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Surface ozone monitoring sites in the tropics are limited, despite the risk that surface ozone poses to human health, tropical forest and crop productivity. Atmospheric chemistry models allow us to assess ozone exposure in unmonitored locations and evaluate the potential influence of changing policies and climate on air quality, human health and ecosystem integrity. Here, we utilise in situ ozone measurements from ground-based stations in the pan-tropics to evaluate ozone from the UK Earth system model, UKESM1, with a focus on remote sites. The study includes ozone data from areas with limited previous data, notably tropical South America, central Africa and tropical northern Australia. Evaluating UKESM1 against observations beginning in 1987 onwards, we show that UKESM1 is able to capture changes in surface ozone concentration at different temporal resolutions, albeit with a systematic high bias of 18.1 nmol mol−1 on average. We use the diurnal ozone range (DOR) as a metric for evaluation and find that UKESM1 captures the observed DOR (mean bias of 2.7 nmol mol−1 and RMSE of 7.1 nmol mol−1) and the trend in DOR with location and season. Results from this study reveal that hourly ozone concentrations from UKESM1 require bias correction before use for impact assessments based on human and ecosystem health. Indeed, hourly surface ozone data have been crucial to this study, and we encourage other modelling groups to include hourly surface ozone output as a default.

Positive trends in tropical free-tropospheric (FT) ozone are frequently ascribed to emissions growth, but less is known about the effects of changing dynamics. Extending a prior study (Thompson et al., 2021; https://doi.org/10.1029/2021JD034691; “T21”), we re-examine Southern Hemisphere Additional Ozonesondes (SHADOZ) ozone trends over equatorial Southeast Asia (ESEA), one of Earth's most convectively active regions, using 25 years (1998–2022) of ozone soundings. T21 posited that early-year positive FT ozone trends at equatorial SHADOZ stations are related to decreasing convection. The 25-year analysis of Kuala Lumpur and Watukosek SHADOZ records finds that FT ozone trends of +5 % to +15 % (+2 to +6 nmol mol−1) per decade from ∼ February–April coincide with large increases in satellite infrared brightness temperatures and outgoing longwave radiation, indicators of declining convective activity. MERRA-2 reanalyses exhibit increases in upper-tropospheric velocity potential and decreases in precipitable water, also indicating diminished convection. In contrast, trends in ozone and convective indicators are weak the rest of the year. These results suggest that decreases in convective intensity and frequency are primary drivers of FT ozone build-up over ESEA early in the year; i.e., waning convection suppresses lofting and dilution of ozone. Decreasing convection promotes accumulation of biomass burning emissions typical of boreal spring even though satellite FT carbon monoxide trends (2002–2022) over ESEA follow a global decrease pattern. Finally, our results demonstrate the advantages of monthly or seasonally resolved analyses over annual means for robust attribution of observed ozone trends, challenging models to reproduce these detailed features in simulations of the past 25 years.

We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure ∼ 50 hPa after applying OMI averaging kernels to ozonesonde data. The MBs of the stratospheric ozone column (SOC, the ozone column from the tropopause pressure to the ozonesonde burst pressure) are within 2 % with SDs of ∼ 50 hPa. The SOC MBs increase up to 3 % with SDs as great as 6 % and the TOC SDs increase up to 30 %. The comparison generally degrades at larger solar zenith angles (SZA) due to weaker signals and additional sources of error, leading to worse performance at high latitudes and during the midlatitude winter. Agreement also degrades with increasing cloudiness for pressure > ∼ 100 hPa and varies with cross-track position, especially with large MBs and SDs at extreme off-nadir positions. In the tropics and midlatitudes, the post-RA comparison is considerably worse with larger SDs reaching 2 % in the stratosphere and 8 % in the troposphere and up to 6 % in TOC. There are systematic differences that vary with latitude compared to the pre-RA comparison. The retrieval comparison demonstrates good long-term stability during the pre-RA period but exhibits a statistically significant trend of 0.14–0.7 % year−1 for pressure −1 in SOC, and −0. 33 DU year−1 in TOC during the post-RA period. The spatiotemporal variation of retrieval performance suggests the need to improve OMI's radiometric calibration especially during the post-RA period to maintain the long-term stability and reduce the latitude/season/SZA and cross-track dependency of retrieval quality.

A network of balloon-borne radiosonde observations employing chilled-mirror hygrometers for water and electrochemical concentration cells for ozone has been operated since the late 1990s in the Tropical Pacific to capture the evolution of dehydration of air parcels advected quasi-horizontally in the Tropical Tropopause Layer (TTL). The analysis of this dataset is made on isentropes taking advantage of the conservative properties of tracers moving adiabatically. The existence of ice particles is diagnosed by lidars simultaneously operated with sonde flights. Characteristics of the TTL dehydration are presented on the basis of individual soundings and statistical features. Supersaturations close to 80% in relative humidity with respect to ice (RHice) have been observed in subvisible cirrus clouds located near the cold point tropopause at extremely low temperatures around 180 K. Although further observational evidence is needed to confirm the credibility of such high values of RHice, the evolution of TTL dehydration is evident from the data in isentropic scatter plots between the sonde-observed mixing ratio (OMR) and the minimum saturation mixing ratio (SMRmin) along the back trajectories associated with the observed air mass. Supersaturation exceeding the critical value of homogeneous ice nucleation (OMR > 1.6 × SMRmin) is frequently observed on the 360 and 365 K surfaces indicating that cold trap dehydration is in progress in the TTL. The near correspondence between the two (OMR ~ SMRmin) at 380 K on the other hand implies that this surface is not sufficiently cold for the advected air parcels to be dehydrated. Above 380 K, cold trap dehydration would scarcely function while some moistening occurs before the air parcels reach the lowermost stratosphere at around 400 K where OMR is generally smaller than SMRmin.

Water vapor observations by chilled-mirror hygrometers were conducted at Bandung, Indonesia (6.90° S, 107.60° E) and Tarawa, Kiribati (1.35° N, 172.91° E) in December 2003 to examine the efficiency of dehydration during horizontal advection in the tropical tropopause layer (TTL). Trajectory analyses based on bundles of isentropic trajectories suggest that the modification of air parcels' identity due to irreversible mixing by the branching-out and merging-in of nearby trajectories is found to be an important factor, in addition to the routes air parcels follow, for interpreting the water vapor concentrations observed by chilled-mirror frostpoint hygrometers in the TTL. Clear correspondence between the observed water vapor concentration and the estimated temperature history of air parcels is found showing that drier air parcels were exposed to lower temperatures than were more humid ones during advection. Although the number of observations is quite limited, the water content in the observed air parcels on many occasions was more than that expected from the minimum saturation mixing ratio during horizontal advection prior to sonde observations.