1 JOVIAN STRATOSPHERE AS A CHEMICAL TRANSPORT 2 SYSTEM: BENCHMARK ANALYTICAL SOLUTIONS 3 4 XI ZHANG1, RUN-LIE SHIA1, AND YUK L. YUNG1 5 6 7 1 8 Pasadena, CA, 91125, USA; xiz@gps.caltech.edu Division of Geological and Planetary Sciences, California Institute of Technology, 9 10 11 12 13 14 15 16 17 To be submitted to 18 The Astrophysical Journal 19 20 21 22 23 24 25 26 27 28 29 30 31 1 32 ABSTRACT 33 34 We systematically investigated the solvable analytical benchmark cases in both one- and 35 two-dimensional (1-D and 2-D) chemical-advective-diffusive systems. We use the 36 stratosphere of Jupiter as an example but the results can be applied to other planetary 37 atmospheres and exoplanetary atmospheres. In the 1-D system, we show that CH4 and 38 C2H6 are mainly in diffusive equilibrium, and the C2H2 profile can be approximated by 39 the modified Bessel functions. In the 2-D system in the meridional plane, analytical 40 solutions for two typical circulation patterns are derived. Simple tracer transport 41 modeling demonstrates that the distribution of a short-lived species (such as C2H2) is 42 dominated by the local chemical sources and sinks, while that of a long-lived species 43 (such as C2H6) is significantly influenced by the circulation pattern. We find an equator- 44 to-pole circulation could qualitatively explain the Cassini observations, but a pure 45 diffusive transport process could not. For slowly rotating planets like the close-in 46 extrasolar planets, the interaction between the advection by the zonal wind and chemistry 47 might cause a phase lag between the final tracer distribution compared and the original 48 source distribution. The numerical simulation results from the 2-D Caltech/JPL 49 chemistry-transport model agree well with the analytical solutions for various cases. 50 51 52 53 54 55 56 57 58 59 60 61 62 2 63 64 1. INTRODUCTION 65 66 The Jovian stratosphere is an ideal laboratory to study atmospheric tracer transport. The 67 stratosphere is dominated by the hydrocarbon photochemistry, driven by the photolysis of 68 the parent species, methane (CH4), which is transported from the deep atmosphere. Two 69 most abundant photochemical products, acetylene (C2H2) and ethane (C2H6), have 70 properties to make them ideal tracers. First, besides CH4, they show the most prominent 71 features in the middle infrared emission spectra of Jupiter. Therefore their latitudinal and 72 vertical distributions can be accurately determined. Second, their chemical lifetimes are 73 different by about two orders of magnitude, ranging from several Earth years (C2H2) to 74 several hundreds of Earth years (C2H6). That means they have different sensitivity to the 75 transport. In fact, their latitudinal profiles (Nixon et al. 2007) show opposite trends, 76 implying that the transport timescale is probably located within the two lifetimes. Third, 77 their chemistry is relatively simple and most of the chemical reaction coefficients have 78 been measured in the laboratory with small uncertainties. Unlike the other possible 79 tracers, such as hydrogen cyanide (HCN) and carbon dioxide (CO2), whose vertical 80 distribution is not known (Lellouch et al. 2006), or aerosol, which might be affected by 81 complicated microphysics, the simple combination of C2H2 and C2H6 contains a wealth 82 of information of the stratospheric circulation on Jupiter. 83 84 Most of the previous studies focused on 1-D chemistry-diffusion models (e.g., Strobel 85 1974; Gladstone et al. 1996; Moses et al. 2005), which essentially ignore the latitudinal 86 transport. The advantages of 1-D model are: (1) it is numerically stable due to the nature 87 of diffusive processes; (2) the computation is usually fast, and therefore it could include a 88 very complicated network of chemical reactions (Moses et al. 2005). Once the horizontal 89 and vertical advection terms are added, the model is subject to the numerical instability 90 and limited by the Courant-Friedrichs-Lewy (CFL) criterion, although the 2-D 91 calculation is more realistic. 92 3 93 There is no definitive 2-D CTM for the stratosphere of Jupiter, taking into account the 94 photochemistry, eddy and molecular diffusion, as well as the vertical and horizontal 95 advection, although the existence of large-scale stratospheric circulation has been 96 hypothesized since the 1990s (e.g., Conrath et al. 1990; West et al. 1992). Friedson et al. 97 (1999) proposed that the horizontal eddy mixing processes dominate the transport of the 98 SL9 debris in the stratosphere of Jupiter. Liang et al. (2005) used a 2-D chemistry- 99 diffusion model and found that the horizontal mixing might be enough to explain the 100 latitudinal profiles of C2H2 and C2H6. A simple 1-D model in the latitudinal coordinate by 101 Lellouch et al. (2006) shows that the dynamical pictures derived from HCN and CO2 are 102 not consistent with each other, and also not with the C2H2 and C2H6 profiles. Both Liang 103 et al. (2005) and Lellouch et al. (2006) suggested that the horizontal eddy diffusivity is 104 required to vary with latitude and altitude, leading to a more complicated picture. Note 105 that the C2H6 distribution cited in their studies is decreasing from low latitudes to high 106 latitudes. The recent analysis of Cassini and Voyager spectra has revealed more accurate 107 latitudinal profiles of C2H6 (Nixon et al. 2010; Zhang et al. 2012a), which are clearly 108 enhanced in the high latitudes, especially in the Voyager era. One might also use a 109 latitudinally varying vertical eddy diffusivity profile to explain the C2H6 horizontal 110 distribution via changing its vertical slope with latitude (Lellouch et al. 2006). However, 111 this approach might be no different to a parameterization of a realistic horizontal and 112 vertical advection process. Instead, a full CTM is needed to understand the tracer 113 transport in the stratosphere of Jupiter. 