Chapter 5 Lake Breeze and Oxidants Over South-Eastern Ontario Due to the thermal inertia of large bodies of water, lakes (or oceans) warm and cool considerably slower than the adjacent land surfaces. On days with limited cloud cover, solar radiation warms land surfaces more rapidly than the lake surface and a temperature dierential between the land and lake surfaces develops. The dierence in temperature between the land and the lake surfaces results in a dierence in the temperature of the atmosphere above, which results in a slight perturbation to the pressure eld. The response of the wind eld to the temperature-induced perturbations in the pressure eld gives rise to a ow from the lake towards the land at the lowest levels of the atmosphere, and a corresponding return ow, from the land towards the lake, aloft. At a certain distance inland, the onshore ow in the lowest levels of the atmosphere rises and return towards the lake as part of the oshore ow aloft, forming the lake breeze front (Simpson, 1977). Interest in the inuence of lake breeze circulations on air quality in the Great Lakes region has existed for more than 20 years. Observations in the early 1970's 189 along the western shore of Lake Michigan found that high concentrations of ozone observed at ground-level were associated with southeasterly or onshore ow as a result of a lake breeze circulation (Lyons and Cole, 1973 1976). Lake breeze or sea breeze circulations have also been found to have signicant eects on air quality along the shore of Lake Erie in southwestern Ontario (Mukammal et al., 1982), in Los Angeles, California (Lu and Turco, 1996), Athens, Greece (Lalas et al., 1983) and along the Mediterranean coast of Spain (Martin et al., 1991 Millan et al., 1996). The eects of lake and sea breeze circulations on air quality have been investigated for a variety of locations with diering topography and meteorology. For example, a modelling study by Lu and Turco (1996) of the eects of a sea breeze circulation on air quality in Los Angeles has shown that the sea breeze can bring relatively unpolluted air inland. The onshore ow of the sea breeze becomes progressively more polluted as the airmass moves over regions with large anthropogenic emissions of hydrocarbons and NOx, while vertical motions at the sea breeze front act to lift ozone and other pollutants and result in layers with higher concentrations of oxidants aloft. These elevated layers of high concentrations of oxidants may be mixed down to the surface the following day. For the case of the interaction of emissions from Toronto with a lake breeze over Lake Ontario, the most applicable study is that performed by Lyons and Cole (1976). They studied the eects of a lake breeze circulation over Lake Michigan on emissions from Chicago and surrounding regions. Observations of the ground-level ozone concentration along the western shore of Lake Michigan showed that under conditions of onshore ow during a lake breeze, ozone concentrations were highest from 1 { 8 kilometres inland from the lakeshore. Ozone concentrations were lower within one 190 kilometre of the lakeshore and also decreased at distances greater than 10 km inland from the lakeshore. To explain the observations which showed the highest ozone concentrations occurring several kilometres inland from the lakeshore, Lyons and Cole suggested that the bulk of the ozone, while over the lake, resides above the conduction inversion. As the airmass is advected onshore, locations near the shoreline are exposed to the less polluted air which was found within the lowest layers of the atmosphere over the lake. As the airmass moves further inland, the thermal internal boundary layer (TIBL) rapidly deepens and the ozone aloft is eventually mixed down to the ground resulting in the higher ground-level concentrations observed just inland of the shoreline. Still further inland, ground-level ozone concentrations decrease due to the continued deepening of the TIBL and loss processes which act on ozone such as dry deposition and titration by freshly emitted NO. Lyons and Cole (1976) proposed that the generation of elevated layers of high ozone concentrations over the lake were the result of the advection of VOCs and NOx out over the lake by the gradient ow or a land-breeze circulation during the early morning. The ozone precursors, released as the nocturnal inversion is breaking down but before the boundary layer has reached its full depth, will ow up and over the conduction inversion present over the lake, leaving the air within the lowest 100 { 150 m of the atmosphere less polluted. With limited vertical mixing over the lake, the VOCs and NOx will remain trapped aloft and during the afternoon ozone will be photochemically produced. Since the ozone is physically separated from the surface, dry deposition will not act to reduce ozone concentrations appreciably. With light gradient winds, a lake breeze develops later in the day and the ozone which had 191 formed over the lake is advected onshore and mixed down to the surface as described above. From an analysis of tetroon ights, Lyons and Cole suggested that recirculation of pollutants in the lake breeze may be a possibility. Pollution advected inland by the onshore ow of the lake breeze could move inland to the lake breeze front, rise, and return towards the lake in the return circulation aloft. Eventually, the pollutants could reenter the onshore ow of the lake breeze and return to land. In this manner, pollutants could be advected along the western shore of Lake Michigan in a broad helical trajectory by a combination of the lake breeze circulation and the gradient wind. A modelling study using the Regional Atmospheric Modeling System (RAMS) in conjunction with a Lagrangian particle dispersion model (Lyons et al., 1995) has reproduced the recirculation phenomenon described by Lyons and Cole (1976), though only approximately 30% of the particles were predicted to reenter the onshore ow and complete a full recirculation. Sillman et al. (1993) have shown that the suppression of vertical mixing and the extremely slow rate of dry deposition of ozone and NOx species over a large body of water is sucient to allow very high concentrations of ozone to be photochemically generated over Lake Michigan. The model meteorology used by Sillman et al. did not include a representation of the lake breeze, though advection of the Chicago urban plume over Lake Michigan, particularly early in the morning before turbulent mixing over land had distributed the precursors over a deeper layer, and the combination of slow rates of vertical mixing and dry deposition were sucient for the model to calculate high concentrations of ozone in a shallow layer over the lake. Therefore it appears that a lake breeze circulation need not necessarily be present for high 192 concentrations of ozone to be generated over large bodies of water, though lake breeze circulations will be important in controlling the dispersion of pollutants over the lake. The motivation for a modelling study of the lake breeze eects on oxidants over Lake Ontario was provided by observations made as part of the SONTOS study during the summers of 1992 and 1993. Figure 5.1 shows the concentration of ozone and NOy measured at the Hastings site on August 26, 1993 (D. R. Hastie, private communication). With the exception of a brief period at approximately 1830 GMT, the concentration of ozone was observed to slowly increase during the afternoon. Between 2040 GMT and 2120 GMT (16:40 and 17:20 EDT) ozone concentrations increased from 46 ppb to 74 ppb and NOy concentrations increased from 2.2 ppb to 4.0 ppb. Concurrent with the increase in concentration of ozone and NOy , the concentration of NOx, CO, SO2 , PAN and HCHO were also observed to increase. Figure 5.1: The concentration of (a) ozone and (b) NOy as observed at the Hastings measurement site from 0600 GMT, August 26 to 0600 GMT, August 27, 1993. 