate light emission and dynamic deformation behaviors, sapphire (single crystal Al2O3) samples with three crystallographic orientations (a, c, and r-cut) were shock-compressed by the planar impact method, with final stress ranges from 47 to 65 GPa. Emission radiance and velocity versus time profiles were simultaneously measured with a fast pyrometer and a Doppler pin system in each experiment. Wave profile results show anisotropic elastic-plastic transitions, which confirm the literature observations. Under final shock stress of about 52 GPa, lower emission intensity is observed in the r-cut sample, in agreement with the previous report in the literature. When final shock stress increases to 57 GPa and 65 GPa, spectral radiance histories of the r-cut show two stages of distinct features. In the first stage, the emission intensity of r-cut is lower than those of the other two, which agrees with the previous report in the literature. In the second stage, spectral radiance of r-cut increases with time at much higher rate and it finally peaks over those of the a and c-cut. These observations (conversion of intensified emission in the r-cut) may indicate activation of a second slip system and formation of shear bands which are discussed with the resolved shear stress calculations for the slip systems in each of the three cuts under shock compression.

Analytical representation of dynamical quantities in G W from a matrix resolvent

NASA Astrophysics Data System (ADS)

Gesenhues, J.; Nabok, D.; Rohlfing, M.; Draxl, C.

2017-12-01

The power of the G W formalism is, to a large extent, based on the explicit treatment of dynamical correlations in the self-energy. This dynamics is taken into account by calculating the energy dependence of the screened Coulomb interaction W , followed by a convolution with the Green's function G . In order to obtain the energy dependence of W the prevalent methods are plasmon-pole models and numerical integration techniques. In this paper, we discuss an alternative approach, in which the energy-dependent screening is calculated by determining the resolvent, which is set up from a matrix representation of the dielectric function. On the one hand, this refrains from a numerical energy convolution and allows one to actually write down the energy dependence of W explicitly (like in the plasmon-pole models). On the other hand, the method is at least as accurate as the numerical approaches due to its multipole nature. We discuss the theoretical setup in some detail, give insight into the computational aspects, and present results for Si, C, GaAs, and LiF. Finally, we argue that the analytic representability is not only useful for educational purposes but may also be of avail for the development of theory that goes beyond G W .

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.

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.

Integration of structural dynamics and molecular evolution via protein interaction networks: a new era in genomic medicine.

PubMed

Kumar, Avishek; Butler, Brandon M; Kumar, Sudhir; Ozkan, S Banu

2015-12-01

Sequencing technologies are revealing many new non-synonymous single nucleotide variants (nsSNVs) in each personal exome. To assess their functional impacts, comparative genomics is frequently employed to predict if they are benign or not. However, evolutionary analysis alone is insufficient, because it misdiagnoses many disease-associated nsSNVs, such as those at positions involved in protein interfaces, and because evolutionary predictions do not provide mechanistic insights into functional change or loss. Structural analyses can aid in overcoming both of these problems by incorporating conformational dynamics and allostery in nSNV diagnosis. Finally, protein-protein interaction networks using systems-level methodologies shed light onto disease etiology and pathogenesis. Bridging these network approaches with structurally resolved protein interactions and dynamics will advance genomic medicine. Copyright © 2015 Elsevier Ltd. All rights reserved.

Bragg coherent diffractive imaging of single-grain defect dynamics in polycrystalline films

DOE PAGES

Yau, Allison; Cha, Wonsuk; Kanan, Matthew W.; ...

2017-05-19

Polycrystalline material properties depend on the distribution and interactions of their crystalline grains. In particular, grain boundaries and defects are crucial in determining their response to external stimuli. A long-standing challenge is thus to observe individual grains, defects, and strain dynamics inside functional materials. Here we report a technique capable of revealing grain heterogeneity, including strain fields and individual dislocations, that can be used under operando conditions in reactive environments: grain Bragg coherent diffractive imaging (gBCDI). Using a polycrystalline gold thin film subjected to heating, we show how gBCDI resolves grain boundary and dislocation dynamics in individual grains in three-dimensionalmore » detail with 10-nanometer spatial and subangstrom displacement field resolution. Finally, these results pave the way for understanding polycrystalline material response under external stimuli and, ideally, engineering particular functions.« less

Dynamic x-ray imaging of laser-driven nanoplasmas

NASA Astrophysics Data System (ADS)

Fennel, Thomas

2016-05-01

A major promise of current x-ray science at free electron lasers is the realization of unprecedented imaging capabilities for resolving the structure and ultrafast dynamics of matter with nanometer spatial and femtosecond temporal resolution or even below via single-shot x-ray diffraction. Laser-driven atomic clusters and nanoparticles provide an ideal platform for developing and demonstrating the required technology to extract the ultrafast transient spatiotemporal dynamics from the diffraction images. In this talk, the perspectives and challenges of dynamic x-ray imaging will be discussed using complete self-consistent microscopic electromagnetic simulations of IR pump x-ray probe imaging for the example of clusters. The results of the microscopic particle-in-cell simulations (MicPIC) enable the simulation-assisted reconstruction of corresponding experimental data. This capability is demonstrated by converting recently measured LCLS data into a ultrahigh resolution movie of laser-induced plasma expansion. Finally, routes towards reaching attosecond time resolution in the visualization of complex dynamical processes in matter by x-ray diffraction will be discussed.

Generation of High Brightness X-rays with the PLEIADES Thomson X-ray Source

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

Brown, W J; Anderson, S G; Barty, C P J

2003-05-28

The use of short laser pulses to generate high peak intensity, ultra-short x-ray pulses enables exciting new experimental capabilities, such as femtosecond pump-probe experiments used to temporally resolve material structural dynamics on atomic time scales. PLEIADES (Picosecond Laser Electron InterAction for Dynamic Evaluation of Structures) is a next generation Thomson scattering x-ray source being developed at Lawrence Livermore National Laboratory (LLNL). Ultra-fast picosecond x-rays (10-200 keV) are generated by colliding an energetic electron beam (20-100 MeV) with a high intensity, sub-ps, 800 nm laser pulse. The peak brightness of the source is expected to exceed 10{sup 20} photons/s/0.1% bandwidth/mm2/mrad2. Simulationsmore » of the electron beam production, transport, and final focus are presented. Electron beam measurements, including emittance and final focus spot size are also presented and compared to simulation results. Measurements of x-ray production are also reported and compared to theoretical calculations.« less

Quantifying time-of-flight-resolved optical field dynamics in turbid media with interferometric near-infrared spectroscopy (iNIRS) (Conference Presentation)

NASA Astrophysics Data System (ADS)

Borycki, Dawid; Kholiqov, Oybek; Zhou, Wenjun; Srinivasan, Vivek J.

2017-03-01

Sensing and imaging methods based on the dynamic scattering of coherent light, including laser speckle, laser Doppler, and diffuse correlation spectroscopy quantify scatterer motion using light intensity (speckle) fluctuations. The underlying optical field autocorrelation (OFA), rather than being measured directly, is typically inferred from the intensity autocorrelation (IA) through the Siegert relationship, by assuming that the scattered field obeys Gaussian statistics. In this work, we demonstrate interferometric near-infrared spectroscopy (iNIRS) for measurement of time-of-flight (TOF) resolved field and intensity autocorrelations in fluid tissue phantoms and in vivo. In phantoms, we find a breakdown of the Siegert relationship for short times-of-flight due to a contribution from static paths whose optical field does not decorrelate over experimental time scales, and demonstrate that eliminating such paths by polarization gating restores the validity of the Siegert relationship. Inspired by these results, we developed a method, called correlation gating, for separating the OFA into static and dynamic components. Correlation gating enables more precise quantification of tissue dynamics. To prove this, we show that iNIRS and correlation gating can be applied to measure cerebral hemodynamics of the nude mouse in vivo using dynamically scattered (ergodic) paths and not static (non-ergodic) paths, which may not be impacted by blood. More generally, correlation gating, in conjunction with TOF resolution, enables more precise separation of diffuse and non-diffusive contributions to OFA than is possible with TOF resolution alone. Finally, we show that direct measurements of OFA are statistically more efficient than indirect measurements based on IA.

Simulation of dental collisions and occlusal dynamics in the virtual environment.

PubMed

Stavness, I K; Hannam, A G; Tobias, D L; Zhang, X

2016-04-01

Semi-adjustable articulators have often been used to simulate occlusal dynamics, but advances in intra-oral scanning and computer software now enable dynamics to be modelled mathematically. Computer simulation of occlusal dynamics requires accurate virtual casts, records to register them and methods to handle mesh collisions during movement. Here, physical casts in a semi-adjustable articulator were scanned with a conventional clinical intra-oral scanner. A coordinate measuring machine was used to index their positions in intercuspation, protrusion, right and left laterotrusion, and to model features of the articulator. Penetrations between the indexed meshes were identified and resolved using restitution forces, and the final registrations were verified by distance measurements between dental landmarks at multiple sites. These sites were confirmed as closely approximating via measurements made from homologous transilluminated vinylpolysiloxane interocclusal impressions in the mounted casts. Movements between the indexed positions were simulated with two models in a custom biomechanical software platform. In model DENTAL, 6 degree-of-freedom movements were made to minimise deviation from a straight line path and also shaped by dynamic mesh collisions detected and resolved mathematically. In model ARTIC, the paths were further constrained by surfaces matching the control settings of the articulator. Despite these differences, the lower mid-incisor point paths were very similar in both models. The study suggests that mathematical simulation utilising interocclusal 'bite' registrations can closely replicate the primary movements of casts mounted in a semi-adjustable articulator. Additional indexing positions and appropriate software could, in some situations, replace the need for mechanical semi-adjustable articulation and/or its virtual representation. © 2015 John Wiley & Sons Ltd.

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

PubMed

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-06-19

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification of transient, excited states, providing quantification of important parameters such as spin and orbital angular momenta as well as the energy gaps that separate electronic fine structure states. Ultrafast two-dimensional electronic spectroscopy (2DES) can be used to understand how these details influence state-to-state carrier dynamics. In combination, VTVH and 2DES methods can provide chemists with detailed information regarding the structure-dependent and state-specific flow of energy through metal nanoclusters. In this Account, we highlight recent advances toward understanding structure-dependent carrier dynamics for metals spanning the sub-nanometer to tens of nanometers length scale. We demonstrate the use of UCLEM methods for arresting interband scattering effects. For sub-nanometer thiol-protected nanoclusters, we discuss the effectiveness of VTVH for distinguishing state-specific radiative recombination originating from a gold core versus organometallic protecting layers. This state specificity is refined further using femtosecond 2DES and two-color methods to isolate so-called superatom state dynamics and vibrationally mediated spin-conversion and emission processes. Finally, we discuss prospects for merging VTVH and 2DES methods into a single platform.

The KMOS Redshift One Spectroscopic Survey (KROSS): dynamical properties, gas and dark matter fractions of typical z ˜ 1 star-forming galaxies

NASA Astrophysics Data System (ADS)

Stott, John P.; Swinbank, A. M.; Johnson, Helen L.; Tiley, Alfie; Magdis, Georgios; Bower, Richard; Bunker, Andrew J.; Bureau, Martin; Harrison, Chris M.; Jarvis, Matt J.; Sharples, Ray; Smail, Ian; Sobral, David; Best, Philip; Cirasuolo, Michele

2016-04-01

The KMOS Redshift One Spectroscopic Survey (KROSS) is an ESO-guaranteed time survey of 795 typical star-forming galaxies in the redshift range z = 0.8-1.0 with the KMOS instrument on the Very Large Telescope. In this paper, we present resolved kinematics and star formation rates for 584 z ˜ 1 galaxies. This constitutes the largest near-infrared Integral Field Unit survey of galaxies at z ˜ 1 to date. We demonstrate the success of our selection criteria with 90 per cent of our targets found to be H α emitters, of which 81 per cent are spatially resolved. The fraction of the resolved KROSS sample with dynamics dominated by ordered rotation is found to be 83 ± 5 per cent. However, when compared with local samples these are turbulent discs with high gas to baryonic mass fractions, ˜35 per cent, and the majority are consistent with being marginally unstable (Toomre Q ˜ 1). There is no strong correlation between galaxy averaged velocity dispersion and the total star formation rate, suggesting that feedback from star formation is not the origin of the elevated turbulence. We postulate that it is the ubiquity of high (likely molecular) gas fractions and the associated gravitational instabilities that drive the elevated star formation rates in these typical z ˜ 1 galaxies, leading to the 10-fold enhanced star formation rate density. Finally, by comparing the gas masses obtained from inverting the star formation law with the dynamical and stellar masses, we infer an average dark matter to total mass fraction within 2.2re (9.5 kpc) of 65 ± 12 per cent, in agreement with the results from hydrodynamic simulations of galaxy formation.

Distribution of phytoplankton functional types in high-nitrate, low-chlorophyll waters in a new diagnostic ecological indicator model

NASA Astrophysics Data System (ADS)

Palacz, A. P.; St. John, M. A.; Brewin, R. J. W.; Hirata, T.; Gregg, W. W.

2013-11-01

Modeling and monitoring plankton functional types (PFTs) is challenged by the insufficient amount of field measurements of ground truths in both plankton models and bio-optical algorithms. In this study, we combine remote sensing data and a dynamic plankton model to simulate an ecologically sound spatial and temporal distribution of phyto-PFTs. We apply an innovative ecological indicator approach to modeling PFTs and focus on resolving the question of diatom-coccolithophore coexistence in the subpolar high-nitrate and low-chlorophyll regions. We choose an artificial neural network as our modeling framework because it has the potential to interpret complex nonlinear interactions governing complex adaptive systems, of which marine ecosystems are a prime example. Using ecological indicators that fulfill the criteria of measurability, sensitivity and specificity, we demonstrate that our diagnostic model correctly interprets some basic ecological rules similar to ones emerging from dynamic models. Our time series highlight a dynamic phyto-PFT community composition in all high-latitude areas and indicate seasonal coexistence of diatoms and coccolithophores. This observation, though consistent with in situ and remote sensing measurements, has so far not been captured by state-of-the-art dynamic models, which struggle to resolve this "paradox of the plankton". We conclude that an ecological indicator approach is useful for ecological modeling of phytoplankton and potentially higher trophic levels. Finally, we speculate that it could serve as a powerful tool in advancing ecosystem-based management of marine resources.

Distribution of phytoplankton functional types in high-nitrate low-chlorophyll waters in a new diagnostic ecological indicator model

NASA Astrophysics Data System (ADS)

Palacz, A. P.; St. John, M. A.; Brewin, R. J. W.; Hirata, T.; Gregg, W. W.

2013-05-01

Modeling and monitoring plankton functional types (PFTs) is challenged by insufficient amount of field measurements to ground-truth both plankton models and bio-optical algorithms. In this study, we combine remote sensing data and a dynamic plankton model to simulate an ecologically-sound spatial and temporal distribution of phyto-PFTs. We apply an innovative ecological indicator approach to modeling PFTs, and focus on resolving the question of diatom-coccolithophore co-existence in the subpolar high-nitrate and low-chlorophyll regions. We choose an artificial neural network as our modeling framework because it has the potential to interpret complex nonlinear interactions governing complex adaptive systems, of which marine ecosystems are a prime example. Using ecological indicators that fulfill the criteria of measurability, sensitivity and specificity, we demonstrate that our diagnostic model correctly interprets some basic ecological rules similar to ones emerging from dynamic models. Our time series highlight a dynamic phyto-PFT community composition in all high latitude areas, and indicate seasonal co-existence of diatoms and coccolithophores. This observation, though consistent with in situ and remote sensing measurements, was so far not captured by state-of-the-art dynamic models which struggle to resolve this "paradox of the plankton". We conclude that an ecological indicator approach is useful for ecological modeling of phytoplankton and potentially higher trophic levels. Finally, we speculate that it could serve as a powerful tool in advancing ecosystem-based management of marine resources.

Cloud-System Resolving Models: Status and Prospects

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Moncreiff, Mitch

2008-01-01

Cloud-system resolving models (CRM), which are based on the nonhydrostatic equations of motion and typically have a grid-spacing of about a kilometer, originated as cloud-process models in the 1970s. This paper reviews the status and prospects of CRMs across a wide range of issues, such as microphysics and precipitation; interaction between clouds and radiation; and the effects of boundary-layer and surface-processes on cloud systems. Since CRMs resolve organized convection, tropical waves and the large-scale circulation, there is the prospect for several advances in both basic knowledge of scale-interaction requisite to parameterizing mesoscale processes in climate models. In superparameterization, CRMs represent convection, explicitly replacing many of the assumptions necessary in contemporary parameterization. Global CRMs have been run on an experimental basis, giving prospect to a new generation of climate weather prediction in a decade, and climate models due course. CRMs play a major role in the retrieval of surface-rain and latent heating from satellite measurements. Finally, enormous wide dynamic ranges of CRM simulations present new challenges for model validation against observations.

Nanoscale Characterization of Carrier Dynamic and Surface Passivation in InGaN/GaN Multiple Quantum Wells on GaN Nanorods.

PubMed

Chen, Weijian; Wen, Xiaoming; Latzel, Michael; Heilmann, Martin; Yang, Jianfeng; Dai, Xi; Huang, Shujuan; Shrestha, Santosh; Patterson, Robert; Christiansen, Silke; Conibeer, Gavin

2016-11-23

Using advanced two-photon excitation confocal microscopy, associated with time-resolved spectroscopy, we characterize InGaN/GaN multiple quantum wells on nanorod heterostructures and demonstrate the passivation effect of a KOH treatment. High-quality InGaN/GaN nanorods were fabricated using nanosphere lithography as a candidate material for light-emitting diode devices. The depth- and time-resolved characterization at the nanoscale provides detailed carrier dynamic analysis helpful for understanding the optical properties. The nanoscale spatially resolved images of InGaN quantum well and defects were acquired simultaneously. We demonstrate that nanorod etching improves light extraction efficiency, and a proper KOH treatment has been found to reduce the surface defects efficiently and enhance the luminescence. The optical characterization techniques provide depth-resolved and time-resolved carrier dynamics with nanoscale spatially resolved mapping, which is crucial for a comprehensive and thorough understanding of nanostructured materials and provides novel insight into the improvement of materials fabrication and applications.

Exciton dynamics in GaAs/(Al,Ga)As core-shell nanowires with shell quantum dots

NASA Astrophysics Data System (ADS)

Corfdir, Pierre; Küpers, Hanno; Lewis, Ryan B.; Flissikowski, Timur; Grahn, Holger T.; Geelhaar, Lutz; Brandt, Oliver

2016-10-01

We study the dynamics of excitons in GaAs/(Al,Ga)As core-shell nanowires by continuous-wave and time-resolved photoluminescence and photoluminescence excitation spectroscopy. Strong Al segregation in the shell of the nanowires leads to the formation of Ga-rich inclusions acting as quantum dots. At 10 K, intense light emission associated with these shell quantum dots is observed. The average radiative lifetime of excitons confined in the shell quantum dots is 1.7 ns. We show that excitons may tunnel toward adjacent shell quantum dots and nonradiative point defects. We investigate the changes in the dynamics of charge carriers in the shell with increasing temperature, with particular emphasis on the transfer of carriers from the shell to the core of the nanowires. We finally discuss the implications of carrier localization in the (Al,Ga)As shell for fundamental studies and optoelectronic applications based on core-shell III-As nanowires.

On Numerical Heating

NASA Astrophysics Data System (ADS)

Liou, Meng-Sing

2013-11-01

The development of computational fluid dynamics over the last few decades has yielded enormous successes and capabilities that are being routinely employed today; however there remain some open problems to be properly resolved. One example is the so-called overheating problem, which can arise in two very different scenarios, from either colliding or receding streams. Common in both is a localized, numerically over-predicted temperature. Von Neumann reported the former, a compressive overheating, nearly 70 years ago and numerically smeared the temperature peak by introducing artificial diffusion. However, the latter is unphysical in an expansive (rarefying) situation; it still dogs every method known to the author. We will present a study aiming at resolving this overheating problem and we find that: (1) the entropy increase is one-to-one linked to the increase in the temperature rise and (2) the overheating is inevitable in the current computational fluid dynamics framework in practice. Finally we will show a simple hybrid method that fundamentally cures the overheating problem in a rarefying flow, but also retains the property of accurate shock capturing. Moreover, this remedy (enhancement of current numerical methods) can be included easily in the present Eulerian codes. This work is performed under NASA's Fundamental Aeronautics Program.

Prediction of Precipitation Strengthening in the Commercial Mg Alloy AZ91 Using Dislocation Dynamics

DOE PAGES

Aagesen, L. K.; Miao, J.; Allison, J. E.; ...

2018-03-05

In this paper, dislocation dynamics simulations were used to predict the strengthening of a commercial magnesium alloy, AZ91, due to β-Mg 17Al 12 formed in the continuous precipitation mode. The precipitate distributions used in simulations were determined based on experimental characterization of the sizes, shapes, and number densities of the precipitates for 10-hour aging and 50-hour aging. For dislocations gliding on the basal plane, which is expected to be the dominant contributor to plastic deformation at room temperature, the critical resolved shear stress to bypass the precipitate distribution was 3.5 MPa for the 10-hour aged sample and 16.0 MPa formore » the 50-hour aged sample. The simulation results were compared to an analytical model of strengthening in this alloy, and the analytical model was found to predict critical resolved shear stresses that were approximately 30 pct lower. A model for the total yield strength was developed and compared with experiment for the 50-hour aged sample. Finally, the predicted yield strength, which included the precipitate strengthening contribution from the DD simulations, was 132.0 MPa, in good agreement with the measured yield strength of 141 MPa.« less

Prediction of Precipitation Strengthening in the Commercial Mg Alloy AZ91 Using Dislocation Dynamics

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

Aagesen, L. K.; Miao, J.; Allison, J. E.

In this paper, dislocation dynamics simulations were used to predict the strengthening of a commercial magnesium alloy, AZ91, due to β-Mg 17Al 12 formed in the continuous precipitation mode. The precipitate distributions used in simulations were determined based on experimental characterization of the sizes, shapes, and number densities of the precipitates for 10-hour aging and 50-hour aging. For dislocations gliding on the basal plane, which is expected to be the dominant contributor to plastic deformation at room temperature, the critical resolved shear stress to bypass the precipitate distribution was 3.5 MPa for the 10-hour aged sample and 16.0 MPa formore » the 50-hour aged sample. The simulation results were compared to an analytical model of strengthening in this alloy, and the analytical model was found to predict critical resolved shear stresses that were approximately 30 pct lower. A model for the total yield strength was developed and compared with experiment for the 50-hour aged sample. Finally, the predicted yield strength, which included the precipitate strengthening contribution from the DD simulations, was 132.0 MPa, in good agreement with the measured yield strength of 141 MPa.« less

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.

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.

Spatially resolved multicolor CsPbX 3 nanowire heterojunctions via anion exchange

DOE PAGES

Dou, Letian; Lai, Minliang; Kley, Christopher S.; ...

2017-06-26

Halide perovskites are promising semiconductor materials for solution-processed optoelectronic devices. Their strong ionic bonding nature results in highly dynamic crystal lattices, inherently allowing rapid ion exchange at the solid–vapor and solid–liquid interface. In this paper, we show that the anion-exchange chemistry can be precisely controlled in single-crystalline halide perovskite nanomaterials when combined with nanofabrication techniques. We demonstrate spatially resolved multicolor CsPbX 3 (X = Cl, Br, I, or alloy of two halides) nanowire heterojunctions with a pixel size down to 500 nm with the photoluminescence tunable over the entire visible spectrum. In addition, the heterojunctions show distinct electronic states acrossmore » the interface, as revealed by Kelvin probe force microscopy. Finally, these perovskite heterojunctions represent key building blocks for high-resolution multicolor displays beyond current state-of-the-art technology as well as high-density diode/transistor arrays.« less

Time-resolved, single-cell analysis of induced and programmed cell death via non-invasive propidium iodide and counterstain perfusion.

PubMed

Krämer, Christina E M; Wiechert, Wolfgang; Kohlheyer, Dietrich

2016-09-01

Conventional propidium iodide (PI) staining requires the execution of multiple steps prior to analysis, potentially affecting assay results as well as cell vitality. In this study, this multistep analysis method has been transformed into a single-step, non-toxic, real-time method via live-cell imaging during perfusion with 0.1 μM PI inside a microfluidic cultivation device. Dynamic PI staining was an effective live/dead analytical tool and demonstrated consistent results for single-cell death initiated by direct or indirect triggers. Application of this method for the first time revealed the apparent antibiotic tolerance of wild-type Corynebacterium glutamicum cells, as indicated by the conversion of violet fluorogenic calcein acetoxymethyl ester (CvAM). Additional implementation of this method provided insight into the induced cell lysis of Escherichia coli cells expressing a lytic toxin-antitoxin module, providing evidence for non-lytic cell death and cell resistance to toxin production. Finally, our dynamic PI staining method distinguished necrotic-like and apoptotic-like cell death phenotypes in Saccharomyces cerevisiae among predisposed descendants of nutrient-deprived ancestor cells using PO-PRO-1 or green fluorogenic calcein acetoxymethyl ester (CgAM) as counterstains. The combination of single-cell cultivation, fluorescent time-lapse imaging, and PI perfusion facilitates spatiotemporally resolved observations that deliver new insights into the dynamics of cellular behaviour.

Role of density modulation in the spatially resolved dynamics of strongly confined liquids

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

Saw, Shibu, E-mail: shibu.saw@sydney.edu.au; Dasgupta, Chandan, E-mail: cdgupta@physics.iisc.ernet.in

Confinement by walls usually produces a strong modulation in the density of dense liquids near the walls. Using molecular dynamics simulations, we examine the effects of the density modulation on the spatially resolved dynamics of a liquid confined between two parallel walls, using a resolution of a fraction of the interparticle distance in the liquid. The local dynamics is quantified by the relaxation time associated with the temporal autocorrelation function of the local density. We find that this local relaxation time varies in phase with the density modulation. The amplitude of the spatial modulation of the relaxation time can bemore » quite large, depending on the characteristics of the wall and thermodynamic parameters of the liquid. To disentangle the effects of confinement and density modulation on the spatially resolved dynamics, we compare the dynamics of a confined liquid with that of an unconfined one in which a similar density modulation is induced by an external potential. We find several differences indicating that density modulation alone cannot account for all the features seen in the spatially resolved dynamics of confined liquids. We also examine how the dynamics near a wall depends on the separation between the two walls and show that the features seen in our simulations persist in the limit of large wall separation.« less

A novel Kinetic Monte Carlo algorithm for Non-Equilibrium Simulations

NASA Astrophysics Data System (ADS)

Jha, Prateek; Kuzovkov, Vladimir; Grzybowski, Bartosz; Olvera de La Cruz, Monica

2012-02-01

We have developed an off-lattice kinetic Monte Carlo simulation scheme for reaction-diffusion problems in soft matter systems. The definition of transition probabilities in the Monte Carlo scheme are taken identical to the transition rates in a renormalized master equation of the diffusion process and match that of the Glauber dynamics of Ising model. Our scheme provides several advantages over the Brownian dynamics technique for non-equilibrium simulations. Since particle displacements are accepted/rejected in a Monte Carlo fashion as opposed to moving particles following a stochastic equation of motion, nonphysical movements (e.g., violation of a hard core assumption) are not possible (these moves have zero acceptance). Further, the absence of a stochastic ``noise'' term resolves the computational difficulties associated with generating statistically independent trajectories with definitive mean properties. Finally, since the timestep is independent of the magnitude of the interaction forces, much longer time-steps can be employed than Brownian dynamics. We discuss the applications of this scheme for dynamic self-assembly of photo-switchable nanoparticles and dynamical problems in polymeric systems.

Resolvent-based modeling of passive scalar dynamics in wall-bounded turbulence

NASA Astrophysics Data System (ADS)

Dawson, Scott; Saxton-Fox, Theresa; McKeon, Beverley

2017-11-01

The resolvent formulation of the Navier-Stokes equations expresses the system state as the output of a linear (resolvent) operator acting upon a nonlinear forcing. Previous studies have demonstrated that a low-rank approximation of this linear operator predicts many known features of incompressible wall-bounded turbulence. In this work, this resolvent model for wall-bounded turbulence is extended to include a passive scalar field. This formulation allows for a number of additional simplifications that reduce model complexity. Firstly, it is shown that the effect of changing scalar diffusivity can be approximated through a transformation of spatial wavenumbers and temporal frequencies. Secondly, passive scalar dynamics may be studied through the low-rank approximation of a passive scalar resolvent operator, which is decoupled from velocity response modes. Thirdly, this passive scalar resolvent operator is amenable to approximation by semi-analytic methods. We investigate the extent to which this resulting hierarchy of models can describe and predict passive scalar dynamics and statistics in wall-bounded turbulence. The support of AFOSR under Grant Numbers FA9550-16-1-0232 and FA9550-16-1-0361 is gratefully acknowledged.

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

PubMed

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

2017-08-02

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

Combining Graphical and Analytical Methods with Molecular Simulations To Analyze Time-Resolved FRET Measurements of Labeled Macromolecules Accurately

PubMed Central

2017-01-01

Förster resonance energy transfer (FRET) measurements from a donor, D, to an acceptor, A, fluorophore are frequently used in vitro and in live cells to reveal information on the structure and dynamics of DA labeled macromolecules. Accurate descriptions of FRET measurements by molecular models are complicated because the fluorophores are usually coupled to the macromolecule via flexible long linkers allowing for diffusional exchange between multiple states with different fluorescence properties caused by distinct environmental quenching, dye mobilities, and variable DA distances. It is often assumed for the analysis of fluorescence intensity decays that DA distances and D quenching are uncorrelated (homogeneous quenching by FRET) and that the exchange between distinct fluorophore states is slow (quasistatic). This allows us to introduce the FRET-induced donor decay, εD(t), a function solely depending on the species fraction distribution of the rate constants of energy transfer by FRET, for a convenient joint analysis of fluorescence decays of FRET and reference samples by integrated graphical and analytical procedures. Additionally, we developed a simulation toolkit to model dye diffusion, fluorescence quenching by the protein surface, and FRET. A benchmark study with simulated fluorescence decays of 500 protein structures demonstrates that the quasistatic homogeneous model works very well and recovers for single conformations the average DA distances with an accuracy of < 2%. For more complex cases, where proteins adopt multiple conformations with significantly different dye environments (heterogeneous case), we introduce a general analysis framework and evaluate its power in resolving heterogeneities in DA distances. The developed fast simulation methods, relying on Brownian dynamics of a coarse-grained dye in its sterically accessible volume, allow us to incorporate structural information in the decay analysis for heterogeneous cases by relating dye states with protein conformations to pave the way for fluorescence and FRET-based dynamic structural biology. Finally, we present theories and simulations to assess the accuracy and precision of steady-state and time-resolved FRET measurements in resolving DA distances on the single-molecule and ensemble level and provide a rigorous framework for estimating approximation, systematic, and statistical errors. PMID:28709377

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

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

PubMed

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

2017-05-05

Time-resolved temperature-jump (T-jump) coupled with fluorescence and infrared (IR) spectroscopy is a powerful technique for monitoring protein dynamics. Although IR spectroscopy of the polypeptide amide I mode is more technically challenging, it offers complementary information because it directly probes changes in the protein backbone, whereas, fluorescence spectroscopy is sensitive to the environment of specific side chains. With the advent of widely tunable quantum cascade lasers (QCL) it is possible to efficiently probe multiple IR frequencies with high sensitivity and reproducibility. Here we describe a dual time-resolved T-jump fluorescence and IR spectrometer and its application to study protein folding dynamics. A Q-switched Ho:YAG laser provides the T-jump source for both time-resolved IR and fluorescence spectroscopy, which are probed by a QCL and Ti:Sapphire laser, respectively. The Ho:YAG laser simultaneously pumps the time-resolved IR and fluorescence spectrometers. The instrument has high sensitivity, with an IR absorbance detection limit of <0.2mOD and a fluorescence sensitivity of 2% of the overall fluorescence intensity. Using a computer controlled QCL to rapidly tune the IR frequency it is possible to create a T-jump induced difference spectrum from 50ns to 0.5ms. This study demonstrates the power of the dual time-resolved T-jump fluorescence and IR spectroscopy to resolve complex folding mechanisms by complementary IR absorbance and fluorescence measurements of protein dynamics. Copyright © 2017 Elsevier B.V. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2017-05-01

Time-resolved temperature-jump (T-jump) coupled with fluorescence and infrared (IR) spectroscopy is a powerful technique for monitoring protein dynamics. Although IR spectroscopy of the polypeptide amide I mode is more technically challenging, it offers complementary information because it directly probes changes in the protein backbone, whereas, fluorescence spectroscopy is sensitive to the environment of specific side chains. With the advent of widely tunable quantum cascade lasers (QCL) it is possible to efficiently probe multiple IR frequencies with high sensitivity and reproducibility. Here we describe a dual time-resolved T-jump fluorescence and IR spectrometer and its application to study protein folding dynamics. A Q-switched Ho:YAG laser provides the T-jump source for both time-resolved IR and fluorescence spectroscopy, which are probed by a QCL and Ti:Sapphire laser, respectively. The Ho:YAG laser simultaneously pumps the time-resolved IR and fluorescence spectrometers. The instrument has high sensitivity, with an IR absorbance detection limit of < 0.2 mOD and a fluorescence sensitivity of 2% of the overall fluorescence intensity. Using a computer controlled QCL to rapidly tune the IR frequency it is possible to create a T-jump induced difference spectrum from 50 ns to 0.5 ms. This study demonstrates the power of the dual time-resolved T-jump fluorescence and IR spectroscopy to resolve complex folding mechanisms by complementary IR absorbance and fluorescence measurements of protein dynamics.

Helix formation via conformation diffusion search

PubMed Central

Huang, Cheng-Yen; Getahun, Zelleka; Zhu, Yongjin; Klemke, Jason W.; DeGrado, William F.; Gai, Feng

2002-01-01

The helix-coil transition kinetics of an α-helical peptide were investigated by time-resolved infrared spectroscopy coupled with laser-induced temperature-jump initiation method. Specific isotope labeling of the amide carbonyl groups with 13C at selected residues was used to obtain site-specific information. The relaxation kinetics following a temperature jump, obtained by probing the amide I′ band of the peptide backbone, exhibit nonexponential behavior and are sensitive to both initial and final temperatures. These data are consistent with a conformation diffusion process on the folding energy landscape, in accord with a recent molecular dynamics simulation study. PMID:11867741

All-Atom Multiscale Molecular Dynamics Theory and Simulation of Self-Assembly, Energy Transfer and Structural Transition in Nanosystems

NASA Astrophysics Data System (ADS)

Espinosa Duran, John Michael

The study of nanosystems and their emergent properties requires the development of multiscale computational models, theories and methods that preserve atomic and femtosecond resolution, to reveal details that cannot be resolved experimentally today. Considering this, three long time scale phenomena were studied using molecular dynamics and multiscale methods: self-assembly of organic molecules on graphite, energy transfer in nanosystems, and structural transition in vault nanoparticles. Molecular dynamics simulations of the self-assembly of alkoxybenzonitriles with different tail lengths on graphite were performed to learn about intermolecular interactions and phases exhibited by self-organized materials. This is important for the design of ordered self-assembled organic photovoltaic materials with greater efficiency than the disordered blends. Simulations revealed surface dynamical behaviors that cannot be resolved experimentally today due to the lack of spatiotemporal resolution. Atom-resolved structures predicted by simulations agreed with scanning tunneling microscopy images and unit cell measurements. Then, a multiscale theory based on the energy density as a field variable is developed to study energy transfer in nanoscale systems. For applications like photothermal microscopy or cancer phototherapy is required to understand how the energy is transferred to/from nanosystems. This multiscale theory could be applied in this context and here is tested for cubic nanoparticles immersed in water for energy being transferred to/from the nanoparticle. The theory predicts the energy transfer dynamics and reveals phenomena that cannot be described by current phenomenological theories. Finally, temperature-triggered structural transitions were revealed for vault nanoparticles using molecular dynamics and multiscale simulations. Vault is a football-shaped supramolecular assembly very distinct from the commonly observed icosahedral viruses. It has very promising applications in drug delivery and has been extensively studied experimentally. Sub-microsecond multiscale simulations at 310 K on the vault revealed the opening and closing of fractures near the shoulder while preserving the overall structure. This fracture mechanism could explain the uptake and release of small drugs while maintaining the overall structure. Higher temperature simulations show the generation of large fractures near the waist, which enables interaction of the external medium with the inner vault residues. Simulation results agreed with microscopy and spectroscopy measurements, and revealed new structures and mechanisms.

Spectrally resolved femtosecond photon echo spectroscopy of astaxanthin

NASA Astrophysics Data System (ADS)

Kumar, Ajitesh; Karthick Kumar, S. K.; Gupta, Aditya; Goswami, Debabrata

2010-12-01

We have studied the coherence and population dynamics of Astaxanthin solution in methanol and acetonitrile by spectrally resolving their photon echo signals. Our experiments indicate that methanol has a much stronger interaction with the ultrafast dynamics of Astaxanthin in comparison to that of acetonitrile.

Spectrally resolved femtosecond photon echo spectroscopy of astaxanthin

NASA Astrophysics Data System (ADS)

Kumar, Ajitesh; Karthick Kumar, S. K.; Gupta, Aditya; Goswami, Debabrata

2011-08-01

We have studied the coherence and population dynamics of Astaxanthin solution in methanol and acetonitrile by spectrally resolving their photon echo signals. Our experiments indicate that methanol has a much stronger interaction with the ultrafast dynamics of Astaxanthin in comparison to that of acetonitrile.

Doppler effects on 3-D non-LTE radiation transport and emission spectra.

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

Giuliani, J. L.; Davis, J.; DasGupta, A.

2010-10-01

Spatially and temporally resolved X-ray emission lines contain information about temperatures, densities, velocities, and the gradients in a plasma. Extracting this information from optically thick lines emitted from complex ions in dynamic, three-dimensional, non-LTE plasmas requires self-consistent accounting for both non-LTE atomic physics and non-local radiative transfer. We present a brief description of a hybrid-structure spectroscopic atomic model coupled to an iterative tabular on-the-spot treatment of radiative transfer that can be applied to plasmas of arbitrary material composition, conditions, and geometries. The effects of Doppler line shifts on the self-consistent radiative transfer within the plasma and the emergent emission andmore » absorption spectra are included in the model. Sample calculations for a two-level atom in a uniform cylindrical plasma are given, showing reasonable agreement with more sophisticated transport models and illustrating the potential complexity - or richness - of radially resolved emission lines from an imploding cylindrical plasma. Also presented is a comparison of modeled L- and K-shell spectra to temporally and radially resolved emission data from a Cu:Ni plasma. Finally, some shortcomings of the model and possible paths for improvement are discussed.« less

Mechanical Modulation of Nascent Stem Cell Lineage Commitment in Tissue Engineering Scaffolds

PubMed Central

Song, Min Jae; Dean, David; Tate, Melissa L. Knothe

2013-01-01

Taking inspiration from tissue morphogenesis in utero, this study tests the concept of using tissue engineering scaffolds as delivery devices to modulate emergent structure-function relationships at early stages of tissue genesis. We report on the use of a combined computational fluid dynamics (CFD) modeling, advanced manufacturing methods, and experimental fluid mechanics (micro-piv and strain mapping) for the prospective design of tissue engineering scaffold geometries that deliver spatially resolved mechanical cues to cells seeded within. When subjected to a constant magnitude global flow regime, the local scaffold geometry dictates the magnitudes of mechanical stresses and strains experienced by a given cell, and in a spatially resolved fashion, similar to patterning during morphogenesis. In addition, early markers of mesenchymal stem cell lineage commitment relate significantly to the local mechanical environment of the cell. Finally, by plotting the range of stress-strain states for all data corresponding to nascent cell lineage commitment (95% CI), we begin to “map the mechanome”, defining stress-strain states most conducive to targeted cell fates. In sum, we provide a library of reference mechanical cues that can be delivered to cells seeded on tissue engineering scaffolds to guide target tissue phenotypes in a temporally and spatially resolved manner. Knowledge of these effects allows for prospective scaffold design optimization using virtual models prior to prototyping and clinical implementation. Finally, this approach enables the development of next generation scaffolds cum delivery devices for genesis of complex tissues with heterogenous properties, e.g., organs, joints or interface tissues such as growth plates. PMID:23660249

Mechanical modulation of nascent stem cell lineage commitment in tissue engineering scaffolds.

PubMed

Song, Min Jae; Dean, David; Knothe Tate, Melissa L

2013-07-01

Taking inspiration from tissue morphogenesis in utero, this study tests the concept of using tissue engineering scaffolds as delivery devices to modulate emergent structure-function relationships at early stages of tissue genesis. We report on the use of a combined computational fluid dynamics (CFD) modeling, advanced manufacturing methods, and experimental fluid mechanics (micro-piv and strain mapping) for the prospective design of tissue engineering scaffold geometries that deliver spatially resolved mechanical cues to stem cells seeded within. When subjected to a constant magnitude global flow regime, the local scaffold geometry dictates the magnitudes of mechanical stresses and strains experienced by a given cell, and in a spatially resolved fashion, similar to patterning during morphogenesis. In addition, early markers of mesenchymal stem cell lineage commitment relate significantly to the local mechanical environment of the cell. Finally, by plotting the range of stress-strain states for all data corresponding to nascent cell lineage commitment (95% CI), we begin to "map the mechanome", defining stress-strain states most conducive to targeted cell fates. In sum, we provide a library of reference mechanical cues that can be delivered to cells seeded on tissue engineering scaffolds to guide target tissue phenotypes in a temporally and spatially resolved manner. Knowledge of these effects allows for prospective scaffold design optimization using virtual models prior to prototyping and clinical implementation. Finally, this approach enables the development of next generation scaffolds cum delivery devices for genesis of complex tissues with heterogenous properties, e.g., organs, joints or interface tissues such as growth plates. Copyright © 2013 Elsevier Ltd. All rights reserved.

Microbial processes in marine ecosystem models: state of the art and future prospective

NASA Astrophysics Data System (ADS)

Polimene, L.; Butenschon, M.; Blackford, J.; Allen, I.

2012-12-01

Heterotrophic bacteria play a key role in the marine biogeochemistry being the main consumer of dissolved organic matter (DOM) and the main producer of carbon dioxide (CO2) by respiration. Quantifying the carbon and energy fluxes within bacteria (i.e. production, respiration, overflow metabolism etc.) is therefore crucial for the assessment of the global ocean carbon and nutrient cycles. Consequently, the description of bacteria dynamic in ecosystem models is a key (although challenging) issue which cannot be overlooked if we want to properly simulate the marine environment. We present an overview of the microbial processes described in the European Sea Regional Ecosystem Model (ERSEM), a state of the art biogeochemical model resolving carbon and nutrient cycles (N, P, Si and Fe) within the low trophic levels (up to mesozooplankton) of the marine ecosystem. The description of the theoretical assumptions and philosophy underpinning the ERSEM bacteria sub-model will be followed by the presentation of some case studies highlighting the relevance of resolving microbial processes in the simulation of ecosystem dynamics at a local scale. Recent results concerning the implementation of ERSEM on a global ocean domain will be also presented. This latter exercise includes a comparison between simulations carried out with the full bacteria sub-model and simulations carried out with an implicit parameterization of bacterial activity. The results strongly underline the importance of explicitly resolved bacteria in the simulation of global carbon fluxes. Finally, a summary of the future developments along with issues still open on the topic will be presented and discussed.

Interferometric Near-Infrared Spectroscopy (iNIRS) for determination of optical and dynamical properties of turbid media

PubMed Central

Borycki, Dawid; Kholiqov, Oybek; Chong, Shau Poh; Srinivasan, Vivek J.

2016-01-01

We introduce and implement interferometric near-infrared spectroscopy (iNIRS), which simultaneously extracts optical and dynamical properties of turbid media through analysis of a spectral interference fringe pattern. The spectral interference fringe pattern is measured using a Mach-Zehnder interferometer with a frequency-swept narrow linewidth laser. Fourier analysis of the detected signal is used to determine time-of-flight (TOF)-resolved intensity, which is then analyzed over time to yield TOF-resolved intensity autocorrelations. This approach enables quantification of optical properties, which is not possible in conventional, continuous-wave near-infrared spectroscopy (NIRS). Furthermore, iNIRS quantifies scatterer motion based on TOF-resolved autocorrelations, which is a feature inaccessible by well-established diffuse correlation spectroscopy (DCS) techniques. We prove this by determining TOF-resolved intensity and temporal autocorrelations for light transmitted through diffusive fluid phantoms with optical thicknesses of up to 55 reduced mean free paths (approximately 120 scattering events). The TOF-resolved intensity is used to determine optical properties with time-resolved diffusion theory, while the TOF-resolved intensity autocorrelations are used to determine dynamics with diffusing wave spectroscopy. iNIRS advances the capabilities of diffuse optical methods and is suitable for in vivo tissue characterization. Moreover, iNIRS combines NIRS and DCS capabilities into a single modality. PMID:26832264

Quarter-flux Hofstadter lattice in a qubit-compatible microwave cavity array

NASA Astrophysics Data System (ADS)

Owens, Clai; LaChapelle, Aman; Saxberg, Brendan; Anderson, Brandon M.; Ma, Ruichao; Simon, Jonathan; Schuster, David I.

2018-01-01

Topological and strongly correlated materials are exciting frontiers in condensed-matter physics, married prominently in studies of the fractional quantum Hall effect [H. L. Stormer et al., Rev. Mod. Phys. 71, S298 (1999), 10.1103/RevModPhys.71.S298], There is an active effort to develop synthetic materials where the microscopic dynamics and ordering arising from the interplay of topology and interaction may be directly explored. In this work, we demonstrate an architecture for exploration of topological matter constructed from tunnel-coupled, time-reversal-broken microwave cavities that are both low loss and compatible with Josephson-junction-mediated interactions [A. Wallraff et al., Nature (London) 431, 162 (2004), 10.1038/nature02851]. Following our proposed protocol [B. M. Anderson et al., Phys. Rev. X 6, 041043 (2016), 10.1103/PhysRevX.6.041043], we implement a square lattice Hofstadter model at a quarter flux per plaquette (α =1 /4 ), with time-reversal symmetry broken through the chiral Wannier orbital of resonators coupled to yttrium-iron-garnet spheres. We demonstrate site-resolved spectroscopy of the lattice, time-resolved dynamics of its edge channels, and a direct measurement of the dispersion of the edge channels. Finally, we demonstrate the flexibility of the approach by erecting a tunnel barrier and investigating dynamics across it. With the introduction of Josephson junctions to mediate interactions between photons, this platform is poised to explore strongly correlated topological quantum science in a synthetic system.

Interaction of Atmospheric Turbulence with Blade Boundary Layer Dynamics on a 5MW Wind Turbine using Blade-Boundary-Layer-Resolved CFD with hybrid URANS-LES.

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

Vijayakumar, Ganesh; Brasseur, James; Lavely, Adam

We describe the response of the NREL 5 MW wind turbine blade boundary layer to the passage of atmospheric turbulence using blade-boundary-layer-resolved computational fluid dynamics with hybrid URANS-LES modeling.

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

Overflow Simulations using MPAS-Ocean in Idealized and Realistic Domains

NASA Astrophysics Data System (ADS)

Reckinger, S.; Petersen, M. R.; Reckinger, S. J.

2016-02-01

MPAS-Ocean is used to simulate an idealized, density-driven overflow using the dynamics of overflow mixing and entrainment (DOME) setup. Numerical simulations are benchmarked against other models, including the MITgcm's z-coordinate model and HIM's isopycnal coordinate model. A full parameter study is presented that looks at how sensitive overflow simulations are to vertical grid type, resolution, and viscosity. Horizontal resolutions with 50 km grid cells are under-resolved and produce poor results, regardless of other parameter settings. Vertical grids ranging in thickness from 15 m to 120 m were tested. A horizontal resolution of 10 km and a vertical resolution of 60 m are sufficient to resolve the mesoscale dynamics of the DOME configuration, which mimics real-world overflow parameters. Mixing and final buoyancy are least sensitive to horizontal viscosity, but strongly sensitive to vertical viscosity. This suggests that vertical viscosity could be adjusted in overflow water formation regions to influence mixing and product water characteristics. Also, the study shows that sigma coordinates produce much less mixing than z-type coordinates, resulting in heavier plumes that go further down slope. Sigma coordinates are less sensitive to changes in resolution but as sensitive to vertical viscosity compared to z-coordinates. Additionally, preliminary measurements of overflow diagnostics on global simulations using a realistic oceanic domain are presented.

Revealing the subfemtosecond dynamics of orbital angular momentum in nanoplasmonic vortices

NASA Astrophysics Data System (ADS)

Spektor, G.; Kilbane, D.; Mahro, A. K.; Frank, B.; Ristok, S.; Gal, L.; Kahl, P.; Podbiel, D.; Mathias, S.; Giessen, H.; Meyer zu Heringdorf, F.-J.; Orenstein, M.; Aeschlimann, M.

2017-03-01

The ability of light to carry and deliver orbital angular momentum (OAM) in the form of optical vortices has attracted much interest. The physical properties of light with a helical wavefront can be confined onto two-dimensional surfaces with subwavelength dimensions in the form of plasmonic vortices, opening avenues for thus far unknown light-matter interactions. Because of their extreme rotational velocity, the ultrafast dynamics of such vortices remained unexplored. Here we show the detailed spatiotemporal evolution of nanovortices using time-resolved two-photon photoemission electron microscopy. We observe both long- and short-range plasmonic vortices confined to deep subwavelength dimensions on the scale of 100 nanometers with nanometer spatial resolution and subfemtosecond time-step resolution. Finally, by measuring the angular velocity of the vortex, we directly extract the OAM magnitude of light.

Excited state and charge-carrier dynamics in perovskite solar cell materials

NASA Astrophysics Data System (ADS)

Ponseca, Carlito S., Jr.; Tian, Yuxi; Sundström, Villy; Scheblykin, Ivan G.

2016-02-01

Organo-metal halide perovskites (OMHPs) have attracted enormous interest in recent years as materials for application in optoelectronics and solar energy conversion. These hybrid semiconductors seem to have the potential to challenge traditional silicon technology. In this review we will give an account of the recent development in the understanding of the fundamental light-induced processes in OMHPs from charge-photo generation, migration of charge carries through the materials and finally their recombination. Our and other literature reports on time-resolved conductivity, transient absorption and photoluminescence properties are used to paint a picture of how we currently see the fundamental excited state and charge-carrier dynamics. We will also show that there is still no fully coherent picture of the processes in OMHPs and we will indicate the problems to be solved by future research.

Improving the Dynamic Emissivity Measurement Above 1000 K by Extending the Spectral Range

NASA Astrophysics Data System (ADS)

Urban, D.; Krenek, S.; Anhalt, K.; Taubert, D. R.

2018-01-01

To improve the dynamic emissivity measurement, which is based on the laser-flash method, an array spectrometer is characterized regarding its spectral radiance responsivity for a spectrally resolved emissivity measurement above 1000 K in the wavelength range between 550 nm and 1100 nm. Influences like dark signals, the nonlinearity of the detector, the size-of-source effect, wavelength calibration and the spectral radiance responsivity of the system are investigated to obtain an uncertainty budget for the spectral radiance and emissivity measurements. Uncertainties for the spectral radiance of lower than a relative 2 % are achieved for wavelengths longer than 550 nm. Finally, the spectral emissivity of a graphite sample was determined in the temperature range between 1000 K and 1700 K, and the experimental data show a good repeatability and agreement with literature data.

Dynamic Smagorinsky model on anisotropic grids

NASA Technical Reports Server (NTRS)

Scotti, A.; Meneveau, C.; Fatica, M.

1996-01-01

Large Eddy Simulation (LES) of complex-geometry flows often involves highly anisotropic meshes. To examine the performance of the dynamic Smagorinsky model in a controlled fashion on such grids, simulations of forced isotropic turbulence are performed using highly anisotropic discretizations. The resulting model coefficients are compared with a theoretical prediction (Scotti et al., 1993). Two extreme cases are considered: pancake-like grids, for which two directions are poorly resolved compared to the third, and pencil-like grids, where one direction is poorly resolved when compared to the other two. For pancake-like grids the dynamic model yields the results expected from the theory (increasing coefficient with increasing aspect ratio), whereas for pencil-like grids the dynamic model does not agree with the theoretical prediction (with detrimental effects only on smallest resolved scales). A possible explanation of the departure is attempted, and it is shown that the problem may be circumvented by using an isotropic test-filter at larger scales. Overall, all models considered give good large-scale results, confirming the general robustness of the dynamic and eddy-viscosity models. But in all cases, the predictions were poor for scales smaller than that of the worst resolved direction.

Probing Cosmic Gas Accretion with RESOLVE and ECO

NASA Astrophysics Data System (ADS)

Kannappan, Sheila; Eckert, Kathleen D.; Stark, David; Lagos, Claudia; Nasipak, Zachary; Moffett, Amanda J.; Baker, Ashley; Berlind, Andreas A.; Hoversten, Erik A.; Norris, Mark A.; RESOLVE Team

2016-01-01

We review results bearing on the existence, controlling factors, and mechanisms of cosmic gas accretion in the RESOLVE and ECO surveys. Volume-limited analysis of RESOLVE's complete census of HI-to-stellar mass ratios and star formation histories for ~1500 galaxies points to the necessity of an "open box" model of galaxy fueling, with the most gas-dominated galaxies doubling their stellar masses on ~Gyr timescales in a regime of rapid accretion. Transitions in gas richness and disk-building activity for isolated or central galaxies with halo masses near ~10^11.5 Msun and ~10^12 Msun plausibly correspond to the endpoints of a theoretically predicted transition in halo gas temperature that slows accretion across this range. The same mass range is associated with the initial grouping of isolated galaxies into common halos, where "isolated" is defined relative to the survey baryonic mass limits of >~10^9 Msun. Above 10^11.5 Msun, patterns in central vs. satellite gas richness as a function of group halo mass suggest that galaxy refueling is valved off from the inside out as the halo grows, with total quenching beyond the virial radius for halo masses >~10^13-13.5 Msun. Within the transition range from ~10^11.5-10^12 Msun, theoretical models predict >3 dex dispersion in ratios of uncooled halo gas to cold gas in galaxies (or more generally gas and stars). In RESOLVE and ECO, the baryonic mass function of galaxies in this transitional halo mass range displays signs of stripping or destruction of satellites, leading us to investigate a possible connection with halo gas heating using central galaxy color and group dynamics to probe group evolutionary state. Finally, we take a first look at how internal variations in metallicity, dynamics, and star formation constrain accretion mechanisms such as cold streams, induced extraplanar gas cooling, isotropic halo gas cooling, and gas-rich merging in different mass and environment regimes. The RESOLVE and ECO surveys have been supported by funding from NSF grants AST-0955368 and OCI-1156614.

Nitrogen dynamics in managed boreal forests: Recent advances and future research directions.

PubMed

Sponseller, Ryan A; Gundale, Michael J; Futter, Martyn; Ring, Eva; Nordin, Annika; Näsholm, Torgny; Laudon, Hjalmar

2016-02-01

Nitrogen (N) availability plays multiple roles in the boreal landscape, as a limiting nutrient to forest growth, determinant of terrestrial biodiversity, and agent of eutrophication in aquatic ecosystems. We review existing research on forest N dynamics in northern landscapes and address the effects of management and environmental change on internal cycling and export. Current research foci include resolving the nutritional importance of different N forms to trees and establishing how tree-mycorrhizal relationships influence N limitation. In addition, understanding how forest responses to external N inputs are mediated by above- and belowground ecosystem compartments remains an important challenge. Finally, forestry generates a mosaic of successional patches in managed forest landscapes, with differing levels of N input, biological demand, and hydrological loss. The balance among these processes influences the temporal patterns of stream water chemistry and the long-term viability of forest growth. Ultimately, managing forests to keep pace with increasing demands for biomass production, while minimizing environmental degradation, will require multi-scale and interdisciplinary perspectives on landscape N dynamics.

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.

Athermal brittle-to-ductile transition in amorphous solids.

PubMed

Dauchot, Olivier; Karmakar, Smarajit; Procaccia, Itamar; Zylberg, Jacques

2011-10-01

Brittle materials exhibit sharp dynamical fractures when meeting Griffith's criterion, whereas ductile materials blunt a sharp crack by plastic responses. Upon continuous pulling, ductile materials exhibit a necking instability that is dominated by a plastic flow. Usually one discusses the brittle to ductile transition as a function of increasing temperature. We introduce an athermal brittle to ductile transition as a function of the cutoff length of the interparticle potential. On the basis of extensive numerical simulations of the response to pulling the material boundaries at a constant speed we offer an explanation of the onset of ductility via the increase in the density of plastic modes as a function of the potential cutoff length. Finally we can resolve an old riddle: In experiments brittle materials can be strained under grip boundary conditions and exhibit a dynamic crack when cut with a sufficiently long initial slot. Mysteriously, in molecular dynamics simulations it appeared that cracks refused to propagate dynamically under grip boundary conditions, and continuous pulling was necessary to achieve fracture. We argue that this mystery is removed when one understands the distinction between brittle and ductile athermal amorphous materials.

Adaptive robust control of a class of non-affine variable-speed variable-pitch wind turbines with unmodeled dynamics.

PubMed

Bagheri, Pedram; Sun, Qiao

2016-07-01

In this paper, a novel synthesis of Nussbaum-type functions, and an adaptive radial-basis function neural network is proposed to design controllers for variable-speed, variable-pitch wind turbines. Dynamic equations of the wind turbine are highly nonlinear, uncertain, and affected by unknown disturbance sources. Furthermore, the dynamic equations are non-affine with respect to the pitch angle, which is a control input. To address these problems, a Nussbaum-type function, along with a dynamic control law are adopted to resolve the non-affine nature of the equations. Moreover, an adaptive radial-basis function neural network is designed to approximate non-parametric uncertainties. Further, the closed-loop system is made robust to unknown disturbance sources, where no prior knowledge of disturbance bound is assumed in advance. Finally, the Lyapunov stability analysis is conducted to show the stability of the entire closed-loop system. In order to verify analytical results, a simulation is presented and the results are compared to both a PI and an existing adaptive controllers. Copyright © 2016 ISA. Published by Elsevier Ltd. All rights reserved.

Attosecond Spectroscopy Probing Electron Correlation Dynamics

NASA Astrophysics Data System (ADS)

Winney, Alexander H.

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

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

"Structure and dynamics in complex chemical systems: Gaining new insights through recent advances in time-resolved spectroscopies.” ACS Division of Physical Chemistry Symposium presented at the Fall National ACS Meeting in Boston, MA, August 2015

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

Crawford, Daniel

8-Session Symposium on STRUCTURE AND DYNAMICS IN COMPLEX CHEMICAL SYSTEMS: GAINING NEW INSIGHTS THROUGH RECENT ADVANCES IN TIME-RESOLVED SPECTROSCOPIES. The intricacy of most chemical, biochemical, and material processes and their applications are underscored by the complex nature of the environments in which they occur. Substantial challenges for building a global understanding of a heterogeneous system include (1) identifying unique signatures associated with specific structural motifs within the heterogeneous distribution, and (2) resolving the significance of each of multiple time scales involved in both small- and large-scale nuclear reorganization. This symposium focuses on the progress in our understanding of dynamics inmore » complex systems driven by recent innovations in time-resolved spectroscopies and theoretical developments. Such advancement is critical for driving discovery at the molecular level facilitating new applications. Broad areas of interest include: Structural relaxation and the impact of structure on dynamics in liquids, interfaces, biochemical systems, materials, and other heterogeneous environments.« less

Metabolic gene regulation in a dynamically changing environment.

PubMed

Bennett, Matthew R; Pang, Wyming Lee; Ostroff, Natalie A; Baumgartner, Bridget L; Nayak, Sujata; Tsimring, Lev S; Hasty, Jeff

2008-08-28

Natural selection dictates that cells constantly adapt to dynamically changing environments in a context-dependent manner. Gene-regulatory networks often mediate the cellular response to perturbation, and an understanding of cellular adaptation will require experimental approaches aimed at subjecting cells to a dynamic environment that mimics their natural habitat. Here we monitor the response of Saccharomyces cerevisiae metabolic gene regulation to periodic changes in the external carbon source by using a microfluidic platform that allows precise, dynamic control over environmental conditions. We show that the metabolic system acts as a low-pass filter that reliably responds to a slowly changing environment, while effectively ignoring fast fluctuations. The sensitive low-frequency response was significantly faster than in predictions arising from our computational modelling, and this discrepancy was resolved by the discovery that two key galactose transcripts possess half-lives that depend on the carbon source. Finally, to explore how induction characteristics affect frequency response, we compare two S. cerevisiae strains and show that they have the same frequency response despite having markedly different induction properties. This suggests that although certain characteristics of the complex networks may differ when probed in a static environment, the system has been optimized for a robust response to a dynamically changing environment.

