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NASA NTRS2013

Modeling Insights into Deuterium Excess as an Indicator of Water Vapor Source Conditions

Deuterium excess (d) is interpreted in conventional paleoclimate reconstructions as a tracer of oceanic source region conditions, such as temperature, where precipitation originates. Previous studies have adopted co-isotopic approaches to estimate past changes in both site and oceanic source temperatures for ice core sites using empirical relationships derived from conceptual distillation models, particularly Mixed Cloud Isotopic Models (MCIMs). However, the relationship between d and oceanic surface conditions remains unclear in past contexts. We investigate this climate-isotope relationship for sites in Greenland and Antarctica using multiple simulations of the water isotope-enabled Goddard Institute for Space Studies (GISS) ModelE-R general circulation model and apply a novel suite of model vapor source distribution (VSD) tracers to assess d as a proxy for source temperature variability under a range of climatic conditions. Simulated average source temperatures determined by the VSDs are compared to synthetic source temperature estimates calculated using MCIM equations linking d to source region conditions. We show that although deuterium excess is generally a faithful tracer of source temperatures as estimated by the MCIM approach, large discrepancies in the isotope-climate relationship occur around Greenland during the Last Glacial Maximum simulation, when precipitation seasonality and moisture source regions were notably different from present. This identified sensitivity in d as a source temperature proxy suggests that quantitative climate reconstructions from deuterium excess should be treated with caution for some sites when boundary conditions are significantly different from the present day. Also, the exclusion of the influence of humidity and other evaporative source changes in MCIM regressions may be a limitation of quantifying source temperature fluctuations from deuterium excess in some instances.

simulation↗

DOE OSTI2025

Environmental Controls on Water Vapor Deuterium Excess in the Coastal Boundary Layer: An Information Theory Perspective

We use information theory to quantify the environmental controls on water vapor deuterium excess (D-excess) in coastal Southern California from June 2023 through February 2024. Using Shannon entropy, mutual information (MI), and joint mutual information, metrics that capture both linear and nonlinear relationships, we identify the most informative variables and variable combinations governing D-excess across contrasting marine and continental regimes. Relative humidity with respect to sea surface temperature (RHS) is consistently the strongest individual predictor, explaining up to 27% of D-excess variability during marine conditions but only 10% in continental air masses. The Relative humidity(RHS) + sea surface temperature (SST) combination demonstrates synergistic effects, where their joint influence (explaining up to 36% of D-excess variability) exceeds what either variable achieves individually, confirming their coupled influence on deuterium excess. Wind direction complements RHS most effectively during continental conditions. The best three-variable combination (RHS + SST + Planetary Boundary Layer height) explains 38% of D-excess variability in marine air, while no combination exceeds 20% explanatory power during continental periods. Information theory shows that heteroscedasticity in D-excess relationships indicates regime shifts in controlling processes and quantifies fundamental constraints on predictor variables: some environmental factors like surface pressure or water vapor flux contain insufficient information content to explain D-excess variability regardless of their physical relevance. These results highlight the different predictability limits between marine and continental regimes, challenging the adequacy of linear models and providing a rigorous framework for quantifying the information content of isotope-climate relationships with implications for both modern and paleoclimate applications.

information theory↗

DOE OSTI2021

Comparing deuterium excess to large-scale precipitation recycling models in the tropics

Precipitation recycling is essential to sustaining regional ecosystems and water supplies, and it is impacted by land development and climate change. This is especially true in the tropics, where dense vegetation greatly influences recycling. Unfortunately, large-scale models of recycling often exhibit high uncertainty, complicating efforts to estimate recycling. Here, we examine how deuterium excess (d-excess), a stable-isotope quantity sensitive to recycling effects, acts as an observational proxy for recycling. While past studies have connected variability in d-excess to precipitation origins at local or regional scales, our study leverages >3000 precipitation isotope samples to quantitatively compare d-excess against three contemporary recycling models across the global tropics. Using rank-correlation, we find statistically significant agreement ( $\bar \tau = 0.52$ τ ¯ = 0.52 to $0.70$ 0.70 ) between tropical d-excess and recycling that is strongly mediated by seasonal precipitation, vegetation density, and scale mismatch. Our results detail the complex relationship between d-excess and precipitation recycling, suggesting avenues for further investigation.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1996

