Tropical Free Troposphere Research Articles

Vapor-Buoyancy Feedback in an Idealized GCM

Abstract Humid air is lighter than dry air at a given temperature and pressure, as the molecular weight of water vapor is less than that of dry air. This effect is known as vapor buoyancy (VB). Although this effect is a well-understood consequence of the ideal gas law, its influence on climate has been under-studied. This study investigates VB’s influence on atmospheric temperature, radiation, and clouds. In mechanism-denial experiments, we remove VB from the dynamics and parameterizations of an idealized general circulation model (GCM). These experiments show that VB warms the tropical free troposphere by approximately 1 K in an Earth-like climate, and the magnitude of this effect increases with warming. This additional atmospheric warming causes greater outgoing longwave radiation (OLR) to be emitted as the climate warms. This constitutes a negative climate feedback which attains a magnitude of 0.1 to 0.2 W/m2/K in the tropics. The simulations further show that, despite warming the atmosphere, VB does not introduce a countervailing positive water vapor feedback. Finally, we find that VB makes the net cloud feedback in the model more negative than it otherwise would be, reinforcing the clear-sky feedback.

Assessing the Tropospheric Temperature and Humidity Simulations in CMIP3/5/6 Models Using the AIRS Obs4MIPs V2.1 Data

AbstractIn this study, the Atmospheric Infrared Sounder (AIRS) Observations for Model Intercomparison Projects (Obs4MIPs) V2.1 tropospheric air temperature, specific humidity, and relative humidity data are utilized to evaluate the global tropospheric temperature and humidity simulations in the fully coupled global climate models from the Coupled Model Intercomparison Project phases 3, 5, and 6 (CMIP3, CMIP5, and CMIP6), and possible simulation improvement in CMIP6 models in comparison to CMIP3 and CMIP5 models. Our analyses indicate that all three phases of CMIP models share similar tropospheric air temperature, specific humidity, and relative humidity biases in their multi‐model ensemble means relative to AIRS. Cold biases up to 4 K and positive relative humidity biases up to 20% are found in the free troposphere almost globally with maxima over the mid‐latitude storm tracks. Warm biases up to 2 K are seen over the Southern Ocean in the lower troposphere. Positive specific and relative humidity biases exist over the off‐equatorial oceans while negative specific and relative humidity biases are seen near the equator in the tropical free troposphere, which are related to the double‐intertropical convergence zone bias in the models. Both the air temperature and specific humidity biases are important to the relative humidity biases except in the tropical free troposphere where the specific humidity biases dominate. The tropospheric air temperature, specific humidity, and relative humidity biases are reduced from CMIP3 to CMIP5 and to CMIP6 at almost all pressure levels except at 300 hPa for specific humidity and in the boundary layer for relative humidity.

New particle formation in the tropical free troposphere during CAMP2Ex: statistics and impact of emission sources, convective activity, and synoptic conditions

Abstract. Nucleation in the free troposphere (FT) and subsequent growth of new particles represent a globally important source of cloud condensation nuclei (CCN). Whereas new particle formation (NPF) has been shown to occur frequently in the upper troposphere over tropical oceans, there have been few studies of NPF at lower altitudes. In addition, the impact of urban emissions and biomass burning on the NPF in tropical marine FT remains poorly understood. In this study, we examine NPF in the lower and mid-troposphere (3–8.5 km) over the tropical ocean and coastal region using airborne measurements during the recent Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex). NPF was mostly observed above 5.5 km and coincided with elevated relative humidity (RH) and reduced condensation sink (CS), suggesting that NPF occurs in convective cloud outflow. The frequency of NPF increases with altitude, reaching ∼ 50 % above 8 km. An abrupt decrease in NPF frequency coincides with early monsoon transition and is attributed to increased CS resulting from reduced convective activity and more frequent transport of aged urban plumes. Surprisingly, a large fraction of NPF events in background air were observed in the early morning, and the NPF is likely made possible by very low CS despite low actinic flux. Convectively detrained biomass-burning plumes and fresh urban emissions enhance NPF as a result of elevated precursor concentrations and scavenging of pre-existing particles. In contrast, NPF is suppressed in aged urban plumes where the reactive precursors are mostly consumed, while CS remains relatively high. This study shows a strong impact of urban and biomass-burning emissions on the NPF in tropical marine FT. The results also illustrate the competing influences of different variables and interactions among anthropogenic emissions, convective clouds, and meteorology, which lead to NPF under a variety of conditions in tropical marine environments.

