Search Results
You are looking at 1 - 10 of 72 items for
- Author or Editor: J. M. Chen x
- Refine by Access: All Content x
Abstract
Slantwise convection, the process by which moist symmetric instability is released, has often been linked to banded clouds and precipitation, especially in frontal zones within extratropical cyclones. Studies also suggest that the latent heat release associated with slantwise convection can lead to a spinup of surface frontogenesis, which can enhance the rapid intensification of extratropical cyclones. However, most of these studies considered only local areas or short time durations. In this study, we provide a novel statistical investigation of the global climatology of the potential occurrence of slantwise convection, in terms of conditional symmetric instability, and its relationship with precipitating systems. Using the 6-hourly ERA-Interim, two different indices are calculated, namely, slantwise convective available potential energy (SCAPE) and vertically integrated extent of realizable symmetric instability (VRS), to assess the likelihood of occurrence of slantwise convection around the globe. The degree of association is quantified between these indices and the observed surface precipitation as well as the cyclone activity. The susceptibility of midlatitude cyclones to slantwise convection at different stages of their life cycle is also investigated. As compared to the nonexplosive cyclone cases, the time evolution of SCAPE and VRS within rapidly deepening cyclones exhibit higher values before, and a more significant drop after, the onset of rapid intensification, supporting the idea that the release of symmetric instability might contribute to the intensification of storms.
Abstract
Slantwise convection, the process by which moist symmetric instability is released, has often been linked to banded clouds and precipitation, especially in frontal zones within extratropical cyclones. Studies also suggest that the latent heat release associated with slantwise convection can lead to a spinup of surface frontogenesis, which can enhance the rapid intensification of extratropical cyclones. However, most of these studies considered only local areas or short time durations. In this study, we provide a novel statistical investigation of the global climatology of the potential occurrence of slantwise convection, in terms of conditional symmetric instability, and its relationship with precipitating systems. Using the 6-hourly ERA-Interim, two different indices are calculated, namely, slantwise convective available potential energy (SCAPE) and vertically integrated extent of realizable symmetric instability (VRS), to assess the likelihood of occurrence of slantwise convection around the globe. The degree of association is quantified between these indices and the observed surface precipitation as well as the cyclone activity. The susceptibility of midlatitude cyclones to slantwise convection at different stages of their life cycle is also investigated. As compared to the nonexplosive cyclone cases, the time evolution of SCAPE and VRS within rapidly deepening cyclones exhibit higher values before, and a more significant drop after, the onset of rapid intensification, supporting the idea that the release of symmetric instability might contribute to the intensification of storms.
Abstract
The National Centers for Environmental Prediction’s operational global data assimilation system’s (GDAS) atmospheric and surface thermodynamic energy cycles are presented for the Mississippi River basin where the Global Energy and Water Cycle Experiment Continental-Scale International Project (GCIP) is under way. At the surface, during the winter, incoming solar radiation is balanced by longwave cooling. During the summer, latent and sensible cooling are equally important. In the atmosphere, thermodynamic energy convergence is also important, especially during the winter. In most places, precipitation is largely balanced by thermodynamic energy divergence. Anomalously high surface temperatures appear to be mainly related to decreased surface evaporation. Anomalously high (low) precipitation variations may also be related to anomalously high thermodynamic energy divergence (convergence). Unfortunately, residual terms, which are slightly noticeable for the GCIP climatological balances, are especially noticeable for the anomalous atmospheric balances.
Abstract
The National Centers for Environmental Prediction’s operational global data assimilation system’s (GDAS) atmospheric and surface thermodynamic energy cycles are presented for the Mississippi River basin where the Global Energy and Water Cycle Experiment Continental-Scale International Project (GCIP) is under way. At the surface, during the winter, incoming solar radiation is balanced by longwave cooling. During the summer, latent and sensible cooling are equally important. In the atmosphere, thermodynamic energy convergence is also important, especially during the winter. In most places, precipitation is largely balanced by thermodynamic energy divergence. Anomalously high surface temperatures appear to be mainly related to decreased surface evaporation. Anomalously high (low) precipitation variations may also be related to anomalously high thermodynamic energy divergence (convergence). Unfortunately, residual terms, which are slightly noticeable for the GCIP climatological balances, are especially noticeable for the anomalous atmospheric balances.