114 115 As mentioned above, a very careful treatment in the numerical scheme is necessary in the 116 CTM since the advection terms might lead to less accurate results. Shia et al. (1990) 117 compared different numerical schemes and adopted the modified Prather scheme (Prather 118 1986) in the Caltech/JPL Kinetics CTM. In that paper, the authors derived several 119 analytical solutions to validate the numerical results, in both 1-D and 2-D. But the authors 120 only used the analytic solutions to test the numerical scheme and did not discuss the 121 underlying physical implications of those analytical results. Therefore, some of their 122 analytical results were only mathematically correct but physically counterintuitive (such 123 as the negative chemical production rate, etc.). 4 124 125 On the other hand, the nonlinear feedbacks in the complicated chemical-advective- 126 diffusive system may blur the physical insights. A simple but realistic analytical solution 127 can be considered as a benchmark case for understanding the basic behavior of the 128 system, under idealized assumptions. Previous studies did not focus on the analytical 129 benchmark cases in the atmospheric tracer transport. In civil engineering, the regional 130 Gaussian-plume dispersion models have been studies for many years, and the analytical 131 solutions for the three-dimensional (3-D) diffusion equation could be obtained, although 132 they may not be in the explicit forms (e.g., Lin and Hildemann, 1997). But those 133 solutions are not useful for this study because (1) they are too complicated to show any 134 physical insight; (2) they are restricted to a nonreactive contaminant; and (3) they are not 135 in the planetary scale in which the sphericity of the planet should be taken into account. 136 For the simple planetary-scale analytical solutions, besides Shia et al. (1990), previous 137 attempts mainly focused on the 1-D solutions. Neglecting the chemistry, Chamberlain 138 and Hunten (1987) derived the 1-D analytical solution with an exponential form of eddy 139 and molecular diffusivities. Yelle et al. (2001) reported a 1-D diffusive equilibrium CH4 140 profile, which is essentially a special case of that by Chamberlain and Hunten (1987). A 141 systematic study of the available analytical cases in the planetary chemical-transport 142 system has been lacking. 143 144 In this study we systematically investigate the behavior of the chemical-advective- 145 diffusive system through various representative analytical benchmark cases, such as for 146 the long-lived species versus the short-lived species. Those analytical formulas will be 147 used to validate the numerical simulations in which the numerical schemes are usually 148 not trivial. We will focus on the hydrocarbons in the stratosphere of Jupiter because the 149 observations of C2H2 and C2H6 show a beautiful example of the tracer transport systems. 150 In order to derive the analytical formulas, we need to make some simplifying 151 assumptions; therefore, we will leave the detailed numerical modeling with realistic 152 hydrocarbon chemistry and circulation pattern inferred from the radiative modeling 153 (Zhang et al. 2012a, 2012b) to a future study. Finally, our results could be applied to 154 other planetary and exoplanetary atmospheres. 5 155 156 This paper is structured as follows. In section 2, we will introduce the chemical- 157 advective-diffusive equation. In section 3, we will solve the equation in the 1-D system. 158 In sections 4 and 5 we will focus on the 2-D systems in the meridional plane and zonal 159 plane, respectively, followed by a summary in section 6. 160 161 2. THE NATURE OF THE PROBLEM 162 163 Let us first consider a chemical system in a fast rotating atmosphere. Every quantity can 164 be zonally averaged. We adopt the Transformed Eulerian Mean (TEM) formulation 165 (Andrews et al. 1987, hereafter AHL1987) here. Chemical species are transported 166 vertically and meridionally by the residue mean circulation driven by the diabatic 167 circulation, with a vertical effective transport velocity π€ and a meridional effective 168 transport velocity π£. We also parameterize the eddy transport in a “diffusion” tensor that 169 governs the tracer mixing processes both vertically and meridionally (See AHL1987, 170 p.354). In the region above the homopause, species with different mass would separate 171 from each other by molecular diffusion. 