Triple oxygen isotopes of lunar water unveil indigenous and cometary heritage.

The origin of water in the Earth-Moon system is a pivotal question in planetary science, particularly with the need for water resources in the race to establish lunar bases. The candidate origins of lunar water are an indigenous lunar component, solar wind water production, and the delivery of meteoritic and cometary material. Characterizing the oxygen isotopic composition of water provides information on lunar oxygen sources.

A mineral-based origin of Earth's initial hydrogen peroxide and molecular oxygen.

Terrestrial reactive oxygen species (ROS) may have played a central role in the formation of oxic environments and evolution of early life. The abiotic origin of ROS on the Archean Earth has been heavily studied, and ROS are conventionally thought to have originated from HO/CO dissociation. Here, we report experiments that lead to a mineral-based source of oxygen, rather than water alone.

New constraints of terrestrial and oceanic global gross primary productions from the triple oxygen isotopic composition of atmospheric CO and O.

Representations of the changing global carbon cycle under climatic and environmental perturbations require highly detailed accounting of all atmosphere and biosphere exchange. These fluxes remain unsatisfactory, as a consequence of only having data with limited spatiotemporal coverage and precision, which restrict accurate assessments. Through the nature of intimate coupling of global carbon and oxygen cycles via O and CO and their unique triple oxygen isotope compositions in the biosphere and atmosphere, greater insight is available.

Isotopic Insights into Organic Composition Differences between Supermicron and Submicron Sea Spray Aerosol.

To elucidate the seawater biological and physicochemical factors driving differences in organic composition between supermicron and submicron sea spray aerosol (SSA and SSA), carbon isotopic composition (δC) measurements were performed on size-segregated, nascent SSA collected during a phytoplankton bloom mesocosm experiment. The δC measurements indicate that SSA contains a mixture of particulate and dissolved organic material in the bulk seawater. After phytoplankton growth, a greater amount of freshly produced carbon was observed in SSA with the proportional contribution being modulated by bacterial activity, emphasizing the importance of the microbial loop in controlling the organic composition of SSA.

Cosmogenic radiosulfur tracking of solar activity and the strong and long-lasting El Niño events.

Reconstruction of past solar activity or high-energy events of our space environment using cosmogenic radionuclides allows evaluation of their intensities, frequencies, and potential damages to humans in near space, modern satellite technologies, and ecosystems. This approach is limited by our understanding of cosmogenic radionuclide production, transformation, and transport in the atmosphere. Cosmogenic radiosulfur (S) provides additional insights due to its ideal half-life (87.

Superconductivity found in meteorites.

Meteorites can contain a wide range of material phases due to the extreme environments found in space and are ideal candidates to search for natural superconductivity. However, meteorites are chemically inhomogeneous, and superconducting phases in them could potentially be minute, rendering detection of these phases difficult. To alleviate this difficulty, we have studied meteorite samples with the ultrasensitive magnetic field modulated microwave spectroscopy (MFMMS) technique [J.

Measurements of I in the Pacific Ocean at Scripps Pier and Pacific Northwest sites: A search for effects from the 2011 Fukushima Daiichi Nuclear Power Plant accident and Hanford.

Radionuclides from the Fukushima Daiichi Nuclear Power Plant were released directly into the ocean as a result of the Great East Japan Earthquake on March 11, 2011. This material became entrained in surface ocean currents and subsequently transported for great distances. In June 2011, a few months after the disaster, we began a surface ocean I monitoring program, with samples from Scripps Pier, La Jolla, California, USA, with the expectation that surface currents originating off the east coast of Japan would eventually carry radionuclides to the La Jolla site.

Linking atmospheric pollution to cryospheric change in the Third Pole region: current progress and future prospects.

The Tibetan Plateau and its surroundings are known as the Third Pole (TP). This region is noted for its high rates of glacier melt and the associated hydrological shifts that affect water supplies in Asia. Atmospheric pollutants contribute to climatic and cryospheric changes through their effects on solar radiation and the albedos of snow and ice surfaces; moreover, the behavior and fates within the cryosphere and environmental impacts of environmental pollutants are topics of increasing concern.

Five-S-isotope evidence of two distinct mass-independent sulfur isotope effects and implications for the modern and Archean atmospheres.

The signature of mass-independent fractionation of quadruple sulfur stable isotopes (S-MIF) in Archean rocks, ice cores, and Martian meteorites provides a unique probe of the oxygen and sulfur cycles in the terrestrial and Martian paleoatmospheres. Its mechanistic origin, however, contains some uncertainties. Even for the modern atmosphere, the primary mechanism responsible for the S-MIF observed in nearly all tropospheric sulfates has not been identified.

Atmospheric sulfur isotopic anomalies recorded at Mt. Everest across the Anthropocene.

Increased anthropogenic-induced aerosol concentrations over the Himalayas and Tibetan Plateau have affected regional climate, accelerated snow/glacier melting, and influenced water supply and quality in Asia. Although sulfate is a predominant chemical component in aerosols and the hydrosphere, the contributions from different sources remain contentious. Here, we report multiple sulfur isotope composition of sedimentary sulfates from a remote freshwater alpine lake near Mount Everest to reconstruct a two-century record of the atmospheric sulfur cycle.

Accurate Quantification of Radiosulfur in Chemically Complex Atmospheric Samples.