Abstract
Black carbon aerosol (BC) has a significant influence on regional climate changes because of its warming effect. Such changes will feed back to BC loadings. Here, the interactions between the BC warming effect and the East Asian monsoon (EAM) in both winter (EAWM) and summer (EASM) are investigated using a regional climate model, RegCM4, that essentially captures the EAM features and the BC variations in China. The seasonal mean BC optical depth is 0.021 over East Asia during winter, which is 10.5% higher than that during summer. Nevertheless, the BC direct radiative forcing is 32% stronger during summer (+1.85 W m−2). The BC direct effect would induce lower air to warm by 0.11–0.12 K, which causes a meridional circulation anomaly associated with a cyclone at 20°–30°N and southerly anomalies at 850 hPa over East Asia. Consequently, the EAM circulation is weakened during winter but enhanced during summer. Precipitation is likely increased, especially in southern China during summer (by 3.73%). Relative to BC changes that result from EAM interannual variations, BC changes from its warming effect are as important but are weaker. BC surface concentrations are decreased by 1%–3% during both winter and summer, whereas the columnar BC is increased in south China during winter. During the strongest monsoon years, the BC loadings are higher at lower latitudes than those during the weakest years, resulting in more southerly meridional circulation anomalies and BC feedbacks during both winter and summer. However, the interactions between the BC warming effect and EAWM/EASM are more intense during the weakest monsoon years.
Abstract
Black carbon aerosol (BC) has a significant influence on regional climate changes because of its warming effect. Such changes will feed back to BC loadings. Here, the interactions between the BC warming effect and the East Asian monsoon (EAM) in both winter (EAWM) and summer (EASM) are investigated using a regional climate model, RegCM4, that essentially captures the EAM features and the BC variations in China. The seasonal mean BC optical depth is 0.021 over East Asia during winter, which is 10.5% higher than that during summer. Nevertheless, the BC direct radiative forcing is 32% stronger during summer (+1.85 W m−2). The BC direct effect would induce lower air to warm by 0.11–0.12 K, which causes a meridional circulation anomaly associated with a cyclone at 20°–30°N and southerly anomalies at 850 hPa over East Asia. Consequently, the EAM circulation is weakened during winter but enhanced during summer. Precipitation is likely increased, especially in southern China during summer (by 3.73%). Relative to BC changes that result from EAM interannual variations, BC changes from its warming effect are as important but are weaker. BC surface concentrations are decreased by 1%–3% during both winter and summer, whereas the columnar BC is increased in south China during winter. During the strongest monsoon years, the BC loadings are higher at lower latitudes than those during the weakest years, resulting in more southerly meridional circulation anomalies and BC feedbacks during both winter and summer. However, the interactions between the BC warming effect and EAWM/EASM are more intense during the weakest monsoon years.
Abstract
The island of Taiwan is situated in the main path of western North Pacific typhoons. Its dominant central mountain range (CMR), with a hoizontal scale comparable to the radius of a typhoon, often produces significant distortions in the typhoon circulation. A 20-year dataset from 22 surface stations is used to describe the effects of the Taiwan terrain on the surface structure of typhoons.
Empirical orthogonal function analysis on the pressure field is used to identify the primary structure modes. The first mode is a uniform-sign anomaly pattern portraying the decrease in pressure as a typhoon is approaching. The second mode represents the strong terrain-induced west-east pressure gradient that is normal to the main axis of the CMR. The third mode results mainly from the west-cast pressure gradient arising from the relative location of the typhoon center to the east or west of Taiwan, but it also contains a weak south-north pressure gradient that can he attributed to the terrain. A regression technique is then used to determine the surface wind, temperature, relative humidity, and hourly rainfall associated with each pressure mode. In all cases, them fields are consistent, showing the effects of the terrain blocking or deflection and their consequent ascending and descending motions.