172 173 We adopt a vertical coordinate π§ = π» ππ(ππ /π) , where π is pressure and ππ is the 174 reference pressure, which is usually taken to be 1 bar for giant planets. π» is the pressure 175 scale height of the background atmosphere. The meridonal coordinate is π¦ = ππ, where π 176 is planetary radius, and π is the latitude. We further define a dimensionless coordinate 177 π = π§/π». The volume mixing ratio of gas (or tracer) π is π = ππ /π, where ππ and π are 178 the concentrations of gas and background atmosphere, respectively. Below the 179 homopause, the full form of zonal-averaged Eulerian mean transport equation for 2-D 180 chemical system is (Shia et al. 1990) 181 ππ ππ ππ 1 π ππ π ππ π−πΏ +π£ +π€ − (πππ π πΎπ¦π¦ ) − π π (π −π πΎπ§π§ ) = . ππ‘ ππ¦ ππ§ πππ π ππ¦ ππ¦ ππ§ ππ§ π 182 where π and πΏ are the chemical source and loss terms, respectively. Here we use only the 183 diagonal term of the diffusion tensor πΎ. This is particularly an advantage of the TEM 184 formulism since the diabatic circulation has already taken into account the y-z direction 6 (1) 185 transport so that we can neglect the πΎπ¦π§ and πΎπ§π¦ terms (AHL 1987, p.380). Above the 186 homopause, strictly speaking, we should also consider the molecular diffusion. However, 187 the transport by the residue circulation is usually more effective in the region where eddy 188 mixing dominates, so we just simply neglect it above the homopause in the 2-D systems. 189 We will consider molecular diffusion in the 1-D system (section 3). 190 191 For the numerical simulation, we use the Caltech/JPL kinetics model. The 1-D model is 192 taken from the state-of-the-art chemical schemes for Jovian stratosphere from Moses et 193 al. (2005). The model integrates the continuity equation including chemistry and vertical 194 diffusion using a matrix inversion method (Allen et al. 1981). We simplify the Moses et 195 al. (2005) model by assuming an isothermal atmosphere and using a simplified molecular 196 and eddy diffusivity profiles, with the chemistry only including the C2 hydrocarbons. 197 This idealized model is indeed very close to the full chemistry model. Fig. 1 shows the 198 numerical results compare with the full chemistry model from Moses (2005), a reduced 199 C2 chemistry model with realistic chemistry and diffusivity, and our idealized model. The 200 idealized model we introduced above agrees well with the full chemistry model. The 201 simplified eddy diffusivity and molecular diffusivity are shown in Fig. 2. For the 2-D 202 simulations in the meridional plane, we adopt the numerical model from Shia et al. 203 (1990) for a single tracer. The details will be referred to section 4. 204 205 3. 1-D SYSTEM 206 207 Consider a 1-D chemical-transport system in the vertical coordinate in the global-average 208 sense. Above the homopause, the vertical diffusive flux ππ§ = ππΎπ§π§ ππ/ππ§ needs to be 209 modified to include moleculardiffusion 210 ππ§ = ππΎπ§π§ π(ππ /πππ,π ) ππ + ππ·π , ππ§ ππ§ (2) 211 where π·π is the molecular diffusivity for gas component π in the background atmosphere, 212 πππ,π is the equilibrium density profile with the scale height of species π. After some 213 manipulation, the continuity equation becomes 214 ππ ππ π ππ ππ·π π−πΏ +π€ − π π {π −π [(πΎπ§π§ + π·π ) + π]} = . ππ‘ ππ§ ππ§ ππ§ π» π 7 (3) 215 where π = ππ /π − 1 , ππ and π are the molecular mass of the species π and the 216 background atmosphere, respectively. In order to derive analytical solutions, we assume 217 some forms for eddy diffusivity and molecular diffusivity. Lindzen (1981) proposed a 218 wave-breaking turbulent mixing diffusivity, which satisfies πΎπ§π§ ∝ π −1/2 . The binary 219 molecular diffusion theory implies π·π ∝ π −1 (Chamberlain and Hunten, 1987). 220 Therefore, in this study we assume πΎπ§π§ = πΎ0 π πΎπ and π·π = π·0 π π . 221 222 For an isothermal atmosphere which approximates Jovian stratosphere, we have π = 223 π0 π −π . For the chemical production and loss terms, we assume π = π0 π0 π πΌπ , and πΏ = 224 πΏ0 πππ½π π=πΏ0 π0 π (π½−1)π π. For a nondivergent flow we take π€ = π€0 π π ∝ π −1 . For steady 225 state with ππ/ππ‘ = 0 in the vertical coordinate π, equation (3) becomes 226 [π·0 +πΎ0 π (πΎ−1)π ] 227 + π0 π» 2 π πΌπ = 0. 228 Equation (4) is the governing equation for the 1-D chemical-advective-diffusive system. 229 There is no general solution for this equation except under some specific conditions. If 230 πΎ = π½ = 1, we could obtain an analytical solution by following the derivation of Shia et 231 al. (1990). If π½ = 1 and π0 = 0 , there could be a solution expressed by the 232 hypergeometric functions. Alternatively, in our idealized model, we consider the cases 233 with πΎ~0.5, which is based on Lindzen’s hypothesis and also approximates the situation 234 in Jovian stratosphere (Moses et al. 2005). For Jupiter, we take π0 = 150πΎ , π» = 235 24.1 ππ , πΎ0 ~280 ππ2 π −1 , and π·0 ~0.04 ππ2 π −1 for CH4 and 0.03 ππ2 π −1 for C2H2 236 and C2H6 (scaled by the square root of molecular mass). Again, the results from this 237 idealized model are very close to those from the state-of-art Jupiter model (Moses et al. 238 2005), as shown in Fig. 1. π2π ππ + [ππ·0 − π€0 π»+πΎ0 (πΎ − 1)π (πΎ−1)π ] − πΏ0 π» 2 π (π½−1)π π 2 ππ ππ (4) 239 240 In principle, it is not proper to include vertical wind in the 1-D model because it will go 241 to infinity when the atmospheric density drops to zero at the top boundary. However, if 242 we artificially add wind in the 1-D case, it is also useful to roughly estimate the effect of 243 vertical transport in the 2-D case. Therefore, we derived the solutions for both wind-free 244 ( π€0 = 0) and wind cases ( π€0 ≠ 0 ). The solutions of the 1-D chemical system are 8 245 summarized in Table 1. The detailed derivations can be found in Zhang (2012, Chapter 246 V, PhD thesis). 