Ozone depletion in the middle atmosphere during solar proton events in October 2003

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itsencs, Upasedlcue uto estimate the rates of ionelectron pair, odd-nitrogen and odd-hydrogen production. Our calculations show that the production of odd-hydrogen causes the ozone depletion by the factor 2 and more at the altitudes higher than 55 km. This depletion is in an agreement withet al., 1981; Solomon et al., 1981, 1983a; Jackman et al.,HOx1 +O!HOx+O2, x=0, 1. 2btion of odd-nitrogen and odd-hydrogen through reactionsselves by the traditional point of view in the calculationof the odd-nitrogen and odd-hydrogen inuence on theozone balance according to processes (1a,b) and (2a,b).The main goal of the paper is to study ozone concentrationdepletions observed in the middle atmosphere during SPEseries in October 2003.* Corresponding author. Tel.: +7 81555 79760.E-mail addresses: sunactivity@yahoo.se (Kh. Fadel), kirillov@pgi.kolasc.net.ru (A.S. Kirillov).Advances in Space Research 382000; Krivolutsky et al., 2001; Kirillov, 2004a). The odd-ni-trogen NOx and odd-hydrogen HOx can cause ozonedepletion in the mesosphere and stratosphere through thecatalytic cycles (including NO + NO2 and H + OH + HO2)(Brasseur and Solomon, 1984):NOx+O3!NOx1 +O2, 1aNOx1 +O!NOx+O2, x=1, 1bandHOx+O3!HOx1 +O2, 2ain the middle atmosphere. Also it was concluded in(Kirillov, 2004a) that there is an eective production ofsinglet molecular oxygen (excited in metastable a1Dg orb1Rg states principally in vibrational level v = 0) and highlyvibrationally excited O2 (in ground X 3Rg state, v > 20)in the middle atmosphere during solar proton events(SPEs).Here we do not consider, however, any role of electronicand vibration kinetics in chemical balance of the middleatmosphere. This is the complicated independent taskwhich is beyond the given study. So here we will limit our-measurements of O3 altitude proles made on POAM-3 satellite. 2006 COSPAR. Published by Elsevier Ltd. All rights reserved.Keywords: Solar proton event; Middle atmosphere; Ozone depletion; Odd-nitrogen; Odd-hydrogen1. IntroductionSolar protons precipitating in the middle atmosphereproduce large amounts of odd-nitrogen, odd-hydrogenand electronically excited atoms and molecules (RuschMoreover, solar protons and secondary electrons causethe eective electronic excitation of main atmospheric com-ponents N2 and O2 in inelastic collisions. It was proposedin (Toumi, 1993; Zipf and Prasad, 1998) that electronicallyexcited molecular oxygen could cause the sucient produc-Ozone depletion in the msolar proton evenKh. Fadel a, E.V. Vasha Swedish Institute of Space Physib Polar Geophysical Institute, AReceived 23 December 2004; received in reviAbstractA one-dimensional time-dependent model has been used to caatmosphere during solar proton precipitations in October 2003. W0273-1177/$30 2006 COSPAR. Published by Elsevier Ltd. All rights reservdoi:10.1016/j.asr.2006.04.015ddle atmosphere duringin October 2003yuk b, A.S. Kirillov b,*mea University, Kiruna, Swedentity, Murmansk region, Russiaform 18 April 2006; accepted 19 April 2006late the production and loss of minor components of the middlesed the solar proton uxes measured on the GOES-11 spacecraftwww.elsevier.com/locate/asr(2006) 18811886ed.ace2. The modelThe model considers a production of a set of minorcomponents in the middle atmosphere by the solar lightabsorption and by energetic proton and secondary electronimpacts. The set includes atomic oxygen O(3P, 1D), ozoneO3, atomic nitrogen N(4S, 2D), odd-nitrogen NOx (nitricoxide, nitrogen dioxide and trioxide), dinitrogen pentoxideN2O5, nitrous oxide N2O, odd-hydrogen HOx (atomichydrogen, hydroxyl and hydroperoxy radicals), even-hy-drogen H2Ox (molecular hydrogen, water vapor andhydrogen peroxide), HNOx (nitrous, nitric and peroxyni-tric acids), COx (carbon monoxide and dioxide), CHx(methyl and methane), CHxOy (formyl radical, formalde-hyde, methoxy and methylperoxy radicals and methylhydroperoxide), chlorine and bromide compounds: X2,X, HX, HOX, XO and XONO2 (here X = Cl or Br),unsymmetric ClOO and symmetric OClO chlorine diox-ides, chlorine oxides Cl2Ox (x = 13), BrCl. One hundredand thirty seven chemical reactions between the compo-nents are included in the model (Atkinson et al., 2005;Sander et al., 2003).Since the reaction of nitrous oxide with electronicallyexcited atomic oxygenN2O+O (1D)!NO+NO 3is the main production channel of odd-nitrogen in thestratosphere during quiet period (Jackman et al., 1980)we input N2O concentrations according to (Olsen et al.,2001). The source of odd-hydrogen is the direct photolysisof H2O and by the reactions (Solomon et al., 1983b; Crut-zen, 1997)H2O+O (1D)!OH+OH, 4H2 +O (1D)!H+OH. 5The concentrations of even hydrogen H2O and H2 weretaken equal to 6 ppmv and 0.5 ppmv, respectively, (Robleand Dickinson, 1989), decreasing at altitudes higher than70 km and lower than 40 km for H2O (Gunson et al.,1990; Zhou et al., 1997). So concentration proles ofN2O, H2O and H2 are taken as invariable in time in ourcalculations.Also we consider concentration proles for carbon diox-ide CO2 and methane CH4 as invariable. Data for CO2were taken according to (Zaragoza et al., 2000) and forCH4 according to (Gunson et al., 1990; Zhou et al.,1997). Seasonal variation of long-lived trace gases (Sum-mers et al., 1997) are neglected in our consideration.We input initial concentration proles for chlorine com-pounds HCl, HOCl, ClO and ClONO2 according to(Michelsen et al., 1996; Zander et al., 1996). Initial concen-tration proles for bromine compounds Br2, Br, HBr,HOBr, BrO, BrONO2 and BrCl were taken according to1882 Kh. Fadel et al. / Advances in SpBrO proles measured in (Harder et al., 1998) and normal-ised to be in agreement with model data of Lary (1996).Dierent spectral intervals of the solar light are impor-tant in the dissociative processes of O2 and minor compo-nents, so the solar spectral irradiance in visible andultraviolet regions used in the model calculations was takenaccording to (Mount and Rottman, 1981; Nicolet, 1989).Absorption cross sections for major gas O2 and minorcomponents were taken mainly according to (Atkinsonet al., 2005; Finlayson-Pitts and Pitts, 2000; Sander et al.,2003). All spectrum diapason 120900 nm is divided inthe intervals with the width of 1 nm. The decrease of theintensity of solar light in the every interval was calculatedaccording to exponential LambertBeer law where theoptical depth at the altitude h includes the contributionof all atmospheric components having non-zero cross sec-tions of solar light absorption.To calculate the rates of ionelectron pair production byprecipitated particles we use the following formula for ratesof solar proton energy dissipated in cubic centimeter persecond at the altitude h (Dorman, 1975, chapter 6):wh qhAZ EmaxEminZ p20f E Em1 Am 1 Xcos h mm1 2p sin hdEdh: 6Here q is the density of the atmosphere, f(E) is the energeticspectrum of solar protons, X is the respective depth ing/cm2, Emin = 1 MeV, Emax = 400 MeV and parameters Aand m are equal to 242 and 0.75, respectively. The rate ofionelectron pair production is related with the valuew(h) by the relationqh whQ; 7where Q is equal to 35 eV. Here we suggest the isotropicdistribution of solar protons on the pitch angle h in allour calculations.The continuity non-stationary equationsoniot oohDonioh 1ToToh 1Hi ni P i Lini 8are solved for minor components of the middle atmo-sphere. Here ni and Hi is the concentration and the scaleheight of the ith component, D is the diusion coecient,T is the temperature, Pi and Li are the production and lossrates of the ith component. The production and loss ratesinclude the contributions from dissociative processes relat-ed with solar light inelastic scattering, chemical reactions,production of minor components in collisions of protonsand secondary electrons with main atmospheric compo-nents. Diusion coecient adopted in our study was takenaccording to (Crutzen et al., 1978). Upper and lower bor-ders in our calculation are at 90 km and 20 km, respective-ly. Border conditions are given uxes at 90 km andphotochemical equilibrium at 20 km. The time integrationof Eq. (8) were carried out explicitly, in which case the spa-Research 38 (2006) 18811886tial derivative terms are only evaluated at known time (pre-ceding step in time) (Rood, 1987). Time and altitude stepsis suggested for spectral interval 120145 nm (Stief et al.,1975). The cross section for solar Lyman-a line (121.6 nm)is equal to 2 1017 cm2 (Sonnemann et al., 1977).Absorption spectrum of carbon dioxide CO2 was takenaccording to (Thompson et al., 1963) for the spectral inter-val 120200 nm. The quantum yield of 1.0 for the processCO2 + hm!CO+O (1D)is suggested for spectral interval 120167 nm (Lin and Bau-er, 1969).3. Experimental data on solar protonsIonization eects in middle atmosphere in late October,2003 were caused by the SPEs of 28 and 29 October. Char-acteristics of the parent solar ares are presented