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Abstract. Tropospheric helium variations are tightly linked to CO2 due to the co-emission of He and CO2 from natural-gasburning. Recently, Birner et al. (2022a) showed that the global consumption of natural gas has measurably increased the He content of theatmosphere. Like CO2, He is also predicted to exhibit complex spatial and temporal variability on shorter timescales, butmeasurements of these short-term variations are lacking. Here, we present the development of an improved gas delivery and purification system for thesemi-continuous mass spectrometric measurement of the atmospheric He-to-nitrogen ratio (He/N2). The method replaces the chemicalgetter used previously by Birner et al. (2021, 2022a) to preconcentrate He in an air stream with a cryogenic trap which can be more simplyregenerated by heating and which improves the precision of the measurement to 22 per meg (i.e., 0.022 ‰) in10 min (1σ). Using this “cryo-enrichment” method, we measured the He/N2 ratios in ambient air at La Jolla (California,USA) over 5 weeks in 2022. During this period, He/N2 was strongly correlated with atmospheric CO2 concentrations, as expectedfrom anthropogenic emissions, with a diurnal cycle of 450–500 per meg (max–min) caused by the sea–land breeze pattern of local winds,which modulates the influence of local pollution sources. 

Abstract The interannual to decadal variability in natural carbon sinks limits the explanation of recent changes in atmospheric CO₂concentration. Here we account for interannual and decadal variability using a simple quasi-mechanistic model of the net land carbon exchange with terms scaling with atmospheric CO₂and a weighted spatial average of temperature anomalies. This approach reduces the unexplained residual in Earth’s carbon cycle budget from ±0.76 GtC per year obtained using process models to ±0.50 GtC per year, with the largest improvements on decadal timescales despite assuming constant dynamics. Our findings reveal remarkable stability of the carbon cycle and allow verification of reported global emissions to within 4.4% (95% confidence level) over the five-year stocktake cycle of the Paris Agreement—half the uncertainty reported previously. 

Abstract. The atmospheric He/N2 ratio is expected to increase due to the emission of He associated with fossil fuels and isexpected to also vary in both space and time due to gravitational separationin the stratosphere. These signals may be useful indicators of fossil fuelexploitation and variability in stratospheric circulation, but directmeasurements of He/N2 ratio are lacking on all timescales. Here wepresent a high-precision custom inlet system for mass spectrometers thatcontinuously stabilizes the flow of gas during sample–standard comparisonand removes all non-noble gases from the gas stream. This enablesunprecedented accuracy in measurement of relative changes in the helium molefraction, which can be directly related to the 4He/N2 ratio usingsupplementary measurements of O2/N2, Ar/N2 and CO2.Repeat measurements of the same combination of high-pressure tanks using ourinlet system achieves a He/N2 reproducibility of∼ 10 per meg (i.e., 0.001 %) in 6–8 h analyses. This compares to interannual changesof gravitational enrichment at ∼ 35 km in the midlatitudestratosphere of order 300–400 per meg and an annual tropospheric increasefrom human fossil fuel activity of less than ∼ 30 per meg yr−1 (bounded by previous work on helium isotopes). The gettering andflow-stabilizing inlet may also be used for the analysis of other noble-gasisotopes and could resolve previously unobserved seasonal cycles inKr/N2 and Xe/N2. 

Abstract. Here we present a newly developed ice core gas-phase proxy that directlysamples a component of the large-scale atmospheric circulation:synoptic-scale pressure variability. Surface pressure changes weakly disrupt gravitational isotopic settling in the firn layer, which is recorded in krypton-86 excess (86Krxs). The 86Krxs may therefore reflect the time-averaged synoptic pressure variability over several years (site “storminess”), but it likely cannot record individual synoptic events as ice core gas samples typically average over several years. We validate 86Krxs using late Holocene ice samples from 11 Antarctic ice cores and 1 Greenland ice core that collectively represent a wide range of surface pressure variability in the modern climate. We find a strong spatial correlation (r=-0.94, p<0.01) between site average 86Krxs and time-averaged synoptic variability from reanalysis data. The main uncertainties in the analysis are the corrections for gas loss and thermal fractionation and the relatively large scatter in the data. Limited scientific understanding of the firn physics and potential biases of 86Krxs require caution in interpreting this proxy at present. We show that Antarctic 86Krxs appears to be linked to the position of the Southern Hemisphere eddy-driven subpolar jet (SPJ), with a southern position enhancing pressure variability. We present a 86Krxs record covering the last 24 kyr from the West Antarctic Ice Sheet (WAIS) Divide ice core. Based on the empirical spatial correlation of synoptic activity and 86Krxs at various Antarctic sites, we interpret this record to show that West Antarctic synoptic activity is slightly below modern levels during the Last Glacial Maximum (LGM), increases during the Heinrich Stadial 1 and Younger Dryas North Atlantic cold periods, weakens abruptly at the Holocene onset, remains low during the early and mid-Holocene, and gradually increases to its modern value. The WAIS Divide 86Krxs record resembles records of monsoon intensity thought to reflect changes in the meridional position of the Intertropical Convergence Zone (ITCZ) on orbital and millennial timescales such that West Antarctic storminess is weaker when the ITCZ is displaced northward and stronger when it is displaced southward. We interpret variations in synoptic activity as reflecting movement of the South Pacific SPJ in parallel to the ITCZ migrations, which is the expected zonal mean response of the eddy-driven jet in models and proxy data. Past changes to Pacific climate and the El Niño–Southern Oscillation (ENSO) may amplify the signal of the SPJ migration. Our interpretation is broadly consistent with opal flux records from the Pacific Antarctic zone thought to reflect wind-driven upwelling. We emphasize that 86Krxs is a new proxy, and more work is called for to confirm, replicate, and better understand these results; until such time, our conclusions regarding past atmospheric dynamics remainspeculative. Current scientific understanding of firn air transport andtrapping is insufficient to explain all the observed variations in86Krxs. A list of suggested future studies is provided.