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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Long Excited-State Lifetimes in Three-Coordinate Copper(I) Complexes via Triplet–Triplet Energy Transfer to Pyrene-Decorated Isocyanides

There has been much effort to improve excited-state lifetimes in photosensitizers based on earth-abundant first-row transition metals. Copper(I) complexes have gained significant attention in this field, and in most cases, sterically driven approaches are used to optimize their lifetimes. This study presents a series of three-coordinate copper(I) complexes (Cu1–Cu3) where the excited-state lifetime is extended by triplet–triplet energy transfer. The heteroleptic compounds feature a cyclohexyl-substituted β-diketiminate (CyNacNac Me ) paired with aryl isocyanide ligands, giving the general formula Cu(CyNacNac Me )(CN-Ar) (CN-dmp = 2,6-dimethylphenyl isocyanide for Cu1; CN-pyr = 1-pyrenyl isocyanide for Cu2; CN-dmp-pyr = 2,6-dimethyl-4-(1-pyrenyl)phenyl isocyanide for Cu3). The nature, energies, and dynamics of the low-energy triplet excited states are assessed with a combination of photoluminescence measurements at room temperature and 77 K, ultrafast transient absorption (UFTA) spectroscopy, and DFT calculations. The complexes with the pyrene-decorated isocyanides (Cu2 and Cu3) exhibit extended excited-state lifetimes resulting from triplet–triplet energy transfer (TTET) between the short-lived charge-transfer excited state ( 3 CT) and the long-lived pyrene-centered triplet state ( 3 pyr). This TTET process is irreversible in Cu3, producing exclusively the 3 pyr state, and in Cu2, the 3 CT and 3 pyr states are nearly isoenergetic, enabling reversible TTET and long-lived 3 CT luminescence. The improved photophysical properties in Cu2 and Cu3 result in improvements in activity for both photocatalytic stilbene E/Z isomerization via triplet energy transfer and photoredox transformations involving hydrodebromination and C–O bond activation. Furthermore, these results illustrate that the extended excited-state lifetimes achieved through TTET result in newly conceived photosynthetically relevant earth-abundant transition metal complexes.

14 SOLAR ENERGY↗
DOE OSTI2024

Sterically Encumbered Aryl Isocyanides Extend Excited-State Lifetimes and Improve the Photocatalytic Performance of Three-Coordinate Copper(I) β-Diketiminate Charge-Transfer Chromophores

Copper(I) complexes are prominent candidates to replace noble metal-based photosensitizers. We recently introduced a three-coordinate design for copper(I) charge-transfer chromophores that pair β-diketiminate ligands with aryl isocyanides. The excited-state lifetime in these compounds can be extended using a bichromophoric “triplet reservoir” strategy, which comes at the expense of a decrease in excited-state energy and reducing power. In this work, we introduce a complementary, sterically driven strategy for increasing the excited-state lifetimes of these photosensitizers, which gives a higher-energy, more strongly reducing charge-transfer triplet state than does the bichromophore approach. The compounds presented (Cu1–Cu4) have the general formula Cu(CyNacNac Me )(CN-Ar), where CyNacNac Me is a cyclohexyl-substituted β-diketiminate and CN-Ar is an aryl isocyanide with a variable steric profile. Their structural features and electrochemical and photophysical properties are described. The complexes with sterically encumbered 2,6-diisopropylphenyl or m-terphenyl isocyanide ligands (Cu2–Cu4) exhibit prolonged excited-state lifetimes relative to those of the parent 2,6-dimethylphenyl isocyanide compound Cu1. Specifically, one of the m-terphenyl isocyanide compounds, Cu3, displays an excited-state lifetime of 276 ns, approximately 30 times longer than that of Cu1 (9.3 ns). The photoluminescence quantum yield of Cu3 (0.09) also increases by two orders of magnitude compared to that of Cu1 (0.0008). Furthermore, the strong excited-state reducing power (*E ox = –2.4 V vs Fc +/0 ) and long lifetime of Cu3 lead to higher yields in photoredox and photocatalytic isomerization reactions, which include dehalogenation and/or hydrodgenation of benzophenone substrates, C–O bond activation of a lignin model substrate, and photocatalytic E/Z isomerization of stilbene.

