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At least 307 records · Page 17

On the uncertainty in single molecule fluorescent lifetime and energy emission measurements

Time-correlated single photon counting has recently been combined with mode-locked picosecond pulsed excitation to measure the fluorescent lifetimes and energy emissions of single molecules in a flow stream. Maximum likelihood (ML) and least square methods agree and are optimal when the number of detected photons is large however, in single molecule fluorescence experiments the number of detected photons can be less than 20, 67% of those can be noise and the detection time is restricted to 10 nanoseconds. Under the assumption that the photon signal and background noise are two independent inhomogeneous poisson processes, we derive the exact joint arrival time probably density of the photons collected in a single counting experiment performed in the presence of background noise. The model obviates the need to bin experimental data for analysis, and makes it possible to analyze formally the effect of background noise on the photon detection experiment using both ML or Bayesian methods. For both methods we derive the joint and marginal probability densities of the fluorescent lifetime and fluorescent emission. the ML and Bayesian methods are compared in an analysis of simulated single molecule fluorescence experiments of Rhodamine 110 using different combinations of expected background nose and expected fluorescence emission. While both the ML or Bayesian procedures perform well for analyzing fluorescence emissions, the Bayesian methods provide more realistic measures of uncertainty in the fluorescent lifetimes. The Bayesian methods would be especially useful for measuring uncertainty in fluorescent lifetime estimates in current single molecule flow stream experiments where the expected fluorescence emission is low. Both the ML and Bayesian algorithms can be automated for applications in molecular biology.

Brown, Emery N.↗

Comparison of predicted and actual orbital lifetimes for the SEDS-2 mission

This paper documents a series of estimates of the orbital lifetime of the SEDS-2 flight configuration made prior to the mission. These estimates were made with program LTIME, which has been in use at MSFC for a number of years. Because of the unusual configuration of upper-stage/tether/endmass flown on this mission, and the type of assumptions and inputs used in LTIME, the effective area used in the drag calculation had to be estimated in an unusual way. The final pre-flight predicted lifetime was 28.35 days. In the actual flight, the tether was cut approximately 5 days into the mission. The instrumented endmass plus about 12 km of tether rapidly reentered the atmosphere, and the Delta II Second Stage plus the remaining 8 km of tether reentered on mission day 60. Tracking data was used to reconstruct reentry sequences for the two parts of the configuration after the cut. The predicted lifetimes for the endmass plus tether-fragment were in the range of 0.2 to 2.8 days, depending on the perigee altitudes assumed. The predicted lifetime of the upper-stage plus tether was 56.4 days, which corresponds to reentry on mission day 61, in good agreement with the actual reentry on day 60.

Evans, Steven W.↗

On the Uncertainty in Single Molecule Fluorescent Lifetime and Energy Emission Measurements

Time-correlated single photon counting has recently been combined with mode-locked picosecond pulsed excitation to measure the fluorescent lifetimes and energy emissions of single molecules in a flow stream. Maximum likelihood (ML) and least squares methods agree and are optimal when the number of detected photons is large, however, in single molecule fluorescence experiments the number of detected photons can be less than 20, 67 percent of those can be noise, and the detection time is restricted to 10 nanoseconds. Under the assumption that the photon signal and background noise are two independent inhomogeneous Poisson processes, we derive the exact joint arrival time probability density of the photons collected in a single counting experiment performed in the presence of background noise. The model obviates the need to bin experimental data for analysis, and makes it possible to analyze formally the effect of background noise on the photon detection experiment using both ML or Bayesian methods. For both methods we derive the joint and marginal probability densities of the fluorescent lifetime and fluorescent emission. The ML and Bayesian methods are compared in an analysis of simulated single molecule fluorescence experiments of Rhodamine 110 using different combinations of expected background noise and expected fluorescence emission. While both the ML or Bayesian procedures perform well for analyzing fluorescence emissions, the Bayesian methods provide more realistic measures of uncertainty in the fluorescent lifetimes. The Bayesian methods would be especially useful for measuring uncertainty in fluorescent lifetime estimates in current single molecule flow stream experiments where the expected fluorescence emission is low. Both the ML and Bayesian algorithms can be automated for applications in molecular biology.