Tropical tropospheric warming pattern explained by shifts in convective heating in the Matsuno–Gill model

AbstractHorizontal temperature gradients in the tropical free troposphere are fairly weak, and tropical tropospheric warming is usually treated as uniform. However, we show here that projected tropospheric warming is spatially inhomogeneous in Coupled Model Intercomparison Project Phase 6 models, as well as in a storm‐resolving climate model. We relate the upper tropospheric warming pattern to sea‐surface temperature changes that reorganise convection and thereby cause spatial shifts in convective heating. Using the classical Gill model for tropical circulation and forcing it with precipitation changes that arise due to greenhouse gas warming, we can understand and reproduce the different warming patterns simulated by a range of global climate models. Forcing the Gill model with precipitation changes from a certain region demonstrates how local tropospheric temperature changes depend on local changes in convective heating. Close to the Equator, anomalous geopotential gradients are balanced by the dissipation term in the Gill model. The optimal dissipation time‐scale to reproduce the warming pattern varies depending on the Coupled Model Intercomparison Project Phase 6 model, and is between 1 and 10 days. We demonstrate that horizontal advection and eddy momentum fluxes have large enough equivalent dissipation time‐scales to balance the gradients in geopotential and thereby shape the warming pattern. Though climate models show a large spread in projections of tropical sea‐surface temperature and precipitation changes, our results imply that, once these predictions improve, our confidence in the predicted upper tropospheric warming pattern should also increase.

Sources of Uncertainty in Mid‐Tropospheric Tropical Humidity in Global Storm‐Resolving Simulations

AbstractWe conduct a series of eight 45‐day experiments with a global storm‐resolving model (GSRM) to test the sensitivity of relative humidity in the tropics to changes in model resolution and parameterizations. These changes include changes in horizontal and vertical grid spacing as well as in the parameterizations of microphysics and turbulence, and are chosen to capture currently existing differences among GSRMs. To link the distribution in the tropical free troposphere with processes in the deep convective regions, we adopt a trajectory‐based assessment of the last‐saturation paradigm. The perturbations we apply to the model result in tropical mean changes ranging from 0.5% to 8% (absolute) in the mid troposphere. The generated spread is similar to that in a multi‐model ensemble of GSRMs and smaller than the spread across conventional general circulation models, supporting that an explicit representation of deep convection reduces the uncertainty in tropical . The largest changes result from changes in parameterizations, suggesting that model physics represent a major source of humidity spread across GSRMs. The in the moist tropical regions is particularly sensitive to vertical mixing processes within the tropics, which impact through their effect on the last‐saturation temperature rather than their effect on the evolution of the humidity since last‐saturation. In our analysis the of the dry tropical regions strongly depends on the exchange with the extratropics. The interaction between tropics and extratropics could change with warming and presage changes in the radiatively sensitive dry regions.

Oxidized organic molecules in the tropical free troposphere over Amazonia.

New particle formation (NPF) in the tropical free troposphere (FT) is a globally important source of cloud condensation nuclei, affecting cloud properties and climate. Oxidized organic molecules (OOMs) produced from biogenic volatile organic compounds are believed to contribute to aerosol formation in the tropical FT, but without direct chemical observations. We performed in situ molecular-level OOMs measurements at the Bolivian station Chacaltaya at 5240 m above sea level, on the western edge of Amazonia. For the first time, we demonstrate the presence of OOMs, mainly with 4-5 carbon atoms, in both gas-phase and particle-phase (in terms of mass contribution) measurements in tropical FT air from Amazonia. These observations, combined with air mass history analyses, indicate that the observed OOMs are linked to isoprene emitted from the rainforests hundreds of kilometers away. Based on particle-phase measurements, we find that these compounds can contribute to NPF, at least the growth of newly formed nanoparticles, in the tropical FT on a continental scale. Thus, our study is a fundamental and significant step in understanding the aerosol formation process in the tropical FT.

