From: Subject: NATURE VOL.315 16 MAY 1985 Date: Mon, 11 May 2015 20:12:51 +0900 MIME-Version: 1.0 Content-Type: multipart/related; type="text/html"; boundary="----=_NextPart_000_0000_01D08C26.DB99CCC0" X-MimeOLE: Produced By Microsoft MimeOLE V6.00.2900.6157 This is a multi-part message in MIME format. ------=_NextPart_000_0000_01D08C26.DB99CCC0 Content-Type: text/html; charset="shift_jis" Content-Transfer-Encoding: quoted-printable Content-Location: http://www.ciesin.org/docs/011-430/011-430.html NATURE VOL.315 16 MAY 1985

= Reproduced, with = permission, from: Farman, J. C., B. G. Gardiner, and J. D. Shanklin. = 1985.=20 Large losses of total ozone in Antarctica reveal seasonal ClOx/NOx = interaction.=20 Nature 315: 207-10.=20

Large losses of total ozone in Antarctica reveal seasonal Cl0x/NOx=20 interaction

J. C. Farman, B. G. Gardiner & J. D. Shanklin

British Antarctic Survey, Natural Environment Research Council, High = Cross,=20 Madingley Road, Cambridge CB3 OET, UK

Recent attempts [1= ,2= ] to=20 consolidate assessments of the effect of human activities on = stratospheric ozone=20 (03) using one-dimensional models for 30deg. N have suggested that = perturbations=20 of total 03 will remain small for at least the next decade. Results from = such=20 models are often accepted by default as global estimates [3= ]. The=20 inadequacy of this approach is here made evident by observations that = the spring=20 values of total O3 in Antarctica have now fallen considerably. The = circulation=20 in the lower stratosphere is apparently unchanged, and possible chemical = causes=20 must be considered. We suggest that the very low temperatures which = prevail from=20 midwinter until several weeks after the spring equinox make the = Antarctic=20 stratosphere uniquely sensitive to growth of inorganic chlorine, ClX, = primarily=20 by the effect of this growth on the NO2/NO ratio. This, with the height=20 distribution of UV irradiation peculiar to the polar stratosphere, could = account=20 for the O3 losses observed.

Total 03 has been measured at the British Antarctic Survey stations,=20 Argentine Islands 65deg. S 64deg. W and Halley Bay 76deg. S 27deg. W, = since=20 1957. Figure = 1a shows=20 data from Halley Bay. The mean and extreme daily values from October = 1957 to=20 March 1973 and the supporting calibrations have been discussed elsewhere = [4= ,5= ]. The=20 mean daily value for the four latest complete observing seasons (October = 1980-March 1984) and the individual daily values for the current = observing=20 season are detailed in Fig.1. The more = recent=20 data are provisional values. Very generous bounds for possible = corrections would=20 be +/-30 matm cm. There was a changeover of spectrophotometers at the = station in=20 January 1982; the replacement instrument had been calibrated against the = UK=20 Meteorological Office standard in June 1981. Thus, two = spectrophotometers have=20 shown October values of total 03 to be much lower than March values, a = feature=20 entirely lacking in the 1957-73 data set. To interpret this difference = as a=20 seasonal instrumental effect would be inconsistent with the results of = routine=20 checks using standard lamps. Instrument temperatures (recorded for each=20 observation) show that the March and October operating conditions were=20 practically identical. Whatever the absolute error of the recent values = may be,=20 within the bounds quoted, the annual variation of total 03 at Halley Bay = has=20 undergone a dramatic change.

Figure 1b = shows=20 data from Argentine Islands in a similar form, except that for clarity = the=20 extreme values for 1957-73 have been omitted. The values for 1980 to the = present=20 are provisional, the extreme error bounds again being +30 matm cm. The = changes=20 are similar to those seen at Halley Bay, but are much smaller in = magnitude.

