Molecular Dynamics Simulation of Sympathetic Crystallization of Molecular Ions

It is shown that the translational degrees of freedom of a large variety of molecules, from light diatomic to heavy organic ones, can be cooled sympathetically and brought to rest (crystallized) in a linear Paul trap. The method relies on endowing the molecules with an appropriate positive charge, storage in a linear radiofrequency trap, and sympathetic cooling. Two well--known atomic coolant species, ${}^9{\hbox{Be}}^+$ and ${}^{137}{\hbox{Ba}}^+$, are sufficient for cooling the molecular mass range from 2 to 20,000 amu. The large molecular charge required for simultaneous trapping of heavy molecules and of the coolant ions can easily be produced using electrospray ionization. Crystallized molecular ions offer vast opportunities for novel studies.Comment: Accepted for publication in Phys. Rev.

Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer–fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5–3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42−] + [NO3−]) is only 0.5–0.7 mol mol−1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8–28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD and we attribute this in part to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available

Interspecific divergence in foliar nutrient dynamics and stem growth in a temperate forest in response to chronic nitrogen inputs

We studied the effects of excessive nitrogen (N) fertilization on foliar nutrient dynamics and stem growth in three important tree species in a mixed-deciduous forest. Stem diameter growth, foliar N concentrations, nitrogen–phosphorus (N/P) ratios, and nutrient resorption were determined for Acer rubrum L. (ACRU), Liriodendron tulipifera L. (LITU), and Prunus serotina Ehrh. (PRSE) on two 30-year-old watersheds at the Fernow Experimental Forest, West Virginia, USA: WS3, fertilized annually with 35 kg ammonium sulfate·ha-1 since 1989, and WS7, an untreated control watershed. In an earlier (1992) study, foliar N concentrations of all three species averaged 11% higher in WS3 than in WS7. By 2000, that was no longer the case for any species; indeed N in ACRU leaves was 13% lower in WS3 that year. N/P ratios were elevated in WS3 only in PRSE in 1992 and in both ACRU and PRSE in 1997, but by 2001, mean N/P for all three species was lower in WS3. N resorption efficiencies were 30% lower in WS3 in ACRU and PRSE, but not in LITU. Stem diameter growth in WS3 was 55% lower in ACRU and 30% lower in LITU and PRSE compared with that in WS7. Results may indicate declining growth vigor in ACRU and, to a lesser extent, PRSE and LITU in the fertilized watershed. Observed interspecific differences in growth and plant nutrition responses suggest eventual changes in species composition under increasing N saturation