Description and Evaluation of a New Deep Convective Cloud Model Considering In‐Cloud Inhomogeneity

AbstractConvections still need to be parameterized in general circulation models (GCMs) in the coming decades. Performances of GCMs are significantly influenced by the convection schemes used. In contrast to most conventional cloud models that ignore in‐cloud inhomogeneities, a new convective cloud model explicitly considering in‐cloud inhomogeneities is developed. The new model adopts a single bulk plume approach, but divides the plume into a series of interacting sub‐plumes in order to mimic the transition from the plume core to its edges. We implemented the new cloud model in NCAR Community Atmosphere Model version 5.0 (CAM5) and evaluated its performance. Single‐column tests show a stronger mass flux profile and low‐level detrainment with the new model. In global simulations, the long‐lasting wet bias in the tropical free troposphere of CAM5 is alleviated. Spatial pattern and intensity distribution of precipitation is improved, but the global hydrological cycle is over‐enhanced. The diurnal cycle of tropical precipitation is also better captured though the precipitation peak still occurs earlier than the observations and the amplitude of the cycle tends to weaken. MJO simulation is slightly improved with the new scheme. In addition, the new cloud model generated more tropical cyclones, in better agreement with observations.

Zonal Temperature Gradients in the Tropical Free Troposphere

Abstract The horizontal temperature gradients in the tropical free troposphere are generally assumed to be weak. We show with ERA5 data that substantial zonal virtual temperature (Tυ) gradients persist climatologically in the tropical free troposphere and investigate their causes. The gradients change seasonally: Tυ at 500 hPa over the equatorial western Pacific Ocean (EWP) is usually much warmer (up to 3 K) than that over the equatorial central Pacific Ocean (ECP) during December–February (DJF), while the temperature differences between EWP and ECP are much smaller during June–August (JJA). During DJF, Tυ gradients over the Pacific prevail throughout the entire free troposphere, especially in the upper troposphere near 300 hPa. We find that the associated hydrostatic pressure gradients are mainly balanced by the nonlinear terms in the momentum equation, in particular via zonal wind advection. Strong zonal winds occur near the equator in boreal winter, transporting zonal momentum so as to balance the pressure gradient force. The zonal winds are due to large-scale equatorial waves, excited by a heating pattern that is relatively symmetric about the equator. In boreal summer, the large-scale equatorial waves are less active in the Pacific region due to a more asymmetric temperature pattern, so the zonal momentum advection and Tυ gradients are both much weaker. The results point to an important role of the nonlinear terms in the tropical balanced dynamics, stressing the need for an improved theoretical understanding and modeling framework of the tropical atmosphere that includes these nonlinear terms, or their net effect.

Brown carbon from biomass burning imposes strong circum-Arctic warming

Brown carbon from biomass burning imposes strong circum-Arctic warming

Wildfire atmospheric chemistry: climate and air quality impacts

Wildfire atmospheric chemistry: climate and air quality impacts

Modeling the global radiative effect of brown carbon: a potentially larger heating source in the tropical free troposphere than black carbon