The relative importance of each mode depends strongly on the location of the typhoon center. No dependence on the direction or speed of motion is discernible when all cases are considered. When different, persistently smooth tracks are identified, the variations due to motion direction can be recognized because the terrain effect is affected by the mean steering flow. Only two types of smooth tracks that represent clearly different steering flows intersect in an area. At the intersection, a subsequent difference in storm structure over Taiwan exists that can be explained by the difference in the steering flows associated with the two track types.
The leeside secondary low that was often observed on the west coast of Taiwan is found to consist of at least two basic modes. It develops only when the typhoon center is in southeastern Taiwan or an ocean area to the east-southeast. The observed scale of this low is significantly smaller than that which can be produced by an interaction of the mean steering flow and the CMR. This smaller scale is due to a local buildup of the surface pressure south of the lee vortex, which results from the against-mountain return flow of the cyclonic circulation.
Abstract
The island of Taiwan is situated in the main path of western North Pacific typhoons. Its dominant central mountain range (CMR), with a hoizontal scale comparable to the radius of a typhoon, often produces significant distortions in the typhoon circulation. A 20-year dataset from 22 surface stations is used to describe the effects of the Taiwan terrain on the surface structure of typhoons.
Empirical orthogonal function analysis on the pressure field is used to identify the primary structure modes. The first mode is a uniform-sign anomaly pattern portraying the decrease in pressure as a typhoon is approaching. The second mode represents the strong terrain-induced west-east pressure gradient that is normal to the main axis of the CMR. The third mode results mainly from the west-cast pressure gradient arising from the relative location of the typhoon center to the east or west of Taiwan, but it also contains a weak south-north pressure gradient that can he attributed to the terrain. A regression technique is then used to determine the surface wind, temperature, relative humidity, and hourly rainfall associated with each pressure mode. In all cases, them fields are consistent, showing the effects of the terrain blocking or deflection and their consequent ascending and descending motions.
The relative importance of each mode depends strongly on the location of the typhoon center. No dependence on the direction or speed of motion is discernible when all cases are considered. When different, persistently smooth tracks are identified, the variations due to motion direction can be recognized because the terrain effect is affected by the mean steering flow. Only two types of smooth tracks that represent clearly different steering flows intersect in an area. At the intersection, a subsequent difference in storm structure over Taiwan exists that can be explained by the difference in the steering flows associated with the two track types.
The leeside secondary low that was often observed on the west coast of Taiwan is found to consist of at least two basic modes. It develops only when the typhoon center is in southeastern Taiwan or an ocean area to the east-southeast. The observed scale of this low is significantly smaller than that which can be produced by an interaction of the mean steering flow and the CMR. This smaller scale is due to a local buildup of the surface pressure south of the lee vortex, which results from the against-mountain return flow of the cyclonic circulation.
Abstract
A novel hybrid vertical mixing scheme, based jointly on the Kraus–Turner-type mixed layer model and Price's dynamic instability model, is introduced to aid in parameterization of vertical turbulent mixing in numerical ocean models. The scheme is computationally efficient and is capable of simulating the three major mechanisms of vertical turbulent mixing in the upper ocean, that is, wind stirring, shear instability, and convective overturning.
The hybrid scheme is first tested in a one-dimensional model against the Kraus–Turner-type bulk mixed layer model and the Mellor–Yamada level 2.5 (MY2.5) turbulence closure model. As compared with those two models, the hybrid model behaves more reasonably in both idealized experiments and realistic simulations. The improved behavior of the hybrid model can be attributed to its more complete physics. For example, the MY2.5 model underpredicts mixed layer depth at high latitudes due to its lack of wind stirring and penetrative convection, while the Kraus–Turner bulk model produces rather shallow mixed layers in the equatorial region because of its lack of shear-produced mixing. The hybrid model reproduces the good results of the MY2.5 model toward the equator and the bulk model toward high latitudes, thereby taking the advantages of those two models while avoiding their shortcomings.