Sulfur and Hydrogen Isotope Anomalies in Organic Compounds from the Murchison Meteorite

Isotopic measurements have been made on organic sulfur and phosphorus compounds recently discovered in the Murchison meteorite. Carbon, hydrogen and sulfur measurements were performed on individual members of the organic sulfur compounds, alkyl sulfonates; and carbon and hydrogen measurements were made on bulk alkyl phosphonates. Cooper and Chang reported the first carbon isotopic measurements of Murchison organic sulfonates, providing insight into the potential synthetic mechanisms of these and, possibly, other organic species. Hydrogen isotopic measurements of the sulforiates now reveal deuterium excesses ranging from +660 to +2730 %. The deuterium enrichments indicate formation of the hydrocarbon portion of these compounds in a low temperature astrophysical environment consistent with that of dense molecular clouds. Measurements of the sulfur isotopes provide further constraints on the origin and mechanism of formation of these organic molecules. Recently, there has been growing documentation of sulfur isotopic anomalies in meteoritic material. Thiemens and Jackson have shown that some bulk ureilites possess excess S-33 and Thiemens et al. have reported excess S-33 in an oldhamite separate from the Norton County meteorite. Rees and Thode reported a large S-33 excess in an Allende acid residue, however, attempts to verify this measurements have been unsuccessful, possibly due to the heterogeneous nature of the carrier phase. With the recognition that sulfur isotopes may reflect chemistry in the protosolar nebula or the precursor molecular cloud, identification of potential carriers is of considerable interest. In the present study, the stable isotopes of sulfur were measured in methane sulfonic acid extracted from the Murchison meteorite. The isotopic composition was found to be: (delta)S-33 = 2.48 %, (delta)S-34 = 2.49 % and (delta)S-36 = 6.76 %. Based upon analysis of more than 60 meteoritic and numerous terrestrial samples, the mass fractionation lines are defined by Delta-33 = (delta)S-33 -0.50(delta)S-34 and Delta-36 = (delta)s-36 - 1.97 (delta)S-34. From these relationships Delta-33 = 1.24 % and Delta-36 = 0.89 % are observed. These anomalies, particularly the Delta-33, lie well outside the range of analytical uncertainty. They are the largest observed in any meteoritic component and the first found in an organosulfur compound. As discussed by Thiemens and Jackson, due to it's position on the periodic chart, sulfur undergoes chemically induced mass independent isotopic fractionations as does oxygen. Experiments by Mauersberger et. al. show that in such processes, the magnitude of fractionation for the different isotopically substituted species varies with mass and angular momentum; thus, anomalies are expected for both S-33 and S-36, but not necessarily of the same magnitude. Laboratory experiments have also confirmed that chemically produced, mass independent fractionations are mediated by molecular symmetry factors. A chemical source of fractionation requires that the sulfur isotopic anomaly was established in the gas phase, probably in reactions involving symmetric CS2. The discovery of an anomalous sulfur isotopic composition in a specific molecule containing excess deuterium is an important advance in the understanding of the cosmochemistry of sulfur. This evidence suggests that methanesulfonic acid was synthesized by interstellar processes. Further measurements and details of possible synthesis and fractionation mechanisms will be presented.

Cooper, G. W.↗

DOE OSTI2025

Groundwater flowpath characteristics drive variability in per- and polyfluoroalkyl substances (PFAS) loading across a stream-wetland system