Abstract. Carbonaceous aerosols significantly affect global radiative forcing and climate through absorption and the scattering of sunlight. Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosols. The direct radiative effect (DRE) of BrC is uncertain. A recent study suggests that BrC absorption is comparable to BC in the upper troposphere over biomass burning regions and that the resulting radiative heating tends to stabilize the atmosphere. Yet current climate models do not include proper physical and chemical treatments of BrC. In this study, we derived a BrC global biomass burning emission inventory on the basis of the Global Fire Emissions Database version 4 (GFED4), developed a module to simulate the light absorption of BrC in the Community Atmosphere Model version 5 (CAM5) of the Community Earth System Model (CESM), and investigated the photobleaching effect and convective transport of BrC on the basis of Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convective Clouds and Chemistry Project (DC3) measurements. The model simulations of BC were also evaluated using HIAPER (High-Performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO) measurements. We found that globally BrC is a significant absorber, the DRE of which is 0.10 W m−2, more than 25 % of BC DRE (+0.39 W m−2). Most significantly, model results indicated that BrC atmospheric heating in the tropical mid and upper troposphere is larger than that of BC. The source of tropical BrC is mainly from wildfires, which are more prevalent in the tropical regions than higher latitudes and release much more BrC relative to BC than industrial sources. While BC atmospheric heating is skewed towards the northern mid-latitude lower atmosphere, BrC heating is more centered in the tropical free troposphere. A possible mechanism for the enhanced convective transport of BrC is that hydrophobic high molecular weight BrC becomes a larger fraction of the BrC and less easily activated in a cloud as the aerosol ages. The contribution of BrC heating to the Hadley circulation and latitudinal expansion of the tropics is likely comparable to BC heating.

Weakened Anomalous Western North Pacific Anticyclone during an El Niño–Decaying Summer under a Warmer Climate: Dominant Role of the Weakened Impact of the Tropical Indian Ocean on the Atmosphere

Abstract The western North Pacific subtropical anticyclone (WNPAC) is the most prominent atmospheric circulation anomaly over the subtropical Northern Hemisphere during the decaying summer of an El Niño event. Based on a comparison between the RCP8.5 and the historical experiments of 30 coupled models from the CMIP5, we show evidence that the anomalous WNPAC during the El Niño–decaying summer is weaker in a warmer climate although the amplitude of the El Niño remains generally unchanged. The weakened impact of the sea surface temperature anomaly (SSTA) over the tropical Indian Ocean (TIO) on the atmosphere is essential for the weakened anomalous WNPAC. In a warmer climate, the warm tropospheric temperature (TT) anomaly in the tropical free troposphere stimulated by the El Niño–related SSTA is enhanced through stronger moist adiabatic adjustment in a warmer mean state, even if the SSTA of El Niño is unchanged. But the amplitude of the warm SSTA over TIO remains generally unchanged in an El Niño–decaying summer, the static stability of the boundary layer over TIO is increased, and the positive rainfall anomaly over TIO is weakened. As a result, the warm Kelvin wave emanating from TIO is weakened because of a weaker latent heating anomaly over TIO, which is responsible for the weakened WNPAC anomaly. Numerical experiments support the weakened sensitivity of precipitation anomaly over TIO to local SSTA under an increase of mean-state SST and its essential role in the weakened anomalous WNPAC, independent of any change in the SSTA.

Transient aspects of the Hadley circulation forced by an idealized off‐equatorial ITCZ

AbstractThis paper presents analytical solutions of large‐scale, zonally symmetric overturning circulations in the tropical free troposphere forced by transient diabatic heating in the off‐equatorial intertropical convergence zone (ITCZ). The dynamics are discussed in the context of the time‐dependent meridional circulation equation arising in an equatorial β‐plane model. The solutions of these differential equations contain terms for the slow, quasi‐balanced part of the response and terms for the transient, zonally symmetric, inertia‐gravity wave part of the response. When the off‐equatorial (north of the equator) ITCZ diabatic heating is switched on at various rates, both parts of the response reveal a basic asymmetry between the southern and northern hemispheres, with the southern hemisphere side containing most of the quasi‐balanced compensating subsidence and transient inertia‐gravity wave activity. The inertia‐gravity waves travel in wave packets that bounce off a spectrum of turning latitudes and are analyzed in the context of an average conservation law approach. These traveling wave packets cause the mass flux in the southern and northern Hadley cells to pulsate on timescales of about 1, 2, and 3 days for diabatic heating of the external, first internal, and second internal vertical modes, respectively. The spectral characteristics of the vertical motion in the ITCZ and subsidence regions are slightly more complicated and depend on ITCZ location.