The Efficacy of Psychophysiological Measures for Implementing Adaptive Technology

NASA Technical Reports Server (NTRS)

Scerbo, Mark W.; Freeman, Frederick G.; Mikulka, Peter J.; Parasuraman, Raja; DiNocero, Francesco; Prinzel, Lawrence J., III

2001-01-01

Adaptive automation refers to technology that can change its mode of operation dynamically. Further, both the technology and the operator can initiate changes in the level or mode of automation. The present paper reviews research on adaptive technology. It is divided into three primary sections. In the first section, issues surrounding the development and implementation of adaptive automation are presented. Because physiological-based measures show much promise for implementing adaptive automation, the second section is devoted to examining candidate indices. In the final section, those techniques that show the greatest promise for adaptive automation as well as issues that still need to be resolved are discussed.

Entering an era of dynamic structural biology….

PubMed

Orville, Allen M

2018-05-31

A recent paper in BMC Biology presents a general method for mix-and-inject serial crystallography, to facilitate the visualization of enzyme intermediates via time-resolved serial femtosecond crystallography (tr-SFX). They apply their method to resolve in near atomic detail the cleavage and inactivation of the antibiotic ceftriaxone by a β-lactamase enzyme from Mycobacterium tuberculosis. Their work demonstrates the general applicability of time-resolved crystallography, from which dynamic structures, at atomic resolution, can be obtained.See research article: https://bmcbiol.biomedcentral.com/articles/10.1186/s12915-018-0524-5 .

Polynomial-time solution of prime factorization and NP-complete problems with digital memcomputing machines

NASA Astrophysics Data System (ADS)

Traversa, Fabio L.; Di Ventra, Massimiliano

2017-02-01

We introduce a class of digital machines, we name Digital Memcomputing Machines, (DMMs) able to solve a wide range of problems including Non-deterministic Polynomial (NP) ones with polynomial resources (in time, space, and energy). An abstract DMM with this power must satisfy a set of compatible mathematical constraints underlying its practical realization. We prove this by making a connection with the dynamical systems theory. This leads us to a set of physical constraints for poly-resource resolvability. Once the mathematical requirements have been assessed, we propose a practical scheme to solve the above class of problems based on the novel concept of self-organizing logic gates and circuits (SOLCs). These are logic gates and circuits able to accept input signals from any terminal, without distinction between conventional input and output terminals. They can solve boolean problems by self-organizing into their solution. They can be fabricated either with circuit elements with memory (such as memristors) and/or standard MOS technology. Using tools of functional analysis, we prove mathematically the following constraints for the poly-resource resolvability: (i) SOLCs possess a global attractor; (ii) their only equilibrium points are the solutions of the problems to solve; (iii) the system converges exponentially fast to the solutions; (iv) the equilibrium convergence rate scales at most polynomially with input size. We finally provide arguments that periodic orbits and strange attractors cannot coexist with equilibria. As examples, we show how to solve the prime factorization and the search version of the NP-complete subset-sum problem. Since DMMs map integers into integers, they are robust against noise and hence scalable. We finally discuss the implications of the DMM realization through SOLCs to the NP = P question related to constraints of poly-resources resolvability.

Dynamical Detection of Topological Phase Transitions in Short-Lived Atomic Systems.

PubMed

Setiawan, F; Sengupta, K; Spielman, I B; Sau, Jay D

2015-11-06

We demonstrate that dynamical probes provide direct means of detecting the topological phase transition (TPT) between conventional and topological phases, which would otherwise be difficult to access because of loss or heating processes. We propose to avoid such heating by rapidly quenching in and out of the short-lived topological phase across the transition that supports gapless excitations. Following the quench, the distribution of excitations in the final conventional phase carries signatures of the TPT. We apply this strategy to study the TPT into a Majorana-carrying topological phase predicted in one-dimensional spin-orbit-coupled Fermi gases with attractive interactions. The resulting spin-resolved momentum distribution, computed by self-consistently solving the time-dependent Bogoliubov-de Gennes equations, exhibits Kibble-Zurek scaling and Stückelberg oscillations characteristic of the TPT. We discuss parameter regimes where the TPT is experimentally accessible.

Dynamical Detection of Topological Phase Transitions in Short-Lived Atomic Systems

NASA Astrophysics Data System (ADS)

Setiawan, F.; Sengupta, K.; Spielman, I. B.; Sau, Jay D.

2015-11-01

We demonstrate that dynamical probes provide direct means of detecting the topological phase transition (TPT) between conventional and topological phases, which would otherwise be difficult to access because of loss or heating processes. We propose to avoid such heating by rapidly quenching in and out of the short-lived topological phase across the transition that supports gapless excitations. Following the quench, the distribution of excitations in the final conventional phase carries signatures of the TPT. We apply this strategy to study the TPT into a Majorana-carrying topological phase predicted in one-dimensional spin-orbit-coupled Fermi gases with attractive interactions. The resulting spin-resolved momentum distribution, computed by self-consistently solving the time-dependent Bogoliubov-de Gennes equations, exhibits Kibble-Zurek scaling and Stückelberg oscillations characteristic of the TPT. We discuss parameter regimes where the TPT is experimentally accessible.

Recombination-enhanced surface expansion of clusters in intense soft x-ray laser pulses

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

Rupp, Daniela; Flückiger, Leonie; Adolph, Marcus

Here, we studied the nanoplasma formation and explosion dynamics of single large xenon clusters in ultrashort, intense x-ray free-electron laser pulses via ion spectroscopy. The simultaneous measurement of single-shot diffraction images enabled a single-cluster analysis that is free from any averaging over the cluster size and laser intensity distributions. The measured charge state-resolved ion energy spectra show narrow distributions with peak positions that scale linearly with final ion charge state. These two distinct signatures are attributed to highly efficient recombination that eventually leads to the dominant formation of neutral atoms in the cluster. The measured mean ion energies exceed themore » value expected without recombination by more than an order of magnitude, indicating that the energy release resulting from electron-ion recombination constitutes a previously unnoticed nanoplasma heating process. This conclusion is supported by results from semiclassical molecular dynamics simulations.« less

Recombination-enhanced surface expansion of clusters in intense soft x-ray laser pulses

DOE PAGES

Rupp, Daniela; Flückiger, Leonie; Adolph, Marcus; ...

2016-10-07

Here, we studied the nanoplasma formation and explosion dynamics of single large xenon clusters in ultrashort, intense x-ray free-electron laser pulses via ion spectroscopy. The simultaneous measurement of single-shot diffraction images enabled a single-cluster analysis that is free from any averaging over the cluster size and laser intensity distributions. The measured charge state-resolved ion energy spectra show narrow distributions with peak positions that scale linearly with final ion charge state. These two distinct signatures are attributed to highly efficient recombination that eventually leads to the dominant formation of neutral atoms in the cluster. The measured mean ion energies exceed themore » value expected without recombination by more than an order of magnitude, indicating that the energy release resulting from electron-ion recombination constitutes a previously unnoticed nanoplasma heating process. This conclusion is supported by results from semiclassical molecular dynamics simulations.« less

Nonequilibrium and nonperturbative dynamics of ultrastrong coupling in open lines.

PubMed

Peropadre, B; Zueco, D; Porras, D; García-Ripoll, J J

2013-12-13

The time and space resolved dynamics of a qubit with an Ohmic coupling to propagating 1D photons is studied, from weak coupling to the ultrastrong coupling regime. A nonperturbative study based on matrix product states shows the following results, (i) The ground state of the combined systems contains excitations of both the qubit and the surrounding bosonic field. (ii) An initially excited qubit equilibrates through spontaneous emission to a state, which under certain conditions is locally close to that ground state, both in the qubit and the field. (iii) The resonances of the combined qubit-photon system match those of the spontaneous emission process and also the predictions of the adiabatic renormalization [A. J. Leggett et al., Rev. Mod. Phys. 59, 1 (1987)]. Finally, nonperturbative ab initio calculations show that this physics can be studied using a flux qubit galvanically coupled to a superconducting transmission line.

Angle-resolved studies of inner shell excitations for argon, krypton and xenon using third-generation synchrotron sources

NASA Astrophysics Data System (ADS)

Farhat, Ahmad H.

This dissertation, which is in the area of atomic physics, concentrates on the study of the interaction between VUV-soft X-ray radiation and atoms in the gas phase. The main area of interest is the study of Auger decay in atoms utilizing the process known as the resonance Auger effect, where an inner shell electron is excited to an unfilled orbital followed by the ejection of an Auger electron. The measurements in this thesis were performed by using the high resolution Atomic, Molecular and Optical Physics undulator beam line, which utilizes a spherical grating monochromator at the Advanced Light Source at Lawrence Berkeley National Laboratory. The research focused on three rare gases, argon, krypton and xenon. For argon, high resolution angular-resolved measurements of the 2p → 4s, 3d, 4d resonant Auger lines have been achieved. By measuring photoelectron spectra simultaneously at two different angles using efficient time of flight spectrometers, the angular distributions anisotropy parameters β have been measured, and relative intensities have been evaluated for each of the resolved final ionic states. For krypton, the resonant Auger decay of all the photoexcited Kr 3d3/2,5/2-1 nl (n = 5-9) states have been studied using an angle resolved two dimensional photoelectron spectroscopic technique, in which the electron yield was measured as a function of both photon energy and electron kinetic energy. Angular distributions, spectator and shake probabilities have been derived for the Kr 3d-1np/to4s- 14p-1mp + e/sp- (n = 5-9, m = 5-11) resonance Auger decay. The results show that the spectator-core coupling is strong at lower n (n = 5,6) but it lessens for higher n, with a shake up of m = n + 1 preferred. Finally for xenon, the autoionization resonances and angular distribution of the 4d → 6p decay spectrum were studied utilizing the Auger resonant Raman effect. Using this technique, β parameters of almost all 5p4/ (3P,/ 1D,/ 1S) 6p final ionic states were determined. These results contribute to our understanding of atomic structure and dynamics of inner shell processes and hopefully will stimulate further experimental and theoretical work.

Energy partitioning in polyatomic chemical reactions: Quantum state resolved studies of highly exothermic atom abstraction reactions from molecules in the gas phase and at the gas-liquid interface

NASA Astrophysics Data System (ADS)

Zolot, Alexander M.

This thesis recounts a series of experiments that interrogate the dynamics of elementary chemical reactions using quantum state resolved measurements of gas-phase products. The gas-phase reactions F + HCl → HF + Cl and F + H2O → HF + OH are studied using crossed supersonic jets under single collision conditions. Infrared (IR) laser absorption probes HF product with near shot-noise limited sensitivity and high resolution, capable of resolving rovibrational states and Doppler lineshapes. Both reactions yield inverted vibrational populations. For the HCl reaction, strongly bimodal rotational distributions are observed, suggesting microscopic branching of the reaction mechanism. Alternatively, such structure may result from a quantum-resonance mediated reaction similar to those found in the well-characterized F + HD system. For the H2O reaction, a small, but significant, branching into v = 2 is particularly remarkable because this manifold is accessible only via the additional center of mass collision energy in the crossed jets. Rotationally hyperthermal HF is also observed. Ab initio calculations of the transition state geometry suggest mechanisms for both rotational and vibrational excitation. Exothermic chemical reaction dynamics at the gas-liquid interface have been investigated by colliding a supersonic jet of F atoms with liquid squalane (C30H62), a low vapor pressure hydrocarbon compatible with the high vacuum environment. IR spectroscopy provides absolute HF( v,J) product densities and Doppler resolved velocity component distributions perpendicular to the surface normal. Compared to analogous gas-phase F + hydrocarbon reactions, the liquid surface is a more effective "heat sink," yet vibrationally excited populations reveal incomplete thermal accommodation with the surface. Non-Boltzmann J-state populations and hot Doppler lineshapes that broaden with HF excitation indicate two competing scattering mechanisms: (i) a direct reactive scattering channel, whereby newly formed molecules leave the surface without equilibrating, and (ii) a partially accommodated fraction that shares vibrational, rotational, and translational energy with the liquid surface before returning to the gas phase. Finally, a velocity map ion imaging apparatus has been implemented to investigate reaction dynamics in crossed molecular beams. Resonantly enhanced multiphoton ionization (REMPI) results in rotational, vibrational, and electronic state selectivity. Velocity map imaging measurements provide differential cross sections and information about the internal energy distribution of the undetected collision partner.

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.

Time-resolved molecular imaging

NASA Astrophysics Data System (ADS)

Xu, Junliang; Blaga, Cosmin I.; Agostini, Pierre; DiMauro, Louis F.

2016-06-01

Time-resolved molecular imaging is a frontier of ultrafast optical science and physical chemistry. In this article, we review present and future key spectroscopic and microscopic techniques for ultrafast imaging of molecular dynamics and show their differences and connections. The advent of femtosecond lasers and free electron x-ray lasers bring us closer to this goal, which eventually will extend our knowledge about molecular dynamics to the attosecond time domain.

40 CFR 310.21 - How does EPA resolve disputes?

Code of Federal Regulations, 2011 CFR

2011-07-01

... 40 Protection of Environment 28 2011-07-01 2011-07-01 false How does EPA resolve disputes? 310.21... HAZARDOUS SUBSTANCE RELEASES Provisions How to Get Reimbursed § 310.21 How does EPA resolve disputes? (a) The EPA reimbursement official's decision is final EPA action unless you file a request for review by...

Structure and dynamics of water in nonionic reverse micelles: a combined time-resolved infrared and small angle x-ray scattering study.

PubMed

van der Loop, Tibert H; Panman, Matthijs R; Lotze, Stephan; Zhang, Jing; Vad, Thomas; Bakker, Huib J; Sager, Wiebke F C; Woutersen, Sander

2012-07-28

We study the structure and reorientation dynamics of nanometer-sized water droplets inside nonionic reverse micelles (water/Igepal-CO-520/cyclohexane) with time-resolved mid-infrared pump-probe spectroscopy and small angle x-ray scattering. In the time-resolved experiments, we probe the vibrational and orientational dynamics of the O-D bonds of dilute HDO:H(2)O mixtures in Igepal reverse micelles as a function of temperature and micelle size. We find that even small micelles contain a large fraction of water that reorients at the same rate as water in the bulk, which indicates that the polyethylene oxide chains of the surfactant do not penetrate into the water volume. We also observe that the confinement affects the reorientation dynamics of only the first hydration layer. From the temperature dependent surface-water dynamics, we estimate an activation enthalpy for reorientation of 45 ± 9 kJ mol(-1) (11 ± 2 kcal mol(-1)), which is close to the activation energy of the reorientation of water molecules in ice.

Performance of Smagorinsky and dynamic models in near surface turbulence

NASA Astrophysics Data System (ADS)

Brasseur, James G.; Juneja, Anurag

1997-11-01

In LES of high-Reynolds-number wall bounded turbulence such as the atmospheric boundary layer (ABL), a viscous sublayer either does not exist or is within the first grid cell, and some integral scale motions are necessarily under-resolved at the first few grid locations. Here the subgrid terms dominate the evolution of resolved velocity and the SGS model performance becomes crucial. To develop improved closures for surface layer turbulence (under-resolved and anisotropic), we explore (a) why current SGS closures fail and (b) what needs to be fixed. We evaluate the performance of the Smagorinsky and dynamic models using DNS data from shear- and buoyancy-driven turbulence as a function of filter cutoff location. We find that the underlying assumption of good alignment between the subgrid stress and resolved strain-rate tensors is not correct in general. More importantly, the Smagorinsky model incorrectly predicts a strong preference in the direction of the SGS stress divergence vector, a spurious prediction that is directly related to the anisotropic structure of the resolved turbulence field. This, and its under-estimation of the SGS pressure gradient, are likely sources of the errors observed in LES of the ABL. Whereas the dynamic formulations do a better job predicting some SGS dynamics, the model fails when the filter cutoff is near an integral scale, and predicts unreasonable fluctuation levels-- although performance is sensitive to type of averaging. *supported by ARO grant DAAL03-92-0117.

Propagation and deposition of non-circular finite release particle-laden currents

NASA Astrophysics Data System (ADS)

Zgheib, Nadim; Bonometti, Thomas; Balachandar, S.

2015-08-01

The dynamics of non-axisymmetric turbidity currents is considered here for a range of Reynolds numbers of O (104) when based on the initial height of the release. The study comprises a series of experiments and highly resolved simulations for which a finite volume of particle-laden solution is released into fresh water. A mixture of water and polystyrene particles of mean diameter d ˜ p = 300 μ m and mixture density ρ ˜ c = 1012 kg / m 3 is initially confined in a hollow cylinder at the centre of a large tank filled with fresh water. Cylinders with two different cross-sectional shapes, but equal cross-sectional areas, are examined: a circle and a rounded rectangle in which the sharp corners are smoothened. The time evolution of the front is recorded as well as the spatial distribution of the thickness of the final deposit via the use of a laser triangulation technique. The dynamics of the front and final deposits are significantly influenced by the initial geometry, displaying substantial azimuthal variation especially for the rectangular case where the current extends farther and deposits more particles along the initial minor axis of the rectangular cross section. Several parameters are varied to assess the dependence on the settling velocity, initial height aspect ratio, and volume fraction. Even though resuspension is not taken into account in our simulations, good agreement with experiments indicates that it does not play an important role in the front dynamics, in terms of velocity and extent of the current. However, wall shear stress measurements show that incipient motion of particles and particle transport along the bed are likely to occur in the body of the current and should be accounted to properly capture the final deposition profile of particles.

New Observations of the Crab Nebula and Pulsar

NASA Technical Reports Server (NTRS)

Weisskopf, Martin C.; Tennant, Allyn F.; ODell, Stephen L.; Elsner, Ronald f.; Yakovlev, Dmitry R.; Zavlin, Vyacheslav E.; Becker, Werner

2010-01-01

We present a phase-resolved study of the X-ray spectrum of the Crab Pulsar, using data obtained in a special mode with the Chandra X-ray Observatory. The superb angular resolution easily enables discerning the Pulsar from the surrounding nebulosity, even at pulse minimum. We find that the Pulsar's X-ray spectral index varies sinusoidally with phase---except over the same phase range for which rather abrupt changes in optical polarization magnitude and position angle have been reported. In addition, we use the X-ray data to constrain the surface temperature for various neutron-star equations of state and atmospheres. Finally, we present new data on dynamical variations of structure within the Nebula.

NICER Packaging for SpaceX CRS-11

NASA Image and Video Library

2017-04-06

Inside the Space Station Processing Facility high bay at NASA's Kennedy Space Center in Florida, technicians prepare the Neutron star Interior Composition Explorer, or NICER, payload for final packaging. NICER will be delivered to the International Space Station aboard the SpaceX Dragon cargo carrier on the company’s 11th commercial resupply services mission to the space station. NICER will study neutron stars through soft X-ray timing. NICER will enable rotation-resolved spectroscopy of the thermal and non-thermal emissions of neutron stars in the soft X-ray band with unprecedented sensitivity, probing interior structure, the origins of dynamic phenomena and the mechanisms that underlie the most powerful cosmic particle accelerators known.

NICER Packaging for SpaceX CRS-11

NASA Image and Video Library

2017-04-06

Inside the Space Station Processing Facility high bay at NASA's Kennedy Space Center in Florida, a technician prepares the Neutron star Interior Composition Explorer, or NICER, payload for final packaging. NICER will be delivered to the International Space Station aboard the SpaceX Dragon cargo carrier on the company’s 11th commercial resupply services mission to the space station. NICER will study neutron stars through soft X-ray timing. NICER will enable rotation-resolved spectroscopy of the thermal and non-thermal emissions of neutron stars in the soft X-ray band with unprecedented sensitivity, probing interior structure, the origins of dynamic phenomena and the mechanisms that underlie the most powerful cosmic particle accelerators known.

NICER Packaging for SpaceX CRS-11

NASA Image and Video Library

2017-04-06

Inside the Space Station Processing Facility high bay at NASA's Kennedy Space Center in Florida, the Neutron star Interior Composition Explorer, or NICER, payload is being prepared for final packaging. NICER will be delivered to the International Space Station aboard the SpaceX Dragon cargo carrier on the company’s 11th commercial resupply services mission to the space station. NICER will study neutron stars through soft X-ray timing. NICER will enable rotation-resolved spectroscopy of the thermal and non-thermal emissions of neutron stars in the soft X-ray band with unprecedented sensitivity, probing interior structure, the origins of dynamic phenomena and the mechanisms that underlie the most powerful cosmic particle accelerators known.

Phase diagram of the ultrafast photoinduced insulator-metal transition in vanadium dioxide

NASA Astrophysics Data System (ADS)

Cocker, T. L.; Titova, L. V.; Fourmaux, S.; Holloway, G.; Bandulet, H.-C.; Brassard, D.; Kieffer, J.-C.; El Khakani, M. A.; Hegmann, F. A.

2012-04-01

We use time-resolved terahertz spectroscopy to probe the ultrafast dynamics of the insulator-metal phase transition induced by femtosecond laser pulses in a nanogranular vanadium dioxide (VO2) film. Based on the observed thresholds for characteristic transient terahertz dynamics, a phase diagram of critical pump fluence versus temperature for the insulator-metal phase transition in VO2 is established for the first time over a broad range of temperatures down to 17 K. We find that both Mott and Peierls mechanisms are present in the insulating state and that the photoinduced transition is nonthermal. We propose a critical-threshold model for the ultrafast photoinduced transition based on a critical density of electrons and a critical density of coherently excited phonons necessary for the structural transition to the metallic state. As a result, evidence is found at low temperatures for an intermediate metallic state wherein the Mott state is melted but the Peierls distortion remains intact, consistent with recent theoretical predictions. Finally, the observed terahertz conductivity dynamics above the photoinduced transition threshold reveal nucleation and growth of metallic nanodomains over picosecond time scales.

Measuring the Nonuniform Evaporation Dynamics of Sprayed Sessile Microdroplets with Quantitative Phase Imaging.

PubMed

Edwards, Chris; Arbabi, Amir; Bhaduri, Basanta; Wang, Xiaozhen; Ganti, Raman; Yunker, Peter J; Yodh, Arjun G; Popescu, Gabriel; Goddard, Lynford L

2015-10-13

We demonstrate real-time quantitative phase imaging as a new optical approach for measuring the evaporation dynamics of sessile microdroplets. Quantitative phase images of various droplets were captured during evaporation. The images enabled us to generate time-resolved three-dimensional topographic profiles of droplet shape with nanometer accuracy and, without any assumptions about droplet geometry, to directly measure important physical parameters that characterize surface wetting processes. Specifically, the time-dependent variation of the droplet height, volume, contact radius, contact angle distribution along the droplet's perimeter, and mass flux density for two different surface preparations are reported. The studies clearly demonstrate three phases of evaporation reported previously: pinned, depinned, and drying modes; the studies also reveal instances of partial pinning. Finally, the apparatus is employed to investigate the cooperative evaporation of the sprayed droplets. We observe and explain the neighbor-induced reduction in evaporation rate, that is, as compared to predictions for isolated droplets. In the future, the new experimental methods should stimulate the exploration of colloidal particle dynamics on the gas-liquid-solid interface.

Many-body interferometry of magnetic polaron dynamics

NASA Astrophysics Data System (ADS)

Ashida, Yuto; Schmidt, Richard; Tarruell, Leticia; Demler, Eugene

2018-02-01

The physics of quantum impurities coupled to a many-body environment is among the most important paradigms of condensed-matter physics. In particular, the formation of polarons, quasiparticles dressed by the polarization cloud, is key to the understanding of transport, optical response, and induced interactions in a variety of materials. Despite recent remarkable developments in ultracold atoms and solid-state materials, the direct measurement of their ultimate building block, the polaron cloud, has remained a fundamental challenge. We propose and analyze a platform to probe time-resolved dynamics of polaron-cloud formation with an interferometric protocol. We consider an impurity atom immersed in a two-component Bose-Einstein condensate where the impurity generates spin-wave excitations that can be directly measured by the Ramsey interference of surrounding atoms. The dressing by spin waves leads to the formation of magnetic polarons and reveals a unique interplay between few- and many-body physics that is signified by single- and multi-frequency oscillatory dynamics corresponding to the formation of many-body bound states. Finally, we discuss concrete experimental implementations in ultracold atoms.

Implementing a Loosely Coupled Fluid Structure Interaction Finite Element Model in PHASTA

NASA Astrophysics Data System (ADS)

Pope, David

Fluid Structure Interaction problems are an important multi-physics phenomenon in the design of aerospace vehicles and other engineering applications. A variety of computational fluid dynamics solvers capable of resolving the fluid dynamics exist. PHASTA is one such computational fluid dynamics solver. Enhancing the capability of PHASTA to resolve Fluid-Structure Interaction first requires implementing a structural dynamics solver. The implementation also requires a correction of the mesh used to solve the fluid equations to account for the deformation of the structure. This results in mesh motion and causes the need for an Arbitrary Lagrangian-Eulerian modification to the fluid dynamics equations currently implemented in PHASTA. With the implementation of both structural dynamics physics, mesh correction, and the Arbitrary Lagrangian-Eulerian modification of the fluid dynamics equations, PHASTA is made capable of solving Fluid-Structure Interaction problems.

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

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

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

2016-04-21

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

Space-resolved diffusing wave spectroscopy measurements of the macroscopic deformation and the microscopic dynamics in tensile strain tests

NASA Astrophysics Data System (ADS)

Nagazi, Med-Yassine; Brambilla, Giovanni; Meunier, Gérard; Marguerès, Philippe; Périé, Jean-Noël; Cipelletti, Luca

2017-01-01

We couple a laser-based, space-resolved dynamic light scattering apparatus to a universal traction machine for mechanical extensional tests. We perform simultaneous optical and mechanical measurements on polyether ether ketone, a semi-crystalline polymer widely used in the industry. Due to the high turbidity of the sample, light is multiply scattered by the sample and the diffusing wave spectroscopy (DWS) formalism is used to interpret the data. Space-resolved DWS yields spatial maps of the sample strain and of the microscopic dynamics. An excellent agreement is found between the strain maps thus obtained and those measured by a conventional stereo-digital image correlation technique. The microscopic dynamics reveals both affine motion and plastic rearrangements. Thanks to the extreme sensitivity of DWS to displacements as small as 1 nm, plastic activity and its spatial localization can be detected at an early stage of the sample strain, making the technique presented here a valuable complement to existing material characterization methods.

Spatial variation in carrier dynamics along a single CdSSe nanowire

NASA Astrophysics Data System (ADS)

Blake, Jolie C.; Eldridge, Peter S.; Gundlach, Lars

2014-10-01

Ultrafast charge carrier dynamics along individual CdSxSe1-x nanowires has been measured. The use of an improved ultrafast Kerr-gated microscope allows for spatially resolved luminescence measurements along a single nanowire. Amplified spontaneous emission (ASE) was observed at high excitation fluences. Position dependent variations of ultrafast ASE dynamics were observed. SEM and colorimetric measurements showed that the difference in dynamics can be attributed to variations in non-radiative recombination rates along the wire. The dominant Shockley-Read recombination rate can be extracted from ASE dynamics and can be directly related to charge carrier mobility and defect density. Employing ASE as a probe for defect densities provides a new sub-micron spatially resolved, contactless method for measurements of charge carrier mobility.

Time-resolved double-slit interference pattern measurement with entangled photons

PubMed Central

Kolenderski, Piotr; Scarcella, Carmelo; Johnsen, Kelsey D.; Hamel, Deny R.; Holloway, Catherine; Shalm, Lynden K.; Tisa, Simone; Tosi, Alberto; Resch, Kevin J.; Jennewein, Thomas

2014-01-01

The double-slit experiment strikingly demonstrates the wave-particle duality of quantum objects. In this famous experiment, particles pass one-by-one through a pair of slits and are detected on a distant screen. A distinct wave-like pattern emerges after many discrete particle impacts as if each particle is passing through both slits and interfering with itself. Here we present a temporally- and spatially-resolved measurement of the double-slit interference pattern using single photons. We send single photons through a birefringent double-slit apparatus and use a linear array of single-photon detectors to observe the developing interference pattern. The analysis of the buildup allows us to compare quantum mechanics and the corpuscular model, which aims to explain the mystery of single-particle interference. Finally, we send one photon from an entangled pair through our double-slit setup and show the dependence of the resulting interference pattern on the twin photon's measured state. Our results provide new insight into the dynamics of the buildup process in the double-slit experiment, and can be used as a valuable resource in quantum information applications. PMID:24770360

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.

Kinematic equations for resolved-rate control of an industrial robot arm

NASA Technical Reports Server (NTRS)

Barker, L. K.

1983-01-01

An operator can use kinematic, resolved-rate equations to dynamically control a robot arm by watching its response to commanded inputs. Known resolved-rate equations for the control of a particular six-degree-of-freedom industrial robot arm and proceeds to simplify the equations for faster computations are derived. Methods for controlling the robot arm in regions which normally cause mathematical singularities in the resolved-rate equations are discussed.

A Dual-Line Detection Rayleigh Scattering Diagnostic Technique for the Combustion of Hydrocarbon Fuels and Filtered UV Rayleigh Scattering for Gas Velocity Measurements

NASA Technical Reports Server (NTRS)

Otugen, M. Volkan

1997-01-01

Non-intrusive techniques for the dynamic measurement of gas flow properties such as density, temperature and velocity, are needed in the research leading to the development of new generation high-speed aircraft. Accurate velocity, temperature and density data obtained in ground testing and in-flight measurements can help understand the flow physics leading to transition and turbulence in supersonic, high-altitude flight. Such non-intrusive measurement techniques can also be used to study combustion processes of hydrocarbon fuels in aircraft engines. Reliable, time and space resolved temperature measurements in various combustor configurations can lead to a better understanding of high temperature chemical reaction dynamics thus leading to improved modeling and better prediction of such flows. In view of this, a research program was initiated at Polytechnic University's Aerodynamics Laboratory with support from NASA Lewis Research Center through grants NAG3-1301 and NAG3-1690. The overall objective of this program has been to develop laser-based, non-contact, space- and time-resolved temperature and velocity measurement techniques. In the initial phase of the program a ND:YAG laser-based dual-line Rayleigh scattering technique was developed and tested for the accurate measurement of gas temperature in the presence of background laser glare. Effort was next directed towards the development of a filtered, spectrally-resolved Rayleigh/Mie scattering technique with the objective of developing an interferometric method for time-frozen velocity measurements in high-speed flows utilizing the uv line of an ND:YAG laser and an appropriate molecular absorption filter. This effort included both a search for an appropriate filter material for the 266 nm laser line and the development and testing of several image processing techniques for the fast processing of Fabry-Perot images for velocity and temperature information. Finally, work was also carried out for the development of a new laser-based strain-rate and vorticity technique for the time-resolved measurement of vorticity and strain-rates in turbulent flows.

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…

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.

Turbulent structures in cylindrical density currents in a rotating frame of reference

NASA Astrophysics Data System (ADS)

Salinas, Jorge S.; Cantero, Mariano I.; Dari, Enzo A.; Bonometti, Thomas

2018-06-01

Gravity currents are flows generated by the action of gravity on fluids with different densities. In some geophysical applications, modeling such flows makes it necessary to account for rotating effects, modifying the dynamics of the flow. While previous works on rotating stratified flows focused on currents of large Coriolis number, the present work focuses on flows with small Coriolis numbers (i.e. moderate-to-large Rossby numbers). In this work, cylindrical rotating gravity currents are investigated by means of highly resolved simulations. A brief analysis of the mean flow evolution to the final state is presented to provide a complete picture of the flow dynamics. The numerical results, showing the well-known oscillatory behavior of the flow (inertial waves) and a final state lens shape (geostrophic adjustment), are in good agreement with experimental observations and theoretical models. The turbulent structures in the flow are visualized and described using, among others, a stereoscopic visualization and videos as supplementary material. In particular, the structure of the lobes and clefts at the front of the current is presented in association to local turbulent structures. In rotating gravity currents, the vortices observed at the lobes front are not of hairpin type but are rather of Kelvin-Helmholtz type.

High Performance Nuclear Magnetic Resonance Imaging Using Magnetic Resonance Force Microscopy

DTIC Science & Technology

2013-12-12

Micron- Size Ferromagnet . Physical Review Letters, 92(3) 037205 (2004) [22] A. Z. Genack and A. G. Redeld. Theory of nuclear spin diusion in a...perform spatially resolved scanned probe studies of spin dynamics in nanoscale ensembles of few electron spins of varying size . Our research culminated...perform spatially resolved scanned probe studies of spin dynamics in nanoscale ensembles of few electron spins of varying size . Our research culminated

Time-resolved photoelectron spectroscopy of nitrobenzene and its aldehydes

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

In Situ Time-Resolved Measurements of Extension Twinning During Dynamic Compression of Polycrystalline Magnesium

NASA Astrophysics Data System (ADS)

Hustedt, C. J.; Lambert, P. K.; Kannan, V.; Huskins-Retzlaff, E. L.; Casem, D. T.; Tate, M. W.; Philipp, H. T.; Woll, A. R.; Purohit, P.; Weiss, J. T.; Gruner, S. M.; Ramesh, K. T.; Hufnagel, T. C.

2018-04-01

We report in situ time-resolved measurements of the dynamic evolution of the volume fraction of extension twins in polycrystalline pure magnesium and in the AZ31B magnesium alloy, using synchrotron x-ray diffraction during compressive loading at high strain rates. The dynamic evolution of the twinning volume fraction leads to a dynamic evolution of the texture. Although both the pure metal and the alloy had similar initial textures, we observe that the evolution of texture is slower in the alloy. We also measured the evolution of the lattice strains in each material during deformation which, together with the twin volume fractions, allows us to place some constraints on the relative contributions of dislocation-based slip and deformation twinning to the overall plastic deformation during the dynamic deformations.

A resolvable subfilter-scale model specific to large-eddy simulation of under-resolved turbulence

NASA Astrophysics Data System (ADS)

Zhou, Yong; Brasseur, James G.; Juneja, Anurag

2001-09-01

Large-eddy simulation (LES) of boundary-layer flows has serious deficiencies near the surface when a viscous sublayer either does not exist (rough walls) or is not practical to resolve (high Reynolds numbers). In previous work, we have shown that the near-surface errors arise from the poor performance of algebraic subfilter-scale (SFS) models at the first several grid levels, where integral scales are necessarily under-resolved and the turbulence is highly anisotropic. In under-resolved turbulence, eddy viscosity and similarity SFS models create a spurious feedback loop between predicted resolved-scale (RS) velocity and modeled SFS acceleration, and are unable to simultaneously capture SFS acceleration and RS-SFS energy flux. To break the spurious coupling in a dynamically meaningful manner, we introduce a new modeling strategy in which the grid-resolved subfilter velocity is estimated from a separate dynamical equation containing the essential inertial interactions between SFS and RS velocity. This resolved SFS (RSFS) velocity is then used as a surrogate for the complete SFS velocity in the SFS stress tensor. We test the RSFS model by comparing LES of highly under-resolved anisotropic buoyancy-generated homogeneous turbulence with a corresponding direct numerical simulation (DNS). The new model successfully suppresses the spurious feedback loop between RS velocity and SFS acceleration, and greatly improves model predictions of the anisotropic structure of SFS acceleration and resolved velocity fields. Unlike algebraic models, the RSFS model accurately captures SFS acceleration intensity and RS-SFS energy flux, even during the nonequilibrium transient, and properly partitions SFS acceleration between SFS stress divergence and SFS pressure force.

Data Assimilation for Applied Meteorology

NASA Astrophysics Data System (ADS)

Haupt, S. E.

2012-12-01

Although atmospheric models provide a best estimate of the future state of the atmosphere, due to sensitivity to initial condition, it is difficult to predict the precise future state. For applied problems, however, users often depend on having accurate knowledge of that future state. To improve prediction of a particular realization of an evolving flow field requires knowledge of the current state of that field and assimilation of local observations into the model. This talk will consider how dynamic assimilation can help address the concerns of users of atmospheric forecasts. First, we will look at the value of assimilation for the renewable energy industry. If the industry decision makers can have confidence in the wind and solar power forecasts, they can build their power allocations around the expected renewable resource, saving money for the ratepayers as well as reducing carbon emissions. We will assess the value to that industry of assimilating local real-time observations into the model forecasts and the value that is provided. The value of the forecasts with assimilation is important on both short (several hour) to medium range (within two days). A second application will be atmospheric transport and dispersion problems. In particular, we will look at assimilation of concentration data into a prediction model. An interesting aspect of this problem is that the dynamics are a one-way coupled system, with the fluid dynamic equations affecting the concentration equation, but not vice versa. So when the observations are of the concentration, one must infer the fluid dynamics. This one-way coupled system presents a challenge: one must first infer the changes in the flow field from observations of the contaminant, then assimilate that to recover both the advecting flow and information on the subgrid processes that provide the mixing. To accomplish such assimilation requires a robust method to match the observed contaminant field to that modeled. One approach is to separate the problem into a transport portion and a dispersion portion, representing the resolved flow and the unresolved portion. One then treats the resolved portion in a Lagrangian framework and the unresolved in an Eulerian framework to pose an optimization problem for both the transport and dispersion variables. We demonstrate how this problem can be solved by assimilating the data dynamically using a genetic algorithm variation approach (GA-Var). This technique is demonstrated on both a basic Gaussian puff problem and a Large Eddy Simulation. Finally we will show how assimilation can help bridge the gap between modeling flows at the mesoscale and flows at the fine scale that is often important for resolving flow around local features. By assimilating mesoscale model data into a computational fluid dynamics model, we can force the fine scale model to with the features at the mesoscale, providing a coupling mechanism.

Highly Resolved Studies of Vacuum Ultraviolet Photoionization Dynamics

NASA Astrophysics Data System (ADS)

Kakar, Sandeep

We use measurements of dispersed fluorescence from electronically excited photoions to study fundamental aspects of intramolecular dynamics. Our experimental innovations make it possible to obtain highly resolved photoionization data that offer qualitative insights into molecular scattering. In particular, we obtain vibrationally resolved data to probe coupling between the electronic and nuclear degrees of freedom by studying the distribution of vibrational energy among photoions. Vibrationally resolved branching ratios are measured over a broad spectral range of excitation energy and their non-Franck-Condon behavior is used as a tool to investigate two diverse aspects of shape resonant photoionization. First, vibrational branching ratios are obtained for the SiF_4 5a _1^{-1} and CS_2 5sigma_{rm u} ^{-1} photoionization channels to help elucidate the microscopic aspects of shape resonant wavefunction for polyatomic molecules. It is shown that in such molecules the shape resonant wavefunction is not necessarily attributable to a specific bond in the molecule. Second, the multichannel aspect of shape resonant photoionization dynamics, reflected in continuum channel coupling, is investigated by obtaining vibrational branching ratios for the 2 sigma_{rm u}^{ -1} and 4sigma^{ -1} photoionization of the isoelectronic molecules N_2 and CO, respectively. These data indicate that effects of continuum coupling may be widespread. We also present the first set of rotationally resolved data over a wide energy range for the 2 sigma_{rm u}^{ -1} photoionization of N_2. These data probe the partitioning of the angular momentum between the photoelectron and photoion, and highlight the multicenter nature of the molecular potential. These case studies illustrate the utility of dispersed fluorescence measurements as a complement to photoelectron spectroscopy for obtaining highly resolved data for molecular photoionization. These measurements makes it possible to probe intrinsically molecular aspects, such as the vibration and rotation, of photoionization dynamics over an extended spectral range when used in conjunction with synchrotron radiation as the exciting source. Furthermore, the high resolution made possible by this technique provides high selectivity for accessing weaker ionization channels which are the ones strongly affected by resonant activity, and the present study repeatedly stresses the importance of this capability in discovering and deciphering new trends in resonant molecular ionization dynamics.

Watching proteins function with 150-ps time-resolved X-ray crystallography

NASA Astrophysics Data System (ADS)

Anfinrud, Philip

2007-03-01

We have used time-resolved Laue crystallography to characterize ligand migration pathways and dynamics in wild-type and several mutant forms of myoglobin (Mb), a ligand-binding heme protein found in muscle tissue. In these pump-probe experiments, which were conducted on the ID09B time-resolved beamline at the European Synchrotron and Radiation Facility, a laser pulse photodissociates CO from an MbCO crystal and a suitably delayed X-ray pulse probes its structure via Laue diffraction. Single-site mutations in the vicinity of the heme pocket docking site were found to have a dramatic effect on ligand migration. To visualize this process, time-resolved electron density maps were stitched together into movies that unveil with <2-å spatial resolution and 150-ps time-resolution the correlated protein motions that accompany and/or mediate ligand migration. These studies help to illustrate at an atomic level relationships between protein structure, dynamics, and function.

Electrically-Generated Spin Polarization in Non-Magnetic Semiconductors

DTIC Science & Technology

2016-03-31

resolved Faraday rotation data due to electron spin polarization from previous pump pulses was characterized, and an analytic solution for this phase...electron spin polarization was shown to produce nuclear hyperpolarization through dynamic nuclear polarization. Time-resolved Faraday rotation...Distribution approved for public release. 3    Figure 3. Total magnetic field measured using time-resolved Faraday rotation with the electrically

Explicit Convection over the Western Pacific Warm Pool in the Community Atmospheric Model.

NASA Astrophysics Data System (ADS)

Ziemiaski, Micha Z.; Grabowski, Wojciech W.; Moncrieff, Mitchell W.

2005-05-01

This paper reports on the application of the cloud-resolving convection parameterization (CRCP) to the Community Atmospheric Model (CAM), the atmospheric component of the Community Climate System Model (CCSM). The cornerstone of CRCP is the use of a two-dimensional zonally oriented cloud-system-resolving model to represent processes on mesoscales at the subgrid scale of a climate model. Herein, CRCP is applied at each climate model column over the tropical western Pacific warm pool, in a domain spanning 10°S-10°N, 150°-170°E. Results from the CRCP simulation are compared with CAM in its standard configuration.The CRCP simulation shows significant improvements of the warm pool climate. The cloud condensate distribution is much improved as well as the bias of the tropopause height. More realistic structure of the intertropical convergence zone (ITCZ) during the boreal winter and better representation of the variability of convection are evident. In particular, the diurnal cycle of precipitation has phase and amplitude in good agreement with observations. Also improved is the large-scale organization of the tropical convection, especially superclusters associated with Madden-Julian oscillation (MJO)-like systems. Location and propagation characteristics, as well as lower-tropospheric cyclonic and upper-tropospheric anticyclonic gyres, are more realistic than in the standard CAM. Finally, the simulations support an analytic theory of dynamical coupling between organized convection and equatorial beta-plane vorticity dynamics associated with MJO-like systems.

A study of overflow simulations using MPAS-Ocean: Vertical grids, resolution, and viscosity

NASA Astrophysics Data System (ADS)

Reckinger, Shanon M.; Petersen, Mark R.; Reckinger, Scott J.

2015-12-01

MPAS-Ocean is used to simulate an idealized, density-driven overflow using the dynamics of overflow mixing and entrainment (DOME) setup. Numerical simulations are carried out using three of the vertical coordinate types available in MPAS-Ocean, including z-star with partial bottom cells, z-star with full cells, and sigma coordinates. The results are first benchmarked against other models, including the MITgcm's z-coordinate model and HIM's isopycnal coordinate model, which are used to set the base case used for this work. A full parameter study is presented that looks at how sensitive overflow simulations are to vertical grid type, resolution, and viscosity. Horizontal resolutions with 50 km grid cells are under-resolved and produce poor results, regardless of other parameter settings. Vertical grids ranging in thickness from 15 m to 120 m were tested. A horizontal resolution of 10 km and a vertical resolution of 60 m are sufficient to resolve the mesoscale dynamics of the DOME configuration, which mimics real-world overflow parameters. Mixing and final buoyancy are least sensitive to horizontal viscosity, but strongly sensitive to vertical viscosity. This suggests that vertical viscosity could be adjusted in overflow water formation regions to influence mixing and product water characteristics. Lastly, the study shows that sigma coordinates produce much less mixing than z-type coordinates, resulting in heavier plumes that go further down slope. Sigma coordinates are less sensitive to changes in resolution but as sensitive to vertical viscosity compared to z-coordinates.

Doppler imaging with dual-detection full-range frequency domain optical coherence tomography

PubMed Central

Meemon, Panomsak; Lee, Kye-Sung; Rolland, Jannick P.

2010-01-01

Most of full-range techniques for Frequency Domain Optical Coherence Tomography (FD-OCT) reported to date utilize the phase relation between consecutive axial lines to reconstruct a complex interference signal and hence may exhibit degradation in either mirror image suppression performance or detectable velocity dynamic range or both when monitoring a moving sample such as flow activity. We have previously reported a technique of mirror image removal by simultaneous detection of the quadrature components of a complex spectral interference called a Dual-Detection Frequency Domain OCT (DD-FD-OCT) [Opt. Lett. 35, 1058-1060 (2010)]. The technique enables full range imaging without any loss of acquisition speed and is intrinsically less sensitive to phase errors generated by involuntary movements of the subject. In this paper, we demonstrate the application of the DD-FD-OCT to a phase-resolved Doppler imaging without degradation in either mirror image suppression performance or detectable velocity dynamic range that were observed in other full-range Doppler methods. In order to accommodate for Doppler imaging, we have developed a fiber-based DD-FD-OCT that more efficiently utilizes the source power compared with the previous free-space DD-FD-OCT. In addition, the velocity sensitivity of the phase-resolved DD-FD-OCT was investigated, and the relation between the measured Doppler phase shift and set flow velocity of a flow phantom was verified. Finally, we demonstrate the Doppler imaging using the DD-FD-OCT in a biological sample. PMID:21258488

Spatially confined low-power optically pumped ultrafast synchrotron x-ray nanodiffraction

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

Park, Joonkyu; Zhang, Qingteng; Chen, Pice

2015-08-27

The combination of ultrafast optical excitation and time-resolved synchrotron x-ray nanodiffraction provides unique insight into the photoinduced dynamics of materials, with the spatial resolution required to probe individual nanostructures or small volumes within heterogeneous materials. Optically excited x-ray nanobeam experiments are challenging because the high total optical power required for experimentally relevant optical fluences leads to mechanical instability due to heating. For a given fluence, tightly focusing the optical excitation reduces the average optical power by more than three orders of magnitude and thus ensures sufficient thermal stability for x-ray nanobeam studies. Delivering optical pulses via a scannable fiber-coupled opticalmore » objective provides a well-defined excitation geometry during rotation and translation of the sample and allows the selective excitation of isolated areas within the sample. Finally, experimental studies of the photoinduced lattice dynamics of a 35 nm BiFeO 3 thin film on a SrTiO 3 substrate demonstrate the potential to excite and probe nanoscale volumes.« less

Ice-nucleating bacteria control the order and dynamics of interfacial water

DOE PAGES

Pandey, Ravindra; Usui, Kota; Livingstone, Ruth A.; ...

2016-04-22

Ice-nucleating organisms play important roles in the environment. With their ability to induce ice formation at temperatures just below the ice melting point, bacteria such as Pseudomonas syringae attack plants through frost damage using specialized ice-nucleating proteins. Besides the impact on agriculture and microbial ecology, airborne P. syringae can affect atmospheric glaciation processes, with consequences for cloud evolution, precipitation, and climate. Biogenic ice nucleation is also relevant for artificial snow production and for biomimetic materials for controlled interfacial freezing. We use interface-specific sum frequency generation (SFG) spectroscopy to show that hydrogen bonding at the water-bacteria contact imposes structural ordering onmore » the adjacent water network. Experimental SFG data and molecular dynamics simulations demonstrate that ice active sites within P. syringae feature unique hydrophilic-hydrophobic patterns to enhance ice nucleation. Finally, the freezing transition is further facilitated by the highly effective removal of latent heat from the nucleation site, as apparent from time-resolved SFG spectroscopy.« less

The impact of plasma dynamics on the self-magnetic-pinch diode impedance

DOE PAGES

Bennett, Nichelle; Crain, M. Dale; Droemer, Darryl W.; ...

2015-03-20

In this study, the self-magnetic-pinch diode is being developed as an intense electron beam source for pulsed-power-driven x-ray radiography. The basic operation of this diode has long been understood in the context of pinched diodes, including the dynamic effect that the diode impedance decreases during the pulse due to electrode plasma formation and expansion. Experiments being conducted at Sandia National Laboratories' RITS-6 accelerator are helping to characterize these plasmas using time-resolved and time-integrated camera systems in the x-ray and visible. These diagnostics are analyzed in conjunction with particle-in-cell simulations of anode plasma formation and evolution. The results confirm the long-standingmore » theory of critical-current operation with the addition of a time-dependent anode-cathode gap length. Finally, the results may suggest that anomalous impedance collapse is driven by increased plasma radial drift, leading to larger-than-average ion v r × B θ acceleration into the gap.« less

Fast blood flow monitoring in deep tissues with real-time software correlators

PubMed Central

Wang, Detian; Parthasarathy, Ashwin B.; Baker, Wesley B.; Gannon, Kimberly; Kavuri, Venki; Ko, Tiffany; Schenkel, Steven; Li, Zhe; Li, Zeren; Mullen, Michael T.; Detre, John A.; Yodh, Arjun G.

2016-01-01

We introduce, validate and demonstrate a new software correlator for high-speed measurement of blood flow in deep tissues based on diffuse correlation spectroscopy (DCS). The software correlator scheme employs standard PC-based data acquisition boards to measure temporal intensity autocorrelation functions continuously at 50 – 100 Hz, the fastest blood flow measurements reported with DCS to date. The data streams, obtained in vivo for typical source-detector separations of 2.5 cm, easily resolve pulsatile heart-beat fluctuations in blood flow which were previously considered to be noise. We employ the device to separate tissue blood flow from tissue absorption/scattering dynamics and thereby show that the origin of the pulsatile DCS signal is primarily flow, and we monitor cerebral autoregulation dynamics in healthy volunteers more accurately than with traditional instrumentation as a result of increased data acquisition rates. Finally, we characterize measurement signal-to-noise ratio and identify count rate and averaging parameters needed for optimal performance. PMID:27231588

Towards integrating extracellular matrix and immunological pathways.

PubMed

Boyd, David F; Thomas, Paul G

2017-10-01

The extracellular matrix (ECM) is a complex and dynamic structure made up of an estimated 300 different proteins. The ECM is also a rich source of cytokines and growth factors in addition to numerous bioactive ECM degradation products that influence cell migration, proliferation, and differentiation. The ECM is constantly being remodeled during homeostasis and in a wide range of pathological contexts. Changes in the ECM modulate immune responses, which in turn regulate repair and regeneration of tissues. Here, we review the many components of the ECM, enzymes involved in ECM remodeling, and the signals that feed into immunological pathways in the context of a dynamic ECM. We highlight studies that have taken an integrative approach to studying immune responses in the context of the ECM and studies that use novel proteomic strategies. Finally, we discuss research challenges relevant to the integration of immune and ECM networks and propose experimental and translational approaches to resolve these issues. Copyright © 2017 Elsevier Ltd. All rights reserved.

New approaches to the analysis of complex samples using fluorescence lifetime techniques and organized media

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

Hertz, P.R.

Fluorescence spectroscopy is a highly sensitive and selective tool for the analysis of complex systems. In order to investigate the efficacy of several steady state and dynamic techniques for the analysis of complex systems, this work focuses on two types of complex, multicomponent samples: petrolatums and coal liquids. It is shown in these studies dynamic, fluorescence lifetime-based measurements provide enhanced discrimination between complex petrolatum samples. Additionally, improved quantitative analysis of multicomponent systems is demonstrated via incorporation of organized media in coal liquid samples. This research provides the first systematic studies of (1) multifrequency phase-resolved fluorescence spectroscopy for dynamic fluorescence spectralmore » fingerprinting of complex samples, and (2) the incorporation of bile salt micellar media to improve accuracy and sensitivity for characterization of complex systems. In the petroleum studies, phase-resolved fluorescence spectroscopy is used to combine spectral and lifetime information through the measurement of phase-resolved fluorescence intensity. The intensity is collected as a function of excitation and emission wavelengths, angular modulation frequency, and detector phase angle. This multidimensional information enhances the ability to distinguish between complex samples with similar spectral characteristics. Examination of the eigenvalues and eigenvectors from factor analysis of phase-resolved and steady state excitation-emission matrices, using chemometric methods of data analysis, confirms that phase-resolved fluorescence techniques offer improved discrimination between complex samples as compared with conventional steady state methods.« less

Decoding the dynamics of cellular metabolism and the action of 3-bromopyruvate and 2-deoxyglucose using pulsed stable isotope-resolved metabolomics.

PubMed

Pietzke, Matthias; Zasada, Christin; Mudrich, Susann; Kempa, Stefan

2014-01-01

Cellular metabolism is highly dynamic and continuously adjusts to the physiological program of the cell. The regulation of metabolism appears at all biological levels: (post-) transcriptional, (post-) translational, and allosteric. This regulatory information is expressed in the metabolome, but in a complex manner. To decode such complex information, new methods are needed in order to facilitate dynamic metabolic characterization at high resolution. Here, we describe pulsed stable isotope-resolved metabolomics (pSIRM) as a tool for the dynamic metabolic characterization of cellular metabolism. We have adapted gas chromatography-coupled mass spectrometric methods for metabolomic profiling and stable isotope-resolved metabolomics. In addition, we have improved robustness and reproducibility and implemented a strategy for the absolute quantification of metabolites. By way of examples, we have applied this methodology to characterize central carbon metabolism of a panel of cancer cell lines and to determine the mode of metabolic inhibition of glycolytic inhibitors in times ranging from minutes to hours. Using pSIRM, we observed that 2-deoxyglucose is a metabolic inhibitor, but does not directly act on the glycolytic cascade.

Forecasting the absolute and relative shortage of physicians in Japan using a system dynamics model approach

PubMed Central

2013-01-01

Background In Japan, a shortage of physicians, who serve a key role in healthcare provision, has been pointed out as a major medical issue. The healthcare workforce policy planner should consider future dynamic changes in physician numbers. The purpose of this study was to propose a physician supply forecasting methodology by applying system dynamics modeling to estimate future absolute and relative numbers of physicians. Method We constructed a forecasting model using a system dynamics approach. Forecasting the number of physician was performed for all clinical physician and OB/GYN specialists. Moreover, we conducted evaluation of sufficiency for the number of physicians and sensitivity analysis. Result & conclusion As a result, it was forecast that the number of physicians would increase during 2008–2030 and the shortage would resolve at 2026 for all clinical physicians. However, the shortage would not resolve for the period covered. This suggests a need for measures for reconsidering the allocation system of new entry physicians to resolve maldistribution between medical departments, in addition, for increasing the overall number of clinical physicians. PMID:23981198

Forecasting the absolute and relative shortage of physicians in Japan using a system dynamics model approach.

PubMed

Ishikawa, Tomoki; Ohba, Hisateru; Yokooka, Yuki; Nakamura, Kozo; Ogasawara, Katsuhiko

2013-08-27

In Japan, a shortage of physicians, who serve a key role in healthcare provision, has been pointed out as a major medical issue. The healthcare workforce policy planner should consider future dynamic changes in physician numbers. The purpose of this study was to propose a physician supply forecasting methodology by applying system dynamics modeling to estimate future absolute and relative numbers of physicians. We constructed a forecasting model using a system dynamics approach. Forecasting the number of physician was performed for all clinical physician and OB/GYN specialists. Moreover, we conducted evaluation of sufficiency for the number of physicians and sensitivity analysis. As a result, it was forecast that the number of physicians would increase during 2008-2030 and the shortage would resolve at 2026 for all clinical physicians. However, the shortage would not resolve for the period covered. This suggests a need for measures for reconsidering the allocation system of new entry physicians to resolve maldistribution between medical departments, in addition, for increasing the overall number of clinical physicians.

Calculations of predissociative lifetimes of RG...Hal2 Van der Waals complexes

NASA Astrophysics Data System (ADS)

Buchachenko, Alexei A.; Stepanov, N. F.

1992-07-01

Good examples of combined energy- and time-resolved techniques linked by the theoretical solution of a nuclear problem may be found in investigations of the dynamics of weakly bound Van der Waals (VdW) complexes, such as Ar-OH and He-stilbene. Our report concerns only the theoretical aspect of this complex approach. However, we shall stress the importance of energy-resolved spectroscopy for the dynamics and try to illustrate this with some numerical results.

Geosynchronous Microwave Atmospheric Sounding Radiometer (MASR) feasibility studies. Volume 1: Management summary

NASA Technical Reports Server (NTRS)

1978-01-01

The mission of the microwave atmospheric sounding radiometer (MASR) is to collect data to aid in the observation and prediction of severe storms. The geosynchronous orbit allows the continuous atmospheric measurement needed to resolve mesoscale dynamics. The instrument may operate in conjunction with this document, Volume 1 - Management, which summarizes the highlights of final reports on both the radiometer instrument and antenna studies. The radiometer instrument summary includes a synopsis of Volume 2 - Radiometer Receiver Feasibility, including design, recommended configuration, performance estimates, and weight and power estimates. The summary of the antenna study includes a synopsis of Volume 3 - Antenna Feasibility, including preliminary design tradeoffs, performance of selected design, and details of the mechanical/thermal design.

Dynamical Evolution of Planetary Embryos

NASA Technical Reports Server (NTRS)

Wetherill, George W.

2002-01-01

During the past decade, progress has been made by relating the 'standard model' for the formation of planetary systems to computational and observational advances. A significant contribution to this has been provided by this grant. The consequence of this is that the rigor of the physical modeling has improved considerably. This has identified discrepancies between the predictions of the standard model and recent observations of extrasolar planets. In some cases, the discrepancies can be resolved by recognition of the stochastic nature of the planetary formation process, leading to variations in the final state of a planetary system. In other cases, it seems more likely that there are major deficiencies in the standard model, requiring our identifying variations to the model that are not so strongly constrained to our Solar System.

High-harmonic spectroscopy of ultrafast many-body dynamics in strongly correlated systems

NASA Astrophysics Data System (ADS)

Silva, R. E. F.; Blinov, Igor V.; Rubtsov, Alexey N.; Smirnova, O.; Ivanov, M.

2018-05-01

We bring together two topics that, until now, have been the focus of intense but non-overlapping research efforts. The first concerns high-harmonic generation in solids, which occurs when an intense light field excites a highly non-equilibrium electronic response in a semiconductor or a dielectric. The second concerns many-body dynamics in strongly correlated systems such as the Mott insulator. We show that high-harmonic generation can be used to time-resolve ultrafast many-body dynamics associated with an optically driven phase transition, with accuracy far exceeding one cycle of the driving light field. Our work paves the way for time-resolving highly non-equilibrium many-body dynamics in strongly correlated systems, with few femtosecond accuracy.

Time-Resolved IR-Absorption Spectroscopy of Hot-Electron Dynamics in Satellite and Upper Conduction Bands in GaP

NASA Technical Reports Server (NTRS)

Cavicchia, M. A.; Alfano, R. R.

1995-01-01

The relaxation dynamics of hot electrons in the X6 and X7 satellite and upper conduction bands in GaP was directly measured by femtosecond UV-pump-IR-probe absorption spectroscopy. From a fit to the induced IR-absorption spectra the dominant scattering mechanism giving rise to the absorption at early delay times was determined to be intervalley scattering of electrons out of the X7 upper conduction-band valley. For long delay times the dominant scattering mechanism is electron-hole scattering. Electron transport dynamics of the upper conduction band of GaP has been time resolved.

Resealable, optically accessible, PDMS-free fluidic platform for ex vivo interrogation of pancreatic islets.

PubMed

Lenguito, Giovanni; Chaimov, Deborah; Weitz, Jonathan R; Rodriguez-Diaz, Rayner; Rawal, Siddarth A K; Tamayo-Garcia, Alejandro; Caicedo, Alejandro; Stabler, Cherie L; Buchwald, Peter; Agarwal, Ashutosh

2017-02-28

We report the design and fabrication of a robust fluidic platform built out of inert plastic materials and micromachined features that promote optimized convective fluid transport. The platform is tested for perfusion interrogation of rodent and human pancreatic islets, dynamic secretion of hormones, concomitant live-cell imaging, and optogenetic stimulation of genetically engineered islets. A coupled quantitative fluid dynamics computational model of glucose stimulated insulin secretion and fluid dynamics was first utilized to design device geometries that are optimal for complete perfusion of three-dimensional islets, effective collection of secreted insulin, and minimization of system volumes and associated delays. Fluidic devices were then fabricated through rapid prototyping techniques, such as micromilling and laser engraving, as two interlocking parts from materials that are non-absorbent and inert. Finally, the assembly was tested for performance using both rodent and human islets with multiple assays conducted in parallel, such as dynamic perfusion, staining and optogenetics on standard microscopes, as well as for integration with commercial perfusion machines. The optimized design of convective fluid flows, use of bio-inert and non-absorbent materials, reversible assembly, manual access for loading and unloading of islets, and straightforward integration with commercial imaging and fluid handling systems proved to be critical for perfusion assay, and particularly suited for time-resolved optogenetics studies.