193 Meteorological parameters measured at the Hastings site showed that a decrease in the dry bulb temperature of 2.5 C and an increase in the specic humidity by 20% was associated with the change in trace species concentrations noted above. The change in meteorological parameters shows that the polluted airmass was cooler and more moist than the less polluted airmass it replaced, suggesting that the more polluted airmass had been modied through contact with a large body of water. It was also possible to identify portions of the lake breeze front on visible satellite imagery for August 26, as it appeared to be marked by a line of broken cumulus clouds. An analysis of the visibly satellite imagery shows that the lake breeze front passed over the Hastings measurement site between 2000 and 2200 GMT (Hastie et al., 1998). Eppley radiometer measurements showed a brief decrease in solar radiation as the chemical and meteorological measruments recorded the change in airmass, presumably as a result of clouds associated with the lake breeze front. Taken together, the meteorological and chemical measurements made at the Hastings site, as well as the position and inland progress of the lake breeze front deduced from satellite imagery, suggest that a lake breeze circulation brought a more polluted airmass north from Lake Ontario to the Hastings measurement site. Given that a westerly to southwesterly gradient ow existed across southern Ontario on August 26, it seems probable that the polluted airmass observed at Hastings originated from Toronto and surrounding urbanized regions around the western end of Lake Ontario. It is hypothesized that, in a situation similar to that described by Lyons and Cole (1976) for the western shoreline of Lake Michigan, VOCs and NOx emitted from Toronto during the early morning are advected over Lake Ontario by the existing gradient ow, possibly aided by a land breeze circulation. During the day, with little 194 vertical mixing and small rates of dry deposition, the photochemical production of ozone gives rise to high concentrations of ozone over the lake which are advected inland by the lake breeze circulation later in the afternoon. Behaviour of chemical and meteorological variables similar to that seen on August 26 was observed on three additional days during the six week intensive measurement campaign in 1993. Given that Hastings is 40 km north of the Lake Ontario shoreline, it appears that lake breeze circulations can signicantly, and regularly, aect air quality along the northern shore of Lake Ontario for a considerable distance inland. Further, since lake breeze circulations over the Great Lakes have been found to occur on 25 { 40% of days during the summer (Comer and McKendry, 1993 Chermack, 1986 Lyons et al., 1972), it seems likely that the inuence of lake breeze circulations on air quality for sites nearer the Lake Ontario shoreline is more frequent than that observed at Hastings. The MC2-online model had been used to test the hypothesis that high concentrations of ozone are generated over Lake Ontario and advected inland by the onshore ow of a lake breeze. The model has been run for two cases in 1993 for which a rapid increase in the concentration of ozone and related trace species were observed to occur at the Hastings site late in the afternoon. The objectives of the modelling study are twofold: 1) to see whether the model qualitatively agrees with the hypothesized mechanism by which high concentrations of oxidants are produced over Lake Ontario and consequently advected northward by the lake breeze and 2) to assess to what degree the model quantitatively agrees with the observed meteorological and chemical elds. 195 5.1 Method The two cases which have been selected for the modelling study are August 8 and 26, 1993. For both study cases an initial run of MC2 without chemistry was performed at a horizontal resolution of 42 km using CMC objective analysis to provide the meteorological boundary conditions. Unfortunately, regional objective analyses in sigma coordinates were not available for these days and it was necessary to use a coarser resolution global analysis in pressure coordinates. The global analysis has a horizontal resolution of 1.5 by 1.5 . The 42 km resolution run was made on the standard 42 km resolution domain discussed in Chapter 2, and used nudging to limit the growth of errors in the synoptic scale features. The run was three days and three hours long, begun at 0000 GMT, two days before the study day and ending at 0300 GMT on the day after the study day. A 21 km horizontal resolution run of MC2 with chemistry was made using meteorological boundary conditions interpolated from the previously completed 42 km resolution run. Initial conditions and time-varying boundary conditions for the advected chemical species were taken from the global CTM as described in Chapter 2. The 21 km resolution run began and ended at the same times as the 42 km resolution run. The nal run of the MC2-online model was made at a horizontal resolution of 5.292 km on an 83 83 grid point domain centered over Lake Ontario. The run was 27 hours long, beginning at 0000 GMT on the study day, and used initial and boundary conditions for the meteorological and chemical variables interpolated from the 21 km horizontal resolution run. Meteorological and chemical boundary conditions 196 were updated every three hours, with linear interpolation used to derive boundary conditions at intermediate times. 5.2 Case Study: August 8, 1993 The rst case chosen for study occurred on August 8, 1993. The concentrations of ozone and NOy as observed at the Hastings eld measurement site are given in Figure 5.2. The observations show that within 15 minutes, beginning at 2221 GMT (1821 EDT), the concentration of ozone increased from 47 to 59 ppb and the concentration of NOy increased from 2.6 to 4.3 ppb. While the increase in ozone on August 8 was rather modest, the time of day at which the increase occurred and the rapidity of the change were similar to other cases observed at Hastings. Figure 5.2: The concentration of (a) ozone and (b) NOy as observed at the Hastings measurement site from 0600 GMT, August 8 to 0600 GMT, August 9, 1993. 197 Figure 5.3 shows the synoptic conditions for 0000 GMT, August 8 and 0000 GMT, August 9, as taken from the CMC objective analysis. A large area of high pressure covered southern Ontario and much of the northeastern United States on August 8. Winds across southern Ontario were light and from the west. Winds recorded at synoptic observing stations in southern Ontario, though away from Lake Ontario, were generally less than 5 km hr;1 and had variable direction during the afternoon. Daytime high temperatures were between 23 and 25 C. Figure 5.3: Sea-level pressure and 850 mb winds taken from the CMC objective analysis for 0000 GMT August 8, 1993 (panel a) and 0000 GMT August 9, 1993 (panel b). Figure 5.4 shows the model calculated wind eld and CO concentration over the 5.3 km resolution domain at 1100 GMT, or 0700 EDT. The horizontal cross-section shows the CO concentration in the lowest model level, approximately 10 m thick, and the wind at 10 m above the surface. The near-surface winds over the western end of Lake Ontario were generally from the north with speeds between 7 and 12 m s;1. The 198 CO concentration eld, used as a long-lived tracer for anthropogenic emissions, shows that emissions from Toronto were being advected to the south across the western end of Lake Ontario. The vertical cross-section of the CO concentrations shows that the plume of CO from Toronto was conned to within 200 m above the surface of the lake. As shown by the 10 m winds in Figure 5.4, a weak cyclonic circulation was calculated by the model to be centred over the southeastern portion of Lake Ontario. The cyclonic circulation is associated with a weak low pressure system that is, erroneously, calculated by the model to be present over eastern Lake Ontario at this time. Observations show that a weak low pressure system was centered over Lake Michigan at 1200 GMT, August 6, though by 1200 GMT, August 7 the low had substantially lled in. The 42 km resolution run of MC2 more or less correctly captures the behaviour of this centre of low pressure. However, the 21 km resolution run allows the low pressure centre to persist, and as can be seen from the 5.3 km resolution wind elds, the low is placed over the eastern end of Lake Ontario by the model during the early morning of August 8. The increased pressure gradient across southern Ontario due to the low pressure centre over eastern Lake Ontario, leads to the strong northerly gradient ow predicted by the model for the early hours of August 8. Figure 5.5 presents the observed 10 m winds from hourly synoptic observations and the Hastings SONTOS site over southern Ontario. Winds at the surface are generally from the west and windspeeds are low: typically less than 1.5 m s;1 . Though the observations are scarce, there is some evidence of a land breeze circulation with winds owing towards the lake at St. Catherines, Toronto Island and Kingston. Compared with observations, the model calculated wind eld is too strong and has limited the 199 Figure 5.4: Horizontal and vertical cross-sections of the CO concentration and wind eld at 1100 GMT, August 8, 1993 calculated by the model at a horizontal resolution of 5.3 km. The horizontal cross-section shows the CO concentration in the lowest 10 m of the model and winds at 10 m above the surface. The position of the vertical cross-section is given by the thick line drawn across the horizontal cross-section panel. 