247 248 3.1 Cases without Wind 249 250 If we set π€0 = 0, the stratosphere of Jupiter can be approximated in a global-average 251 sense. Three typical cases are used to explain the distributions of CH4, C2H6 and C2H2 in 252 the Jovian stratosphere. 253 254 3.1.1 CH4 255 256 CH4 is transported upward from the interior. If we neglect photolysis, CH4 will be 257 governed by the diffusion equilibrium, corresponding to the case I in Table 1. This is 258 generally true because the strong self-shielding effect will limit its photolysis efficiency 259 below some pressure level. The upward flux is on the order of 109 ππ2 π −1 , so πΉπ»/ 260 ππ0 π·0 is ~10−5. Compared with the CH4 mixing ratio in the deep interior, determined by 261 the thermochemistry (π0 ~1.8 × 10−3 ), the flux term can be ignored. Rewrite the solution 262 as π π·0 π (1−πΎ)π +πΎ0 πΎ−1 π(π) = π0 ( ) . π·0 +πΎ0 263 (5) 264 Fig. 3 shows the profile for CH4 (π~6). We can see that the analytical solution matches 265 the numerical model very well; in the lower atmosphere, where π·0 βͺ πΎ0, it behaves as a 266 constant mixing ratio profile; and in the upper atmosphere, where π·0 β« πΎ0 and the 267 pressure π ∝ π −π , it behaves as π ∝ π π . 268 269 3.1.2 C2H6 270 271 On the other hand, Jupiter’s C2H6 is formed around the homopause region and 272 transported downward. Therefore the flux term cannot be ignored. Interestingly, the flux 273 is also on the order of 109 ππ2 π −1, so πΉπ»/ππ0 π·0 is ~10−5 . For C2H6, π~12. Since the 9 274 source of C2H6 is in the upper atmosphere, we can set the lower boundary condition as 275 π0 = 0, so the solution becomes π 276 πΉπ» π·0 π (1−πΎ)π +πΎ0 πΎ−1 π(π) = [1 − ( ) ]. ππ0 π·0 π·0 +πΎ0 277 Fig. 4 shows that the analytical solution matches the model result very well below the 278 homopause. In the lower atmosphere, where π·0 βͺ πΎ0 , we take the Taylor expansion of 279 the solution and obtain πΉπ»(π (1−πΎ)π − 1) π(π, π·0 βͺ πΎ0 ) = , πΎ0 π0 (1 − πΎ) 280 (6) (7) 281 which is consistent with the solution with π·0 = 0 (case II). The solution implies that the 282 C2H6 mixing ratio profile should asymptotically behave as π ∝ π(πΎ−1) (Fig. 4). 283 284 Above the source region the flux changes sign (upward), but since the flux drops fast, we 285 can still ignore it, and the following analytical solution still matches the model result 286 well, similar to the condition of CH4. Let πΉ = 0 in the solution of case I and note that at 287 the homopause π·0 π (1−πΎ)π = πΎ0 , π π·0 π (1−πΎ)π +πΎ0 πΎ−1 π(π) = πβ [ ] , 2πΎ0 288 289 (8) where πβ is the volume mixing ratio at the homopause. 290 291 Therefore, we conclude that in the Jovian stratosphere CH4 and C2H6 are mostly in 292 diffusive equilibrium, especially in the region where transport is much faster than the 293 chemical processes. 294 295 3.1.3 C2H2 296 297 Above the homopause, the C2H2 profile can be approximated by the diffusive equilibrium 298 (case I, with πΉ = 0), as we showed for the C2H6 profile above the homopause. It agrees 299 very well with the numerical simulations (Fig. 5). In the eddy diffusion dominated region, 300 the solution of case III is a good approximation for the vertical profile of C2H2. C2H2 is 10 301 transported downward, with a major chemical loss by combining with a hydrogen atom to 302 form C2H3. This is a three-body reaction so the rate is given by πΏ = π[πΆ2 π»2 ][π»]π, where 303 [π»] is the number density of hydrogen atom. In fact the product π[π»]π is approximately 304 constant through the lower region (~108 ππ−3 π −1). Therefore π½ is roughly 0 for C2H2. 305 This is not surprising because the major sources of hydrogen atoms are from (1) C2H2 306 photolysis directly; (2) C2H+H2; (3) C2+H2. Note that the latter two reactions are actually 307 driven by C2H2 photolysis as well. So the production rate of hydrogen atom is 308 proportional to the C2H2 abundance. On the other hand, the loss of hydrogen atom is also 309 through combining with C2H2 and C2H3, these reaction rates are also roughly 310 proportional to C2H2 and background atmospheric abundance. Therefore by equating the 311 sources and sinks of the hydrogen atom, the product π[π»]π can be expressed in terms of 312 several reaction constants and therefore is roughly a constant. 313 314 In the solution of case III, we assume π½~0 and πΏ0 ~π[π»]π~108 ππ−3 π −1, and we obtain 315 2π»√πΏ0 /πΎ0 ~30. We have to ignore the πΌπ term because the π(π) is expected to increase 316 with altitude for the source region above. In this case, we have π = |π½−πΎ| = 1. $$$ The 317 analytical C2H2 profile, as shown in Fig. 5, is 318 π(π) = πΆ1 π 1−πΎ (1−πΎ)π 2π»√πΏ0 /πΎ0 (π½−πΎ)π 2 πΎπ ( π 2 ) |π½ − πΎ| π π = πΆ1 π 4 πΎ1 (15π 4 ), (9) 319 The profile qualitatively agrees with the model result, although not good as the CH4 and 320 C2H6 cases in section 3.1.1 because we simplified the chemistry. But we conclude that 321 the C2H2 profile on Jupiter can be approximated by the modified Bessel function πΎπ . 322 323 3.2 Cases with Wind 324 π€0 π» 325 If we define a new “mass factor” π ∗ = π − 326 free case that we discussed in Section 3.1. The physical meaning of the correct factor 327 π€0 π»/π·0 is the ratio of molecular diffusive timescale to the vertical advection time scale. 