Upper-air temperatures and winds are available for these stations = from 1956.=20 There are no indications of recent departures from established mean = values=20 sufficient to attribute the changes in total O3 to changes in the = circulation.=20 The present-day atmosphere differs most prominently from that of = previous=20 decades in the higher concentrations of halocarbons. Figure 2a shows = the=20 monthly mean total O3 in October at Halley Bay, for 1957-84, and Fig. 2b that in = February,=20 1958-84. Tropospheric concentrations of the halocarbons F-11 (CFCl3) and = F-12=20 (CF2Cl2) in the Southern Hemisphere [3= ] are=20 also shown, plotted to give greatest emphasis to a possible = relationship. Their=20 growth, from which increase of stratospheric ClX is inferred, is not = evidently=20 dependent on season. The contrast between spring and autumn O3 losses = and the=20 striking enhancement of spring loss at Halley Bay need to be explained. = In=20 Antarctica, the lower stratosphere is ~40 K colder in October than in = February.=20 The stratosphere over Halley Bay experiences a polar night and a polar = day (many=20 weeks of darkness, and of continuous photolysis, respectively); that = over=20 Argentine Islands does not. Figure 3 shows = calculated=20 amounts of NOx in the polar night and the partitioning between the = species [6= ]. Of=20 these, only NO3 and NO2 are dissociated rapidly by visible light. The = major=20 reservoir, N2O5, which only absorbs strongly below 280 nm, should be = relatively=20 long-lived. Daytime levels of NO and NO2 should be much less in early = spring,=20 following the polar night, than in autumn, following the polar day. = Recent=20 measurements [7= ] support=20 these inferences. The effect of these seasonal variations on the = strongly=20 interdependent ClOx and NOx cycles is examined below.

The 03 loss rate resulting from NOx and Cl0x may be written [8= ]=20

3DFORMULA L accounts for = over 85% of=20 O3 destruction in the altitude range 20-40 km. At 40 km, N and C are = roughly=20 equal. Lower down, C decreases rapidly to 10% of L at 30 km, 3% at 20 km = (refs=20 6, 8). Equation (1) is based on two steady-state approximations, (see Table 1a for = the=20 reactions involved)=20

3DFORMULA and=20

3DFORMULA valid in daytime, = with [O]=20 in steady state with [03]. Reaction (4) has a negative temperature = coefficient,=20 whereas reaction (1) has large positive activation energy [9= ], with=20 the result that u is strongly dependent on [Cl0] at low temperature, as = shown in=20 Fig. 4. = [Cl0] is not=20 simply proportional to total ClX, because ClONO2 formation (reaction = (10))=20 intervenes. Throughout the stratosphere, X<<1, so that = [ClO]~[Cl+ClO].=20 From a steady-state analysis of the reactions given in Table 1b,=20

3DFORMULA Values of u, X and = [Cl+Cl0]=20 obtained from equations (2), (3) and (4) are in good accord with full=20 one-dimensional model results for late summer in Antarctica [6= ].=20 Neglecting seasonal effects other than those resulting from temperature = and from=20 variation of [NO+ NO2], it is possible to solve simultaneously for [NO2] = and=20 [Cl0], and to derive L. Results are shown in Table 2 as = relaxation=20 times [8= ],=20 [03]/L, for various conditions. The spring values (lines 2, 3 and 4) are = highly=20 dependent on ClX amount (compare columns a and b), the autumn values = (line 1)=20 much less so. At Argentine Islands, the sensitivity to ClX growth should = resemble that seen in line 2, attributable solely to low temperature. = Lines 3=20 and 4 show the enhanced sensitivity possible at stations within the = Antarctic=20 Circle, such as Halley Bay, arising from slow release of [NO+NO2] = following the=20 polar night. It remains to be shown how stable 03 budgets were achieved = with the=20 relaxation times for the lower chlorine level (Table 2, a).=20

Much 03 destruction is driven by visible light, but production = requires=20 radiation below 242 nm. On the dates shown (Table 2), = destruction=20 persists for some 11 h, while, because of the long UV paths, production = is weak=20 (except around noon) at 29 km, and is virtually absent below that = altitude. Line=20 1 of Table 2 = then=20 demands 03 transport in autumn from the upper to the lower stratosphere, = which=20 is consistent with inferred thermally-driven lagrangian-mean = circulations [10]. A=20 mean vertical velocity of 45 m per day is in good accord with = calculations of=20 net diabatic cooling [11] and=20 gives a realistic total 03 decay rate in an otherwise conventional=20 one-dimensional model [6= ]. The=20 short relaxation times in the lower stratosphere in autumn are = tolerable, with=20 adequate transport compensating for lack of 03 production.