in Table1. Fig. 1 shows intensity proles of solar protons with ener-gies >10 MeV, >30 MeV and >100 MeV as measured atGOES-11 spacecraft. Two maxima on the intensity curvescorrespond to the two SPEs: on 28 and 29 October. Byarrows at the time axis are shown the times of the relevantares (Table 1). The date, the time of X-ray maximum(probable moment of particle acceleration), are impor-tance and heliocoordinates are shown in respective col-umns of Table 1.The dierential energy spectra of solar protons werederived using the GOES-11 data in the integral energyace Research 38 (2006) 18811886 1883for the integration in our calculation were taken equal to0.1 s and 1 km, respectively.Since electronically excited atomic oxygen participatingin chemical reactions (3)(5) is responsible for the produc-tion of odd-nitrogen and odd-hydrogen in the quiet atmo-sphere. The atoms are produced mainly inphotodissociation processes related with molecular oxygenO2, ozone O3, nitrous oxide N2O, water vapor H2O andcarbon dioxide CO2.The production of electronically excited atomic oxygenO(1D) in the processO2 + hm!O+O (1D)is believed to be possible only in the Schumann-Rungecontinuum and by Lyman-a line. Cross sections for thespectrum interval 130175 nm have been taken accordingto (Watanabe et al., 1953; Goldstein and Mastrup, 1966).A quantum yield of unity is for the interval 139175 nmand with oscillating structure for the interval 130138 nm(Nee and Lee, 1997). Although the results of (Lacour-siere et al., 1999) have revealed a strongly wavelength-de-pendent window in the O(1D) yield, we have acceptedthe value of 0.44 from suciently earlier laboratorystudy (Lee et al., 1977). The solar light absorption inthe Herzberg continuum and in the Schumann-Rungebands for O2 is supposed to cause a production of twooxygen atoms in the ground state 3P (Yoshino et al.,1988, 1992).The solar light absorption of O3 in the Hartley, Hugginsand Chappuis bands causes the dissociation of ozone mol-ecule. Only the scattering in Hartley and Huggins bands isbelieved to have the production of O(1D) (Matsumi andKawasaki, 2003) in the processO3 + hm!O2 +O (1D).We suggest the quantum yield of O(1D) about 0.90 forspin-allowed channel with the production of O2(a1Dg) forthe 185305 nm interval (Atkinson et al., 2005) anddecreasing yield for higher k (305330 nm) according to(Armerding et al., 1995; Talukdar et al., 1998). The solarlight scattering in Huggins (330350 nm) and Chappuisbands (440750 nm) causes only the production of twooxygen atoms in ground state.Absorption spectrum of nitrous oxide N2O was takenaccording to (Finlayson-Pitts and Pitts, 2000) for the spec-tral interval 173240 nm. The molecule absorbs and disso-ciates with unit quantum yield to N2 and electronicallyexcited atomic oxygenN2O+ hm!N2 +O (1D)(Sander et al., 2003; Atkinson et al., 2005).Absorption spectrum of water vapor H2O was takenaccording to (Brasseur and Solomon, 1984) for the spectralinterval 120200 nm. The quantum yield of 0.11 for theprocessKh. Fadel et al. / Advances in SpH2O+ hm!H2 +O (1D)Table 1Characteristics of solar aresDate X-ray 1-8 A max Flare importance Heliocoordinates28. 10. 2003 11.10 4B/X17.2 S16E0829. 10. 2003 20.49 2B/X10.0 S15W02Fig. 1. Intensity proles of energetic solar protons on October 2830,2003: 1 E > 10 MeV, 2 E > 30 MeV and 3 E > 100 MeV; a 6.00 UTof 28.10, b 18.00 UT of 28.10, c 6.00 UT of 29.10, d 18.00 UT of29.10 and e 6.00 UT of 30.10.1884 Kh. Fadel et al. / Advances in Spacechannels: >1 MeV, >5 MeV, >10 MeV, >30 MeV,>50 MeV and >100 MeV for every hour in the period from11.00 UT of 28.10 to the end of day of 30.10. The spectraderived in ve moments of time, corresponding to markedby characters a, b, c, d and e in Fig. 1 are shown inFig. 2. The relevant position of the spectra in vertical axiscorrespond to the intensity variations of solar protons dur-ing the considered period (Fig. 1).Fig. 3 shows the ionization proles calculated usingspectra ae and formulas (6) and (7). The prole a cor-responds to ionization state before the start of SPE of28.10. Proles b and c correspond to the intensity max-imum of the SPE of 28.10. The prole d is calculated forthe period before the start of SPE of 29.10, and the prolee is for its maximum. A little dierence between the spec-Fig. 2. Derived spectra of solar protons for ve times (ae) as in Fig. 1.tra d and e was because of suciently high intensity ofsolar protons produced in SPE of 28.10 retained up toFig. 