328 Naively we can imagine an upward wind tends to make the gas molecule “lighter,” while 329 a downward wind will make the species “heavier.” This result can be directly applied to π·0 11 , equation (7) will be reduced to the wind- 330 CH4, as shown in Fig. 6, with π€0 = ±5 × 10−8 ππ π −1 . Since it is not proper to put the 331 wind into numerical simulations, as it will cause numerical problems. We only show the 332 analytical solutions for qualitative illustration. The results show that the upward wind 333 will lift up the homopause and downward wind will push it down. It actually transports 334 the more (less) abundant species from below (above) and thus increases (decreases) the 335 mixing ratio of CH4. 336 337 Since in the 2-D simulation we generally care about is the region below the homopause 338 and also most of the latitudinal observations are located around 1 mbar or below for 339 Jupiter, we present solutions with only eddy diffusivity and wind transport. If we neglect 340 the chemical production and loss terms, the solution (case VII) would have a different 341 slope from the solutions in the wind-free cases. The solution depends on the ratio of 342 diffusion timescale to the advection timescale, π€0 π»/πΎ0 . Fig. 7 shows two typical vertical 343 profiles of C2H6, with an upward wind and downward wind (~π€0 = ±1 × 10−6 ππ π −1 ) 344 respectively, compared with the wind-free theoretical curve. It shows an upward wind 345 will increase the mixing ratio in the higher altitude by preventing it from being 346 transported downward but a downward wind tends to lower down the mixing ratio of 347 C2H6. Therefore, if we neglect the horizontal transport, the rising air at the equator and 348 sinking air at the poles will result in more C2H6 at equator and less C2H6 at poles, which 349 is opposite to the CIRS measurements (Zhang 2012). $$$ zhang 2012 is Thesis $$$ That 350 suggests the horizontal transport is actually important and a “pseudo-2D” photochemical 351 model is not sufficient to explain the observations. When we add the chemical 352 source/loss, the equation cannot be solved analytically in general, unless we neglect the 353 eddy diffusion term and assume πΌ = π½ − 1 and π½ ≠ 0, the solution is shown in case VIII 354 in Table 1. 355 356 4. 2-D SYSTEM IN THE MERIDIONAL PLANE 357 358 Consider a 2-D chemical-advective-diffusive system below the homopause in the 359 latitudinal and vertical coordinate. We still assume the atmosphere to be isothermal and 360 barotropic. From previous experience, we note that the equation with eddy diffusion 12 361 (πΎ~0.5), advection and chemistry all together cannot be solved analytically, even in the 362 1-D case. Therefore we are trying to decouple the processes. We need to introduce the 363 streamfunction π so that 364 π£=− 365 1 π π π (π −π π), cos π ππ§ 1 ππ π€= . cos π ππ¦ (10π) (10π) 366 367 4.1 Without Chemistry, π·π = π³π = π 368 369 370 If the chemistry can be ignored, the steady state of equation (1) becomes π£ ππ ππ 1 π ππ π ππ +π€ − (cos π πΎπ¦π¦ ) − π π (π −π πΎπ§π§ ) = 0. ππ¦ ππ§ cos π ππ¦ ππ¦ ππ§ ππ§ (11) 371 If we also neglect the eddy diffusion term, the solution would be trivial: for any given 372 streamfunction π, the solution is π(π, π) = πΊ(π −π π(π, π)), where πΊ is any functional 373 form determined by the boundary conditions and π −π π is the mass-weighted 374 streamfunction. On the other hand, by ignoring the advection term, we have a 2-D 375 diffusion equation. But this solution will be trivial too because there is no horizontal 376 diffusion flux without chemical source. It will be reduced to the 1-D case. 377 378 4.2 With Chemistry 379 380 Let us introduce the chemistry. The source and sink terms are parameterized as: 381 π(π, π) = π0 π0 π πΌπ π(π) , and πΏ(π, π) = πΏ0 πππ½π π(π)π = πΏ0 π0 π (π½−1)π π(π)π . The 382 chemical sourc function, π(π) is more likely to be symmetric with latitude for Jupiter 383 (obliquity is almost zero), for example, π(π)~(cos π)π . 384 385 4.2.1 Pure Advection Cases 386 387 The general approach to solve the pure advection 2-D cases is discussed in Appendix A. 388 We introduced two typical circulation patterns: (1) an axis-symmetric equator-to-pole 13 389 circulation pattern in each hemisphere, called ππ΄ , and (2) a pole-to-pole circulation 390 pattern in the entire hemisphere, called ππ΅ . The solutions are summarized in Table 2. 391 392 We now test our numerical model against analytical solutions. The numerical model has 393 dimensions 80×33, with 80 pressure grid points from 100 mbar to 5 mbar, and 33 394 latitudes from 85°S to 85°N with increments of 5°. Two numerical schemes are tested. In 395 the first scheme, called the “normal 2-D” mode, the photochemistry, diffusion, and 396 advection are solved together using a time-marching method (Shia et al. 1990). In the 397 second scheme, called the “quasi 2-D” mode (Liang et al. 2005), first we perform a series 398 of 1-D chemical-diffusive calculations at different latitudes using the matrix inversion 399 method (see Section 3), and then the meridional advection and horizontal diffusion are 400 applied to connect different latitudes. Our calculations show that, when reaching the 401 steady state, the two modes converge in the same solution. But the “quasi 2-D” mode 402 takes shorter time to reach the steady state than the “normal 2-D” mode, because the 403 former allows very large time step in the 1-D diffusion calculation but the latter is limited 404 by the CFL criterion for every time step. 405 406 We assume the Jupiter value π0 = 4.83 × 1018 π ππ−3 at 100 mbar, and planetary 407 radius π = 7.1824 × 109 ππ . We assume π0 = 10−16 ππ−3 π −1 , π€0 = 10−3 ππ π −1 , 408 π» = 2.5 × 105 ππ, and π = 0.3. So the transport timescale is about 3 × 109 π . For each 409 circulation pattern, we tested two fictitious chemical tracers, the short-lived tracer with 410 9 loss rate faster than transport (πΏ−1 0 = 10 π ) and the long-lived tracer with loss rate 411 11 slower than transport (πΏ−1 π ). 