14 SOLAR ENERGY↗
DOE OSTI2026

Steric augmentation of three-coordinate Cu( I ) β-diketiminate isocyanide chromophores to achieve microsecond excited-state lifetime

Copper(I) complexes are promising alternatives to noble metal-based photosensitizers. A recently developed class of three-coordinate copper(I) charge-transfer chromophores, pairing β-diketiminate ligands with aryl isocyanides, exhibits excited-state lifetimes that are responsive to the steric profile of the isocyanide, reaching a value of nearly 300 nanoseconds when a substituted m-terphenyl isocyanide was used. In this work, we show that extreme steric augmentation of the β-diketiminate and m-terphenyl isocyanide ligands can lead to further improvements in excited-state lifetime, with one example surpassing 1 µs. This study includes a series of eight compounds of the general formula Cu(RNacNac)(CN-Ar X2 ), where RNacNac is the substituted β-diketiminate and CN-Ar X2 is the substituted m-terphenyl isocyanide. All eight compounds are crystallographically characterized, and their excited-state properties are thoroughly evaluated by a combination of steady-state and time-resolved photoluminescence studies. This combined structural/photophysical approach unveils a correlation between common steric parameters, derived from buried volume (%V bur ) and solid angle analysis, and the excited-state lifetime. Our investigation reveals that the steric profile of the β-diketiminate has a much larger impact on the steric profile and lifetime, whereas the m-terphenyl isocyanide substituents have an unsystematic and subtle influence on these two correlated parameters. Nevertheless, judicious pairing of the two ligands is critical for achieving long excited-state lifetimes.

Kumar, Ashish [University of Houston, TX (United S↗
DOE OSTI2024

Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy

The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited 1 P o 2 s n p Rydberg series and the 1 S e 2 p 2 dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024

Rupprecht, Patrick (ORCID:000000026491793X)↗
DOE OSTI2025

Precision measurement of the B0 meson lifetime using B0→J/ψK∗0 decays with the ATLAS detector

A measurement of the B0$$B^{0}$$ meson lifetime using B0→J/ψK∗0$$ B^{0} \rightarrow J/\psi K^{*0} $$ decays in data from 13 TeV$$\text {TeV}$$ proton–proton collisions with an integrated luminosity of 140fb-1$$ 140~\mathrm {fb^{-1}} $$ recorded by the ATLAS detector at the LHC is presented. The measured effective lifetime is τ=1.5053±0.0012(stat.)±0.0035(syst.)ps.$$ \tau = 1.5053\pm 0.0012~\mathrm {(stat.)} \pm 0.0035~\mathrm {(syst.)~ps}. $$The average decay width extracted from the effective lifetime, using parameters from external sources, is Γd=0.6639±0.0005(stat.)±0.0016(syst.)±0.0038(ext.)ps-1,$$\begin{aligned} \Gamma _d = 0.6639\pm 0.0005~\mathrm {(stat.)} \pm 0.0016~\mathrm {(syst.)}\\ \pm 0.0038~\text {(ext.)} \text {~ps}^{-1}, \end{aligned}$$where the uncertainties are statistical, systematic and from external sources. The earlier ATLAS measurement of Γs$$\Gamma _s$$ in the Bs0→J/ψϕ$$B^{0}_{s} \rightarrow J/\psi \phi $$ decay was used to derive a value for the ratio of the average decay widths Γd$$\Gamma _d$$ and Γs$$\Gamma _s$$ for B0$$B^{0} $$ and Bs0$$B^{0}_{s} $$ mesons respectively, of ΓdΓs=0.9905±0.0022(stat.)±0.0036(syst.)±0.0057(ext.).$$ \frac{\Gamma _d }{\Gamma _s } = 0.9905\pm 0.0022~\text {(stat.)} \pm 0.0036~\text {(syst.)} \pm 0.0057~\text {(ext.)}. $$The measured lifetime, average decay width and decay width ratio are in agreement with theoretical predictions and with measurements by other experiments. This measurement provides the most precise result of the effective lifetime of the B0$$B^{0}$$ meson to date.

Aad, G↗
NASA NTRS1980

The lifetime of the OH radical in comets at 1 AU

It has been shown that the photochemical lifetime of OH in comets is a function of the comet's radial velocity. The calculated lifetime at 1 AU can vary between 69,000 and 210,000 sec for radial velocities that vary from -58 to +59 km/sec. A comparison between the scale lengths observed for three comets and those calculated based upon the theoretical lifetime has been made. This comparison shows that in two of the comets the lifetime derived from the scale lengths is a factor of 1.7 larger than the theoretical lifetime. Suggestions are made about the origin of this discrepancy.