Groundwater dependent ecosystems in areas with industrial and military land use are at risk of direct exposure to a wide range of contaminants, including PFAS chemicals. Glaciated terrain often has mixed high and low permeability sediments coupled with groundwater flow-through lake features. These hydrogeologic attributes create highly complex ‘source to seep’ dynamics that make spatiotemporal contaminant transport patterns difficult to predict. We investigated one such system in detail using a suite of heat-tracing and chemical methods. Numerous (n=57) preferential groundwater discharge zones (vertical flux rates ranging 0.2 to 3.2 m/d) were identified across the upper Quashnet River stream-wetland system in Mashpee, MA, USA, adjacent to an Air Force Base with several known PFAS source areas. Surface-water and groundwater samples were collected and analyzed (n=145) for precursors and terminal PFAS compounds between March and September 2022. Samples were collected at identified seeps along the Quashnet River (n=59), from wells upgradient from the stream-wetland system (n= 44), from contributing flow-through kettle lakes (n=8), and at multiple locations along the Quashnet River (n=34). Samples from seeps and wells had measured PFAS concentrations ranging from non-detect to approximate 3,500 ng/L (mean= 1,650 ng/L), and a range of deuterium excess values (3.2 to 15.9 per mil) indicative of varying degrees of groundwater-lake interaction prior to emergence at the discharge zones. Groundwater-lake interaction along flowpaths that sourced the sampled seeps was farther supported by significant correlations (p < 0.01) between deuterium excess and %PFAS precursors, and between %PFAS precursors and multiple terminal PFAS compounds (e.g., PFPeS, PFBS, PFHxS). However, some sampled seeps contributing groundwater to the stream-wetland system had much higher total PFAS concentrations (>1000 ng/L) than the upgradient kettle lakes, despite showing lake (evaporative) isotopic signatures, indicating the potential for groundwater flowpath convergence at wetland discharge zones and the influence of lakebed PFAS precursor reactions. PFAS compounds and water isotopic composition at sampled multilevel groundwater wells, rivers, lakes, and seeps suggest that a complex mixture of source groundwater and flowpath characteristics are responsible for diverse observed PFAS mixtures at preferential discharge zones across the stream-wetland system. Further, total PFAS loading patterns to the Quashnet River via groundwater discharge remained remarkably similar from winter to summer to fall conditions, despite a regional dry period in late summer 2022 with the upper river channel completely drying. This work addresses gaps in the existing PFAS literature by demonstrating the importance of subsurface fate and transport on PFAS compound concentrations in controlling contaminant mass loading in preferential groundwater discharge zones and presents a transferrable field toolkit for efficient characterization of spatially preferential PFAS transport dynamics.

Contaminant transport↗

DOE OSTI2026

A New Theoretical Framework for Parameterizing Nonequilibrium Fractionation During Evaporation From the Ocean

The evaporation model for water isotopes proposed by Craig and Gordon (1965, https://books.google.co.in/books?id=6wIKAQAAIAAJ) is used in most isotope-enabled atmospheric models for the parameterization of nonequilibrium fractionation during evaporation from the ocean. In this model, one of the most uncertain parameters is the nonequilibrium fractionation factor 𝛼 𝑘 . Many isotope models use the formulation of Merlivat and Jouzel (1979, https://doi.org/10.1029/jc084ic08p05029), which parameterizes 𝛼 𝑘 as a function of wind speed and distinguishes between a smooth and a rough regime to account for the effect of ocean waves. The resulting discontinuity in 𝛼 𝑘 between smooth and rough regimes has been disputed by several empirical studies. Here, we present a new approach to parameterizing 𝛼𝑘 by explicitly accounting for the influence of wave drag on the momentum flux near the surface. Following Cifuentes-Lorenzen et al. (2018, https://doi.org/10.1007/s10546-018-0376-0), we add a third wave-induced component to the total momentum flux, in addition to the viscous and turbulent components, and extend the definition of the eddy viscosity to account for the momentum flux due to waves and turbulent dissipation near the surface. The new scheme predicts a slight decrease of 𝛼 𝑘 with wind speed, similar to the smooth-regime parameterization of Merlivat and Jouzel (1979, https://doi.org/10.1029/jc084ic08p05029). This new parameterization is incorporated into the isotope-enabled Community Atmosphere Model, where it improves the correlation of simulated and measured vapor deuterium excess relative to the default version and a version with constant 𝛼 𝑘 , suggesting that it may be used as a valid representation of fractionation during evaporation from the ocean in future isotope models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Stream water sourcing from high-elevation snowpack inferred from stable isotopes of water: a novel application of d-excess values