0 = 10 412 413 In the case of Jupiter with nearly no obliquity, we hypothesize the circulation pattern to 414 be axis-symmetric (ππ΄ ), in which air rises at the equator and sinks at the poles, our 415 analytical solution is given in case IX, with πΊ(π −π π) = 5 × 10−19 (π −π π) . For the 416 other circulation pattern, which might be relevant to the planets with large obliquity, such 417 as Earth or Titan, air rises at the south pole and sinks at the north pole, and our analytical 418 solution is given in case X, with πΊ(π −π π) = −0.26(π −π π) 2 14 −1 . We use the boundary 419 values from the analytical solutions for the numerical model. The mass stream functions 420 (scaled by the air density for each layer) are shown in Figs. 8 and 9, respectively. 421 422 The results from case IX are plotted in Fig. 8, with the numerical simulation results (dots) 423 on top of each curve. For the short-lived tracer, chemical production and loss dominates 424 its local abundances. Because the production is higher at equator and loss is higher at the 425 poles, the steady-state mixing ratio of the short-lived tracer is higher in the low latitudes 426 and lower in the high latitudes in the upper pressure levels (~5-10 mbar), while in the 427 lower pressure levels (~50-100 mbar), its latitudinal distribution is also affected by the 428 lower boundary conditions. On the other hand, although with the production and loss rate, 429 the latitudinal distribution of the long-lived species has the opposite trend as the short- 430 lived species, with higher mixing ratio in the higher latitudes and lower mixing ratio in 431 the lower latitudes in the upper pressure levels, showing the transport dominant results. In 432 the lower pressure levels, the solutions are also affected by the lower boundary 433 conditions. The numerical results are based on our 2-D CTM (Caltech/JPL Kinetics 434 Model), which is able to reproduce the analytical results almost perfectly. The largest 435 differences between the analytical and numerical simulations are found in two poles, but 436 still less than 4%. Case IX qualitatively interprets the opposite latitudinal distributions 437 between C2H2 (a short-live species) and C2H6 (a long-lived species), as revealed by the 438 Cassini and Voyager spectra (Nixon et al. 2010; Zhang et al. 2012a). 439 440 Similar behavior is revealed by the results from case X (Fig. 9). Although both tracers 441 have higher production rate in the southern hemisphere and linear loss rate coefficient 442 independent of latitude, their steady-state latitudinal distributions are significantly 443 different. Again, the short-lived tracer is dominated by the chemistry, while the long- 444 lived tracer shows transport-dominant behavior. 445 446 4.2.3 Pure Diffusive Cases 447 448 Ignoring the advection terms, we now have a 2-D diffusion equation 15 449 1 π ππ ππ π ππ (cos π πΎπ¦π¦ ) + 2 (πΎ0 π (πΎ−1)π ) + π0 π (πΌ+1)π π(π) − πΏ0 π π½π π(π)π 2 π cos π ππ ππ π» ππ ππ 450 = 0. (13) 451 452 Generally there is no analytical solution for this equation. If we further assume the 453 solution of the 2-D diffusion equation can be expressed as: π(π, π) = π΄(π)πΊ(π), and let 454 πΊ(π) = πΆ1 π (1−πΎ)π , πΌ = −πΎ, and π½ = 0, the solutions for the pure diffusion 2-D cases are 455 discussed in Appendix B. Four typical cases are summarized in Table 3. In the numerical 456 11 simulations, we assume π0 = 10−16 ππ−3 π −1 , πΏ−1 0 = 10 π , πΎ = 0.1 . The results are 457 plotted in Fig. 10. 458 459 In case XI, we assume the production rate is uniform at the top and a linear loss rate. 460 πΆ1 = 0 in the solution leads to a trivial case with a constant mixing ratio with latitude. If 461 πΆ1 ≠ 0, the solution will end up with a horizontal diffusional equilibrium solution. We 462 assume πΎπ¦π¦ = 2.1 × 109 ππ2 π −1 in the numerical simulations. The solution shows a 463 bowl-shaped distribution with a minimum value at the equator and maximum value at the 464 poles (Fig. 10). So the horizontal flux is from pole to equator. At any latitude there 465 should be a flux convergence to balance the chemical loss. And the area weighted loss 466 rate has a maximum at equator, therefore a maximum flux convergence as well. 467 468 If the production rate is not uniform at the top and there is no chemical loss, the analytical 469 solutions for case XII (π = 0) and case XIII (π = 1) exist. In the numerical simulations, 470 we assume πΎπ¦π¦ = 1 × 109 ππ2 π −1 . The solutions show an upside-down bowl-shaped 471 distribution with the maximum value at the equator and a sharp falloff in the polar region 472 (Fig. 10). So the horizontal flux is from equator to pole. Since there is no chemical loss in 473 these cases, at any latitude there should be a flux divergence to balance the chemical 474 production. The solutions demonstrate that, if the chemical loss can be ignored, any 475 diffusive transport process with a chemical production rate that is either flat (π = 0) or 476 peak (π = 1) in the low latitudes will result in a high mixing ratio in the low latitudes. 