Brown, Emery N.↗

The Effect of Tic Coated Balls and Stress on the Lubricant Lifetime of a Synthetic Hydrocarbon (pennzane 2001A) Using a Vacuum Spiral Orbit Tribometer

A vacuum spiral orbit rolling contact tribometer was used to determine effect of varying mean Hertzian stress (1.0, 1.5, 2.0 GPa) and the use of 440C and TiC coated 440C balls on lubricant lifetime of a synthetic hydrocarbon (Pennzane 2001A) on 440C stainless steel. Conditions included 210 rpm, approx. 50 micrograms lubricant, an initial vacuum < 1.3xl0(exp-6) Pa, and room temperature (approx. 23 C). Increasing the mean Hertzian stress resulted in an exponential decrease in lubricant lifetime for both material combinations. Substituting a TiC coated 440C ball showed no increase in lifetime over the 440C ball. The decreasing lifetime with increasing stress level correlated well with energy dissipation calculations.

Jansen, Mark J.↗

Simulations of the Vertical Redistribution of HNO3 by NAT or NAD PSCs: The Sensitivity to the Number of Cloud Particles Formed and the Cloud Lifetime

Recent satellite and in situ measurements have indicated that limited denitrification can occur in the Arctic stratosphere. In situ measurements from the SOLVE campaign indicate polar stratospheric clouds (PSCs) composed of small numbers (about 3 x 10^ -4 cm^-3) of 10-20 micron particles (probably NAT or NAD). These observations raise the issue of whether low number density NAT PSCs can substantially denitrify the air with reasonable cloud lifetimes. In this study, we use a one dimensional cloud model to investigate the verticle redistribution of HNO3 by NAT/NAD PSCs. The cloud formation is driven by a temperature oscillation which drops the temperature below the NAT/NAD formation threshold (about 195 K) for a few days. We assume that a small fraction of the available aerosols act as NAT nuclei when the saturation ratio of HNO3 over NAT(NAD) exceeds 10(l.5). The result is a cloud between about 16 and 20 km in the model, with NAT/NAD particle effective radii as large as about 10 microns (in agreement with the SOLVE data). We find that for typical cloud lifetimes of 2-3 days or less, the net depletion of HNO3 is no more than 1-2 ppbv, regardless of the NAT or NAD particle number density. Repeated passes of the air column through the cold pool build up the denitrification to 3-4 ppbv, and the cloud altitude steadily decreases due to the downward transport of nitric acid. Increasing the cloud lifetime results in considerably more effective denitrification, even with very low cloud particle number densities. As expected, the degree of denitrification by NAT clouds is much larger than that by NAD Clouds. Significant denitrification by NAD Clouds is only possible if the cloud lifetime is several days or more. The clouds also cause a local maximum HNO3 mixing ratio at cloud base where the cloud particles sublimate.

Jensen, Eric J.↗

Lifetime of a Chemically Bound Helium Compound

The rare-gas atoms are chemically inert, to an extent unique among all elements. This is due to the stable electronic structure of the atoms. Stable molecules with chemically bound rare-gas atoms are, however, known. A first such compound, XePtF6, W2S prepared in 1962 and since then a range of molecules containing radon, xenon and krypton have been obtained. Most recently, a first stable chemically bound compound of argon was prepared, leaving neon and helium as the only elements for which stable chemically bound molecules are not yet known. Electronic structure calculations predict that a metastable species HHeF exists, but significance of the result depends on the unknown lifetime. Here we report quantum dynamics calculations of the lifetime of HHeF, using accurate interactions computed from electronic structure theory. HHeF is shown to disintegrate by tunneling through energy barriers into He + HF and H + He + F the first channel greatly dominating. The lifetime of HHeF is more than 120 picoseconds, that of DHeF is 14 nanoseconds. The relatively long lifetimes are encouraging for the preparation prospects of this first chemically bound helium compound.

Chaban, Galina M.↗

The Use of Chlorophyll Fluorescence Lifetime to Assess Phytoplankton Physiology within a River-Dominated Environment

Chlorophyll a fluorescence lifetime was measured for phytoplankton populations inhabiting the three physical zones surrounding the Mississippi River's terminus in the Gulf of Mexico. Observations of river discharge volume, nitrate + nitrite, silicate, phosphate, PAR (Photosynthetically Active Radiation) diffuse attenuation within the water column, salinity, temperature, SPM, and chl a concentration were used to characterize the distribution of chl fluorescence lifetime within a given region within restricted periods of time. 33 stations extending from the Mississippi River plume to the shelf break of the Louisiana coast were surveyed for analysis of chlorophyll fluorescence lifetime during two cruises conducted March 31 - April 6, 2000, and October 24 - November 1, 2000. At each station, two to three depths were chosen for fluorescence lifetime measurement to represent the vertical characteristics of the water column. Where possible, samples were taken from just below the surface and from just above and below the pycnocline. All samples collected were within the 1% light level of the water column (the euphotic zone). Upon collection, samples were transferred to amber Nalgene bottles and left in the dark for at least 15 minutes to reduce the effects of non-photochemical quenching and to insure that photosynthetic reaction centers were open. Before measurements within the phase fluorometer were begun, the instrument was allowed to warm up for no less than one hour.