The hybrid scheme is then implemented in a three-dimensional model of the tropical Pacific Ocean. This leads to an improved simulation of the large-scale equatorial circulation. Compared with the other two commonly used mixing schemes tested in this experiment, the hybrid scheme helps to produce more realistic velocity profiles in the eastern and central equatorial Pacific. This is mainly due to the improved parameterization of interior mixing related to the large shears of the Equatorial Undercurrent. Another feature in this model that is sensitive to the vertical mixing scheme is the equatorial instability waves; in the eastern Pacific Ocean these waves are most energetic when the hybrid scheme is used. The meridional heat flux associated with these waves can be locally important in the mixed layer heat budget.
Abstract
A novel hybrid vertical mixing scheme, based jointly on the Kraus–Turner-type mixed layer model and Price's dynamic instability model, is introduced to aid in parameterization of vertical turbulent mixing in numerical ocean models. The scheme is computationally efficient and is capable of simulating the three major mechanisms of vertical turbulent mixing in the upper ocean, that is, wind stirring, shear instability, and convective overturning.
The hybrid scheme is first tested in a one-dimensional model against the Kraus–Turner-type bulk mixed layer model and the Mellor–Yamada level 2.5 (MY2.5) turbulence closure model. As compared with those two models, the hybrid model behaves more reasonably in both idealized experiments and realistic simulations. The improved behavior of the hybrid model can be attributed to its more complete physics. For example, the MY2.5 model underpredicts mixed layer depth at high latitudes due to its lack of wind stirring and penetrative convection, while the Kraus–Turner bulk model produces rather shallow mixed layers in the equatorial region because of its lack of shear-produced mixing. The hybrid model reproduces the good results of the MY2.5 model toward the equator and the bulk model toward high latitudes, thereby taking the advantages of those two models while avoiding their shortcomings.
The hybrid scheme is then implemented in a three-dimensional model of the tropical Pacific Ocean. This leads to an improved simulation of the large-scale equatorial circulation. Compared with the other two commonly used mixing schemes tested in this experiment, the hybrid scheme helps to produce more realistic velocity profiles in the eastern and central equatorial Pacific. This is mainly due to the improved parameterization of interior mixing related to the large shears of the Equatorial Undercurrent. Another feature in this model that is sensitive to the vertical mixing scheme is the equatorial instability waves; in the eastern Pacific Ocean these waves are most energetic when the hybrid scheme is used. The meridional heat flux associated with these waves can be locally important in the mixed layer heat budget.
Abstract
An analysis is performed on a microburst line-producing cloud that occurred near Denver, Colorado on 13 July 1982. The cloud line developed in an environment conducive to the production of low-reflectivity microbursts. Doppler radar analysis revealed strong convergence above cloud base into the region of downdraft 3.5 to 4.5 km above ground. Aircraft measurements detected light rain with graupel aloft in microburst downdrafts. A two-dimensional cloud model simulation captured many of the observed features of the cloud line structure and wind fields. In particular, both the development of multiple microbursts and the convergence aloft were well simulated. The formation of graupel/hail was important to the precipitation process in the model. The loading of rain and graupel and the cooling effect of rain evaporation and graupel melting were all important in microburst production—the graupel in the formative stages of the downdraft, and the rain in the further intensification of the downdraft and enhancement of the microburst outflow.
Abstract
An analysis is performed on a microburst line-producing cloud that occurred near Denver, Colorado on 13 July 1982. The cloud line developed in an environment conducive to the production of low-reflectivity microbursts. Doppler radar analysis revealed strong convergence above cloud base into the region of downdraft 3.5 to 4.5 km above ground. Aircraft measurements detected light rain with graupel aloft in microburst downdrafts. A two-dimensional cloud model simulation captured many of the observed features of the cloud line structure and wind fields. In particular, both the development of multiple microbursts and the convergence aloft were well simulated. The formation of graupel/hail was important to the precipitation process in the model. The loading of rain and graupel and the cooling effect of rain evaporation and graupel melting were all important in microburst production—the graupel in the formative stages of the downdraft, and the rain in the further intensification of the downdraft and enhancement of the microburst outflow.