About 80 % of the precipitation at the Colorado River's headwaters is snow, and the resulting snowmelt-driven hydrograph is a crucial water source for about 40 million people. Snowmelt from alpine and subalpine snowpack contributes substantially to groundwater recharge and river flow. However, the dynamics of snowmelt progression are not well understood because observations of the high-elevation snowpack are difficult due to challenging access in complex mountainous terrain as well as the cost and labor intensity of currently available methods. We present a novel approach to infer the processes and dynamics of high-elevation snowmelt contributions predicated upon stable hydrogen and oxygen isotope ratios observed in streamflow. We show that deuterium-excess (d-excess) values of stream water could serve as a comparatively cost-effective proxy for a catchment-integrated signal of high-elevation snowmelt contributions to catchment runoff. We sampled stable hydrogen and oxygen isotope ratios of the precipitation, snowpack, and stream water in the East River, a headwater catchment of the Colorado River, and the stream water of larger catchments at sites on the Gunnison River and Colorado River. The d-excess of snowpack increased with elevation; the upper subalpine and alpine snowpack (> 3200 m) had substantially higher d-excess compared to lower elevations (< 3200 m) in the study area. The d-excess values of stream water reflected this because d-excess values increased as the higher-elevation snowpack contributed more to stream water generation later in the snowmelt/runoff season. End-member mixing analyses based on the d-excess data showed that the share of high-elevation snowmelt contributions within the snowmelt hydrograph was on average 44 % and generally increased during melt period progression, up to 70 %. The observed pattern was consistent during 6 years for the East River, and a similar relation was found for the larger catchments on the Gunnison and Colorado rivers. High-elevation snowpack contributions were found to be higher for years with lower snowpack and warmer spring temperatures. Thus, we conclude that the d-excess of stream water is a viable proxy to observe changes in high-elevation snowmelt contributions in catchments at various scales. Inter-catchment comparisons and temporal trends of the d-excess of stream water could therefore serve as a catchment-integrated measure to monitor if mountain systems rely on high-elevation water inputs more during snow drought compared to years of average snowpack depths.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Deep desert aquifers as an archive for Mid- to Late Pleistocene hydroclimate: An example from the southeastern Mediterranean

Many efforts have been made to illuminate the nature of past hydroclimates in semi-arid and arid regions, where current and future shifts in water availability have enormous consequences on human subsistence. Deep desert aquifers, where groundwater is stored for prolonged periods, might serve as a direct record of major paleo-recharge events. To date, groundwater-based paleoclimate reconstructions have mainly focused on a relatively narrow timescale (up to ∼40 kyr), limited by the relatively short half-life of the widely used radiocarbon (5.73 kyr). Here we demonstrate the usage of deep regional aquifers in the arid southeastern Mediterranean as a hydroclimate archive for earlier Mid-to-Late Pleistocene epochs. State-of-the-art dating tools, primarily the 81 Kr radioisotope (t 1/2 = 229 kyr), were combined with other atmosphere-derived tracers to illuminate the impact of four distinguishable wetter episodes over the past 400 kyr, with differences in climatic conditions and paleo-recharge locations. Variations in stable water isotope composition suggest moisture transport from more proximal (Mediterranean) and distal (Atlantic) sources to different parts of the region at distinct times. Large variability in the computed noble gas-based recharge temperature (NGT), ranging ~15–30 °C, cannot be explained by climate variations solely, and points to different recharge pathways, including geothermal heating in the deep unsaturated zone and recharge from high-elevation (colder) regions. The obtained groundwater record complements and enhances the interpretation of other terrestrial archives in the arid region, including a contribution of valuable information regarding the moisture source origin as reflected in the deuterium-excess values, which is unattainable from the common practice analysis of calcitic cave deposits. We conclude that similar applications in other deep (hundred-m-order) regional groundwater systems (e.g., the Sahara desert aquifers) can significantly advance our understanding of long-term (up to 1 Myr) paleo-hydroclimate in arid regions, including places where no terrestrial remnants, such as cave, lake, and spring sediments, are available.