200 formation of a land breeze circulation. .. . . . . . . . Figure 5.5: The observed wind at 10 m above the ground for 1100 GMT (0700 EDT) on August 8, 1993. The station location is given by the solid dot at the end of each barb. The direction of the wind is given by the direction of the barb and an observation of calm conditions is denoted by an unlled circle. Wind speed is given by the tick marks attached to each barb. Windspeeds less than 1.3 m s;1 are given by a barb with no ticks. Windspeeds between 1.3 and 3.8 m s;1 are denoted by a barb with a half tick mark and windspeeds between 3.8 and 6.4 m s;1 are shown by a barb with a full tick mark. The stations plotted are: 1) Toronto International Airport 2) Toronto Island 3) Peterborough 4) Hastings 5) Waterloo 6) Hamilton 7) St. Catherines 8) Kingston and 9) Ottawa. The wind eld and CO concentration predicted by the model at 1600 GMT on August 8 is given in Figure 5.6. By 1600 GMT the model has begun to produce onshore ow associated with a lake breeze in the lowest layers of the model (panel a). The strong northerly ow across the western end of Lake Ontario has been replaced by light winds which, though not well represented in Figure 5.6, show several poorly dened centres of divergent ow. During the initial development of the lake breeze the gradient ow over the lake weakens for levels less than 200 m above the surface. The eect on precursor emissions 201 Figure 5.6: Horizontal and vertical cross-sections of the model calculated CO concentration and wind eld at 1600 GMT, August 8, 1993. The horizontal cross-sections show these elds at 10 m (panel a) and 435 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. 202 can be seen in the distribution of CO near the surface (panel a). With the weakening of the gradient ow over the lake, precursors emitted from Toronto have become trapped over the lake and have formed a `pool' of precursors over the surface of the lake and below approximately 200 m. With the strengthening of the onshore ow of the lake breeze, the precursors are advected both towards the shore around the western end of Lake Ontario, and in an easterly direction along the long axis of the lake. The onshore ow component of the lake breeze is initially quite shallow and deepens with time. As can be seen in the east{west vertical cross-section of Figure 5.6 (panel a), the advection of precursors towards the east only occurs for levels below approximately 100 m above the surface. The initially shallow onshore components of the lake breeze circulation results in a vertically thin layer of precursors advected towards the east. At greater heights above the surface, shown in panel (b) of Figure 5.6, the direction of the gradient wind has been largely unaected by the lake breeze, and emissions from Toronto are still advected towards the south. The north{south vertical cross-section shown in panel (b) of Figure 5.6 shows that the depth of the Toronto plume decreases towards the south. Portions of the Toronto plume near the southern shore of Lake Ontario had been emitted from Toronto earlier in the morning and were trapped by a shallow boundary layer before being advected over the lake. As the boundary layer increased in depth during the morning, emissions from Toronto were mixed over a deeper and deeper layer before being advected over the lake. The changing vertical depth of the plume over the lake is a reection of the boundary layer depth over Toronto at the time the emissions occurred. The observed 10 m winds at 1600 GMT are shown in Figure 5.7. Away from 203 Lake Ontario the windspeeds were generally less than 2 m s;1 and the winds were from a westerly to northwesterly direction. Formation of a lake breeze over Lake Ontario is evidenced by the onshore ow observed at St. Catherines, Toronto Island and Kingston. The winds observed at Kingston, for example, were from the southwest at 4 m s;1 . . .. . . . . . . . Figure 5.7: The observed wind at 10 m above the ground for 1600 GMT (1200 EDT) on August 8, 1993. A comparison of the model wind elds with observations shows that the model predicts winds inland from Lake Ontario to be from a northerly to northeasterly direction, while observations show winds were from a more westerly direction. Errors in the direction of the gradient wind calculated by the model appear to be largely the result of the erroneous centre of low pressure, positioned just to the southeast of Lake Ontario at 1600 GMT. Eects of the low pressure centre on the model solution decrease with time as the low moves further to the east and the central pressure is calculated by the model to increase. Windspeeds calculated by the model north of Lake Ontario are between 2 and 3 m s;1 and agree reasonably well with the observed 204 windspeeds. Winds observed at Toronto Island were calm or light from the north until 1300 GMT, 0900 EDT. Beginning at 1300 GMT the winds were from the south to southwest at speeds from 1 to 2 m s;1 . Observations at St. Catherines and Kingston show onshore ow beginning an hour later, at 1400 GMT. The MC2 model does not show the onset of an onshore ow until 1600 GMT, and appears to be late in developing a lake breeze circulation on this day. Figure 5.8 shows the model CO concentration and wind elds at 2100 GMT (1700 EDT). The 10 m winds, given in the horizontal cross-section of panel (a), show the development of a mesohigh over the extreme southwestern corner of Lake Ontario. A broad band of southwesterly winds, with speeds between 4 and 6 m s;1 , exist over much of the lake. From the vertical cross-sections shown, the onshore ow of the lake breeze is approximately 300 - 400 m deep at 2100 GMT. The winds at 435 m above the surface, shown in the horizontal cross-section of panel (b), are, therefore, near the top or slightly above the onshore ow of the lake breeze circulation. The `pool' of CO which was present over the western end of Lake Ontario at 1600 GMT, just as the lake breeze was beginning to form, has been dispersed by the strengthening lake breeze circulation. A signicant fraction has been advected inland around the western end of Lake Ontario, while a second portion of the CO has been advected towards the northeast over the lake. The plume of CO advected towards the northeast can be seen in the horizontal cross-section of panel (a) to the southeast of Toronto. Vertically, this plume is less than 100 m thick and is not separated from the surface of the lake. As shown by the north-south vertical cross-section of panel (b), the plume of CO 205 Figure 5.8: Horizontal and vertical cross-sections of the model calculated CO concentration and wind eld at 2100 GMT, August 8, 1993. The horizontal cross-sections show these elds at 10 m (panel a) and 435 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. 