Jackson, W. M.↗
NASA NTRS1988

Minority-carrier lifetime analysis of silicon epitaxy and bulk crystals with nonuniformly distributed defects

Existing analyses of the pulsed response of an MOS capacitor for minority-carrier lifetime determination result in a lifetime value averaged over most of the depletion region width. In this report, an analysis of MOS C-t data is presented that enables minority-carrier generation lifetime to be plotted as a function of depletion region depth. The technique is shown to be useful for samples with bulk or buried interfacial layer defects that have defect-free surfaces. Data are presented for intrinsically gettered bulk crystals and extrinsically gettered Si(2-pct Ge) epitaxial layers with misfit dislocations. In addition, for samples that do have uniform lifetimes, the measurement time required for determining carrier lifetime has been reduced by more than an order of magnitude.

Radzimski, Zbignew↗
NASA NTRS1989

Lifetime predictions for the Solar Maximum Mission (SMM) and San Marco spacecraft

Lifetime prediction techniques developed by the Goddard Space Flight Center (GSFC) Flight Dynamics Division (FDD) are described. These techniques were developed to predict the Solar Maximum Mission (SMM) spacecraft orbit, which is decaying due to atmospheric drag, with reentry predicted to occur before the end of 1989. Lifetime predictions were also performed for the Long Duration Exposure Facility (LDEF), which was deployed on the 1984 SMM repair mission and is scheduled for retrieval on another Space Transportation System (STS) mission later this year. Concepts used in the lifetime predictions were tested on the San Marco spacecraft, which reentered the Earth's atmosphere on December 6, 1988. Ephemerides predicting the orbit evolution of the San Marco spacecraft until reentry were generated over the final 90 days of the mission when the altitude was less than 380 kilometers. The errors in the predicted ephemerides are due to errors in the prediction of atmospheric density variations over the lifetime of the satellite. To model the time dependence of the atmospheric densities, predictions of the solar flux at the 10.7-centimeter wavelength were used in conjunction with Harris-Priester (HP) atmospheric density tables. Orbital state vectors, together with the spacecraft mass and area, are used as input to the Goddard Trajectory Determination System (GTDS). Propagations proceed in monthly segments, with the nominal atmospheric drag model scaled for each month according to the predicted monthly average value of F10.7. Calibration propagations are performed over a period of known orbital decay to obtain the effective ballistic coefficient. Progagations using plus or minus 2 sigma solar flux predictions are also generated to estimate the despersion in expected reentry dates. Definitive orbits are compared with these predictions as time expases. As updated vectors are received, these are also propagated to reentryto continually update the lifetime predictions.

Smith, E. A.↗
NASA NTRS1990

Tropospheric OH and the lifetimes of hydrochlorofluorocarbons

Hydrochlorofluorocarbons (HCFCs) may be used as alternatives for the chlorofluorocarbons (CFCs). Lifetimes for the HCFCs are predicted here in two ways: integrating their loss with a global model and scaling to another compound with a better known lifetime. Both approaches are shown to yield similar results. Three-dimensional fields of modeled tropospheric OH concentrations are used to calculate lifetimes against destruction by OH for the HCFCs and other hydrogenated halocarbons. The lifetimes of various hydro-halocarbons are shown to be insensitive to possible spatial variations and seasonal cycles. It is possible to scale the HCFC lifetimes to that of methyl chloroform or methane by using a ratio of the rate coefficients for reaction with OH at an appropriate temperature, about 277 K.

Prather, Michael↗
NASA NTRS1990

Lifetime measurements by open circuit voltage decay in GaAs and InP diodes

Minority carrier lifetimes in the base of solar cells made on GaAs and InP were measured by the open-circuit voltage decay method. The measurement technique and the conditions under which the minority carrier lifetimes can be measured are described. Minority carrier lifetimes ranging from 1.6 to 34 ns in InP of different doping concentrations were measured. A minority carrier lifetime of 6 ns was measured in n-type GaAs, which agrees well with the lifetime of 5.7 ns measured by transient microwave reflection.

Bhimnathwala, H. G.↗
NASA NTRS1984

Moisture dependence of positron lifetime in Kevlar-49

Because of filamentary character of Kevlar-49 aramid fibers, there is some concern about the moisture uptake and its effect on plastic composites reinforced with Kevlar-49 fibers. As part of continuing studies of positron lifetime in polymers, we have measured positron lifetime spectra in Kevlar-49 fibers as a function of their moisture content. The long lifetime component intensities are rather low, being only of the order of 2-3 percent. The measured values of long component lifetimes at various moisture levels in the specimens are as follows: 2072 +/- 173 ps (dry); 2013 +/- 193 ps (20.7 percent saturation); 1665 +/- 85 ps (25.7 percent saturation); 1745 +/- 257 ps (32.1 percent saturation); and 1772 +/- 217 ps (100 percent saturation). It is apparent that the long component lifetime at first decreases and then increases as the specimen moisture content increases. These results have been compared with those inferred from Epon-815 and Epon-815/K-49 composite data.