Nonequilibrium lattice-driven dynamics of stripes in nickelates using time-resolved x-ray scattering

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

Lee, W. S.; Kung, Y. F.; Moritz, B.

We investigate the lattice coupling to the spin and charge orders in the striped nickelate, La 1.75 Sr 0.25 NiO 4 , using time-resolved resonant x-ray scattering. Lattice-driven dynamics of both spin and charge orders are observed when the pump photon energy is tuned to that of an E u bond- stretching phonon. We present a likely scenario for the behavior of the spin and charge order parameters and its implications using a Ginzburg-Landau theory.

Molecular frame photoemission by a comb of elliptical high-order harmonics: a sensitive probe of both photodynamics and harmonic complete polarization state.

PubMed

Veyrinas, K; Gruson, V; Weber, S J; Barreau, L; Ruchon, T; Hergott, J-F; Houver, J-C; Lucchese, R R; Salières, P; Dowek, D

2016-12-16

Due to the intimate anisotropic interaction between an XUV light field and a molecule resulting in photoionization (PI), molecular frame photoelectron angular distributions (MFPADs) are most sensitive probes of both electronic/nuclear dynamics and the polarization state of the ionizing light field. Consequently, they encode the complex dipole matrix elements describing the dynamics of the PI transition, as well as the three normalized Stokes parameters s 1 , s 2 , s 3 characterizing the complete polarization state of the light, operating as molecular polarimetry. The remarkable development of advanced light sources delivering attosecond XUV pulses opens the perspective to visualize the primary steps of photochemical dynamics in time-resolved studies, at the natural attosecond to few femtosecond time-scales of electron dynamics and fast nuclear motion. It is thus timely to investigate the feasibility of measurement of MFPADs when PI is induced e.g., by an attosecond pulse train (APT) corresponding to a comb of discrete high-order harmonics. In the work presented here, we report MFPAD studies based on coincident electron-ion 3D momentum imaging in the context of ultrafast molecular dynamics investigated at the PLFA facility (CEA-SLIC), with two perspectives: (i) using APTs generated in atoms/molecules as a source for MFPAD-resolved PI studies, and (ii) taking advantage of molecular polarimetry to perform a complete polarization analysis of the harmonic emission of molecules, a major challenge of high harmonic spectroscopy. Recent results illustrating both aspects are reported for APTs generated in unaligned SF 6 molecules by an elliptically polarized infrared driving field. The observed fingerprints of the elliptically polarized harmonics include the first direct determination of the complete s 1 , s 2 , s 3 Stokes vector, equivalent to (ψ, ε, P), the orientation and the signed ellipticity of the polarization ellipse, and the degree of polarization P. They are compared to so far incomplete results of XUV optical polarimetry. We finally discuss the comparison between the outcomes of photoionization and high harmonic spectroscopy for the description of molecular photodynamics.

Banding of NMR-derived Methyl Order Parameters: Implications for Protein Dynamics

PubMed Central

Sharp, Kim A.; Kasinath, Vignesh; Wand, A. Joshua

2014-01-01

Our understanding of protein folding, stability and function has begun to more explicitly incorporate dynamical aspects. Nuclear magnetic resonance has emerged as a powerful experimental method for obtaining comprehensive site-resolved insight into protein motion. It has been observed that methyl-group motion tends to cluster into three “classes” when expressed in terms of the popular Lipari-Szabo model-free squared generalized order parameter. Here the origins of the three classes or bands in the distribution of order parameters are examined. As a first step, a Bayesian based approach, which makes no a priori assumption about the existence or number of bands, is developed to detect the banding of O2axis values derived either from NMR experiments or molecular dynamics simulations. The analysis is applied to seven proteins with extensive molecular dynamics simulations of these proteins in explicit water to examine the relationship between O2 and fine details of the motion of methyl bearing side chains. All of the proteins studied display banding, with some subtle differences. We propose a very simple yet plausible physical mechanism for banding. Finally, our Bayesian method is used to analyze the measured distributions of methyl group motions in the catabolite activating protein and several of its mutants in various liganded states and discuss the functional implications of the observed banding to protein dynamics and function. PMID:24677353

Aeroservoelastic Modeling of Body Freedom Flutter for Control System Design

NASA Technical Reports Server (NTRS)

Ouellette, Jeffrey

2017-01-01

One of the most severe forms of coupling between aeroelasticity and flight dynamics is an instability called freedom flutter. The existing tools often assume relatively weak coupling, and are therefore unable to accurately model body freedom flutter. Because the existing tools were developed from traditional flutter analysis models, inconsistencies in the final models are not compatible with control system design tools. To resolve these issues, a number of small, but significant changes have been made to the existing approaches. A frequency domain transformation is used with the unsteady aerodynamics to ensure a more physically consistent stability axis rational function approximation of the unsteady aerodynamic model. The aerodynamic model is augmented with additional terms to account for limitations of the baseline unsteady aerodynamic model and to account for the gravity forces. An assumed modes method is used for the structural model to ensure a consistent definition of the aircraft states across the flight envelope. The X-56A stiff wing flight-test data were used to validate the current modeling approach. The flight-test data does not show body-freedom flutter, but does show coupling between the flight dynamics and the aeroelastic dynamics and the effects of the fuel weight.

Substituent effects on the relaxation dynamics of furan, furfural and β-furfural: a combined theoretical and experimental approach.

PubMed

Oesterling, Sven; Schalk, Oliver; Geng, Ting; Thomas, Richard D; Hansson, Tony; de Vivie-Riedle, Regina

2017-01-18

For the series furan, furfural and β-furfural we investigated the effect of substituents and their positioning on the photoinduced relaxation dynamics in a combined theoretical and experimental approach. Using time resolved photoelectron spectroscopy with a high intensity probe pulse, we can, for the first time, follow the whole deactivation process of furan through a two photon probe signal. Using the extended 2-electron 2-orbital model [Nenov et al., J. Chem. Phys., 2011, 135, 034304] we explain the formation of one central conical intersection and predict the influence of the aldehyde group of the derivatives on its geometry. This, as well as the relaxation mechanisms from photoexcitation to the final outcome was investigated using a variety of theoretical methods. Complete active space self consistent field was used for on-the-fly calculations while complete active space perturbation theory and coupled cluster theory were used to accurately describe critical configurations. Experiment and theory show the relaxation dynamics of furfural and β-furfural to be slowed down, and together they disclose an additional deactivation pathway, which is attributed to the n O lonepair state introduced with the aldehyde group.

Dynamics of temporal variations in phonatory flow.

PubMed

Krane, Michael H; Barry, Michael; Wei, Timothy

2010-07-01

This paper addresses the dynamic relevance of time variations of phonatory airflow, commonly neglected under the quasisteady phonatory flow assumption. In contrast to previous efforts, which relied on direct measurement of glottal impedance, this work uses spatially and temporally resolved measurements of the velocity field to estimate the unsteady and convective acceleration terms in the unsteady Bernoulli equation. Theoretical considerations suggest that phonatory flow is inherently unsteady when two related conditions apply: (1) that the unsteady and convective accelerations are commensurate, and (2) that the inertia of the glottal jet is non-negligible. Acceleration waveforms, computed from experimental data, show that unsteady and convective accelerations to be the same order of magnitude, throughout the cycle, and that the jet flow contributes significantly to the unsteady acceleration. In the middle of the cycle, however, jet inertia is negligible because the convective and unsteady accelerations nearly offset one another in the jet region. These results, consistent with previous findings treating quasisteady phonatory flow, emphasize that unsteady acceleration cannot be neglected during the final stages of the phonation cycle, during which voice sound power and spectral content are largely determined. Furthermore, glottal jet dynamics must be included in any model of phonatory airflow.

Dynamics of temporal variations in phonatory flow1

PubMed Central

Krane, Michael H.; Barry, Michael; Wei, Timothy

2010-01-01

This paper addresses the dynamic relevance of time variations of phonatory airflow, commonly neglected under the quasisteady phonatory flow assumption. In contrast to previous efforts, which relied on direct measurement of glottal impedance, this work uses spatially and temporally resolved measurements of the velocity field to estimate the unsteady and convective acceleration terms in the unsteady Bernoulli equation. Theoretical considerations suggest that phonatory flow is inherently unsteady when two related conditions apply: (1) that the unsteady and convective accelerations are commensurate, and (2) that the inertia of the glottal jet is non-negligible. Acceleration waveforms, computed from experimental data, show that unsteady and convective accelerations to be the same order of magnitude, throughout the cycle, and that the jet flow contributes significantly to the unsteady acceleration. In the middle of the cycle, however, jet inertia is negligible because the convective and unsteady accelerations nearly offset one another in the jet region. These results, consistent with previous findings treating quasisteady phonatory flow, emphasize that unsteady acceleration cannot be neglected during the final stages of the phonation cycle, during which voice sound power and spectral content are largely determined. Furthermore, glottal jet dynamics must be included in any model of phonatory airflow. PMID:20649231

Dynamics of a Cr spin in a semiconductor quantum dot: Hole-Cr flip-flops and spin-phonon coupling

NASA Astrophysics Data System (ADS)

Lafuente-Sampietro, A.; Utsumi, H.; Sunaga, M.; Makita, K.; Boukari, H.; Kuroda, S.; Besombes, L.

2018-04-01

A detailed analysis of the photoluminescence (PL) intensity distribution in singly Cr-doped CdTe/ZnTe quantum dots (QDs) is performed. First of all, we demonstrate that hole-Cr flip-flops induced by an interplay of the hole-Cr exchange interaction and the coupling with acoustic phonons are the main source of spin relaxation within the exciton-Cr complex. This spin flip mechanism appears in the excitation power dependence of the PL of the exciton as well as in the intensity distribution of the resonant PL. The resonant optical pumping of the Cr spin which was recently demonstrated can also be explained by these hole-Cr flip-flops. Despite the fast exciton-Cr spin dynamics, an analysis of the PL intensity under magnetic field shows that the hole-Cr exchange interaction in CdTe/ZnTe QDs is antiferromagnetic. In addition to the Cr spin dynamics induced by the interaction with carriers' spin, we finally demonstrate using time resolved optical pumping measurements that a Cr spin interacts with nonequilibrium acoustic phonons generated during the optical excitation inside or near the QD.

Coordinating cell and tissue behavior during zebrafish neural tube morphogenesis.

PubMed

Araya, Claudio; Ward, Laura C; Girdler, Gemma C; Miranda, Miguel

2016-03-01

The development of a vertebrate neural epithelium with well-organized apico-basal polarity and a central lumen is essential for its proper function. However, how this polarity is established during embryonic development and the potential influence of surrounding signals and tissues on such organization has remained less understood. In recent years the combined superior transparency and genetics of the zebrafish embryo has allowed for in vivo visualization and quantification of the cellular and molecular dynamics that govern neural tube structure. Here, we discuss recent studies revealing how co-ordinated cell-cell interactions coupled with adjacent tissue dynamics are critical to regulate final neural tissue architecture. Furthermore, new findings show how the spatial regulation and timing of orientated cell division is key in defining precise lumen formation at the tissue midline. In addition, we compare zebrafish neurulation with that of amniotes and amphibians in an attempt to understand the conserved cellular mechanisms driving neurulation and resolve the apparent differences among animals. Zebrafish neurulation not only offers fundamental insights into early vertebrate brain development but also the opportunity to explore in vivo cell and tissue dynamics during complex three-dimensional animal morphogenesis. © 2015 Wiley Periodicals, Inc.

Photoemission and photoionization time delays and rates

PubMed Central

Gallmann, L.; Jordan, I.; Wörner, H. J.; Castiglioni, L.; Hengsberger, M.; Osterwalder, J.; Arrell, C. A.; Chergui, M.; Liberatore, E.; Rothlisberger, U.; Keller, U.

2017-01-01

Ionization and, in particular, ionization through the interaction with light play an important role in fundamental processes in physics, chemistry, and biology. In recent years, we have seen tremendous advances in our ability to measure the dynamics of photo-induced ionization in various systems in the gas, liquid, or solid phase. In this review, we will define the parameters used for quantifying these dynamics. We give a brief overview of some of the most important ionization processes and how to resolve the associated time delays and rates. With regard to time delays, we ask the question: how long does it take to remove an electron from an atom, molecule, or solid? With regard to rates, we ask the question: how many electrons are emitted in a given unit of time? We present state-of-the-art results on ionization and photoemission time delays and rates. Our review starts with the simplest physical systems: the attosecond dynamics of single-photon and tunnel ionization of atoms in the gas phase. We then extend the discussion to molecular gases and ionization of liquid targets. Finally, we present the measurements of ionization delays in femto- and attosecond photoemission from the solid–vacuum interface. PMID:29308414

Dynamic Appliances Scheduling in Collaborative MicroGrids System

PubMed Central

Bilil, Hasnae; Aniba, Ghassane; Gharavi, Hamid

2017-01-01

In this paper a new approach which is based on a collaborative system of MicroGrids (MG’s), is proposed to enable household appliance scheduling. To achieve this, appliances are categorized into flexible and non-flexible Deferrable Loads (DL’s), according to their electrical components. We propose a dynamic scheduling algorithm where users can systematically manage the operation of their electric appliances. The main challenge is to develop a flattening function calculus (reshaping) for both flexible and non-flexible DL’s. In addition, implementation of the proposed algorithm would require dynamically analyzing two successive multi-objective optimization (MOO) problems. The first targets the activation schedule of non-flexible DL’s and the second deals with the power profiles of flexible DL’s. The MOO problems are resolved by using a fast and elitist multi-objective genetic algorithm (NSGA-II). Finally, in order to show the efficiency of the proposed approach, a case study of a collaborative system that consists of 40 MG’s registered in the load curve for the flattening program has been developed. The results verify that the load curve can indeed become very flat by applying the proposed scheduling approach. PMID:28824226

Trp zipper folding kinetics by molecular dynamics and temperature-jump spectroscopy

PubMed Central

Snow, Christopher D.; Qiu, Linlin; Du, Deguo; Gai, Feng; Hagen, Stephen J.; Pande, Vijay S.

2004-01-01

We studied the microsecond folding dynamics of three β hairpins (Trp zippers 1–3, TZ1–TZ3) by using temperature-jump fluorescence and atomistic molecular dynamics in implicit solvent. In addition, we studied TZ2 by using time-resolved IR spectroscopy. By using distributed computing, we obtained an aggregate simulation time of 22 ms. The simulations included 150, 212, and 48 folding events at room temperature for TZ1, TZ2, and TZ3, respectively. The all-atom optimized potentials for liquid simulations (OPLSaa) potential set predicted TZ1 and TZ2 properties well; the estimated folding rates agreed with the experimentally determined folding rates and native conformations were the global potential-energy minimum. The simulations also predicted reasonable unfolding activation enthalpies. This work, directly comparing large simulated folding ensembles with multiple spectroscopic probes, revealed both the surprising predictive ability of current models as well as their shortcomings. Specifically, for TZ1–TZ3, OPLS for united atom models had a nonnative free-energy minimum, and the folding rate for OPLSaa TZ3 was sensitive to the initial conformation. Finally, we characterized the transition state; all TZs fold by means of similar, native-like transition-state conformations. PMID:15020773

Trp zipper folding kinetics by molecular dynamics and temperature-jump spectroscopy

NASA Astrophysics Data System (ADS)

Snow, Christopher D.; Qiu, Linlin; Du, Deguo; Gai, Feng; Hagen, Stephen J.; Pande, Vijay S.

2004-03-01

We studied the microsecond folding dynamics of three hairpins (Trp zippers 1-3, TZ1-TZ3) by using temperature-jump fluorescence and atomistic molecular dynamics in implicit solvent. In addition, we studied TZ2 by using time-resolved IR spectroscopy. By using distributed computing, we obtained an aggregate simulation time of 22 ms. The simulations included 150, 212, and 48 folding events at room temperature for TZ1, TZ2, and TZ3, respectively. The all-atom optimized potentials for liquid simulations (OPLSaa) potential set predicted TZ1 and TZ2 properties well; the estimated folding rates agreed with the experimentally determined folding rates and native conformations were the global potential-energy minimum. The simulations also predicted reasonable unfolding activation enthalpies. This work, directly comparing large simulated folding ensembles with multiple spectroscopic probes, revealed both the surprising predictive ability of current models as well as their shortcomings. Specifically, for TZ1-TZ3, OPLS for united atom models had a nonnative free-energy minimum, and the folding rate for OPLSaa TZ3 was sensitive to the initial conformation. Finally, we characterized the transition state; all TZs fold by means of similar, native-like transition-state conformations.

Developing Structure-Property Relationships in Branched Wormlike Micelles via Advanced Rheological and Neutron Scattering Techniques

NASA Astrophysics Data System (ADS)

Calabrese, Michelle A.

Surfactant wormlike micelles (WLMs) are of particular scientific interest due to their ability to branch, break, and reform under shear, which can lead to shear banding flow instabilities. The tunable self-assembly of WLMs makes them ubiquitous in applications ranging from consumer products to energy recovery fluids. Altering the topology of WLMs by inducing branching provides a microstructural pathway to design and optimize the flow properties for such targeted applications. The goal of this thesis is to understand the role of micellar branching on the resulting equilibrium and non-equilibrium properties, while advancing instrumentation and analysis methods in rheology and neutron scattering. The degree of branching in the mixed cationic/anionic surfactant solutions is controlled by the addition of sodium tosylate. The equilibrium properties are characterized via small angle neutron scattering (SANS), linear viscoelastic rheology, neutron spin echo, and dynamic light scattering. Combining rheology with spatiotemporally-resolved SANS enables unambiguous identification of non-equilibrium rheological and scattering signatures of branching and shear banding. The nonlinear WLM response is characterized via flow-SANS under steady shear, shear startup, and large amplitude oscillatory shear. New methods of time-resolved data analysis are developed, which improve experimental resolution by several-fold. Shear-induced orientation is a complex function of branching level, radial position, and deformation type. The structural mechanisms behind shear band formation are elucidated for steady and dynamic flows, which depend on branching level. Shear banding disappears at high branching levels for all deformation types. These responses are used to validate constitutive modeling predictions of dynamic shear banding for the first time. Finally, quantitative metrics to predict shear banding from rheology or flow-induced orientation are developed. Together, advanced rheological and neutron techniques provide a platform for creating structure-property relationships that predict flow and structural phenomena in WLMs and other soft materials. These methods have enabled characteristic differences in linear versus branched WLMs to be determined. This research is part of a broader effort to characterize branching in polymers and self-assembled systems, and may aid in the formulation of WLMs for specific applications. Finally, this work provides a basis for testing and developing microstructure-based constitutive equations that incorporate micellar breakage and branching.

A Superintendent's Final Announcement!

ERIC Educational Resources Information Center

Jazzar, Michael

2006-01-01

Superintendent Gillet, lacking sensitivity to the environment of the school, allows issues to surface without resolving them within the context of the prevailing climate. He discovers the hard way that shared decision making, collaboration, and other participatory governance models should be implemented for resolving divergent issues. Rather than…

Paul Oil Company, Inc. Consent Agreements and Proposed Final Orders

EPA Pesticide Factsheets

Proposed settlements, recorded in two Consent Agreements and Final Orders (“Proposed Consent Agreements”), between EPA and Paul Oil Company, Inc., to resolve two civil administrative penalty proceedings.

Direct Observation of Insulin Association Dynamics with Time-Resolved X-ray Scattering

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

Rimmerman, Dolev; Leshchev, Denis; Hsu, Darren J.

Biological functions frequently require protein-protein interactions that involve secondary and tertiary structural perturbation. Here we study protein-protein dissociation and reassociation dynamics in insulin, a model system for protein oligomerization. Insulin dimer dissociation into monomers was induced by a nanosecond temperature-jump (T-jump) of ~8 °C in aqueous solution, and the resulting protein and solvent dynamics were tracked by time-resolved X-ray solution scattering (TRXSS) on time scales of 10 ns to 100 ms. The protein scattering signals revealed the formation of five distinguishable transient species during the association process that deviate from simple two state kinetics. Our results show that the combinationmore » of T-jump pump coupled to TRXSS probe allows for direct tracking of structural dynamics in nonphotoactive proteins.« less

20 CFR 404.1694 - Final accounting by the State.

Code of Federal Regulations, 2010 CFR

2010-04-01

... function. Disputes concerning final accounting issues which cannot be resolved between the State and us... 20 Employees' Benefits 2 2010-04-01 2010-04-01 false Final accounting by the State. 404.1694... DISABILITY INSURANCE (1950- ) Determinations of Disability Assumption of Disability Determination Function...

Nanoparticle motion on the surface of drying droplets

NASA Astrophysics Data System (ADS)

Zhao, Mingfei; Yong, Xin

2018-03-01

Advances in solution-based printing and surface patterning techniques for additive manufacturing demand a clear understanding of particle dynamics in drying colloidal droplets and its relationship with deposit structure. Although the evaporation-driven deposition has been studied thoroughly for the particles dispersed in the bulk of the droplet, few investigations have focused on the particles strongly adsorbed to the droplet surface. We modeled the assembly and deposition of the surface-active particles in a drying sessile droplet with a pinned contact line by the multiphase lattice Boltzmann-Brownian dynamics method. The particle trajectory and its area density profile characterize the assembly dynamics and deposition pattern development during evaporation. While the bulk-dispersed particles continuously move to the contact line, forming the typical "coffee-ring" deposit, the interface-bound particles migrate first toward the apex and then to the contact line as the droplet dries out. To understand this unexpected behavior, we resolve the droplet velocity field both in the bulk and within the interfacial region. The simulation results agree well with the analytical solution for the Stokes flow inside an evaporating droplet. At different stages of evaporation, our study reveals that the competition between the tangential surface flow and the downward motion of the evaporating liquid-vapor interface governs the dynamics of the interface-bound particles. In particular, the interface displacement contributes to the particle motion toward the droplet apex in a short phase, while the outward advective flow prevails at the late stage of drying and carries the particles to the contact line. The final deposit of the surface-adsorbed particles exhibits a density enhancement at the center, in addition to a coffee ring. Despite its small influence on the final deposit in the present study, the distinct dynamics of surface-active particles due to the interfacial confinement could offer a new route to deposition control when combined with Marangoni effects.

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.

MPACT Theory Manual, Version 2.2.0

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

Downar, Thomas; Collins, Benjamin S.; Gehin, Jess C.

2016-06-09

This theory manual describes the three-dimensional (3-D) whole-core, pin-resolved transport calculation methodology employed in the MPACT code. To provide sub-pin level power distributions with sufficient accuracy, MPACT employs the method of characteristics (MOC) solutions in the framework of a 3-D coarse mesh finite difference (CMFD) formulation. MPACT provides a 3D MOC solution, but also a 2D/1D solution in which the 2D planar solution is provided by MOC and the axial coupling is resolved by one-dimensional (1-D) lower order (diffusion or P3) solutions. In Chapter 2 of the manual, the MOC methodology is described for calculating the regional angular and scalarmore » fluxes from the Boltzmann transport equation. In Chapter 3, the 2D/1D methodology is described, together with the description of the CMFD iteration process involving dynamic homogenization and solution of the multigroup CMFD linear system. A description of the MPACT depletion algorithm is given in Chapter 4, followed by a discussion of the subgroup and ESSM resonance processing methods in Chapter 5. The final Chapter 6 describes a simplified thermal hydraulics model in MPACT.« less

Dual Brushless Resolver Rate Sensor

NASA Technical Reports Server (NTRS)

Howard, David E. (Inventor)

1996-01-01

This invention relates to dual analog angular rate sensors which are implemented without the use of mechanical brushes. A resolver rate sensor which includes two brushless resolvers which are mechanically coupled to the same output shaft is provided with inputs which are provided to each resolver by providing the first resolver with a DC input and the second resolver with an AC sinusoidal input. A trigonometric identity in which the sum of the squares of the sin and cosine components equal one is used to advantage in providing a sensor of increased accuracy. The first resolver may have a fixed or variable DC input to permit dynamic adjustment of resolver sensitivity thus permitting a wide range of coverage. Novelty and advantages of the invention reside in the excitation of a resolver with a DC signal and in the utilization of two resolvers and the trigonometric identity of cos(exp 2)(theta) + sin(exp 2)(theta) = 1 to provide an accurate rate sensor which is sensitive to direction and accurate through zero rate.

Toward Seamless Weather-Climate Prediction with a Global Cloud Resolving Model

DTIC Science & Technology

2016-01-14

distribution is unlimited. TOWARD SEAMLESS WEATHER- CLIMATE PREDICTION WITH A GLOBAL CLOUD RESOLVING MODEL PI: Tim Li IPRC/SOEST, University of Hawaii at...Project Final Report 3. DATES COVERED (From - To) 1 May 2012 - 30 September 2015 4. TITLE AND SUBTITLE TOWARD SEAMLESS WEATHER- CLIMATE PREDICTION WITH...A GLOBAL CLOUD RESOLVING MODEL 5a. CONTRACT NUMBER 5b. GRANT NUMBER N000141210450 5c. PROGRAM ELEMENT NUMBER ONR Marine Meteorology Program 6

Millifluidics for Chemical Synthesis and Time-resolved Mechanistic Studies

PubMed Central

Krishna, Katla Sai; Biswas, Sanchita; Navin, Chelliah V.; Yamane, Dawit G.; Miller, Jeffrey T.; Kumar, Challa S.S.R.

2013-01-01

Procedures utilizing millifluidic devices for chemical synthesis and time-resolved mechanistic studies are described by taking three examples. In the first, synthesis of ultra-small copper nanoclusters is described. The second example provides their utility for investigating time resolved kinetics of chemical reactions by analyzing gold nanoparticle formation using in situ X-ray absorption spectroscopy. The final example demonstrates continuous flow catalysis of reactions inside millifluidic channel coated with nanostructured catalyst. PMID:24327099

Femtosecond/picosecond time-resolved fluorescence study of hydrophilic polymer fine particles.

PubMed

Nanjo, Daisuke; Hosoi, Haruko; Fujino, Tatsuya; Tahara, Tahei; Korenaga, Takashi

2007-03-22

Femtosecond/picosecond time-resolved fluorescence study of hydrophilic polymer fine particles (polyacrylamide, PAAm) was reported. Ultrafast fluorescence dynamics of polymer/water solution was monitored using a fluorescent probe molecule (C153). In the femtosecond time-resolved fluorescence measurement at 480 nm, slowly decay components having lifetimes of tau(1) approximately 53 ps and tau(2) approximately 5 ns were observed in addition to rapid fluorescence decay. Picosecond time-resolved fluorescence spectra of C153/PAAm/H2O solution were also measured. In the time-resolved fluorescence spectra of C153/PAAm/H2O, a peak shift from 490 to 515 nm was measured, which can be assigned to the solvation dynamics of polymer fine particles. The fluorescence peak shift was related to the solvation response function and two time constants were determined (tau(3) approximately 50 ps and tau(4) approximately 467 ps). Therefore, the tau(1) component observed in the femtosecond time-resolved fluorescence measurement was assigned to the solvation dynamics that was observed only in the presence of polymer fine particles. Rotational diffusion measurements were also carried out on the basis of the picosecond time-resolved fluorescence spectra. In the C153/PAAm/H2O solution, anisotropy decay having two different time constants was also derived (tau(6) approximately 76 ps and tau(7) approximately 676 ps), indicating the presence of two different microscopic molecular environments around the polymer surface. Using the Stokes-Einstein-Debye (SED) equation, microscopic viscosity around the polymer surface was evaluated. For the area that gave a rotational diffusion time of tau(6) approximately 76 ps, the calculated viscosity is approximately 1.1 cP and for tau(7) approximately 676 ps, it is approximately 10 cP. The calculated viscosity values clearly revealed that there are two different molecular environments around the polyacrylamide fine particles.

Sensitivity of airborne geophysical data to sublacustrine permafrost thaw

NASA Astrophysics Data System (ADS)

Minsley, B. J.; Wellman, T. P.; Walvoord, M. A.; Revil, A.

2014-12-01

A coupled hydrogeophysical forward and inverse modeling approach is developed to illustrate the ability of frequency-domain airborne electromagnetic (AEM) data to characterize subsurface physical properties associated with sublacustrine permafrost thaw during lake talik formation. Several scenarios are evaluated that consider the response to variable hydrologic forcing from different lake depths and hydrologic gradients. The model includes a physical property relationship that connects the dynamic distribution of subsurface electrical resistivity based on lithology as well as ice-saturation and temperature outputs from the SUTRA groundwater simulator with freeze/thaw physics. Electrical resistivity models are used to simulate AEM data in order to explore the sensitivity of geophysical observations to permafrost thaw. Simulations of sublacustrine talik formation over a 1000 year period modeled after conditions found in the Yukon Flats, Alaska, are evaluated. Synthetic geophysical data are analyzed with a Bayesian Markov chain Monte Carlo algorithm that provides a probabilistic assessment of geophysical model uncertainty and resolution. Major lithological and permafrost features are well resolved in the examples considered. The subtle geometry of partial ice-saturation beneath lakes during talik formation cannot be resolved using AEM data, but the gross characteristics of sub-lake resistivity models reflect bulk changes in ice content and can be used to determine the presence of a talik. A final example compares AEM and ground-based electromagnetic responses for their ability to resolve shallow permafrost and thaw features in the upper 1-2 m below ground.

Non-Intrusive, Time-Resolved Hall Thruster Near-Field Electron Temperature Measurements

DTIC Science & Technology

2011-08-01

With the growing interest in Hall thruster technology, comes the need to fully characterize the plasma dynamics that determine performance. Of...instabilities characteristic of Hall thruster behavior, time resolved techniques must be developed. This study presents a non-intrusive method of

Lipidic cubic phase injector is a viable crystal delivery system for time-resolved serial crystallography

DOE PAGES

Nogly, Przemyslaw; Panneels, Valerie; Nelson, Garrett; ...

2016-08-22

Serial femtosecond crystallography (SFX) using X-ray free-electron laser sources is an emerging method with considerable potential for time-resolved pump-probe experiments. Here we present a lipidic cubic phase SFX structure of the light-driven proton pump bacteriorhodopsin (bR) to 2.3 Å resolution and a method to investigate protein dynamics with modest sample requirement. Time-resolved SFX (TR-SFX) with a pump-probe delay of 1 ms yields difference Fourier maps compatible with the dark to M state transition of bR. Importantly, the method is very sample efficient and reduces sample consumption to about 1 mg per collected time point. Accumulation of M intermediate within themore » crystal lattice is confirmed by time-resolved visible absorption spectroscopy. Furthermore, this study provides an important step towards characterizing the complete photocycle dynamics of retinal proteins and demonstrates the feasibility of a sample efficient viscous medium jet for TR-SFX.« less

Adjoint Sensitivity Analysis for Scale-Resolving Turbulent Flow Solvers

NASA Astrophysics Data System (ADS)

Blonigan, Patrick; Garai, Anirban; Diosady, Laslo; Murman, Scott

2017-11-01

Adjoint-based sensitivity analysis methods are powerful design tools for engineers who use computational fluid dynamics. In recent years, these engineers have started to use scale-resolving simulations like large-eddy simulations (LES) and direct numerical simulations (DNS), which resolve more scales in complex flows with unsteady separation and jets than the widely-used Reynolds-averaged Navier-Stokes (RANS) methods. However, the conventional adjoint method computes large, unusable sensitivities for scale-resolving simulations, which unlike RANS simulations exhibit the chaotic dynamics inherent in turbulent flows. Sensitivity analysis based on least-squares shadowing (LSS) avoids the issues encountered by conventional adjoint methods, but has a high computational cost even for relatively small simulations. The following talk discusses a more computationally efficient formulation of LSS, ``non-intrusive'' LSS, and its application to turbulent flows simulated with a discontinuous-Galkerin spectral-element-method LES/DNS solver. Results are presented for the minimal flow unit, a turbulent channel flow with a limited streamwise and spanwise domain.

Lipidic cubic phase injector is a viable crystal delivery system for time-resolved serial crystallography

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

Nogly, Przemyslaw; Panneels, Valerie; Nelson, Garrett

Serial femtosecond crystallography (SFX) using X-ray free-electron laser sources is an emerging method with considerable potential for time-resolved pump-probe experiments. Here we present a lipidic cubic phase SFX structure of the light-driven proton pump bacteriorhodopsin (bR) to 2.3 Å resolution and a method to investigate protein dynamics with modest sample requirement. Time-resolved SFX (TR-SFX) with a pump-probe delay of 1 ms yields difference Fourier maps compatible with the dark to M state transition of bR. Importantly, the method is very sample efficient and reduces sample consumption to about 1 mg per collected time point. Accumulation of M intermediate within themore » crystal lattice is confirmed by time-resolved visible absorption spectroscopy. Furthermore, this study provides an important step towards characterizing the complete photocycle dynamics of retinal proteins and demonstrates the feasibility of a sample efficient viscous medium jet for TR-SFX.« less

Lipidic cubic phase injector is a viable crystal delivery system for time-resolved serial crystallography

PubMed Central

Nogly, Przemyslaw; Panneels, Valerie; Nelson, Garrett; Gati, Cornelius; Kimura, Tetsunari; Milne, Christopher; Milathianaki, Despina; Kubo, Minoru; Wu, Wenting; Conrad, Chelsie; Coe, Jesse; Bean, Richard; Zhao, Yun; Båth, Petra; Dods, Robert; Harimoorthy, Rajiv; Beyerlein, Kenneth R.; Rheinberger, Jan; James, Daniel; DePonte, Daniel; Li, Chufeng; Sala, Leonardo; Williams, Garth J.; Hunter, Mark S.; Koglin, Jason E.; Berntsen, Peter; Nango, Eriko; Iwata, So; Chapman, Henry N.; Fromme, Petra; Frank, Matthias; Abela, Rafael; Boutet, Sébastien; Barty, Anton; White, Thomas A.; Weierstall, Uwe; Spence, John; Neutze, Richard; Schertler, Gebhard; Standfuss, Jörg

2016-01-01

Serial femtosecond crystallography (SFX) using X-ray free-electron laser sources is an emerging method with considerable potential for time-resolved pump-probe experiments. Here we present a lipidic cubic phase SFX structure of the light-driven proton pump bacteriorhodopsin (bR) to 2.3 Å resolution and a method to investigate protein dynamics with modest sample requirement. Time-resolved SFX (TR-SFX) with a pump-probe delay of 1 ms yields difference Fourier maps compatible with the dark to M state transition of bR. Importantly, the method is very sample efficient and reduces sample consumption to about 1 mg per collected time point. Accumulation of M intermediate within the crystal lattice is confirmed by time-resolved visible absorption spectroscopy. This study provides an important step towards characterizing the complete photocycle dynamics of retinal proteins and demonstrates the feasibility of a sample efficient viscous medium jet for TR-SFX. PMID:27545823

Ultrafast photodimerization dynamics in α-cyano-4-hydroxycinnamic and sinapinic acid crystals

NASA Astrophysics Data System (ADS)

Hoyer, Theo; Tuszynski, Wilfried; Lienau, Christoph

2007-07-01

We report a sub-picosecond time-resolved fluorescence spectroscopic study of different cinnamic acid crystals, model systems for solid-state photodimerization reactions. For α-cyano-4-hydroxycinnamic acid (α-CHC), we identify the emission spectra of both monomers and dimers, allowing us to directly probe the photoinduced dynamics of both species. The dimerization occurs on a timescale of 10 ps and results in a long-lived dimer product, stable for hours. For sinapinic acid, we find an extremely fast, sub-picosecond dimerization reaction and a short-lived dimer. This first sub-picosecond time-resolved dimerization study in cinnamic acid crystals provides a new basis for relating their structural properties and microscopic reaction dynamics.

Tetragonal and collapsed-tetragonal phases of CaFe2As2 : A view from angle-resolved photoemission and dynamical mean-field theory

NASA Astrophysics Data System (ADS)

van Roekeghem, Ambroise; Richard, Pierre; Shi, Xun; Wu, Shangfei; Zeng, Lingkun; Saparov, Bayrammurad; Ohtsubo, Yoshiyuki; Qian, Tian; Sefat, Athena S.; Biermann, Silke; Ding, Hong

2016-06-01

We present a study of the tetragonal to collapsed-tetragonal transition of CaFe2As2 using angle-resolved photoemission spectroscopy and dynamical mean field theory-based electronic structure calculations. We observe that the collapsed-tetragonal phase exhibits reduced correlations and a higher coherence temperature due to the stronger Fe-As hybridization. Furthermore, a comparison of measured photoemission spectra and theoretical spectral functions shows that momentum-dependent corrections to the density functional band structure are essential for the description of low-energy quasiparticle dispersions. We introduce those using the recently proposed combined "screened exchange + dynamical mean field theory" scheme.

Towards Measurement of the Time-resolved Heat Release of Protein Conformation Dynamics

NASA Technical Reports Server (NTRS)

Puchalla, Jason; Adamek, Daniel; Austin, Robert

2004-01-01

We present a way to observe time-resolved heat release using a laminar flow diffusional mixer coupled with a highly sensitive infrared camera which measures the temperature change of the solvent. There are significant benefits to the use of laminar flow mixers for time-resolved calorimetry: (1) The thermal signal can be made position and time- stationary to allow for signal integration; (2) Extremely small volumes (nl/s) of sample are required for a measurement; (3) The same mixing environment can be observed spectroscopically to obtain state occupation information; (4) The mixer allows one to do out of equilibrium dynamic studies. The hope is that these measurements will allow us probe the non-equilibrium thermodynamics as a protein moves along a free energy trajectory from one state to another.

20 CFR 416.1094 - Final accounting by the State.

Code of Federal Regulations, 2010 CFR

2010-04-01

... function. Disputes concerning final accounting issues which cannot be resolved between the State and us... 20 Employees' Benefits 2 2010-04-01 2010-04-01 false Final accounting by the State. 416.1094... AGED, BLIND, AND DISABLED Determinations of Disability Assumption of Disability Determination Function...

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

Chain-Length-Dependent Exciton Dynamics in Linear Oligothiophenes Probed Using Ensemble and Single-Molecule Spectroscopy.

PubMed

Kim, Tae-Woo; Kim, Woojae; Park, Kyu Hyung; Kim, Pyosang; Cho, Jae-Won; Shimizu, Hideyuki; Iyoda, Masahiko; Kim, Dongho

2016-02-04

Exciton dynamics in π-conjugated molecular systems is highly susceptible to conformational disorder. Using time-resolved and single-molecule spectroscopic techniques, the effect of chain length on the exciton dynamics in a series of linear oligothiophenes, for which the conformational disorder increased with increasing chain length, was investigated. As a result, extraordinary features of the exciton dynamics in longer-chain oligothiophene were revealed. Ultrafast fluorescence depolarization processes were observed due to exciton self-trapping in longer and bent chains. Increase in exciton delocalization during dynamic planarization processes was also observed in the linear oligothiophenes via time-resolved fluorescence spectra but was restricted in L-10T because of its considerable conformational disorder. Exciton delocalization was also unexpectedly observed in a bent chain using single-molecule fluorescence spectroscopy. Such delocalization modulates the fluorescence spectral shape by attenuating the 0-0 peak intensity. Collectively, these results provide significant insights into the exciton dynamics in conjugated polymers.

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

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

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.

Nonequilibrium lattice-driven dynamics of stripes in nickelates using time-resolved x-ray scattering

DOE PAGES

Lee, W. S.; Kung, Y. F.; Moritz, B.; ...

2017-03-13

Here, we investigate the lattice coupling to the spin and charge orders in the striped nickelate, La 1.75 Sr 0.25 NiO 4, using time-resolved resonant x-ray scattering. Lattice-driven dynamics of both spin and charge orders are observed when the pump photon energy is tuned to that of an E u bond- stretching phonon. We present a likely scenario for the behavior of the spin and charge order parameters and its implications using a Ginzburg-Landau theory.

Electron-spin dynamics in Mn-doped GaAs using time-resolved magneto-optical techniques

NASA Astrophysics Data System (ADS)

Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Zhukov, E. A.; Yakovlev, D. R.; Bayer, M.

2009-08-01

We study the electron-spin dynamics in p -type GaAs doped with magnetic Mn acceptors by means of time-resolved pump-probe and photoluminescence techniques. Measurements in transverse magnetic fields show a long spin-relaxation time of 20 ns that can be uniquely related to electrons. Application of weak longitudinal magnetic fields above 100 mT extends the spin-relaxation times up to microseconds which is explained by suppression of the Bir-Aronov-Pikus spin relaxation for the electron on the Mn acceptor.

Beam-dynamics codes used at DARHT

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

Ekdahl, Jr., Carl August

Several beam simulation codes are used to help gain a better understanding of beam dynamics in the DARHT LIAs. The most notable of these fall into the following categories: for beam production – Tricomp Trak orbit tracking code, LSP Particle in cell (PIC) code, for beam transport and acceleration – XTR static envelope and centroid code, LAMDA time-resolved envelope and centroid code, LSP-Slice PIC code, for coasting-beam transport to target – LAMDA time-resolved envelope code, LSP-Slice PIC code. These codes are also being used to inform the design of Scorpius.

Nonequilibrium lattice-driven dynamics of stripes in nickelates using time-resolved x-ray scattering

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

Lee, W. S.; Kung, Y. F.; Moritz, B.

Here, we investigate the lattice coupling to the spin and charge orders in the striped nickelate, La 1.75 Sr 0.25 NiO 4, using time-resolved resonant x-ray scattering. Lattice-driven dynamics of both spin and charge orders are observed when the pump photon energy is tuned to that of an E u bond- stretching phonon. We present a likely scenario for the behavior of the spin and charge order parameters and its implications using a Ginzburg-Landau theory.

Plastique: A synchrotron radiation beamline for time resolved fluorescence in the frequency domain

NASA Astrophysics Data System (ADS)

De Stasio, Gelsomina; Zema, N.; Antonangeli, F.; Savoia, A.; Parasassi, T.; Rosato, N.

1991-06-01

PLASTIQUE is the only synchrotron radiation beamline in the world that performs time resolved fluorescence experiments in frequency domain. These experiments are extremely valuable sources of information on the structure and dynamics of molecules. We describe the beamline and some initial data.

A Method on Dynamic Path Planning for Robotic Manipulator Autonomous Obstacle Avoidance Based on an Improved RRT Algorithm.

PubMed

Wei, Kun; Ren, Bingyin

2018-02-13

In a future intelligent factory, a robotic manipulator must work efficiently and safely in a Human-Robot collaborative and dynamic unstructured environment. Autonomous path planning is the most important issue which must be resolved first in the process of improving robotic manipulator intelligence. Among the path-planning methods, the Rapidly Exploring Random Tree (RRT) algorithm based on random sampling has been widely applied in dynamic path planning for a high-dimensional robotic manipulator, especially in a complex environment because of its probability completeness, perfect expansion, and fast exploring speed over other planning methods. However, the existing RRT algorithm has a limitation in path planning for a robotic manipulator in a dynamic unstructured environment. Therefore, an autonomous obstacle avoidance dynamic path-planning method for a robotic manipulator based on an improved RRT algorithm, called Smoothly RRT (S-RRT), is proposed. This method that targets a directional node extends and can increase the sampling speed and efficiency of RRT dramatically. A path optimization strategy based on the maximum curvature constraint is presented to generate a smooth and curved continuous executable path for a robotic manipulator. Finally, the correctness, effectiveness, and practicability of the proposed method are demonstrated and validated via a MATLAB static simulation and a Robot Operating System (ROS) dynamic simulation environment as well as a real autonomous obstacle avoidance experiment in a dynamic unstructured environment for a robotic manipulator. The proposed method not only provides great practical engineering significance for a robotic manipulator's obstacle avoidance in an intelligent factory, but also theoretical reference value for other type of robots' path planning.

Can memory and conformism resolve the vaccination dilemma?

NASA Astrophysics Data System (ADS)

Han, Dun; Sun, Mei

2014-12-01

Considering that memory and conformity could affect the agent’s decision, in this paper, we propose a novel model to describe the vaccination dilemma by entangling the spreading dynamics with an evolutionary framework. Our results indicate that if the individuals make decision mostly depending on their own payoffs and do not believe too much in the celebrity, the final infected number will be significantly reduced. Comparing with the individuals in the BA network, people in the ER network escape from contagion much more easily and could get bigger payoffs. For the countries, strengthening the medical security system and reducing the cost of immunity can curb the spread of viruses effectively. From an individual’s viewpoint, people just remember their own last season’s payoffs can urge them to vaccinate.

Direct simulation Monte Carlo investigation of the Rayleigh-Taylor instability

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

Gallis, M. A.; Koehler, T. P.; Torczynski, J. R.

In this paper, the Rayleigh-Taylor instability (RTI) is investigated using the direct simulation Monte Carlo (DSMC) method of molecular gas dynamics. Here, fully resolved two-dimensional DSMC RTI simulations are performed to quantify the growth of flat and single-mode perturbed interfaces between two atmospheric-pressure monatomic gases as a function of the Atwood number and the gravitational acceleration. The DSMC simulations reproduce many qualitative features of the growth of the mixing layer and are in reasonable quantitative agreement with theoretical and empirical models in the linear, nonlinear, and self-similar regimes. In some of the simulations at late times, the instability enters themore » self-similar regime, in agreement with experimental observations. Finally, for the conditions simulated, diffusion can influence the initial instability growth significantly.« less

Accurate quantum yields by laser gain vs absorption spectroscopy - Investigation of Br/Br(asterisk) channels in photofragmentation of Br2 and IBr

NASA Technical Reports Server (NTRS)

Haugen, H. K.; Weitz, E.; Leone, S. R.

1985-01-01

Various techniques have been used to study photodissociation dynamics of the halogens and interhalogens. The quantum yields obtained by these techniques differ widely. The present investigation is concerned with a qualitatively new approach for obtaining highly accurate quantum yields for electronically excited states. This approach makes it possible to obtain an accuracy of 1 percent to 3 percent. It is shown that measurement of the initial transient gain/absorption vs the final absorption in a single time-resolved signal is a very accurate technique in the study of absolute branching fractions in photodissociation. The new technique is found to be insensitive to pulse and probe laser characteristics, molecular absorption cross sections, and absolute precursor density.

Direct simulation Monte Carlo investigation of the Rayleigh-Taylor instability

DOE PAGES

Gallis, M. A.; Koehler, T. P.; Torczynski, J. R.; ...

2016-08-31

In this paper, the Rayleigh-Taylor instability (RTI) is investigated using the direct simulation Monte Carlo (DSMC) method of molecular gas dynamics. Here, fully resolved two-dimensional DSMC RTI simulations are performed to quantify the growth of flat and single-mode perturbed interfaces between two atmospheric-pressure monatomic gases as a function of the Atwood number and the gravitational acceleration. The DSMC simulations reproduce many qualitative features of the growth of the mixing layer and are in reasonable quantitative agreement with theoretical and empirical models in the linear, nonlinear, and self-similar regimes. In some of the simulations at late times, the instability enters themore » self-similar regime, in agreement with experimental observations. Finally, for the conditions simulated, diffusion can influence the initial instability growth significantly.« less

Plasma Outflows: Known Knowns, Known Unknowns, and The Unknown

NASA Technical Reports Server (NTRS)

Moore, T. E.

2012-01-01

A brief summary is given of i) what we know from observing ionospheric outflows and ii) how outflow parameterizations are being used in global simulations to evaluate their effects on magnetospheric dynamics. Then, a list of unanswered questions and issues to be resolved is given, followed by a description of the known future mission plans expressed in the Heliophysics Roadmap, such as Origin of Near-Earth Plasmas (ONEP), and Ion-Neutral Coupling in the Atmosphere (INCA). Finally, a set of requirements for definitive plasma outflow observations are identified, along with possible methods for fulfilling them in future missions. Since results of the current Heliophysics Decadal Survey are expected soon, it is hoped that future plans can be summarized and discussed without speculation at the GEM 2012 meeting.

A Shock-Adaptive Godunov Scheme Based on the Generalised Lagrangian Formulation

NASA Astrophysics Data System (ADS)

Lepage, C. Y.; Hui, W. H.

1995-12-01

Application of the Godunov scheme to the Euler equations of gas dynamics based on the Eulerian formulation of flow smears discontinuities, sliplines especially, over several computational cells, while the accuracy in the smooth flow region is of the order O( h), where h is the cell width. Based on the generalised Lagrangian formulation (GLF) of Hui et al., the Godunov scheme yields superior accuracy. By the use of coordinate streamlines in the GLF, the slipline—itself a streamline—is resolved crisply. Infinite shock resolution is achieved through the splitting of shock-cells. An improved entropy-conservation formulation of the governing equations is also proposed for computations in smooth flow regions. Finally, the use of the GLF substantially simplifies the programming logic resulting in a very robust, accurate, and efficient scheme.

Development of 2D imaging of SXR plasma radiation by means of GEM detectors

NASA Astrophysics Data System (ADS)

Chernyshova, M.; Czarski, T.; Jabłoński, S.; Kowalska-Strzeciwilk, E.; Poźniak, K.; Kasprowicz, G.; Zabołotny, W.; Wojeński, A.; Byszuk, A.; Burza, M.; Juszczyk, B.; Zienkiewicz, P.

2014-11-01

Presented 2D gaseous detector system has been developed and designed to provide energy resolved fast dynamic plasma radiation imaging in the soft X-Ray region with 0.1 kHz exposure frequency for online, made in real time, data acquisition (DAQ) mode. The detection structure is based on triple Gas Electron Multiplier (GEM) amplification structure followed by the pixel readout electrode. The efficiency of detecting unit was adjusted for the radiation energy region of tungsten in high-temperature plasma, the main candidate for the plasma facing material for future thermonuclear reactors. Here we present preliminary laboratory results and detector parameters obtained for the developed system. The operational characteristics and conditions of the detector were designed to work in the X-Ray range of 2-17 keV. The detector linearity was checked using the fluorescence lines of different elements and was found to be sufficient for good photon energy reconstruction. Images of two sources through various screens were performed with an X-Ray laboratory source and 55Fe source showing a good imaging capability. Finally offline stream-handling data acquisition mode has been developed for the detecting system with timing down to the ADC sampling frequency rate (~13 ns), up to 2.5 MHz of exposure frequency, which could pave the way to invaluable physics information about plasma dynamics due to very good time resolving ability. Here we present results of studied spatial resolution and imaging properties of the detector for conditions of laboratory moderate counting rates and high gain.

A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

NASA Astrophysics Data System (ADS)

Zhu, S.; Sartelet, K. N.; Seigneur, C.

2015-06-01

The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

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.

Dual Brushless Resolver Rate Sensor

NASA Technical Reports Server (NTRS)

Howard, David E. (Inventor)

1997-01-01

A resolver rate sensor is disclosed in which dual brushless resolvers are mechanically coupled to the same output shaft. Diverse inputs are provided to each resolver by providing the first resolver with a DC input and the second resolver with an AC sinusoidal input. A trigonometric identity in which the sum of the squares of the sin and cosine components equal one is used to advantage in providing a sensor of increased accuracy. The first resolver may have a fixed or variable DC input to permit dynamic adjustment of resolver sensitivity thus permitting a wide range of coverage. In one embodiment of the invention the outputs of the first resolver are directly inputted into two separate multipliers and the outputs of the second resolver are inputted into the two separate multipliers, after being demodulated in a pair of demodulator circuits. The multiplied signals are then added in an adder circuit to provide a directional sensitive output. In another embodiment the outputs from the first resolver is modulated in separate modulator circuits and the output from the modulator circuits are used to excite the second resolver. The outputs from the second resolver are demodulated in separate demodulator circuit and added in an adder circuit to provide a direction sensitive rate output.

Resolved motion rate and resolved acceleration servo-control of wheeled mobile robots

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

Muir, P.F.; Neuman, C.P.; Carnegie-Mellon Univ., Pittsburgh, PA

1989-01-01

Accurate motion control of wheeled mobile robots (WMRs) is required for their application to autonomous, semi-autonomous and teleoperated tasks. The similarities between WMRs and stationary manipulators suggest that current, successful, model-based manipulator control algorithms may be applied to WMRs. Special characteristics of WMRs including higher-pairs, closed-chains, friction and unactuated and unsensed joints require innovative modeling methodologies. The WMR modeling challenge has been recently overcome, thus enabling the application of manipulator control algorithms to WMRs. This realization lays the foundation for significant technology transfer from manipulator control to WMR control. We apply two Cartesian-space manipulator control algorithms: resolved motion rate (kinematics-based)more » and resolved acceleration (dynamics-based) control to WMR servo-control. We evaluate simulation studies of two exemplary WMRs: Uranus (a three degree-of-freedom WMR constructed at Carnegie Mellon University), and Bicsun-Bicas (a two degree-of-freedom WMR being constructed at Sandia National Laboratories) under the control of these algorithms. Although resolved motion rate servo-control is adequate for the control of Uranus, resolved acceleration servo-control is required for the control of the mechanically simpler Bicsun-Bicas because it exhibits more dynamic coupling and nonlinearities. Successful accurate motion control of these WMRs in simulation is driving current experimental research studies. 18 refs., 7 figs., 5 tabs.« less

Security Paving Company, Inc.: Consent Agreement and Proposed Final Order

EPA Pesticide Factsheets

Consent Agreement and Proposed Final Order (“Proposed Consent Agreement”), between the U.S. Environmental Protection Agency, Region 9 (“EPA”), and Security Paving Company (“Respondent”) to resolve a civil administrative penalty proceeding.

Parallel Multiscale Algorithms for Astrophysical Fluid Dynamics Simulations

NASA Technical Reports Server (NTRS)

Norman, Michael L.

1997-01-01

Our goal is to develop software libraries and applications for astrophysical fluid dynamics simulations in multidimensions that will enable us to resolve the large spatial and temporal variations that inevitably arise due to gravity, fronts and microphysical phenomena. The software must run efficiently on parallel computers and be general enough to allow the incorporation of a wide variety of physics. Cosmological structure formation with realistic gas physics is the primary application driver in this work. Accurate simulations of e.g. galaxy formation require a spatial dynamic range (i.e., ratio of system scale to smallest resolved feature) of 104 or more in three dimensions in arbitrary topologies. We take this as our technical requirement. We have achieved, and in fact, surpassed these goals.

Controlling the influence of elastic eigenmodes on nanomagnet dynamics through pattern geometry

NASA Astrophysics Data System (ADS)

Berk, C.; Yahagi, Y.; Dhuey, S.; Cabrini, S.; Schmidt, H.

2017-03-01

The effect of the nanoscale array geometry on the interaction between optically generated surface acoustic waves (SAWs) and nanomagnet dynamics is investigated using Time-Resolved Magneto-Optical Kerr Effect Microscopy (TR-MOKE). It is demonstrated that altering the nanomagnet geometry from a periodic to a randomized aperiodic pattern effectively removes the magneto-elastic effect of SAWs on the magnetization dynamics. The efficiency of this method depends on the extent of any residual spatial correlations and is quantified by spatial Fourier analysis of the two structures. Randomization allows observation and extraction of intrinsic magnetic parameters such as spin wave frequencies and damping to be resolvable using all-optical methods, enabling the conclusion that the fabrication process does not affect the damping.

The Resolvent Algebra of Non-relativistic Bose Fields: Observables, Dynamics and States

NASA Astrophysics Data System (ADS)

Buchholz, Detlev

2018-05-01

The structure of the gauge invariant (particle number preserving) C*-algebra generated by the resolvents of a non-relativistic Bose field is analyzed. It is shown to form a dense subalgebra of the bounded inverse limit of a directed system of approximately finite dimensional C*-algebras. Based on this observation, it is proven that the closure of the gauge invariant algebra is stable under the dynamics induced by Hamiltonians involving pair potentials. These facts allow to proceed to a description of interacting Bosons in terms of C*-dynamical systems. It is outlined how the present approach leads to simplifications in the construction of infinite bosonic states and sheds new light on topics in many body theory.

32-channel pyrometer with high dynamic range for studies of shocked nanothermites

NASA Astrophysics Data System (ADS)

Bassett, Will P.; Dlott, Dana D.

2017-01-01

A 32-channel optical pyrometer has been developed for studying temperature dynamics of shock-initiated reactive materials with one nanosecond time resolution and high dynamic range. The pyrometer consists of a prism spectrograph which directs the spectrally-resolved emission to 32 fiber optics and 32 photomultiplier tubes and digitizers. Preliminary results show shock-initiated reactions of a nanothermite composite, nano CuO/Al in nitrocellulose binder, consists of three stages. The first stage occurred at 30 ns, right after the shock unloaded, the second stage at 100 ns and the third at 1 μs, and the temperatures ranged from 2100K to 3000K. Time-resolved emission spectra suggest hot spots formed during shock unloading, which initiated the bulk thermite/nitrocellulose reaction.

Unsteady, one-dimensional gas dynamics computations using a TVD type sequential solver

NASA Technical Reports Server (NTRS)

Thakur, Siddharth; Shyy, Wei

1992-01-01

The efficacy of high resolution convection schemes to resolve sharp gradient in unsteady, 1D flows is examined using the TVD concept based on a sequential solution algorithm. Two unsteady flow problems are considered which include the problem involving the interaction of the various waves in a shock tube with closed reflecting ends and the problem involving the unsteady gas dynamics in a tube with closed ends subject to an initial pressure perturbation. It is concluded that high accuracy convection schemes in a sequential solution framework are capable of resolving discontinuities in unsteady flows involving complex gas dynamics. However, a sufficient amount of dissipation is required to suppress oscillations near discontinuities in the sequential approach, which leads to smearing of the solution profiles.

Quasiparticle dynamics across the full Brillouin zone of Bi 2Sr 2CaCu 2O 8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy

DOE PAGES

Dakovski, Georgi L.; Durakiewicz, Tomasz; Zhu, Jian-Xin; ...

2015-10-12

A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy which significantly limits the accessible momentum space. Using 20.15eV, 12 fs pulses we show for the first time the evolution of quasiparticles in the antinodal region of Bi 2Sr 2CaCu 2Omore » 8+δ and demonstrate that nonmonotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in severe contrast to the monotonic relaxation in the nodal and off-nodal regions.« less

Control integration concept for hypersonic cruise-turn maneuvers

NASA Technical Reports Server (NTRS)

Raney, David L.; Lallman, Frederick J.

1992-01-01

Piloting difficulties associated with conducting aircraft maneuvers in hypersonic flight are caused in part by the nonintuitive nature of the aircraft response and the stringent constraints anticipated on allowable angle of attack and dynamic pressure variations. An approach is documented that provides precise, coordinated maneuver control during excursions from a hypersonic cruise flight path and the necessary flight condition constraints. The approach is to achieve specified guidance commands by resolving altitude and cross range errors into a load factor and bank angle command by using a coordinate transformation that acts as an interface between outer and inner loop flight controls. This interface, referred to as a 'resolver', applies constraints on angle of attack and dynamic pressure perturbations while prioritizing altitude regulation over cross range. An unpiloted test simulation, in which the resolver was used to drive inner loop flight controls, produced time histories of responses to guidance commands and atmospheric disturbances at Mach numbers of 6, 10, 15, and 20. Angle of attack and throttle perturbation constraints, combined with high speed flight effects and the desire to maintain constant dynamic pressure, significantly impact the maneuver envelope for a hypersonic vehicle.

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.

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.

Imaging Magnetization Structure and Dynamics in Ultrathin Y3Fe5O12/Pt Bilayers with High Sensitivity Using the Time-Resolved Longitudinal Spin Seebeck Effect

NASA Astrophysics Data System (ADS)

Bartell, Jason M.; Jermain, Colin L.; Aradhya, Sriharsha V.; Brangham, Jack T.; Yang, Fengyuan; Ralph, Daniel C.; Fuchs, Gregory D.

2017-04-01

We demonstrate an instrument for time-resolved magnetic imaging that is highly sensitive to the in-plane magnetization state and dynamics of thin-film bilayers of yttrium iron garnet [Y3Fe5O12(YIG )]/Pt : the time-resolved longitudinal spin Seebeck (TRLSSE) effect microscope. We detect the local in-plane magnetic orientation within the YIG by focusing a picosecond laser to generate thermally driven spin current from the YIG into the Pt by the spin Seebeck effect and then use the inverse spin Hall effect in the Pt to transduce this spin current to an output voltage. To establish the time resolution of TRLSSE, we show that pulsed optical heating of patterned YIG (20 nm )/Pt (6 nm )/Ru (2 nm ) wires generates a magnetization-dependent voltage pulse of less than 100 ps. We demonstrate TRLSSE microscopy to image both static magnetic structure and gigahertz-frequency magnetic resonance dynamics with submicron spatial resolution and a sensitivity to magnetic orientation below 0.3 °/√{H z } in ultrathin YIG.