206 from Toronto has been undercut by less polluted air within the northward, onshore ow of the lake breeze. The less polluted air originated along the southern shore of Lake Ontario, between 200 and 500 m above the surface. Entrained into the lake breeze as the circulation strengthened between 1600 and 2000 GMT, the less polluted air was advected towards the north and eventually brought to the surface by the subsidence associated with the lake breeze. At this point in time, the bulk of the emissions from Toronto are being forced over top of the onshore ow of the lake-breeze, resulting in the formation of an elevated plume. The model CO and wind elds at 0000 GMT, August 9 are illustrated in Figure 5.9. As above, the CO and wind elds are shown for two horizontal cross-sections, at 10 and 435 m above the surface. Note that the scale used to contour the CO concentration has changed from that used above. The 10 m wind eld shows that the mesohigh remains in the southwest corner of Lake Ontario, with the near-surface component of the lake breeze circulation consisting of a band of southwesterly to westerly winds which cover most of the lake. The onshore ow of the lake breeze is now approximately 500 m deep and the winds at 435 m above the surface (panel b) show a considerable onshore component. One of the dominant features of the CO concentration eld at 10 m is the increase in concentration of CO over regions with high emissions. The nocturnal inversion has begun to form over land and, with slower rates of vertical mixing, the CO concentration rapidly increases for regions where emissions occur. The concentration of CO in the lowest model layer over the western end of Lake Ontario has increased from approximately 140 ppb at 2100 GMT to 180 ppb at 0000 GMT, August 9. The increase is caused by the entrainment of emissions from 207 Figure 5.9: Horizontal and vertical cross-sections of the model calculated CO concentration and wind eld at 0000 GMT, August 9, 1993. The horizontal cross-sections show these elds at 10 m (panel a) and 435 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. 208 Toronto into the return ow of the lake breeze. As was noted above, during the late afternoon emissions from Toronto, advected to the south by the gradient ow, are forced to rise over the onshore ow of the lake breeze. A certain fraction of the emissions that rise over the onshore ow are entrained in the return ow, eventually to enter the onshore ow. The increase in the near-surface CO concentration over the western end of Lake Ontario is caused by this phenomenon. Panel (a) of Figure 5.9 shows a north{south vertical cross-section through a shallow layer with higher concentrations of CO. This shallow plume, calculated by the model to be less than 100 m thick, is being advected inland along the north shore of Lake Ontario by the lake breeze circulation. The plume was originally a portion of the `pool' of CO which formed over the western end of Lake Ontario as the lake breeze circulation was beginning at 1600 GMT. The CO distribution at 435 m above the ground, panel (b) of Figure 5.9, shows the eects of the increasing depth of the lake breeze onshore ow. As was discussed above, at 2100 GMT the onshore ow only weakly aected the wind at 435 m and CO emitted from Toronto was advected to the south, across the lake, in the gradient ow (for the moment we are ignoring the fraction of the plume entrained within the lake breeze circulation). As the lake breeze onshore ow continues to deepen with time, portions of the plume which had been advected to the south, in the gradient ow, are caught in the onshore ow and advected to the northeast. The gradual deepening of the onshore ow appears to result in the entrainment of a signicant amount of ozone precursors into the onshore ow of the lake breeze for situations where the gradient ow advects material from urban areas over the lake. The observed 10 m winds at 0000 GMT, August 9 are shown in Figure 5.10. 209 Winds observed at Toronto Island and St. Catherines were calm, suggesting that the lake breeze circulation had weakened considerably by this time. In fact, observations at St. Catherines show the wind becoming oshore one hour later. . .. . . . . . Figure 5.10: The observed wind at 10 m above the ground for 0000 GMT, August 9, 1993 (2000 EDT, August 8). While observations suggest a weakening of the lake breeze circulation, the model continues to show strong onshore ow associated with the lake breeze at this time. A tendency of models to be too slow in terminating onshore ow was noted by Lyons et al. (1995), where it was found that the termination of onshore ow predicted by RAMS, for a case study over Lake Michigan, was as much as 3.5 hours later than observed. The observed winds at Peterborough changed from northwesterly at 2200 GMT to southwesterly at 2300 GMT. The change in wind direction observed at Peterborough occurred at approximately the same time as the putative lake breeze front was observed to arrive at Hastings, 30 km to the west of Peterborough. The observed surface winds at Peterborough and the observed chemical and meteorological variables 210 at Hastings suggest that the lake breeze front had penetrated at least 40 km to the north of the Lake Ontario shoreline by 2300 GMT. From Figure 5.9, it can be seen that the inland penetration of the lake breeze is signicantly underpredicted by the model for this day. The model lake breeze never penetrates far enough inland to arrive at the Hastings eld measurement site. At its closest, the model lake breeze front is approximately 20 km south of Hastings. As was discussed earlier, the incorrect treatment of a low pressure centre contributed to the model calculating a northerly gradient ow, during the early morning hours, that was stronger than observed. Later in the period the inuence of the low pressure system on the 5.3 km resolution results has weakened, however the model continues to predict northwesterly ow from Georgian Bay. Typical 10 m windspeeds calculated by the model north of Lake Ontario are between 5 and 7 m s;1 , while observations show variable winds, though generally from a westerly direction, with speeds less than 2 m s;1 . Errors in the gradient ow to the north of Lake Ontario undoubtedly contribute to limiting the inland penetration of the lake breeze front on this day. Figure 5.11 shows the model calculated ozone concentration and wind eld at 2100 GMT for the model levels at 10 m (panel a) and 220 m (panel b) above the surface. The ozone concentration in the lowest model level shows concentrations greater than 70 ppb along the north shore of Lake Ontario, just to the east of Toronto. This area of higher ozone concentrations is associated with the thin layer of CO, and other ozone precursors, advected to the northeast from the `pool' of precursors which formed over the western end of Lake Ontario. As can be seen from the vertical crosssection in panel (a), the higher ozone concentrations are found at heights below 250 m, 211 with even higher ozone concentrations below 100 m. The ground-level concentration of ozone decreases rapidly as this plume is advected onshore due to increased vertical mixing over land. Figure 5.11: Horizontal and vertical cross-sections of the model calculated ozone concentration and wind eld at 2100 GMT, August 8, 1993. The horizontal crosssections show these elds at 10 m (panel a) and 240 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. A second region of high ground-level ozone concentrations is predicted at the western end of Lake Ontario. This region of high ozone concentrations is associated with the onshore ow of the lake breeze bringing higher ozone concentrations from over the lake. Panel (b) of Figure 5.11 shows the model ozone concentration and wind eld at 240 m above the surface and a north{south vertical cross-section across the western end of Lake Ontario. The vertical cross-section shows that over the lake, the 212 highest concentrations of ozone are found aloft. As was discussed earlier, the ozone precursors emitted from Toronto and advected southward in the gradient ow are forced to rise over the onshore ow of the lake breeze which is bringing less polluted air northward along the surface of the lake. The resulting layer of ozone aloft is advected towards land by the lake breeze and mixes down to ground-level due to increased vertical mixing over land. 5.2.1 Forward Trajectory Analysis For the purpose of visualizing how the lake breeze aects the dispersion of emissions from Toronto, three-dimensional forward trajectories have been generated from the model calculated wind elds. Figure 