Singh, Jag J.↗
NASA NTRS1994

Lifetimes of lunar satellite orbits

The Space Exploration Initiative has generated a renewed interest in lunar mission planning. The lunar missions currently under study, unlike the Apollo missions, involve long stay times. Several lunar gravity models have been formulated, but mission planners do not have enough confidence in the proposed models to conduct detailed studies of missions with long stay times. In this report, a particular lunar gravitational model, the Ferrari 5 x 5 model, was chosen to determine the lifetimes for 100-km and 300-km perilune altitude, near-circular parking orbits. The need to analyze orbital lifetimes for a large number of initial orbital parameters was the motivation for the formulation of a simplified gravitational model from the original model. Using this model, orbital lifetimes were found to be heavily dependent on the initial conditions of the nearly circular orbits, particularly the initial inclination and argument of perilune. This selected model yielded lifetime predictions of less than 40 days for some orbits, and other orbits had lifetimes exceeding a year. Although inconsistencies and limitations are inherent in all existing lunar gravity models, primarily because of a lack of information about the far side of the moon, the methods presented in this analysis are suitable for incorporating the moon's nonspherical gravitational effects on the preliminary design level for future lunar mission planning.

Meyer, Kurt W.↗
NASA NTRS1994

Report on concentrations, lifetimes, and trends of CFCs, halons, and related species

The atmospheric lifetimes of molecules containing chlorine and bromine are the dominant parameters influencing their ability to promote enhanced ozone destruction in the stratosphere. The purpose of this report is to assess the present state of knowledge of the lifetimes of halocarbons using two complementary approaches. First, a time series of measurements of gas concentrations is used together with information on their emissions histories and a computational model of atmospheric circulation and chemistry to infer lifetimes through a mass balance approach. Second, an atmospheric chemical-dynamical model is used with detailed information on the chemistry and spectroscopy of the molecules of interest to calculate lifetimes. The lifetimes determined by these two methods are then compared. Attention is focused most closely on fully halogenated chlorine- and bromine-containing molecules, primarily the chlorofluorocarbons, and the halons, because of their ability to deliver chlorine and bromine to the stratosphere. Some attention will be given to those molecules containing hydrogen, which are subject to removal in the troposphere primarily by reaction with OH and by other processes.

Kaye, J. A.↗
NASA NTRS1999

The Effect of Stress and TiC Coated Balls on Lubricant Lifetimes Using a Vacuum Ball-on-Plate Rolling Contact Tribometer

A vacuum ball-on-plate rolling contact tribometer was used to determine the relative lifetimes of a perfluoropolyether (Krytox 143 AC) on 440C stainless steel. The effect of mean Hertzian stresses (0.75, 1.0, 1.5 and 2.0 GPa) and the use of TiC coated balls on lubricant lifetime was studied. Other conditions included: approximately 100 rpm, approximately 50 micrograms of lubricant, an initial vacuum level of less than 1.0 x 1O(exp -8) Torr, and room temperature (approximately 23 C). increasing the mean Hertzian stress from 0.75 to 2.0 GPa results in an exponential decrease in lubricant lifetime for both material combinations. However. substituting a TiC ball for the 440C ball quadrupled lifetime at low stress levels (0.75 and 1.0 GPa) and doubled life at higher stresses (1.5 and 2.0 GPa). The reduced reactivity of the TiC surface with the PFPE lubricant is considered to be the reason for this enhancement. Decreasing lifetime with increasing stress levels correlated well with energy dissipation calculations.

Jones, William R., Jr.↗
NASA NTRS1999

The Effect of Stress and TiC Coated Balls on Lubricant Lifetimes Using a Vacuum Ball-on-Plate Rolling Contact Tribometer

A vacuum ball-on-plate rolling contact tribometer was used to determine the relative lifetimes of a perfluoropolyether (Krytox 143 AC) on 440C stainless steel. The effect of mean Hertzian stresses (0.75, 1.0, 1.5, and 2.0 GPa) and the use of TiC-coated balls on lubricant lifetime was studied. Other conditions included: 100 rpm, 50 micro-g of lubricant, an initial vacuum level of less than 1.0 x 10(exp -8) Torr, and room temperature (23 C). Increasing the mean Hertzian stress from 0.75 to 2.0 GPa results in an exponential decrease in lubricant lifetime for both material combinations. However, substituting a TiC ball for the 440C ball quadrupled lifetime at low stress levels (0.75 and 1.0 GPa) and doubled life at higher stresses (1.5 and 2.0 GPa). The reduced reactivity of the TiC surface with the PFPE lubricant is considered to be the reason for this enhancement. Decreasing lifetime with increasing stress levels correlated well with energy dissipation calculations.