Hall, Callie M.↗

Lifetimes of bacteriochlorophyll fluorescence in Rhodopseudomonas viridis and Heliobacterium chlorum at low temperatures

Fluorescence lifetimes of isolated membranes of Rhodopseudomonas viridis were measured in the temperature range of 77 K to 25 K. At room temperature, the main component of the fluorescence decay of bacteriochlorophyll (BChl) b had a time constant of 50 ps. In contrast to other purple bacteria, the emission at low temperature was spectrally homogeneous and showed essentially single lifetimes of 140 ps at 77 K and 180 ps at 25 K, with the primary electron donor in the oxidized state. Taking into account the relative fluorescence yields with open and closed reaction centers, we arrive at numbers of 125 ps and 215 ps, respectively, for open reaction centers. These numbers are significantly smaller than expected on the basis of measurements of the efficiency of charge separation, perhaps suggesting that the excitation decay in the absence of reaction centers is considerably faster at low temperature than at room temperature. At least four different spectral components with different lifetimes were observed at 25 K in the emission of Heliobacterium chlorum, a short-wavelength component of about 30 ps and three longer-wavelength components of about 100 ps, 300 ps, and 900 ps. This indicates a strong heterogeneity in the emitting pigment, BChl g-808. The component with the shortest lifetime does not appear to be affected by the redox state of the reaction center and might reflect energy transfer to BChl g species which are connected to the reaction center.

NASA Discipline Number 52-30↗

Chemometric analysis for extraction of individual fluorescence spectrum and lifetimes from a target mixture

The present invention is a system for chemometric analysis for the extraction of the individual component fluorescence spectra and fluorescence lifetimes from a target mixture. The present invention combines a processor with an apparatus for generating an excitation signal to transmit at a target mixture and an apparatus for detecting the emitted signal from the target mixture. The present invention extracts the individual fluorescence spectrum and fluorescence lifetime measurements from the frequency and wavelength data acquired from the emitted signal. The present invention uses an iterative solution that first requires the initialization of several decision variables and the initial approximation determinations of intermediate matrices. The iterative solution compares the decision variables for convergence to see if further approximation determinations are necessary. If the solution converges, the present invention then determines the reduced best fit error for the analysis of the individual fluorescence lifetime and the fluorescence spectrum before extracting the individual fluorescence lifetime and fluorescence spectrum from the emitted signal of the target mixture.

Hallidy, William H.↗

The Effect of a Potentially Low Solar Cycle #24 on Orbital Lifetimes of Fengyun 1-C Debris

The magnitude of Solar Cycle #24 will have a non-trivial impact on the lifetimes of debris pieces that resulted from the intentional hypervelocity impact of the Fengyun 1-C satellite in January 2007. Recent solar flux measurements indicate Solar Cycle #24 has begun in the last few months, and will continue until approximately 2019. While there have been differing opinions on whether the intensity of this solar cycle will be higher or lower than usual, the Space Weather Prediction Center within the National Oceanic Atmospheric Administration (NOAA/SWPC) has recently forecast unusually low solar activity, which would result in longer orbital lifetimes. Using models for both the breakup of Fengyun 1-C and the propagation of the resultant debris cloud, the Orbital Debris Program Office at NASA Johnson Space Center conducted a study to better understand the impact of the solar cycle on lifetimes for pieces as small as 1 mm. Using a modified collision breakup model and PROP3D propagation software, the orbits of nearly 2 million objects 1 mm and larger were propagated for up to 200 years. By comparing a normal solar cycle with that of the NOAA/SWPC forecast low cycle, the effect of the solar flux on the lifetimes of the debris pieces is evaluated. The modeling of the low solar cycle shows an additional debris count of 12% for pieces larger than 10 cm by 2019 when compared to the resultant debris count using a normal cycle. The difference becomes more exaggerated (over 15%) for debris count in the smaller size regimes. However, in 50 years, the models predict the differences in debris count from differing models of Solar Cycle #24 to be less than 10% for all size regimes, with less variance in the smaller sizes. Understanding the longevity of the debris cloud will affect collision probabilities for both operational spacecraft and large derelict objects over the next century and beyond.