5.12 shows seven dierent forward trajectories from Toronto. The rst forward trajectory was begun at 1000 GMT and a new trajectory was started every hour. This set of trajectories were all begun at a height of 20 m above the surface. Trajectory (a) left Toronto in the early morning, before the lake breeze had developed, and continued south across the western end of Lake Ontario. Trajectory (b) initially followed a similar path as trajectory (a), though became caught in the lake breeze circulation as it developed and was eventually advected towards the north-east within the onshore ow of the lake breeze. Several of the subsequent trajectories (trajectories c, d, e and f) became entrained within the lake breeze in a similar manner as trajectory (b), though were initially advected towards the northwest by the onshore ow of the lake breeze. This set of trajectories ascended at the lake breeze front, to the west of where they were released, returned towards the center of the lake in the return ow aloft, then re-entered the onshore ow of the lake breeze and were 213 Figure 5.12: Three-dimensional forward trajectories from Toronto for August 8, 1993. The trajectories were begun at one hour intervals between 1000 and 1600 GMT and were released at a height of 20 m above the surface. The colour of the line represents the height of the trajectory in metres above ground level. advected towards the northeast. Trajectory (g) shows an example of emissions from Toronto entrained into the onshore ow of the lake breeze aloft. Trajectory (g) initially moved towards the south, then was forced to rise over the lake breeze front before descending while over the lake and eventually becoming entrained in the onshore ow of the lake breeze. Note that many of the forward trajectories complete at least one full recirculation within the lake breeze circulation, however trajectories calculated in the manner used here ignore the eects of turbulent mixing on the dispersion of pollutants. While many of the trajectories show a tendency to undergo recirculation within the lake breeze, the fraction of precursors that undergo recirculation may be considerably smaller than one (Lyons et al., 1995) 214 5.2.2 Eects of Dry Deposition The slow rate of dry deposition for many species over water has been suggested as a contributing factor in the production of high concentrations of ozone over lakes (Sillman et al., 1993). The slow rate of dry deposition results from the low solubility of certain species and the high degree of atmospheric stability over water, due to the formation of a conduction inversion during the daytime. Model calculated dry deposition rates for ozone over Lake Ontario are not larger than 0.04 cm s;1 . For a layer of ozone 100 m deep, a deposition velocity of 0.04 cm s;1 gives a time constant for the loss of ozone by dry deposition of approximately 70 hours. Thus, over the course of a day, loss of ozone by dry deposition to the lake surface is negligible, even for the case of a shallow layer of higher ozone concentrations in physical contact with the lake surface. For elevated layers of ozone, loss by dry deposition will be even smaller. Similarly, dry deposition velocities for NO2 and PAN are smaller over water than over land. Typical midday deposition velocities for NO2 over land are calculated to be between 0.4 and 0.6 cm s;1 , while over water the NO2 deposition velocities are no larger than 0.002 cm s;1. The dierence in dry deposition velocities between land and water surfaces for PAN is not as large as that calculated for NO2, with PAN deposition velocities typically a factor of three times smaller over water than over land. Henry's Law constants for NO2 and PAN show that NO2 is considerably less soluble than PAN and therefore NO2 has a smaller deposition velocity over water surfaces. For the more water soluble oxidation products such as HNO3 and H2O2 , the lower rates of dry deposition calculated over the lake are the result of greater aerodynamic 215 resistance, due to the increased stability over the lake. During the daytime, model dry deposition velocities for HNO3 range from 0.01 to 0.4 cm s;1 over the lake, while over land the range is from 1.5 to 4.0 cm s;1 . For H2O2 , deposition velocities over water are calculated to vary between 0.01 and 0.4 cm s;1 , while over land the range is from 0.7 to 1.5 cm s;1 . From the brief analysis of dry deposition velocities over water, it appears that the loss of ozone and NO2 by dry deposition will be negligible for an airmass over water. As suggested by Sillman et al. (1993), higher rates of dry deposition would most certainly have resulted in considerably lower concentrations of ozone over the lake. This is particularly true for shallow plumes of ozone, predicted by the model to be less than 100 m deep, for which appreciable ozone deposition velocities would have had a signicant eect. The model also calculates the generation of elevated plumes of ozone, and for these elevated plumes it can reasonably be expected that higher deposition velocities will have less of an eect since the plumes are physically separated from the surface. 5.3 Case Study: August 26, 1993 The second lake-breeze case study occurred on August 26, 1993. Chemical observations at the Hastings eld site showed that within 10 minutes, beginning at 2039 GMT (1639 EDT), the concentration of ozone increased from 46 to 59 ppb. The concentration of ozone continued to increase, though more slowly, until 2144 GMT, at which time a concentration of 79 ppb was observed. Likewise, the concentration of NOy increased from 2.2 to 3.8 ppb during the rst 10 minutes of the event, then continued to increase to 4.6 ppb at 2144 GMT. See Figure 5.1 for the observed ozone and NOy 216 concentrations at Hastings on August 26. Figure 5.13 shows the synoptic conditions for 0000 GMT, August 26 and 0000 GMT, August 27, 1993 as taken from the CMC objective analysis. A large ridge of high pressure lay just to the west of Lake Ontario at 0000 GMT, August 26 and winds from from the northwest. Over the course of the day the ridge moved across southern Ontario to lie to the south and east of Lake Ontario, and the 850 mb winds backed to become southwesterly by 0000 GMT, August 27. Figure 5.13: Sea-level pressure and 850 mb winds taken from the CMC objective analysis for 0000 GMT August 26, 1993 (panel a) and 0000 GMT August 27, 1993 (panel b). Surface observations, from stations away from Lake Ontario, showed that winds were from a west to southwesterly direction during the afternoon of August 26 with speeds less than 2 m s;1 . Daytime high temperatures from 31 to 33 C were recorded across southeastern Ontario. Kingston was an exception. With winds from the lake for most of the day, the high temperature at Kingston was 26 C. 217 Figure 5.14 shows the CO concentration and wind eld in the second model layer, approximately 20 m above the surface, at 1100 GMT. The wind eld aloft is quite weak, with model winds at 1 km above ground less than 2 m s;1 . With no strong synoptic forcing the wind eld near the surface is predicted by the model to be quite complex. A region of strong convergence is predicted by the model along the southern shore of Lake Ontario. A second region of strong convergence is predicted along the northern shore of Lake Erie. Northerly ow across Lake Ontario bifurcates along the southern shore with one branch moving to the southwest and the other branch moving to the east. Emissions from Toronto are advected to the southwest and eventually exit the 5.3 km resolution domain along the western edge of the model. The observed surface winds at 1100 GMT are shown in Figure 5.15. The model wind eld shows a signicant region of convergence over Lake Ontario as part of a land breeze circulation. Observations at Toronto Island and St. Catherines seem to support the occurrence of a land breeze with both stations reporting oshore ow with windspeeds of 1.7 m s;1. Aside from the probable occurrence of a land breeze circulation, the observations are not suciently numerous to support or refute other features of the model wind eld. Figure 5.16 presents horizontal and vertical cross-sections of the CO concentration and wind eld calculated by the model for 1600 GMT. The 10 m winds show a centre of divergence to the south and east of Toronto and onshore ow over all shores of Lake Ontario. Inland penetration of the lake breeze appears to be particularly deep to the northwest of Lake Ontario, in the vicinity of Toronto. As will be seen in the results for subsequent hours, the deep inland penetration of the onshore ow over this region collapses and a new lake breeze front forms nearer the lakeshore. It is unclear 218 Figure 5.14: Horizontal and vertical cross-sections of the CO concentration and wind eld at 1100 GMT, August 26, 1993. The horizontal cross-section shows the CO concentration and wind eld at 20 m above the surface. The position of the vertical cross-section is given by the thick line drawn across the horizontal cross-section panel. 