Abstract
This study evaluates, for the first time, the impact of airborne global positioning system radio occultation (ARO) observations on a hurricane forecast. A case study was conducted of Hurricane Karl during the Pre-Depression Investigation of Cloud-Systems in the Tropics (PREDICT) field campaign in 2010. The assimilation of ARO data was developed for the three-dimensional variational (3DVAR) analysis system of the Weather Research and Forecasting (WRF) Model version 3.2. The impact of ARO data on Karl forecasts was evaluated through data assimilation (DA) experiments of local refractivity and nonlocal excess phase (EPH), in which the latter accounts for the integrated horizontal sampling along the signal ray path. The tangent point positions (closest point of an RO ray path to Earth’s surface) drift horizontally, and the drifting distance of ARO data is about 2 to 3 times that of spaceborne RO, which was taken into account in these simulations.
Results indicate that in the absence of other satellite observations, the assimilation of ARO EPH resulted in a larger impact on the analysis than local refractivity did. In particular, the assimilation of ARO observations at the actual tangent point locations resulted in more accurate forecasts of the rapid intensification of the storm. Among all experiments, the best forecast was obtained by assimilating ARO data with the most accurate geometric representation, that is, the use of nonlocal EPH operators with tangent point drift, which reduced the error in the storm’s predicted minimum sea level pressure (SLP) by 43% beyond that of the control experiment.
Abstract
This study evaluates, for the first time, the impact of airborne global positioning system radio occultation (ARO) observations on a hurricane forecast. A case study was conducted of Hurricane Karl during the Pre-Depression Investigation of Cloud-Systems in the Tropics (PREDICT) field campaign in 2010. The assimilation of ARO data was developed for the three-dimensional variational (3DVAR) analysis system of the Weather Research and Forecasting (WRF) Model version 3.2. The impact of ARO data on Karl forecasts was evaluated through data assimilation (DA) experiments of local refractivity and nonlocal excess phase (EPH), in which the latter accounts for the integrated horizontal sampling along the signal ray path. The tangent point positions (closest point of an RO ray path to Earth’s surface) drift horizontally, and the drifting distance of ARO data is about 2 to 3 times that of spaceborne RO, which was taken into account in these simulations.
Results indicate that in the absence of other satellite observations, the assimilation of ARO EPH resulted in a larger impact on the analysis than local refractivity did. In particular, the assimilation of ARO observations at the actual tangent point locations resulted in more accurate forecasts of the rapid intensification of the storm. Among all experiments, the best forecast was obtained by assimilating ARO data with the most accurate geometric representation, that is, the use of nonlocal EPH operators with tangent point drift, which reduced the error in the storm’s predicted minimum sea level pressure (SLP) by 43% beyond that of the control experiment.
Abstract
The possible relationship between northwestward-propagating wave disturbances and tropical cyclones over the tropical western North Pacific during summer is studied using data assimilated by the navy's global model during May–September 1989–91. A multiple-set canonical correlation (MCC) analysis is applied to the 850-hPa meridional (v) component over a core domain covering the western Pacific. The analysis seeks the maximal geometrically averaged correlation between 12 consecutive twice-daily fields. Two MCC components, with a 90° phase difference and comparable variances that combine to nearly one-third of the total variance, describe the northwestward-propagating pattern with a period near 8–9 days. Upstream of this steady northwestward-propagating pattern there is a weaker, westward propagation along 5°N that may be traced back to 170°E.
