H. Nakane

Chemical depletion of Arctic ozone in winter 1999/2000

During Arctic winters with a cold, stable stratospheric circulation, reactions on the surface of polar stratospheric clouds (PSCs) lead to elevated abundances of chlorine monoxide (ClO) that, in the presence of sunlight, destroy ozone. Here we show that PSCs were more widespread during the 1999/2000 Arctic winter than for any other Arctic winter in the past two decades. We have used three fundamentally different approaches to derive the degree of chemical ozone loss from ozonesonde, balloon, aircraft, and satellite instruments. We show that the ozone losses derived from these different instruments and approaches agree very well, resulting in a high level of confidence in the results. Chemical processes led to a 70% reduction of ozone for a region ∼1 km thick of the lower stratosphere, the largest degree of local loss ever reported for the Arctic. The Match analysis of ozonesonde data shows that the accumulated chemical loss of ozone inside the Arctic vortex totaled 117 ± 14 Dobson units (DU) by the end of winter. This loss, combined with dynamical redistribution of air parcels, resulted in a 88 ± 13 DU reduction in total column ozone compared to the amount that would have been present in the absence of any chemical loss. The chemical loss of ozone throughout the winter was nearly balanced by dynamical resupply of ozone to the vortex, resulting in a relatively constant value of total ozone of 340 ± 50 DU between early January and late March. This observation of nearly constant total ozone in the Arctic vortex is in contrast to the increase of total column ozone between January and March that is observed during most years.

Ozone depletion in and below the Arctic vortex for 1997

The winter 1996/97 was quite unusual with late vortex formation and polar stratospheric cloud (PSC) development and subsequent record low temperatures in March. Ozone depletion in the Arctic vortex is determined using ozonesondes. The diabatic cooling is calculated with PV-theta mapped ozone mixing ratios and the large ozone depletions, especially at the center of the vortex where most PSC existence was predicted, enhances the diabatic cooling by up to 80%. The average vortex chemical ozone depletion from January 6 to April 6 is 33, 46, 46, 43, 35, 33, 32 and 21 % in air masses ending at 375, 400, 425, 450, 475, 500, 525, and 550 K (about 14–22 km). This depletion is corrected for transport of ozone across the vortex edge calculated with reverse domain-filling trajectories. 375 K is in fact below the vortex, but the calculation method is applicable at this level with small changes. The column integrated chemical ozone depletion amounts to about 92 DU (21%), which is comparable to the depletions observed during the previous four winters.

Lower tropospheric ozone trend observed in 1989–1997 at Okinawa, Japan

In order to elucidate recent tropospheric ozone trends in Northeast Asia, 8 year-long ozone sounding data obtained between 1989 and 1997 at Naha (Okinawa Island), Japan, were analyzed incorporating with backward trajectory categorization. Focusing on the regionally polluted continental outflow, only data associated with air masses that reached Naha from northern, northwestern, and western directions during autumn/winter/early spring seasons (from October to March) were selected for analysis. The concentration of ozone shows an increase of about 2.5±0.6% (one standard deviation) per year for a 0-2 km layer from the ground representing the planetary boundary. The surface ozone concentrations obtained at Cape Hedo (northern tip of Okinawa Island) at the same timing as the selected ozone sounding also showed an increasing trend of 2.6% per year but with a large statistical uncertainty of ±2.0%. This result is in accordance with the 22-year period (1969–1990) of tropospheric ozone trends, 1.5–2.5% per year, obtained previously at three other Japanese ozone sounding stations, Kagoshima, Tsukuba, and Sapporo [Akimoto et al. 1994], demonstrating the continuous increase of tropospheric ozone in Northeast Asia in 1990s. It is suggested that this tropospheric ozone trend would be related to the increasing emission of NOx from Northeast Asian region (China, Japan, South Korea, Taiwan) during this period with a rate of 3.9% per year.

Arctic Ozone Loss in Threshold Conditions: Match Observations in 1997/1998 and 1998/1999

Chemical ozone loss rates inside the Arctic polar vortex were determined in early 1998 and early 1999 by using the Match technique based on coordinated ozonesonde measurements. These two winters provide the only opportunities in recent years to investigate chemical ozone loss in a warm Arctic vortex under threshold conditions, i.e., where the preconditions for chlorine activation, and hence ozone destruction, only occurred occasionally. In 1998, results were obtained in January and February between 410 and 520 K. The overall ozone loss was observed to be largely insignificant, with the exception of late February, when those air parcels exposed to temperatures below 195 K were affected by chemical ozone loss. In 1999, results are confined to the 475 K isentropic level, where no significant ozone loss was observed. Average temperatures were some 8°–10° higher than those in 1995, 1996, and 1997, when substantial chemical ozone loss occurred. The results underline the strong dependence of the chemical ozone loss on the stratospheric temperatures. This study shows that enhanced chlorine alone does not provide a sufficient condition for ozone loss. The evolution of stratospheric temperatures over the next decade will be the determining factor for the amount of wintertime chemical ozone loss in the Arctic stratosphere.