219 . . . . . Figure 5.15: The observed wind at 10 m above the ground for 1100 GMT (0700 EDT) on August 26, 1993. whether such behaviour is realistic and the factors which have caused it have not been analyzed. One possible cause may be instabilities in the model solution caused by the application of boundary conditions, since the region in which this feature occurred is quite close to the western boundary of the model domain. The concentration of CO in the lowest model layer shows a plume from Toronto spreading along the northern shore of the lake. A vertical cross-section through the eastern edge of the plume shows weak onshore ow, approximately 100 m deep. Over the lake the plume is less than 200 m deep, while over land, due to greater vertical mixing, the plume is approximately 500 m deep. Panel (b) of Figure 5.16 shows the concentrations of CO and the wind eld at 435 m above the surface. The vertical cross-section in panel (b) shows that the boundary layer over Toronto at 1600 GMT is calculated by the model to be approximately 600 m deep. Winds at 435 m are from the west and are advecting the Toronto plume along the northern shore of Lake Ontario. 220 Figure 5.16: Horizontal and vertical cross-sections of the model calculated CO concentration and wind eld at 1600 GMT, August 26, 1993. The horizontal cross-sections show these elds at 10 m (panel a) and 435 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. 221 A comparison of the model calculated winds at 10 m above the ground with observations at 1600 GMT, shown in Figure 5.17, suggest no signicant errors in the model simulation of the surface winds. An exception to the general agreement between observations and the model is the observed wind at St. Catherines. Observations show that the wind at St. Catherines at 1600 GMT was from the south-southwest at 4 m s;1 , while the model is calculating light onshore, or northerly, ow associated with the lake breeze. The disagreement suggests that the model lake breeze front was too far inland along the southwestern shoreline of Lake Ontario. However, the winds observed at St. Catherines do become onshore the following hour. .. .. .. . . . . . . Figure 5.17: The observed wind at 10 m above the ground for 1600 GMT (1200 EDT) on August 26, 1993. The CO concentration and wind eld calculated by the model for 2000 GMT are shown in Figure 5.18. The model shows a well developed lake breeze circulation with strong onshore ow over all shores of the lake. A mesohigh is centered over the western half of Lake Ontario. The model lake breeze front has moved inland approximately 15 to 20 km along the north shore of Lake Ontario in the vicinity of Hastings. Analysis 222 of the inland penetration of the lake breeze front from visible satellite imagery for this day suggests that the front was approximately 30 km north of the Lake Ontario shoreline by 2000 GMT (Hastie et al., 1998). Figure 5.18: Horizontal and vertical cross-sections of the model calculated CO concentration and wind eld at 2000 GMT, August 26, 1993. The horizontal cross-sections show these elds at 10 m (panel a) and 435 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. An interesting feature of the spatial distribution of CO in the lowest model level is the lower concentrations present over the lake and the much higher concentrations just inland over the northwestern shore of Lake Ontario. Panel (b) of Figure 5.18 shows the model CO concentration and wind eld at 435 m above the surface. The winds at this level are from the west along the northern shore of Lake Ontario and act to advect the Toronto plume to the east. Near the surface, in the lake breeze onshore 223 ow, the winds are from the southwest and undercut the Toronto plume. The onshore circulation of the lake breeze is advecting less polluted air onshore, underneath the eastward progressing plume from Toronto. As the onshore ow moves further inland, vertical mixing rapidly mixes the higher concentrations of CO down to ground-level, giving rise to the strong horizontal concentration gradients seen at the surface. Though the model resolution is not sucient to resolve such a feature, the onshore advection of less polluted air near the surface, with higher concentrations of pollutants aloft, could be expected to result in a ground-level concentration pattern similar to that found by Lyons and Cole (1976) along the western shore of Lake Michigan: within 1 km of the shoreline concentrations of ozone were found to be lower than those observed further inland. The explanation proposed by Lyons and Cole was that an elevated plume of ozone, which existed over the lake, was mixed down to the surface by a deepening TIBL as the onshore ow moved further inland. Though there are no observations of a similar phenomenon occurring along the shores of Lake Ontario, the large scale features predicted by the model for this case would result in a similar pattern in the ground-level concentration. The nal hour analyzed is 0000 GMT, August 27 (2000 EDT, August 26). The CO and wind elds calculated by the model for this time are shown in Figure 5.19. The wind elds and the spatial distribution of CO are largely a natural evolution of the patterns found in the model output for 2000 GMT. The plume of CO has advected further to the east along the north shore of Lake Ontario and continues to be undercut by less polluted air in the onshore ow of the lake breeze. In regions where the onshore ow is undercutting the Toronto plume the horizontal concentration gradient at ground-level is not as strong as was seen earlier. With slower vertical mixing over 224 land, the onshore ow of less polluted air is able to penetrate further inland before the higher concentrations of CO aloft are mixed down. Figure 5.19: Horizontal and vertical cross-sections of the model calculated CO concentration and wind eld at 0000 GMT, August 27, 1993. The horizontal cross-sections show these elds at 10 m (panel a) and 435 m (panel b) above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. Note that the concentration of CO in the plume is decreasing as the plume is advected further to the east, presumably as a result of the entrainment of less polluted air into the solenoidal circulation of the lake-breeze. The northern end of the vertical cross-section drawn through panel (a) corresponds to the approximate location of the Hastings observation site. As can be seen from the surface wind eld, the model is not able to reproduce the observed inland penetration of the lake breeze front. At 0000 GMT, August 27 the model lake breeze front was 225 still approximately 15 km south of Hastings. Note that the lake breeze front was observed to arrive at Hastings at 2030 GMT. The vertical cross-sections presented above suggest signicant horizontal and vertical motions aect the Toronto plume as it is advected towards the east along the north shore of Lake Ontario. For example, the vertical cross-section in panel (a) of Figure 5.19 shows the lake breeze inow layer is approximately 500 m deep. Above the onshore ow the return circulation extends to approximately 1000 m above the surface. Vertical motions, such as ascent at the lake breeze front and subsidence behind the front, are also evident in the ow elds. Figure 5.20 shows a series of forward trajectories from Toronto, released at one hour intervals beginning at 1200 GMT. The forward trajectories suggest a solenoidal circulation as the plume is advected towards the east. As rst proposed by Lyons and Cole (1976), with gradient ow roughly parallel to the lakeshore material is advected in the general direction of the gradient ow, though undergoes solenoidal circulations due to the inuence of the lake breeze circulation. Figure 5.21 shows the concentration of ozone calculated for the lowest model level at 2000 GMT, August 26 and 0000 GMT August 27. The spatial distribution and interaction of ozone with the lake breeze is quite similar to that described above for CO: ozone is photochemically generated within the Toronto plume and advected towards the east, along the north shore of Lake Ontario by a combination of the gradient ow and lake breeze circulation. The model calculates a ground-level ozone concentration of 84 ppb approximately 15 km to the south of Hastings at 0000 GMT, August 27 (2000 EDT). 