Airborne measurements of BrO and the sum of HOBr and Br2 over the Tropical West Pacific from 1 to 15 km during the CONvective TRansport of Active Species in the Tropics (CONTRAST) experiment

AbstractA chemical ionization mass spectrometer was used to measure BrO and HOBr + Br2 over the Tropical West Pacific Ocean within the altitude range of 1 to 15 km, during the CONvective TRansport of Active Species in the Tropics (CONTRAST) campaign in 2014. Isolated episodes of elevated BrO (up to 6.6 pptv) and/or HOBr + Br2 (up to 7.3 pptv) were observed in the tropical free troposphere (TFT) and were associated with biomass burning. However, most of the time we did not observe significant BrO or HOBr + Br2 in the TFT and the tropical tropopause layer (TTL) above our limits of detection (LOD). The 1 min average LOD for BrO ranged from 0.6 to 1.6 pptv and for HOBr + Br2 ranged from 1.3 to 3.5 pptv. During one flight, BrO observations from the TTL to the extratropical lowermost stratosphere were used to infer a profile of inorganic bromine (Bry). Based on this profile, we estimated the product gas injection of bromine species into the stratosphere to be 2 pptv. Analysis of Bry partitioning further indicates that BrO levels are likely very low in the TFT environment and that future studies should target the measurement of HBr or atomic Br.

Active and widespread halogen chemistry in the tropical and subtropical free troposphere

Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10 °N to 40 °S), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (∼ 3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.

Aircraft measurements of BrO, IO, glyoxal, NO<sub>2</sub>, H<sub>2</sub>O, O<sub>2</sub>–O<sub>2</sub> and aerosol extinction profiles in the tropics: comparison with aircraft-/ship-based in situ and lidar measurements

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.

Influence of corona discharge on the ozone budget in the tropical free troposphere: a case study of deep convection during GABRIEL

Abstract. Convective redistribution of ozone and its precursors between the boundary layer (BL) and the free troposphere (FT) influences photochemistry, in particular in the middle and upper troposphere (UT). We present a case study of convective transport during the GABRIEL campaign over the tropical rain forest in Suriname in October 2005. During one measurement flight the inflow and outflow regions of a cumulonimbus cloud (Cb) have been characterized. We identified a distinct layer between 9 and 11 km altitude with enhanced mixing ratios of CO, O3, HOx, acetone and acetonitrile. The elevated O3 contradicts the expectation that convective transport brings low-ozone air from the boundary layer to the outflow region. Entrainment of ozone-rich air is estimated to account for 62% (range: 33–91%) of the observed O3. Ozone is enhanced by only 5–6% by photochemical production in the outflow due to enhanced NO from lightning, based on model calculations using observations including the first reported HOx measurements over the tropical rainforest. The "excess" ozone in the outflow is most probably due to direct production by corona discharge associated with lightning. We deduce a production rate of 5.12 × 1028 molecules O3 flash−1 (range: 9.89 × 1026–9.82 × 1028 molecules O3 flash−1), which is at the upper limit of the range reported previously.

Detection of iodine monoxide in the tropical free troposphere

Atmospheric iodine monoxide (IO) is a radical that catalytically destroys heat trapping ozone and reacts further to form aerosols. Here, we report the detection of IO in the tropical free troposphere (FT). We present vertical profiles from airborne measurements over the Pacific Ocean that show significant IO up to 9.5 km altitude and locate, on average, two-thirds of the total column above the marine boundary layer. IO was observed in both recent deep convective outflow and aged free tropospheric air, suggesting a widespread abundance in the FT over tropical oceans. Our vertical profile measurements imply that most of the IO signal detected by satellites over tropical oceans could originate in the FT, which has implications for our understanding of iodine sources. Surprisingly, the IO concentration remains elevated in a transition layer that is decoupled from the ocean surface. This elevated concentration aloft is difficult to reconcile with our current understanding of iodine lifetimes and may indicate heterogeneous recycling of iodine from aerosols back to the gas phase. Chemical model simulations reveal that the iodine-induced ozone loss occurs mostly above the marine boundary layer (34%), in the transition layer (40%) and FT (26%) and accounts for up to 20% of the overall tropospheric ozone loss rate in the upper FT. Our results suggest that the halogen-driven ozone loss in the FT is currently underestimated. More research is needed to quantify the widespread impact that iodine species of marine origin have on free tropospheric composition, chemistry, and climate.