Atom Trap Trace Analysis↗

DOE OSTI2026

Water Vapor Isotopic Measurements during CAPE-K Field Campaign Report

CAPE-K_ISO deployed a Picarro L-2130 water vapor isotope analyzer to the Kennaook/Cape Grim Baseline Air Pollution Station in northwest Tasmania as a guest instrument within the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) User Facility’s Cloud and Precipitation Experiment at Kennaook (CAPE-K). The project was led by Joseph Galewsky at the University of New Mexico and supported the second ARM Mobile Facility (AMF2) deployment by adding continuous measurements of water vapor mixing ratio, delta-18O, delta-D, and deuterium excess in marine boundary-layer air.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

CAPE-K_ISO: Water vapor isotopic measurements from Western Tasmania

This dataset provides processed 1-minute water vapor isotope observations from the Water Vapor Isotopic Measurements During CAPE-K project at the Kennaook/Cape Grim Baseline Air Pollution Station in northwestern Tasmania. Measurements were made with a Picarro L-2130 cavity ring-down spectroscopy analyzer during the CAPE-K deployment. The dataset includes water vapor mixing ratio, d18O, dD, deuterium excess, and propagated 1-sigma uncertainties. Isotope ratios are calibrated to the VSMOW/SLAP scale. Calibration intervals, transition periods, and obvious isotope outliers have been removed. The processed record spans 11 June 2024 to 15 October 2025 and is intended for studies of Southern Ocean marine boundary-layer moisture, isotope variability, air-sea exchange, and cloud and precipitation processes.

Water Vapor Isotopic Composition↗

NASA NTRS1991

Simulations of the HDO and H2O-18 atmospheric cycles using the NASA GISS general circulation model - Sensitivity experiments for present-day conditions

Incorporating the full geochemical cycles of stable water isotopes (HDO and H2O-18) into an atmospheric general circulation model (GCM) allows an improved understanding of global delta-D and delta-O-18 distributions and might even allow an analysis of the GCM's hydrological cycle. A detailed sensitivity analysis using the NASA/Goddard Institute for Space Studies (GISS) model II GCM is presented that examines the nature of isotope modeling. The tests indicate that delta-D and delta-O-18 values in nonpolar regions are not strongly sensitive to details in the model precipitation parameterizations. This result, while implying that isotope modeling has limited potential use in the calibration of GCM convection schemes, also suggests that certain necessarily arbitrary aspects of these schemes are adequate for many isotope studies. Deuterium excess, a second-order variable, does show some sensitivity to precipitation parameterization and thus may be more useful for GCM calibration.

Jouzel, Jean↗

NASA NTRS1993

A search for C60 in carbonaceous chondrites

Analysis of interior samples of the Murchison meteorite by two routes yielded an upper limit of 2 ppb for its C60 content, as compared to parts per million levels for individual polycyclic aromatic hydrocarbons (PAHs ). Provided the samples contain an interstellar component, which is probable since Murchison hydrocarbons contain excess deuterium, this result argues against the ubiquitous presence of C60 in the interstellar medium. A possible explanation for the absence of C60 was found in experiments showing how PAHs replace fullerenes as stable end products when hydrogen is present during carbon condensation. As a secondary result we found high molecular weight PAHs in the Murchison and Allende meteorites. Coronene and its methyl derivatives are especially interesting since features in the coronene spectrum have been shown to match some of the unidentified interstellar infrared emission bands.

De Vries, M. S.↗

NASA NTRS1998

Water Isotopes in Precipitation: Data/Model Comparison for Present-Day and Past Climates