Whitlock, David↗

CFCI3 (CFC-11): UV Absorption Spectrum Temperature Dependence Measurements and the Impact on Atmospheric Lifetime and Uncertainty

CFCl3 (CFC-11) is both an atmospheric ozone-depleting and potent greenhouse gas that is removed primarily via stratospheric UV photolysis. Uncertainty in the temperature dependence of its UV absorption spectrum is a significant contributing factor to the overall uncertainty in its global lifetime and, thus, model calculations of stratospheric ozone recovery and climate change. In this work, the CFC-11 UV absorption spectrum was measured over a range of wavelength (184.95 - 230 nm) and temperature (216 - 296 K). We report a spectrum temperature dependence that is less than currently recommended for use in atmospheric models. The impact on its atmospheric lifetime was quantified using a 2-D model and the spectrum parameterization developed in this work. The obtained global annually averaged lifetime was 58.1 +- 0.7 years (2 sigma uncertainty due solely to the spectrum uncertainty). The lifetime is slightly reduced and the uncertainty significantly reduced from that obtained using current spectrum recommendations

photolysis↗

Lifetimes and Occurrence Rates of Dark Vortices on Neptune from 25 Years of Hubble Space Telescope Images

We scoured the full set of blue-wavelength Hubble Space Telescope images of Neptune, finding one additional dark spot in new Hubble data beyond those discovered in 1989, 1994, 1996, and 2015. We report the complete disappearance of the SDS-2015 dark spot, using new Hubble data taken on 2018 September 9–10, as part of the Outer Planet Atmospheres Legacy (OPAL) program. Overall, dark spots in the full Hubble data set have lifetimes of at least one to two years, and no more than six years. We modeled a set of dark spots randomly distributed in time over the latitude range on Neptune that is visible from Earth, finding that the cadence of archival Hubble images would have detected about 70% of these spots if their lifetimes are only one year, or about 85%–95% of simulated spots with lifetimes of two or more years. Based on the Hubble data set, we conclude that dark spots have average occurrence rates of one dark spot every four to six years. Many numerical models to date have simulated much shorter vortex lifetimes, so our findings provide constraints that may lead to improved understanding of Neptune’s wind field, stratification, and humidity.

Hsu, Andrew I.↗

Development of Luminescence Lifetime-Based Surface Temperature Mapping for Environmental Barrier Coatings

Luminescence lifetime-based temperature mapping for thermal barrier coatings (TBCs) has been previously demonstrated up to temperatures approaching 1200 °C. Advantages of this method include insensitivities to reflected radiation and emissivity uncertainties. Because of a push towards greater efficiency turbine engine operation using higher turbine inlet temperatures, there is an ongoing movement from TBC-coated superalloy turbine engine components to SiC/SiC ceramic matrix composite components protected by environmental barrier coatings (EBCs). The useful application of luminescence lifetime-based temperature mapping to EBCs requires a significant increase in high temperature capability from below 1200 °C up into the 1300 to 1500 °C temperature range where the much higher background thermal radiation is a challenging issue. In addition, the luminescing sensing layer must exhibit thermochemical compatibility with the EBC. To meet these requirements, Er-doped Y 2 SiO 5 was selected as the luminescing sensor layer material both for its enhanced temperature sensitivity above 1300 °C and its compatibility with rare-earth disilicate EBC topcoats. Both localized spot temperature measurements as well as luminescence lifetime imaging-based temperature mapping were demonstrated up to 1560 °C for Er-doped Y 2 SiO 5 disks. In addition, temperature mapping capability was demonstrated from a 15 µm thick Er-doped Y 2 SiO 5 layer at the surface of a Sc 2 Si 2 O 7 based EBC topcoat. Both localized spot and temperature mapping by luminescence lifetime imaging were demonstrated up to 1380 °C (upper temperature limit of this slurry-based layered EBC) with excellent suppression of background thermal radiation and no degradation of the Er-doped Y 2 SiO 5 temperature sensing surface layer. The source of the novel enhanced temperature sensitivity above 1300 °C will be discussed as well as a path towards compatibility between sensing layer and EBC topcoat to higher temperatures.

temperature measurement↗

Prediction of the Creep-Fatigue Lifetime of Alloy 617: An Application of Non-destructive Evaluation and Information Integration