The surface pressure cell advancing east of the Philippines is consistent with low-level winds for a circulation in gradient wind balance. It has a zonal wavelength near 28° longitude, a northeast–southwest meridional tilt, a slightly forward tilt from 850 to 300 hPa, and a phase reversal above 200 hPa. The warm core extends from 925 to 200 hPa over the surface low with maximum at 200 hPa. Although there is a positive correlation, the low-level moisture structure is different from the surface pressure and v 850. A poleward moisture flux is clearly seen around the leading cell, but in the adjacent cell (with opposite polarity) to the southeast, moisture is nearly out of phase with pressure. This asymmetric moisture distribution is similar to that normally found in a tropical cyclone and its associated anticyclone where widespread subsidence dominates.
Both the structure and a comparison of named storm center locations against the various phases of the MCC modes suggest that the disturbance cyclonic cells during periods of high wave amplitudes are associated with tropical cyclone occurrences. During such periods either the wave disturbances modulate the sensitivity of the tropical atmosphere to the various physical mechanisms associated with tropical cyclone occurrences, or the presence of tropical cyclones modulate the amplitude of the wave disturbances.
Abstract
The possible relationship between northwestward-propagating wave disturbances and tropical cyclones over the tropical western North Pacific during summer is studied using data assimilated by the navy's global model during May–September 1989–91. A multiple-set canonical correlation (MCC) analysis is applied to the 850-hPa meridional (v) component over a core domain covering the western Pacific. The analysis seeks the maximal geometrically averaged correlation between 12 consecutive twice-daily fields. Two MCC components, with a 90° phase difference and comparable variances that combine to nearly one-third of the total variance, describe the northwestward-propagating pattern with a period near 8–9 days. Upstream of this steady northwestward-propagating pattern there is a weaker, westward propagation along 5°N that may be traced back to 170°E.
The surface pressure cell advancing east of the Philippines is consistent with low-level winds for a circulation in gradient wind balance. It has a zonal wavelength near 28° longitude, a northeast–southwest meridional tilt, a slightly forward tilt from 850 to 300 hPa, and a phase reversal above 200 hPa. The warm core extends from 925 to 200 hPa over the surface low with maximum at 200 hPa. Although there is a positive correlation, the low-level moisture structure is different from the surface pressure and v 850. A poleward moisture flux is clearly seen around the leading cell, but in the adjacent cell (with opposite polarity) to the southeast, moisture is nearly out of phase with pressure. This asymmetric moisture distribution is similar to that normally found in a tropical cyclone and its associated anticyclone where widespread subsidence dominates.
Both the structure and a comparison of named storm center locations against the various phases of the MCC modes suggest that the disturbance cyclonic cells during periods of high wave amplitudes are associated with tropical cyclone occurrences. During such periods either the wave disturbances modulate the sensitivity of the tropical atmosphere to the various physical mechanisms associated with tropical cyclone occurrences, or the presence of tropical cyclones modulate the amplitude of the wave disturbances.
Abstract
A recent advance in the Coupled Ocean–Atmosphere Mesoscale Prediction System (COAMPS) is described and used to study two-way air–sea coupling and its impact on two different weather scenarios. The first case examines the impact of a hurricane-induced cold ocean wake on simulated changes in the structure of Hurricane Katrina. The second case investigates the effect of wind- and current-induced island wakes and their impact on the local electromagnetic (EM) and acoustic propagation characteristics in the Southern California Bight region. In the Katrina case, both the atmosphere and ocean show a strong response from air–sea interaction. The model results show that wind-induced turbulent mixing, vertical advection, and horizontal advection are the three primary causes of the development of the trailing cold ocean wake. A distinct spatial separation is seen in these three primary forcing terms that are generating the bulk of the cooling in the ocean mixed layer. An asymmetric tropical cyclone structure change has been documented in detail from a more realistic, full physics, and tightly coupled model. These changes include a broadening of the eye, a reduced radius of hurricane-force wind, and a pronounced inner-core dry slot on the west side of the storm. In the island wake experiment, many finescale variations in the wind, current, and static stability structure resulting from the two-way interaction are described. These variations take the form of narrow vorticity and temperature anomalies that are found to reside in the ocean and atmosphere well downwind from the Channel Islands. Upwind differences in the lower-atmospheric wind and thermal structure also arise and are found to have a small impact on the lee-flow structure and EM characteristics of the southernmost Channel Islands.
