David W. Tarasick

Trends of ozone in the troposphere

Using a set of selected surface ozone (nine stations) and ozone vertical profile measurements (from six stations), we have documented changes in tropospheric ozone at a number of locations. From two stations at high northern hemisphere (NH) latitudes there has been a significant decline in ozone amounts throughout the troposphere since the early 1980s. At midlatitudes of the NH where data are the most abundant, on the other hand, important regional differences prevail. The two stations in the eastern United States show that changes in ozone concentrations since the early 1970s have been relatively small. At the two sites in Europe, however, ozone amounts increased rapidly into the mid-1980s, but have increased less rapidly (or in some places not at all) since then. Increases at the Japanese ozonesonde station have been largest in the lower troposphere, but have slowed in the recent decade. The tropics are sparsely sampled but do not show significant changes. Small increases are suggested at southern hemisphere (SH) midlatitudes by the two surface data records. In Antarctica large declines in the ozone concentration are noted in the South Pole data, and like those at high latitudes of the NH, seem to parallel the large decreases in the stratosphere.

Validation of Aura Microwave Limb Sounder Ozone by ozonesonde and lidar measurements

We present validation studies of MLS version 2.2 upper tropospheric and stratospheric ozone profiles using ozonesonde and lidar data as well as climatological data. Ozone measurements from over 60 ozonesonde stations worldwide and three lidar stations are compared with coincident MLS data. The MLS ozone stratospheric data between 150 and 3 hPa agree well with ozonesonde measurements, within 8% for the global average. MLS values at 215 hPa are biased high compared to ozonesondes by A`20% at middle to high latitude, although there is a lot of variability in this altitude region. Comparisons between MLS and ground-based lidar measurements from Mauna Loa, Hawaii, from the Table Mountain Facility, California, and from the Observatoire de Haute-Provence, France, give very good agreement, within A`5%, for the stratospheric values. The comparisons between MLS and the Table Mountain Facility tropospheric ozone lidar show that MLS data are biased high by A`30% at 215 hPa, consistent with that indicated by the ozonesonde data. We obtain better global average agreement between MLS and ozonesonde partial column values down to 215 hPa, although the average MLS values at low to middle latitudes are higher than the ozonesonde values by up to a few percent. MLS v2.2 ozone data agree better than the MLS v1.5 data with ozonesonde and lidar measurements. MLS tropical data show the wave one longitudinal pattern in the upper troposphere, with similarities to the average distribution from ozonesondes. High upper tropospheric ozone values are also observed by MLS in the tropical Pacific from June to November.

Ozone in the Arctic lower troposphere during winter and spring 2000 (ALERT2000)

Abstract A summary of the temporal and vertical characteristics of ozone in the Arctic boundary layer as observed during winter and spring 2000 near Alert, Nunavut, Canada (82°N, 62°W) is presented. The measurements were made during the Polar Sunrise Experiments ALERT2000. Particular attention is given to identifying chemical and atmospheric characteristics of short-lived (

A trajectory-based estimate of the tropospheric ozone column using the residual method

We estimate the tropospheric column ozone using a forward trajectory model to increase the horizontal resolution of the Aura Microwave Limb Sounder (MLS) derived stratospheric column ozone. Subtracting the MLS stratospheric column from Ozone Monitoring Instrument total column measurements gives the trajectory enhanced tropospheric ozone residual (TTOR). Because of different tropopause definitions, we validate the basic residual technique by computing the 200-hPa-to-surface column and comparing it to the same product from ozonesondes and Tropospheric Emission Spectrometer measurements. Comparisons show good agreement in the tropics and reasonable agreement at middle latitudes, but there is a persistent low bias in the TTOR that may be due to a slight high bias in MLS stratospheric column. With the improved stratospheric column resolution, we note a strong correlation of extratropical tropospheric ozone column anomalies with probable troposphere-stratosphere exchange events or folds. The folds can be identified by their colocation with strong horizontal tropopause gradients. TTOR anomalies due to folds may be mistaken for pollution events since folds often occur in the Atlantic and Pacific pollution corridors. We also compare the 200-hPa-to-surface column with Global Modeling Initiative chemical model estimates of the same quantity. While the tropical comparisons are good, we note that chemical model variations in 200-hPa-to-surface column at middle latitudes are much smaller than seen in the TTOR.

Intercontinental Chemical Transport Experiment Ozonesonde Network Study (IONS) 2004: 1. Summertime upper troposphere/lower stratosphere ozone over northeastern North America

Coordinated ozonesonde launches from the Intercontinental Transport Experiment (INTEX) Ozonesonde Network Study (IONS) (http://croc.gsfc.nasa.gov/intex/ions.html) in July-August 2004 provided nearly 300 O3 profiles from eleven North American sites and the R/V Ronald H. Brown in the Gulf of Maine. With the IONS period dominated by low-pressure conditions over northeastern North America (NENA), the free troposphere in that region was frequently enriched by stratospheric O3. Stratospheric O3 contributions to the NENA tropospheric O3 budget are computed through analyses of O3 laminae (Pierce and Grant, 1998; Teitelbaum et al., 1996), tracers (potential vorticity, water vapor), and trajectories. The lasting influence of stratospheric incursions into the troposphere is demonstrated, and the computed stratospheric contribution to tropospheric column O3 over the R/V Ronald H. Brown and six sites in Michigan, Virginia, Maryland, Rhode Island, and Nova Scotia, 23% ± 3%, is similar to summertime budgets derived from European O3 profiles (Collette and Ancellet, 2005). Analysis of potential vorticity, Wallops ozonesondes (37.9°N, 75.5°W), and Measurements of Ozone by Airbus In-service Aircraft (MOZAIC) O3 profiles for NENA airports in June-July-August 1996–2004 shows that the stratospheric fraction in 2004 may be typical. Boundary layer O3 at Wallops and northeast U.S. sites during IONS also resembled O3 climatology (June-July-August 1996–2003). However, statistical classification of Wallops O3 profiles shows the frequency of profiles with background, nonpolluted boundary layer O3 was greater than normal during IONS.