Resolving the Schwarzschild singularity in both classic and quantum gravity

NASA Astrophysics Data System (ADS)

Zeng, Ding-fang

2017-04-01

The Schwarzschild singularity's resolution has key values in cracking the key mysteries related with black holes, the origin of their horizon entropy and the information missing puzzle involved in their evaporations. We provide in this work the general dynamic inner metric of collapsing stars with horizons and with non-trivial radial mass distributions. We find that static central singularities are not the final state of the system. Instead, the final state of the system is a periodically zero-cross breathing ball. Through 3+1 decomposed general relativity and its quantum formulation, we establish a functional Schrödinger equation controlling the micro-state of this breathing ball and show that, the system configuration with all the matter concentrating on the central point is not the unique eigen-energy-density solution. Using a Bohr-Sommerfield like "orbital" quantisation assumption, we show that for each black hole of horizon radius rh, there are about e rh2 / ℓpl2 allowable eigen-energy-density profiles. This naturally leads to physic interpretations for the micro-origin of horizon entropy, as well as solutions to the information missing puzzle involved in Hawking radiations.

Vortex dynamics and heat transfer behind self-oscillating inverted flags of various lengths in channel flow

NASA Astrophysics Data System (ADS)

Yu, Yuelong; Liu, Yingzheng; Chen, Yujia

2018-04-01

The influence of an inverted flag's length-to-channel-width ratio (C* = L/W) on its oscillating behavior in a channel flow and the resultant vortex dynamics and heat transfer are determined experimentally. Three systems with C* values of 0.125, 0.250, and 0.375 were chosen for comparison. The interaction of highly unsteady flow with the inverted flag is measured with time-resolved particle image velocimetry. Variations in the underlying flow physics are discussed in terms of the statistical flow quantities, flag displacement, phase-averaged flow field, and vortex dynamics. The results show that the increase in C* shifts the occurrence of the flapping regime at high dimensionless bending stiffness. With the flag in the flapping region, three distinct vortex dynamics—the von Kármán vortex street, the G mode, and the singular mode—are identified at C* values of 0.375, 0.250, and 0.125, respectively. Finally, the heat transfer enhancement from the self-oscillating inverted flag is measured to serve as complementary information to quantify the cause-and-effect relationship between vortex dynamics and wall heat transfer. The increase in C* strongly promotes wall heat removal because disruption of the boundary layer by the energetic vortices is substantially intensified. Among all systems, wall heat transfer removal is most efficient at the intermediate C* value of 0.250.

Formulation of state projected centroid molecular dynamics: Microcanonical ensemble and connection to the Wigner distribution.

PubMed

Orr, Lindsay; Hernández de la Peña, Lisandro; Roy, Pierre-Nicholas

2017-06-07

A derivation of quantum statistical mechanics based on the concept of a Feynman path centroid is presented for the case of generalized density operators using the projected density operator formalism of Blinov and Roy [J. Chem. Phys. 115, 7822-7831 (2001)]. The resulting centroid densities, centroid symbols, and centroid correlation functions are formulated and analyzed in the context of the canonical equilibrium picture of Jang and Voth [J. Chem. Phys. 111, 2357-2370 (1999)]. The case where the density operator projects onto a particular energy eigenstate of the system is discussed, and it is shown that one can extract microcanonical dynamical information from double Kubo transformed correlation functions. It is also shown that the proposed projection operator approach can be used to formally connect the centroid and Wigner phase-space distributions in the zero reciprocal temperature β limit. A Centroid Molecular Dynamics (CMD) approximation to the state-projected exact quantum dynamics is proposed and proven to be exact in the harmonic limit. The state projected CMD method is also tested numerically for a quartic oscillator and a double-well potential and found to be more accurate than canonical CMD. In the case of a ground state projection, this method can resolve tunnelling splittings of the double well problem in the higher barrier regime where canonical CMD fails. Finally, the state-projected CMD framework is cast in a path integral form.

Formulation of state projected centroid molecular dynamics: Microcanonical ensemble and connection to the Wigner distribution

NASA Astrophysics Data System (ADS)

Orr, Lindsay; Hernández de la Peña, Lisandro; Roy, Pierre-Nicholas

2017-06-01

A derivation of quantum statistical mechanics based on the concept of a Feynman path centroid is presented for the case of generalized density operators using the projected density operator formalism of Blinov and Roy [J. Chem. Phys. 115, 7822-7831 (2001)]. The resulting centroid densities, centroid symbols, and centroid correlation functions are formulated and analyzed in the context of the canonical equilibrium picture of Jang and Voth [J. Chem. Phys. 111, 2357-2370 (1999)]. The case where the density operator projects onto a particular energy eigenstate of the system is discussed, and it is shown that one can extract microcanonical dynamical information from double Kubo transformed correlation functions. It is also shown that the proposed projection operator approach can be used to formally connect the centroid and Wigner phase-space distributions in the zero reciprocal temperature β limit. A Centroid Molecular Dynamics (CMD) approximation to the state-projected exact quantum dynamics is proposed and proven to be exact in the harmonic limit. The state projected CMD method is also tested numerically for a quartic oscillator and a double-well potential and found to be more accurate than canonical CMD. In the case of a ground state projection, this method can resolve tunnelling splittings of the double well problem in the higher barrier regime where canonical CMD fails. Finally, the state-projected CMD framework is cast in a path integral form.

Mathematical improvement of the Hopfield model for feasible solutions to the traveling salesman problem by a synapse dynamical system.

PubMed

Takahashi, Y

1998-01-01

It is well known that the Hopfield Model (HM) for neural networks to solve the Traveling Salesman Problem (TSP) suffers from three major drawbacks. (1) It can converge on nonoptimal locally minimum solutions. (2) It can converge on infeasible solutions. (3) Results are very sensitive to the careful tuning of its parameters. A number of methods have been proposed to overcome (a) well. In contrast, work on (b) and (c) has not been sufficient; techniques have not been generalized to more general optimization problems. Thus this paper mathematically resolves (b) and (c) to such an extent that the resolution can be applied to solving with some general network continuous optimization problems including the Hopfield version of the TSP. It first constructs an Extended HM (E-HM) that overcomes both (b) and (c). Fundamental techniques of the E-HM lie in the addition of a synapse dynamical system cooperated with the current HM unit dynamical system. It is this synapse dynamical system that makes the TSP constraint hold at any final states for whatever choices of the IIM parameters and an initial state. The paper then generalizes the E-HM further to a network that can solve a class of continuous optimization problems with a constraint equation where both of the objective function and the constraint function are nonnegative and continuously differentiable.

Exploring size and state dynamics in CdSe quantum dots using two-dimensional electronic spectroscopy

PubMed Central

Caram, Justin R.; Zheng, Haibin; Dahlberg, Peter D.; Rolczynski, Brian S.; Griffin, Graham B.; Dolzhnikov, Dmitriy S.; Talapin, Dmitri V.; Engel, Gregory S.

2014-01-01

Development of optoelectronic technologies based on quantum dots depends on measuring, optimizing, and ultimately predicting charge carrier dynamics in the nanocrystal. In such systems, size inhomogeneity and the photoexcited population distribution among various excitonic states have distinct effects on electron and hole relaxation, which are difficult to distinguish spectroscopically. Two-dimensional electronic spectroscopy can help to untangle these effects by resolving excitation energy and subsequent nonlinear response in a single experiment. Using a filament-generated continuum as a pump and probe source, we collect two-dimensional spectra with sufficient spectral bandwidth to follow dynamics upon excitation of the lowest three optical transitions in a polydisperse ensemble of colloidal CdSe quantum dots. We first compare to prior transient absorption studies to confirm excitation-state-dependent dynamics such as increased surface-trapping upon excitation of hot electrons. Second, we demonstrate fast band-edge electron-hole pair solvation by ligand and phonon modes, as the ensemble relaxes to the photoluminescent state on a sub-picosecond time-scale. Third, we find that static disorder due to size polydispersity dominates the nonlinear response upon excitation into the hot electron manifold; this broadening mechanism stands in contrast to that of the band-edge exciton. Finally, we demonstrate excitation-energy dependent hot-carrier relaxation rates, and we describe how two-dimensional electronic spectroscopy can complement other transient nonlinear techniques. PMID:24588185

Dynamics of electron solvation in I(-)(CH3OH)n clusters (4 ≤ n ≤ 11).

PubMed

Young, Ryan M; Yandell, Margaret A; Neumark, Daniel M

2011-03-28

The dynamics of electron solvation following excitation of the charge-transfer-to-solvent precursor state in iodide-doped methanol clusters, I(-)(CH(3)OH)(n = 4-11), are studied with time-resolved photoelectron imaging. This excitation produces a I···(CH(3)OH)(n)(-) cluster that is unstable with respect to electron autodetachment and whose autodetachment lifetime increases monotonically from ~800 fs to 85 ps as n increases from 4 to 11. The vertical detachment energy (VDE) and width of the excited state feature in the photoelectron spectrum show complex time dependence during the lifetime of this state. The VDE decreases over the first 100-400 fs, then rises exponentially to a maximum with a ~1 ps time constant, and finally decreases by as much as 180 meV with timescales of 3-20 ps. The early dynamics are associated with electron transfer from the iodide to the methanol cluster, while the longer-time changes in VDE are attributed to solvent reordering, possibly in conjunction with ejection of neutral iodine from the cluster. Changes in the observed width of the spectrum largely follow those of the VDEs; the dynamics of both are attributed to the major rearrangement of the solvent cluster during relaxation. The relaxation dynamics are interpreted as a reorientation of at least one methanol molecule and the disruption and formation of the solvent network in order to accommodate the excess charge.

An information entropy model on clinical assessment of patients based on the holographic field of meridian

NASA Astrophysics Data System (ADS)

Wu, Jingjing; Wu, Xinming; Li, Pengfei; Li, Nan; Mao, Xiaomei; Chai, Lihe

2017-04-01

Meridian system is not only the basis of traditional Chinese medicine (TCM) method (e.g. acupuncture, massage), but also the core of TCM's basic theory. This paper has introduced a new informational perspective to understand the reality and the holographic field of meridian. Based on maximum information entropy principle (MIEP), a dynamic equation for the holographic field has been deduced, which reflects the evolutionary characteristics of meridian. By using self-organizing artificial neural network as algorithm, the evolutionary dynamic equation of the holographic field can be resolved to assess properties of meridians and clinically diagnose the health characteristics of patients. Finally, through some cases from clinical patients (e.g. a 30-year-old male patient, an apoplectic patient, an epilepsy patient), we use this model to assess the evolutionary properties of meridians. It is proved that this model not only has significant implications in revealing the essence of meridian in TCM, but also may play a guiding role in clinical assessment of patients based on the holographic field of meridians.

On the dynamics of implicit emotion regulation: counter-regulation after remembering events of high but not of low emotional intensity.

PubMed

Schwager, Susanne; Rothermund, Klaus

2014-01-01

Valence biases in attention allocation were assessed after remembering positive or negative personal events that were either still emotionally hot or to which the person had already adapted psychologically. Differences regarding the current state of psychological adjustment were manipulated experimentally by instructing participants to recall distant vs. recent events (Experiment 1) or affectively hot events vs. events to which the person had accommodated already (Experiment 2). Valence biases in affective processing were measured with a valence search task. Processes of emotional counter-regulation (i.e., attention allocation to stimuli of opposite valence to the emotional event) were elicited by remembering affectively hot events, whereas congruency effects (i.e., attention allocation to stimuli of the same valence as the emotional event) were obtained for events for which a final appraisal had already been established. The results of our study help to resolve conflicting findings from the literature regarding congruent vs. incongruent effects of remembering emotional events on affective processing. We discuss implications of our findings for the conception of emotions and for the dynamics of emotion regulation processes.

Resolving coiled shapes reveals new reorientation behaviors in C. elegans

PubMed Central

Broekmans, Onno D; Rodgers, Jarlath B; Ryu, William S; Stephens, Greg J

2016-01-01

We exploit the reduced space of C. elegans postures to develop a novel tracking algorithm which captures both simple shapes and also self-occluding coils, an important, yet unexplored, component of 2D worm behavior. We apply our algorithm to show that visually complex, coiled sequences are a superposition of two simpler patterns: the body wave dynamics and a head-curvature pulse. We demonstrate the precise Ω-turn dynamics of an escape response and uncover a surprising new dichotomy in spontaneous, large-amplitude coils; deep reorientations occur not only through classical Ω-shaped postures but also through larger postural excitations which we label here as δ-turns. We find that omega and delta turns occur independently, suggesting a distinct triggering mechanism, and are the serpentine analog of a random left-right step. Finally, we show that omega and delta turns occur with approximately equal rates and adapt to food-free conditions on a similar timescale, a simple strategy to avoid navigational bias. DOI: http://dx.doi.org/10.7554/eLife.17227.001 PMID:27644113

Sedimentation dynamics and equilibrium profiles in multicomponent mixtures of colloidal particles.

PubMed

Spruijt, E; Biesheuvel, P M

2014-02-19

In this paper we give a general theoretical framework that describes the sedimentation of multicomponent mixtures of particles with sizes ranging from molecules to macroscopic bodies. Both equilibrium sedimentation profiles and the dynamic process of settling, or its converse, creaming, are modeled. Equilibrium profiles are found to be in perfect agreement with experiments. Our model reconciles two apparently contradicting points of view about buoyancy, thereby resolving a long-lived paradox about the correct choice of the buoyant density. On the one hand, the buoyancy force follows necessarily from the suspension density, as it relates to the hydrostatic pressure gradient. On the other hand, sedimentation profiles of colloidal suspensions can be calculated directly using the fluid density as apparent buoyant density in colloidal systems in sedimentation-diffusion equilibrium (SDE) as a result of balancing gravitational and thermodynamic forces. Surprisingly, this balance also holds in multicomponent mixtures. This analysis resolves the ongoing debate of the correct choice of buoyant density (fluid or suspension): both approaches can be used in their own domain. We present calculations of equilibrium sedimentation profiles and dynamic sedimentation that show the consequences of these insights. In bidisperse mixtures of colloids, particles with a lower mass density than the homogeneous suspension will first cream and then settle, whereas particles with a suspension-matched mass density form transient, bimodal particle distributions during sedimentation, which disappear when equilibrium is reached. In all these cases, the centers of the distributions of the particles with the lowest mass density of the two, regardless of their actual mass, will be located in equilibrium above the so-called isopycnic point, a natural consequence of their hard-sphere interactions. We include these interactions using the Boublik-Mansoori-Carnahan-Starling-Leland (BMCSL) equation of state. Finally, we demonstrate that our model is not limited to hard spheres, by extending it to charged spherical particles, and to dumbbells, trimers and short chains of connected beads.

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.

Dynamics of a pulsed laser generated tin plasma expanding in an oxygen atmosphere

NASA Astrophysics Data System (ADS)

Barreca, F.; Fazio, E.; Neri, F.; Barletta, E.; Trusso, S.; Fazio, B.

2005-10-01

Semiconducting tin oxide can be successfully deposited by means of the laser ablation technique. In particular by ablating metallic tin in a controlled oxygen atmosphere, thin films of SnOx have been deposited. The partial oxygen pressure at which the films are deposited strongly influences both the stoichiometry and the structural properties of the films. In this work, we present a study of the expansion dynamics of the plasma generated by ablating a tin target by means of a pulsed laser using time and space resolved optical emission spectroscopy and fast photography imaging of the expanding plasma. Both Sn I and Sn II optical emission lines have been observed from the time-integrated spectroscopy. Time resolved-measurements revealed the dynamics of the expanding plasma in the ambient oxygen atmosphere. Stoichiometry of the films has been determined by means of X-ray photoelectron spectroscopy and correlated to the expansion dynamics of the plasma.

Conflict and convention in dynamic networks.

PubMed

Foley, Michael; Forber, Patrick; Smead, Rory; Riedl, Christoph

2018-03-01

An important way to resolve games of conflict (snowdrift, hawk-dove, chicken) involves adopting a convention: a correlated equilibrium that avoids any conflict between aggressive strategies. Dynamic networks allow individuals to resolve conflict via their network connections rather than changing their strategy. Exploring how behavioural strategies coevolve with social networks reveals new dynamics that can help explain the origins and robustness of conventions. Here, we model the emergence of conventions as correlated equilibria in dynamic networks. Our results show that networks have the tendency to break the symmetry between the two conventional solutions in a strongly biased way. Rather than the correlated equilibrium associated with ownership norms (play aggressive at home, not away), we usually see the opposite host-guest norm (play aggressive away, not at home) evolve on dynamic networks, a phenomenon common to human interaction. We also show that learning to avoid conflict can produce realistic network structures in a way different than preferential attachment models. © 2017 The Author(s).

Time-resolved fluorescence microscopy to study biologically related applications using sol-gel derived and cellular media

NASA Astrophysics Data System (ADS)

Toury, Marion; Chandler, Lin; Allison, Archie; Campbell, David; McLoskey, David; Holmes-Smith, A. Sheila; Hungerford, Graham

2011-03-01

Fluorescence microscopy provides a non-invasive means for visualising dynamic protein interactions. As well as allowing the calculation of kinetic processes via the use of time-resolved fluorescence, localisation of the protein within cells or model systems can be monitored. These fluorescence lifetime images (FLIM) have become the preferred technique for elucidating protein dynamics due to the fact that the fluorescence lifetime is an absolute measure, in the main independent of fluorophore concentration and intensity fluctuations caused by factors such as photobleaching. In this work we demonstrate the use of a time-resolved fluorescence microscopy, employing a high repetition rate laser excitation source applied to study the influence of a metal surface on fluorescence tagged protein and to elucidate viscosity using the fluorescence lifetime probe DASPMI. These were studied in a cellular environment (yeast) and in a model system based on a sol-gel derived material, in which silver nanostructures were formed in situ using irradiation from a semiconductor laser in CW mode incorporated on a compact time-resolved fluorescence microscope (HORIBA Scientific DeltaDiode and DynaMyc).

Grain orientation effects on dynamic strength of FCC multicrystals at low shock pressures: a hydrodynamic instability study

DOE PAGES

Peralta, P.; Loomis, E.; Chen, Y.; ...

2015-04-09

Variability in local dynamic plasticity due to material anisotropy in polycrystalline metals is likely to be important on damage nucleation and growth at low pressures. Hydrodynamic instabilities could be used to study these plasticity effects by correlating measured changes in perturbation amplitudes at free surfaces to local plastic behaviour and grain orientation, but amplitude changes are typically too small to be measured reliably at low pressures using conventional diagnostics. Correlations between strength at low shock pressures and grain orientation were studied in copper (grain size ≈ 800 μm) using the Richtmyer–Meshkov instability with a square-wave surface perturbation (wavelength = 150 μm, amplitude = 5 μm), shocked at 2.7 GPa using symmetric plate impacts. A Plexiglas window was pressed against the peaks of the perturbation, keeping valleys as free surfaces. This produced perturbation amplitude changes much larger than those predicted without the window. Amplitude reductions from 64 to 88% were measured in recovered samples and grains oriented close tomore » $$\\langle$$0 0 1$$\\rangle$$ parallel to the shock had the largest final amplitude, whereas grains with shocks directions close to $$\\langle$$1 0 1$$\\rangle$$ had the lowest. Finite element simulations were performed with elastic-perfectly plastic models to estimate yield strengths leading lead to those final amplitudes. Anisotropic elasticity and these yield strengths were used to calculate the resolved shear stresses at yielding for the two orientations. In conclusion, results are compared with reports on orientation dependence of dynamic yielding in Cu single crystals and the higher values obtained suggest that strength estimations via hydrodynamic instabilities are sensitive to strain hardening and strain rate effects.« less

A Framework for Personalized Dynamic Cross-Selling in E-Commerce Retailing

ERIC Educational Resources Information Center

Timalsina, Arun Kumar

2012-01-01

Cross-selling and product bundling are prevalent strategies in the retail sector. Instead of static bundling offers, i.e. giving the same offer to everyone, personalized dynamic cross-selling generates targeted bundle offers and can help maximize revenues and profits. In resolving the two basic problems of dynamic cross-selling, which involves…

A hot tip: imaging phenomena using in situ multi-stimulus probes at high temperatures

NASA Astrophysics Data System (ADS)

Nonnenmann, Stephen S.

2016-02-01

Accurate high temperature characterization of materials remains a critical challenge to the continued advancement of various important energy, nuclear, electronic, and aerospace applications. Future experimental studies must assist these communities to progress past empiricism and derive deliberate, predictable designs of material classes functioning within active, extreme environments. Successful realization of systems ranging from fuel cells and batteries to electromechanical nanogenerators and turbines requires a dynamic understanding of the excitation, surface-mediated, and charge transfer phenomena which occur at heterophase interfaces (i.e. vapor-solid, liquid-solid, solid-solid) and impact overall performance. Advancing these frontiers therefore necessitates in situ (operando) characterization methods capable of resolving, both spatially and functionally, the coherence between these complex, collective excitations, and their respective response dynamics, through studies within the operating regime. This review highlights recent developments in scanning probe microscopy in performing in situ imaging at high elevated temperatures. The influence of and evolution from vacuum-based electron and tunneling microscopy are briefly summarized and discussed. The scope includes the use of high temperature imaging to directly observe critical phase transition, electronic, and electrochemical behavior under dynamic temperature settings, thus providing key physical parameters. Finally, both challenges and directions in combined instrumentation are proposed and discussed towards the end.

Differential Enzyme Flexibility Probed Using Solid-State Nanopores.

PubMed

Hu, Rui; Rodrigues, João V; Waduge, Pradeep; Yamazaki, Hirohito; Cressiot, Benjamin; Chishti, Yasmin; Makowski, Lee; Yu, Dapeng; Shakhnovich, Eugene; Zhao, Qing; Wanunu, Meni

2018-05-22

Enzymes and motor proteins are dynamic macromolecules that coexist in a number of conformations of similar energies. Protein function is usually accompanied by a change in structure and flexibility, often induced upon binding to ligands. However, while measuring protein flexibility changes between active and resting states is of therapeutic significance, it remains a challenge. Recently, our group has demonstrated that breadth of signal amplitudes in measured electrical signatures as an ensemble of individual protein molecules is driven through solid-state nanopores and correlates with protein conformational dynamics. Here, we extend our study to resolve subtle flexibility variation in dihydrofolate reductase mutants from unlabeled single molecules in solution. We first demonstrate using a canonical protein system, adenylate kinase, that both size and flexibility changes can be observed upon binding to a substrate that locks the protein in a closed conformation. Next, we investigate the influence of voltage bias and pore geometry on the measured electrical pulse statistics during protein transport. Finally, using the optimal experimental conditions, we systematically study a series of wild-type and mutant dihydrofolate reductase proteins, finding a good correlation between nanopore-measured protein conformational dynamics and equilibrium bulk fluorescence probe measurements. Our results unequivocally demonstrate that nanopore-based measurements reliably probe conformational diversity in native protein ensembles.

Efficient non-hydrostatic modelling of 3D wave-induced currents using a subgrid approach

NASA Astrophysics Data System (ADS)

Rijnsdorp, Dirk P.; Smit, Pieter B.; Zijlema, Marcel; Reniers, Ad J. H. M.

2017-08-01

Wave-induced currents are an ubiquitous feature in coastal waters that can spread material over the surf zone and the inner shelf. These currents are typically under resolved in non-hydrostatic wave-flow models due to computational constraints. Specifically, the low vertical resolutions adequate to describe the wave dynamics - and required to feasibly compute at the scales of a field site - are too coarse to account for the relevant details of the three-dimensional (3D) flow field. To describe the relevant dynamics of both wave and currents, while retaining a model framework that can be applied at field scales, we propose a two grid approach to solve the governing equations. With this approach, the vertical accelerations and non-hydrostatic pressures are resolved on a relatively coarse vertical grid (which is sufficient to accurately resolve the wave dynamics), whereas the horizontal velocities and turbulent stresses are resolved on a much finer subgrid (of which the resolution is dictated by the vertical scale of the mean flows). This approach ensures that the discrete pressure Poisson equation - the solution of which dominates the computational effort - is evaluated on the coarse grid scale, thereby greatly improving efficiency, while providing a fine vertical resolution to resolve the vertical variation of the mean flow. This work presents the general methodology, and discusses the numerical implementation in the SWASH wave-flow model. Model predictions are compared with observations of three flume experiments to demonstrate that the subgrid approach captures both the nearshore evolution of the waves, and the wave-induced flows like the undertow profile and longshore current. The accuracy of the subgrid predictions is comparable to fully resolved 3D simulations - but at much reduced computational costs. The findings of this work thereby demonstrate that the subgrid approach has the potential to make 3D non-hydrostatic simulations feasible at the scale of a realistic coastal region.

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.

Sensitivity of airborne geophysical data to sublacustrine and near-surface permafrost thaw

USGS Publications Warehouse

Minsley, Burke J.; Wellman, Tristan; Walvoord, Michelle Ann; Revil, Andre

2014-01-01

A coupled hydrogeophysical forward and inverse modeling approach is developed to illustrate the ability of frequency-domain airborne electromagnetic (AEM) data to characterize subsurface physical properties associated with sublacustrine permafrost thaw during lake-talik formation. Numerical modeling scenarios are evaluated that consider non-isothermal hydrologic responses to variable forcing from different lake depths and for different hydrologic gradients. A novel physical property relationship connects the dynamic distribution of electrical resistivity to ice saturation and temperature outputs from the SUTRA groundwater simulator with freeze–thaw physics. The influence of lithology on electrical resistivity is controlled by a surface conduction term in the physical property relationship. Resistivity models, which reflect changes in subsurface conditions, are used as inputs to simulate AEM data in order to explore the sensitivity of geophysical observations to permafrost thaw. Simulations of sublacustrine talik formation over a 1000-year period are modeled after conditions found in the Yukon Flats, Alaska. Synthetic AEM data are analyzed with a Bayesian Markov chain Monte Carlo algorithm that quantifies geophysical parameter uncertainty and resolution. Major lithological and permafrost features are well resolved by AEM data in the examples considered. The subtle geometry of partial ice saturation beneath lakes during talik formation cannot be resolved using AEM data, but the gross characteristics of sub-lake resistivity models reflect bulk changes in ice content and can identify the presence of a talik. A final synthetic example compares AEM and ground-based electromagnetic responses for their ability to resolve shallow permafrost and thaw features in the upper 1–2 m below ground outside the lake margin.

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.

4D blood flow mapping using SPIM-microPIV in the developing zebrafish heart

NASA Astrophysics Data System (ADS)

Zickus, Vytautas; Taylor, Jonathan M.

2018-02-01

Fluid-structure interaction in the developing heart is an active area of research in developmental biology. However, investigation of heart dynamics is mostly limited to computational uid dynamics simulations using heart wall structure information only, or single plane blood ow information - so there is a need for 3D + time resolved data to fully understand cardiac function. We present an imaging platform combining selective plane illumination microscopy (SPIM) with micro particle image velocimetry (μPIV) to enable 3D-resolved flow mapping in a microscopic environment, free from many of the sources of error and bias present in traditional epi uorescence-based μPIV systems. By using our new system in conjunction with optical heart beat synchronization, we demonstrate the ability obtain non-invasive 3D + time resolved blood flow measurements in the heart of a living zebrafish embryo.

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

Dou, Letian; Lai, Minliang; Kley, Christopher S.

Halide perovskites are promising semiconductor materials for solution-processed optoelectronic devices. Their strong ionic bonding nature results in highly dynamic crystal lattices, inherently allowing rapid ion exchange at the solid–vapor and solid–liquid interface. In this paper, we show that the anion-exchange chemistry can be precisely controlled in single-crystalline halide perovskite nanomaterials when combined with nanofabrication techniques. We demonstrate spatially resolved multicolor CsPbX 3 (X = Cl, Br, I, or alloy of two halides) nanowire heterojunctions with a pixel size down to 500 nm with the photoluminescence tunable over the entire visible spectrum. In addition, the heterojunctions show distinct electronic states acrossmore » the interface, as revealed by Kelvin probe force microscopy. Finally, these perovskite heterojunctions represent key building blocks for high-resolution multicolor displays beyond current state-of-the-art technology as well as high-density diode/transistor arrays.« less

Validation of Model Simulations of Anvil Cirrus Properties During TWP-ICE: Final Report

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

Zipser, Edward J.

2013-05-20

This 3-year grant, with two extensions, resulted in a successful 5-year effort, led by Ph.D. student Adam Varble, to compare cloud resolving model (CRM) simulations with the excellent database obtained during the TWP-ICE field campaign. The objective, largely achieved, is to undertake these comparisons comprehensively and quantitatively, informing the community in ways that goes beyond pointing out errors in the models, but points out ways to improve both cloud dynamics and microphysics parameterizations in future modeling efforts. Under DOE support, Adam Varble, with considerable assistance from Dr. Ann Fridlind and others, entrained scientists who ran some 10 different CRMs andmore » 4 different limited area models (LAMs) using a variety of microphysics parameterizations, to ensure that the conclusions of the study will have considerable generality.« less

Terrestrial Applications of a Nano-g Accelerometer

NASA Technical Reports Server (NTRS)

Hartley, Frank T.

1996-01-01

The ultra-sensitive accelerometer, developed for NASA to monitor the microgravity environments of Space Shuttle, five orbiters and Space Station, needed to measure accelerations up to 10 mg with an absolute accuracy of 10 nano-g (10(exp -8)g) for at least two orbits (10(exp 4) seconds) to resolve accelerations associated with orbital drag. Also, the accelerometers needed to have less than 10(exp -9) F.S. off-axis sensitivity; to be thermally and magnetically inert; to be immune to quiescent shock, and to have an in-situ calibration capability. Multi-axis compact seismometers, designs that have twelve decades of dynamic range will be described. Density profilometers, precision gradiometers, gyros and vibration isolation designs and applications will be discussed. Finally, examples of transformations of the accelerometer into sensitive anemometers and imaging spectrometers will be presented.

Cavitation erosion prediction based on analysis of flow dynamics and impact load spectra

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

Mihatsch, Michael S., E-mail: michael.mihatsch@aer.mw.tum.de; Schmidt, Steffen J.; Adams, Nikolaus A.

2015-10-15

Cavitation erosion is the consequence of repeated collapse-induced high pressure-loads on a material surface. The present paper assesses the prediction of impact load spectra of cavitating flows, i.e., the rate and intensity distribution of collapse events based on a detailed analysis of flow dynamics. Data are obtained from a numerical simulation which employs a density-based finite volume method, taking into account the compressibility of both phases, and resolves collapse-induced pressure waves. To determine the spectrum of collapse events in the fluid domain, we detect and quantify the collapse of isolated vapor structures. As reference configuration we consider the expansion ofmore » a liquid into a radially divergent gap which exhibits unsteady sheet and cloud cavitation. Analysis of simulation data shows that global cavitation dynamics and dominant flow events are well resolved, even though the spatial resolution is too coarse to resolve individual vapor bubbles. The inviscid flow model recovers increasingly fine-scale vapor structures and collapses with increasing resolution. We demonstrate that frequency and intensity of these collapse events scale with grid resolution. Scaling laws based on two reference lengths are introduced for this purpose. We show that upon applying these laws impact load spectra recorded on experimental and numerical pressure sensors agree with each other. Furthermore, correlation between experimental pitting rates and collapse-event rates is found. Locations of high maximum wall pressures and high densities of collapse events near walls obtained numerically agree well with areas of erosion damage in the experiment. The investigation shows that impact load spectra of cavitating flows can be inferred from flow data that captures the main vapor structures and wave dynamics without the need for resolving all flow scales.« less

Lifecycle of laser-produced air sparks

DOE PAGES

Harilal, S. S.; Brumfield, B. E.; Phillips, M. C.

2015-06-03

Here, we investigated the lifecycle of laser-generated air sparks or plasmas using multiple plasma diagnostic tools. The sparks were generated by focusing the fundamental radiation from an Nd:YAG laser in air, and studies included early and late time spark dynamics, decoupling of the shock wave from the plasma core, emission from the spark kernel, cold gas excitation by UV radiation, shock waves produced by the air spark, and the spark's final decay and turbulence formation. The shadowgraphic and self-emission images showed similar spark morphology at earlier and late times of its lifecycle; however, significant differences are seen in the midlifemore » images. Spectroscopic studies in the visible region showed intense blackbody-type radiation at early times followed by clearly resolved ionic, atomic, and molecular emission. The detected spectrum at late times clearly contained emission from both CN and N 2 +. Additional spectral features have been identified at late times due to emission from O and N atoms, indicating some degree of molecular dissociation and excitation. Detailed spatially and temporally resolved emission analysis provides insight about various physical mechanisms leading to molecular and atomic emission by air sparks, including spark plasma excitation, heating of cold air by UV radiation emitted by the spark, and shock-heating.« less

Velocity landscape correlation resolves multiple flowing protein populations from fluorescence image time series.

PubMed

Pandžić, Elvis; Abu-Arish, Asmahan; Whan, Renee M; Hanrahan, John W; Wiseman, Paul W

2018-02-16

Molecular, vesicular and organellar flows are of fundamental importance for the delivery of nutrients and essential components used in cellular functions such as motility and division. With recent advances in fluorescence/super-resolution microscopy modalities we can resolve the movements of these objects at higher spatio-temporal resolutions and with better sensitivity. Previously, spatio-temporal image correlation spectroscopy has been applied to map molecular flows by correlation analysis of fluorescence fluctuations in image series. However, an underlying assumption of this approach is that the sampled time windows contain one dominant flowing component. Although this was true for most of the cases analyzed earlier, in some situations two or more different flowing populations can be present in the same spatio-temporal window. We introduce an approach, termed velocity landscape correlation (VLC), which detects and extracts multiple flow components present in a sampled image region via an extension of the correlation analysis of fluorescence intensity fluctuations. First we demonstrate theoretically how this approach works, test the performance of the method with a range of computer simulated image series with varying flow dynamics. Finally we apply VLC to study variable fluxing of STIM1 proteins on microtubules connected to the plasma membrane of Cystic Fibrosis Bronchial Epithelial (CFBE) cells. Copyright © 2018 Elsevier Inc. All rights reserved.

V-T theory for the Self-Intermediate Scattering Function in a Monatomic Liquid

DOE PAGES

Wallace, Duane C.; Chisolm, Eric D.; De Lorenzi-Venneri, Giulia

2016-12-12

In V-T theory the atomic motion is harmonic vibrations in a liquid-specific potential energy valley, plus transits, which move the system rapidly among the multitude of such valleys. Here, in its first application to the self intermediate scattering function (SISF), V-T theory produced an accurate account of molecular dynamics (MD) data at all wave numbers q and time t. Recently, analysis of the mean square displacement (MSD) resolved a crossover behavior that was not observed in the SISF study. Our purpose here is to apply the more accurate MSD calibration to the SISF, and assess the results. We derive andmore » discuss the theoretical equations for vibrational and transit contributions to the SISF. The time evolution is divided into three successive intervals: the vibrational interval when the vibrational contribution alone accurately accounts for the MD data; the crossover when the vibrational contribution saturates and the transit contribution becomes resolved; and the diffusive interval when the transit contribution alone accurately accounts for the MD data. Finally, the resulting theoretical error is extremely small at all q and t. V-T theory is compared to mode-coupling theories for the MSD and SISF, and to recent developments in Brownian motion experiments and theory.« less

Lifecycle of laser-produced air sparks

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

Harilal, S. S., E-mail: hari@pnnl.gov; Brumfield, B. E.; Phillips, M. C.

2015-06-15

We investigated the lifecycle of laser-generated air sparks or plasmas using multiple plasma diagnostic tools. The sparks were generated by focusing the fundamental radiation from an Nd:YAG laser in air, and studies included early and late time spark dynamics, decoupling of the shock wave from the plasma core, emission from the spark kernel, cold gas excitation by UV radiation, shock waves produced by the air spark, and the spark's final decay and turbulence formation. The shadowgraphic and self-emission images showed similar spark morphology at earlier and late times of its lifecycle; however, significant differences are seen in the midlife images.more » Spectroscopic studies in the visible region showed intense blackbody-type radiation at early times followed by clearly resolved ionic, atomic, and molecular emission. The detected spectrum at late times clearly contained emission from both CN and N{sub 2}{sup +}. Additional spectral features have been identified at late times due to emission from O and N atoms, indicating some degree of molecular dissociation and excitation. Detailed spatially and temporally resolved emission analysis provides insight about various physical mechanisms leading to molecular and atomic emission by air sparks, including spark plasma excitation, heating of cold air by UV radiation emitted by the spark, and shock-heating.« less

A New Conflict Resolution Method for Multiple Mobile Robots in Cluttered Environments With Motion-Liveness.

PubMed

Shahriari, Mohammadali; Biglarbegian, Mohammad

2018-01-01

This paper presents a new conflict resolution methodology for multiple mobile robots while ensuring their motion-liveness, especially for cluttered and dynamic environments. Our method constructs a mathematical formulation in a form of an optimization problem by minimizing the overall travel times of the robots subject to resolving all the conflicts in their motion. This optimization problem can be easily solved through coordinating only the robots' speeds. To overcome the computational cost in executing the algorithm for very cluttered environments, we develop an innovative method through clustering the environment into independent subproblems that can be solved using parallel programming techniques. We demonstrate the scalability of our approach through performing extensive simulations. Simulation results showed that our proposed method is capable of resolving the conflicts of 100 robots in less than 1.23 s in a cluttered environment that has 4357 intersections in the paths of the robots. We also developed an experimental testbed and demonstrated that our approach can be implemented in real time. We finally compared our approach with other existing methods in the literature both quantitatively and qualitatively. This comparison shows while our approach is mathematically sound, it is more computationally efficient, scalable for very large number of robots, and guarantees the live and smooth motion of robots.

Spatially resolved estimation of ozone-related mortality in the United States under two representative concentration pathways (RCPs) and their uncertainty

DOE PAGES

Kim, Young-Min; Zhou, Ying; Gao, Yang; ...

2014-11-16

We report that the spatial pattern of the uncertainty in air pollution-related health impacts due to climate change has rarely been studied due to the lack of high-resolution model simulations, especially under the Representative Concentration Pathways (RCPs), the latest greenhouse gas emission pathways. We estimated future tropospheric ozone (O 3) and related excess mortality and evaluated the associated uncertainties in the continental United States under RCPs. Based on dynamically downscaled climate model simulations, we calculated changes in O 3 level at 12 km resolution between the future (2057 and 2059) and base years (2001–2004) under a low-to-medium emission scenario (RCP4.5)more » and a fossil fuel intensive emission scenario (RCP8.5). We then estimated the excess mortality attributable to changes in O 3. Finally, we analyzed the sensitivity of the excess mortality estimates to the input variables and the uncertainty in the excess mortality estimation using Monte Carlo simulations. O 3-related premature deaths in the continental U.S. were estimated to be 1312 deaths/year under RCP8.5 (95 % confidence interval (CI): 427 to 2198) and ₋2118 deaths/year under RCP4.5 (95 % CI: ₋3021 to ₋1216), when allowing for climate change and emissions reduction. The uncertainty of O 3-related excess mortality estimates was mainly caused by RCP emissions pathways. Finally, excess mortality estimates attributable to the combined effect of climate and emission changes on O 3 as well as the associated uncertainties vary substantially in space and so do the most influential input variables. Spatially resolved data is crucial to develop effective community level mitigation and adaptation policy.« less

Spatially resolved estimation of ozone-related mortality in the United States under two representative concentration pathways (RCPs) and their uncertainty

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

Kim, Young-Min; Zhou, Ying; Gao, Yang

We report that the spatial pattern of the uncertainty in air pollution-related health impacts due to climate change has rarely been studied due to the lack of high-resolution model simulations, especially under the Representative Concentration Pathways (RCPs), the latest greenhouse gas emission pathways. We estimated future tropospheric ozone (O 3) and related excess mortality and evaluated the associated uncertainties in the continental United States under RCPs. Based on dynamically downscaled climate model simulations, we calculated changes in O 3 level at 12 km resolution between the future (2057 and 2059) and base years (2001–2004) under a low-to-medium emission scenario (RCP4.5)more » and a fossil fuel intensive emission scenario (RCP8.5). We then estimated the excess mortality attributable to changes in O 3. Finally, we analyzed the sensitivity of the excess mortality estimates to the input variables and the uncertainty in the excess mortality estimation using Monte Carlo simulations. O 3-related premature deaths in the continental U.S. were estimated to be 1312 deaths/year under RCP8.5 (95 % confidence interval (CI): 427 to 2198) and ₋2118 deaths/year under RCP4.5 (95 % CI: ₋3021 to ₋1216), when allowing for climate change and emissions reduction. The uncertainty of O 3-related excess mortality estimates was mainly caused by RCP emissions pathways. Finally, excess mortality estimates attributable to the combined effect of climate and emission changes on O 3 as well as the associated uncertainties vary substantially in space and so do the most influential input variables. Spatially resolved data is crucial to develop effective community level mitigation and adaptation policy.« less

Multimodal Kelvin Probe Force Microscopy Investigations of a Photovoltaic WSe2/MoS2 Type-II Interface.

PubMed

Almadori, Yann; Bendiab, Nedjma; Grévin, Benjamin

2018-01-10

Atomically thin transition-metal dichalcogenides (TMDC) have become a new platform for the development of next-generation optoelectronic and light-harvesting devices. Here, we report a Kelvin probe force microscopy (KPFM) investigation carried out on a type-II photovoltaic heterojunction based on WSe 2 monolayer flakes and a bilayer MoS 2 film stacked in vertical configuration on a Si/SiO 2 substrate. Band offset characterized by a significant interfacial dipole is pointed out at the WSe 2 /MoS 2 vertical junction. The photocarrier generation process and phototransport are studied by applying a differential technique allowing to map directly two-dimensional images of the surface photovoltage (SPV) over the vertical heterojunctions (vHJ) and in its immediate vicinity. Differential SPV reveals the impact of chemical defects on the photocarrier generation and that negative charges diffuse in the MoS 2 a few hundreds of nanometers away from the vHJ. The analysis of the SPV data confirms unambiguously that light absorption results in the generation of free charge carriers that do not remain coulomb-bound at the type-II interface. A truly quantitative determination of the electron-hole (e-h) quasi-Fermi levels splitting (i.e., the open-circuit voltage) is achieved by measuring the differential vacuum-level shift over the WSe 2 flakes and the MoS 2 layer. The dependence of the energy-level splitting as a function of the optical power reveals that Shockley-Read-Hall processes significantly contribute to the interlayer recombination dynamics. Finally, a newly developed time-resolved mode of the KPFM is applied to map the SPV decay time constants. The time-resolved SPV images reveal the dynamics of delayed recombination processes originating from photocarriers trapping at the SiO 2 /TMDC interfaces.

Low Frequency Predictive Skill Despite Structural Instability and Model Error

DTIC Science & Technology

2014-09-30

Majda, based on earlier theoretical work. 1. Dynamic Stochastic Superresolution of sparseley observed turbulent systems M. Branicki (Post doc...of numerical models. Here, we introduce and study a suite of general Dynamic Stochastic Superresolution (DSS) algorithms and show that, by...resolving subgridscale turbulence through Dynamic Stochastic Superresolution utilizing aliased grids is a potential breakthrough for practical online

Observing Holliday junction branch migration one step at a time

NASA Astrophysics Data System (ADS)

Ha, Taekjip

2004-03-01

During genetic recombination, two homologous DNA molecules undergo strand exchange to form a four-way DNA (Holliday) junction and the recognition and processing of this species by branch migration and junction resolving enzymes determine the outcome. We have used single molecule fluorescence techniques to study two intrinsic structural dynamics of the Holliday junction, stacking conformer transitions and spontaneous branch migration. Our studies show that the dynamics of branch migration, resolved with one base pair resolution, is determined by the stability of conformers which in turn depends on the local DNA sequences. Therefore, the energy landscape of Holliday junction branch migation is not uniform, but is rugged.

Resolving Nonadiabatic Dynamics of Hydrated Electrons Using Ultrafast Photoemission Anisotropy.

PubMed

Karashima, Shutaro; Yamamoto, Yo-Ichi; Suzuki, Toshinori

2016-04-01

We have studied ultrafast nonadiabatic dynamics of excess electrons trapped in the band gap of liquid water using time- and angle-resolved photoemission spectroscopy. Anisotropic photoemission from the first excited state was discovered, which enabled unambiguous identification of nonadiabatic transition to the ground state in 60 fs in H_{2}O and 100 fs in D_{2}O. The photoelectron kinetic energy distribution exhibited a rapid spectral shift in ca. 20 fs, which is ascribed to the librational response of a hydration shell to electronic excitation. Photoemission anisotropy indicates that the electron orbital in the excited state is depolarized in less than 40 fs.

Understanding Unimer Exchange Processes in Block Copolymer Micelles using NMR Diffusometry, Time-Resolved NMR, and SANS

NASA Astrophysics Data System (ADS)

Madsen, Louis; Kidd, Bryce; Li, Xiuli; Miller, Katherine; Cooksey, Tyler; Robertson, Megan

Our team seeks to understand dynamic behaviors of block copolymer micelles and their interplay with encapsulated cargo molecules. Quantifying unimer and cargo exchange rates micelles can provide critical information for determining mechanisms of unimer exchange as well as designing systems for specific cargo release dynamics. We are exploring the utility of NMR spectroscopy and diffusometry techniques as complements to existing SANS and fluorescence methods. One promising new method involves time-resolved NMR spin relaxation measurements, wherein mixing of fully protonated and 2H-labeled PEO-b-PCL micelles solutions shows an increase in spin-lattice relaxation time (T1) with time after mixing. This is due to a weakening in magnetic environment surrounding 1H spins as 2H-bearing unimers join fully protonated micelles. We are measuring time constants for unimer exchange of minutes to hours, and we expect to resolve times of <1 min. This method can work on any solution NMR spectrometer and with minimal perturbation to chemical structure (as in dye-labelled fluorescence methods). Multimodal NMR can complement existing characterization tools, expanding and accelerating dynamics measurements for polymer micelle, nanogel, and nanoparticle developers.

Time-resolved methods in biophysics. 7. Photon counting vs. analog time-resolved singlet oxygen phosphorescence detection.

PubMed

Jiménez-Banzo, Ana; Ragàs, Xavier; Kapusta, Peter; Nonell, Santi

2008-09-01

Two recent advances in optoelectronics, namely novel near-IR sensitive photomultipliers and inexpensive yet powerful diode-pumped solid-state lasers working at kHz repetition rate, enable the time-resolved detection of singlet oxygen (O2(a1Deltag)) phosphorescence in photon counting mode, thereby boosting the time-resolution, sensitivity, and dynamic range of this well-established detection technique. Principles underlying this novel approach and selected examples of applications are provided in this perspective, which illustrate the advantages over the conventional analog detection mode.

Consent Agreement and [Proposed] Final Order: N.F. Kawakami Store Ltd.

EPA Pesticide Factsheets

Consent Agreement and [Proposed] Final Order between the EPA Region 9, and N.F. Kawakami Store Ltd. to resolve a civil administrative proceeding under Sections 1423(c)(3)(B) of the Safe Drinking Water Act. Docket No. UIC-09-2018-0003.

Two-site ionic labeling with pyranine: implications for structural dynamics studies of polymers and polypeptides by time-resolved fluorescence anisotropy.

PubMed

Sharma, Jai; Tleugabulova, Dina; Czardybon, Wojciech; Brennan, John D

2006-04-26

Time-resolved fluorescence anisotropy (TRFA) is widely used to study dynamic motions of biomolecules in a variety of environments. However, depolarization due to rapid side chain motions often complicates the interpretation of anisotropy decay data and interferes with the accurate observation of segmental motions. Here, we demonstrate a new method for two-point ionic labeling of polymers and biomolecules that have appropriately spaced amino groups using the fluorescent probe 8-hydroxyl-1,3,6-trisulfonated pyrene (pyranine). TRFA analysis shows that such labeling provides a more rigid attachment of the fluorophore to the macromolecule than the covalent or single-point ionic labeling of amino groups, leading to time-resolved anisotropy decays that better reflect the backbone motion of the labeled polymer segment. Optimal coupling of pyranine to biomolecule dynamics is shown to be obtained for appropriately spaced Arg groups, and in such cases the ionic binding is stable up to 150 mM ionic strength. TRFA was used to monitor the behavior of pyranine-labeled poly(allylamine) (PAM) and poly-d-lysine (PL) in sodium silicate derived sol-gel materials and revealed significant restriction of backbone motion upon entrapment for both polymers, an observation that was not readily apparent in a previous study with entrapped fluorescein-labeled PAM and PL. The implications of these findings for fluorescence studies of polymer and biomolecule dynamics are discussed.

Density relaxation and particle motion characteristics in a non-ionic deep eutectic solvent (acetamide + urea): time-resolved fluorescence measurements and all-atom molecular dynamics simulations.

PubMed

Das, Anuradha; Das, Suman; Biswas, Ranjit

2015-01-21

Temperature dependent relaxation dynamics, particle motion characteristics, and heterogeneity aspects of deep eutectic solvents (DESs) made of acetamide (CH3CONH2) and urea (NH2CONH2) have been investigated by employing time-resolved fluorescence measurements and all-atom molecular dynamics simulations. Three different compositions (f) for the mixture [fCH3CONH2 + (1 - f)NH2CONH2] have been studied in a temperature range of 328-353 K which is ∼120-145 K above the measured glass transition temperatures (∼207 K) of these DESs but much lower than the individual melting temperature of either of the constituents. Steady state fluorescence emission measurements using probe solutes with sharply different lifetimes do not indicate any dependence on excitation wavelength in these metastable molten systems. Time-resolved fluorescence anisotropy measurements reveal near-hydrodynamic coupling between medium viscosity and rotation of a dissolved dipolar solute. Stokes shift dynamics have been found to be too fast to be detected by the time-resolution (∼70 ps) employed, suggesting extremely rapid medium polarization relaxation. All-atom simulations reveal Gaussian distribution for particle displacements and van Hove correlations, and significant overlap between non-Gaussian (α2) and new non-Gaussian (γ) heterogeneity parameters. In addition, no stretched exponential relaxations have been detected in the simulated wavenumber dependent acetamide dynamic structure factors. All these results are in sharp contrast to earlier observations for ionic deep eutectics with acetamide [Guchhait et al., J. Chem. Phys. 140, 104514 (2014)] and suggest a fundamental difference in interaction and dynamics between ionic and non-ionic deep eutectic solvent systems.

Density relaxation and particle motion characteristics in a non-ionic deep eutectic solvent (acetamide + urea): Time-resolved fluorescence measurements and all-atom molecular dynamics simulations

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

Das, Anuradha; Das, Suman; Biswas, Ranjit, E-mail: ranjit@bose.res.in

2015-01-21

Temperature dependent relaxation dynamics, particle motion characteristics, and heterogeneity aspects of deep eutectic solvents (DESs) made of acetamide (CH{sub 3}CONH{sub 2}) and urea (NH{sub 2}CONH{sub 2}) have been investigated by employing time-resolved fluorescence measurements and all-atom molecular dynamics simulations. Three different compositions (f) for the mixture [fCH{sub 3}CONH{sub 2} + (1 − f)NH{sub 2}CONH{sub 2}] have been studied in a temperature range of 328-353 K which is ∼120-145 K above the measured glass transition temperatures (∼207 K) of these DESs but much lower than the individual melting temperature of either of the constituents. Steady state fluorescence emission measurements using probemore » solutes with sharply different lifetimes do not indicate any dependence on excitation wavelength in these metastable molten systems. Time-resolved fluorescence anisotropy measurements reveal near-hydrodynamic coupling between medium viscosity and rotation of a dissolved dipolar solute. Stokes shift dynamics have been found to be too fast to be detected by the time-resolution (∼70 ps) employed, suggesting extremely rapid medium polarization relaxation. All-atom simulations reveal Gaussian distribution for particle displacements and van Hove correlations, and significant overlap between non-Gaussian (α{sub 2}) and new non-Gaussian (γ) heterogeneity parameters. In addition, no stretched exponential relaxations have been detected in the simulated wavenumber dependent acetamide dynamic structure factors. All these results are in sharp contrast to earlier observations for ionic deep eutectics with acetamide [Guchhait et al., J. Chem. Phys. 140, 104514 (2014)] and suggest a fundamental difference in interaction and dynamics between ionic and non-ionic deep eutectic solvent systems.« less

Density relaxation and particle motion characteristics in a non-ionic deep eutectic solvent (acetamide + urea): Time-resolved fluorescence measurements and all-atom molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Das, Anuradha; Das, Suman; Biswas, Ranjit

2015-01-01

Temperature dependent relaxation dynamics, particle motion characteristics, and heterogeneity aspects of deep eutectic solvents (DESs) made of acetamide (CH3CONH2) and urea (NH2CONH2) have been investigated by employing time-resolved fluorescence measurements and all-atom molecular dynamics simulations. Three different compositions (f) for the mixture [fCH3CONH2 + (1 - f)NH2CONH2] have been studied in a temperature range of 328-353 K which is ˜120-145 K above the measured glass transition temperatures (˜207 K) of these DESs but much lower than the individual melting temperature of either of the constituents. Steady state fluorescence emission measurements using probe solutes with sharply different lifetimes do not indicate any dependence on excitation wavelength in these metastable molten systems. Time-resolved fluorescence anisotropy measurements reveal near-hydrodynamic coupling between medium viscosity and rotation of a dissolved dipolar solute. Stokes shift dynamics have been found to be too fast to be detected by the time-resolution (˜70 ps) employed, suggesting extremely rapid medium polarization relaxation. All-atom simulations reveal Gaussian distribution for particle displacements and van Hove correlations, and significant overlap between non-Gaussian (α2) and new non-Gaussian (γ) heterogeneity parameters. In addition, no stretched exponential relaxations have been detected in the simulated wavenumber dependent acetamide dynamic structure factors. All these results are in sharp contrast to earlier observations for ionic deep eutectics with acetamide [Guchhait et al., J. Chem. Phys. 140, 104514 (2014)] and suggest a fundamental difference in interaction and dynamics between ionic and non-ionic deep eutectic solvent systems.

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

NASA Astrophysics Data System (ADS)

Ponseca, C. S., Jr.; Sundström, V.

2016-03-01

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

Impact of doping on the carrier dynamics in graphene

PubMed Central

Kadi, Faris; Winzer, Torben; Knorr, Andreas; Malic, Ermin

2015-01-01

We present a microscopic study on the impact of doping on the carrier dynamics in graphene, in particular focusing on its influence on the technologically relevant carrier multiplication in realistic, doped graphene samples. Treating the time- and momentum-resolved carrier-light, carrier-carrier, and carrier-phonon interactions on the same microscopic footing, the appearance of Auger-induced carrier multiplication up to a Fermi level of 300 meV is revealed. Furthermore, we show that doping favors the so-called hot carrier multiplication occurring within one band. Our results are directly compared to recent time-resolved ARPES measurements and exhibit an excellent agreement on the temporal evolution of the hot carrier multiplication for n- and p-doped graphene. The gained insights shed light on the ultrafast carrier dynamics in realistic, doped graphene samples. PMID:26577536

Examination of laser microbeam cell lysis in a PDMS microfluidic channel using time-resolved imaging

PubMed Central

Quinto-Su, Pedro A.; Lai, Hsuan-Hong; Yoon, Helen H.; Sims, Christopher E.; Allbritton, Nancy L.; Venugopalan, Vasan

2008-01-01

We use time-resolved imaging to examine the lysis dynamics of non-adherent BAF-3 cells within a microfluidic channel produced by the delivery of single highly-focused 540 ps duration laser pulses at λ = 532 nm. Time-resolved bright-field images reveal that the delivery of the pulsed laser microbeam results in the formation of a laser-induced plasma followed by shock wave emission and cavitation bubble formation. The confinement offered by the microfluidic channel constrains substantially the cavitation bubble expansion and results in significant deformation of the PDMS channel walls. To examine the cell lysis and dispersal of the cellular contents, we acquire time-resolved fluorescence images of the process in which the cells were loaded with a fluorescent dye. These fluorescence images reveal cell lysis to occur on the nanosecond to microsecond time scale by the plasma formation and cavitation bubble dynamics. Moreover, the time-resolved fluorescence images show that while the cellular contents are dispersed by the expansion of the laser-induced cavitation bubble, the flow associated with the bubble collapse subsequently re-localizes the cellular contents to a small region. This capacity of pulsed laser microbeam irradiation to achieve rapid cell lysis in microfluidic channels with minimal dilution of the cellular contents has important implications for their use in lab-on-a-chip applications. PMID:18305858

Femtosecond-resolved ablation dynamics of Si in the near field of a small dielectric particle

PubMed Central

Kühler, Paul; Puerto, Daniel; Mosbacher, Mario; Leiderer, Paul; Garcia de Abajo, Francisco Javier

2013-01-01

Summary In this work we analyze the ablation dynamics of crystalline Si in the intense near field generated by a small dielectric particle located at the material surface when being irradiated with an infrared femtosecond laser pulse (800 nm, 120 fs). The presence of the particle (7.9 μm diameter) leads to a strong local enhancement (ca. 40 times) of the incoming intensity of the pulse. The transient optical response of the material has been analyzed by means of fs-resolved optical microscopy in reflection configuration over a time span from 0.1 ps to about 1 ns. Characteristic phenomena like electron plasma formation, ultrafast melting and ablation, along with their characteristic time scales are observed in the region surrounding the particle. The use of a time resolved imaging technique allows us recording simultaneously the material response at ordinary and large peak power densities enabling a direct comparison between both scenarios. The time resolved images of near field exposed regions are consistent with a remarkable temporal shift of the ablation onset which occurs in the sub-picosend regime, from about 500 to 800 fs after excitation. PMID:24062976

Extreme scale multi-physics simulations of the tsunamigenic 2004 Sumatra megathrust earthquake

NASA Astrophysics Data System (ADS)

Ulrich, T.; Gabriel, A. A.; Madden, E. H.; Wollherr, S.; Uphoff, C.; Rettenberger, S.; Bader, M.

2017-12-01

SeisSol (www.seissol.org) is an open-source software package based on an arbitrary high-order derivative Discontinuous Galerkin method (ADER-DG). It solves spontaneous dynamic rupture propagation on pre-existing fault interfaces according to non-linear friction laws, coupled to seismic wave propagation with high-order accuracy in space and time (minimal dispersion errors). SeisSol exploits unstructured meshes to account for complex geometries, e.g. high resolution topography and bathymetry, 3D subsurface structure, and fault networks. We present the up-to-date largest (1500 km of faults) and longest (500 s) dynamic rupture simulation modeling the 2004 Sumatra-Andaman earthquake. We demonstrate the need for end-to-end-optimization and petascale performance of scientific software to realize realistic simulations on the extreme scales of subduction zone earthquakes: Considering the full complexity of subduction zone geometries leads inevitably to huge differences in element sizes. The main code improvements include a cache-aware wave propagation scheme and optimizations of the dynamic rupture kernels using code generation. In addition, a novel clustered local-time-stepping scheme for dynamic rupture has been established. Finally, asynchronous output has been implemented to overlap I/O and compute time. We resolve the frictional sliding process on the curved mega-thrust and a system of splay faults, as well as the seismic wave field and seafloor displacement with frequency content up to 2.2 Hz. We validate the scenario by geodetic, seismological and tsunami observations. The resulting rupture dynamics shed new light on the activation and importance of splay faults.

Inference of physical/biological dynamics from synthetic ocean colour images

NASA Technical Reports Server (NTRS)

Eert, J.; Holloway, G.; Gower, J. F. R.; Denman, K.; Abbott, M.

1987-01-01

High resolution numerical experiments with well resolved eddies are performed including advection of a biologically active plankton field. Shelf wave propagation and bottom topographic features are included. The resulting synthetic ocean color fields are examined for sensitivity to the (known) underlying physical dynamics.

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

Capturing Structural Dynamics in Crystalline Silicon Using Chirped Electrons from a Laser Wakefield Accelerator

PubMed Central

He, Z.-H.; Beaurepaire, B.; Nees, J. A.; Gallé, G.; Scott, S. A.; Pérez, J. R. Sánchez; Lagally, M. G.; Krushelnick, K.; Thomas, A. G. R.; Faure, J.