3. Calculated ion production rate due to solar protons for ve times(ae) as in Fig. 1.the start of SPE of 29.10. The proles are in good agree-ment with similar calculations in (Jackman et al., 2005)showing the ion pair production more than 104 cm3 s1at the altitude interval 4580 km of 2829.10.4. Results of calculations and comparisons with experimentaldataAltitude proles of O3 concentration measured onPOAM-3 satellite are shown in Fig. 4. The altitude prolesat the point (70N and 110W) are presented for 22.00 UTof 27.10 (quiet) and 22.00 UT of 28.10 and 30.10 (after SPEseries). As it is seen from Fig. 1 during the period of 2830October a series of powerful SPEs has occurred. The ozonedepletion at the altitudes higher than about 50 km after theFig. 4. Proles of O3 concentrations measured on POAM-3 satellite: 1 22.00 UT of 27.10, 2 22.00 UT of 28.10 and 3 22.00 UT of 30.10.Research 38 (2006) 18811886series of very strong SPEs can be seen in the gure. A littledecrease at smaller altitudes (3040 km) can be to consideras negligible.The results of our calculations of ozone concentrationsfor a quiet period for 12.00 LT of 27.10 and for 12.00LT of 29.10 and 30.10 are shown in Fig. 5. The signicantozone depletions (factor 2 and more) is obtained for alti-tude interval higher than 55 km. We suggested in the calcu-lations that in the middle atmosphere the odd-nitrogen andodd-hydrogen produced per ionelectron pair has theratios of 1.3 and 2.0, respectively (Heaps, 1978; Ruschet al., 1981; Solomon et al., 1981). The averaged GOES-11 solar proton data for 00.0012.00 UT on 26 Octoberare taken as background proton intensities for quietperiods.We see from Fig. 3 that the processes of the ionizationand odd-nitrogen and odd-hydrogen production are eec-tive only at the altitudes higher than 40 km for isotropicdistribution on pitch angles for solar protons. The calcula-tions of altitude proles of atmospheric components haveshown the obtained decrease in ozone concentrations iscaused by OH production and the chemical processace(2a,b) having high rate coecients of the interaction. Thisdecrease of ozone concentrations in northern hemisphere isin good agreement with ozone estimations made accordingto limb scatter measurements with the SCIAMACHYinstrument on the Envisat spacecraft in (Rohen et al.,2005). Similar ozone depletion on October 28, 2003 wasobserved on the Odin satellite over the southern polarcap in (Degenstein et al., 2005). The production of odd-ni-trogen and the chemical process (1a,b) during SPEs doesnot cause the ozone decrease for the considered period(23 days). Stratospheric eects of the particle precipita-tions in the reduction of O3 are strongly pronounced onlyfew months later (Randall et al., 2005).5. ConclusionsFig. 5. Calculated proles of O3 concentrations: 1 12.00 LT of 27.10,2 12.00 LT of 29.10 and 3 12.00 LT of 30.10.Kh. Fadel et al. / Advances in SpA one-dimensional time-dependent model of the mid-dle atmosphere is applied to estimate the changes ofminor components during SPEs of 2830 October of2003. Following Heaps (1978), Rusch et al. (1981) andSolomon et al. (1981) we use the ratios of 1.3 and 2.0of the production of the odd-nitrogen and odd-hydrogenper ionelectron pair. Our calculations have shown thatthe main factor causing the ozone content decrease inthe middle atmosphere during solar proton precipitationsis the odd-hydrogen species production through the mul-tiple hydrogen and subsequent recombination in theionization products. Here we have not considered theinuence of electronically excited atomic and molecularcomponents on the production of odd-hydrogen andodd-nitrogen and ozone balance in the middle atmo-sphere during SPE discussed in (Toumi, 1993; Zipf andPrasad, 1998; Kirillov, 2004a) but leave the issue forfuture investigations. The conclusion of (Kirillov, 2004a)about eective production of singlet oxygen in the middleatmosphere during SPE is based on good agreement ofcalculated quenching rate coecients of electronicallyPfeilsticker, K. Stratospheric BrO proles measured at dierentlatitudes and seasons: atmospheric observations. Geophys. Res. Lett.25, 38433846, 1998.Heaps, M.G. 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Science 279, 211213, 1998.Research 38 (2006) 18811886Ozone depletion in the middle atmosphere during solar proton events in October 2003IntroductionThe modelExperimental data on solar protonsResults of calculations and comparisons with experimental dataConclusionsAcknowledgementsReferences


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