226 Figure 5.20: Three-dimensional forward trajectories from Toronto for August 26, 1993. The trajectories began at one hour intervals between 1200 and 1600 GMT and were released at a height of 160 m above the surface. The height of the trajectory, in metres above ground level, is given by the colour of the line. 5.3.1 Aircraft Observations The SONTOS 1993 study did include a series of aircraft ights, during which ozone, NO2 and NOx were measured. Hydrocarbon samples were also taken, though these are not discussed here. One of these ights occurred on August 26, and the observed ozone and NOx concentrations from this ight have been compared with the model calculations. The aircraft ight on August 26 was divided into two parts a ight from Guelph to Peterborough, and a return ight from Peterborough to Guelph. Figure 5.22 shows the path of the Guelph to Peterborough ight, which took place between approximately 1615 and 1800 GMT (1215 and 1400 EDT). Figure 5.23 shows the observed and modelled concentrations of ozone and NOx, and the altitude of the aircraft, as a function of time during the ight. To the west and south of Toronto, both over land and over Lake Ontario, the aircraft measurements 227 Figure 5.21: Horizontal and vertical cross-sections of the model calculated O3 concentration and wind eld at 2000 GMT, August 26 (panel a) and 0000 GMT, August 27, 1993 (panel b). The horizontal cross-sections show these elds at 10 m above the surface. The position of the vertical cross-sections are denoted by the thick solid lines drawn over the horizontal cross-sections. 228 Figure 5.22: Path for the Guelph to Peterborough ight of August 26, 1993. The labelled points along the path correspond to features in the observed ozone concentration and are referenced below. showed a relatively homogeneous distribution of ozone, with concentrations between 80 and 90 ppb. While slightly higher concentrations of ozone were observed over Lake Ontario south of Toronto, denoted by point (b), these concentrations were not greatly dierent from those found between Guelph and Binbrook. The most signicant feature in the observed ozone concentration eld was found over Lake Ontario to the east of Toronto, where ozone concentrations between approximately 90 and 105 ppb were observed. The aircraft was approximately 300 to 400 m above the lake during this portion of the ight. The region with these higher concentrations of ozone lie between points (c) and (d) on Figure 5.22. Ozone concentrations abruptly decreased as the aircraft passed point (d), though it is not clear whether this was a result of horizontal or vertical gradients in the ozone eld, as the 229 Figure 5.23: The observed and modelled concentration of ozone (panel a) and NOx (panel b), in ppb, as a function of time for the Guelph to Peterborough aircraft ight of August 26, 1993. The aircraft altitude is also shown on both panels. The labelled points along the time axis of the graph correspond to the position of the aircraft as given by the labelled points along the aircraft path shown in Figure 5.22. altitude of the aircraft was increasing during this time. Lower ozone concentrations, between 50 and 60 ppb, were observed north of Lake Ontario. The model ozone and NOx elds have been interpolated, in space and time, onto the aircraft position and plotted as a function of time alongside the observations in Figure 5.23. Upwind of Toronto the model underpredicts ozone: from takeo until approximately 1735 GMT the model ozone is approximately 15 { 20 ppb lower than the observed concentration. Nearer to Binbrook, denoted by point (a), the model ozone is in better agreement with observations, as the model predicts higher ozone concentrations associated with emissions from Hamilton and surrounding regions. 230 The model predicts ozone concentrations that are signicantly lower than observed for almost the entire time the aircraft is over Lake Ontario. Over the western end of Lake Ontario, denoted by point (b), the model underpredicts ozone by between 15 and 20 ppb, while within the area of higher ozone concentrations to the east of Toronto, ozone is underpredicted by as much as 40 ppb. Aircraft observations of NOx show two distinct regions over the lake where NOx concentrations were found to be higher than the background concentration: over the western end of Lake Ontario, between points (a) and (b), and within the region of higher ozone concentrations to the east of Toronto, noted above, between points (c) and (d). The model NOx concentration over the extreme western end of Lake Ontario agrees reasonably well with the observations, though further to the east, particularly south of Toronto, denoted by point (b), the model underpredicts NOx. The model shows emissions from urbanized regions around the western end of Lake Ontario, advected over the lake by the westerly gradient ow at levels greater than 300 m above the ground. At lower levels, the onshore ow of the lake breeze brings less polluted air from over the lake, towards land. The model also predicts higher NOx concentrations to the east of Toronto, associated with the Toronto urban plume being advected along the north shore of Lake Ontario. As discussed above, the model predicts that the Toronto urban plume is advected to the east within the solenoidal circulation of the lake breeze (see Figure 5.18). Observations show a rapid increase in the concentration of NOx as the aircraft passed point (c). The model predicts a similar feature in the NOx eld, though the Toronto plume is positioned slightly to the south of where observations suggest it is. 231 The return ight, from Peterborough to Guelph, took place between approximately 1930 and 2100 GMT (1530 and 1700 EDT), and followed an almost identical path as the ight to Peterborough. The path of the return ight is shown in Figure 5.24. Figure 5.24: Path for the Peterborough to Guelph ight of August 26, 1993. The labelled points along the path correspond to features in the observed ozone concentration and are referenced below. As above, the observed and modelled concentrations of ozone and NOx are presented as a function of time during the aircraft ight in Figure 5.25. As shown in Figure 5.24, the aircraft began at Peterborough and initially ew to the northeast, passing over the Hastings eld site, before heading south towards Lake Ontario. Approximately 10 km south of Hastings, denoted by point (e), ozone measured onboard the aircraft increased rapidly from 60 to 90 ppb. It seems plausible that the airmass encountered by the aircraft at point (e) was the same airmass that resulted in the 232 increase in ozone and other trace species concentrations at the Hastings eld site one hour later. For the remainder of the ight ozone concentrations were observed to range between 75 and 90 ppb, with the highest concentrations south of Toronto, in the vicinity of point (g). Figure 5.25: The observed and modelled concentration of ozone (panel a) and NOx (panel b), in ppb, as a function of time for the Peterborough to Guelph aircraft ight of August 26, 1993. The aircraft altitude is also shown on both panels. The labelled points along the time axis of the graph correspond to the position of the aircraft as given by the labelled points along the aircraft path shown in Figure 5.24. The model ozone concentration, interpolated onto the aircraft position, shows little evidence of a more polluted airmass moving north with the lake breeze front. The model ozone does show a gradual increase after the aircraft passes point (f), though much of the increase occurs while the aircraft is ying to the west, towards Toronto. 