2016-01-01

Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scale by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes. PMID:27824086

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

Time-resolved observation of protein allosteric communication

PubMed Central

Buchenberg, Sebastian; Sittel, Florian; Stock, Gerhard

2017-01-01

Allostery represents a fundamental mechanism of biological regulation that is mediated via long-range communication between distant protein sites. Although little is known about the underlying dynamical process, recent time-resolved infrared spectroscopy experiments on a photoswitchable PDZ domain (PDZ2S) have indicated that the allosteric transition occurs on multiple timescales. Here, using extensive nonequilibrium molecular dynamics simulations, a time-dependent picture of the allosteric communication in PDZ2S is developed. The simulations reveal that allostery amounts to the propagation of structural and dynamical changes that are genuinely nonlinear and can occur in a nonlocal fashion. A dynamic network model is constructed that illustrates the hierarchy and exceeding structural heterogeneity of the process. In compelling agreement with experiment, three physically distinct phases of the time evolution are identified, describing elastic response (≲0.1 ns), inelastic reorganization (∼100 ns), and structural relaxation (≳1μs). Issues such as the similarity to downhill folding as well as the interpretation of allosteric pathways are discussed. PMID:28760989

Capturing Structural Dynamics in Crystalline Silicon Using Chirped Electrons from a Laser Wakefield Accelerator

DOE PAGES

He, Z. -H.; Beaurepaire, B.; Nees, J. A.; ...

2016-11-08

Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here in this paper, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scalemore » by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes.« less

Picosecond Thermal Dynamics in an Underdense Plasma Measured with Thomson Scattering

NASA Astrophysics Data System (ADS)

Haberberger, D.; Katz, J.; Bucht, S.; Davies, A.; Bromage, J.; Zuegel, J. D.; Froula, D. H.; Trines, R.; Bingham, R.; Sadler, J.; Norreys, P. A.

2017-10-01

Field-ionized underdense plasmas have many promising applications within the laser-plasma interaction field: nuclear fusion, particle accelerators, x-ray sources, and laser-plasma amplification. Having complete knowledge of the plasma dynamics is essential to establishing optimal parameters for a given application. Here picosecond-resolved Thomson scattering measurements have been used to determine the electron thermal dynamics of an underdense ( 1019/cm) H2 plasma irradiated by a 60-ps, 1053-nm laser pulse with an intensity of 2 × 1014 W/cm2. The picosecond-resolved spectra were obtained with a novel pulse-front tilt compensated streaked optical spectrometer. The electron temperature was observed to rise from an initial 5 eV to a density-dependent plateau in 23 ps. Simulation results indicate that inverse bremsstrahlung heating, radiative cooling, and radial conduction cooling all play an important role in modeling the thermal dynamics. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

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.

Massive black hole and gas dynamics in galaxy nuclei mergers - I. Numerical implementation

NASA Astrophysics Data System (ADS)

Lupi, Alessandro; Haardt, Francesco; Dotti, Massimo

2015-01-01

Numerical effects are known to plague adaptive mesh refinement (AMR) codes when treating massive particles, e.g. representing massive black holes (MBHs). In an evolving background, they can experience strong, spurious perturbations and then follow unphysical orbits. We study by means of numerical simulations the dynamical evolution of a pair MBHs in the rapidly and violently evolving gaseous and stellar background that follows a galaxy major merger. We confirm that spurious numerical effects alter the MBH orbits in AMR simulations, and show that numerical issues are ultimately due to a drop in the spatial resolution during the simulation, drastically reducing the accuracy in the gravitational force computation. We therefore propose a new refinement criterion suited for massive particles, able to solve in a fast and precise way for their orbits in highly dynamical backgrounds. The new refinement criterion we designed enforces the region around each massive particle to remain at the maximum resolution allowed, independently upon the local gas density. Such maximally resolved regions then follow the MBHs along their orbits, and effectively avoids all spurious effects caused by resolution changes. Our suite of high-resolution, AMR hydrodynamic simulations, including different prescriptions for the sub-grid gas physics, shows that the new refinement implementation has the advantage of not altering the physical evolution of the MBHs, accounting for all the non-trivial physical processes taking place in violent dynamical scenarios, such as the final stages of a galaxy major merger.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches.

PubMed

Antipov, Sergey V; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2017-11-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research "Molecular Ultrafast Science and Technology," are presented: These include Bohmian dynamics description of the collision of H with H 2 , local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches

PubMed Central

Antipov, Sergey V.; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2018-01-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research “Molecular Ultrafast Science and Technology,” are presented: These include Bohmian dynamics description of the collision of H with H2, local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase. PMID:29376107

Ultrafast Structural Dynamics in Combustion Relevant Model Systems

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

Weber, Peter M.

2014-03-31

The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energymore » of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or excited valence states is measured by inducing the dynamics using a near UV laser pulse, and employing a multi-photon ionization scheme via the Rydberg states as a probe process. Thus, the technique is capable of measuring the reaction dynamics in any electronic state of neutral molecules.« less

State-resolved three-dimensional electron-momentum correlation in nonsequential double ionization of benzene

NASA Astrophysics Data System (ADS)

Winney, Alexander H.; Lin, Yun Fei; Lee, Suk Kyoung; Adhikari, Pradip; Li, Wen

2016-03-01

We report state-resolved electron-momentum correlation measurement of strong-field nonsequential double ionization in benzene. With a novel coincidence detection apparatus, highly efficient triple coincidence (electron-electron dication) and quadruple coincidence (electron-electron-cation-cation) are used to resolve the final ionic states and to characterize three-dimensional (3D) electron-momentum correlation. The primary states associated with dissociative and nondissociative dications are assigned. A 3D momentum anticorrelation is observed for the electrons in coincidence with dissociative benzene dication states whereas such a correlation is absent for nondissociative dication states.

Constraining earthquake source inversions with GPS data: 1. Resolution-based removal of artifacts

USGS Publications Warehouse

Page, M.T.; Custodio, S.; Archuleta, R.J.; Carlson, J.M.

2009-01-01

We present a resolution analysis of an inversion of GPS data from the 2004 Mw 6.0 Parkfield earthquake. This earthquake was recorded at thirteen 1-Hz GPS receivers, which provides for a truly coseismic data set that can be used to infer the static slip field. We find that the resolution of our inverted slip model is poor at depth and near the edges of the modeled fault plane that are far from GPS receivers. The spatial heterogeneity of the model resolution in the static field inversion leads to artifacts in poorly resolved areas of the fault plane. These artifacts look qualitatively similar to asperities commonly seen in the final slip models of earthquake source inversions, but in this inversion they are caused by a surplus of free parameters. The location of the artifacts depends on the station geometry and the assumed velocity structure. We demonstrate that a nonuniform gridding of model parameters on the fault can remove these artifacts from the inversion. We generate a nonuniform grid with a grid spacing that matches the local resolution length on the fault and show that it outperforms uniform grids, which either generate spurious structure in poorly resolved regions or lose recoverable information in well-resolved areas of the fault. In a synthetic test, the nonuniform grid correctly averages slip in poorly resolved areas of the fault while recovering small-scale structure near the surface. Finally, we present an inversion of the Parkfield GPS data set on the nonuniform grid and analyze the errors in the final model. Copyright 2009 by the American Geophysical Union.

Population Pulsation Resonances of Excitons in Monolayer MoSe 2 with Sub-1 μeV Linewidths

DOE PAGES

Schaibley, John R.; Karin, Todd; Yu, Hongyi; ...

2015-04-01

Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. In this paper, we investigate exciton relaxation in monolayer MoSe 2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 and <0.2 μeV at low temperature. These linewidths are more than 3 orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on time scalesmore » longer than 1 ns. Finally, the ultranarrow resonance (<0.2 μeV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.« less

Weak ergodicity of population evolution processes.

PubMed

Inaba, H

1989-10-01

The weak ergodic theorems of mathematical demography state that the age distribution of a closed population is asymptotically independent of the initial distribution. In this paper, we provide a new proof of the weak ergodic theorem of the multistate population model with continuous time. The main tool to attain this purpose is a theory of multiplicative processes, which was mainly developed by Garrett Birkhoff, who showed that ergodic properties generally hold for an appropriate class of multiplicative processes. First, we construct a general theory of multiplicative processes on a Banach lattice. Next, we formulate a dynamical model of a multistate population and show that its evolution operator forms a multiplicative process on the state space of the population. Subsequently, we investigate a sufficient condition that guarantees the weak ergodicity of the multiplicative process. Finally, we prove the weak and strong ergodic theorems for the multistate population and resolve the consistency problem.

Laser shocking of materials: Toward the national ignition facility

DOE PAGES

Meyers, M. A.; Remington, B. A.; Maddox, B.; ...

2010-01-16

In recent years a powerful experimental tool has been added to the arsenal at the disposal of the materials scientist investigating materials response at extreme regimes of strain rates, temperatures, and pressures: laser compression. In this paper, this technique has been applied successfully to mono-, poly-, and nanocrystalline metals and the results have been compared with predictions from analytical models and molecular dynamics simulations. Special flash x-ray radiography and flash x-ray diffraction, combined with laser shock propagation, are yielding the strength of metals at strain rates on the order of 10 7–10 8 s -1 and resolving details of themore » kinetics of phase transitions. A puzzling result is that experiments, analysis, and simulations predict dislocation densities that are off by orders of magnitude. Finally, other surprises undoubtedly await us as we explore even higher pressure/strain rate/temperature regimes enabled by the National Ignition Facility.« less

Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

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

Fang, Yin; Jiang, Yuanwen; Cherukara, Mathew J.

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similarmore » to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.« less

Spatial resolution of the electrical conductance of ionic fluids using a Green-Kubo method.

PubMed

Jones, R E; Ward, D K; Templeton, J A

2014-11-14

We present a Green-Kubo method to spatially resolve transport coefficients in compositionally heterogeneous mixtures. We develop the underlying theory based on well-known results from mixture theory, Irving-Kirkwood field estimation, and linear response theory. Then, using standard molecular dynamics techniques, we apply the methodology to representative systems. With a homogeneous salt water system, where the expectation of the distribution of conductivity is clear, we demonstrate the sensitivities of the method to system size, and other physical and algorithmic parameters. Then we present a simple model of an electrochemical double layer where we explore the resolution limit of the method. In this system, we observe significant anisotropy in the wall-normal vs. transverse ionic conductances, as well as near wall effects. Finally, we discuss extensions and applications to more realistic systems such as batteries where detailed understanding of the transport properties in the vicinity of the electrodes is of technological importance.

Investigation of laser induced breakdown in liquid nitromethane using nanosecond shadowgraphy

NASA Astrophysics Data System (ADS)

Guo, Wencan; Zheng, Xianxu; Yu, Guoyang; Zhao, Jun; Zeng, Yangyang; Liu, Cangli

2016-09-01

A nanosecond time-resolved shadowgraphy is performed to observe a laser-induced breakdown in nitromethane. The digital delays are introduced between a pump beam and an illumination light to achieve a measuring range from 40 ns to 100 ms, which enable us to study the shock wave propagation, bubble dynamics, and other process of the laser-induced breakdown. Compared with distilled water, there are two obvious differences observed in nitromethane: (1) the production of a non-evaporative gas at the final stage, and (2) an absence of the secondary shock wave after the first collapse of the bubble. We also calculated the bubble energy in nitromethane and distilled water under a different incident energy. The results indicate that the bubble energy in nitromethane is more than twice as large as that in water. It is suggested that chemical reactions contribute to the releasing of energy.

Double-shot MeV electron diffraction and microscopy

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

Musumeci, P.; Cesar, D.; Maxson, J.

Here in this paper, we study by numerical simulations a time-resolved MeV electron scattering mode where two consecutive electron pulses are used to capture the evolution of a material sample on 10 ps time scales. The two electron pulses are generated by illuminating a photocathode in a radiofrequency photogun by two short laser pulses with adjustable delay. A streak camera/deflecting cavity is used after the sample to project the two electron bunches on two well separated regions of the detector screen. By using sufficiently short pulses, the 2D spatial information from each snapshot can be preserved. This “double-shot” technique enablesmore » the efficient capture of irreversible dynamics in both diffraction and imaging modes. Finally, in this work, we demonstrate both modes in start-to-end simulations of the UCLA Pegasus MeV microscope column.« less

Double-shot MeV electron diffraction and microscopy

DOE PAGES

Musumeci, P.; Cesar, D.; Maxson, J.

2017-05-19

Here in this paper, we study by numerical simulations a time-resolved MeV electron scattering mode where two consecutive electron pulses are used to capture the evolution of a material sample on 10 ps time scales. The two electron pulses are generated by illuminating a photocathode in a radiofrequency photogun by two short laser pulses with adjustable delay. A streak camera/deflecting cavity is used after the sample to project the two electron bunches on two well separated regions of the detector screen. By using sufficiently short pulses, the 2D spatial information from each snapshot can be preserved. This “double-shot” technique enablesmore » the efficient capture of irreversible dynamics in both diffraction and imaging modes. Finally, in this work, we demonstrate both modes in start-to-end simulations of the UCLA Pegasus MeV microscope column.« less

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

Pandey, Ravindra; Usui, Kota; Livingstone, Ruth A.

Ice-nucleating organisms play important roles in the environment. With their ability to induce ice formation at temperatures just below the ice melting point, bacteria such as Pseudomonas syringae attack plants through frost damage using specialized ice-nucleating proteins. Besides the impact on agriculture and microbial ecology, airborne P. syringae can affect atmospheric glaciation processes, with consequences for cloud evolution, precipitation, and climate. Biogenic ice nucleation is also relevant for artificial snow production and for biomimetic materials for controlled interfacial freezing. We use interface-specific sum frequency generation (SFG) spectroscopy to show that hydrogen bonding at the water-bacteria contact imposes structural ordering onmore » the adjacent water network. Experimental SFG data and molecular dynamics simulations demonstrate that ice active sites within P. syringae feature unique hydrophilic-hydrophobic patterns to enhance ice nucleation. Finally, the freezing transition is further facilitated by the highly effective removal of latent heat from the nucleation site, as apparent from time-resolved SFG spectroscopy.« less

Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

DOE PAGES

Fang, Yin; Jiang, Yuanwen; Cherukara, Mathew J.; ...

2017-12-08

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similarmore » to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.« less

Anomalous heating and plasmoid formation in a driven magnetic reconnection experiment

DOE PAGES

Hare, J. D.; Suttle, L.; Lebedev, S. V.; ...

2017-02-21

We present a detailed study of magnetic reconnection in a quasi-two-dimensional pulsed-power driven laboratory experiment. Oppositely directed magnetic fields (B=3 T), advected by supersonic, sub-Alfvénic carbon plasma flows (V in = 50 km/s), are brought together and mutually annihilate inside a thin current layer (δ = 0.6 mm). Temporally and spatially resolved optical diagnostics, including interferometry, Faraday rotation imaging, and Thomson scattering, allow us to determine the structure and dynamics of this layer, the nature of the inflows and outflows, and the detailed energy partition during the reconnection process. We measure high electron and ion temperatures (T e = 100more » eV, T i = 600 eV), far in excess of what can be attributed to classical (Spitzer) resistive and viscous dissipation. Finally, we observe the repeated formation and ejection of plasmoids, consistent with the predictions from semicollisional plasmoid theory.« less

Time-resolved structural studies at synchrotrons and X-ray free electron lasers: opportunities and challenges

PubMed Central

Neutze, Richard; Moffat, Keith

2012-01-01

X-ray free electron lasers (XFELs) are potentially revolutionary X-ray sources because of their very short pulse duration, extreme peak brilliance and high spatial coherence, features that distinguish them from today’s synchrotron sources. We review recent time-resolved Laue diffraction and time-resolved wide angle X-ray scattering (WAXS) studies at synchrotron sources, and initial static studies at XFELs. XFELs have the potential to transform the field of time-resolved structural biology, yet many challenges arise in devising and adapting hardware, experimental design and data analysis strategies to exploit their unusual properties. Despite these challenges, we are confident that XFEL sources are poised to shed new light on ultrafast protein reaction dynamics. PMID:23021004

An approach to spin-resolved molecular gas microscopy

NASA Astrophysics Data System (ADS)

Covey, Jacob P.; De Marco, Luigi; Acevedo, Óscar L.; Rey, Ana Maria; Ye, Jun

2018-04-01

Ultracold polar molecules are an ideal platform for studying many-body physics with long-range dipolar interactions. Experiments in this field have progressed enormously, and several groups are pursuing advanced apparatus for manipulation of molecules with electric fields as well as single-atom-resolved in situ detection. Such detection has become ubiquitous for atoms in optical lattices and tweezer arrays, but has yet to be demonstrated for ultracold polar molecules. Here we present a proposal for the implementation of site-resolved microscopy for polar molecules, and specifically discuss a technique for spin-resolved molecular detection. We use numerical simulation of spin dynamics of lattice-confined polar molecules to show how such a scheme would be of utility in a spin-diffusion experiment.

Toward automated denoising of single molecular Förster resonance energy transfer data

NASA Astrophysics Data System (ADS)

Lee, Hao-Chih; Lin, Bo-Lin; Chang, Wei-Hau; Tu, I.-Ping

2012-01-01

A wide-field two-channel fluorescence microscope is a powerful tool as it allows for the study of conformation dynamics of hundreds to thousands of immobilized single molecules by Förster resonance energy transfer (FRET) signals. To date, the data reduction from a movie to a final set containing meaningful single-molecule FRET (smFRET) traces involves human inspection and intervention at several critical steps, greatly hampering the efficiency at the post-imaging stage. To facilitate the data reduction from smFRET movies to smFRET traces and to address the noise-limited issues, we developed a statistical denoising system toward fully automated processing. This data reduction system has embedded several novel approaches. First, as to background subtraction, high-order singular value decomposition (HOSVD) method is employed to extract spatial and temporal features. Second, to register and map the two color channels, the spots representing bleeding through the donor channel to the acceptor channel are used. Finally, correlation analysis and likelihood ratio statistic for the change point detection (CPD) are developed to study the two channels simultaneously, resolve FRET states, and report the dwelling time of each state. The performance of our method has been checked using both simulation and real data.

Dynamic tissue analysis using time- and wavelength-resolved fluorescence spectroscopy for atherosclerosis diagnosis

PubMed Central

Sun, Yinghua; Sun, Yang; Stephens, Douglas; Xie, Hongtao; Phipps, Jennifer; Saroufeem, Ramez; Southard, Jeffrey; Elson, Daniel S.; Marcu, Laura

2011-01-01

Simultaneous time- and wavelength-resolved fluorescence spectroscopy (STWRFS) was developed and tested for the dynamic characterization of atherosclerotic tissue ex vivo and arterial vessels in vivo. Autofluorescence, induced by a 337 nm, 700 ps pulsed laser, was split to three wavelength sub-bands using dichroic filters, with each sub-band coupled into a different length of optical fiber for temporal separation. STWRFS allows for fast recording/analysis (few microseconds) of time-resolved fluorescence emission in these sub-bands and rapid scanning. Distinct compositions of excised human atherosclerotic aorta were clearly discriminated over scanning lengths of several centimeters based on fluorescence lifetime and the intensity ratio between 390 and 452 nm. Operation of STWRFS blood flow was further validated in pig femoral arteries in vivo using a single-fiber probe integrated with an ultrasound imaging catheter. Current results demonstrate the potential of STWRFS as a tool for real-time optical characterization of arterial tissue composition and for atherosclerosis research and diagnosis. PMID:21369214

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide

PubMed Central

Plechinger, Gerd; Nagler, Philipp; Arora, Ashish; Schmidt, Robert; Chernikov, Alexey; del Águila, Andrés Granados; Christianen, Peter C.M.; Bratschitsch, Rudolf; Schüller, Christian; Korn, Tobias

2016-01-01

Monolayer transition-metal dichalcogenides have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. The optical properties of these two-dimensional crystals are dominated by tightly bound electron–hole pairs (excitons) and more complex quasiparticles such as charged excitons (trions). Here we investigate monolayer WS2 samples via photoluminescence and time-resolved Kerr rotation. In photoluminescence and in energy-dependent Kerr rotation measurements, we are able to resolve two different trion states, which we interpret as intravalley and intervalley trions. Using time-resolved Kerr rotation, we observe a rapid initial valley polarization decay for the A exciton and the trion states. Subsequently, we observe a crossover towards exciton–exciton interaction-related dynamics, consistent with the formation and decay of optically dark A excitons. By contrast, resonant excitation of the B exciton transition leads to a very slow decay of the Kerr signal. PMID:27586517

Time-resolved proton polarisation (TPP) images tyrosyl radical sites in bovine liver catalase.

NASA Astrophysics Data System (ADS)

Zimmer, Oliver; Jouve, Hélène M.; Stuhrmann, Heinrich B.

2017-05-01

A differentiation between dynamic polarised protons close to tyrosyl radical sites in catalase and those of the bulk is achieved by time-resolved polarised neutron scattering. Three radical sites, all of them being close to the molecular centre and the heme, appear to be equally possible. Among these is tyr-369 the radial site of which had previously been proven by EPR.

State-resolved Thermal/Hyperthermal Dynamics of Atmospheric Species

DTIC Science & Technology

2015-06-23

gas -room temperature ionic liquid (RTIL) interfaces. 2) Large scale trajectory simulations for theoretical analysis of gas - liquid scattering studies...areas: 1) Diode laser and LIF studies of hyperthermal CO2 and NO collisions at the gas -room temperature ionic liquid (RTIL) interfaces. 2) Large...scale trajectory simulations for theoretical analysis of gas - liquid scattering studies, 3) LIF data for state-resolved scattering of hyperthermal NO at

Diagnosing the Kinematics of the Tori in Active Galactic Nuclei with the Velocity-resolved Reverberation Mapping of the Narrow Iron K α Line

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

Liu Yuan; Li Xiaobo, E-mail: liuyuan@ihep.ac.cn, E-mail: lixb@ihep.ac.cn

The properties of the dusty tori in active galactic nuclei (AGNs) have been investigated in detail, mainly focusing on the geometry and components; however, the kinematics of the torus are still not clear. The narrow iron K α line at 6.4 keV is thought to be produced by the X-ray reflection from the torus. Thus, the velocity-resolved reverberation mapping of it is able to constrain the kinematics of the torus. Such effort is limited by the spectral resolution of current charged coupled device (CCD) detectors and should be possible with the microcalorimeter on the next generation X-ray satellite. In thismore » paper, we first construct the response functions of the torus under a uniform inflow, a Keplerian rotation, and a uniform outflow. Then the energy-dependent light curve of the narrow iron K α line is simulated according to the performance of the X-ray Integral Field Unit in Athena. Finally, the energy-dependent cross-correlation function is calculated to reveal the kinematic signal. According to our results, 100 observations with 5 ks exposure of each are sufficient to distinguish the above three velocity fields. Although the real geometry and velocity field of the torus could be more complex than we assumed, the present result proves the feasibility of the velocity-resolved reverberation mapping of the narrow iron K α line. The combination of the dynamics of the torus with those of the broad-line region and the host galaxy is instructive for the understanding of the feeding and feedback process of AGNs.« less

Nanoscale magnetic imaging using picosecond thermal gradients

NASA Astrophysics Data System (ADS)

Fuchs, Gregory

Research and development in spintronics is challenged by the lack of table-top magnetic imaging technologies that posses the simultaneous temporal resolution and spatial resolution to characterize magnetization dynamics in emerging spintronic devices. In addition, many of the most exciting magnetic material systems for spintronics are difficult to image with any method. To address this challenge, we developed a spatiotemporal magnetic microscope based on picosecond heat pulses that stroboscopically transduces an in-plane magnetization into a voltage signal. When the magnetic device contains a magnetic metal like FeCoB or NiFe, we use the time-resolved anomalous Nernst effect. When it contains a magnetic insulator/normal metal bilayer like yttrium iron garnet/platinum, we use the combination of the time-resolved longitudinal spin Seebeck effect and the inverse spin Hall effect. We demonstrate that these imaging modalities have time resolutions in the range of 10-100 ps and sensitivities in the range of 0.1 - 0.3° /√{Hz} , which enables not only static magnetic imaging, but also phase-sensitive ferromagnetic resonance imaging. One application of this technology is for magnetic torque vector imaging, which we apply to a spin Hall device. We find an unexpected variation in the spin torque vector that suggests conventional, all-electrical FMR measurements of spin torque vectors can produce a systematic error as large as 30% when quantifying the spin Hall efficiency. Finally, I will describe how time-resolved magnetic imaging can greatly exceed the spatial resolution of optical diffraction. We demonstrate scanning a sharp gold tip to create near-field thermal transfer from a picosecond laser pulse to a magnetic sample as the basis of a nanoscale spatiotemporal microscope. We gratefully acknowledge support from the AFOSR (FA9550-14-1-0243) and the NSF through the Cornell Center for Materials Research (DMR-1120296).

Comparison of one-dimensional probabilistic finite element method with direct numerical simulation of dynamically loaded heterogeneous materials

NASA Astrophysics Data System (ADS)

Robbins, Joshua; Voth, Thomas

2011-06-01

Material response to dynamic loading is often dominated by microstructure such as grain topology, porosity, inclusions, and defects; however, many models rely on assumptions of homogeneity. We use the probabilistic finite element method (WK Liu, IJNME, 1986) to introduce local uncertainty to account for material heterogeneity. The PFEM uses statistical information about the local material response (i.e., its expectation, coefficient of variation, and autocorrelation) drawn from knowledge of the microstructure, single crystal behavior, and direct numerical simulation (DNS) to determine the expectation and covariance of the system response (velocity, strain, stress, etc). This approach is compared to resolved grain-scale simulations of the equivalent system. The microstructures used for the DNS are produced using Monte Carlo simulations of grain growth, and a sufficient number of realizations are computed to ensure a meaningful comparison. Finally, comments are made regarding the suitability of one-dimensional PFEM for modeling material heterogeneity. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

The birth of a supermassive black hole binary

NASA Astrophysics Data System (ADS)

Pfister, Hugo; Lupi, Alessandro; Capelo, Pedro R.; Volonteri, Marta; Bellovary, Jillian M.; Dotti, Massimo

2017-11-01

We study the dynamical evolution of supermassive black holes, in the late stage of galaxy mergers, from kpc to pc scales. In particular, we capture the formation of the binary, a necessary step before the final coalescence, and trace back the main processes causing the decay of the orbit. We use hydrodynamical simulations of galaxy mergers with different resolutions, from 20 pc down to 1 pc, in order to study the effects of the resolution on our results, remove numerical effects, and assess that resolving the influence radius of the orbiting black hole is a minimum condition to fully capture the formation of the binary. Our simulations include the relevant physical processes, namely star formation, supernova feedback, accretion on to the black holes and the ensuing feedback. We find that, in these mergers, dynamical friction from the smooth stellar component of the nucleus is the main process that drives black holes from kpc to pc scales. Gas does not play a crucial role and even clumps do not induce scattering or perturb the orbits. We compare the time needed for the formation of the binary to analytical predictions and suggest how to apply such analytical formalism to obtain estimates of binary formation times in lower resolution simulations.

An improvement in rollover detection of articulated vehicles using the grey system theory

NASA Astrophysics Data System (ADS)

Chou, Tao; Chu, Tzyy-Wen

2014-05-01

A Rollover Index combined with the grey system theory, called a Grey Rollover Index (GRI), is proposed to assess the rollover threat for articulated vehicles with a tractor-semitrailer combination. This index can predict future trends of vehicle dynamics based on current vehicle motion; thus, it is suitable for vehicle-rollover detection. Two difficulties are encountered when applying the GRI for rollover detection. The first difficulty is effectively predicting the rollover threat of the vehicles, and the second difficulty is achieving a definite definition of the real rollover timing of a vehicle. The following methods are used to resolve these problems. First, a nonlinear mathematical model is constructed to accurately describe the vehicle dynamics of articulated vehicles. This model is combined with the GRI to predict rollover propensity. Finally, TruckSim™ software is used to determine the real rollover timing and facilitate the accurate supply of information to the rollover detection system through the GRI. This index is used to verify the simulation based on the common manoeuvres that cause rollover accidents to reduce the occurrence of false signals and effectively increase the efficiency of the rollover detection system.

Generalized multiband typical medium dynamical cluster approximation: Application to (Ga,Mn)N

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

Zhang, Yi; Nelson, R.; Siddiqui, Elisha

We generalize the multiband typical medium dynamical cluster approximation and the formalism introduced by Blackman, Esterling, and Berk so that it can deal with localization in multiband disordered systems with both diagonal and off-diagonal disorder with complicated potentials. We also introduce an ansatz for the momentum-resolved typical density of states that greatly improves the numerical stability of the method while preserving the independence of scattering events at different frequencies. Starting from the first-principles effective Hamiltonian, we apply this method to the diluted magnetic semiconductor Ga 1 - x Mn x N , and find the impurity band is completely localizedmore » for Mn concentrations x < 0.03 , while for 0.03 < x < 0.10 the impurity band has delocalized states but the chemical potential resides at or above the mobility edge. So, the system is always insulating within the experimental compositional limit ( x ≈ 0.10 ) due to Anderson localization. But, for 0.03 < x < 0.10 hole doping could make the system metallic, allowing double-exchange mediated, or enhanced, ferromagnetism. Finally, this developed method is expected to have a large impact on first-principles studies of Anderson localization.« less

Dielectronic recombination data for dynamic finite-density plasmas. XV. The silicon isoelectronic sequence

NASA Astrophysics Data System (ADS)

Kaur, Jagjit; Gorczyca, T. W.; Badnell, N. R.

2018-02-01

Context. We aim to present a comprehensive theoretical investigation of dielectronic recombination (DR) of the silicon-like isoelectronic sequence and provide DR and radiative recombination (RR) data that can be used within a generalized collisional-radiative modelling framework. Aims: Total and final-state level-resolved DR and RR rate coefficients for the ground and metastable initial levels of 16 ions between P+ and Zn16+ are determined. Methods: We carried out multi-configurational Breit-Pauli DR calculations for silicon-like ions in the independent processes, isolated resonance, distorted wave approximation. Both Δnc = 0 and Δnc = 1 core excitations are included using LS and intermediate coupling schemes. Results: Results are presented for a selected number of ions and compared to all other existing theoretical and experimental data. The total dielectronic and radiative recombination rate coefficients for the ground state are presented in tabulated form for easy implementation into spectral modelling codes. These data can also be accessed from the Atomic Data and Analysis Structure (ADAS) OPEN-ADAS database. This work is a part of an assembly of a dielectronic recombination database for the modelling of dynamic finite-density plasmas.

Nuclear quantum effects in electronically adiabatic quantum time correlation functions: Application to the absorption spectrum of a hydrated electron

NASA Astrophysics Data System (ADS)

Turi, László; Hantal, György; Rossky, Peter J.; Borgis, Daniel

2009-07-01

A general formalism for introducing nuclear quantum effects in the expression of the quantum time correlation function of an operator in a multilevel electronic system is presented in the adiabatic limit. The final formula includes the nuclear quantum time correlation functions of the operator matrix elements, of the energy gap, and their cross terms. These quantities can be inferred and evaluated from their classical analogs obtained by mixed quantum-classical molecular dynamics simulations. The formalism is applied to the absorption spectrum of a hydrated electron, expressed in terms of the time correlation function of the dipole operator in the ground electronic state. We find that both static and dynamic nuclear quantum effects distinctly influence the shape of the absorption spectrum, especially its high energy tail related to transitions to delocalized electron states. Their inclusion does improve significantly the agreement between theory and experiment for both the low and high frequency edges of the spectrum. It does not appear sufficient, however, to resolve persistent deviations in the slow Lorentzian-like decay part of the spectrum in the intermediate 2-3 eV region.

Generalized multiband typical medium dynamical cluster approximation: Application to (Ga,Mn)N

DOE PAGES

Zhang, Yi; Nelson, R.; Siddiqui, Elisha; ...

2016-12-29

We generalize the multiband typical medium dynamical cluster approximation and the formalism introduced by Blackman, Esterling, and Berk so that it can deal with localization in multiband disordered systems with both diagonal and off-diagonal disorder with complicated potentials. We also introduce an ansatz for the momentum-resolved typical density of states that greatly improves the numerical stability of the method while preserving the independence of scattering events at different frequencies. Starting from the first-principles effective Hamiltonian, we apply this method to the diluted magnetic semiconductor Ga 1 - x Mn x N , and find the impurity band is completely localizedmore » for Mn concentrations x < 0.03 , while for 0.03 < x < 0.10 the impurity band has delocalized states but the chemical potential resides at or above the mobility edge. So, the system is always insulating within the experimental compositional limit ( x ≈ 0.10 ) due to Anderson localization. But, for 0.03 < x < 0.10 hole doping could make the system metallic, allowing double-exchange mediated, or enhanced, ferromagnetism. Finally, this developed method is expected to have a large impact on first-principles studies of Anderson localization.« less

An innovative Yb-based ultrafast deep ultraviolet source for time-resolved photoemission experiments

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

Boschini, F.; Hedayat, H.; Dallera, C.

2014-12-15

Time- and angle-resolved photoemission spectroscopy is a powerful technique to study ultrafast electronic dynamics in solids. Here, an innovative optical setup based on a 100-kHz Yb laser source is presented. Exploiting non-collinear optical parametric amplification and sum-frequency generation, ultrashort pump (hν = 1.82 eV) and ultraviolet probe (hν = 6.05 eV) pulses are generated. Overall temporal and instrumental energy resolutions of, respectively, 85 fs and 50 meV are obtained. Time- and angle-resolved measurements on BiTeI semiconductor are presented to show the capabilities of the setup.

Energetics and dynamics through time-resolved measurements in mass spectrometry

NASA Astrophysics Data System (ADS)

Lifshitz, Chava

Results of recent work on time-resolved photoionization and electron ionization mass spectrometry carried out in Jerusalem are reviewed. Time-resolved photoionization mass spectrometry in the vacuum ultraviolet is applied to polycyclic aromatic hydrocarbons, for example naphthalene, pyrene and fluoranthene as well as to some bromo derivatives (bromonaphthalene and bromoanthracene). Time-resolved photoionization efficiency curves are modelled by Rice-Ramsperger-Kassel-Marcus QET rate-energy k ( E ) dependences of the unimolecular dissociative processes and by the rate process infrared radiative relaxation k . Experimental results are augmented by time-resolved photorad dissociation data for the same species, whenever available. Kinetic shifts, conventional and intrinsic (due to competition between dissociative and radiative decay), are evaluated. Activation parameters (activation energies and entropies) are deduced. Thermochemical information is obtained including bond energies and ionic heats of formation. Fullerenes, notably C , are studied by time-resolved electron ionization and a large intrinsic shift, due to competition with black-bodylike radiative decay in the visible is discussed.

On kinetics of a dynamically unbalanced rotator with sliding friction in supports

NASA Astrophysics Data System (ADS)

Chistyakov, Viktor V.

2018-05-01

The dynamics is analytically and numerically modelled for both free and forced rotations of a rigid body around the central but non-principal vertical axis Oz under action of dry friction forces in plain bearings and heel supports in combination with other dissipative and conservative axial torques. The inertia forces due to D'Alembert principle cause the supports' reactions and hence the decelerating friction torque depending on not only angular speed but acceleration too. This dependence makes the dynamical equations not resolved with regard to the senior derivative and ambiguous, and being thus resolved they have an irrational or singular right hand side. This irrationality/singularity results in their featured solutions or paradoxical absence of those in frames of absolutely rigid body approach. The kinetics obtained is analyzed and compared with the standard ones of rotation under action of conservative elastic and drag torques.

CellCognition: time-resolved phenotype annotation in high-throughput live cell imaging.

PubMed

Held, Michael; Schmitz, Michael H A; Fischer, Bernd; Walter, Thomas; Neumann, Beate; Olma, Michael H; Peter, Matthias; Ellenberg, Jan; Gerlich, Daniel W

2010-09-01

Fluorescence time-lapse imaging has become a powerful tool to investigate complex dynamic processes such as cell division or intracellular trafficking. Automated microscopes generate time-resolved imaging data at high throughput, yet tools for quantification of large-scale movie data are largely missing. Here we present CellCognition, a computational framework to annotate complex cellular dynamics. We developed a machine-learning method that combines state-of-the-art classification with hidden Markov modeling for annotation of the progression through morphologically distinct biological states. Incorporation of time information into the annotation scheme was essential to suppress classification noise at state transitions and confusion between different functional states with similar morphology. We demonstrate generic applicability in different assays and perturbation conditions, including a candidate-based RNA interference screen for regulators of mitotic exit in human cells. CellCognition is published as open source software, enabling live-cell imaging-based screening with assays that directly score cellular dynamics.

Quantitative mass imaging of single biological macromolecules.

PubMed

Young, Gavin; Hundt, Nikolas; Cole, Daniel; Fineberg, Adam; Andrecka, Joanna; Tyler, Andrew; Olerinyova, Anna; Ansari, Ayla; Marklund, Erik G; Collier, Miranda P; Chandler, Shane A; Tkachenko, Olga; Allen, Joel; Crispin, Max; Billington, Neil; Takagi, Yasuharu; Sellers, James R; Eichmann, Cédric; Selenko, Philipp; Frey, Lukas; Riek, Roland; Galpin, Martin R; Struwe, Weston B; Benesch, Justin L P; Kukura, Philipp

2018-04-27

The cellular processes underpinning life are orchestrated by proteins and their interactions. The associated structural and dynamic heterogeneity, despite being key to function, poses a fundamental challenge to existing analytical and structural methodologies. We used interferometric scattering microscopy to quantify the mass of single biomolecules in solution with 2% sequence mass accuracy, up to 19-kilodalton resolution, and 1-kilodalton precision. We resolved oligomeric distributions at high dynamic range, detected small-molecule binding, and mass-imaged proteins with associated lipids and sugars. These capabilities enabled us to characterize the molecular dynamics of processes as diverse as glycoprotein cross-linking, amyloidogenic protein aggregation, and actin polymerization. Interferometric scattering mass spectrometry allows spatiotemporally resolved measurement of a broad range of biomolecular interactions, one molecule at a time. Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

Resolving Properties of Polymers and Nanoparticle Assembly through Coarse-Grained Computational Studies.

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

Grest, Gary S.

2017-09-01

Coupled length and time scales determine the dynamic behavior of polymers and polymer nanocomposites and underlie their unique properties. To resolve the properties over large time and length scales it is imperative to develop coarse grained models which retain the atomistic specificity. Here we probe the degree of coarse graining required to simultaneously retain significant atomistic details a nd access large length and time scales. The degree of coarse graining in turn sets the minimum length scale instrumental in defining polymer properties and dynamics. Using polyethylene as a model system, we probe how the coarse - graining scale affects themore » measured dynamics with different number methylene group s per coarse - grained beads. Using these models we simulate polyethylene melts for times over 500 ms to study the viscoelastic properties of well - entangled polymer melts and large nanoparticle assembly as the nanoparticles are driven close enough to form nanostructures.« less

Exciton dynamics at a single dislocation in GaN probed by picosecond time-resolved cathodoluminescence

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

Liu, W., E-mail: we.liu@epfl.ch, E-mail: gwenole.jacopin@epfl.ch; Carlin, J.-F.; Grandjean, N.

2016-07-25

We investigate the dynamics of donor bound excitons (D°X{sub A}) at T = 10 K around an isolated single edge dislocation in homoepitaxial GaN, using a picosecond time-resolved cathodoluminescence (TR-CL) setup with high temporal and spatial resolutions. An ∼ 1.3 meV dipole-like energy shift of D°X{sub A} is observed around the dislocation, induced by the local strain fields. By simultaneously recording the variations of both the exciton lifetime and the CL intensity across the dislocation, we directly assess the dynamics of excitons around the defect. Our observations are well reproduced by a diffusion model. It allows us to deduce an exciton diffusion length ofmore » ∼24 nm as well as an effective area of the dislocation with a radius of ∼95 nm, where the recombination can be regarded as entirely non-radiative.« less

ULTRAFAST CHEMISTRY: Using Time-Resolved Vibrational Spectroscopy for Interrogation of Structural Dynamics

NASA Astrophysics Data System (ADS)

Nibbering, Erik T. J.; Fidder, Henk; Pines, Ehud

2005-05-01

Time-resolved infrared (IR) and Raman spectroscopy elucidates molecular structure evolution during ultrafast chemical reactions. Following vibrational marker modes in real time provides direct insight into the structural dynamics, as is evidenced in studies on intramolecular hydrogen transfer, bimolecular proton transfer, electron transfer, hydrogen bonding during solvation dynamics, bond fission in organometallic compounds and heme proteins, cis-trans isomerization in retinal proteins, and transformations in photochromic switch pairs. Femtosecond IR spectroscopy monitors the site-specific interactions in hydrogen bonds. Conversion between excited electronic states can be followed for intramolecular electron transfer by inspection of the fingerprint IR- or Raman-active vibrations in conjunction with quantum chemical calculations. Excess internal vibrational energy, generated either by optical excitation or by internal conversion from the electronic excited state to the ground state, is observable through transient frequency shifts of IR-active vibrations and through nonequilibrium populations as deduced by Raman resonances.

Inverting dynamic force microscopy: From signals to time-resolved interaction forces

PubMed Central

Stark, Martin; Stark, Robert W.; Heckl, Wolfgang M.; Guckenberger, Reinhard

2002-01-01

Transient forces between nanoscale objects on surfaces govern friction, viscous flow, and plastic deformation, occur during manipulation of matter, or mediate the local wetting behavior of thin films. To resolve transient forces on the (sub) microsecond time and nanometer length scale, dynamic atomic force microscopy (AFM) offers largely unexploited potential. Full spectral analysis of the AFM signal completes dynamic AFM. Inverting the signal formation process, we measure the time course of the force effective at the sensing tip. This approach yields rich insight into processes at the tip and dispenses with a priori assumptions about the interaction, as it relies solely on measured data. Force measurements on silicon under ambient conditions demonstrate the distinct signature of the interaction and reveal that peak forces exceeding 200 nN are applied to the sample in a typical imaging situation. These forces are 2 orders of magnitude higher than those in covalent bonds. PMID:12070341

Frontiers in Chemical Physics

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

Bowlan, Pamela Renee

2016-05-02

These are slides dealing with frontiers in chemical physics. The following topics are covered: Time resolving chemistry with ultrashort pulses in the 0.1-40 THz spectral range; Example: Mid-infrared absorption spectrum of the intermediate state CH 2OO; Tracking reaction dynamics through changes in the spectra; Single-shot measurement of the mid-IR absorption dynamics; Applying 2D coherent mid-IR spectroscopy to learn more about transition states; Time resolving chemical reactions at a catalysis using mid-IR and THz pulses; Studying topological insulators requires a surface sensitive probe; Nonlinear phonon dynamics in Bi 2Se 3; THz-pump, SHG-probe as a surface sensitive coherent 2D spectroscopy; Nanometer andmore » femtosecond spatiotemporal resolution mid-IR spectroscopy; Coherent two-dimensional THz/mid-IR spectroscopy with 10nm spatial resolution; Pervoskite oxides as catalysts; Functionalized graphene for catalysis; Single-shot spatiotemporal measurements; Spatiotemporal pulse measurement; Intense, broad-band THz/mid-IR generation with organic crystals.« less

Simulation Based Exploration of Critical Zone Dynamics in Intensively Managed Landscapes

NASA Astrophysics Data System (ADS)

Kumar, P.

2017-12-01

The advent of high-resolution measurements of topographic and (vertical) vegetation features using areal LiDAR are enabling us to resolve micro-scale ( 1m) landscape structural characteristics over large areas. Availability of hyperspectral measurements is further augmenting these LiDAR data by enabling the biogeochemical characterization of vegetation and soils at unprecedented spatial resolutions ( 1-10m). Such data have opened up novel opportunities for modeling Critical Zone processes and exploring questions that were not possible before. We show how an integrated 3-D model at 1m grid resolution can enable us to resolve micro-topographic and ecological dynamics and their control on hydrologic and biogeochemical processes over large areas. We address the computational challenge of such detailed modeling by exploiting hybrid CPU and GPU computing technologies. We show results of moisture, biogeochemical, and vegetation dynamics from studies in the Critical Zone Observatory for Intensively managed Landscapes (IMLCZO) in the Midwestern United States.

An Optimization Principle for Deriving Nonequilibrium Statistical Models of Hamiltonian Dynamics

NASA Astrophysics Data System (ADS)

Turkington, Bruce

2013-08-01

A general method for deriving closed reduced models of Hamiltonian dynamical systems is developed using techniques from optimization and statistical estimation. Given a vector of resolved variables, selected to describe the macroscopic state of the system, a family of quasi-equilibrium probability densities on phase space corresponding to the resolved variables is employed as a statistical model, and the evolution of the mean resolved vector is estimated by optimizing over paths of these densities. Specifically, a cost function is constructed to quantify the lack-of-fit to the microscopic dynamics of any feasible path of densities from the statistical model; it is an ensemble-averaged, weighted, squared-norm of the residual that results from submitting the path of densities to the Liouville equation. The path that minimizes the time integral of the cost function determines the best-fit evolution of the mean resolved vector. The closed reduced equations satisfied by the optimal path are derived by Hamilton-Jacobi theory. When expressed in terms of the macroscopic variables, these equations have the generic structure of governing equations for nonequilibrium thermodynamics. In particular, the value function for the optimization principle coincides with the dissipation potential that defines the relation between thermodynamic forces and fluxes. The adjustable closure parameters in the best-fit reduced equations depend explicitly on the arbitrary weights that enter into the lack-of-fit cost function. Two particular model reductions are outlined to illustrate the general method. In each example the set of weights in the optimization principle contracts into a single effective closure parameter.

Final Report: Resolving and Discriminating Overlapping Anomalies from Multiple Objects in Cluttered Environments

DTIC Science & Technology

2015-12-15

UXO community . NAME Total Number: PERCENT_SUPPORTEDNAME FTE Equivalent: Total Number: Irma Shamatava 0.50 0.50 1 Resolving and Discriminating...Distinguishing an object of interest from innocuous items is the main problem that the UXO community is facing currently. This inverse problem...innocuous items is the main problem that the UXO community is facing currently. This inverse problem demands fast and accurate representation of

Site-specific structural dynamics of α-Synuclein revealed by time-resolved fluorescence spectroscopy: a review

NASA Astrophysics Data System (ADS)

Sahay, Shruti; Krishnamoorthy, G.; Maji, Samir K.

2016-12-01

Aggregation of α-Synuclein (α-Syn) into amyloid fibrils is known to be associated with the pathogenesis of Parkinson’s disease (PD). Several missense mutations of the α-Syn gene have been associated with rare, early onset familial forms of PD. Despite several studies done so far, the local/residue-level structure and dynamics of α-Syn in its soluble and aggregated fibril form and how these are affected by the familial PD associated mutations are still not clearly understood. Here, we review studies performed by our group as well as other research groups, where time-resolved fluorescence spectroscopy has been used to understand the site-specific structure and dynamics of α-Syn under physiological conditions as well as under conditions that alter the aggregation properties of the protein such as low pH, high temperature, presence of membrane mimics and familial PD associated mutations. These studies have provided important insights into the critical structural properties of α-Syn that may govern its aggregation. The review also highlights time-resolved fluorescence as a promising tool to study the critical conformational transitions associated with early oligomerization of α-Syn, which are otherwise not accessible using other commonly used techniques such as thioflavin T (ThT) binding assay.

Quantifying the size-resolved dynamics of indoor bioaerosol transport and control.

PubMed

Kunkel, S A; Azimi, P; Zhao, H; Stark, B C; Stephens, B

2017-09-01

Understanding the bioaerosol dynamics of droplets and droplet nuclei emitted during respiratory activities is important for understanding how infectious diseases are transmitted and potentially controlled. To this end, we conducted experiments to quantify the size-resolved dynamics of indoor bioaerosol transport and control in an unoccupied apartment unit operating under four different HVAC particle filtration conditions. Two model organisms (Escherichia coli K12 and bacteriophage T4) were aerosolized under alternating low and high flow rates to roughly represent constant breathing and periodic coughing. Size-resolved aerosol sampling and settle plate swabbing were conducted in multiple locations. Samples were analyzed by DNA extraction and quantitative polymerase chain reaction (qPCR). DNA from both organisms was detected during all test conditions in all air samples up to 7 m away from the source, but decreased in magnitude with the distance from the source. A greater fraction of T4 DNA was recovered from the aerosol size fractions smaller than 1 μm than E. coli K12 at all air sampling locations. Higher efficiency HVAC filtration also reduced the amount of DNA recovered in air samples and on settle plates located 3-7 m from the source. © 2017 John Wiley & Sons A/S. Published by John Wiley & Sons Ltd.

Characteristics of subgrid-resolved-scale dynamics in anisotropic turbulence, with application to rough-wall boundary layers

NASA Astrophysics Data System (ADS)

Juneja, Anurag; Brasseur, James G.

1999-10-01

Large-eddy simulation (LES) of the atmospheric boundary layer (ABL) using eddy viscosity subgrid-scale (SGS) models is known to poorly predict mean shear at the first few grid cells near the ground, a rough surface with no viscous sublayer. It has recently been shown that convective motions carry this localized error vertically to infect the entire ABL, and that the error is more a consequence of the SGS model than grid resolution in the near-surface inertial layer. Our goal was to determine what first-order errors in the predicted SGS terms lead to spurious expectation values, and what basic dynamics in the filtered equation for resolved scale (RS) velocity must be captured by SGS models to correct the deficiencies. Our analysis is of general relevance to LES of rough-wall high Reynolds number boundary layers, where the essential difficulty in the closure is the importance of the SGS acceleration terms, a consequence of necessary under-resolution of relevant energy-containing motions at the first few grid levels, leading to potentially strong couplings between the anisotropies in resolved velocity and predicted SGS dynamics. We analyze these two issues (under-resolution and anisotropy) in the absence of a wall using two direct numerical simulation datasets of homogeneous turbulence with very different anisotropic structure characteristic of the near-surface ABL: shear- and buoyancy-generated turbulence. We uncover three important issues which should be addressed in the design of SGS closures near rough walls and we provide a priori tests for the SGS model. First, we identify a strong spurious coupling between the anisotropic structure of the resolved velocity field and predicted SGS dynamics which can create a feedback loop to incorrectly enhance certain components of the predicted velocity field. Second, we find that eddy viscosity and "similarity" SGS models do not contain enough degrees of freedom to capture, at a sufficient level of accuracy, both RS-SGS energy flux and SGS-RS dynamics. Third, to correctly capture pressure transport near a wall, closures must be made more flexible to accommodate proper partitioning between SGS stress divergence and SGS pressure gradient.

Insights into soil carbon dynamics across climatic and geologic gradients from temporally-resolved radiocarbon measurements

NASA Astrophysics Data System (ADS)

van der Voort, T. S.; Hagedorn, F.; Mannu, U.; Walthert, L.; McIntyre, C.; Eglinton, T. I.

2016-12-01

Soil carbon constitutes the largest terrestrial reservoir of organic carbon, and therefore quantifying soil organic matter dynamics (carbon turnover, stocks and fluxes) across spatial gradients is essential for an understanding of the carbon cycle and the impacts of global change. In particular, links between soil carbon dynamics and different climatic and compositional factors remains poorly understood. Radiocarbon constitutes a powerful tool for unraveling soil carbon dynamics. Temporally-resolved radiocarbon measurements, which take advantage of "bomb-radiocarbon"-driven changes in atmospheric 14C, enable further constraints to be placed on C turnover times. These in turn can yield more precise flux estimates for both upper and deeper soil horizons. This project combines bulk radiocarbon measurements on a suite of soil profiles spanning strong climatic (MAT 1.3-9.2°C, MAP 600 to 2100 mm m-2y-1) and geologic gradients with a more in-depth approach for a subset of locations. For this subset, temporal and carbon-fraction specific radiocarbon data has been acquired for both topsoil and deeper soils. These well-studied sites are part of the Long-Term Forest Ecosystem Research (LWF) program of the Swiss Federal Institute for Forest, Snow and Landscape research (WSL). Resulting temporally-resolved turnover estimates are coupled to carbon stocks, fluxes across this wide range of forest ecosystems and are examined in the context of environmental drivers (temperature, precipitation, primary production and soil moisture) as well as composition (sand, silt and clay content). Statistical analysis on the region-scale - correlating radiocarbon signature with climatic variables such as temperature, precipitation, primary production and elevation - indicates that composition rather than climate is a key driver of ­­Δ14C signatures. Estimates of carbon turnover, stocks and fluxes derived from temporally-resolved measurements highlight the pivotal role of soil moisture as a key driver of soil carbon turnover and associated fluxes. Overall, this study has afforded a uniquely comprehensive dataset that improves our understanding of controls on carbon dynamics across spatial and temporal scales, as well as the pool-specific and long-term trends in soil carbon (de)stabilization and vulnerability.

Determination of errors in derived magnetic field directions in geosynchronous orbit: results from a statistical approach

DOE PAGES

Chen, Yue; Cunningham, Gregory; Henderson, Michael

2016-09-21

Our study aims to statistically estimate the errors in local magnetic field directions that are derived from electron directional distributions measured by Los Alamos National Laboratory geosynchronous (LANL GEO) satellites. First, by comparing derived and measured magnetic field directions along the GEO orbit to those calculated from three selected empirical global magnetic field models (including a static Olson and Pfitzer 1977 quiet magnetic field model, a simple dynamic Tsyganenko 1989 model, and a sophisticated dynamic Tsyganenko 2001 storm model), it is shown that the errors in both derived and modeled directions are at least comparable. Furthermore, using a newly developedmore » proxy method as well as comparing results from empirical models, we are able to provide for the first time circumstantial evidence showing that derived magnetic field directions should statistically match the real magnetic directions better, with averaged errors < ~2°, than those from the three empirical models with averaged errors > ~5°. In addition, our results suggest that the errors in derived magnetic field directions do not depend much on magnetospheric activity, in contrast to the empirical field models. Finally, as applications of the above conclusions, we show examples of electron pitch angle distributions observed by LANL GEO and also take the derived magnetic field directions as the real ones so as to test the performance of empirical field models along the GEO orbits, with results suggesting dependence on solar cycles as well as satellite locations. Finally, this study demonstrates the validity and value of the method that infers local magnetic field directions from particle spin-resolved distributions.« less

Determination of errors in derived magnetic field directions in geosynchronous orbit: results from a statistical approach

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

Chen, Yue; Cunningham, Gregory; Henderson, Michael

Our study aims to statistically estimate the errors in local magnetic field directions that are derived from electron directional distributions measured by Los Alamos National Laboratory geosynchronous (LANL GEO) satellites. First, by comparing derived and measured magnetic field directions along the GEO orbit to those calculated from three selected empirical global magnetic field models (including a static Olson and Pfitzer 1977 quiet magnetic field model, a simple dynamic Tsyganenko 1989 model, and a sophisticated dynamic Tsyganenko 2001 storm model), it is shown that the errors in both derived and modeled directions are at least comparable. Furthermore, using a newly developedmore » proxy method as well as comparing results from empirical models, we are able to provide for the first time circumstantial evidence showing that derived magnetic field directions should statistically match the real magnetic directions better, with averaged errors < ~2°, than those from the three empirical models with averaged errors > ~5°. In addition, our results suggest that the errors in derived magnetic field directions do not depend much on magnetospheric activity, in contrast to the empirical field models. Finally, as applications of the above conclusions, we show examples of electron pitch angle distributions observed by LANL GEO and also take the derived magnetic field directions as the real ones so as to test the performance of empirical field models along the GEO orbits, with results suggesting dependence on solar cycles as well as satellite locations. Finally, this study demonstrates the validity and value of the method that infers local magnetic field directions from particle spin-resolved distributions.« less

Demonstration of the Competency-Based Curriculum for Distributive Education and Distributive Cooperative Training Programs. Final Report.

ERIC Educational Resources Information Center

Marshall Univ., Huntington, WV. Dept. of Occupational, Adult, and Safety Education.

A core curriculum, training plans, and implementation guide developed by the project are included in this final report, which describes activities to resolve problems encountered by teachers using the IDECC (Interstate Distributive Education Curriculum Consortium) system designed for distributive education (DE) and diversified cooperative training…

Study of Varying Boundary Layer Height on Turret Flow Structures

DTIC Science & Technology

2011-06-01

fluid dynamics. The difficulties of the problem arise in modeling several complex flow features including separation, reattachment, three-dimensional...impossible. In this case, the approach is to create a model to calculate the properties of interest. The main issue with resolving turbulent flows...operation and their effect is modeled through subgrid scale models . As a result, the the most important turbulent scales are resolved and the

Bypassing the energy-time uncertainty in time-resolved photoemission

NASA Astrophysics Data System (ADS)

Randi, Francesco; Fausti, Daniele; Eckstein, Martin

2017-03-01

The energy-time uncertainty is an intrinsic limit for time-resolved experiments imposing a tradeoff between the duration of the light pulses used in experiments and their frequency content. In standard time-resolved photoemission, this limitation maps directly onto a tradeoff between the time resolution of the experiment and the energy resolution that can be achieved on the electronic spectral function. Here we propose a protocol to disentangle the energy and time resolutions in photoemission. We demonstrate that dynamical information on all time scales can be retrieved from time-resolved photoemission experiments using suitably shaped light pulses of quantum or classical nature. As a paradigmatic example, we study the dynamical buildup of the Kondo peak, a narrow feature in the electronic response function arising from the screening of a magnetic impurity by the conduction electrons. After a quench, the electronic screening builds up on timescales shorter than the inverse width of the Kondo peak and we demonstrate that the proposed experimental scheme could be used to measure the intrinsic time scales of such electronic screening. The proposed approach provides an experimental framework to access the nonequilibrium response of collective electronic properties beyond the spectral uncertainty limit and will enable the direct measurement of phenomena such as excited Higgs modes and, possibly, the retarded interactions in superconducting systems.

Angle-resolved effective potentials for disk-shaped molecules

NASA Astrophysics Data System (ADS)

Heinemann, Thomas; Palczynski, Karol; Dzubiella, Joachim; Klapp, Sabine H. L.

2014-12-01

We present an approach for calculating coarse-grained angle-resolved effective pair potentials for uniaxial molecules. For integrating out the intramolecular degrees of freedom we apply umbrella sampling and steered dynamics techniques in atomistically-resolved molecular dynamics (MD) computer simulations. Throughout this study we focus on disk-like molecules such as coronene. To develop the methods we focus on integrating out the van der Waals and intramolecular interactions, while electrostatic charge contributions are neglected. The resulting coarse-grained pair potential reveals a strong temperature and angle dependence. In the next step we fit the numerical data with various Gay-Berne-like potentials to be used in more efficient simulations on larger scales. The quality of the resulting coarse-grained results is evaluated by comparing their pair and many-body structure as well as some thermodynamic quantities self-consistently to the outcome of atomistic MD simulations of many-particle systems. We find that angle-resolved potentials are essential not only to accurately describe crystal structures but also for fluid systems where simple isotropic potentials start to fail already for low to moderate packing fractions. Further, in describing these states it is crucial to take into account the pronounced temperature dependence arising in selected pair configurations due to bending fluctuations.

Time-Resolved Optical Measurements of Fuel-Air Mixedness in Windowless High Speed Research Combustors

NASA Technical Reports Server (NTRS)

Nguyen, Quang-Viet

1998-01-01

Fuel distribution measurements in gas turbine combustors are needed from both pollution and fuel-efficiency standpoints. In addition to providing valuable data for performance testing and engine development, measurements of fuel distributions uniquely complement predictive numerical simulations. Although equally important as spatial distribution, the temporal distribution of the fuel is an often overlooked aspect of combustor design and development. This is due partly to the difficulties in applying time-resolved diagnostic techniques to the high-pressure, high-temperature environments inside gas turbine engines. Time-resolved measurements of the fuel-to-air ratio (F/A) can give researchers critical insights into combustor dynamics and acoustics. Beginning in early 1998, a windowless technique that uses fiber-optic, line-of-sight, infrared laser light absorption to measure the time-resolved fluctuations of the F/A (refs. 1 and 2) will be used within the premixer section of a lean-premixed, prevaporized (LPP) combustor in NASA Lewis Research Center's CE-5 facility. The fiber-optic F/A sensor will permit optical access while eliminating the need for film-cooled windows, which perturb the flow. More importantly, the real-time data from the fiber-optic F/A sensor will provide unique information for the active feedback control of combustor dynamics. This will be a prototype for an airborne sensor control system.

Geometric phase effects in ultracold hydrogen exchange reaction

DOE PAGES

Hazra, Jisha; Kendrick, Brian K.; Balakrishnan, Naduvalath

2016-10-14

The role of the geometric phase effect on chemical reaction dynamics is explored by examining the hydrogen exchange process in the fundamental H+HD reaction. Results are presented for vibrationally excited HD molecules in the v = 4 vibrational level and for collision energies ranging from 1 μK to 100 K. It is found that, for collision energies below 3 K, inclusion of the geometric phase leads to dramatic enhancement or suppression of the reaction rates depending on the final quantum state of the HD molecule. The effect was found to be the most prominent for rotationally resolved integral and differential cross sections but it persists to a lesser extent in the vibrationally resolved and total reaction rate coefficients. However, no significant GP effect is present in the reactive channel leading to the D+H 2 product or in the D+H 2more » $$(v=4,j=0)\\,\\to $$ HD+H reaction. A simple interference mechanism involving inelastic (nonreactive) and exchange scattering amplitudes is invoked to account for the observed GP effects. The computed results also reveal a shape resonance in the H+HD reaction near 1 K and the GP effect is found to influence the magnitude of the resonant part of the cross section. In conclusion, experimental detection of the resonance may allow a sensitive probe of the GP effect in the H+HD reaction.« less

The Application of LT-Table in TRIZ Contradiction Resolving Process

NASA Astrophysics Data System (ADS)

Wei, Zihui; Li, Qinghai; Wang, Donglin; Tian, Yumei

TRIZ is used to resolve invention problems. ARIZ is the most powerful systematic method which integrates all of TRIZ heuristics. Definition of ideal final result (IFR), identification of contradictions and resource utilization are main lines of ARIZ. But resource searching of ARIZ has fault of blindness. Alexandr sets up mathematical model of transformation of the hereditary information in an invention problem using the theory of catastrophes, and provides method of resource searching using LT-table. The application of LT-table on contradiction resolving is introduced. Resource utilization using LT-table is joined into ARIZ step as an addition of TRIZ, apply this method in separator paper punching machine design.

Mathematical Models to Determine Stable Behavior of Complex Systems

NASA Astrophysics Data System (ADS)

Sumin, V. I.; Dushkin, A. V.; Smolentseva, T. E.

2018-05-01

The paper analyzes a possibility to predict functioning of a complex dynamic system with a significant amount of circulating information and a large number of random factors impacting its functioning. Functioning of the complex dynamic system is described as a chaotic state, self-organized criticality and bifurcation. This problem may be resolved by modeling such systems as dynamic ones, without applying stochastic models and taking into account strange attractors.

Predictions of Crystal Structures from First Principles

DTIC Science & Technology

2007-06-01

RDX crystal in hoped that the problem could be resolved by the molecular dynamics simulations . The fully ab initio development of density functional... Molecular Dynamics Simulations of RDX i.e., without any use of experimental results (except that Crystal the geometry of monomers was derived from X-ray...applied in molecular dynamics simulations of the RDX system, due to its size, is intractable by any high-level ab crystal. We performed isothermal

Photochemical tools to study dynamic biological processes

PubMed Central

Specht, Alexandre; Bolze, Frédéric; Omran, Ziad; Nicoud, Jean-François; Goeldner, Maurice

2009-01-01

Light-responsive biologically active compounds offer the possibility to study the dynamics of biological processes. Phototriggers and photoswitches have been designed, providing the capability to rapidly cause the initiation of wide range of dynamic biological phenomena. We will discuss, in this article, recent developments in the field of light-triggered chemical tools, specially how two-photon excitation, “caged” fluorophores, and the photoregulation of protein activities in combination with time-resolved x-ray techniques should break new grounds in the understanding of dynamic biological processes. PMID:20119482

Spatio-temporal dynamics of a tree-killing beetle and its predator

Treesearch

Aaron S. Weed; Matthew P. Ayres; Andrew M. Liebhold; Ronald F. Billings

2016-01-01

Resolving linkages between local-scale processes and regional-scale patterns in abundance of interacting species is important for understanding long-term population stability across spatial scales. Landscape patterning in consumer population dynamics may be largely the result of interactions between consumers and their predators, or driven by spatial variation in basal...

Earle K. Plyler Prize Lecture: The Three Pillars of Ultrafast Molecular Science - Time, Phase, Intensity

NASA Astrophysics Data System (ADS)

Stolow, Albert

We discuss the probing and control of molecular wavepacket dynamics in the context of three main `pillars' of light-matter interaction: time, phase, intensity. Time: Using short, coherent laser pulses and perturbative matter-field interactions, we study molecular wavepackets with a focus on the ultrafast non-Born-Oppenheimer dynamics, that is, the coupling of electronic and nuclear motions. Time-Resolved Photoelectron Spectroscopy (TRPES) is a powerful ultrafast probe of these processes in polyatomic molecules because it is sensitive both electronic and vibrational dynamics. Ideally, one would like to observe these ultrafast processes from the molecule's point of view - the Molecular Frame - thereby avoiding loss of information due to orientational averaging. This can be achieved by Time-Resolved Coincidence Imaging Spectroscopy (TRCIS) which images 3D recoil vectors of both photofragments and photoelectrons, in coincidence and as a function of time, permitting direct Molecular Frame imaging of valence electronic dynamics during a molecular dynamics. Phase: Using intermediate strength non-perturbative interactions, we apply the second order (polarizability) Non-Resonant Dynamic Stark Effect (NRDSE) to control molecular dynamics without any net absorption of light. NRDSE is also the interaction underlying molecular alignment and applies to field-free 1D of linear molecules and field-free 3D alignment of general (asymmetric) molecules. Using laser alignment, we can transiently fix a molecule in space, yielding a more general approach to direct Molecular Frame imaging of valence electronic dynamics during a chemical reaction. Intensity: In strong (ionizing) laser fields, a new laser-matter physics emerges for polyatomic systems wherein both the single active electron picture and the adiabatic electron response, both implicit in the standard 3-step models, can fail dramatically. This has important consequences for all attosecond strong field spectroscopies of polyatomic molecules, including high harmonic generation (HHG). We discuss an experimental method, Channel-Resolved Above Threshold Ionization (CRATI), which directly unveils the electronic channels participating in the attosecond molecular strong field ionization response [10]. This work was supported by the National Research Council of Canada and the Natural Sciences & Engineering Research Council.

Dynamical photo-induced electronic properties of molecular junctions

NASA Astrophysics Data System (ADS)

Beltako, K.; Michelini, F.; Cavassilas, N.; Raymond, L.

2018-03-01

Nanoscale molecular-electronic devices and machines are emerging as promising functional elements, naturally flexible and efficient, for next-generation technologies. A deeper understanding of carrier dynamics in molecular junctions is expected to benefit many fields of nanoelectronics and power devices. We determine time-resolved charge current flowing at the donor-acceptor interface in molecular junctions connected to metallic electrodes by means of quantum transport simulations. The current is induced by the interaction of the donor with a Gaussian-shape femtosecond laser pulse. Effects of the molecular internal coupling, metal-molecule tunneling, and light-donor coupling on photocurrent are discussed. We then define the time-resolved local density of states which is proposed as an efficient tool to describe the absorbing molecule in contact with metallic electrodes. Non-equilibrium reorganization of hybridized molecular orbitals through the light-donor interaction gives rise to two phenomena: the dynamical Rabi shift and the appearance of Floquet-like states. Such insights into the dynamical photoelectronic structure of molecules are of strong interest for ultrafast spectroscopy and open avenues toward the possibility of analyzing and controlling the internal properties of quantum nanodevices with pump-push photocurrent spectroscopy.

More reliable forecasts with less precise computations: a fast-track route to cloud-resolved weather and climate simulators?

PubMed Central

Palmer, T. N.

2014-01-01

This paper sets out a new methodological approach to solving the equations for simulating and predicting weather and climate. In this approach, the conventionally hard boundary between the dynamical core and the sub-grid parametrizations is blurred. This approach is motivated by the relatively shallow power-law spectrum for atmospheric energy on scales of hundreds of kilometres and less. It is first argued that, because of this, the closure schemes for weather and climate simulators should be based on stochastic–dynamic systems rather than deterministic formulae. Second, as high-wavenumber elements of the dynamical core will necessarily inherit this stochasticity during time integration, it is argued that the dynamical core will be significantly over-engineered if all computations, regardless of scale, are performed completely deterministically and if all variables are represented with maximum numerical precision (in practice using double-precision floating-point numbers). As the era of exascale computing is approached, an energy- and computationally efficient approach to cloud-resolved weather and climate simulation is described where determinism and numerical precision are focused on the largest scales only. PMID:24842038

More reliable forecasts with less precise computations: a fast-track route to cloud-resolved weather and climate simulators?

PubMed

Palmer, T N

2014-06-28

This paper sets out a new methodological approach to solving the equations for simulating and predicting weather and climate. In this approach, the conventionally hard boundary between the dynamical core and the sub-grid parametrizations is blurred. This approach is motivated by the relatively shallow power-law spectrum for atmospheric energy on scales of hundreds of kilometres and less. It is first argued that, because of this, the closure schemes for weather and climate simulators should be based on stochastic-dynamic systems rather than deterministic formulae. Second, as high-wavenumber elements of the dynamical core will necessarily inherit this stochasticity during time integration, it is argued that the dynamical core will be significantly over-engineered if all computations, regardless of scale, are performed completely deterministically and if all variables are represented with maximum numerical precision (in practice using double-precision floating-point numbers). As the era of exascale computing is approached, an energy- and computationally efficient approach to cloud-resolved weather and climate simulation is described where determinism and numerical precision are focused on the largest scales only.

Nonperturbative Quantum Nature of the Dislocation–Phonon Interaction

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

Li, Mingda; Ding, Zhiwei; Meng, Qingping

Despite the long history of dislocation–phonon interaction studies, there are many problems that have not been fully resolved during this development. These include an incompatibility between a perturbative approach and the long-range nature of a dislocation, the relation between static and dynamic scattering, and their capability of dealing with thermal transport phenomena for bulk material only. Here in this paper, by utilizing a fully quantized dislocation field, which we called a “dislon”, a phonon interacting with a dislocation is renormalized as a quasi-phonon, with shifted quasi-phonon energy, and accompanied by a finite quasi-phonon lifetime, which are reducible to classical results.more » A series of outstanding legacy issues including those above can be directly explained within this unified phonon renormalization approach. For instance, a renormalized phonon naturally resolves the decade-long debate between dynamic and static dislocation–phonon scattering approaches, as two limiting cases. In particular, at nanoscale, both the dynamic and static approaches break down, while the present renormalization approach remains valid by capturing the size effect, showing good agreement with lattice dynamics simulations.« less

Computational Models for Nanoscale Fluid Dynamics and Transport Inspired by Nonequilibrium Thermodynamics1

PubMed Central

Radhakrishnan, Ravi; Yu, Hsiu-Yu; Eckmann, David M.; Ayyaswamy, Portonovo S.

2017-01-01

Traditionally, the numerical computation of particle motion in a fluid is resolved through computational fluid dynamics (CFD). However, resolving the motion of nanoparticles poses additional challenges due to the coupling between the Brownian and hydrodynamic forces. Here, we focus on the Brownian motion of a nanoparticle coupled to adhesive interactions and confining-wall-mediated hydrodynamic interactions. We discuss several techniques that are founded on the basis of combining CFD methods with the theory of nonequilibrium statistical mechanics in order to simultaneously conserve thermal equipartition and to show correct hydrodynamic correlations. These include the fluctuating hydrodynamics (FHD) method, the generalized Langevin method, the hybrid method, and the deterministic method. Through the examples discussed, we also show a top-down multiscale progression of temporal dynamics from the colloidal scales to the molecular scales, and the associated fluctuations, hydrodynamic correlations. While the motivation and the examples discussed here pertain to nanoscale fluid dynamics and mass transport, the methodologies presented are rather general and can be easily adopted to applications in convective heat transfer. PMID:28035168

Nonperturbative Quantum Nature of the Dislocation–Phonon Interaction

DOE PAGES

Li, Mingda; Ding, Zhiwei; Meng, Qingping; ...

2017-01-31

Despite the long history of dislocation–phonon interaction studies, there are many problems that have not been fully resolved during this development. These include an incompatibility between a perturbative approach and the long-range nature of a dislocation, the relation between static and dynamic scattering, and their capability of dealing with thermal transport phenomena for bulk material only. Here in this paper, by utilizing a fully quantized dislocation field, which we called a “dislon”, a phonon interacting with a dislocation is renormalized as a quasi-phonon, with shifted quasi-phonon energy, and accompanied by a finite quasi-phonon lifetime, which are reducible to classical results.more » A series of outstanding legacy issues including those above can be directly explained within this unified phonon renormalization approach. For instance, a renormalized phonon naturally resolves the decade-long debate between dynamic and static dislocation–phonon scattering approaches, as two limiting cases. In particular, at nanoscale, both the dynamic and static approaches break down, while the present renormalization approach remains valid by capturing the size effect, showing good agreement with lattice dynamics simulations.« less

Kinematic scaling relations of CALIFA galaxies: A dynamical mass proxy for galaxies across the Hubble sequence.

NASA Astrophysics Data System (ADS)

Aquino-Ortíz, E.; Valenzuela, O.; Sánchez, S. F.; Hernández-Toledo, H.; Ávila-Reese, V.; van de Ven, G.; Rodríguez-Puebla, A.; Zhu, L.; Mancillas, B.; Cano-Díaz, M.; García-Benito, R.

2018-06-01

We used ionized gas and stellar kinematics for 667 spatially resolved galaxies publicly available from the Calar Alto Legacy Integral Field Area survey (CALIFA) 3rd Data Release with the aim of studying kinematic scaling relations as the Tully & Fisher (TF) relation using rotation velocity, Vrot, the Faber & Jackson (FJ) relation using velocity dispersion, σ, and also a combination of Vrot and σ through the SK parameter defined as SK^2 = KV_{rot}^2 + σ ^2 with constant K. Late-type and early-type galaxies reproduce the TF and FJ relations. Some early-type galaxies also follow the TF relation and some late-type galaxies the FJ relation, but always with larger scatter. On the contrary, when we use the SK parameter, all galaxies, regardless of the morphological type, lie on the same scaling relation, showing a tight correlation with the total stellar mass, M⋆. Indeed, we find that the scatter in this relation is smaller or equal to that of the TF and FJ relations. We explore different values of the K parameter without significant differences (slope and scatter) in our final results with respect the case K = 0.5 besides than a small change in the zero point. We calibrate the kinematic SK^2 dynamical mass proxy in order to make it consistent with sophisticated published dynamical models within 0.15 dex. We show that the SK proxy is able to reproduce the relation between the dynamical mass and the stellar mass in the inner regions of galaxies. Our result may be useful in order to produce fast estimations of the central dynamical mass in galaxies and to study correlations in large galaxy surveys.

Transitions between multiple equilibria of paleo climate: a glimpse in to the dynamics of abrupt climate change

NASA Astrophysics Data System (ADS)

Ferreira, David; Marshall, John; Ito, Takamitsu; McGee, David; Moreno-Chamarro, Eduardo

2017-04-01

The dynamics regulating large climatic transitions such as glacial-interglacial cycles or DO events remains a puzzle. Forcings behind these transitions are not robustly identified and potential candidates (e.g. Milankovitch cycles, freshwater perturbations) often appear too weak to explain such dramatic transitions. A potential solution to this long-standing puzzle is that Earth's climate is endowed with multiple equilibrium states of global extent. Such states are commonly found in low-order or conceptual climate models, but it is unclear whether a system as complex as Earth's climate can sustain multiple equilibrium states. Here we report that multiple equilibrium states of the climate system are also possible in a complex, fully dynamical coupled ocean-atmosphere-sea ice GCM with idealized Earth-like geometry, resolved weather systems and a hydrological cycle. In our model, two equilibrium states coexist for the same parameters and external forcings: a Warm climate with a small Northern hemisphere sea ice cap and a large southern one and a Cold climate with large ice caps at both poles. The dynamical states of the Warm and Cold solutions exhibit striking similarities with our present-day climate and the climate of the Last Glacial Maximum, respectively. A carbon cycle model driven by the two dynamical states produces an atmospheric pCO2 draw-down of about 110 pm between the Warm and Cold states, close to Glacial-Interglacial differences found in ice cores. Mechanism controlling the existence of the multiple states and changes in the atmospheric CO2 will be briefly presented. Finally we willdescribe transition experiments from the Cold to the Warm state, focusing on the lead-lags in the system, notably between the Northern and Southern Hemispheres climates.

Prospective time-resolved LCA of fully electric supercap vehicles in Germany.

PubMed

Zimmermann, Benedikt M; Dura, Hanna; Baumann, Manuel J; Weil, Marcel R

2015-07-01

The ongoing transition of the German electricity supply toward a higher share of renewable and sustainable energy sources, called Energiewende in German, has led to dynamic changes in the environmental impact of electricity over the last few years. Prominent scenario studies predict that comparable dynamics will continue in the coming decades, which will further improve the environmental performance of Germany's electricity supply. Life cycle assessment (LCA) is the methodology commonly used to evaluate environmental performance. Previous LCA studies on electric vehicles have shown that the electricity supply for the vehicles' operation is responsible for the major part of their environmental impact. The core question of this study is how the prospective dynamic development of the German electricity mix will affect the impact of electric vehicles operated in Germany and how LCA can be adapted to analyze this impact in a more robust manner. The previously suggested approach of time-resolved LCA, which is located between static and dynamic LCA, is used in this study and compared with several static approaches. Furthermore, the uncertainty issue associated with scenario studies is addressed in general and in relation to time-resolved LCA. Two scenario studies relevant to policy making have been selected, but a moderate number of modifications have been necessary to adapt the data to the requirements of a life cycle inventory. A potential, fully electric vehicle powered by a supercapacitor energy storage system is used as a generic example. The results show that substantial improvements in the environmental repercussions of the electricity supply and, consequentially, of electric vehicles will be achieved between 2020 and 2031 on the basis of the energy mixes predicted in both studies. This study concludes that although scenarios might not be able to predict the future, they should nonetheless be used as data sources in prospective LCA studies, because in many cases historic data appears to be unsuitable for providing realistic information on the future. The time-resolved LCA approach improves the assessment's robustness substantially, especially when nonlinear developments are foreseen in the future scenarios. This allows for a reduction of bias in LCA-based decision making. However, a deeper integration of time-resolved data in the life cycle inventory and the implementation of a more suitable software framework are desirable. The study describes how life cycle assessment's (LCA) robustness can be improved by respecting prospective fluctuations, like the transition of the German electricity mix, in the modeling of the life cycle inventory. It presents a feasible and rather simple process to add time-resolved data to LCA. The study selects 2 different future scenarios from important German studies and processes their data systematically to make them compatible with the requirements of a life cycle inventory. The use of external scenarios as basis for future-oriented LCA is reflected critically. A case study on electric mobility is presented and used to compare historic, prospective static, and prospective time-resolved electricity mix modeling approaches. The case study emphasizes the benefits of time-resolved LCA in direct comparison with the currently used approaches. © 2015 SETAC.

From ab Initio Potential Energy Surfaces to State-Resolved Reactivities: X + H 2O ↔ HX + OH [X = F, Cl, and O( 3P)] Reactions

DOE PAGES

Li, Jun; Jiang, Bin; Song, Hongwei; ...

2015-04-17

Here, we survey the recent advances in theoretical understanding of quantum state resolved dynamics, using the title reactions as examples. It is shown that the progress was made possible by major developments in two areas. First, an accurate analytical representation of many high-level ab initio points over a large configuration space can now be made with high fidelity and the necessary permutation symmetry. The resulting full-dimensional global potential energy surfaces enable dynamical calculations using either quasi-classical trajectory or more importantly quantum mechanical methods. The second advance is the development of accurate and efficient quantum dynamical methods, which are necessary formore » providing a reliable treatment of quantum effects in reaction dynamics such as tunneling, resonances, and zero-point energy. The powerful combination of the two advances has allowed us to achieve a quantitatively accurate characterization of the reaction dynamics, which unveiled rich dynamical features such as steric steering, strong mode specificity, and bond selectivity. The dependence of reactivity on reactant modes can be rationalized by the recently proposed sudden vector projection model, which attributes the mode specificity and bond selectivity to the coupling of reactant modes with the reaction coordinate at the relevant transition state. The deeper insights provided by these theoretical studies have advanced our understanding of reaction dynamics to a new level.« less

Real-time measurement of size-resolved elemental composition ratio for flame synthesized composite nanoparticle aggregates using a tandem SMPS-ICP-OES

PubMed Central

Reed, Nathan; Fang, Jiaxi; Chavalmane, Sanmathi; Biswas, Pratim

2017-01-01

Composite nanoparticles find application in catalysis, drug delivery, and energy storage and require increasingly fine control of their physical properties and composition. While composite nanoparticles have been widely synthesized and characterized, little work has systematically correlated the initial concentration of precursors and the final composition of flame synthesized composite nanoparticles. This relationship is explored in a diffusion flame aerosol reactor by coupling a scanning mobility particle sizer (SMPS) with an inductively coupled plasma optical emission spectrometer (ICP-OES). A framework for studying the relationship between the initial precursor concentrations of different elements and the final nanoparticle composition is explored. The size-resolved elemental composition was measured by directly injecting size-selected fractions of aggregated magnetite and silicon dioxide composite nanoparticles into the ICP-OES plasma. This work showed a correlation between precursor molar ratio and the measured elemental ratio in the mobility size range of 50 to 140 nm. Building on previous work studying size resolved elemental composition of engineered nanoparticles, the analysis is extended to flame synthesized composite nanoparticle aggregates in this work. PMID:28435179

Real-time measurement of size-resolved elemental composition ratio for flame synthesized composite nanoparticle aggregates using a tandem SMPS-ICP-OES.

PubMed

Reed, Nathan; Fang, Jiaxi; Chavalmane, Sanmathi; Biswas, Pratim

2017-01-01

Composite nanoparticles find application in catalysis, drug delivery, and energy storage and require increasingly fine control of their physical properties and composition. While composite nanoparticles have been widely synthesized and characterized, little work has systematically correlated the initial concentration of precursors and the final composition of flame synthesized composite nanoparticles. This relationship is explored in a diffusion flame aerosol reactor by coupling a scanning mobility particle sizer (SMPS) with an inductively coupled plasma optical emission spectrometer (ICP-OES). A framework for studying the relationship between the initial precursor concentrations of different elements and the final nanoparticle composition is explored. The size-resolved elemental composition was measured by directly injecting size-selected fractions of aggregated magnetite and silicon dioxide composite nanoparticles into the ICP-OES plasma. This work showed a correlation between precursor molar ratio and the measured elemental ratio in the mobility size range of 50 to 140 nm. Building on previous work studying size resolved elemental composition of engineered nanoparticles, the analysis is extended to flame synthesized composite nanoparticle aggregates in this work.

Vertical resolution of baroclinic modes in global ocean models

NASA Astrophysics Data System (ADS)

Stewart, K. D.; Hogg, A. McC.; Griffies, S. M.; Heerdegen, A. P.; Ward, M. L.; Spence, P.; England, M. H.

2017-05-01

Improvements in the horizontal resolution of global ocean models, motivated by the horizontal resolution requirements for specific flow features, has advanced modelling capabilities into the dynamical regime dominated by mesoscale variability. In contrast, the choice of the vertical grid remains a subjective choice, and it is not clear that efforts to improve vertical resolution adequately support their horizontal counterparts. Indeed, considering that the bulk of the vertical ocean dynamics (including convection) are parameterized, it is not immediately obvious what the vertical grid is supposed to resolve. Here, we propose that the primary purpose of the vertical grid in a hydrostatic ocean model is to resolve the vertical structure of horizontal flows, rather than to resolve vertical motion. With this principle we construct vertical grids based on their abilities to represent baroclinic modal structures commensurate with the theoretical capabilities of a given horizontal grid. This approach is designed to ensure that the vertical grids of global ocean models complement (and, importantly, to not undermine) the resolution capabilities of the horizontal grid. We find that for z-coordinate global ocean models, at least 50 well-positioned vertical levels are required to resolve the first baroclinic mode, with an additional 25 levels per subsequent mode. High-resolution ocean-sea ice simulations are used to illustrate some of the dynamical enhancements gained by improving the vertical resolution of a 1/10° global ocean model. These enhancements include substantial increases in the sea surface height variance (∼30% increase south of 40°S), the barotropic and baroclinic eddy kinetic energies (up to 200% increase on and surrounding the Antarctic continental shelf and slopes), and the overturning streamfunction in potential density space (near-tripling of the Antarctic Bottom Water cell at 65°S).

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

Graph Theoretic Foundations of Multibody Dynamics Part I: Structural Properties

PubMed Central

Jain, Abhinandan

2011-01-01

This is the first part of two papers that use concepts from graph theory to obtain a deeper understanding of the mathematical foundations of multibody dynamics. The key contribution is the development of a unifying framework that shows that key analytical results and computational algorithms in multibody dynamics are a direct consequence of structural properties and require minimal assumptions about the specific nature of the underlying multibody system. This first part focuses on identifying the abstract graph theoretic structural properties of spatial operator techniques in multibody dynamics. The second part paper exploits these structural properties to develop a broad spectrum of analytical results and computational algorithms. Towards this, we begin with the notion of graph adjacency matrices and generalize it to define block-weighted adjacency (BWA) matrices and their 1-resolvents. Previously developed spatial operators are shown to be special cases of such BWA matrices and their 1-resolvents. These properties are shown to hold broadly for serial and tree topology multibody systems. Specializations of the BWA and 1-resolvent matrices are referred to as spatial kernel operators (SKO) and spatial propagation operators (SPO). These operators and their special properties provide the foundation for the analytical and algorithmic techniques developed in the companion paper. We also use the graph theory concepts to study the topology induced sparsity structure of these operators and the system mass matrix. Similarity transformations of these operators are also studied. While the detailed development is done for the case of rigid-link multibody systems, the extension of these techniques to a broader class of systems (e.g. deformable links) are illustrated. PMID:22102790

The MUSE Hubble Ultra Deep Field Survey. V. Spatially resolved stellar kinematics of galaxies at redshift 0.2 ≲ z ≲ 0.8

NASA Astrophysics Data System (ADS)

Guérou, Adrien; Krajnović, Davor; Epinat, Benoit; Contini, Thierry; Emsellem, Eric; Bouché, Nicolas; Bacon, Roland; Michel-Dansac, Leo; Richard, Johan; Weilbacher, Peter M.; Schaye, Joop; Marino, Raffaella Anna; den Brok, Mark; Erroz-Ferrer, Santiago

2017-11-01

We present spatially resolved stellar kinematic maps, for the first time, for a sample of 17 intermediate redshift galaxies (0.2 ≲ z ≲ 0.8). We used deep MUSE/VLT integral field spectroscopic observations in the Hubble Deep Field South (HDFS) and Hubble Ultra Deep Field (HUDF), resulting from ≈30 h integration time per field, each covering 1' × 1' field of view, with ≈ 0.̋65 spatial resolution. We selected all galaxies brighter than 25 mag in the I band and for which the stellar continuum is detected over an area that is at least two times larger than the spatial resolution. The resulting sample contains mostly late-type disk, main-sequence star-forming galaxies with 108.5 M⊙ ≲ M∗ ≲ 1010.5 M⊙. Using a full-spectrum fitting technique, we derive two-dimensional maps of the stellar and gas kinematics, including the radial velocity V and velocity dispersion σ. We find that most galaxies in the sample are consistent with having rotating stellar disks with roughly constant velocity dispersions and that the second order velocity moments Vrms = √V2+σ2 of the gas and stars, a scaling proxy for the galaxy gravitational potential, compare well to each other. These spatially resolved observations of the stellar kinematics of intermediate redshift galaxies suggest that the regular stellar kinematics of disk galaxies that is observed in the local Universe was already in place 4-7 Gyr ago and that their gas kinematics traces the gravitational potential of the galaxy, thus is not dominated by shocks and turbulent motions. Finally, we build dynamical axisymmetric Jeans models constrained by the derived stellar kinematics for two specific galaxies and derive their dynamical masses. These are in good agreement (within 25%) with those derived from simple exponential disk models based on the gas kinematics. The obtained mass-to-light ratios hint towards dark matter dominated systems within a few effective radii. Based on observations made with ESO telescopes at the La Silla-Paranal Observatory under programmes 094.A-0289(B), 095.A-0010(A), 096.A-0045(A) and 096.A-0045(B).

A high-order time-accurate interrogation method for time-resolved PIV

NASA Astrophysics Data System (ADS)

Lynch, Kyle; Scarano, Fulvio

2013-03-01

A novel method is introduced for increasing the accuracy and extending the dynamic range of time-resolved particle image velocimetry (PIV). The approach extends the concept of particle tracking velocimetry by multiple frames to the pattern tracking by cross-correlation analysis as employed in PIV. The working principle is based on tracking the patterned fluid element, within a chosen interrogation window, along its individual trajectory throughout an image sequence. In contrast to image-pair interrogation methods, the fluid trajectory correlation concept deals with variable velocity along curved trajectories and non-zero tangential acceleration during the observed time interval. As a result, the velocity magnitude and its direction are allowed to evolve in a nonlinear fashion along the fluid element trajectory. The continuum deformation (namely spatial derivatives of the velocity vector) is accounted for by adopting local image deformation. The principle offers important reductions of the measurement error based on three main points: by enlarging the temporal measurement interval, the relative error becomes reduced; secondly, the random and peak-locking errors are reduced by the use of least-squares polynomial fits to individual trajectories; finally, the introduction of high-order (nonlinear) fitting functions provides the basis for reducing the truncation error. Lastly, the instantaneous velocity is evaluated as the temporal derivative of the polynomial representation of the fluid parcel position in time. The principal features of this algorithm are compared with a single-pair iterative image deformation method. Synthetic image sequences are considered with steady flow (translation, shear and rotation) illustrating the increase of measurement precision. An experimental data set obtained by time-resolved PIV measurements of a circular jet is used to verify the robustness of the method on image sequences affected by camera noise and three-dimensional motions. In both cases, it is demonstrated that the measurement time interval can be significantly extended without compromising the correlation signal-to-noise ratio and with no increase of the truncation error. The increase of velocity dynamic range scales more than linearly with the number of frames included for the analysis, which supersedes by one order of magnitude the pair correlation by window deformation. The main factors influencing the performance of the method are discussed, namely the number of images composing the sequence and the polynomial order chosen to represent the motion throughout the trajectory.

High-resolution structure, interactions, and dynamics of self-assembled virus-like partilces

NASA Astrophysics Data System (ADS)

Raviv, Uri; Asor, R.; Ben-Shaul, O.; Oppenheim, A.; Schlicksup, L. C.; Seltzer, L.; Jarrold, M. F.; Zlotnick, A.

Using SAXS, in combination with Monte Carlo simulations, and our unique solution x-ray scattering data analysis program, we resolved at high spatial resolution, the manner by which wtSV40 packages its 5.2kb circular DNA about 20 histone octamers in the virus capsid (Figure 1). This structure, known as a mini-chromosome, is highly dynamic and could not be resolved by microscopy methods. Using time-resolved solution SAXS, stopped-flow, and flow-through setups the assembly process of VP1, the major caspid protein of the SV40 virus, with RNA or DNA to form virus-like particles (VLPs) was studied in msec temporal resolution. By mixing the nucleotides and the capsid protein, virus-like particles formed within 35 msec, in the case of RNA that formed T =1 particles, and within 15 seconds in the case of DNA that formed T =7 particles, similar to wt SV40. The structural changes leading to the particle formation were followed in detail. More recently, we have extended this work to study the assembly of HBV virus-like particles.

Regioisomeric and enantiomeric analyses of 24 designer cathinones and phenethylamines using ultra high performance liquid chromatography and capillary electrophoresis with added cyclodextrins.

PubMed

Li, Li; Lurie, Ira S

2015-09-01

DESIGNER: phenethylamines (PEAs) and cathinones have been encountered worldwide. Complete characterization of these substances can be challenging due to their chirality and variably substituted phenyl rings. In this study, 24 PEAs and cathinones were analyzed by ultra high performance liquid chromatography with photo diode array detection (UHPLC-PDA) on a variety of stationary phases, and by capillary electrophoresis on a dynamically coated capillary with PDA detection (CE-PDA). In the UHPLC-PDA study, a BEH Phenyl column resolved 18 of the 24 regioisomers in 8min, with good discrimination of the PEAs. In contrast, capillary zone electrophoresis (CZE) on a dynamically coated capillary partially or baseline resolved only 10 of the 24 regioisomers, but with improved discrimination of mono-substituted cathinones. A second series of CE-PDA experiments using 80mM (2-hydroxypropyl)-β-cyclodextrin (HP-β-CD) in the run buffer resolved all 24 regioisomers and all but two sets of enantiomers within 18min. Five illicit samples were successfully analyzed using the described methods. Published by Elsevier Ireland Ltd.

A priori testing of subgrid-scale models for large-eddy simulation of the atmospheric boundary layer

NASA Astrophysics Data System (ADS)

Juneja, Anurag; Brasseur, James G.

1996-11-01

Subgrid-scale models are generally developed assuming homogeneous isotropic turbulence with the filter cutoff lying in the inertial range. In the surface layer and capping inversion regions of the atmospheric boundary layer, the turbulence is strongly anisotropic and, in general, influenced by both buoyancy and shear. Furthermore, the integral scale motions are under-resolved in these regions. Herein we perform direct numerical simulations of shear and buoyancy-generated homogeneous anisotropic turbulence to compute and analyze the actual subgrid-resolved-scale (SGS-RS) dynamics as the filter cutoff moves into the energy-containing scales. These are compared with the SGS-RS dynamics predicted by Smagorinsky-based models with a focus on motivating improved closures. We find that, in general, the underlying assumption of such models, that the anisotropic part of the subgrid stress tensor be aligned with the resolved strain rate tensor, is a poor approximation. Similarly, we find poor alignment between the actual and predicted stress divergence, and find low correlations between the actual and modeled subgrid-scale contribution to the pressure and pressure gradient. Details will be given in the talk.

Thermodynamic properties of water solvating biomolecular surfaces

NASA Astrophysics Data System (ADS)

Heyden, Matthias

Changes in the potential energy and entropy of water molecules hydrating biomolecular interfaces play a significant role for biomolecular solubility and association. Free energy perturbation and thermodynamic integration methods allow calculations of free energy differences between two states from simulations. However, these methods are computationally demanding and do not provide insights into individual thermodynamic contributions, i.e. changes in the solvent energy or entropy. Here, we employ methods to spatially resolve distributions of hydration water thermodynamic properties in the vicinity of biomolecular surfaces. This allows direct insights into thermodynamic signatures of the hydration of hydrophobic and hydrophilic solvent accessible sites of proteins and small molecules and comparisons to ideal model surfaces. We correlate dynamic properties of hydration water molecules, i.e. translational and rotational mobility, to their thermodynamics. The latter can be used as a guide to extract thermodynamic information from experimental measurements of site-resolved water dynamics. Further, we study energy-entropy compensations of water at different hydration sites of biomolecular surfaces. This work is supported by the Cluster of Excellence RESOLV (EXC 1069) funded by the Deutsche Forschungsgemeinschaft.

Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites.

PubMed

Straus, Daniel B; Hurtado Parra, Sebastian; Iotov, Natasha; Gebhardt, Julian; Rappe, Andrew M; Subotnik, Joseph E; Kikkawa, James M; Kagan, Cherie R

2016-10-05

Quantum and dielectric confinement effects in 2D hybrid perovskites create excitons with a binding energy exceeding 150 meV. We exploit the large exciton binding energy to study exciton and carrier dynamics as well as electron-phonon coupling in hybrid perovskites using absorption and photoluminescence (PL) spectroscopies. At temperatures below 75 K, we resolve splitting of the excitonic absorption and PL into multiple regularly-spaced resonances every 40-46 meV, consistent with electron-phonon coupling to phonons located on the organic cation. We also resolve resonances with a 14 meV spacing, in accord with coupling to phonons with mixed organic and inorganic character, and these assignments are supported by density-functional theory calculations. Hot exciton PL and time-resolved PL measurements show that vibrational relaxation occurs on a picosecond timescale competitive with that for PL. At temperatures above 75 K, excitonic absorption and PL exhibit homogeneous broadening. While absorption remains homogeneous, PL becomes inhomogeneous below 75K, which we speculate is caused by the formation and subsequent dynamics of a polaronic exciton.

Excitation-resolved multispectral method for imaging pharmacokinetic parameters in dynamic fluorescent molecular tomography

NASA Astrophysics Data System (ADS)

Chen, Maomao; Zhou, Yuan; Su, Han; Zhang, Dong; Luo, Jianwen

2017-04-01

Imaging of the pharmacokinetic parameters in dynamic fluorescence molecular tomography (DFMT) can provide three-dimensional metabolic information for biological studies and drug development. However, owing to the ill-posed nature of the FMT inverse problem, the relatively low quality of the parametric images makes it difficult to investigate the different metabolic processes of the fluorescent targets with small distances. An excitation-resolved multispectral DFMT method is proposed; it is based on the fact that the fluorescent targets with different concentrations show different variations in the excitation spectral domain and can be considered independent signal sources. With an independent component analysis method, the spatial locations of different fluorescent targets can be decomposed, and the fluorescent yields of the targets at different time points can be recovered. Therefore, the metabolic process of each component can be independently investigated. Simulations and phantom experiments are carried out to evaluate the performance of the proposed method. The results demonstrated that the proposed excitation-resolved multispectral method can effectively improve the reconstruction accuracy of the parametric images in DFMT.

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.

Vibrationally-Resolved Kinetic Isotope Effects in the Proton-Transfer Dynamics of Ground-State Tropolone

NASA Astrophysics Data System (ADS)

Chew, Kathryn; Vealey, Zachary; Vaccaro, Patrick

2015-06-01

The vibrational and isotopic dependence of the hindered (tunneling-mediated) proton-transfer reaction taking place in the ground electronic state ( X1{A}1) of monodeuterated tropolone (TrOD) has been explored under ambient (bulk-gas) conditions by applying two-color variants of resonant four-wave mixing (RFWM) spectroscopy in conjunction with polarization-resolved detection schemes designed to alleviate spectral complexity and facilitate rovibrational assignments. Full rotation-tunneling analyses of high-resolution spectral profiles acquired for the fundamental and first-overtone bands of a reaction-promoting O-D\\cdotsO deformation/ring-breathing mode, νb{36}(a1), were performed, thereby extracting refined structural and dynamical information that affords benchmarks for the quantitative interpretation of tunneling-induced signatures found in long-range scans of X1{A}1 vibrational levels residing below Etilde{X}vib = 1700 wn}. Observed kinetic isotope effects, which reflect changes in both reaction kinematics and vibrational displacements, will be discussed, with high-level quantum-chemical calculations serving to elucidate state-resolved propensities for proton transfer in TrOH and TrOD.

Effect of the N-terminal residues on the quaternary dynamics of human adult hemoglobin

NASA Astrophysics Data System (ADS)

Chang, Shanyan; Mizuno, Misao; Ishikawa, Haruto; Mizutani, Yasuhisa

2016-05-01

The protein dynamics of human hemoglobin following ligand photolysis was studied by time-resolved resonance Raman spectroscopy. The time-resolved spectra of two kinds of recombinant hemoglobin expressed in Escherichia coli, normal recombinant hemoglobin and the α(V1M)/β(V1M) double mutant, were compared with those of human adult hemoglobin (HbA) purified from blood. A frequency shift of the iron-histidine stretching [ν(Fe-His)] band was observed in the time-resolved spectra of all three hemoglobin samples, indicative of tertiary and quaternary changes in the protein following photolysis. The spectral changes of the α(V1M)/β(V1M) double mutant were distinct from those of HbA in the tens of microseconds region, whereas the spectral changes of normal recombinant hemoglobin were similar to those of HbA isolated from blood. These results demonstrated that a structural change in the N-termini is involved in the second step of the quaternary structure change of hemoglobin. We discuss the implications of these results for understanding the allosteric pathway of HbA.

Quasilinear models through the lens of resolvent analysis

NASA Astrophysics Data System (ADS)

McKeon, Beverley; Chini, Greg

2017-11-01

Quasilinear (QL) and generalized quasilinear (GQL) analyses, e.g. Marston et al., also variously described as statistical state dynamics models, e.g., Farrell et al., restricted nonlinear models, e.g. Thomas et al., or 2D/3C models, e.g. Gayme et al., have achieved considerable success in recovering the mean velocity profile for a range of turbulent flows. In QL approaches, the portion of the velocity field that can be represented as streamwise constant, i.e. with streamwise wavenumber kx = 0 , is fully resolved, while the streamwise-varying dynamics are linearized about the streamwise-constant field; that is, only those nonlinear interactions that drive the streamwise-constant field are retained, and the non-streamwise constant ``fluctuation-fluctuation'' interactions are ignored. Here, we show how these QL approaches can be reformulated in terms of the closed-loop resolvent analysis of McKeon & Sharma (2010), which enables us to identify reasons for their evident success as well as algorithms for their efficient computation. The support of ONR through Grant No. N00014-17-2307 is gratefully acknowledged.

Magnetic field effects on spectrally resolved lifetime of on-line oxygen monitoring using magneto-optic probes

NASA Astrophysics Data System (ADS)

Mermut, O.; Gallant, P.; Le Bouch, N.; Leclair, S.; Noiseux, I.; Vernon, M.; Morin, J.-F.; Diamond, K.; Patterson, M. S.; Samkoe, K.; Pogue, B.

2009-02-01

Multimodal agents that serve as both probes for contrast and light-activated effectors of cellular processes in diseased tissue were developed. These agents were introduced into multicellular tumor spheroids (3D tissue models) and in the chorioallantoic membrane (CAM) of a chicken embryo. The luminescence decay was examined using a novel technique involving a spectrally-resolved fluorescence lifetime apparatus integrated with a weak electromagnet. A spectrallyresolved lifetime setup was used to identify magneto-optic species sensitive to magnetic field effects and distinguish from background emissions. We demonstrate that the applied magnetic fields can alter reaction rates and product distribution of some dyes detected by time- and spectrally-resolved luminescence changes. We will discuss the use of exogenous magneto-optical probes taken up in tumors to both induce phototoxicity, a process that is governed by complex and dynamically evolving mechanisms involving reactive oxygen species, and monitor treatment progress. The magnetic field enhancement, measured over a range of weak fields (0-300 mT) is correlated to oxygenation and may be used to monitor dynamic changes occurring due to oxygen consumption over the course of photodynamic therapy. Such online measurements provide the possibility to derive real-time information about response to treatment via monitoring magnetic field enhancement/suppression of the time-resolved, spectrally-resolved luminescence of the probe at the site of the treatment directly. Magnetic perturbation of lifetime can serve as a status reporter, providing optical feedback of oxygen-mediated treatments in situ and allowing for real-time adjustment of a phototherapy treatment plan.

Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

NASA Astrophysics Data System (ADS)

Brauße, Felix; Goldsztejn, Gildas; Amini, Kasra; Boll, Rebecca; Bari, Sadia; Bomme, Cédric; Brouard, Mark; Burt, Michael; de Miranda, Barbara Cunha; Düsterer, Stefan; Erk, Benjamin; Géléoc, Marie; Geneaux, Romain; Gentleman, Alexander S.; Guillemin, Renaud; Ismail, Iyas; Johnsson, Per; Journel, Loïc; Kierspel, Thomas; Köckert, Hansjochen; Küpper, Jochen; Lablanquie, Pascal; Lahl, Jan; Lee, Jason W. L.; Mackenzie, Stuart R.; Maclot, Sylvain; Manschwetus, Bastian; Mereshchenko, Andrey S.; Mullins, Terence; Olshin, Pavel K.; Palaudoux, Jérôme; Patchkovskii, Serguei; Penent, Francis; Piancastelli, Maria Novella; Rompotis, Dimitrios; Ruchon, Thierry; Rudenko, Artem; Savelyev, Evgeny; Schirmel, Nora; Techert, Simone; Travnikova, Oksana; Trippel, Sebastian; Underwood, Jonathan G.; Vallance, Claire; Wiese, Joss; Simon, Marc; Holland, David M. P.; Marchenko, Tatiana; Rouzée, Arnaud; Rolles, Daniel

2018-04-01

Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I ) is investigated by ionization above the iodine 4 d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

Alignment of time-resolved data from high throughput experiments.

PubMed

Abidi, Nada; Franke, Raimo; Findeisen, Peter; Klawonn, Frank

2016-12-01

To better understand the dynamics of the underlying processes in cells, it is necessary to take measurements over a time course. Modern high-throughput technologies are often used for this purpose to measure the behavior of cell products like metabolites, peptides, proteins, [Formula: see text]RNA or mRNA at different points in time. Compared to classical time series, the number of time points is usually very limited and the measurements are taken at irregular time intervals. The main reasons for this are the costs of the experiments and the fact that the dynamic behavior usually shows a strong reaction and fast changes shortly after a stimulus and then slowly converges to a certain stable state. Another reason might simply be missing values. It is common to repeat the experiments and to have replicates in order to carry out a more reliable analysis. The ideal assumptions that the initial stimulus really started exactly at the same time for all replicates and that the replicates are perfectly synchronized are seldom satisfied. Therefore, there is a need to first adjust or align the time-resolved data before further analysis is carried out. Dynamic time warping (DTW) is considered as one of the common alignment techniques for time series data with equidistant time points. In this paper, we modified the DTW algorithm so that it can align sequences with measurements at different, non-equidistant time points with large gaps in between. This type of data is usually known as time-resolved data characterized by irregular time intervals between measurements as well as non-identical time points for different replicates. This new algorithm can be easily used to align time-resolved data from high-throughput experiments and to come across existing problems such as time scarcity and existing noise in the measurements. We propose a modified method of DTW to adapt requirements imposed by time-resolved data by use of monotone cubic interpolation splines. Our presented approach provides a nonlinear alignment of two sequences that neither need to have equi-distant time points nor measurements at identical time points. The proposed method is evaluated with artificial as well as real data. The software is available as an R package tra (Time-Resolved data Alignment) which is freely available at: http://public.ostfalia.de/klawonn/tra.zip .

The heart of parenting: Parent HR dynamics and negative parenting while resolving conflict with child.

PubMed

Zhang, Xutong; Cui, Lixian; Han, Zhuo Rachel; Yan, Jia

2017-03-01

The current study examined parent heart rate (HR) dynamic changing patterns and their links to observed negative parenting (i.e., emotional unavailability and psychological control) during a parent-child conflict resolution task among 150 parent-child dyads (child age ranged from 6 to 12 years, Mage = 8.54 ± 1.67). Parent HR was obtained from electrocardiogram (ECG) data collected during the parent-child conflict resolution task. Negative parenting was coded offline based on the video recording of the same task. Results revealed that emotionally sensitive parents during the task showed greater HR increases while discussing a conflict and greater HR decreases while resolving the conflict, whereas emotionally unavailable parents showed no changes in HR. However, parent psychological control was not associated with HR dynamics during the task. These findings indicated the physiological underpinnings of parent emotional sensitivity and responsiveness during parent-child interactions. The potential association between HR baseline levels and parenting behaviors was also discussed. (PsycINFO Database Record (c) 2017 APA, all rights reserved).

Fast, label-free super-resolution live-cell imaging using rotating coherent scattering (ROCS) microscopy

NASA Astrophysics Data System (ADS)

Jünger, Felix; Olshausen, Philipp V.; Rohrbach, Alexander

2016-07-01

Living cells are highly dynamic systems with cellular structures being often below the optical resolution limit. Super-resolution microscopes, usually based on fluorescence cell labelling, are usually too slow to resolve small, dynamic structures. We present a label-free microscopy technique, which can generate thousands of super-resolved, high contrast images at a frame rate of 100 Hertz and without any post-processing. The technique is based on oblique sample illumination with coherent light, an approach believed to be not applicable in life sciences because of too many interference artefacts. However, by circulating an incident laser beam by 360° during one image acquisition, relevant image information is amplified. By combining total internal reflection illumination with dark-field detection, structures as small as 150 nm become separable through local destructive interferences. The technique images local changes in refractive index through scattered laser light and is applied to living mouse macrophages and helical bacteria revealing unexpected dynamic processes.

Protein analysis by time-resolved measurements with an electro-switchable DNA chip

PubMed Central

Langer, Andreas; Hampel, Paul A.; Kaiser, Wolfgang; Knezevic, Jelena; Welte, Thomas; Villa, Valentina; Maruyama, Makiko; Svejda, Matej; Jähner, Simone; Fischer, Frank; Strasser, Ralf; Rant, Ulrich

2013-01-01

Measurements in stationary or mobile phases are fundamental principles in protein analysis. Although the immobilization of molecules on solid supports allows for the parallel analysis of interactions, properties like size or shape are usually inferred from the molecular mobility under the influence of external forces. However, as these principles are mutually exclusive, a comprehensive characterization of proteins usually involves a multi-step workflow. Here we show how these measurement modalities can be reconciled by tethering proteins to a surface via dynamically actuated nanolevers. Short DNA strands, which are switched by alternating electric fields, are employed as capture probes to bind target proteins. By swaying the proteins over nanometre amplitudes and comparing their motional dynamics to a theoretical model, the protein diameter can be quantified with Angström accuracy. Alterations in the tertiary protein structure (folding) and conformational changes are readily detected, and even post-translational modifications are revealed by time-resolved molecular dynamics measurements. PMID:23839273

Annually resolved North Atlantic marine climate over the last millennium

NASA Astrophysics Data System (ADS)

Reynolds, D. J.; Scourse, J. D.; Halloran, P. R.; Nederbragt, A. J.; Wanamaker, A. D.; Butler, P. G.; Richardson, C. A.; Heinemeier, J.; Eiríksson, J.; Knudsen, K. L.; Hall, I. R.

2016-12-01

Owing to the lack of absolutely dated oceanographic information before the modern instrumental period, there is currently significant debate as to the role played by North Atlantic Ocean dynamics in previous climate transitions (for example, Medieval Climate Anomaly-Little Ice Age, MCA-LIA). Here we present analyses of a millennial-length, annually resolved and absolutely dated marine δ18O archive. We interpret our record of oxygen isotope ratios from the shells of the long-lived marine bivalve Arctica islandica (δ18O-shell), from the North Icelandic shelf, in relation to seawater density variability and demonstrate that solar and volcanic forcing coupled with ocean circulation dynamics are key drivers of climate variability over the last millennium. During the pre-industrial period (AD 1000-1800) variability in the sub-polar North Atlantic leads changes in Northern Hemisphere surface air temperatures at multi-decadal timescales, indicating that North Atlantic Ocean dynamics played an active role in modulating the response of the atmosphere to solar and volcanic forcing.

Fast, label-free super-resolution live-cell imaging using rotating coherent scattering (ROCS) microscopy

PubMed Central

Jünger, Felix; Olshausen, Philipp v.; Rohrbach, Alexander

2016-01-01

Living cells are highly dynamic systems with cellular structures being often below the optical resolution limit. Super-resolution microscopes, usually based on fluorescence cell labelling, are usually too slow to resolve small, dynamic structures. We present a label-free microscopy technique, which can generate thousands of super-resolved, high contrast images at a frame rate of 100 Hertz and without any post-processing. The technique is based on oblique sample illumination with coherent light, an approach believed to be not applicable in life sciences because of too many interference artefacts. However, by circulating an incident laser beam by 360° during one image acquisition, relevant image information is amplified. By combining total internal reflection illumination with dark-field detection, structures as small as 150 nm become separable through local destructive interferences. The technique images local changes in refractive index through scattered laser light and is applied to living mouse macrophages and helical bacteria revealing unexpected dynamic processes. PMID:27465033

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.

Photon echo spectroscopy reveals structure-dynamics relationships in carotenoids

NASA Astrophysics Data System (ADS)

Christensson, N.; Polivka, T.; Yartsev, A.; Pullerits, T.

2009-06-01

Based on simultaneous analysis of the frequency-resolved transient grating, peak shift, and echo width signals, we present a model for the third-order optical response of carotenoids including population dynamics and system-bath interactions. Our frequency-resolved photon echo experiments show that the model needs to incorporate the excited-state absorption from both the S2 and the S1 states. We apply our model to analyze the experimental results on astaxanthin and lycopene, aiming to elucidate the relation between structure and system-bath interactions. Our analysis allows us to relate structural motifs to changes in the energy-gap correlation functions. We find that the terminal rings of astaxanthin lead to increased coupling between slow molecular motions and the electronic transition. We also find evidence for stronger coupling to higher frequency overdamped modes in astaxanthin, pointing to the importance of the functional groups in providing coupling to fluctuations influencing the dynamics in the passage through the conical intersection governing the S2-S1 relaxation.

Femtosecond electron imaging of defect-modulated phonon dynamics

PubMed Central

Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.

2016-01-01

Precise manipulation and control of coherent lattice oscillations via nanostructuring and phonon-wave interference has the potential to significantly impact a broad array of technologies and research areas. Resolving the dynamics of individual phonons in defect-laden materials presents an enormous challenge, however, owing to the interdependent nanoscale and ultrafast spatiotemporal scales. Here we report direct, real-space imaging of the emergence and evolution of acoustic phonons at individual defects in crystalline WSe2 and Ge. Via bright-field imaging with an ultrafast electron microscope, we are able to image the sub-picosecond nucleation and the launch of wavefronts at step edges and resolve dispersion behaviours during propagation and scattering. We discover that the appearance of speed-of-sound (for example, 6 nm ps−1) wavefronts are influenced by spatially varying nanoscale strain fields, taking on the appearance of static bend contours during propagation. These observations provide unprecedented insight into the roles played by individual atomic and nanoscale features on acoustic-phonon dynamics. PMID:27079790

Ribosome dynamics and tRNA movement by time-resolved electron cryomicroscopy.

PubMed

Fischer, Niels; Konevega, Andrey L; Wintermeyer, Wolfgang; Rodnina, Marina V; Stark, Holger

2010-07-15

The translocation step of protein synthesis entails large-scale rearrangements of the ribosome-transfer RNA (tRNA) complex. Here we have followed tRNA movement through the ribosome during translocation by time-resolved single-particle electron cryomicroscopy (cryo-EM). Unbiased computational sorting of cryo-EM images yielded 50 distinct three-dimensional reconstructions, showing the tRNAs in classical, hybrid and various novel intermediate states that provide trajectories and kinetic information about tRNA movement through the ribosome. The structures indicate how tRNA movement is coupled with global and local conformational changes of the ribosome, in particular of the head and body of the small ribosomal subunit, and show that dynamic interactions between tRNAs and ribosomal residues confine the path of the tRNAs through the ribosome. The temperature dependence of ribosome dynamics reveals a surprisingly flat energy landscape of conformational variations at physiological temperature. The ribosome functions as a Brownian machine that couples spontaneous conformational changes driven by thermal energy to directed movement.

Dynamic Computation of Change Operations in Version Management of Business Process Models

NASA Astrophysics Data System (ADS)

Küster, Jochen Malte; Gerth, Christian; Engels, Gregor

Version management of business process models requires that changes can be resolved by applying change operations. In order to give a user maximal freedom concerning the application order of change operations, position parameters of change operations must be computed dynamically during change resolution. In such an approach, change operations with computed position parameters must be applicable on the model and dependencies and conflicts of change operations must be taken into account because otherwise invalid models can be constructed. In this paper, we study the concept of partially specified change operations where parameters are computed dynamically. We provide a formalization for partially specified change operations using graph transformation and provide a concept for their applicability. Based on this, we study potential dependencies and conflicts of change operations and show how these can be taken into account within change resolution. Using our approach, a user can resolve changes of business process models without being unnecessarily restricted to a certain order.

Watching proteins function with picosecond X-ray crystallography and molecular dynamics simulations.

NASA Astrophysics Data System (ADS)

Anfinrud, Philip

2006-03-01

Time-resolved electron density maps of myoglobin, a ligand-binding heme protein, have been stitched together into movies that unveil with < 2-å spatial resolution and 150-ps time-resolution the correlated protein motions that accompany and/or mediate ligand migration within the hydrophobic interior of a protein. A joint analysis of all-atom molecular dynamics (MD) calculations and picosecond time-resolved X-ray structures provides single-molecule insights into mechanisms of protein function. Ensemble-averaged MD simulations of the L29F mutant of myoglobin following ligand dissociation reproduce the direction, amplitude, and timescales of crystallographically-determined structural changes. This close agreement with experiments at comparable resolution in space and time validates the individual MD trajectories, which identify and structurally characterize a conformational switch that directs dissociated ligands to one of two nearby protein cavities. This unique combination of simulation and experiment unveils functional protein motions and illustrates at an atomic level relationships among protein structure, dynamics, and function. In collaboration with Friedrich Schotte and Gerhard Hummer, NIH.

Time-resolved photoelectron spectroscopy of adenosine and adenosine monophosphate photodeactivation dynamics in water microjets

NASA Astrophysics Data System (ADS)

Williams, Holly L.; Erickson, Blake A.; Neumark, Daniel M.

2018-05-01

The excited state relaxation dynamics of adenosine and adenosine monophosphate were studied at multiple excitation energies using femtosecond time-resolved photoelectron spectroscopy in a liquid water microjet. At pump energies of 4.69-4.97 eV, the lowest ππ* excited state, S1, was accessed and its decay dynamics were probed via ionization at 6.20 eV. By reversing the role of the pump and probe lasers, a higher-lying ππ* state was excited at 6.20 eV and its time-evolving photoelectron spectrum was monitored at probe energies of 4.69-4.97 eV. The S1 ππ* excited state was found to decay with a lifetime ranging from ˜210 to 250 fs in adenosine and ˜220 to 250 fs in adenosine monophosphate. This lifetime drops with increasing pump photon energy. Signal from the higher-lying ππ* excited state decayed on a time scale of ˜320 fs and was measureable only in adenosine monophosphate.

State-to-state rotational energy-transfer measurements in the nu(2) = 1 state of ammonia by infrared-infrared double resonance

NASA Technical Reports Server (NTRS)

Abel, Bernd; Coy, Stephen L.; Klaassen, Jody J.; Steinfeld, Jeffrey I.

1992-01-01

The state-resolved rotational (R-R, R-T) energy transfer in (N-14)H3 (for NH3-NH3 and NH3-Ar collisions) was studied using an IR double-resonance laser spectroscopic technique. Measurements of both the total rate of depopulation by collisions, and the rates of transfer into specific final rovibrational states (v,J,K) were performed using time-resolved tunable diode laser absorption spectroscopy. A kinetic master-equation analysis of time-resolved level populatons was carried out, yielding state-to-state rate constants and propensity rules for NH3-NH3 and NH3-Ar collisions.

Minimum resolvable power contrast model

NASA Astrophysics Data System (ADS)

Qian, Shuai; Wang, Xia; Zhou, Jingjing

2018-01-01

Signal-to-noise ratio and MTF are important indexs to evaluate the performance of optical systems. However,whether they are used alone or joint assessment cannot intuitively describe the overall performance of the system. Therefore, an index is proposed to reflect the comprehensive system performance-Minimum Resolvable Radiation Performance Contrast (MRP) model. MRP is an evaluation model without human eyes. It starts from the radiance of the target and the background, transforms the target and background into the equivalent strips,and considers attenuation of the atmosphere, the optical imaging system, and the detector. Combining with the signal-to-noise ratio and the MTF, the Minimum Resolvable Radiation Performance Contrast is obtained. Finally the detection probability model of MRP is given.

Sensitivity simulations of superparameterised convection in a general circulation model

NASA Astrophysics Data System (ADS)

Rybka, Harald; Tost, Holger

2015-04-01

Cloud Resolving Models (CRMs) covering a horizontal grid spacing from a few hundred meters up to a few kilometers have been used to explicitly resolve small-scale and mesoscale processes. Special attention has been paid to realistically represent cloud dynamics and cloud microphysics involving cloud droplets, ice crystals, graupel and aerosols. The entire variety of physical processes on the small-scale interacts with the larger-scale circulation and has to be parameterised on the coarse grid of a general circulation model (GCM). Since more than a decade an approach to connect these two types of models which act on different scales has been developed to resolve cloud processes and their interactions with the large-scale flow. The concept is to use an ensemble of CRM grid cells in a 2D or 3D configuration in each grid cell of the GCM to explicitly represent small-scale processes avoiding the use of convection and large-scale cloud parameterisations which are a major source for uncertainties regarding clouds. The idea is commonly known as superparameterisation or cloud-resolving convection parameterisation. This study presents different simulations of an adapted Earth System Model (ESM) connected to a CRM which acts as a superparameterisation. Simulations have been performed with the ECHAM/MESSy atmospheric chemistry (EMAC) model comparing conventional GCM runs (including convection and large-scale cloud parameterisations) with the improved superparameterised EMAC (SP-EMAC) modeling one year with prescribed sea surface temperatures and sea ice content. The sensitivity of atmospheric temperature, precipiation patterns, cloud amount and types is observed changing the embedded CRM represenation (orientation, width, no. of CRM cells, 2D vs. 3D). Additionally, we also evaluate the radiation balance with the new model configuration, and systematically analyse the impact of tunable parameters on the radiation budget and hydrological cycle. Furthermore, the subgrid variability (individual CRM cell output) is analysed in order to illustrate the importance of a highly varying atmospheric structure inside a single GCM grid box. Finally, the convective transport of Radon is observed comparing different transport procedures and their influence on the vertical tracer distribution.