An ultralow-level liquid scintillation counting (LSC) technique has been used in measuring radiosulfur (cosmogenic S) in natural samples. The ideal half-life of S (∼87 days) renders it a new way to examine various biogeochemical problems. A major limitation of the technique is that complex chemical compositions in atmospheric samples may lead to color quenching of LSC cocktails, a serious problem prolonging the pretreatment time (>1 week) and hampering the accurate determination of S.

Oxygen isotope anomaly in tropospheric CO and implications for CO residence time in the atmosphere and gross primary productivity.

The abundance variations of near surface atmospheric CO isotopologues (primarily OCO, OCO, OCO, and OCO) represent an integrated signal from anthropogenic/biogeochemical processes, including fossil fuel burning, biospheric photosynthesis and respiration, hydrospheric isotope exchange with water, and stratospheric photochemistry. Oxygen isotopes, in particular, are affected by the carbon and water cycles. Being a useful tracer that directly probes governing processes in CO biogeochemical cycles, ΔO (=ln(1 + δO) - 0.

Efficiency of Launching Highly Confined Polaritons by Infrared Light Incident on a Hyperbolic Material.

We investigated phonon-polaritons in hexagonal boron nitride-a naturally hyperbolic van der Waals material-by means of the scattering-type scanning near-field optical microscopy. Real-space nanoimages we have obtained detail how the polaritons are launched when the light incident on a thin hexagonal boron nitride slab is scattered by various intrinsic and extrinsic inhomogeneities, including sample edges, metallic nanodisks deposited on its top surface, random defects, and surface impurities. The scanned tip of the near-field microscope is itself a polariton launcher whose efficiency proves to be superior to all the other types of polariton launchers we studied.

Simple Method for High-Sensitivity Determination of Cosmogenic S in Snow and Water Samples Collected from Remote Regions.

Cosmogenic S is useful in understanding a wide variety of chemical and physical processes in the atmosphere, the hydrosphere, and the cryosphere. The 87.4-day half-life and the ubiquity of sulfur in natural environments renders it an ideal tracer of many phenomena.

Detection of deep stratospheric intrusions by cosmogenic 35S.

The extent to which stratospheric intrusions on synoptic scales influence the tropospheric ozone (O) levels remains poorly understood, because quantitative detection of stratospheric air has been challenging. Cosmogenic S mainly produced in the stratosphere has the potential to identify stratospheric air masses at ground level, but this approach has not yet been unambiguously shown. Here, we report unusually high S concentrations (7,390 atoms m; ∼16 times greater than annual average) in fine sulfate aerosols (aerodynamic diameter less than 0.

Graphene-Based Platform for Infrared Near-Field Nanospectroscopy of Water and Biological Materials in an Aqueous Environment.

Scattering scanning near-field optical microscopy (s-SNOM) has emerged as a powerful nanoscale spectroscopic tool capable of characterizing individual biomacromolecules and molecular materials. However, applications of scattering-based near-field techniques in the infrared (IR) to native biosystems still await a solution of how to implement the required aqueous environment. In this work, we demonstrate an IR-compatible liquid cell architecture that enables near-field imaging and nanospectroscopy by taking advantage of the unique properties of graphene.

Carbonate formation events in ALH 84001 trace the evolution of the Martian atmosphere.

Carbonate minerals provide critical information for defining atmosphere-hydrosphere interactions. Carbonate minerals in the Martian meteorite ALH 84001 have been dated to ∼ 3.9 Ga, and both C and O-triple isotopes can be used to decipher the planet's climate history.

Nanoscale infrared spectroscopy as a non-destructive probe of extraterrestrial samples.

Advances in the spatial resolution of modern analytical techniques have tremendously augmented the scientific insight gained from the analysis of natural samples. Yet, while techniques for the elemental and structural characterization of samples have achieved sub-nanometre spatial resolution, infrared spectral mapping of geochemical samples at vibrational 'fingerprint' wavelengths has remained restricted to spatial scales >10 μm. Nevertheless, infrared spectroscopy remains an invaluable contactless probe of chemical structure, details of which offer clues to the formation history of minerals.

Massive isotopic effect in vacuum UV photodissociation of N2 and implications for meteorite data.

Nitrogen isotopic distributions in the solar system extend across an enormous range, from -400‰, in the solar wind and Jovian atmosphere, to about 5,000‰ in organic matter in carbonaceous chondrites. Distributions such as these require complex processing of nitrogen reservoirs and extraordinary isotope effects. While theoretical models invoke ion-neutral exchange reactions outside the protoplanetary disk and photochemical self-shielding on the disk surface to explain the variations, there are no experiments to substantiate these models.

Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere.

Sulfur-isotopic anomalies have been used to trace the evolution of oxygen in the Precambrian atmosphere and to document past volcanic eruptions. High-precision sulfur quadruple isotope measurements of sulfate aerosols extracted from a snow pit at the South Pole (1984-2001) showed the highest S-isotopic anomalies (Δ(33)S = +1.66‰ and Δ(36)S = +2‰) in a nonvolcanic (1998-1999) period, similar in magnitude to Pinatubo and Agung, the largest volcanic eruptions of the 20th century.

Ultrafast and nanoscale plasmonic phenomena in exfoliated graphene revealed by infrared pump-probe nanoscopy.

Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ∼ 20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM).