No abstract

Cloud observations over the past decade from six Arctic atmospheric observatories are investigated to derive estimates of cloud occurrence fraction, vertical distribution, persistence in time, diurnal cycle, and boundary statistics. Each observatory has some combination of cloud lidar, radar, ceilometer, and/or interferometer for identifying and characterizing clouds. By optimally combining measurements from these instruments, it is found that annual cloud occurrence fractions are 58%-83% at the Arctic observatories. There is a clear annual cycle wherein clouds are least frequent in the winter and most frequent in the late summer and autumn. Only in Eureka, Nunavut, Canada, is the annual cycle shifted such that the annual minimum is in the spring with the maximum in the winter. Intersite monthly variability is typically within 10%-15% of the all-site average. Interannual variability at specific sites is less than 13% for any given month and, typically, is less than 3% for annual total cloud fractions. Low-level clouds are most persistent at the observatories. The median cloud persistence for all observatories is 3-5 h; however, 5% of cloud systems at far western Arctic sites are observed to occur for longer than 100 consecutive hours. Weak diurnal variability in cloudiness is observed at some sites, with a daily minimum in cloud occurrence near solar noon for those seasons for which the sun is above the horizon for at least part of the day.

An assessment of the performance of the Moderate Resolution Imaging Spectroradiometer (MODIS) cloud mask algorithm for Terra and Aqua satellites is presented. The MODIS cloud mask algorithm output is compared with lidar observations from ground [Arctic High-Spectral Resolution Lidar (AHSRL)], aircraft [Cloud Physics Lidar (CPL)], and satellite-borne [Geoscience Laser Altimeter System (GLAS)] platforms. The comparison with 3 yr of coincident observations of MODIS and combined radar and lidar cloud product from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Program Southern Great Plains (SGP) site in Lamont, Oklahoma, indicates that the MODIS algorithm agrees with the lidar about 85% of the time. A comparison with the CPL and AHSRL indicates that the optical depth limitation of the MODIS cloud mask is approximately 0.4. While MODIS algorithm flags scenes with a cloud optical depth of 0.4 as cloudy, approximately 90% of the mislabeled scenes have optical depths less than 0.4. A comparison with the GLAS cloud dataset indicates that cloud detection in polar regions at night remains challenging with the passive infrared imager approach.In anticipation of comparisons with other satellite instruments, the sensitivity of the cloud mask algorithm to instrument characteristics (e.g., instantaneous field of view and viewing geometry) and thresholds is demonstrated. As expected, cloud amount generally increases with scan angle and instantaneous field of view (IFOV). Nadir sampling represents zonal monthly mean cloud amounts but can have large differences for regional studies when compared to full-swath-width analysis.

Abstract. Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2–O2 collision complexes (O4) were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAX-DOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2–0.55 pptv IO and 32–36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and aircraft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6° N; 101.2 to 97.4° W). At 14.5 km, 5–10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12–20 degrees of freedom (DoF) and up to 500 m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 × 1013 molec cm−2 (RF12) and at least 0.5 × 1013 molec cm−2 (RF17, 0–10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 × 1012 molec cm−2 (RF12) and 2.5 × 1012 molec cm−2 (RF17) and glyoxal VCDs of 2.6 × 1014 molec cm−2 (RF12) and 2.7 × 1014 molec cm−2 (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 ± 5%, 0.1–0.2 pptv; glyoxal: 52 ± 5%, 3–20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

An equation to predict the intensity of the multiply scattered lidar return is presented. Both the scattering cross section and the scattering phase function can be specified as a function of range. This equation applies when the cloud particles are larger than the lidar wavelength. This approximation considers photon trajectories with multiple small-angle forward-scattering events and one large-angle scattering that directs the photon back toward the receiver. Comparisons with Monte Carlo simulations, exact double-scatter calculations, and lidar data demonstrate that this model provides accurate results.

A high spectral resolution lidar technique to measure optical scattering properties of atmospheric aerosols is described. Light backscattered by the atmosphere from a narrowband optically pumped oscillator-amplifier dye laser is separated into its Doppler broadened molecular and elastically scattered aerosol components by a two-channel Fabry-Perot polyetalon interferometer. Aerosol optical properties, such as the backscatter ratio, optical depth, extinction cross section, scattering cross section, and the backscatter phase function, are derived from the two-channel measurements.

Macro-and microphysical properties of single-layer stratiform mixed-phase clouds are derived from multiple years of lidar, radar, and radiosonde observations. Measurements were made as part of the MixedPhase Arctic Clouds Experiment (MPACE) and the Study of Environmental Arctic Change (SEARCH) in Barrow, Alaska, and Eureka, Nunavut, Canada, respectively. Single-layer mixed-phase clouds occurred between 4% and 26% of the total time observed, varying with season and location. They had mean cloud-base heights between ;700 and 2100 m and thicknesses between ;200 and 700 m. Seasonal mean cloud optical depths ranged from 2.2 up. The clouds existed at temperatures of ;242-271 K and occurred under different wind conditions, depending on season. Utilizing retrievals from a combination of lidar, radar, and microwave radiometer, mean cloud microphysical properties were derived, with mean liquid effective diameters estimated from 16 to 49 mm, mean liquid number densities on the order of 10 4 -10 5 L 21, and mean water contents estimated between 0.07 and 0.28 g m 23 . Ice precipitation was shown to have mean ice effective diameters of 50-125 mm, mean ice number densities on the order of 10 L 21 , and mean water contents estimated between 0.012 and 0.031 g m 23. Mean cloud liquid water paths ranged from 25 to 100 g m 22. All results are compared to previous studies, and potential retrieval errors are discussed. Additionally, seasonal variation in macro-and microphysical properties was highlighted. Finally, fraction of liquid water to ice mass was shown to decrease with decreasing temperature.

In an environment with many local, remote, persistent, and episodic sources of pollution, meteorology is the primary factor that drives periods of unhealthy air quality and reduced visibility. The 2016 Korea-UnitedStatesAirQuality(KORUS-AQ)fieldstudyprovidesauniqueopportunitytoexaminethe impactofmeteorologyontherelativeinfluenceoflocalandtransboundarypollution.MuchoftheKORUS-AQ campaign can be grouped into four distinct research periods based on observed synoptic meteorology, includingaperiodofcomplexaerosolverticalprofilesdrivenbydynamicmeteorology,stagnationundera persistent anticyclone, low-level transport and haze development, and a blocking pattern. These episodes areexaminedusingadiversearchiveofground,airborne,andsatellitedata.Whilefrontalboundaries are recognized as the primary mechanism driving pollution transport in eastern Asia, results show that they are not always related to sustained periods of hazardous air quality and reduced visibility at the surface.Significantlong-rangetransportofpollutionanddustwasconstrainedtoafewshortevents, suggesting that the majority of pollutants sampled during KORUS-AQ originated from local sources. A severeregionalpollutionepisodeisexaminedindetail,featuringdensehazeandsignificantsecondary particle formation within a shallow moist boundary layer. Observations during KORUS-AQ also highlight a rapid,40ppbvincreaseinozonepollutionasastrongseabreezefronttraversedtheSeoulMetropolitan Area. Representativeness of meteorology and pollution conditions measured by KORUS-AQ is considered by comparison with climatology. This analysis is an essential step toward improved local and regional forecasting of air quality and visibility.