Dynamics of monochromatically generated nonequilibrium phonons in LaF3:Pr3+

NASA Astrophysics Data System (ADS)

Tolbert, W. A.; Dennis, W. M.; Yen, W. M.

1990-07-01

The temporal evolution of nonequilibrium phonon populations in LaF3:Pr3+ is investigated at low temperatures (1.8 K) utilizing pulsed, tunable, monochromatic generation and time-resolved, tunable, narrow-band detection. High occupation number, narrow-band phonon populations are generated via far-infrared pumping of defect-induced one-phonon absorption. Time-resolved, frequency-selective detection is provided by optical sideband absorption. Nonequilibrium phonon decay times are measured and attributed to anharmonic decay.

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

NASA Astrophysics Data System (ADS)

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

2016-07-01

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

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

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

Kang, Zhitao; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0245; Banishev, Alexandr A.

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

Spectral characteristics of time resolved magnonic spin Seebeck effect

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

Etesami, S. R.; Chotorlishvili, L.; Berakdar, J.

2015-09-28

Spin Seebeck effect (SSE) holds promise for new spintronic devices with low-energy consumption. The underlying physics, essential for a further progress, is yet to be fully clarified. This study of the time resolved longitudinal SSE in the magnetic insulator yttrium iron garnet concludes that a substantial contribution to the spin current stems from small wave-vector subthermal exchange magnons. Our finding is in line with the recent experiment by S. R. Boona and J. P. Heremans [Phys. Rev. B 90, 064421 (2014)]. Technically, the spin-current dynamics is treated based on the Landau-Lifshitz-Gilbert equation also including magnons back-action on thermal bath, whilemore » the formation of the time dependent thermal gradient is described self-consistently via the heat equation coupled to the magnetization dynamics.« less

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.

Conformational States of the Rapana thomasiana Hemocyanin and Its Substructures Studied by Dynamic Light Scattering and Time-Resolved Fluorescence Spectroscopy

PubMed Central

Georgieva, Dessislava; Schwark, Daniel; Nikolov, Peter; Idakieva, Krassimira; Parvanova, Katja; Dierks, Karsten; Genov, Nicolay; Betzel, Christian

2005-01-01

Hemocyanins are dioxygen-transporting proteins freely dissolved in the hemolymph of mollusks and arthropods. Dynamic light scattering and time-resolved fluorescence measurements show that the oxygenated and apo-forms of the Rapana thomasiana hemocyanin, its structural subunits RtH1 and RtH2, and those of the functional unit RtH2e, exist in different conformations. The oxygenated respiratory proteins are less compact and more asymmetric than the respective apo-forms. Different conformational states were also observed for the R. thomasiana hemocyanin in the absence and presence of an allosteric regulator. The results are in agreement with a molecular mechanism for cooperative dioxygen binding in molluscan hemocyanins including transfer of conformational changes from one functional unit to another. PMID:15533921

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.

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.

Ocean dynamics in the Nordic Seas using satellite altimetry

NASA Technical Reports Server (NTRS)

Pettersson, Lasse H.; Johannessen, O. M.; Olaussen, T. I.

1991-01-01

The main objective of this TOPEX/POSEIDON project is to integrate the accurately measured sea surface topography, as resolved by both TOPEX/POSEIDON radar altimeters, into the above-mentioned quantitative studies of the short- and long-term variations in the mesoscale ocean dynamics of the Nordic Seas south of 66 deg N. This implies: (1) comparison and validation of the capability to resolve the general basin-scale circulation and the mesoscale variability by, respectively, radar altimeters and numerical ocean circulation models; (2) calibration and validation of the altimeter-derived sea surface topography against in situ measurements from research vessels and moorings, particularly under extreme wind and wave conditions; and (3) improved monitoring and understanding of the flux variations between the North Atlantic and the Nordic Seas, both on the short and seasonal time scales.

Mesoscopic modelling and simulation of soft matter.

PubMed

Schiller, Ulf D; Krüger, Timm; Henrich, Oliver

2017-12-20

The deformability of soft condensed matter often requires modelling of hydrodynamical aspects to gain quantitative understanding. This, however, requires specialised methods that can resolve the multiscale nature of soft matter systems. We review a number of the most popular simulation methods that have emerged, such as Langevin dynamics, dissipative particle dynamics, multi-particle collision dynamics, sometimes also referred to as stochastic rotation dynamics, and the lattice-Boltzmann method. We conclude this review with a short glance at current compute architectures for high-performance computing and community codes for soft matter simulation.

Multiscale equation-free algorithms for molecular dynamics

NASA Astrophysics Data System (ADS)

Abi Mansour, Andrew

Molecular dynamics is a physics-based computational tool that has been widely employed to study the dynamics and structure of macromolecules and their assemblies at the atomic scale. However, the efficiency of molecular dynamics simulation is limited because of the broad spectrum of timescales involved. To overcome this limitation, an equation-free algorithm is presented for simulating these systems using a multiscale model cast in terms of atomistic and coarse-grained variables. Both variables are evolved in time in such a way that the cross-talk between short and long scales is preserved. In this way, the coarse-grained variables guide the evolution of the atom-resolved states, while the latter provide the Newtonian physics for the former. While the atomistic variables are evolved using short molecular dynamics runs, time advancement at the coarse-grained level is achieved with a scheme that uses information from past and future states of the system while accounting for both the stochastic and deterministic features of the coarse-grained dynamics. To complete the multiscale cycle, an atom-resolved state consistent with the updated coarse-grained variables is recovered using algorithms from mathematical optimization. This multiscale paradigm is extended to nanofluidics using concepts from hydrodynamics, and it is demonstrated for macromolecular and nanofluidic systems. A toolkit is developed for prototyping these algorithms, which are then implemented within the GROMACS simulation package and released as an open source multiscale simulator.

Spectrally- and Time-Resolved Sum Frequency Generation (STiR-SFG): a new tool for ultrafast hydrogen bond dynamics at interfaces.

NASA Astrophysics Data System (ADS)

Benderskii, Alexander; Bordenyuk, Andrey; Weeraman, Champika

2006-03-01

The recently developed spectrally- and time-resolved Sum Frequency Generation (STiR-SFG) is a surface-selective 3-wave mixing (IR+visible) spectroscopic technique capable of measuring ultrafast spectral evolution of vibrational coherences. A detailed description of this measurement will be presented, and a noniterative method or deconvolving the laser pulses will be introduced to obtain the molecular response function. STiR-SFG, combined with the frequency-domain SFG spectroscopy, was applied to study hydrogen bonding dynamics at aqueous interfaces (D2O/CaF2). Spectral dynamics of the OD-stretch on the 50-150 fs time scale provides real-time observation of ultrafast H-bond rearrangement. Tuning the IR wavelength to the blue or red side of the OD-stretch transition, we selectively monitor the dynamics of different sub-ensembles in the distribution of the H-bond structures. The blue-side excitation (weaker H-bonding) shows monotonic red-shift of the OD-frequency. In contrast, the red-side excitation (stronger H-bonding structures) produces a blue-shift and a recursion, which may indicate the presence of an underdamped intermolecular mode of interfacial water. Effect of electrolyte concentration on the H-bond dynamics will be discussed.

Direct evidence of atomic-scale structural fluctuations in catalyst nanoparticles.

PubMed

Lin, Pin Ann; Gomez-Ballesteros, Jose L; Burgos, Juan C; Balbuena, Perla B; Natarajan, Bharath; Sharma, Renu

2017-05-01

Rational catalyst design requires an atomic scale mechanistic understanding of the chemical pathways involved in the catalytic process. A heterogeneous catalyst typically works by adsorbing reactants onto its surface, where the energies for specific bonds to dissociate and/or combine with other species (to form desired intermediate or final products) are lower. Here, using the catalytic growth of single-walled carbon nanotubes (SWCNTs) as a prototype reaction, we show that the chemical pathway may in-fact involve the entire catalyst particle, and can proceed via the fluctuations in the formation and decomposition of metastable phases in the particle interior. We record in situ and at atomic resolution, the dynamic phase transformations occurring in a Cobalt catalyst nanoparticle during SWCNT growth, using a state-of-the-art environmental transmission electron microscope (ETEM). The fluctuations in catalyst carbon content are quantified by the automated, atomic-scale structural analysis of the time-resolved ETEM images and correlated with the SWCNT growth rate. We find the fluctuations in the carbon concentration in the catalyst nanoparticle and the fluctuations in nanotube growth rates to be of complementary character. These findings are successfully explained by reactive molecular dynamics (RMD) simulations that track the spatial and temporal evolution of the distribution of carbon atoms within and on the surface of the catalyst particle. We anticipate that our approach combining real-time, atomic-resolution image analysis and molecular dynamics simulations will facilitate catalyst design, improving reaction efficiencies and selectivity towards the growth of desired structure.

Dynamic measurements and simulations of airborne picolitre-droplet coalescence in holographic optical tweezers

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

Bzdek, Bryan R.; Reid, Jonathan P., E-mail: j.p.reid@bristol.ac.uk; Collard, Liam

We report studies of the coalescence of pairs of picolitre aerosol droplets manipulated with holographic optical tweezers, probing the shape relaxation dynamics following coalescence by simultaneously monitoring the intensity of elastic backscattered light (EBL) from the trapping laser beam (time resolution on the order of 100 ns) while recording high frame rate camera images (time resolution <10 μs). The goals of this work are to: resolve the dynamics of droplet coalescence in holographic optical traps; assign the origin of key features in the time-dependent EBL intensity; and validate the use of the EBL alone to precisely determine droplet surface tensionmore » and viscosity. For low viscosity droplets, two sequential processes are evident: binary coalescence first results from the overlap of the optical traps on the time scale of microseconds followed by the recapture of the composite droplet in an optical trap on the time scale of milliseconds. As droplet viscosity increases, the relaxation in droplet shape eventually occurs on the same time scale as recapture, resulting in a convoluted evolution of the EBL intensity that inhibits quantitative determination of the relaxation time scale. Droplet coalescence was simulated using a computational framework to validate both experimental approaches. The results indicate that time-dependent monitoring of droplet shape from the EBL intensity allows for robust determination of properties such as surface tension and viscosity. Finally, the potential of high frame rate imaging to examine the coalescence of dissimilar viscosity droplets is discussed.« less

Dynamical implantation of objects in the Kuiper Belt

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

Brasil, P. I. O.; Nesvorný, D.; Gomes, R. S., E-mail: pedro_brasil87@hotmail.com, E-mail: davidn@boulder.swri.edu, E-mail: rodney@on.br

Several models have been suggested in the past to describe the dynamical formation of hot Kuiper Belt objects (hereafter Hot Classicals or HCs for short). Here, we discuss a dynamical mechanism that allows orbits to evolve from the primordial planetesimal disk at ≲ 35 AU to reach the orbital region now occupied by HCs. We performed three different sets of numerical simulations to illustrate this mechanism. Two of these simulations were based on modern theories for the early evolution of the solar system (the Nice and jumping-Jupiter models). The third simulation was performed with the purpose of increasing the resolutionmore » at 41-46 AU. The common aspect of these simulations is that Neptune scatters planetesimals from ≲ 35 AU to >40 AU and then undergoes a long phase of slow residual migration. Our results show that to reach an HC orbit, a scattered planetesimal needs to be captured in a mean motion resonance (MMR) with Neptune where the perihelion distance rises due to the Kozai resonance (which occurs in MMRs even for moderate inclinations). Finally, while Neptune is still migrating, the planetesimal is released from the MMR on a stable HC orbit. We show that the orbital distribution of HCs expected from this process provides a reasonable match to observations. The capture efficiency and the mass deposited into the HC region appears to be sensitive to the maximum eccentricity reached by Neptune during the planetary instability phase. Additional work will be needed to resolve this dependency in detail.« less

Decay of aftershock density with distance does not indicate triggering by dynamic stress

USGS Publications Warehouse

Richards-Dinger, K.; Stein, R.S.; Toda, S.

2010-01-01

Resolving whether static or dynamic stress triggers most aftershocks and subsequent mainshocks is essential to understand earthquake interaction and to forecast seismic hazard. Felzer and Brodsky examined the distance distribution of earthquakes occurring in the first five minutes after 2 ≤ M  M  M ≥ 2 aftershocks showed a uniform power-law decay with slope −1.35 out to 50 km from the mainshocks. From this they argued that the distance decay could be explained only by dynamic triggering. Here we propose an alternative explanation for the decay, and subject their hypothesis to a series of tests, none of which it passes. At distances more than 300 m from the 2 ≤  M< 3 mainshocks, the seismicity decay 5 min before the mainshocks is indistinguishable from the decay five minutes afterwards, indicating that the mainshocks have no effect at distances outside their static triggering range. Omori temporal decay, the fundamental signature of aftershocks, is absent at distances exceeding 10 km from the mainshocks. Finally, the distance decay is found among aftershocks that occur before the arrival of the seismic wave front from the mainshock, which violates causality. We argue that Felzer and Brodsky implicitly assume that the first of two independent aftershocks along a fault rupture triggers the second, and that the first of two shocks in a creep- or intrusion-driven swarm triggers the second, when this need not be the case.

Space-by-time manifold representation of dynamic facial expressions for emotion categorization

PubMed Central

Delis, Ioannis; Chen, Chaona; Jack, Rachael E.; Garrod, Oliver G. B.; Panzeri, Stefano; Schyns, Philippe G.

2016-01-01

Visual categorization is the brain computation that reduces high-dimensional information in the visual environment into a smaller set of meaningful categories. An important problem in visual neuroscience is to identify the visual information that the brain must represent and then use to categorize visual inputs. Here we introduce a new mathematical formalism—termed space-by-time manifold decomposition—that describes this information as a low-dimensional manifold separable in space and time. We use this decomposition to characterize the representations used by observers to categorize the six classic facial expressions of emotion (happy, surprise, fear, disgust, anger, and sad). By means of a Generative Face Grammar, we presented random dynamic facial movements on each experimental trial and used subjective human perception to identify the facial movements that correlate with each emotion category. When the random movements projected onto the categorization manifold region corresponding to one of the emotion categories, observers categorized the stimulus accordingly; otherwise they selected “other.” Using this information, we determined both the Action Unit and temporal components whose linear combinations lead to reliable categorization of each emotion. In a validation experiment, we confirmed the psychological validity of the resulting space-by-time manifold representation. Finally, we demonstrated the importance of temporal sequencing for accurate emotion categorization and identified the temporal dynamics of Action Unit components that cause typical confusions between specific emotions (e.g., fear and surprise) as well as those resolving these confusions. PMID:27305521

Excitation mechanisms in 1 mJ picosecond laser induced low pressure He plasma and the resulting spectral quality enhancement

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

Idris, Nasrullah; Lahna, Kurnia; Abdulmadjid, Syahrun Nur

2015-06-14

We report in this paper the results of an experimental study on the spectral and dynamical characteristics of plasma emission induced by 1 mJ picoseconds (ps) Nd-YAG laser using spatially resolved imaging and time resolved measurement of the emission intensities of copper sample. This study has provided the experimental evidence concerning the dynamical characteristics of the excitation mechanisms in various stages of the plasma formation, which largely consolidate the basic scenarios of excitation processes commonly accepted so far. However, it is also clearly shown that the duration of the shock wave excitation process induced by ps laser pulses is muchmore » shorter than those observed in laser induced breakdown spectroscopy employing nanosecond laser at higher output energy. This allows the detection of atomic emission due exclusively to He assisted excitation in low pressure He plasma by proper gating of the detection time. Furthermore, the triplet excited state associated with He I 587.6 nm is shown to be the one most likely involved in the process responsible for the excellent spectral quality as evidenced by its application to spectrochemical analysis of a number of samples. The use of very low energy laser pulses also leads to minimal destructive effect marked by the resulted craters of merely about 10 μm diameter and only 10 nm deep. It is especially noteworthy that the excellent emission spectrum of deuterium detected from D-doped titanium sample is free of spectral interference from the undesirable ubiquitous water molecules without a precleaning procedure as applied previously and yielding an impressive detection limit of less than 10 μg/g. Finally, the result of this study also shows a promising application to depth profiling of impurity distribution in the sample investigated.« less

Temporally and Spatially Resolved x-ray Fluorescence Measurements of in-situ Drug Concentration in Metered-Dose Inhaler Sprays

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

Duke, Daniel J.; Kastengren, Alan L.; Mason-Smith, Nicholas

Drug concentration measurements in MDI sprays are typically performed using particle filtration or laser scattering. These techniques are ineffective in proximity to the nozzle, making it difficult to determine how factors such as nozzle design will affect the precipitation of co-solvent droplets in solution-based MDIs, and the final particle distribution. In optical measurements, scattering from the constituents is difficult to separate. We present a novel technique to directly measure drug distribution. A focused x-ray beam was used to stimulate x-ray fluorescence from the bromine in a solution containing 85% HFA, 15% ethanol co-solvent, and 1 / IPBr. Instantaneous concentration measurementsmore » were obtained with 1 ms temporal resolution and 5 spatial resolution, providing information in a region that is inaccessible to many other diagnostics. The drug remains homogeneously mixed over time, but was found to be higher at the centerline than at the periphery. This may have implications for oropharyngeal deposition in vivo. Measurements in the dynamic, turbulent region of MDIs allow us to understand the physical links between formulation, inspiration, and geometry on final particle size and distribution. This will ultimately lead to a better understanding of how MDI design can be improved to enhance respirable fraction.« less

Substellar Companions to weak-line TTauri Stars

NASA Astrophysics Data System (ADS)

Brandner, W.; Alcala, J. M.; Covino, E.; Frink, S.

1997-05-01

Weak-line TTauri stars, contrary to classical TTauri stars, no longer possess massive circumstellar disks. In weak-line TTauri stars, the circumstellar matter was either accreted onto the TTauri star or has been redistributed. Disk instabilities in the outer disk might result in the formation of brown dwarfs and giant planets. Based on photometric and spectroscopic studies of ROSAT sources, we have selected an initial sample of 200 weak-line TTauri stars in the Chamaeleon T association and the Scorpius Centaurus OB association. In the course of follow-up observations we identified visual and spectroscopic binary stars and excluded them from our final list, as the complex dynamics and gravitational interaction in binary systems might aggravate or even completely inhibit the formation of planets (depending on physical separation of the binary components and their mass-ratio). The membership of individual stars to the associations was established from proper motion studies and radial velocity surveys. Our final sample consists of 70 single weak-line TTauri stars. We have initiated a program to spatially RESOLVE young brown dwarfs and young giant planets as companions to single weak-line TTauri stars using adaptive optics at the ESO 3.6m telescope and HST/NICMOS. In this poster we describe the observing strategy and present first results of our adaptive optics observations.

A spatially resolved pyrometer for measuring the blackbody temperature of a warm dense plasma

DOE PAGES

Coleman, Joshua Eugene

2016-12-30

A pyrometer has been developed to spatially resolve the blackbody temperature of a radiatively cooling warm dense plasma. The pyrometer is composed of a lens coupled fiber array, Czerny-Turner visible spectrometer, and an intensified gated CCD for the detector. The radiatively cooling warm dense plasma is generated by a ~100-ns-long intense relativistic electron bunch with an energy of 19.1 MeV and a current of 0.2 kA interacting with 100-μm-thick low-Z foils. The continuum spectrum is measured over 250 nm with a low groove density grating. These plasmas emit visible light or blackbody radiation on relatively long time scales (~0.1 tomore » 100 μs). Finally, we presented the diagnostic layout, calibration, and proof-of-principle measurement of a radiatively cooling aluminum plasma, which includes a spatially resolved temperature gradient and the ability to temporally resolve it also.« less

The time resolved SBS and SRS research in heavy water and its application in CARS

NASA Astrophysics Data System (ADS)

Liu, Jinbo; Gai, Baodong; Yuan, Hong; Sun, Jianfeng; Zhou, Xin; Liu, Di; Xia, Xusheng; Wang, Pengyuan; Hu, Shu; Chen, Ying; Guo, Jingwei; Jin, Yuqi; Sang, Fengting

2018-05-01

We present the time-resolved character of stimulated Brillouin scattering (SBS) and backward stimulated Raman scattering (BSRS) in heavy water and its application in Coherent Anti-Stokes Raman Scattering (CARS) technique. A nanosecond laser from a frequency-doubled Nd: YAG laser is introduced into a heavy water cell, to generate SBS and BSRS beams. The SBS and BSRS beams are collinear, and their time resolved characters are studied by a streak camera, experiment show that they are ideal source for an alignment-free CARS system, and the time resolved property of SBS and BSRS beams could affect the CARS efficiency significantly. By inserting a Dye cuvette to the collinear beams, the time-overlapping of SBS and BSRS could be improved, and finally the CARS efficiency is increased, even though the SBS energy is decreased. Possible methods to improve the efficiency of this CARS system are discussed too.

Spectral reconstruction analysis for enhancing signal-to-noise in time-resolved spectroscopies

NASA Astrophysics Data System (ADS)

Wilhelm, Michael J.; Smith, Jonathan M.; Dai, Hai-Lung

2015-09-01

We demonstrate a new spectral analysis for the enhancement of the signal-to-noise ratio (SNR) in time-resolved spectroscopies. Unlike the simple linear average which produces a single representative spectrum with enhanced SNR, this Spectral Reconstruction analysis (SRa) improves the SNR (by a factor of ca. 0 . 6 √{ n } ) for all n experimentally recorded time-resolved spectra. SRa operates by eliminating noise in the temporal domain, thereby attenuating noise in the spectral domain, as follows: Temporal profiles at each measured frequency are fit to a generic mathematical function that best represents the temporal evolution; spectra at each time are then reconstructed with data points from the fitted profiles. The SRa method is validated with simulated control spectral data sets. Finally, we apply SRa to two distinct experimentally measured sets of time-resolved IR emission spectra: (1) UV photolysis of carbonyl cyanide and (2) UV photolysis of vinyl cyanide.

Matching time and spatial scales of rapid solidification: dynamic TEM experiments coupled to CALPHAD-informed phase-field simulations

NASA Astrophysics Data System (ADS)

Perron, Aurelien; Roehling, John D.; Turchi, Patrice E. A.; Fattebert, Jean-Luc; McKeown, Joseph T.

2018-01-01

A combination of dynamic transmission electron microscopy (DTEM) experiments and CALPHAD-informed phase-field simulations was used to study rapid solidification in Cu-Ni thin-film alloys. Experiments—conducted in the DTEM—consisted of in situ laser melting and determination of the solidification kinetics by monitoring the solid-liquid interface and the overall microstructure evolution (time-resolved measurements) during the solidification process. Modelling of the Cu-Ni alloy microstructure evolution was based on a phase-field model that included realistic Gibbs energies and diffusion coefficients from the CALPHAD framework (thermodynamic and mobility databases). DTEM and post mortem experiments highlighted the formation of microsegregation-free columnar grains with interface velocities varying from ˜0.1 to ˜0.6 m s-1. After an ‘incubation’ time, the velocity of the planar solid-liquid interface accelerated until solidification was complete. In addition, a decrease of the temperature gradient induced a decrease in the interface velocity. The modelling strategy permitted the simulation (in 1D and 2D) of the solidification process from the initially diffusion-controlled to the nearly partitionless regimes. Finally, results of DTEM experiments and phase-field simulations (grain morphology, solute distribution, and solid-liquid interface velocity) were consistent at similar time (μs) and spatial scales (μm).

Catching ghosts with a coarse net: use and abuse of spatial sampling data in detecting synchronization

PubMed Central

2017-01-01

Synchronization of population dynamics in different habitats is a frequently observed phenomenon. A common mathematical tool to reveal synchronization is the (cross)correlation coefficient between time courses of values of the population size of a given species where the population size is evaluated from spatial sampling data. The corresponding sampling net or grid is often coarse, i.e. it does not resolve all details of the spatial configuration, and the evaluation error—i.e. the difference between the true value of the population size and its estimated value—can be considerable. We show that this estimation error can make the value of the correlation coefficient very inaccurate or even irrelevant. We consider several population models to show that the value of the correlation coefficient calculated on a coarse sampling grid rarely exceeds 0.5, even if the true value is close to 1, so that the synchronization is effectively lost. We also observe ‘ghost synchronization’ when the correlation coefficient calculated on a coarse sampling grid is close to 1 but in reality the dynamics are not correlated. Finally, we suggest a simple test to check the sampling grid coarseness and hence to distinguish between the true and artifactual values of the correlation coefficient. PMID:28202589

Resolving the neural dynamics of visual and auditory scene processing in the human brain: a methodological approach

PubMed Central

Teng, Santani

2017-01-01

In natural environments, visual and auditory stimulation elicit responses across a large set of brain regions in a fraction of a second, yielding representations of the multimodal scene and its properties. The rapid and complex neural dynamics underlying visual and auditory information processing pose major challenges to human cognitive neuroscience. Brain signals measured non-invasively are inherently noisy, the format of neural representations is unknown, and transformations between representations are complex and often nonlinear. Further, no single non-invasive brain measurement technique provides a spatio-temporally integrated view. In this opinion piece, we argue that progress can be made by a concerted effort based on three pillars of recent methodological development: (i) sensitive analysis techniques such as decoding and cross-classification, (ii) complex computational modelling using models such as deep neural networks, and (iii) integration across imaging methods (magnetoencephalography/electroencephalography, functional magnetic resonance imaging) and models, e.g. using representational similarity analysis. We showcase two recent efforts that have been undertaken in this spirit and provide novel results about visual and auditory scene analysis. Finally, we discuss the limits of this perspective and sketch a concrete roadmap for future research. This article is part of the themed issue ‘Auditory and visual scene analysis’. PMID:28044019

A control-oriented dynamic wind farm flow model: “WFSim”

NASA Astrophysics Data System (ADS)

Boersma, S.; Gebraad, P. M. O.; Vali, M.; Doekemeijer, B. M.; van Wingerden, J. W.

2016-09-01

In this paper, we present and extend the dynamic medium fidelity control-oriented Wind Farm Simulator (WFSim) model. WFSim resolves flow fields in wind farms in a horizontal, two dimensional plane. It is based on the spatially and temporally discretised two dimensional Navier-Stokes equations and the continuity equation and solves for a predefined grid and wind farm topology. The force on the flow field generated by turbines is modelled using actuator disk theory. Sparsity in system matrices is exploited in WFSim, which enables a relatively fast flow field computation. The extensions to WFSim we present in this paper are the inclusion of a wake redirection model, a turbulence model and a linearisation of the nonlinear WFSim model equations. The first is important because it allows us to carry out wake redirection control and simulate situations with an inflow that is misaligned with the rotor plane. The wake redirection model is validated against a theoretical wake centreline known from literature. The second extension makes WFSim more realistic because it accounts for wake recovery. The amount of recovery is validated using a high fidelity simulation model Simulator fOr Wind Farm Applications (SOWFA) for a two turbine test case. Finally, a linearisation is important since it allows the application of more standard analysis, observer and control techniques.

Quantum state-to-state dynamics for the quenching process of Br(2P1/2) + H2(v(i) = 0, 1, j(i) = 0).

PubMed

Xie, Changjian; Jiang, Bin; Xie, Daiqian; Sun, Zhigang

2012-03-21

Quantum state-to-state dynamics for the quenching process Br((2)P(1/2)) + H(2)(v(i) = 0, 1, j(i) = 0) → Br((2)P(3/2)) + H(2)(v(f), j(f)) has been studied based on two-state model on the recent coupled potential energy surfaces. It was found that the quenching probabilities have some oscillatory structures due to the interference of reflected flux in the Br((2)P(1/2)) + H(2) and Br((2)P(3/2)) + H(2) channels by repulsive potential in the near-resonant electronic-to-vibrational energy transfer process. The final vibrational state resolved integral cross sections were found to be dominated by the quenching process Br((2)P(1/2)) + H(2)(v) → Br((2)P(3/2)) + H(2)(v+1) and the nonadiabatic reaction probabilities for Br((2)P(1/2)) + H(2)(v = 0, 1, j(i) = 0) are quite small, which are consistent with previous theoretical and experimental results. Our calculated total quenching rate constant for Br((2)P(1/2)) + H(2)(v(i) = 0, j(i) = 0) at room temperature is in good agreement with the available experimental data. © 2012 American Institute of Physics

Resolving the neural dynamics of visual and auditory scene processing in the human brain: a methodological approach.

PubMed

Cichy, Radoslaw Martin; Teng, Santani

2017-02-19

In natural environments, visual and auditory stimulation elicit responses across a large set of brain regions in a fraction of a second, yielding representations of the multimodal scene and its properties. The rapid and complex neural dynamics underlying visual and auditory information processing pose major challenges to human cognitive neuroscience. Brain signals measured non-invasively are inherently noisy, the format of neural representations is unknown, and transformations between representations are complex and often nonlinear. Further, no single non-invasive brain measurement technique provides a spatio-temporally integrated view. In this opinion piece, we argue that progress can be made by a concerted effort based on three pillars of recent methodological development: (i) sensitive analysis techniques such as decoding and cross-classification, (ii) complex computational modelling using models such as deep neural networks, and (iii) integration across imaging methods (magnetoencephalography/electroencephalography, functional magnetic resonance imaging) and models, e.g. using representational similarity analysis. We showcase two recent efforts that have been undertaken in this spirit and provide novel results about visual and auditory scene analysis. Finally, we discuss the limits of this perspective and sketch a concrete roadmap for future research.This article is part of the themed issue 'Auditory and visual scene analysis'. © 2017 The Authors.

Dynamic pictures of membrane proteins in two-dimensional crystal, lipid bilayer and detergent as revealed by site-directed solid-state 13C NMR.

PubMed

Saitô, Hazime

2004-11-01

We have compared site-directed 13C solid-state NMR spectra of [3-13C]Ala- and/or [1-13C]Val-labeled membrane proteins, including bacteriorhodopsin (bR), pharaonis phoborhodopin (ppR), its cognate transducer (pHtrII) and Escherichia coli diacylglycerol kinase (DGK), in two-dimensional (2D) crystal, lipid bilayers, and detergent. Restricted fluctuation motions of these membrane proteins due to oligomerization of bR by specific protein-protein interactions in the 2D crystalline lattice or protein complex between ppR and pHtrII provide the most favorable environment to yield well-resolved, fully visible 13C NMR signals for [3-13C]Ala-labeled proteins. In contrast, several signals from such membrane proteins were broadened or lost owing to interference of inherent fluctuation frequencies (10(4)-10(5)Hz) with frequency of either proton decoupling or magic angle spinning, if their 13C NMR spectra were recorded as a monomer in lipid bilayers at ambient temperature. The presence of such protein dynamics is essential for the respective proteins to achieve their own biological functions. Finally, spectral broadening found for bR and DGK in detergents were discussed.

Modeling High-Impact Weather and Climate: Lessons From a Tropical Cyclone Perspective

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

Done, James; Holland, Greg; Bruyere, Cindy

2013-10-19

Although the societal impact of a weather event increases with the rarity of the event, our current ability to assess extreme events and their impacts is limited by not only rarity but also by current model fidelity and a lack of understanding of the underlying physical processes. This challenge is driving fresh approaches to assess high-impact weather and climate. Recent lessons learned in modeling high-impact weather and climate are presented using the case of tropical cyclones as an illustrative example. Through examples using the Nested Regional Climate Model to dynamically downscale large-scale climate data the need to treat bias inmore » the driving data is illustrated. Domain size, location, and resolution are also shown to be critical and should be guided by the need to: include relevant regional climate physical processes; resolve key impact parameters; and to accurately simulate the response to changes in external forcing. The notion of sufficient model resolution is introduced together with the added value in combining dynamical and statistical assessments to fill out the parent distribution of high-impact parameters. Finally, through the example of a tropical cyclone damage index, direct impact assessments are resented as powerful tools that distill complex datasets into concise statements on likely impact, and as highly effective communication devices.« less

Quantitative sampling of conformational heterogeneity of a DNA hairpin using molecular dynamics simulations and ultrafast fluorescence spectroscopy

PubMed Central

Voltz, Karine; Léonard, Jérémie; Touceda, Patricia Tourón; Conyard, Jamie; Chaker, Ziyad; Dejaegere, Annick; Godet, Julien; Mély, Yves; Haacke, Stefan; Stote, Roland H.

2016-01-01

Molecular dynamics (MD) simulations and time resolved fluorescence (TRF) spectroscopy were combined to quantitatively describe the conformational landscape of the DNA primary binding sequence (PBS) of the HIV-1 genome, a short hairpin targeted by retroviral nucleocapsid proteins implicated in the viral reverse transcription. Three 2-aminopurine (2AP) labeled PBS constructs were studied. For each variant, the complete distribution of fluorescence lifetimes covering 5 orders of magnitude in timescale was measured and the populations of conformers experimentally observed to undergo static quenching were quantified. A binary quantification permitted the comparison of populations from experimental lifetime amplitudes to populations of aromatically stacked 2AP conformers obtained from simulation. Both populations agreed well, supporting the general assumption that quenching of 2AP fluorescence results from pi-stacking interactions with neighboring nucleobases and demonstrating the success of the proposed methodology for the combined analysis of TRF and MD data. Cluster analysis of the latter further identified predominant conformations that were consistent with the fluorescence decay times and amplitudes, providing a structure-based rationalization for the wide range of fluorescence lifetimes. Finally, the simulations provided evidence of local structural perturbations induced by 2AP. The approach presented is a general tool to investigate fine structural heterogeneity in nucleic acid and nucleoprotein assemblies. PMID:26896800

Cda Science Today and in Cassini's Final Three Years

NASA Astrophysics Data System (ADS)

Srama, R.

2014-12-01

Today, the German-lead Cosmic Dust Analyser (CDA) is operated continuously for 10 years in orbit around Saturn. The first discovery of CDA related to Saturn was the measurement of nanometer sized dust particles ejected by to interplanetary space with speeds higher than 100 km/s. Their origin and composition was analysed and and their dynamical studies showed a strong link to the conditions of the solar wind plasma flow. A recent surprising result was, that stream particles stem from the interior of Enceladus. Since 2004 CDA measured millions of dust impacts characterizing the dust environment of Saturn. The instrument showed strong evidence for ice geysers located at the south pole of Saturn's moon Enceladus in 2005. Later, a detailed compositional analysis of the salt-rich water ice grains in Saturn's E ring system lead to the discovery of liquid water below the icy crust connected to an ocean at depth feeding the icy jets. CDA was even capable to derive a spatially resolved compositional profile of the plume during close Enceladus flybys. A determination of the dust-magnetosphere interaction and the discovery of the extended E ring allowed the definition of a dynamical dust model of Saturn's E ring describing the observed properties. The measured dust density profiles in the dense E ring revealed geometric asymmetries.In the final three years CDA performs exogenous and interstellar dust campaigns, studies of the composition and origin of Saturn's main rings by unique ring ejecta measurements, long-duration nano-dust stream observations, high-resolution maps of small moon orbit crossings, studies of the dust cloud around Dione and studies of the E-ring interaction with the large moon Titan.

Femtosecond dynamics in hydrogen-bonded solvents

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

Castner, E.W. Jr.; Chang, Y.J.

1993-09-01

We present results on the ultrafast dynamics of pure hydrogen-bonding solvents, obtained using femtosecond Fourier-transform optical-heterodyne-detected, Raman-induced Kerr effect spectroscopy. Solvent systems we have studied include the formamides, water, ethylene glycol, and acetic acid. Inertial and diffusive motions are clearly resolved. We comment on the effect that such ultrafast solvent motions have on chemical reactions in solution.

Ultrafast Multi-Level Logic Gates with Spin-Valley Coupled Polarization Anisotropy in Monolayer MoS2

PubMed Central

Wang, Yu-Ting; Luo, Chih-Wei; Yabushita, Atsushi; Wu, Kaung-Hsiung; Kobayashi, Takayoshi; Chen, Chang-Hsiao; Li, Lain-Jong

2015-01-01

The inherent valley-contrasting optical selection rules for interband transitions at the K and K′ valleys in monolayer MoS2 have attracted extensive interest. Carriers in these two valleys can be selectively excited by circularly polarized optical fields. The comprehensive dynamics of spin valley coupled polarization and polarized exciton are completely resolved in this work. Here, we present a systematic study of the ultrafast dynamics of monolayer MoS2 including spin randomization, exciton dissociation, free carrier relaxation, and electron-hole recombination by helicity- and photon energy-resolved transient spectroscopy. The time constants for these processes are 60 fs, 1 ps, 25 ps, and ~300 ps, respectively. The ultrafast dynamics of spin polarization, valley population, and exciton dissociation provides the desired information about the mechanism of radiationless transitions in various applications of 2D transition metal dichalcogenides. For example, spin valley coupled polarization provides a promising way to build optically selective-driven ultrafast valleytronics at room temperature. Therefore, a full understanding of the ultrafast dynamics in MoS2 is expected to provide important fundamental and technological perspectives. PMID:25656222

Quantum-state-resolved CO2 scattering dynamics at the gas-liquid interface: dependence on incident angle.

PubMed

Perkins, Bradford G; Nesbitt, David J

2007-08-09

Energy transfer dynamics at the gas-liquid interface have been probed with a supersonic molecular beam of CO2 and a clean perfluorinated-liquid surface in vacuum. High-resolution infrared spectroscopy measures both the rovibrational state populations and the translational distributions for the scattered CO2 flux. The present study investigates collision dynamics as a function of incident angle (thetainc = 0 degrees, 30 degrees, 45 degrees, and 60 degrees), where column-integrated quantum state populations are detected along the specular-scattering direction (i.e., thetascat approximately thetainc). Internal state rovibrational and Doppler translational distributions in the scattered CO2 yield clear evidence for nonstatistical behavior, providing quantum-state-resolved support for microscopic branching of the gas-liquid collision dynamics into multiple channels. Specifically, the data are remarkably well described by a two-temperature model, which can be associated with both a trapping desorption (TD) component emerging at the surface temperature (Trot approximately TS) and an impulsive scattering (IS) component appearing at hyperthermal energies (Trot > TS). The branching ratio between the TD and IS channels is found to depend strongly on thetainc, with the IS component growing dramatically with increasingly steeper angle of incidence.

High-resolution time series of Pseudomonas aeruginosa gene expression and rhamnolipid secretion through growth curve synchronization.

PubMed

van Ditmarsch, Dave; Xavier, João B

2011-06-17

Online spectrophotometric measurements allow monitoring dynamic biological processes with high-time resolution. Contrastingly, numerous other methods require laborious treatment of samples and can only be carried out offline. Integrating both types of measurement would allow analyzing biological processes more comprehensively. A typical example of this problem is acquiring quantitative data on rhamnolipid secretion by the opportunistic pathogen Pseudomonas aeruginosa. P. aeruginosa cell growth can be measured by optical density (OD600) and gene expression can be measured using reporter fusions with a fluorescent protein, allowing high time resolution monitoring. However, measuring the secreted rhamnolipid biosurfactants requires laborious sample processing, which makes this an offline measurement. Here, we propose a method to integrate growth curve data with endpoint measurements of secreted metabolites that is inspired by a model of exponential cell growth. If serial diluting an inoculum gives reproducible time series shifted in time, then time series of endpoint measurements can be reconstructed using calculated time shifts between dilutions. We illustrate the method using measured rhamnolipid secretion by P. aeruginosa as endpoint measurements and we integrate these measurements with high-resolution growth curves measured by OD600 and expression of rhamnolipid synthesis genes monitored using a reporter fusion. Two-fold serial dilution allowed integrating rhamnolipid measurements at a ~0.4 h-1 frequency with high-time resolved data measured at a 6 h-1 frequency. We show how this simple method can be used in combination with mutants lacking specific genes in the rhamnolipid synthesis or quorum sensing regulation to acquire rich dynamic data on P. aeruginosa virulence regulation. Additionally, the linear relation between the ratio of inocula and the time-shift between curves produces high-precision measurements of maximum specific growth rates, which were determined with a precision of ~5.4%. Growth curve synchronization allows integration of rich time-resolved data with endpoint measurements to produce time-resolved quantitative measurements. Such data can be valuable to unveil the dynamic regulation of virulence in P. aeruginosa. More generally, growth curve synchronization can be applied to many biological systems thus helping to overcome a key obstacle in dynamic regulation: the scarceness of quantitative time-resolved data.

Dynamically consistent parameterization of mesoscale eddies. Part III: Deterministic approach

NASA Astrophysics Data System (ADS)

Berloff, Pavel

2018-07-01

This work continues development of dynamically consistent parameterizations for representing mesoscale eddy effects in non-eddy-resolving and eddy-permitting ocean circulation models and focuses on the classical double-gyre problem, in which the main dynamic eddy effects maintain eastward jet extension of the western boundary currents and its adjacent recirculation zones via eddy backscatter mechanism. Despite its fundamental importance, this mechanism remains poorly understood, and in this paper we, first, study it and, then, propose and test its novel parameterization. We start by decomposing the reference eddy-resolving flow solution into the large-scale and eddy components defined by spatial filtering, rather than by the Reynolds decomposition. Next, we find that the eastward jet and its recirculations are robustly present not only in the large-scale flow itself, but also in the rectified time-mean eddies, and in the transient rectified eddy component, which consists of highly anisotropic ribbons of the opposite-sign potential vorticity anomalies straddling the instantaneous eastward jet core and being responsible for its continuous amplification. The transient rectified component is separated from the flow by a novel remapping method. We hypothesize that the above three components of the eastward jet are ultimately driven by the small-scale transient eddy forcing via the eddy backscatter mechanism, rather than by the mean eddy forcing and large-scale nonlinearities. We verify this hypothesis by progressively turning down the backscatter and observing the induced flow anomalies. The backscatter analysis leads us to formulating the key eddy parameterization hypothesis: in an eddy-permitting model at least partially resolved eddy backscatter can be significantly amplified to improve the flow solution. Such amplification is a simple and novel eddy parameterization framework implemented here in terms of local, deterministic flow roughening controlled by single parameter. We test the parameterization skills in an hierarchy of non-eddy-resolving and eddy-permitting modifications of the original model and demonstrate, that indeed it can be highly efficient for restoring the eastward jet extension and its adjacent recirculation zones. The new deterministic parameterization framework not only combines remarkable simplicity with good performance but also is dynamically transparent, therefore, it provides a powerful alternative to the common eddy diffusion and emerging stochastic parameterizations.

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

Dynamic Data-Driven Reduced-Order Models of Macroscale Quantities for the Prediction of Equilibrium System State for Multiphase Porous Medium Systems

NASA Astrophysics Data System (ADS)

Talbot, C.; McClure, J. E.; Armstrong, R. T.; Mostaghimi, P.; Hu, Y.; Miller, C. T.

2017-12-01

Microscale simulation of multiphase flow in realistic, highly-resolved porous medium systems of a sufficient size to support macroscale evaluation is computationally demanding. Such approaches can, however, reveal the dynamic, steady, and equilibrium states of a system. We evaluate methods to utilize dynamic data to reduce the cost associated with modeling a steady or equilibrium state. We construct data-driven models using extensions to dynamic mode decomposition (DMD) and its connections to Koopman Operator Theory. DMD and its variants comprise a class of equation-free methods for dimensionality reduction of time-dependent nonlinear dynamical systems. DMD furnishes an explicit reduced representation of system states in terms of spatiotemporally varying modes with time-dependent oscillation frequencies and amplitudes. We use DMD to predict the steady and equilibrium macroscale state of a realistic two-fluid porous medium system imaged using micro-computed tomography (µCT) and simulated using the lattice Boltzmann method (LBM). We apply Koopman DMD to direct numerical simulation data resulting from simulations of multiphase fluid flow through a 1440x1440x4320 section of a full 1600x1600x5280 realization of imaged sandstone. We determine a representative set of system observables via dimensionality reduction techniques including linear and kernel principal component analysis. We demonstrate how this subset of macroscale quantities furnishes a representation of the time-evolution of the system in terms of dynamic modes, and discuss the selection of a subset of DMD modes yielding the optimal reduced model, as well as the time-dependence of the error in the predicted equilibrium value of each macroscale quantity. Finally, we describe how the above procedure, modified to incorporate methods from compressed sensing and random projection techniques, may be used in an online fashion to facilitate adaptive time-stepping and parsimonious storage of system states over time.

10 CFR 603.660 - Other audit requirements.

Code of Federal Regulations, 2011 CFR

2011-01-01

... Affecting Participants' Financial, Property, and Purchasing Systems Financial Matters § 603.660 Other audit... working papers until the matter is resolved and final action taken). (g) Who will have access to the IPA's...

24 CFR 7.12 - Responsibilities of the EEO Counselors.

Code of Federal Regulations, 2010 CFR

2010-04-01

... and the traditional EEO counseling process. The EEO Counselor shall conduct the final interview with... taken and an attempt to resolve any jurisdictional questions was made. The report shall include a...

24 CFR 7.12 - Responsibilities of the EEO Counselors.

Code of Federal Regulations, 2011 CFR

2011-04-01

... and the traditional EEO counseling process. The EEO Counselor shall conduct the final interview with... taken and an attempt to resolve any jurisdictional questions was made. The report shall include a...

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.

Advances in the use of DNA barcodes to build a community phylogeny for tropical trees in a Puerto Rican forest dynamics plot.

PubMed

Kress, W John; Erickson, David L; Swenson, Nathan G; Thompson, Jill; Uriarte, Maria; Zimmerman, Jess K

2010-11-09

Species number, functional traits, and phylogenetic history all contribute to characterizing the biological diversity in plant communities. The phylogenetic component of diversity has been particularly difficult to quantify in species-rich tropical tree assemblages. The compilation of previously published (and often incomplete) data on evolutionary relationships of species into a composite phylogeny of the taxa in a forest, through such programs as Phylomatic, has proven useful in building community phylogenies although often of limited resolution. Recently, DNA barcodes have been used to construct a robust community phylogeny for nearly 300 tree species in a forest dynamics plot in Panama using a supermatrix method. In that study sequence data from three barcode loci were used to generate a well-resolved species-level phylogeny. Here we expand upon this earlier investigation and present results on the use of a phylogenetic constraint tree to generate a community phylogeny for a diverse, tropical forest dynamics plot in Puerto Rico. This enhanced method of phylogenetic reconstruction insures the congruence of the barcode phylogeny with broadly accepted hypotheses on the phylogeny of flowering plants (i.e., APG III) regardless of the number and taxonomic breadth of the taxa sampled. We also compare maximum parsimony versus maximum likelihood estimates of community phylogenetic relationships as well as evaluate the effectiveness of one- versus two- versus three-gene barcodes in resolving community evolutionary history. As first demonstrated in the Panamanian forest dynamics plot, the results for the Puerto Rican plot illustrate that highly resolved phylogenies derived from DNA barcode sequence data combined with a constraint tree based on APG III are particularly useful in comparative analysis of phylogenetic diversity and will enhance research on the interface between community ecology and evolution.

Transient binding of CO to Cu(B) in cytochrome c oxidase is dynamically linked to structural changes around a carboxyl group: a time-resolved step-scan Fourier transform infrared investigation.

PubMed Central

Heitbrink, Dirk; Sigurdson, Håkan; Bolwien, Carsten; Brzezinski, Peter; Heberle, Joachim

2002-01-01

The redox-driven proton pump cytochrome c oxidase is that enzymatic machinery of the respiratory chain that transfers electrons from cytochrome c to molecular oxygen and thereby splits molecular oxygen to form water. To investigate the reaction mechanism of cytochrome c oxidase on the single vibrational level, we used time-resolved step-scan Fourier transform infrared spectroscopy and studied the dynamics of the reduced enzyme after photodissociation of bound carbon monoxide across the mid-infrared range (2300-950 cm(-1)). Difference spectra of the bovine complex were obtained at -20 degrees C with 5 micros time resolution. The data demonstrate a dynamic link between the transient binding of CO to Cu(B) and changes in hydrogen bonding at the functionally important residue E(I-286). Variation of the pH revealed that the pK(a) of E(I-286) is >9.3 in the fully reduced CO-bound oxidase. Difference spectra of cytochrome c oxidase from beef heart are compared with those of the oxidase isolated from Rhodobacter sphaeroides. The bacterial enzyme does not show the environmental change in the vicinity of E(I-286) upon CO dissociation. The characteristic band shape appears, however, in redox-induced difference spectra of the bacterial enzyme but is absent in redox-induced difference spectra of mammalian enzyme. In conclusion, it is demonstrated that the dynamics of a large protein complex such as cytochrome c oxidase can be resolved on the single vibrational level with microsecond Fourier transform infrared spectroscopy. The applied methodology provides the basis for future investigations of the physiological reaction steps of this important enzyme. PMID:11751290

Time-resolved photoluminescence in Mobil Composition of Matter-48

NASA Astrophysics Data System (ADS)

Liu, Y. L.; Lee, W. Z.; Shen, J. L.; Lee, Y. C.; Cheng, P. W.; Cheng, C. F.

2004-12-01

Dynamical properties of Mobil Composition of Matter (MCM)-48 were studied by time-resolved photoluminescence (PL). The PL intensity exhibits a clear nonexponential profile, which can be fitted by a stretched exponential function. In the temperature range from 50to300K, the PL decay lifetime becomes thermally activated by a characteristic energy of 25meV, which is suggested to be an indication of the phonon-assisted nonradiative process. A model is proposed to explain the relaxation behavior of the PL in MCM-48.

Time-resolved explosion of intense-laser-heated clusters.

PubMed

Kim, K Y; Alexeev, I; Parra, E; Milchberg, H M

2003-01-17

We investigate the femtosecond explosive dynamics of intense laser-heated argon clusters by measuring the cluster complex transient polarizability. The time evolution of the polarizability is characteristic of competition in the optical response between supercritical and subcritical density regions of the expanding cluster. The results are consistent with time-resolved Rayleigh scattering measurements, and bear out the predictions of a recent laser-cluster interaction model [H. M. Milchberg, S. J. McNaught, and E. Parra, Phys. Rev. E 64, 056402 (2001)

Ultrafast time-resolved spectroscopy of lead halide perovskite films

NASA Astrophysics Data System (ADS)

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

2015-09-01

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

Demonstration of coherent-state discrimination using a displacement-controlled photon-number-resolving detector.

PubMed

Wittmann, Christoffer; Andersen, Ulrik L; Takeoka, Masahiro; Sych, Denis; Leuchs, Gerd

2010-03-12

We experimentally demonstrate a new measurement scheme for the discrimination of two coherent states. The measurement scheme is based on a displacement operation followed by a photon-number-resolving detector, and we show that it outperforms the standard homodyne detector which we, in addition, prove to be optimal within all Gaussian operations including conditional dynamics. We also show that the non-Gaussian detector is superior to the homodyne detector in a continuous variable quantum key distribution scheme.

Photon structure studied at an electron ion collider

DOE PAGES

Chu, X.; Aschenauer, E. C.; Lee, J. H.; ...

2017-10-30

We report that a future electron ion collider (EIC) will be able to provide collisions of polarized electrons with protons and heavy ions over a wide range of center-of-mass energies (20 GeV to 140 GeV) at an instantaneous luminosity of 10 33 - 10 34cm -2s -1. One of its promising physics programs is the study of the partonic structure of quasireal photons. Measuring dijets in quasireal photoproduction events, one can effectively access the underlying parton dynamics of the photons. In this paper, we discuss the feasibility of tagging resolved photon processes and measuring the dijet cross section as a function of jet transverse momentum in the range of 0.01 < xmore » $$rec\\atop{γ}$$ < 1 at an EIC. Finally, it will be shown that both unpolarized and polarized parton distributions in the photon can be extracted, and that the flavor of the parton can be tagged at an EIC.« less

Epidural Hematoma Complication after Rapid Chronic Subdural Hematoma Evacuation: A Case Report

PubMed Central

Akpinar, Aykut; Ucler, Necati; Erdogan, Uzay; Yucetas, Cem Seyho

2015-01-01

Patient: Male, 41 Final Diagnosis: Healty Symptoms: Headache Medication: — Clinical Procedure: Chronic subdural hematoma Specialty: Neurosurgery Objective: Diagnostic/therapeutic accidents Background: Chronic subdural hematoma generally occurs in the elderly. After chronic subdural hematoma evacuation surgery, the development of epidural hematoma is a very rare entity. Case Report: We report the case of a 41-year-old man with an epidural hematoma complication after chronic subdural hematoma evacuation. Under general anesthesia, the patient underwent a large craniotomy with closed system drainage performed to treat the chronic subdural hematoma. After chronic subdural hematoma evacuation, there was epidural leakage on the following day. Conclusions: Although trauma is the most common risk factor in young CSDH patients, some other predisposing factors may exist. Intracranial hypotension can cause EDH. Craniotomy and drainage surgery can usually resolve the problem. Because of rapid dynamic intracranial changes, epidural leakages can occur. A large craniotomy flap and silicone drainage in the operation area are key safety points for neurosurgeons and hydration is essential. PMID:26147957

Steady-State Acceptor Fluorescence Anisotropy Imaging under Evanescent Excitation for Visualisation of FRET at the Plasma Membrane

PubMed Central

Devauges, Viviane; Matthews, Daniel R.; Aluko, Justin; Nedbal, Jakub; Levitt, James A.; Poland, Simon P.; Coban, Oana; Weitsman, Gregory; Monypenny, James; Ng, Tony; Ameer-Beg, Simon M.

2014-01-01

We present a novel imaging system combining total internal reflection fluorescence (TIRF) microscopy with measurement of steady-state acceptor fluorescence anisotropy in order to perform live cell Förster Resonance Energy Transfer (FRET) imaging at the plasma membrane. We compare directly the imaging performance of fluorescence anisotropy resolved TIRF with epifluorescence illumination. The use of high numerical aperture objective for TIRF required correction for induced depolarization factors. This arrangement enabled visualisation of conformational changes of a Raichu-Cdc42 FRET biosensor by measurement of intramolecular FRET between eGFP and mRFP1. Higher activity of the probe was found at the cell plasma membrane compared to intracellularly. Imaging fluorescence anisotropy in TIRF allowed clear differentiation of the Raichu-Cdc42 biosensor from negative control mutants. Finally, inhibition of Cdc42 was imaged dynamically in live cells, where we show temporal changes of the activity of the Raichu-Cdc42 biosensor. PMID:25360776

A dual systems account of visual perception: Predicting candy consumption from distance estimates.

PubMed

Krpan, Dario; Schnall, Simone

2017-04-01

A substantial amount of evidence shows that visual perception is influenced by forces that control human actions, ranging from motivation to physiological potential. However, studies have not yet provided convincing evidence that perception itself is directly involved in everyday behaviors such as eating. We suggest that this issue can be resolved by employing the dual systems account of human behavior. We tested the link between perceived distance to candies and their consumption for participants who were tired or depleted (impulsive system), versus those who were not (reflective system). Perception predicted eating only when participants were tired (Experiment 1) or depleted (Experiments 2 and 3). In contrast, a rational determinant of behavior-eating restraint towards candies-predicted eating for non-depleted individuals (Experiment 2). Finally, Experiment 3 established that perceived distance was correlated with participants' self-reported motivation to consume candies. Overall, these findings suggest that the dynamics between perception and behavior depend on the interplay of the two behavioral systems. Copyright © 2017 Elsevier B.V. All rights reserved.

Virus maturation: dynamics and mechanism of a stabilizing structural transition that leads to infectivity.

PubMed

Steven, Alasdair C; Heymann, J Bernard; Cheng, Naiqian; Trus, Benes L; Conway, James F

2005-04-01

For many viruses, the final stage of assembly involves structural transitions that convert an innocuous precursor particle into an infectious agent. This process -- maturation -- is controlled by proteases that trigger large-scale conformational changes. In this context, protease inhibitor antiviral drugs act by blocking maturation. Recent work has succeeded in determining the folds of representative examples of the five major proteins -- major capsid protein, scaffolding protein, portal, protease and accessory protein -- that are typically involved in capsid assembly. These data provide a framework for detailed mechanistic investigations and elucidation of mutations that affect assembly in various ways. The nature of the conformational change has been elucidated: it entails rigid-body rotations and translations of the arrayed subunits that transfer the interactions between them to different molecular surfaces, accompanied by refolding and redeployment of local motifs. Moreover, it has been possible to visualize maturation at the submolecular level in movies based on time-resolved cryo-electron microscopy.

A short story of imaging and spectroscopy of two-dimensional materials by scanning transmission electron microscopy.

PubMed

Idrobo, Juan C; Zhou, Wu

2017-09-01

Here we present a short historical account of when single adatom impurities where first identified in two-dimensional materials by scanning transmission electron microscopy (STEM). We also present a study of the graphene low-loss (below 50eV) response as a function of number of layers using electron energy-loss spectroscopy (EELS). The study shows that as few as three layers of graphene behave as bulk graphite for losses above 10eV We also show examples of how point and extended defects can easily be resolved and structural dynamics can be readily capture by using aberration-corrected STEM imaging. Finally, we show that the new generation of monochromators has opened up possibilities to explore new physics with an electron microscope. All these capabilities were enabled by the development of spherical aberration correctors and monochromators, where Ondrej Krivanek has played a key role. Copyright © 2017. Published by Elsevier B.V.

Time-resolved imaging of domain pattern destruction and recovery via nonequilibrium magnetization states

NASA Astrophysics Data System (ADS)

Wessels, Philipp; Ewald, Johannes; Wieland, Marek; Nisius, Thomas; Vogel, Andreas; Viefhaus, Jens; Meier, Guido; Wilhein, Thomas; Drescher, Markus

2014-11-01

The destruction and formation of equilibrium multidomain patterns in permalloy (Ni80Fe20 ) microsquares has been captured using pump-probe x-ray magnetic circular dichroism (XMCD) spectromicroscopy at a new full-field magnetic transmission soft x-ray microscopy endstation with subnanosecond time resolution. The movie sequences show the dynamic magnetization response to intense Oersted field pulses of approximately 200-ps root mean square (rms) duration and the magnetization reorganization to the ground-state domain configuration. The measurements display how a vortex flux-closure magnetization distribution emerges out of a nonequilibrium uniform single-domain state. During the destruction of the initial vortex pattern, we have traced the motion of the central vortex core that is ejected out of the microsquare at high velocities exceeding 1 km/s. A reproducible recovery into a defined final vortex state with stable chirality and polarity could be achieved. Using an additional external bias field, the transient reversal of the square magnetization direction could be monitored and consistently reproduced by micromagnetic simulations.

Forgetting motor programmes: retrieval dynamics in procedural memory.

PubMed

Tempel, Tobias; Frings, Christian

2014-01-01

When motor sequences are stored in memory in a categorised manner, selective retrieval of some sequences can induce forgetting of the non-retrieved sequences. We show that such retrieval-induced forgetting (RIF) occurs not only in cued recall but also in a test assessing memory indirectly by providing novel test cues without involving recall of items. Participants learned several sequential finger movements (SFMs), each consisting of the movement of two fingers of either the left or the right hand. Subsequently, they performed retrieval practice on half of the sequences of one hand. A final task then required participants to enter letter dyads. A subset of these dyads corresponded to the previously learned sequences. RIF was present in the response times during the entering of the dyads. The finding of RIF in the slowed-down execution of motor programmes overlapping with initially trained motor sequences suggests that inhibition resolved interference between procedural representations of the acquired motor sequences of one hand during retrieval practice.

Dynamic Substrate for the Physical Encoding of Sensory Information in Bat Biosonar

NASA Astrophysics Data System (ADS)

Müller, Rolf; Gupta, Anupam K.; Zhu, Hongxiao; Pannala, Mittu; Gillani, Uzair S.; Fu, Yanqing; Caspers, Philip; Buck, John R.

2017-04-01

Horseshoe bats have dynamic biosonar systems with interfaces for ultrasonic emission (reception) that change shape while diffracting the outgoing (incoming) sound waves. An information-theoretic analysis based on numerical and physical prototypes shows that these shape changes add sensory information (mutual information between distant shape conformations <20 %), increase the number of resolvable directions of sound incidence, and improve the accuracy of direction finding. These results demonstrate that horseshoe bats have a highly effective substrate for dynamic encoding of sensory information.

Dynamic Substrate for the Physical Encoding of Sensory Information in Bat Biosonar.