477 Therefore, the horizontal mixing solution of C2H6, whose chemical loss can be ignored, 478 will have an upside-down bowl shape. Our simple analytical cases are consistent with the 16 479 model results in Liang et al. (2005) and Lellouch et al. (2006), but contrary to the 480 Voyager and Cassini data (Zhang et al. 2012a). We note that the ratio of production rate 481 with the horizontal mixing determines the ‘flatness’ of the bowl-shape distribution. A 482 more efficient horizontal mixing leads to a flatter distribution. The horizontal timescale 483 should be much shorter than the chemical production timescale in the Liang et al. (2005) 484 case, which is correct because in the lower atmosphere chemical production of C 2H6 is 485 not efficient. The observed latitudinal distribution from CIRS implies either the mean 486 residue circulation plays an important role, or there could be a chemical source of C2H6 in 487 the polar regions, although there is no evidence for any possible ion chemistry initiated 488 by precipitating particles in the aurora region that could enhance the ethane abundances. 489 But this possible chemical mechanism should not significantly enhance the abundances 490 of C2H2, which, in principle, is much more sensitive to the local chemical source but the 491 observations do not show any enhancement of C2H2 in the polar region. 492 493 However, the solution (case XIV) also shows a bowl-shaped distribution with the 494 maximum value at the equator and minimum value at the poles (Fig. 10). So if we ignore 495 the advection terms, the required latitudinal slope of the production rate of C2H6 should 496 be much steeper than the sin2 π in order to explain the CIRS observations. Numerical 497 simulations with more realistic chemistry and eddy mixing are needed to confirm this 498 hypothesis. 499 500 5. 2-D SYSTEM IN THE ZONAL PLANE 501 502 If we consider the system in an altitude-longitude plane, which is appropriate for slowly 503 rotating planets such as Venus and hot Jupiters, a strong subsolar-anti-solar circulation 504 coupled with the zonal jets, and with the inhomogeneous production rate, will lead to a 505 different scenario. In the zonal plane, the horizontal eddy diffusion can be neglected. In 506 the steady state, the governing equation is 507 π’ ππ ππ π ππ π−πΏ +π€ − π π (π −π πΎπ§π§ ) = . π ππ ππ§ ππ§ ππ§ π 17 (14) 508 where π is longitude, π is radius of the latitude circle. We can formulate the 509 streamfunction π in the longitude and vertical plane: π −π (π π), ππ§ 1 ππ π€= . π ππ 510 π’ = −π π 511 (15π) (15π) 512 If we neglect the diffusion term, this is basically the same as the 2-D problem in the 513 meridional plane, but without the cos π factor. The solution is related to the subsolar-anti- 514 solar circulation, which is analogous to that in the equator-pole circulation problem (case 515 IX). 516 517 We can also simply solve the problem by neglecting the vertical advection term in 518 equation (14). Suppose a fast jets rapidly flows along the latitude circle with a constant 519 velocity π’, the air mass is approximately conserved in that altitude over a short timescale, 520 such as the four-day zonal wind on Venus and fast zonal jets on hot Jupiters. The vertical 521 profile is modified by the eddy diffusion. As usual, we assume π(π, π) = π0 π0 π πΌπ π(π), 522 πΏ(π, π) = πΏ0 π0 π (π½−1)π π(π)π, and πΎπ§π§ = πΎ0 π πΎπ . Equation (14) becomes 523 π’ ππ π ππ − π π (πΎ0 π (πΎ−1)π ) − π0 π (πΌ+1)π π(π) + πΏ0 π π½π π(π)π = 0. π ππ ππ§ ππ§ 524 Let us check a simple case with a special solution. Similar to the argument of the 2-D 525 diffusive system, we let πΌ = −πΎ and π½ = 0, we assume the solution can be expressed as: 526 π(π, π) = π΄(π)πΊ(π), where πΊ(π) = πΆ1 π (1−πΎ)π . The solution is 527 π(π, π) = e− ππΏ0 π(π)ππ π’ ∫ [πΆ1 + ππΏ0 ππ0 ∫ π(π)e π’ ∫ π(π)ππ ππ] π (1−πΎ)π . π’ (16) (17) 528 The periodic boundary condition, i.e., π(0, π) = π(2π, π), requires πΆ1 to be 0. A simple 529 case would be π(π) = 1 + cos ππ, where π = 1 stands for the two-modal production rate 530 (day-night contrast). The solution would be 531 π(π, π) = π0 1 [1 + cos(ππ − π)]π (1−πΎ)π . 2 πΏ0 √1 + π (18) 532 where the dimensionless variable π = ππ’/ππΏ0 measures chemical loss timescale versus 533 the advection timescale (across an envelope of the production rate distribution). π = 534 tan−1 π can be regarded as the phase lag of the mixing ratio distribution compared with 18 535 the production rate distribution and the amplitude of the mixing ratio variation is smaller 536 than the production rate variation by a factor of √1 + π 2 . When the advection timescale 537 and the chemical loss timescale are comparable, i.e., π = 1, the phase shift is 45°. If π is 538 large, i.e., when the chemical loss is slower than the advection timescale, the zonal wind 539 will quickly redistribute the chemicals and lead to a large phase lag and smooth the 540 mixing ratio profile in longitude. On the other hand, if π is small, chemistry will 541 dominate the distribution. Therefore the phase lag due