In early spring, on the other hand, wave activity scarcely penetrates = the=20 cold dense core of the Antarctic polar vortex and with very low = temperatures the=20 net diabatic cooling is very weak [11].=20 Lagrangian transport in the vortex should then be almost negligible. = (The=20 virtual exclusion of Agung dust from the vortex supports this view [5= ].) The=20 final warming signals the end of this period of inactivity and is = accompanied by=20 large dynamically induced changes in 03 distribution. However, before = the=20 warming, with low chlorine, total 03 was in a state of near-neutral = equilibrium,=20 sustained primarily by the long relaxation times. With higher chlorine,=20 relaxation times of the order seen in line 4, Table 2, entail = more=20 rapid 03 losses. With negligible production below 29 km and only weak = transport,=20 large total 03 perturbation is possible. The extreme effects could be = highly=20 localized, restricted to the period with diurnal photolysis between = polar night=20 and the earlier of either the onset of polar day or the final spring = warming. At=20 the pole [NO+NO2] rises continuously after the polar night, with the = Sun. The=20 final warming always begins over east Antarctica and spreads westwards = across=20 the pole. At Halley Bay the warming is typically some 14 days later than = at the=20 pole. Maximum O3 depletion could be confined to the Atlantic half of the = zone=20 bordered roughly by latitudes 70 and 80deg. S.

Comparable effects should not be expected in the Northern Hemisphere, = where=20 the winter polar stratospheric vortex is less cold and less stable than = its=20 southern counterpart. The vortex is broken down, usually well before the = end of=20 the polar night, by major warmings. These are accompanied by large-scale = subsidence and strong mixing, in the course of which peak O3 values for = the year=20 are attained. Hence, sensitivity to ClX growth should be minimal if, as=20 suggested above, this primarily results from 03 destruction at low = temperatures=20 in regions where 03 transport is weak.

We have shown how additional chlorine might enhance 03 destruction in = the=20 cold spring Antarctic stratosphere. At this time of the year, the long = slant=20 paths for sunlight make reservoir species absorbing strongly only below = 280 nm,=20 such as N2O5, ClONO2 and HO2NO2, relatively long-lived. The role of = these=20 reservoir species should be more readily demonstrated in Antarctica,=20 particularly the way in which they hold the balance between the NOx and = ClOx=20 cycles. An intriguing feature could be the homogeneous reaction (Table 1c) = between HCl and=20 ClONO2. If this process has a rate constant as large as 10(-16) cm3 = s(-1) (ref.=20 2) and a negligible temperature coefficient, the reaction would go = almost to=20 completion in the polar night, leaving inorganic chlorine partitioned = between=20 HCl and Cl2, almost equally at 22 km for example. Photolysis of Cl2 at=20 near-visible wavelengths would provide a rapid source of [Cl + ClO] at = sunrise,=20 not treated in equation (4). The polar-night boundary is, therefore, the = natural=20 testing ground for the theory of linear response to chlorine [1= , 2= ]. It=20 might be asked whether a nonlinear response is already evident (Fig.2a). An = intensive=20 programme of trace-species measurements on the polar-night boundary = could add=20 greatly to our understanding of stratospheric chemistry, and thereby = improve=20 considerably the prediction of effects on the ozone layer of future = halocarbon=20 releases.

We thank B. A. Thrush and R. J. Murgatroyd for helpful suggestions.

Received 24 December 1984; accepted 28 March 1985.

1. Cicerone, R. J., Walters, S. & Liu, S. C. J = geophys. Res.=20 l8, 3647-3661 (1983).

2. Prather, M. J., McElroy, M. B. & Wofsy, S. C. = Nature 312,=20 227-231 (1984).

3. The Stratosphere 1981, Theory and Measurements (WMO = Global=20 Ozone Research Monitoring Project Rep. No. 11, 1981).

4. Farman, J. C. & Hamilton, R. A. Br. Antarct. = Surv. Sci.=20 Rep. No 90 (1975).

5. Farman, J. C. Phil. Trans. R. Soc. B279, 261-271 = (1977).

6. Farman, J. C., Murgatroyd, R. J., Silnickas, A. M. = &=20 Thrush, B. A. Q. Jl R. met. Soc.(submitted).

7. McKenzie, R. L. & Johnston, P. V. Geophys. Res. = Lett, 11,=20 73-75 (1984).

8. Johnston, H. S. & Podolske, J. Rev. Geophys. = Space Phys.=20 16, 491-519 (1978).

9. Chemical Kinetics and Photochemical Data for Use in=20 Stratospheric Modelling, Evaluation No. 6 (JPL Publ. 83-62, 1983).

10. Dunkerton, T. J. atmos. Sci. 35, 2325-2333 = (1978).

11. Dopplick, T. G. J. atmos. Sci 29, 1278-1294 = (1972).

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