PubMed

Müller, Rolf; Gupta, Anupam K; Zhu, Hongxiao; Pannala, Mittu; Gillani, Uzair S; Fu, Yanqing; Caspers, Philip; Buck, John R

2017-04-14

Horseshoe bats have dynamic biosonar systems with interfaces for ultrasonic emission (reception) that change shape while diffracting the outgoing (incoming) sound waves. An information-theoretic analysis based on numerical and physical prototypes shows that these shape changes add sensory information (mutual information between distant shape conformations <20%), increase the number of resolvable directions of sound incidence, and improve the accuracy of direction finding. These results demonstrate that horseshoe bats have a highly effective substrate for dynamic encoding of sensory information.

Static harmonization of dynamically harmonized Fourier transform ion cyclotron resonance cell.

PubMed

Zhdanova, Ekaterina; Kostyukevich, Yury; Nikolaev, Eugene

2017-08-01

Static harmonization in the Fourier transform ion cyclotron resonance cell improves the resolving power of the cell and prevents dephasing of the ion cloud in the case of any trajectory of the charged particle, not necessarily axisymmetric cyclotron (as opposed to dynamic harmonization). We reveal that the Fourier transform ion cyclotron resonance cell with dynamic harmonization (paracell) is proved to be statically harmonized. The volume of the statically harmonized potential distribution increases with an increase in the number of trap segments.

Numerical simulation of turbulent forced convection in liquid metals

NASA Astrophysics Data System (ADS)

Vodret, S.; Vitale Di Maio, D.; Caruso, G.

2014-11-01

In the frame of the future generation of nuclear reactors, liquid metals are foreseen to be used as a primary coolant. Liquid metals are characterized by a very low Prandtl number due to their very high heat diffusivity. As such, they do not meet the so-called Reynolds analogy which assumes a complete similarity between the momentum and the thermal boundary layers via the use of the turbulent Prandtl number. Particularly, in the case of industrial fluid-dynamic calculations where a resolved computation near walls could be extremely time consuming and could need very large computational resources, the use of the classical wall function approach could lead to an inaccurate description of the temperature profile close to the wall. The first aim of the present study is to investigate the ability of a well- established commercial code (ANSYS FLUENT v.14) to deal with this issue, validating a suitable expression for the turbulent Prandtl number. Moreover, a thermal wall-function developed at Universite Catholique de Louvain has been implemented in FLUENT and validated, overcoming the limits of the solver to define it directly. Both the resolved and unresolved approaches have been carried out for a channel flow case and assessed against available direct numerical and large eddy simulations. A comparison between the numerically evaluated Nusselt number and the main correlations available in the literature has been also carried out. Finally, an application of the proposed methodology to a typical sub-channel case has been performed, comparing the results with literature correlations for tube banks.

Interaction and dynamics of (alkylamide + electrolyte) deep eutectics: Dependence on alkyl chain-length, temperature, and anion identity

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

Guchhait, Biswajit; Das, Suman; Daschakraborty, Snehasis

Here we investigate the solute-medium interaction and solute-centered dynamics in (RCONH{sub 2} + LiX) deep eutectics (DEs) via carrying out time-resolved fluorescence measurements and all-atom molecular dynamics simulations at various temperatures. Alkylamides (RCONH{sub 2}) considered are acetamide (CH{sub 3}CONH{sub 2}), propionamide (CH{sub 3}CH{sub 2}CONH{sub 2}), and butyramide (CH{sub 3}CH{sub 2}CH{sub 2}CONH{sub 2}); the electrolytes (LiX) are lithium perchlorate (LiClO{sub 4}), lithium bromide (LiBr), and lithium nitrate (LiNO{sub 3}). Differential scanning calorimetric measurements reveal glass transition temperatures (T{sub g}) of these DEs are ∼195 K and show a very weak dependence on alkyl chain-length and electrolyte identity. Time-resolved and steady statemore » fluorescence measurements with these DEs have been carried out at six-to-nine different temperatures that are ∼100–150 K above their individual T{sub g}s. Four different solute probes providing a good spread of fluorescence lifetimes have been employed in steady state measurements, revealing strong excitation wavelength dependence of probe fluorescence emission peak frequencies. Extent of this dependence, which shows sensitivity to anion identity, has been found to increase with increase of amide chain-length and decrease of probe lifetime. Time-resolved measurements reveal strong fractional power dependence of average rates for solute solvation and rotation with fraction power being relatively smaller (stronger viscosity decoupling) for DEs containing longer amide and larger (weaker decoupling) for DEs containing perchlorate anion. Representative all-atom molecular dynamics simulations of (CH{sub 3}CONH{sub 2} + LiX) DEs at different temperatures reveal strongly stretched exponential relaxation of wavevector dependent acetamide self dynamic structure factor with time constants dependent both on ion identity and temperature, providing justification for explaining the fluorescence results in terms of temporal heterogeneity and amide clustering in these multi-component melts.« less

Israel: Background and U.S. Relations in Brief

DTIC Science & Technology

2017-02-24

further negotiation . The status of the Gaza Strip is a final status issue to be resolved through negotiations . Israel proclaimed Jerusalem as its...largely anticipated a negotiated conflict-ending outcome that would result in two states.8 In a White House press conference on February 15, 2017...pending negotiations between Israel, Egypt, Jordan, and Palestinian representatives on the territories’ final status. April 1987 – Secret London

Fort Benning Land-Use Planning and Management Study

DTIC Science & Technology

1990-04-01

process is three-tiered: (a) an initial phase that results in preliminary allocations for natural resources, (b) a second phase that focuses on...allocations of military training requirements, and (c) a final phase that resolves conflicts between the military and natural resource requirements and...assigns final allocations. 34. Initial phase : Natural resource allocations. The first step in this phase was to make allocations among natural resource

Collaborative Research: Process-Resolving Decomposition of the Global Temperature Response to Modes of Low Frequency Variability in a Changing Climate

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

Deng, Yi

2014-11-24

DOE-GTRC-05596 11/24/2104 Collaborative Research: Process-Resolving Decomposition of the Global Temperature Response to Modes of Low Frequency Variability in a Changing Climate PI: Dr. Yi Deng (PI) School of Earth and Atmospheric Sciences Georgia Institute of Technology 404-385-1821, yi.deng@eas.gatech.edu El Niño-Southern Oscillation (ENSO) and Annular Modes (AMs) represent respectively the most important modes of low frequency variability in the tropical and extratropical circulations. The projection of future changes in the ENSO and AM variability, however, remains highly uncertain with the state-of-the-science climate models. This project conducted a process-resolving, quantitative evaluations of the ENSO and AM variability in the modern reanalysis observationsmore » and in climate model simulations. The goal is to identify and understand the sources of uncertainty and biases in models’ representation of ENSO and AM variability. Using a feedback analysis method originally formulated by one of the collaborative PIs, we partitioned the 3D atmospheric temperature anomalies and surface temperature anomalies associated with ENSO and AM variability into components linked to 1) radiation-related thermodynamic processes such as cloud and water vapor feedbacks, 2) local dynamical processes including convection and turbulent/diffusive energy transfer and 3) non-local dynamical processes such as the horizontal energy transport in the oceans and atmosphere. In the past 4 years, the research conducted at Georgia Tech under the support of this project has led to 15 peer-reviewed publications and 9 conference/workshop presentations. Two graduate students and one postdoctoral fellow also received research training through participating the project activities. This final technical report summarizes key scientific discoveries we made and provides also a list of all publications and conference presentations resulted from research activities at Georgia Tech. The main findings include: 1) the distinctly different roles played by atmospheric dynamical processes in establishing surface temperature response to ENSO at tropics and extratropics (i.e., atmospheric dynamics disperses energy out of tropics during ENSO warm events and modulate surface temperature at mid-, high-latitudes through controlling downward longwave radiation); 2) the representations of ENSO-related temperature response in climate models fail to converge at the process-level particularly over extratropics (i.e., models produce the right temperature responses to ENSO but with wrong reasons); 3) water vapor feedback contributes substantially to the temperature anomalies found over U.S. during different phases of the Northern Annular Mode (NAM), which adds new insight to the traditional picture that cold/warm advective processes are the main drivers of local temperature responses to the NAM; 4) the overall land surface temperature biases in the latest NCAR model (CESM1) are caused by biases in surface albedo while the surface temperature biases over ocean are related to multiple factors including biases in model albedo, cloud and oceanic dynamics, and the temperature biases over different ocean basins are also induced by different process biases. These results provide a detailed guidance for process-level model turning and improvement, and thus contribute directly to the overall goal of reducing model uncertainty in projecting future changes in the Earth’s climate system, especially in the ENSO and AM variability.« less

Macular retinoschisis in eyes with glaucomatous optic neuropathy: Vitrectomy and natural course.

PubMed

Yoshikawa, Tadanobu; Yamanaka, Chihiro; Kinoshita, Takamasa; Morikawa, Shohei; Ogata, Nahoko

2018-02-01

Our purpose was to determine the effectiveness of vitrectomy in resolving the macular retinoschisis in an eye with glaucomatous optic neuropathy and also to determine the natural course of macular retinoschisis. This was a retrospective case series of patients who were diagnosed with macular retinoschisis and glaucomatous optic neuropathy. Fourteen eyes of 13 patients were studied. Patients with high myopia, vitreomacular traction syndrome, and the pit macular syndrome were excluded. There were three men and ten women, and 12 had unilateral and one had bilateral macular retinoschisis. Vitrectomy was performed for a serous retinal detachment, macular hole, or severe visual loss in five eyes. The mean follow-up time was 68.8 months in these five eyes, and the macular retinoschisis was resolved and the best-corrected visual acuity (BCVA) at the final visit was significantly improved in all eyes (P = 0.007). However, two of these fiv e eyes developed a macular hole and required a second vitrectomy. Of the nine eyes without treatment with a mean follow-up time of 29.0 months, the BCVA at the final visit remained unchanged from the baseline BCVA in all eyes. The macular retinoschisis was resolved or reduced in three eyes without treatment. Vitrectomy was effective for the resolution of macular retinoschisis in eyes with glaucomatous optic neuropathy and serous retinal detachment or macular hole or severe reduction of the BCVA. Macular retinoschisis can be resolved without a reduction of the BCVA in some cases without treatment.

Constraints Imposed by the Membrane Selectively Guide the Alternating Access Dynamics of the Glutamate Transporter GltPh

PubMed Central

Lezon, Timothy R.; Bahar, Ivet

2012-01-01

Substrate transport in sodium-coupled amino acid symporters involves a large-scale conformational change that shifts the access to the substrate-binding site from one side of the membrane to the other. The structural change is particularly substantial and entails a unique piston-like quaternary rearrangement in glutamate transporters, as evidenced by the difference between the outward-facing and inward-facing structures resolved for the archaeal aspartate transporter GltPh. These structural changes occur over time and length scales that extend beyond the reach of current fully atomic models, but are regularly explored with the use of elastic network models (ENMs). Despite their success with other membrane proteins, ENM-based approaches for exploring the collective dynamics of GltPh have fallen short of providing a plausible mechanism. This deficiency is attributed here to the anisotropic constraints imposed by the membrane, which are not incorporated into conventional ENMs. Here we employ two novel (to our knowledge) ENMs to demonstrate that one can largely capture the experimentally observed structural change using only the few lowest-energy modes of motion that are intrinsically accessible to the transporter, provided that the surrounding lipid molecules are incorporated into the ENM. The presence of the membrane reduces the overall energy of the transition compared with conventional models, showing that the membrane not only guides the selected mechanism but also acts as a facilitator. Finally, we show that the dynamics of GltPh is biased toward transitions of individual subunits of the trimer rather than cooperative transitions of all three subunits simultaneously, suggesting a mechanism of transport that exploits the intrinsic dynamics of individual subunits. Our software is available online at http://www.membranm.csb.pitt.edu. PMID:22455916

Constraints imposed by the membrane selectively guide the alternating access dynamics of the glutamate transporter GltPh.

PubMed

Lezon, Timothy R; Bahar, Ivet

2012-03-21

Substrate transport in sodium-coupled amino acid symporters involves a large-scale conformational change that shifts the access to the substrate-binding site from one side of the membrane to the other. The structural change is particularly substantial and entails a unique piston-like quaternary rearrangement in glutamate transporters, as evidenced by the difference between the outward-facing and inward-facing structures resolved for the archaeal aspartate transporter Glt(Ph). These structural changes occur over time and length scales that extend beyond the reach of current fully atomic models, but are regularly explored with the use of elastic network models (ENMs). Despite their success with other membrane proteins, ENM-based approaches for exploring the collective dynamics of Glt(Ph) have fallen short of providing a plausible mechanism. This deficiency is attributed here to the anisotropic constraints imposed by the membrane, which are not incorporated into conventional ENMs. Here we employ two novel (to our knowledge) ENMs to demonstrate that one can largely capture the experimentally observed structural change using only the few lowest-energy modes of motion that are intrinsically accessible to the transporter, provided that the surrounding lipid molecules are incorporated into the ENM. The presence of the membrane reduces the overall energy of the transition compared with conventional models, showing that the membrane not only guides the selected mechanism but also acts as a facilitator. Finally, we show that the dynamics of Glt(Ph) is biased toward transitions of individual subunits of the trimer rather than cooperative transitions of all three subunits simultaneously, suggesting a mechanism of transport that exploits the intrinsic dynamics of individual subunits. Our software is available online at http://www.membranm.csb.pitt.edu. Copyright © 2012 Biophysical Society. Published by Elsevier Inc. All rights reserved.

Design and implementation of an optimal laser pulse front tilting scheme for ultrafast electron diffraction in reflection geometry with high temporal resolution.

PubMed

Pennacchio, Francesco; Vanacore, Giovanni M; Mancini, Giulia F; Oppermann, Malte; Jayaraman, Rajeswari; Musumeci, Pietro; Baum, Peter; Carbone, Fabrizio

2017-07-01

Ultrafast electron diffraction is a powerful technique to investigate out-of-equilibrium atomic dynamics in solids with high temporal resolution. When diffraction is performed in reflection geometry, the main limitation is the mismatch in group velocity between the overlapping pump light and the electron probe pulses, which affects the overall temporal resolution of the experiment. A solution already available in the literature involved pulse front tilt of the pump beam at the sample, providing a sub-picosecond time resolution. However, in the reported optical scheme, the tilted pulse is characterized by a temporal chirp of about 1 ps at 1 mm away from the centre of the beam, which limits the investigation of surface dynamics in large crystals. In this paper, we propose an optimal tilting scheme designed for a radio-frequency-compressed ultrafast electron diffraction setup working in reflection geometry with 30 keV electron pulses containing up to 10 5 electrons/pulse. To characterize our scheme, we performed optical cross-correlation measurements, obtaining an average temporal width of the tilted pulse lower than 250 fs. The calibration of the electron-laser temporal overlap was obtained by monitoring the spatial profile of the electron beam when interacting with the plasma optically induced at the apex of a copper needle (plasma lensing effect). Finally, we report the first time-resolved results obtained on graphite, where the electron-phonon coupling dynamics is observed, showing an overall temporal resolution in the sub-500 fs regime. The successful implementation of this configuration opens the way to directly probe structural dynamics of low-dimensional systems in the sub-picosecond regime, with pulsed electrons.

Design and implementation of an optimal laser pulse front tilting scheme for ultrafast electron diffraction in reflection geometry with high temporal resolution

PubMed Central

Pennacchio, Francesco; Vanacore, Giovanni M.; Mancini, Giulia F.; Oppermann, Malte; Jayaraman, Rajeswari; Musumeci, Pietro; Baum, Peter; Carbone, Fabrizio

2017-01-01

Ultrafast electron diffraction is a powerful technique to investigate out-of-equilibrium atomic dynamics in solids with high temporal resolution. When diffraction is performed in reflection geometry, the main limitation is the mismatch in group velocity between the overlapping pump light and the electron probe pulses, which affects the overall temporal resolution of the experiment. A solution already available in the literature involved pulse front tilt of the pump beam at the sample, providing a sub-picosecond time resolution. However, in the reported optical scheme, the tilted pulse is characterized by a temporal chirp of about 1 ps at 1 mm away from the centre of the beam, which limits the investigation of surface dynamics in large crystals. In this paper, we propose an optimal tilting scheme designed for a radio-frequency-compressed ultrafast electron diffraction setup working in reflection geometry with 30 keV electron pulses containing up to 105 electrons/pulse. To characterize our scheme, we performed optical cross-correlation measurements, obtaining an average temporal width of the tilted pulse lower than 250 fs. The calibration of the electron-laser temporal overlap was obtained by monitoring the spatial profile of the electron beam when interacting with the plasma optically induced at the apex of a copper needle (plasma lensing effect). Finally, we report the first time-resolved results obtained on graphite, where the electron-phonon coupling dynamics is observed, showing an overall temporal resolution in the sub-500 fs regime. The successful implementation of this configuration opens the way to directly probe structural dynamics of low-dimensional systems in the sub-picosecond regime, with pulsed electrons. PMID:28713841

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.

High resolution x-ray Thomson scattering measurements from cryogenic hydrogen jets using the linac coherent light source

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

Fletcher, L. B., E-mail: lbfletch@slac.stanford.edu; Galtier, E.; Gamboa, E. J.

2016-11-15

We present the first spectrally resolved measurements of x-rays scattered from cryogenic hydrogen jets in the single photon counting limit. The 120 Hz capabilities of the LCLS, together with a novel hydrogen jet design [J. B. Kim et al., Rev. Sci. Instrum. (these proceedings)], allow for the ability to record a near background free spectrum. Such high-dynamic-range x-ray scattering measurements enable a platform to study ultra-fast, laser-driven, heating dynamics of hydrogen plasmas. This measurement has been achieved using two highly annealed pyrolytic graphite crystal spectrometers to spectrally resolve 5.5 keV x-rays elastically and inelastically scattered from cryogenic hydrogen and focusedmore » on Cornell-SLAC pixel array detectors [S. Herrmann et al., Nucl. Instrum. Methods Phys. Res., Sect. A 718, 550 (2013)].« less

An ultrafast programmable electrical tester for enabling time-resolved, sub-nanosecond switching dynamics and programming of nanoscale memory devices.

PubMed

Shukla, Krishna Dayal; Saxena, Nishant; Manivannan, Anbarasu

2017-12-01

Recent advancements in commercialization of high-speed non-volatile electronic memories including phase change memory (PCM) have shown potential not only for advanced data storage but also for novel computing concepts. However, an in-depth understanding on ultrafast electrical switching dynamics is a key challenge for defining the ultimate speed of nanoscale memory devices that demands for an unconventional electrical setup, specifically capable of handling extremely fast electrical pulses. In the present work, an ultrafast programmable electrical tester (PET) setup has been developed exceptionally for unravelling time-resolved electrical switching dynamics and programming characteristics of nanoscale memory devices at the picosecond (ps) time scale. This setup consists of novel high-frequency contact-boards carefully designed to capture extremely fast switching transient characteristics within 200 ± 25 ps using time-resolved current-voltage measurements. All the instruments in the system are synchronized using LabVIEW, which helps to achieve various programming characteristics such as voltage-dependent transient parameters, read/write operations, and endurance test of memory devices systematically using short voltage pulses having pulse parameters varied from 1 ns rise/fall time and 1.5 ns pulse width (full width half maximum). Furthermore, the setup has successfully demonstrated strikingly one order faster switching characteristics of Ag 5 In 5 Sb 60 Te 30 (AIST) PCM devices within 250 ps. Hence, this novel electrical setup would be immensely helpful for realizing the ultimate speed limits of various high-speed memory technologies for future computing.

An ultrafast programmable electrical tester for enabling time-resolved, sub-nanosecond switching dynamics and programming of nanoscale memory devices

NASA Astrophysics Data System (ADS)

Shukla, Krishna Dayal; Saxena, Nishant; Manivannan, Anbarasu

2017-12-01

Recent advancements in commercialization of high-speed non-volatile electronic memories including phase change memory (PCM) have shown potential not only for advanced data storage but also for novel computing concepts. However, an in-depth understanding on ultrafast electrical switching dynamics is a key challenge for defining the ultimate speed of nanoscale memory devices that demands for an unconventional electrical setup, specifically capable of handling extremely fast electrical pulses. In the present work, an ultrafast programmable electrical tester (PET) setup has been developed exceptionally for unravelling time-resolved electrical switching dynamics and programming characteristics of nanoscale memory devices at the picosecond (ps) time scale. This setup consists of novel high-frequency contact-boards carefully designed to capture extremely fast switching transient characteristics within 200 ± 25 ps using time-resolved current-voltage measurements. All the instruments in the system are synchronized using LabVIEW, which helps to achieve various programming characteristics such as voltage-dependent transient parameters, read/write operations, and endurance test of memory devices systematically using short voltage pulses having pulse parameters varied from 1 ns rise/fall time and 1.5 ns pulse width (full width half maximum). Furthermore, the setup has successfully demonstrated strikingly one order faster switching characteristics of Ag5In5Sb60Te30 (AIST) PCM devices within 250 ps. Hence, this novel electrical setup would be immensely helpful for realizing the ultimate speed limits of various high-speed memory technologies for future computing.

Laser angle-resolved photoemission as a probe of initial state k z dispersion, final-state band gaps, and spin texture of Dirac states in the Bi 2Te 3 topological insulator

DOE PAGES

Ärrälä, Minna; Hafiz, Hasnain; Mou, Daixiang; ...

2016-10-27

Here, we have obtained angle-resolved photoemission (ARPES) spectra from single crystals of the topological insulator material Bi 2Te 3 using tunable laser spectrometer. The spectra were collected for eleven different photon energies ranging from 5.57 to 6.70 eV for incident light polarized linearly along two different in-plane directions. Parallel first-principles, fully relativistic computations of photo-intensities were carried out using the experimental geometry within the framework of the one-step model of photoemission. Good overall accord between theory and experiment is used to gain insight into how properties of the initial and final state band structures as well as those of themore » topological surface states and their spin-textures are reflected in the laser-ARPES spectra. In conclusion, our analysis reveals that laser-ARPES is sensitive to both the initial state k z dispersion and the presence of delicate gaps in the final state electronic spectrum.« less

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

Heinemann, Thomas, E-mail: thomas.heinemann@tu-berlin.de; Klapp, Sabine H. L., E-mail: klapp@physik.tu-berlin.de; Palczynski, Karol, E-mail: karol.palczynski@helmholtz-berlin.de

We present an approach for calculating coarse-grained angle-resolved effective pair potentials for uniaxial molecules. For integrating out the intramolecular degrees of freedom we apply umbrella sampling and steered dynamics techniques in atomistically-resolved molecular dynamics (MD) computer simulations. Throughout this study we focus on disk-like molecules such as coronene. To develop the methods we focus on integrating out the van der Waals and intramolecular interactions, while electrostatic charge contributions are neglected. The resulting coarse-grained pair potential reveals a strong temperature and angle dependence. In the next step we fit the numerical data with various Gay-Berne-like potentials to be used in moremore » efficient simulations on larger scales. The quality of the resulting coarse-grained results is evaluated by comparing their pair and many-body structure as well as some thermodynamic quantities self-consistently to the outcome of atomistic MD simulations of many-particle systems. We find that angle-resolved potentials are essential not only to accurately describe crystal structures but also for fluid systems where simple isotropic potentials start to fail already for low to moderate packing fractions. Further, in describing these states it is crucial to take into account the pronounced temperature dependence arising in selected pair configurations due to bending fluctuations.« less

SPORT: A new sub-nanosecond time-resolved instrument to study swift heavy ion-beam induced luminescence - Application to luminescence degradation of a fast plastic scintillator

NASA Astrophysics Data System (ADS)

Gardés, E.; Balanzat, E.; Ban-d'Etat, B.; Cassimi, A.; Durantel, F.; Grygiel, C.; Madi, T.; Monnet, I.; Ramillon, J.-M.; Ropars, F.; Lebius, H.

2013-02-01

We developed a new sub-nanosecond time-resolved instrument to study the dynamics of UV-visible luminescence under high stopping power heavy ion irradiation. We applied our instrument, called SPORT, on a fast plastic scintillator (BC-400) irradiated with 27-MeV Ar ions having high mean electronic stopping power of 2.6 MeV/μm. As a consequence of increasing permanent radiation damages with increasing ion fluence, our investigations reveal a degradation of scintillation intensity together with, thanks to the time-resolved measurement, a decrease in the decay constant of the scintillator. This combination indicates that luminescence degradation processes by both dynamic and static quenching, the latter mechanism being predominant. Under such high density excitation, the scintillation deterioration of BC-400 is significantly enhanced compared to that observed in previous investigations, mainly performed using light ions. The observed non-linear behaviour implies that the dose at which luminescence starts deteriorating is not independent on particles' stopping power, thus illustrating that the radiation hardness of plastic scintillators can be strongly weakened under high excitation density in heavy ion environments.

Concept Demonstration of Dopant Selective Reactive Etching (DSRIE) in Silicon Carbide

NASA Technical Reports Server (NTRS)

Okojie, Robert S.

2015-01-01

Accurate quantification of combustor pressure dynamics for the primary purpose of experimental validation of computational fluid dynamics (CFD) codes requires the use of robust, reliable and sensitive pressure sensors that can resolve sub--pound-per-square-inch pressure levels in high temperature environments (i.e., combustor). The state of the art microfabricated piezoresistive silicon carbide (SiC) pressure sensors that we have developed are capable of operating reliably at 600 degrees Centigrade. This technology was used in support of the ARMD ISRP-ERA (NASA's Aeronautics Research Mission Directorate, Integrated System Research Project - Environmentally Responsible Aviation) program to quantify combustor thermoacoustic instabilities. The results showed that while the SiC pressure sensors survived the high temperature and measured instabilities, the diaphragm (force collector) was not thin enough to be sensitive in resolving sub-pound-per-square-inch pressures; 30 meters is the thinnest diaphragm achievable with conventional reactive ion etching (RIE) processes. Therefore, this precludes its use for sub-pound-per-square-inch pressure measurement with high fidelity. In order to effectively resolve sub-pound-per-square-inch pressures, a thinner more sensitive diaphragm (10 meters) is needed. To achieve this would require a new and innovative fabrication process technique.

Dynamical mass measurement of the young spectroscopic binary V343 Normae AaAb resolved with the Gemini Planet Imager

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

Nielsen, Eric L.; De Rosa, Robert J.; Wang, Jason

Here, we present new spatially resolved astrometry and photometry from the Gemini Planet Imager of the inner binary of the young multiple star system V343 Normae, which is a member of the β Pictoris (β Pic) moving group. V343 Normae comprises a K0 and mid-M star in a ~4.5 year orbit (AaAb) and a wide 10'' M5 companion (B). By combining these data with archival astrometry and radial velocities we fit the orbit and measure individual masses for both components ofmore » $${M}_{\\mathrm{Aa}}=1.10\\pm 0.10\\,{M}_{\\odot }$$ and $${M}_{\\mathrm{Ab}}=0.290\\pm 0.018\\,{M}_{\\odot }$$. Comparing to theoretical isochrones, we find good agreement for the measured masses and JHK band magnitudes of the two components consistent with the age of the β Pic moving group. We derive a model-dependent age for the β Pic moving group of 26 ± 3 Myr by combining our results for V343 Normae with literature measurements for GJ 3305, which is another group member with resolved binary components and dynamical masses.« less

Ultrafast nuclear dynamics in halomethanes studied with time-resolved Coulomb explosion imaging and channel-selective Fourier spectroscopy

NASA Astrophysics Data System (ADS)

Malakar, Y.; Kaderiya, B.; Pearson, W. L.; Ziaee, F.; Kanaka Raju, P.; Zohrabi, M.; Jensen, K.; Rajput, J.; Ben-Itzhak, I.; Rolles, D.; Rudenko, A.

2016-05-01

Halomethanes have recently attracted considerable attention since they often serve as prototype systems for laser-controlled chemistry (e.g., selective bond breaking or concerted elimination reactions), and are important molecules in atmospheric chemistry. Here we combine a femtosecond laser pump-probe setup with coincident 3D ion momentum imaging apparatus to study strong-field induced nuclear dynamics in methane and several of its halogenated derivatives (CH3 I, CH2 I2, CH2 ICl). We apply a time-resolved Coulomb explosion imaging technique to map the nuclear motion on both, bound and continuum potential surfaces, disentangle different fragmentation pathways and, for halogenated molecules, observe clear signatures of vibrational wave packets in neutral or ionized states. Channel-selective and kinetic-energy resolved Fourier analysis of these data allows for unique identification of different electronic states and vibrational modes responsible for a particular structure. Supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. DOE. K. R. P. and W. L. P. supported by NSF Award No. IIA-143049. K.J. supported by the NSF-REU Grant No. PHYS-1461251.

Time-resolved Analysis of Proteome Dynamics by Tandem Mass Tags and Stable Isotope Labeling in Cell Culture (TMT-SILAC) Hyperplexing*

PubMed Central

Welle, Kevin A.; Zhang, Tian; Hryhorenko, Jennifer R.; Shen, Shichen; Qu, Jun; Ghaemmaghami, Sina

2016-01-01

Recent advances in mass spectrometry have enabled system-wide analyses of protein turnover. By globally quantifying the kinetics of protein clearance and synthesis, these methodologies can provide important insights into the regulation of the proteome under varying cellular and environmental conditions. To facilitate such analyses, we have employed a methodology that combines metabolic isotopic labeling (Stable Isotope Labeling in Cell Culture - SILAC) with isobaric tagging (Tandem Mass Tags - TMT) for analysis of multiplexed samples. The fractional labeling of multiple time-points can be measured in a single mass spectrometry run, providing temporally resolved measurements of protein turnover kinetics. To demonstrate the feasibility of the approach, we simultaneously measured the kinetics of protein clearance and accumulation for more than 3000 proteins in dividing and quiescent human fibroblasts and verified the accuracy of the measurements by comparison to established non-multiplexed approaches. The results indicate that upon reaching quiescence, fibroblasts compensate for lack of cellular growth by globally downregulating protein synthesis and upregulating protein degradation. The described methodology significantly reduces the cost and complexity of temporally-resolved dynamic proteomic experiments and improves the precision of proteome-wide turnover data. PMID:27765818

Towards higher stability of resonant absorption measurements in pulsed plasmas.

PubMed

Britun, Nikolay; Michiels, Matthieu; Snyders, Rony

2015-12-01

Possible ways to increase the reliability of time-resolved particle density measurements in pulsed gaseous discharges using resonant absorption spectroscopy are proposed. A special synchronization, called "dynamic source triggering," between a gated detector and two pulsed discharges, one representing the discharge of interest and another being used as a reference source, is developed. An internal digital delay generator in the intensified charge coupled device camera, used at the same time as a detector, is utilized for this purpose. According to the proposed scheme, the light pulses from the reference source follow the gates of detector, passing through the discharge of interest only when necessary. This allows for the utilization of short-pulse plasmas as reference sources, which is critical for time-resolved absorption analysis of strongly emitting pulsed discharges. In addition to dynamic source triggering, the reliability of absorption measurements can be further increased using simultaneous detection of spectra relevant for absorption method, which is also demonstrated in this work. The proposed methods are illustrated by the time-resolved measurements of the metal atom density in a high-power impulse magnetron sputtering (HiPIMS) discharge, using either a hollow cathode lamp or another HiPIMS discharge as a pulsed reference source.

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

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

Li, Deyong; Li, Yunliang; Li, Hao

2015-05-15

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

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.

Dynamical mass measurement of the young spectroscopic binary V343 Normae AaAb resolved with the Gemini Planet Imager

DOE PAGES

Nielsen, Eric L.; De Rosa, Robert J.; Wang, Jason; ...

2016-11-22

Here, we present new spatially resolved astrometry and photometry from the Gemini Planet Imager of the inner binary of the young multiple star system V343 Normae, which is a member of the β Pictoris (β Pic) moving group. V343 Normae comprises a K0 and mid-M star in a ~4.5 year orbit (AaAb) and a wide 10'' M5 companion (B). By combining these data with archival astrometry and radial velocities we fit the orbit and measure individual masses for both components ofmore » $${M}_{\\mathrm{Aa}}=1.10\\pm 0.10\\,{M}_{\\odot }$$ and $${M}_{\\mathrm{Ab}}=0.290\\pm 0.018\\,{M}_{\\odot }$$. Comparing to theoretical isochrones, we find good agreement for the measured masses and JHK band magnitudes of the two components consistent with the age of the β Pic moving group. We derive a model-dependent age for the β Pic moving group of 26 ± 3 Myr by combining our results for V343 Normae with literature measurements for GJ 3305, which is another group member with resolved binary components and dynamical masses.« less

Study of Near-Surface Models in Large-Eddy Simulations of a Neutrally Stratified Atmospheric Boundary Layer

NASA Technical Reports Server (NTRS)

Senocak, I.; Ackerman, A. S.; Kirkpatrick, M. P.; Stevens, D. E.; Mansour, N. N.

2004-01-01

Large-eddy simulation (LES) is a widely used technique in armospheric modeling research. In LES, large, unsteady, three dimensional structures are resolved and small structures that are not resolved on the computational grid are modeled. A filtering operation is applied to distinguish between resolved and unresolved scales. We present two near-surface models that have found use in atmospheric modeling. We also suggest a simpler eddy viscosity model that adopts Prandtl's mixing length model (Prandtl 1925) in the vicinity of the surface and blends with the dynamic Smagotinsky model (Germano et al, 1991) away from the surface. We evaluate the performance of these surface models by simulating a neutraly stratified atmospheric boundary layer.

Dynamic modeling and optimal joint torque coordination of advanced robotic systems

NASA Astrophysics Data System (ADS)

Kang, Hee-Jun

The development is documented of an efficient dynamic modeling algorithm and the subsequent optimal joint input load coordination of advanced robotic systems for industrial application. A closed-form dynamic modeling algorithm for the general closed-chain robotic linkage systems is presented. The algorithm is based on the transfer of system dependence from a set of open chain Lagrangian coordinates to any desired system generalized coordinate set of the closed-chain. Three different techniques for evaluation of the kinematic closed chain constraints allow the representation of the dynamic modeling parameters in terms of system generalized coordinates and have no restriction with regard to kinematic redundancy. The total computational requirement of the closed-chain system model is largely dependent on the computation required for the dynamic model of an open kinematic chain. In order to improve computational efficiency, modification of an existing open-chain KIC based dynamic formulation is made by the introduction of the generalized augmented body concept. This algorithm allows a 44 pct. computational saving over the current optimized one (O(N4), 5995 when N = 6). As means of resolving redundancies in advanced robotic systems, local joint torque optimization is applied for effectively using actuator power while avoiding joint torque limits. The stability problem in local joint torque optimization schemes is eliminated by using fictitious dissipating forces which act in the necessary null space. The performance index representing the global torque norm is shown to be satisfactory. In addition, the resulting joint motion trajectory becomes conservative, after a transient stage, for repetitive cyclic end-effector trajectories. The effectiveness of the null space damping method is shown. The modular robot, which is built of well defined structural modules from a finite-size inventory and is controlled by one general computer system, is another class of evolving, highly versatile, advanced robotic systems. Therefore, finally, a module based dynamic modeling algorithm is presented for the dynamic coordination of such reconfigurable modular robotic systems. A user interactive module based manipulator analysis program (MBMAP) has been coded in C language running on 4D/70 Silicon Graphics.

Time-Resolved Fluorescent Immunochromatography of Aflatoxin B1 in Soybean Sauce: A Rapid and Sensitive Quantitative Analysis.

PubMed

Wang, Du; Zhang, Zhaowei; Li, Peiwu; Zhang, Qi; Zhang, Wen

2016-07-14

Rapid and quantitative sensing of aflatoxin B1 with high sensitivity and specificity has drawn increased attention of studies investigating soybean sauce. A sensitive and rapid quantitative immunochromatographic sensing method was developed for the detection of aflatoxin B1 based on time-resolved fluorescence. It combines the advantages of time-resolved fluorescent sensing and immunochromatography. The dynamic range of a competitive and portable immunoassay was 0.3-10.0 µg·kg(-1), with a limit of detection (LOD) of 0.1 µg·kg(-1) and recoveries of 87.2%-114.3%, within 10 min. The results showed good correlation (R² > 0.99) between time-resolved fluorescent immunochromatographic strip test and high performance liquid chromatography (HPLC). Soybean sauce samples analyzed using time-resolved fluorescent immunochromatographic strip test revealed that 64.2% of samples contained aflatoxin B1 at levels ranging from 0.31 to 12.5 µg·kg(-1). The strip test is a rapid, sensitive, quantitative, and cost-effective on-site screening technique in food safety analysis.

Structure-Preserving Variational Multiscale Modeling of Turbulent Incompressible Flow with Subgrid Vortices

NASA Astrophysics Data System (ADS)

Evans, John; Coley, Christopher; Aronson, Ryan; Nelson, Corey

2017-11-01

In this talk, a large eddy simulation methodology for turbulent incompressible flow will be presented which combines the best features of divergence-conforming discretizations and the residual-based variational multiscale approach to large eddy simulation. In this method, the resolved motion is represented using a divergence-conforming discretization, that is, a discretization that preserves the incompressibility constraint in a pointwise manner, and the unresolved fluid motion is explicitly modeled by subgrid vortices that lie within individual grid cells. The evolution of the subgrid vortices is governed by dynamical model equations driven by the residual of the resolved motion. Consequently, the subgrid vortices appropriately vanish for laminar flow and fully resolved turbulent flow. As the resolved velocity field and subgrid vortices are both divergence-free, the methodology conserves mass in a pointwise sense and admits discrete balance laws for energy, enstrophy, and helicity. Numerical results demonstrate the methodology yields improved results versus state-of-the-art eddy viscosity models in the context of transitional, wall-bounded, and rotational flow when a divergence-conforming B-spline discretization is utilized to represent the resolved motion.

The roles of competition and habitat in the dynamics of populations and species distributions Ecology

Treesearch

Charles B. Yackulic; Janice Reid; James D. Nichols; James E. Hines; Raymond Davis; Eric Forsman

2014-01-01

The role of competition in structuring biotic communities at fine spatial scales is well known from detailed process-based studies. Our understanding of competition’s importance at broader scales is less resolved and mainly based on static species distribution maps. Here, we bridge this gap by examining the joint occupancy dynamics of an invading species (Barred Owl,...

Use of computer modeling to investigate a dynamic interaction problem in the Skylab TACS quad-valve package

NASA Technical Reports Server (NTRS)

Hesser, R. J.; Gershman, R.

1975-01-01

A valve opening-response problem encountered during development of a control valve for the Skylab thruster attitude control system (TACS) is described. The problem involved effects of dynamic interaction among valves in the quad-redundant valve package. Also described is a detailed computer simulation of the quad-valve package which was helpful in resolving the problem.

A portable low-cost long-term live-cell imaging platform for biomedical research and education.

PubMed

Walzik, Maria P; Vollmar, Verena; Lachnit, Theresa; Dietz, Helmut; Haug, Susanne; Bachmann, Holger; Fath, Moritz; Aschenbrenner, Daniel; Abolpour Mofrad, Sepideh; Friedrich, Oliver; Gilbert, Daniel F

2015-02-15

Time-resolved visualization and analysis of slow dynamic processes in living cells has revolutionized many aspects of in vitro cellular studies. However, existing technology applied to time-resolved live-cell microscopy is often immobile, costly and requires a high level of skill to use and maintain. These factors limit its utility to field research and educational purposes. The recent availability of rapid prototyping technology makes it possible to quickly and easily engineer purpose-built alternatives to conventional research infrastructure which are low-cost and user-friendly. In this paper we describe the prototype of a fully automated low-cost, portable live-cell imaging system for time-resolved label-free visualization of dynamic processes in living cells. The device is light-weight (3.6 kg), small (22 × 22 × 22 cm) and extremely low-cost (<€1250). We demonstrate its potential for biomedical use by long-term imaging of recombinant HEK293 cells at varying culture conditions and validate its ability to generate time-resolved data of high quality allowing for analysis of time-dependent processes in living cells. While this work focuses on long-term imaging of mammalian cells, the presented technology could also be adapted for use with other biological specimen and provides a general example of rapidly prototyped low-cost biosensor technology for application in life sciences and education. Copyright © 2014 The Authors. Published by Elsevier B.V. All rights reserved.

Generalized thick strip modelling for vortex-induced vibration of long flexible cylinders

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

Bao, Y., E-mail: ybao@sjtu.edu.cn; Department of Aeronautics, Imperial College London, South Kensington Campus, London; Palacios, R., E-mail: r.palacios@imperial.ac.uk

2016-09-15

We propose a generalized strip modelling method that is computationally efficient for the VIV prediction of long flexible cylinders in three-dimensional incompressible flow. In order to overcome the shortcomings of conventional strip-theory-based 2D models, the fluid domain is divided into “thick” strips, which are sufficiently thick to locally resolve the small scale turbulence effects and three dimensionality of the flow around the cylinder. An attractive feature of the model is that we independently construct a three-dimensional scale resolving model for individual strips, which have local spanwise scale along the cylinder's axial direction and are only coupled through the structural modelmore » of the cylinder. Therefore, this approach is able to cover the full spectrum for fully resolved 3D modelling to 2D strip theory. The connection between these strips is achieved through the calculation of a tensioned beam equation, which is used to represent the dynamics of the flexible body. In the limit, however, a single “thick” strip would fill the full 3D domain. A parallel Fourier spectral/hp element method is employed to solve the 3D flow dynamics in the strip-domain, and then the VIV response prediction is achieved through the strip–structure interactions. Numerical tests on both laminar and turbulent flows as well as the comparison against the fully resolved DNS are presented to demonstrate the applicability of this approach.« less

New disk discovered with VLT/SPHERE around the M star GSC 07396-00759

NASA Astrophysics Data System (ADS)

Sissa, E.; Olofsson, J.; Vigan, A.; Augereau, J. C.; D'Orazi, V.; Desidera, S.; Gratton, R.; Langlois, M.; Rigliaco, E.; Boccaletti, A.; Kral, Q.; Lazzoni, C.; Mesa, D.; Messina, S.; Sezestre, E.; Thébault, P.; Zurlo, A.; Bhowmik, T.; Bonnefoy, M.; Chauvin, G.; Feldt, M.; Hagelberg, J.; Lagrange, A.-M.; Janson, M.; Maire, A.-L.; Ménard, F.; Schlieder, J.; Schmidt, T.; Szulágyi, J.; Stadler, E.; Maurel, D.; Delboulbé, A.; Feautrier, P.; Ramos, J.; Rigal, F.

2018-05-01

Debris disks are usually detected through the infrared excess over the photospheric level of their host star. The most favorable stars for disk detection are those with spectral types between A and K, while the statistics for debris disks detected around low-mass M-type stars is very low, either because they are rare or because they are more difficult to detect. Terrestrial planets, on the other hand, may be common around M-type stars. Here, we report on the discovery of an extended (likely) debris disk around the M-dwarf GSC 07396-00759. The star is a wide companion of the close accreting binary V4046 Sgr. The system probably is a member of the β Pictoris Moving Group. We resolve the disk in scattered light, exploiting high-contrast, high-resolution imagery with the two near-infrared subsystems of the VLT/SPHERE instrument, operating in the Y J bands and the H2H3 doublet. The disk is clearly detected up to 1.5'' ( 110 au) from the star and appears as a ring, with an inclination i 83°, and a peak density position at 70 au. The spatial extension of the disk suggests that the dust dynamics is affected by a strong stellar wind, showing similarities with the AU Mic system that has also been resolved with SPHERE. The images show faint asymmetric structures at the widest separation in the northwest side. We also set an upper limit for the presence of giant planets to 2 MJ. Finally, we note that the 2 resolved disks around M-type stars of 30 such stars observed with SPHERE are viewed close to edge-on, suggesting that a significant population of debris disks around M dwarfs could remain undetected because of an unfavorable orientation. Based on data collected at the European Southern Observatory, Chile (ESO Program 198.C-0298).

CRF-PEPICO: Double velocity map imaging photoelectron photoion coincidence spectroscopy for reaction kinetics studies

NASA Astrophysics Data System (ADS)

Sztáray, Bálint; Voronova, Krisztina; Torma, Krisztián G.; Covert, Kyle J.; Bodi, Andras; Hemberger, Patrick; Gerber, Thomas; Osborn, David L.

2017-07-01

Photoelectron photoion coincidence (PEPICO) spectroscopy could become a powerful tool for the time-resolved study of multi-channel gas phase chemical reactions. Toward this goal, we have designed and tested electron and ion optics that form the core of a new PEPICO spectrometer, utilizing simultaneous velocity map imaging for both cations and electrons, while also achieving good cation mass resolution through space focusing. These optics are combined with a side-sampled, slow-flow chemical reactor for photolytic initiation of gas-phase chemical reactions. Together with a recent advance that dramatically increases the dynamic range in PEPICO spectroscopy [D. L. Osborn et al., J. Chem. Phys. 145, 164202 (2016)], the design described here demonstrates a complete prototype spectrometer and reactor interface to carry out time-resolved experiments. Combining dual velocity map imaging with cation space focusing yields tightly focused photoion images for translationally cold neutrals, while offering good mass resolution for thermal samples as well. The flexible optics design incorporates linear electric fields in the ionization region, surrounded by dual curved electric fields for velocity map imaging of ions and electrons. Furthermore, the design allows for a long extraction stage, which makes this the first PEPICO experiment to combine ion imaging with the unimolecular dissociation rate constant measurements of cations to detect and account for kinetic shifts. Four examples are shown to illustrate some capabilities of this new design. We recorded the threshold photoelectron spectrum of the propargyl and the iodomethyl radicals. While the former agrees well with a literature threshold photoelectron spectrum, we have succeeded in resolving the previously unobserved vibrational structure in the latter. We have also measured the bimolecular rate constant of the CH2I + O2 reaction and observed its product, the smallest Criegee intermediate, CH2OO. Finally, the second dissociative photoionization step of iodocyclohexane ions, the loss of ethylene from the cyclohexyl cation, is slow at threshold, as illustrated by the asymmetric threshold photoionization time-of-flight distributions.

Time, Dynamics and Chaos: Integrating Poincare's 'Non-Integrable Systems'

DOE R&D Accomplishments Database

Prigogine, I.

1990-10-01

This report discusses the nature of time. The author attempts to resolve the conflict between the concept of time reversibility in classical and quantum mechanics with the macroscopic world's irreversibility of time. (LSP)

Non-Gaussian lineshapes and dynamics of time-resolved linear and nonlinear (correlation) spectra.

PubMed

Dinpajooh, Mohammadhasan; Matyushov, Dmitry V

2014-07-17

Signatures of nonlinear and non-Gaussian dynamics in time-resolved linear and nonlinear (correlation) 2D spectra are analyzed in a model considering a linear plus quadratic dependence of the spectroscopic transition frequency on a Gaussian nuclear coordinate of the thermal bath (quadratic coupling). This new model is contrasted to the commonly assumed linear dependence of the transition frequency on the medium nuclear coordinates (linear coupling). The linear coupling model predicts equality between the Stokes shift and equilibrium correlation functions of the transition frequency and time-independent spectral width. Both predictions are often violated, and we are asking here the question of whether a nonlinear solvent response and/or non-Gaussian dynamics are required to explain these observations. We find that correlation functions of spectroscopic observables calculated in the quadratic coupling model depend on the chromophore's electronic state and the spectral width gains time dependence, all in violation of the predictions of the linear coupling models. Lineshape functions of 2D spectra are derived assuming Ornstein-Uhlenbeck dynamics of the bath nuclear modes. The model predicts asymmetry of 2D correlation plots and bending of the center line. The latter is often used to extract two-point correlation functions from 2D spectra. The dynamics of the transition frequency are non-Gaussian. However, the effect of non-Gaussian dynamics is limited to the third-order (skewness) time correlation function, without affecting the time correlation functions of higher order. The theory is tested against molecular dynamics simulations of a model polar-polarizable chromophore dissolved in a force field water.

Dynamically Consistent Parameterization of Mesoscale Eddies This work aims at parameterization of eddy effects for use in non-eddy-resolving ocean models and focuses on the effect of the stochastic part of the eddy forcing that backscatters and induces eastward jet extension of the western boundary currents and its adjacent recirculation zones.

NASA Astrophysics Data System (ADS)

Berloff, P. S.

2016-12-01

This work aims at developing a framework for dynamically consistent parameterization of mesoscale eddy effects for use in non-eddy-resolving ocean circulation models. The proposed eddy parameterization framework is successfully tested on the classical, wind-driven double-gyre model, which is solved both with explicitly resolved vigorous eddy field and in the non-eddy-resolving configuration with the eddy parameterization replacing the eddy effects. The parameterization focuses on the effect of the stochastic part of the eddy forcing that backscatters and induces eastward jet extension of the western boundary currents and its adjacent recirculation zones. The parameterization locally approximates transient eddy flux divergence by spatially localized and temporally periodic forcing, referred to as the plunger, and focuses on the linear-dynamics flow solution induced by it. The nonlinear self-interaction of this solution, referred to as the footprint, characterizes and quantifies the induced eddy forcing exerted on the large-scale flow. We find that spatial pattern and amplitude of each footprint strongly depend on the underlying large-scale flow, and the corresponding relationships provide the basis for the eddy parameterization and its closure on the large-scale flow properties. Dependencies of the footprints on other important parameters of the problem are also systematically analyzed. The parameterization utilizes the local large-scale flow information, constructs and scales the corresponding footprints, and then sums them up over the gyres to produce the resulting eddy forcing field, which is interactively added to the model as an extra forcing. Thus, the assumed ensemble of plunger solutions can be viewed as a simple model for the cumulative effect of the stochastic eddy forcing. The parameterization framework is implemented in the simplest way, but it provides a systematic strategy for improving the implementation algorithm.

Orientational Dynamics of a Functionalized Alkyl Planar Monolayer Probed by Polarization-Selective Angle-Resolved Infrared Pump-Probe Spectroscopy.

PubMed

Nishida, Jun; Yan, Chang; Fayer, Michael D

2016-10-12

Polarization-selective angle-resolved infrared pump-probe spectroscopy was developed and used to study the orientational dynamics of a planar alkylsiloxane monolayer functionalized with a rhenium metal carbonyl headgroup on an SiO 2 surface. The technique, together with a time-averaged infrared linear dichroism measurement, characterized picosecond orientational relaxation of the headgroup occurring at the monolayer-air interface by employing several sets of incident angles of the infrared pulses relative to the sample surface. By application of this method and using a recently developed theory, it was possible to extract both the out-of-plane and "mainly"-in-plane orientational correlation functions in a model-independent manner. The observed correlation functions were compared with theoretically derived correlation functions based on several dynamical models. The out-of-plane correlation function reveals the highly restricted out-of-plane motions of the head groups and also suggests that the angular distribution of the transition dipole moments is bimodal. The mainly-in-plane correlation function, for the sample studied here with the strongly restricted out-of-plane motions, essentially arises from the purely in-plane dynamics. In contrast to the out-of-plane dynamics, significant in-plane motions occurring over various time scales were observed including an inertial motion, a restricted wobbling motion of ∼3 ps, and complete randomization occurring in ∼25 ps.

Biological sensing and control of emission dynamics of quantum dot bioconjugates using arrays of long metallic nanorods.

PubMed

Sadeghi, Seyed M; Gutha, Rithvik R; Wing, Waylin J; Sharp, Christina; Capps, Lucas; Mao, Chuanbin

2017-01-01

We study biological sensing using plasmonic and photonic-plasmonic resonances of arrays of ultralong metallic nanorods and analyze the impact of these resonances on emission dynamics of quantum dot bioconjugates. We demonstrate that the LSPRs and plasmonic lattice modes of such array can be used to detect a single self-assembled monolayer of alkanethiol at the visible (550 nm) and near infrared (770 nm) range with well resolved shifts. We study adsorption of streptavidin-quantum dot conjugates to this monolayer, demonstrating that formation of nearly two dimensional arrays of quantum dots with limited emission blinking can lead to extra well-defined wavelength shifts in these modes. Using spectrally-resolved lifetime measurements we study the emission dynamics of such quantum dot bioconjugates within their monodispersed size distribution. We show that, despite their close vicinity to the nanorods, the rate of energy transfer from these quantum dots to nanorods is rather weak, while the plasmon field enhancement can be strong. Our results reveal that the nanorods present a strongly wavelength or size-dependent non-radiative decay channel to the quantum dot bioconjugates.

Laser fluence dependence on emission dynamics of ultrafast laser induced copper plasma

DOE PAGES

Anoop, K. K.; Harilal, S. S.; Philip, Reji; ...

2016-11-14

The characteristic emission features of a laser-produced plasma strongly depend strongly on the laser fluence. We investigated the spatial and temporal dynamics of neutrals and ions in femtosecond laser (800 nm, ≈ 40 fs, Ti:Sapphire) induced copper plasma in vacuum using both optical emission spectroscopy (OES) and spectrally resolved two-dimensional (2D) imaging methods over a wide fluence range of 0.5 J/cm 2-77.5 J/cm 2. 2D fast gated monochromatic images showed distinct plume splitting between the neutral and ions especially at moderate to higher fluence ranges. OES studies at low to moderate laser fluence regime confirm intense neutral line emission overmore » the ion emission whereas this trend changes at higher laser fluence with dominance of the latter. This evidences a clear change in the physical processes involved in femtosecond laser matter interaction at high input laser intensity. The obtained ion dynamics resulting from the OES, and spectrally resolved 2D imaging are compared with charged particle measurement employing Faraday cup and Langmuir probe and results showed good correlation.« less

Fluorescence from Multiple Chromophore Hydrogen-Bonding States in the Far-Red Protein TagRFP675.

PubMed

Konold, Patrick E; Yoon, Eunjin; Lee, Junghwa; Allen, Samantha L; Chapagain, Prem P; Gerstman, Bernard S; Regmi, Chola K; Piatkevich, Kiryl D; Verkhusha, Vladislav V; Joo, Taiha; Jimenez, Ralph

2016-08-04

Far-red fluorescent proteins are critical for in vivo imaging applications, but the relative importance of structure versus dynamics in generating large Stokes-shifted emission is unclear. The unusually red-shifted emission of TagRFP675, a derivative of mKate, has been attributed to the multiple hydrogen bonds with the chromophore N-acylimine carbonyl. We characterized TagRFP675 and point mutants designed to perturb these hydrogen bonds with spectrally resolved transient grating and time-resolved fluorescence (TRF) spectroscopies supported by molecular dynamics simulations. TRF results for TagRFP675 and the mKate/M41Q variant show picosecond time scale red-shifts followed by nanosecond time blue-shifts. Global analysis of the TRF spectra reveals spectrally distinct emitting states that do not interconvert during the S1 lifetime. These dynamics originate from photoexcitation of a mixed ground-state population of acylimine hydrogen bond conformers. Strategically tuning the chromophore environment in TagRFP675 might stabilize the most red-shifted conformation and result in a variant with a larger Stokes shift.

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.

A Nonlinear Dynamic Subscale Model for Partially Resolved Numerical Simulation (PRNS)/Very Large Eddy Simulation (VLES) of Internal Non-Reacting Flows

NASA Technical Reports Server (NTRS)

Shih, Tsan-Hsing; Liu, nan-Suey

2010-01-01

A brief introduction of the temporal filter based partially resolved numerical simulation/very large eddy simulation approach (PRNS/VLES) and its distinct features are presented. A nonlinear dynamic subscale model and its advantages over the linear subscale eddy viscosity model are described. In addition, a guideline for conducting a PRNS/VLES simulation is provided. Results are presented for three turbulent internal flows. The first one is the turbulent pipe flow at low and high Reynolds numbers to illustrate the basic features of PRNS/VLES; the second one is the swirling turbulent flow in a LM6000 single injector to further demonstrate the differences in the calculated flow fields resulting from the nonlinear model versus the pure eddy viscosity model; the third one is a more complex turbulent flow generated in a single-element lean direct injection (LDI) combustor, the calculated result has demonstrated that the current PRNS/VLES approach is capable of capturing the dynamically important, unsteady turbulent structures while using a relatively coarse grid.

A reconstruction of global hydroclimate and dynamical variables over the Common Era.

PubMed

Steiger, Nathan J; Smerdon, Jason E; Cook, Edward R; Cook, Benjamin I

2018-05-22

Hydroclimate extremes critically affect human and natural systems, but there remain many unanswered questions about their causes and how to interpret their dynamics in the past and in climate change projections. These uncertainties are due, in part, to the lack of long-term, spatially resolved hydroclimate reconstructions and information on the underlying physical drivers for many regions. Here we present the first global reconstructions of hydroclimate and associated climate dynamical variables over the past two thousand years. We use a data assimilation approach tailored to reconstruct hydroclimate that optimally combines 2,978 paleoclimate proxy-data time series with the physical constraints of an atmosphere-ocean climate model. The global reconstructions are annually or seasonally resolved and include two spatiotemporal drought indices, near-surface air temperature, an index of North Atlantic variability, the location of the intertropical convergence zone, and monthly Niño indices. This database, called the Paleo Hydrodynamics Data Assimilation product (PHYDA), will provide a critical new platform for investigating the causes of past climate variability and extremes, while informing interpretations of future hydroclimate projections.

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

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.

Research on Product Conceptual Design Based on Integrated of TRIZ and HOQ

NASA Astrophysics Data System (ADS)

Xie, Jianmin; Tang, Xiaowo; Shao, Yunfei

The conceptual design determines the success of the final product quality and competition of market. The determination of design parameters and the effective method to resolve parameters contradiction are the key to success. In this paper, the concept of HOQ products designed to determine the parameters, then using the TRIZ contradiction matrix and inventive principles of design parameters to solve the problem of contradictions. Facts have proved that the effective method is to obtain the product concept design parameters and to resolve contradictions line parameters.

Quantitative depth resolved microcirculation imaging with optical coherence tomography angiography (Part ΙΙ): Microvascular network imaging.

PubMed

Gao, Wanrong

2017-04-17

In this work, we review the main phenomena that have been explored in OCT angiography to image the vessels of the microcirculation within living tissues with the emphasis on how the different processing algorithms were derived to circumvent specific limitations. Parameters are then discussed that can quantitatively describe the depth-resolved microvascular network for possible clinic diagnosis applications. Finally,future directions in continuing OCT development are discussed. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved.

Reversible grasp reflexes in normal pressure hydrocephalus.

PubMed

Thomas, Rhys H; Bennetto, Luke; Silva, Mark T

2009-05-01

We present two cases of normal pressure hydrocephalus in combination with grasp reflexes. In both cases the grasp reflexes disappeared following high volume cerebrospinal fluid removal. In one of the cases the grasp reflexes returned over a period of weeks but again resolved following definitive cerebrospinal fluid shunting surgery, and remained absent until final follow up at 9 months. We hypothesise that resolving grasp reflexes following high volume CSF removal has both diagnostic and prognostic value in normal pressure hydrocephalus, encouraging larger studies on the relevance of primitive reflexes in NPH.

Long residence times of rapidly decomposable soil organic matter: application of a multi-phase, multi-component, and vertically-resolved model (TOUGHREACTv1) to soil carbon dynamics

NASA Astrophysics Data System (ADS)

Riley, W. J.; Maggi, F. M.; Kleber, M.; Torn, M. S.; Tang, J. Y.; Dwivedi, D.; Guerry, N.

2014-01-01

Accurate representation of soil organic matter (SOM) dynamics in Earth System Models is critical for future climate prediction, yet large uncertainties exist regarding how, and to what extent, the suite of proposed relevant mechanisms should be included. To investigate how various mechanisms interact to influence SOM storage and dynamics, we developed a SOM reaction network integrated in a one-dimensional, multi-phase, and multi-component reactive transport solver. The model includes representations of bacterial and fungal activity, multiple archetypal polymeric and monomeric carbon substrate groups, aqueous chemistry, aqueous advection and diffusion, gaseous diffusion, and adsorption (and protection) and desorption from the soil mineral phase. The model predictions reasonably matched observed depth-resolved SOM and dissolved organic carbon (DOC) stocks in grassland ecosystems as well as lignin content and fungi to aerobic bacteria ratios. We performed a suite of sensitivity analyses under equilibrium and dynamic conditions to examine the role of dynamic sorption, microbial assimilation rates, and carbon inputs. To our knowledge, observations do not exist to fully test such a complicated model structure or to test the hypotheses used to explain observations of substantial storage of very old SOM below the rooting depth. Nevertheless, we demonstrated that a reasonable combination of sorption parameters, microbial biomass and necromass dynamics, and advective transport can match observations without resorting to an arbitrary depth-dependent decline in SOM turnover rates, as is often done. We conclude that, contrary to assertions derived from existing turnover time based model formulations, observed carbon content and δ14C vertical profiles are consistent with a representation of SOM dynamics consisting of (1) carbon compounds without designated intrinsic turnover times, (2) vertical aqueous transport, and (3) dynamic protection on mineral surfaces.