A relatively simple method using the nominal constant average stress information and the creep rupture model is developed to predict the creep-fatigue lifetime of Alloy 617, in terms of time to rupture. The nominal constant average stress is computed using the stress relaxation curve. The predicted time to rupture can be converted to number of cycles to failure using the strain range, the strain rate during each cycle, and the hold time information. The predicted creep-fatigue lifetime is validated against the experimental measurements of the creep-fatigue lifetime collected using conventional laboratory creep-fatigue tests. High temperature creep-fatigue tests of Alloy 617 were conducted in air at 950°C with a tensile hold period of up to 1800s in a cycle at total strain ranges of 0.3% and 0.6%. It was observed that the proposed method is conservative in that the predicted lifetime is less than the experimentally determined values. The approach would be relevant to calculate the remaining useful life to a component like a steam generator that might fail by the creep-fatigue mechanism.

36 MATERIALS SCIENCE↗

High Temperature Oxidation Lifetime Modelling of thin-walled components

High temperature material solutions for future power generation applications require longer component lifetimes at higher temperatures to improve durability and efficiency. From a research and development point of view, the lifetimes are too long for experimental verification. Thus, accurate lifetime models are needed. Examples are provided where modeling is being applied to lifetime prediction of thin-walled NiCr wrought alloy components. Specific laboratory experiments have been conducted for alloy X at 900°-950°C in dry air and air with water vapor with cycle times from 1 to 500 h. Along with microstructure characterization, comparisons are made between experiment and model predictions. The eventual goal is to predict both oxidation and mechanical behavior.

Pillai, Rishi↗

Non-Hermitian Topological Theory of Finite-Lifetime Quasiparticles: Prediction of Bulk Fermi Arc Due to Exceptional Point

We introduce a topological theory to study quasiparticles in interacting and/or disordered many-body systems, which have a finite lifetime due to inelastic and/or elastic scattering. The one-body quasiparticle Hamiltonian includes both the Bloch Hamiltonian of band theory and the self-energy due to interactions, which is non-Hermitian when quasiparticle lifetime is finite. We study the topology of non-Hermitian quasiparticle Hamiltonians in momentum space, whose energy spectrum is complex. The interplay of band structure and quasiparticle lifetime is found to have remarkable consequences in zero- and small-gap systems. In particular, we predict the existence of topological exceptional point and bulk Fermi arc in Dirac materials with two distinct quasiparticle lifetimes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Fill and dump measurement of the neutron lifetime using an asymmetric magneto-gravitational trap

The past two decades have yielded several new measurements and reanalysis of older measurements of the neutron lifetime. These have led to a 4.4 standard deviation discrepancy between the most precise measurements of the neutron decay rate producing protons in cold neutron beams and the most precise lifetime measured in neutron storage experiments. Measurements using different techniques are important for investigating whether there are unidentified systematic effects in any of the measurements. In this paper we report a new measurement using the Los Alamos asymmetric magneto-gravitational trap where the surviving neutrons are counted external to the trap using the fill and dump method. In this work, the new measurement gives a free neutron lifetime of $τ_n$ = 876.3(2.4) stat (0.8) syst . Although this measurement is not as precise, it is in statistical agreement with previous results using in situ counting in the same apparatus.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Machine-Learning Assisted Identification of Accurate Battery Lifetime Models with Uncertainty

Reduced-order battery lifetime models, which consist of algebraic expressions for various aging modes, are widely utilized for extrapolating degradation trends from accelerated aging tests to real-world aging scenarios. Identifying models with high accuracy and low uncertainty is crucial for ensuring that model extrapolations are believable, however, it is difficult to compose expressions that accurately predict multivariate data trends; a review of cycling degradation models from literature reveals a wide variety of functional relationships. Here, a machine-learning assisted model identification method is utilized to fit degradation in a stand-out LFP-Gr aging data set, with uncertainty quantified by bootstrap resampling. The model identified in this work results in approximately half the mean absolute error of a human expert model. Models are validated by converting to a state-equation form and comparing predictions against cells aging under varying loads. Parameter uncertainty is carried forward into an energy storage system simulation to estimate the impact of aging model uncertainty on system lifetime. The new model identification method used here reduces life-prediction uncertainty by more than a factor of three (86% ± 5% relative capacity at 10 years for human-expert model, 88.5% ± 1.5% for machine-learning assisted model), empowering more confident estimates of energy storage system lifetime.

25 ENERGY STORAGE↗