Jones, William R., Jr.↗
NASA NTRS1998

Perimeter Governed Minority Carrier Lifetimes in 4H-SiC p(+)-n Diodes Measured by Reverse Recovery Switching Transient Analysis

Minority carrier lifetimes in epitaxial 4H-SiC p(+)-n junction diodes were measured via an analysis of reverse recovery switching characteristics. Behavior of reverse recovery storage time (t(s)) as a function of initial ON-state forward current (I(F)) and OFF-state reverse current (I(R)) followed well-documented trends which have been observed for decades in silicon p-n rectifiers. Average minority carrier (hole) lifetimes (tau(p)) calculated from plots of t(s) vs I(R)/I(F) strongly decreased with decreasing device area. Bulk and perimeter components of average hole lifetimes were separated by plotting 1/tau(p) as a function of device perimeter-to- area ratio (P/A). This plot reveals that perimeter recombination is dominant in these devices, whose areas are all less than 1 sq mm. The bulk minority carrier (hole) lifetime extracted from the 1/tau(p) vs P/A plot is approximately 0.7 micro-s, well above the 60 ns to 300 ns average iit'eptimes obtained when perimeter recombination effects are ignored in the analysis. Given the fact that there has been little previous investigation of bipolar diode and transistor performance as a function of perimeter-to-area ratio, this work raises the possibility that perimeter recombination may be partly responsible for poor effective minority carrier lifetimes and limited performance obtained in many previous SiC bipolar junction devices.

Neudeck, Philip G.↗
NASA NTRS2000

The Effect of Stress and TiC Coated Balls on Lifetime of a Perfluoropolyalkylether Using a Vacuum Rolling Contact Tribometer

A vacuum spiral orbit tribometer (SOT) was used to determine the relative lifetimes of a branched perfluoropolyalkylether (PFPAE) on 440 C stainless steel. The effect of varying the mean Hertzian stress (0.75, 1.0, 1.5 and 2.0 GPa) and the use of TiC coated balls on lubricant lifetime was studied. Other conditions included: approx. 100 rpm, approx. 50 micro-g of lubricant, an initial vacuum level of less than 1.3 x 10(exp -6) Pa (less than 10 x 10(exp -8) Torr), and room temperature (approx. 23 C). Increasing the mean Hertzian stress from 0.75 to 2.0 GPa results in an exponential decrease in lubricant lifetime for both material combinations. However, substituting a TiC ball for the 440 C ball quadrupled lifetime at low stress levels (0.75 and 1.0 GPa) and doubled life at higher stresses (1.5 and 2.0 GPa), The reduced reactivity of the TiC surface with the PFPAE lubricant is considered to be the reason for this enhancement. Decreasing lifetime with increasing stress levels correlated well with energy dissipation calculations.

Jones, William R., Jr.↗
NASA NTRS2001

Relative Lifetimes of Several Space Liquid Lubricants Using a Vacuum Spiral Orbit Tribometer (SOT)

A vacuum spiral orbit rolling contact tribometer (SOT) was used to determine the relative lifetimes of several unformulated space liquid lubricants. The lubricants tested included a synthetic hydrocarbon (Pennzane 2001 A), three perfluoropolyethers (Krytox 143AC, Fomblin Z25, and Brayco 815Z), three silahydrocarbons (a tri, a tetra, and a penta) and a polyalphaolefin (Nye PAO-100). The SOT simulates the ball motions in an angular contact bearing and tribochemically degrades microgram quantities of lubricant. Test failure is determined when a preset friction coefficient is exceeded. Relative lifetime (orbits/micro-g) is defined as the number of ball orbits to failure divided by the amount of lubricant on the ball. Conditions included 10 to 200 rpm rotational speed, approximately 50 micro-g lubricant, an initial vacuum < 1.3x10(exp -6) Pa, room temperature (approximately 23 C), a mean Hertzian stress of 1.5 GPa, and 440 C stainless steel specimens. Lubricated lifetimes from longest to shortest were Pennzane 2001 A, the silahydrocarbons and the PAO-100, 143AC, ZI-5, and then 815Z. Relative lifetimes compare favorably to full-scale vacuum gimbal bearing tests. The effect of varying the mean Hertzian stress on the lifetime of some of the lubricants was examined.

Jansen, Mark J.↗