Variations of HDO and H2O-18 concentrations are observed in precipitation both on a geographical and on a temporal basis. These variations, resulting from successive isotopic fractionation processes at each phase change of water during its atmospheric cycle, are well documented through the IAEA/WMO network and other sources. Isotope concentrations are, in middle and high latitudes, linearly related to the annual mean temperature at the precipitation site. Paleoclimatologists have used this relationship to infer paleotemperatures from isotope paleodata extractable from ice cores, deep groundwater and other such sources. For this application to be valid, however, the spatial relationship must also hold in time at a given location as the location undergoes a series of climatic changes. Progress in water isotope modeling aimed at examining and evaluating this assumption has been recently reviewed with a focus on polar regions and, more specifically, on Greenland. This article was largely based on the results obtained using the isotopic version of the NASA/GISS Atmospheric General Circulation Model (AGCM) fitted with isotope tracer diagnostics. We extend this review in comparing the results of two different isotopic AGCMs (NASA/GISS and ECHAM) and in examining, with a more global perspective, the validity of the above assumption, i.e. the equivalence of the spatial and temporal isotope-temperature relationship. We also examine recent progress made in modeling the relationship between the conditions prevailing in moisture source regions for precipitation and the deuterium-excess of that precipitation.

Jouzel, J.↗

NASA NTRSDate not supplied

LENR Products: Lattice Confinement Fusion (LCF), Fission, or Both?

Lattice Confinement Fusion (LCF) or Low Energy Nuclear Reactions (LENR) generate heat from the high energy products they produce. Conventionally, d-d fusion reactions may produce either 2.45 MeV neutrons, 3 MeV protons, or high energy gammas. Generally, fission will give 5-10x the excess energy of fusion. However, aneutronic “cold fusion” would provide 24 MeV/reaction, D(d,γ) 4 He, where the gamma is suppressed. In a series of pressurized gas cycling experiments with a palladium silver (75 wt.% Pd and 25 wt.% Ag or Pd25Ag) alloy [1], samples cycled with deuterium showed excess heat via unexplained temperature rises. Post-test analysis of the Pd25Ag samples using a Scanning Electron Microscope (SEM/EDX) showed several molten features containing anomalous elements other than Pd and Ag. Researchers such as Liu et al [2] have also observed transmutations under similar conditions. These molten areas and anomalous elements suggest Pd fission. This nuclear process has been referred to as nuclear disintegration. Either nuclear fission or disintegration may result in neutron rich fragments. The fragments would rapidly beta decay to shorter lived daughters until they reach stability. We’ve observed evidence of both fusion and fission products [3]. Figure 1 shows neutron spectroscopy showing fusion and boosted neutron energies in bremsstrahlung-initiated fusion of TiD2. Figure 2 shows possible fission products from D 2 gas cycled Pd25Ag alloy. Alternatively, Oppenheimer-Phillips stripping reactions, enhanced by electron screening [4] may also occur. In this case, the 8.6 MeV binding energy per Pd or Ag minus the 2.2 MeV deuteron binding energy leaves 6.4 MeV distributed between the reaction products. The energy is shared inversely proportional to the masses of the stripped off nucleon, p or n, and the new target nucleus.

Theresa L. Benyo↗

NASA NTRSDate not supplied

LENR Products: Lattice Confinement Fusion (LCF), Fission, or Both?

Lattice Confinement Fusion (LCF) or Low Energy Nuclear Reactions (LENR) generate heat from the high energy products they produce. Conventionally, d-d fusion reactions may produce either 2.45 MeV neutrons, 3 MeV protons, or high energy gammas. Generally, fission will give 5-10x the excess energy of fusion. However, aneutronic “cold fusion” would provide 24 MeV/reaction, D(d,γ) 4 He, where the gamma is suppressed. In a series of pressurized gas cycling experiments with a palladium silver (75 wt.% Pd and 25 wt.% Ag or Pd25Ag) alloy [1], samples cycled with deuterium showed excess heat via unexplained temperature rises. Post-test analysis of the Pd25Ag samples using a Scanning Electron Microscope (SEM/EDX) showed several molten features containing anomalous elements other than Pd and Ag. Researchers such as Liu et al [2] have also observed transmutations under similar conditions. These molten areas and anomalous elements suggest Pd fission. This nuclear process has been referred to as nuclear disintegration. Either nuclear fission or disintegration may result in neutron rich fragments. The fragments would rapidly beta decay to shorter lived daughters until they reach stability. We’ve observed evidence of both fusion and fission products [3]. Figure 1 shows neutron spectroscopy showing fusion and boosted neutron energies in bremsstrahlung-initiated fusion of TiD2. Figure 2 shows possible fission products from D2 gas cycled Pd25Ag alloy. Alternatively, Oppenheimer-Phillips stripping reactions, enhanced by electron screening [4] may also occur. In this case, the 8.6 MeV binding energy per Pd or Ag minus the 2.2 MeV deuteron binding energy leaves 6.4 MeV distributed between the reaction products. The energy is shared inversely proportional to the masses of the stripped off nucleon, p or n, and the new target nucleus.