to advection would be smaller 542 since the local chemical equilibrium will be established more quickly, leading to a large 543 mixing ratio bulge along the latitude circle. Fig. 11 illustrates some typical results at π = 544 0 for a range of values of π. 545 546 6. CONCLUDING REMARKS 547 548 In this study we systematically investigated the possible analytical benchmark cases in 549 the chemical-advective-diffusive system. Although our solutions are highly idealized, we 550 can still gain physical insights on what control the vertical and latitudinal profiles of the 551 short-lived and long-lived species in the stratosphere of Jupiter. In the 1-D system, we 552 show that CH4 and C2H6 are mainly in diffusive equilibrium, and C2H2 profile can be 553 approximated by the modified Bessel functions. Those analytical solutions could be used 554 for the simple treatment of photochemistry in climate models or general circulation 555 models. In the 2-D system in the meridional plane, analytical solutions for two typical 556 circulation patterns are derived. Simple tracer transport cases demonstrate that the 557 distribution of short-lived species is dominated by the local chemical sources and sinks, 558 while that of the long-lived species is significantly influenced by the circulation. This 559 may help solve the difference in the latitudinal distribution between C2H2 and C2H6, as 560 revealed by the Cassini and Voyager spectra. On the other hand, it seems difficult for a 561 pure diffusive transport process to produce a similar latitudinal profile of C2H6 whose 562 chemical loss can be neglected. Intuitively it also makes sense because the horizontal 563 eddy mixing is not able to reverse the latitudinal gradient driven by the photochemistry. 564 Therefore, unless there is a missing chemical source for C2H6 (but not for C2H2) in the 565 polar region, the most probable solution is a meridional circulation from equator to pole. 19 566 The detailed structure of the residue circulation in the stratosphere of Jupiter requires a 567 realistic numerical simulation. For the slowly rotating planet, which might have 568 longitudinal heterogeneous chemical sources, the interaction between the advection by 569 the zonal wind and chemistry might cause a phase lag between the final tracer 570 distribution and the original source distribution. The magnitude of the phase lag and 571 longitudinal contrast of the tracer profile depends on the relative strength between the 572 advection timescale and the lifetime of the tracer. This is similar to the mechanism that 573 causes a phase shift between the locations of the atmospheric temperature maximum and 574 sub-solar point (where heating is a maximum) on close-in giant planets (Knutson et al. 575 2007). 576 577 The analytical solutions have been used to validate the numerical simulations from our 2- 578 D Caltech/JPL CTM and show good agreement for various cases. The largest discrepancy 579 usually happens in the polar region, especially when the analytical solutions have 580 singular values at the poles, such as case XI. Increasing the horizontal and vertical 581 resolution would lead to better agreement. This study lays the theoretical basis and 582 numerical tools for future realistic chemistry-transport modeling in planetary and 583 exoplanetary atmospheres. 584 585 586 587 588 589 590 591 592 593 594 595 596 20 597 598 FIGURE CAPTIONS 599 600 Fig. 1. Simulated hydrocarbon profiles from the idealized model, the C2 chemistry model 601 (with realistic eddy and molecular diffusivities as the full chemistry model) and the full 602 chemistry model. 603 604 Fig. 2. Profiles of eddy diffusivity and molecular diffusivity (for CH4) in the idealized 605 model (eddy profile I) compared with the full chemistry models (eddy profile II). The 606 blue curve is the total diffusivity for the idealized model. 607 608 Fig. 3. CH4 from numerical simulations compared with analytical solutions. The dashed 609 lines are asymptotic profiles. 610 611 Fig. 4. C2H6 from numerical simulations compared with analytical solutions. The dashed 612 lines are asymptotic profiles. 613 614 Fig. 5. C2H2 from numerical simulations compared with analytical solutions. The dashed 615 lines are asymptotic profiles. 616 617 Fig. 6. Analytical CH4 profiles from the cases with and without wind. π€0 = 618 ±5 × 10−8 ππ π −1 . 619 620 Fig. 7. Analytical C2H6 profiles from the cases with and without wind. π€0 = 621 ±1 × 10−6 ππ π −1 . The dotted line is with the molecular diffusion in the upper 622 atmosphere. 623 624 Fig. 8. Plots of case IX. Upper panel: Analytic mass stream functions in units of 625 π ππ−1 π −1 . Bottom panel: comparison of analytical (lines) and numerical (dots) 626 solutions for two fictitious chemical tracers, the short-lived tracer (orange) and the long- 21 627 lived tracer (blue). The solid and dashed curves correspond to 5 and 50 mbar, 628 respectively. 629 630 Fig. 9. Plots of case X. Upper panel: Analytic mass stream functions in units of 631 π ππ−1 π −1 . Bottom panel: comparison of analytical (lines) and numerical (dots) 632 solutions for two fictitious chemical tracers, the short-lived tracer (orange) and the long- 633 lived tracer (blue). The solid and dashed curves correspond to 5 and 50 mbar, 634 respectively. 635 636 Fig. 10. 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