Data assimilation with the Canadian Middle Atmosphere Model

Abstract A data assimilation scheme has been coupled to the Canadian Middle Atmosphere Model, providing, for the first time, the capability of assimilating data from the ground to the top of the mesosphere (about 95 km). This model is a full general circulation model with on‐line fully interactive chemistry involving 127 gas‐phase and heterogeneous reactions. Thus, feedback between dynamics, chemistry and radiation occurs in every model time step. In this work, validation of the system for tropospheric and lower stratospheric analyses is undertaken with the standard observation set used in operational weather forecasting. Results are found to agree reasonably well with radiosonde observations and with Met Office (UK) analyses. Although ozone is not assimilated, ozone fields match total column observations well in terms of synoptic patterns. However, due to model biases, total column values are too large at mid‐latitudes and too small in the tropics. Since the assimilation scheme was designed for tropospheric weather prediction, its application to a middle atmosphere model can help to identify the challenges of assimilating data from this region of the atmosphere.

Record low ozone values over Canada in early 1993

Measurements of ozone made over Canada during the first four months of 1993 indicate that total ozone has been about 11 to 17% below normal. These low values were recorded, without exception, at all nine of the Canadian mid-latitude ground-based monitoring sites. Record low averages for the period from January to April were measured at three of the four mid-latitude stations where measurements have been made since the 1960’s. Comparison of January to April, 1993 ozonesonde profile measurements with those from earlier years indicates that the ozone deficit is in the lower stratosphere between 40 and 200 mb, the same altitudes where aerosols from the Mount Pinatubo volcanic eruption have been observed. The peak loss is 30% at 100 mb (16 Km).

Effects of gravity waves on complex airglow chemistries: 2. OH emission

The theory of Hines and Tarasick (1987) for the effects of gravity waves on airglow emissions is extended to consider more complex airglow chemistries, including multiple and mutiple-step production mechanisms, quenching, and other loss processes. Attention is given to nonsteady state chemistry, since the time constants of some species involved in OH* production are comparable with gravity wave periods. Relations for the dependence of η, the ratio of brightness to temperature fluctuations, on emission chemistry are presented in a generalized form which is readily applicable to other emissions. The specific case of OH airglow is examined in detail for the quenching rates of Llewellyn et al. (1978) and for those of Lowe (1991). Quenching is found to be important to predictions of η The results obtained are compared with the limited set of published observations of gravity waves in OH airglow. Although the theory predicts significant differences in the behavior of η for the two sets of rates, the existing data are not adequate to draw firm conclusions.

Influence of transport and ocean ice extent on biogenic aerosol sulfur in the Arctic atmosphere

The recent decline in sea ice cover in the Arctic Ocean could affect the regional radiative forcing via changes in sea ice-atmosphere exchange of dimethyl sulfide (DMS) and biogenic aerosols formed from its atmospheric oxidation, such as methanesulfonic acid (MSA). This study examines relationships between changes in total sea ice extent north of 70 degrees N and atmospheric MSA measurement at Alert, Nunavut, during 1980-2009; at Barrow, Alaska, during 1997-2008; and at Ny-Alesund, Svalbard, for 1991-2004. During the 1980-1989 and 1990-1997 periods, summer (July-August) and June MSA concentrations at Alert decreased. In general, MSA concentrations increased at all locations since 2000 with respect to 1990 values, specifically during June and summer at Alert and in summer at Barrow and Ny-Alesund. Our results show variability in MSA at all sites is related to changes in the source strengths of DMS, possibly linked to changes in sea ice extent as well as to changes in atmospheric transport patterns. Since 2000, a late spring increase in atmospheric MSA at the three sites coincides with the northward migration of the marginal ice edge zone where high DMS emissions from ocean to atmosphere have previously been reported. Significant negative correlations are found between sea ice extent and MSA concentrations at the three sites during the spring and June. These results suggest that a decrease in seasonal ice cover influencing other mechanisms of DMS production could lead to higher atmospheric MSA concentrations.

Long‐term ozone decline over the Canadian Arctic to early 1997 from ground‐based and balloon observations

Column ozone measurements in the Canadian High Arctic (north of 70°N) started in 1957 and there have been regular ozone sonde flights there since 1966. Column ozone values over the High Arctic were as much as 45% below normal for some days in March 1997. During March 1996 arctic ozone values were also very low. In both years, temperatures in the arctic stratosphere were extremely cold and, especially in 1997, the vortex wind pattern was unusual for the arctic and quite similar to the antarctic spring vortex. Similar cold stratospheric temperatures were present in 1967, but ozone deviations were much smaller. Despite the very low values in the High Arctic during March 1997, the average column ozone from three Canadian sites in the 50–60°N latitude range was only 3.5% below normal.