Theresa L. Benyo↗

NASA NTRS2003

Interstellar Deuterium Chemistry

The presence of isotopic anomalies is the most unequivocal demonstration that meteoritic material contains circumstellar or interstellar components. In the case of organic compounds in meteorites and interplanetary dust particles (IDPs), the most useful isotopic tracer of interstellar components has been deuterium (D) excesses. In some cases these enrichments are seen in bulk meteoritic materials, but D enrichments have also been observed in meteoritic subfractions and even within specific classes of molecular species, such as amino and carboxylic acids. These anomalies are not thought to be the result of nucleosynthetic processes, but are instead ascribed to chemical and physical processes occurring in the interstellar medium (ISM). The traditional explanation of these D excesses has been to invoke the presence of materials made in the ISM by low temperature gas phase ion-molecule reactions. Indeed, the DM ratios seen in the simple interstellar gas phase molecules in cold dense clouds amenable to measurement using radio spectral techniques are generally considerably higher than the values seen in enriched Solar System materials. However, the true linkage between the DM ratios in interstellar and meteoritic materials is obscured by several effects. First, current observations of D enrichment in the ISM have been made of only a few simple molecules, molecules that are not the main carriers of D in Solar System materials. Second, some of the interstellar D enrichment is likely to reside on labile moieties that will have exchanged to some degree with more isotopically normal material during incorporation into the warm protosolar nebula, parent body processing, delivery, recovery, and analysis. Third, ion-molecule reactions represent only one of at least four processes that can produce strong D-H fractionation in the ISM.

Sandford, S. A.↗

NASA NTRS2004

Organic Globules with Anomalous Nitrogen Isotopic Compositions in the Tagish Lake Meteorite: Products of Primitive Organic Reactions

Interstellar grains in molecular clouds consist primarily of silicate minerals, organic material, and ices. These interstellar materials are heated and partially evaporated during the birth of the protosolar nebula, and the remaining core-mantle grains grow into large aggregates by collision and subsequent sticking to become planetesimals. The chemical diversity of meteoritic material such as chondrules, Ca-Al rich inclusions and amoeboid-olivine aggregates reflects the material distribution in the late stage of the disk evolution before planetesimal formation began. Organic matter in carbonaceous chondrites should also be considered as a sensitive probe for the extent and timing of high temperature processes in the solar nebula. Current models suggest that many of the organic molecules found in the hydrated carbonaceous chondrite meteorites were synthesized by aqueous processing of a suite of precursor molecules, some of which were interstellar with significant isotopic anomalies, such as excesses of deuterium (D), and 15N.

Nakamura, K.↗

NASA NTRS2002

Racemic amino acids from the ultraviolet photolysis of interstellar ice analogues

The delivery of extraterrestrial organic molecules to Earth by meteorites may have been important for the origin and early evolution of life. Indigenous amino acids have been found in meteorites-over 70 in the Murchison meteorite alone. Although it has been generally accepted that the meteoritic amino acids formed in liquid water on a parent body, the water in the Murchison meteorite is depleted in deuterium relative to the indigenous organic acids. Moreover, the meteoritical evidence for an excess of laevo-rotatory amino acids is hard to understand in the context of liquid-water reactions on meteorite parent bodies. Here we report a laboratory demonstration that glycine, alanine and serine naturally form from ultraviolet photolysis of the analogues of icy interstellar grains. Such amino acids would naturally have a deuterium excess similar to that seen in interstellar molecular clouds, and the formation process could also result in enantiomeric excesses if the incident radiation is circularly polarized. These results suggest that at least some meteoritic amino acids are the result of interstellar photochemistry, rather than formation in liquid water on an early Solar System body.

Amino Acids/chemistry↗