Match observations in the Arctic winter 1996/97: High stratospheric ozone loss rates correlate with low temperatures deep inside the polar vortex

With the Match technique, which is based on the coordinated release of ozonesondes, chemical ozone loss rates in the Arctic stratospheric vortex in early 1997 have been quantified in a vertical region between 400 K and 550 K. Ozone destruction was observed from mid February to mid March in most of these levels, with maximum loss rates between 25 and 45 ppbv/day. The vortex averaged loss rates and the accumulated vertically integrated ozone loss have been smaller than in the previous two winters, indicating that the record low ozone columns observed in spring 1997 were partly caused by dynamical effects. The observed ozone loss is inhomogeneous through the vortex with the highest loss rates located in the vortex centre, coinciding with the lowest temperatures. Here the loss rates per sunlit hour reached 6 ppbv/h, while the corresponding vortex averaged rates did not exceed 3.9 ppbv/h.

Ozone differential absorption lidar algorithm intercomparison

An intercomparison of ozone differential absorption lidar algorithms was performed in 1996 within the framework of the Network for the Detection of Stratospheric Changes (NDSC) lidar working group. The objective of this research was mainly to test the differentiating techniques used by the various lidar teams involved in the NDSC for the calculation of the ozone number density from the lidar signals. The exercise consisted of processing synthetic lidar signals computed from simple Rayleigh scattering and three initial ozone profiles. Two of these profiles contained perturbations in the low and the high stratosphere to test the vertical resolution of the various algorithms. For the unperturbed profiles the results of the simulations show the correct behavior of the lidar processing methods in the low and the middle stratosphere with biases of less than 1% with respect to the initial profile to as high as 30 km in most cases. In the upper stratosphere, significant biases reaching 10% at 45 km for most of the algorithms are obtained. This bias is due to the decrease in the signal-to-noise ratio with altitude, which makes it necessary to increase the number of points of the derivative low-pass filter used for data processing. As a consequence the response of the various retrieval algorithms to perturbations in the ozone profile is much better in the lower stratosphere than in the higher range. These results show the necessity of limiting the vertical smoothing in the ozone lidar retrieval algorithm and questions the ability of current lidar systems to detect long-term ozone trends above 40 km. Otherwise the simulations show in general a correct estimation of the ozone profile random error and, as shown by the tests involving the perturbed ozone profiles, some inconsistency in the estimation of the vertical resolution among the lidar teams involved in this experiment.

Large scale laser radar for measuring aerosol distribution over a wide area

A large scale laser radar was constructed to measure aerosol distribution over a wide area. It is composed of a high-power YAG laser with an average output energy of 30 W (at 1.064 μm) and 10 W (at 532 nm) a 25-pps repetition rate, and a large (effective diameter 1.5 m) receiving telescope. Three problems which degrade the accuracy of the measurement are noted, and a discussion of how to improve the accuracy of the system is included. Noise analysis shows that this system works within theoretical limits.

Numerical simulation of the retrieval of aerosol size distribution from multiwavelength laser radar measurements

A numerical investigation was carried out into the feasibility of deriving the aerosol size distribution from aerosol volume extinction and backscattering coefficient measurements by a multiwavelength laser radar. This study employs the regularization method for matrix inversion with the first-order B-spline function as basis functions to approximate the aerosol size distribution. The results of numerical simulations show that (1) the effects of roundoff errors in the numerical calculation are negligible and the approximation errors in the size distribution by the B-spline function are small, (2) the reconstruction errors in the size distribution at its peak are about twice as large as the relative measurement errors when the Lagrange multiplier, which determines the degree of smoothness in the reconstruction, is suitably chosen, and (3) the variation in the complex refractive index due to the humidity change does not produce large errors in the size distribution.

ILAS observations of chemical ozone loss in the Arctic vortex during early spring 1997

Chemical ozone loss rates were estimated for the Arctic stratospheric vortex by using ozone profile data (Version 3.10) obtained with the Improved Limb Atmospheric Spectrometer (ILAS) for the spring of 1997. The analysis method is similar to the Match technique, in which an air parcel that the ILAS sounded twice at different locations and at different times was searched from the ILAS data set, and an ozone change rate was calculated from the two profiles. A statistical analysis indicates that the maximum ozone loss rate was found on the 450 K potential temperature surface in February, amounting to 84 ppbv/day. The integrated ozone loss for two months from February to March 1997 showed its maximum of 1.5±0.1 ppmv at the surface that followed the diabatic descent of the air parcels and reached the 425 K level on March 31. This is about 50% of the initial (February 1) ozone concentration. The present study demonstrated that data from a solar occultation sensor with a moderate altitude resolution can be used for the Match analysis.

Validation of ILAS Version 3.10 ozone with ozonesonde measurements

Ozone (O3) measurements made with the Improved Limb Atmospheric Spectrometer (ILAS) onboard the Advanced Earth Observing Satellite (ADEOS) were validated with correlative ozonesonde measurements conducted at five stations, Andoya, Kiruna and Yakutsk in the Northern Hemisphere, and Neumayer and Syowa in the Southern Hemisphere. The ILAS Version 3.10 O3 vertical profiles were compared with 79 correlative ozonesonde measurements that were made within 500 km and 3 hours in distance and time differences, respectively. The comparisons indicate that ILAS O3 typically has an accuracy within 20% between 12 and 35 km. The precision of the ILAS O3 is estimated to be ±10–25% between 12 and 20 km, ±5–7% between 20 and 30 km, and ±5% between 30 and 40 km.