233 Referring to Figure 5.21 above, which shows the model ozone eld at 2000 GMT, approximately the time of the Peterborough to Guelph ight, it can be seen that the model calculates much of ozone in the Toronto plume to be well to the west of the Hastings-Peterborough area at 2000 GMT. Though a lake breeze front is calculated by the model to lie to the south of Hastings, the airmass behind the front is not signicantly polluted. These results suggest that the eastern edge of the Toronto plume is placed too far to the west by the model. Whether this is caused by a too slow eastward advection of the Toronto plume by the model or other causes is not clear. It is not until approximately 2200 GMT that the model calculates the Toronto plume to have advanced far enough east to result in ozone concentrations which are greater than 80 ppb as far east as Hastings. Note that the eastward advection of the Toronto plume discussed here is somewhat separate from the northward, or inland, penetration of the plume with the lake breeze front. A comparison of the modelled and observed NOx, shown in panel (b) of Figure 5.25, shows that the model signicantly overpredicts the concentration of NOx along the northern edge of Lake Ontario, between Peterborough and Toronto. The model calculates the Toronto plume to lie across the path of the airplane, which it clearly does not. Underprediction, by the model, of the inland penetration of the lake breeze, discussed above, may be contributing to the large error in NOx, though it is not clear if this is the cause of the discrepancy. Note that while the model ozone agrees fairly well with the observations for the portion of the ight over Lake Ontario, the magnitude of the error in NOx would suggest the agreement for ozone is fortuitous. 234 5.4 Summary The MC2-online model has been used to study the interaction of the Lake Ontario lake breeze with the Toronto plume on two dierent days. On both of the days chosen for study, observations at the Hastings eld site showed the inuence of the lake breeze circulation on air quality. For the rst day studied, August 8, 1993, the simulation develops signicant errors at the synoptic scale, which adversely aect the development of the lake breeze. While the model results for August 8 appear to be a poor simulation of the meteorology, and by extension the chemistry, of August 8, an analysis of the model results does suggest some possible ways in which lake breeze circulations aect urban plumes and the photochemical formation of ozone. The MC2-online simulation for August 8 shows gradient ow from the north during the early morning. Before the onshore ow of the lake breeze circulation begins, precursors are advected over the lake and remain conned within 100 to 200 m of the surface. During the early morning, as the gradient wind, or land breeze circulation, weakens, during the initial development of onshore ow of the lake breeze, the precursors already over the lake are temporarily trapped over the lake. As the onshore ow of the lake breeze strengthens, the precursors trapped near the lake surface are advected onshore. For the simulation of August 8, one centre of divergence formed almost directly to the south of Toronto, within the plume of precursors which had been advected over the lake earlier in the morning. The formation of the centre of divergence results in a bifurcation of the plume, with part of the material advected inland around the western end of Lake Ontario, and the remaining material advected to the north-east, along the longer axis of the lake. Subsidence near the centre of 235 divergence brings less polluted air to the surface over the lake. Once the onshore ow of the lake breeze is established, over the western end of Lake Ontario the northerly gradient ow is opposed by the southerly onshore ow of the lake breeze. Emissions from Toronto are forced to rise over the lake breeze front and continue to the south under the inuence of the gradient ow and the lake breeze return ow. The forced ascent over the lake breeze front results in the formation of some elevated plumes over the lake. As the depth of the onshore ow of the lake breeze increases with time, emissions from Toronto which had been forced to rise over the lake breeze front are entrained in the onshore ow. For the simulation of August 8, a centre of divergence forms over the extreme southwest corner of Lake Ontario and a band of southwesterly winds develops, which ow inland along the north shore of Lake Ontario to the east of Toronto. Portions of the Toronto plume are carried to the south by the gradient wind, become entrained within the southwesterly onshore ow of the lake breeze and are advected towards the northeast. Signicant fractions of the Toronto plume are not entrained within the lake breeze circulation and are advected to the south, completely crossing the lake. The model calculated distribution of ozone shows the formation of a vertically thin layer with high concentrations of ozone associated with the portions of the Toronto plume advected onto the lake in the early morning. This thin layer of ozone has only a minimal eect on ozone concentrations inland as it is rapidly mixed and diluted as it is advected inland. The model does predict signicant formation of ozone in elevated layers over the western end of Lake Ontario, due to precursors from Toronto which were forced to 236 rise over the lake breeze front and subsequently entrained within the lake breeze circulation. These elevated layers of ozone are largely advected towards the northeast by the onshore ow of the lake breeze, though they do not have sucient time to advect inland and remain over the lake at the end of the simulation. The model simulation of the second day chosen for study, August 26, 1993, does not show any signicant errors in the synoptic features. Winds during the morning are light and from the west, slowly backing to a more southwesterly direction during the afternoon. The model predicts the formation of a signicant land breeze during the early morning of August 26. A strong region of convergence is calculated by the model along the southern shore of Lake Ontario, with northerly wind crossing the lake. Over the western end of Lake Ontario, the northerly winds are deected towards the southwest, with the result that precursors emitted from Toronto early in the morning are advected to the southwest, and do not `pool' over the lake. Later in the morning, as the lake breeze circulation develops, the westerly gradient ow advects the Toronto plume to the east, along the north shore of Lake Ontario. A combination of the westerly gradient ow, and the solenoidal circulation of the lake breeze, results in helical trajectories for material in the plume as it is advected along the north shore of Lake Ontario. Near the surface, the onshore ow of the lake breeze brings less polluted air, from the centre of the lake, inland along the north shore of Lake Ontario. The less polluted air in the lowest levels of the lake breeze onshore ow, undercuts the more polluted air being advected to the east in the lake breeze solenoid. As the onshore ow moves inland, greater vertical mixing brings the more polluted air aloft, down 237 to the surface. Though poorly resolved by the model, this scenario would seem to result in a distribution of ground-level ozone similar to that observed by Lyons and Cole (1976) along the western shore of Lake Michigan. A comparison of the model lake breeze with a variety of observations suggests that the model signicantly underpredicts the inland penetration of the lake breeze front for this case. A comparison of the model ozone and NOx concentrations with aircraft observations nds some anecdotal evidence supporting, qualitatively, the interaction of the Toronto plume with the lake breeze predicted by the model. A more thorough test of the model would require a more intensive aircraft campaign with ights which more fully map the spatial distribution of the Toronto plume. 238
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