Evaluating CMIP5 models using AIRS tropospheric air temperature and specific humidity climatology

This paper documents the climatological mean features of the Atmospheric Infrared Sounder (AIRS) monthly mean tropospheric air temperature (ta, K) and specific humidity (hus, kg/kg) products as part of the Obs4MIPs project and compares them to those from NASA's Modern Era Retrospective analysis for Research and Applications (MERRA) for validation and 16 models from the fifth phase of the Coupled Model Intercomparison Project (CMIP5) for CMIP5 model evaluation. MERRA is warmer than AIRS in the free troposphere but colder in the boundary layer with differences typically less than 1 K. MERRA is also drier (~10%) than AIRS in the tropical boundary layer but wetter (~30%) in the tropical free troposphere and the extratropical troposphere. In particular, the large MERRA‐AIRS specific humidity differences are mainly located in the deep convective cloudy regions indicating that the low sampling of AIRS in the cloudy regions may be the main reason for these differences. In comparison to AIRS and MERRA, the sixteen CMIP5 models can generally reproduce the climatological features of tropospheric air temperature and specific humidity well, but several noticeable biases exist. The models have a tropospheric cold bias (around 2 K), especially in the extratropical upper troposphere, and a double‐ITCZ problem in the troposphere from 1000 hPa to 300 hPa, especially in the tropical Pacific. The upper‐tropospheric cold bias exists in the most (13 of 16) models, and the double‐ITCZ bias is found in all 16 CMIP5 models. Both biases are independent of the reference dataset used (AIRS or MERRA).

The lofting of Western Pacific regional aerosol by island thermodynamics as observed around Borneo

Abstract. Vertical profiles of aerosol chemical composition, number concentration and size were measured throughout the lower troposphere of Borneo, a large tropical island in the western Pacific Ocean. Aerosol composition, size and number concentration measurements (using an Aerodyne Aerosol Mass Spectrometer, Passive Cavity Aerosol Spectrometer Probe and Condensation Particle Counter, respectively) were made both upwind and downwind of Borneo, as well as over the island itself, on board the UK BAe-146 research aircraft as part of the OP3 project. Two meteorological regimes were identified – one dominated by isolated terrestrial convection (ITC) which peaked in the afternoon, and the other characterised by more regionally active mesoscale convective systems (MCS). Upwind profiles show aerosol to be confined to a shallow marine boundary layer below 930 ± 10 hPa (~760 m above sea level, a.s.l.). As this air mass advects over the island with the mean free troposphere synoptic flow during the ITC-dominated regime, it is convectively lofted above the terrestrial surface mixed layer to heights of between 945 ± 22 (~630 m a.s.l.) and 740 ± 44 hPa (~2740 m a.s.l.), consistent with a coupling between the synoptic steering level flow and island sea breeze circulations. Terrestrial aerosol was observed to be lofted into this higher layer through both moist convective uplift and transport through turbulent diurnal sea-breeze cells. At the peak of convective activity in the mid-afternoons, organic aerosol loadings in the lofted layer were observed to be substantially higher than in the morning (by a mean factor of three). This organic matter is dominated by secondary aerosol from processing of biogenic gas phase precursors. Aerosol number concentration profiles suggest formation of new particles aloft in the atmosphere. By the time the air mass reaches the west coast of the island, terrestrial aerosol is enhanced in the lofted layer. Such uplift of aerosol in Borneo is expected to increase aerosol lifetimes in the lower free troposphere downwind, as they are above the boundary layer and therefore less likely to be lost by wet or dry deposition. It is also likely to change the role they play in the semi-direct and direct aerosol effects. The long chain of islands extending from Malaysia to Australia may all similarly be expected to present an orographic barrier to low level mean flow. This would lead to significant transport of aerosol into the tropical free troposphere across the Western Pacific region.