Abstract
A recent advance in the Coupled Ocean–Atmosphere Mesoscale Prediction System (COAMPS) is described and used to study two-way air–sea coupling and its impact on two different weather scenarios. The first case examines the impact of a hurricane-induced cold ocean wake on simulated changes in the structure of Hurricane Katrina. The second case investigates the effect of wind- and current-induced island wakes and their impact on the local electromagnetic (EM) and acoustic propagation characteristics in the Southern California Bight region. In the Katrina case, both the atmosphere and ocean show a strong response from air–sea interaction. The model results show that wind-induced turbulent mixing, vertical advection, and horizontal advection are the three primary causes of the development of the trailing cold ocean wake. A distinct spatial separation is seen in these three primary forcing terms that are generating the bulk of the cooling in the ocean mixed layer. An asymmetric tropical cyclone structure change has been documented in detail from a more realistic, full physics, and tightly coupled model. These changes include a broadening of the eye, a reduced radius of hurricane-force wind, and a pronounced inner-core dry slot on the west side of the storm. In the island wake experiment, many finescale variations in the wind, current, and static stability structure resulting from the two-way interaction are described. These variations take the form of narrow vorticity and temperature anomalies that are found to reside in the ocean and atmosphere well downwind from the Channel Islands. Upwind differences in the lower-atmospheric wind and thermal structure also arise and are found to have a small impact on the lee-flow structure and EM characteristics of the southernmost Channel Islands.
Abstract
Ice formation in ammoniated sulfate and sulfuric acid aerosol particles under upper-tropospheric conditions was studied using a continuous flow thermal diffusion chamber. This technique allowed for particle exposure to controlled temperatures and relative humidities for known residence times. The phase states of (NH4)2SO4 and NH4HSO4 particles were found to have important impacts on their ice formation capabilities. Dry (NH4)2SO4 particles nucleated ice only at high relative humidity (RH ≥ 94%) with respect to water at temperatures between −40° and −60°C. This result suggested either an impedance or finite time dependence to deliquescence and subsequent homogeneous freezing nucleation. Ammonium sulfate particles that entered the diffusion chamber in a liquid state froze homogeneously at relative humidities that were 10% lower than where ice nucleated on initially dry particles. Likewise, crystalline or partially crystallized (as letovicite) NH4HSO4 particles required higher relative humidities for ice nucleation than did initially liquid bisulfate particles. Liquid particles of size 0.2 μm composed of either ammonium sulfate or bisulfate froze at lower relative humidity at upper-tropospheric temperatures than did 0.05-μm sulfuric acid aerosol particles. Comparison of calculated homogeneous freezing point depressions suggest that size effects on freezing may be more important than the degree of ammoniation of the sulfate compound.
Abstract
Ice formation in ammoniated sulfate and sulfuric acid aerosol particles under upper-tropospheric conditions was studied using a continuous flow thermal diffusion chamber. This technique allowed for particle exposure to controlled temperatures and relative humidities for known residence times. The phase states of (NH4)2SO4 and NH4HSO4 particles were found to have important impacts on their ice formation capabilities. Dry (NH4)2SO4 particles nucleated ice only at high relative humidity (RH ≥ 94%) with respect to water at temperatures between −40° and −60°C. This result suggested either an impedance or finite time dependence to deliquescence and subsequent homogeneous freezing nucleation. Ammonium sulfate particles that entered the diffusion chamber in a liquid state froze homogeneously at relative humidities that were 10% lower than where ice nucleated on initially dry particles. Likewise, crystalline or partially crystallized (as letovicite) NH4HSO4 particles required higher relative humidities for ice nucleation than did initially liquid bisulfate particles. Liquid particles of size 0.2 μm composed of either ammonium sulfate or bisulfate froze at lower relative humidity at upper-tropospheric temperatures than did 0.05-μm sulfuric acid aerosol particles. Comparison of calculated homogeneous freezing point depressions suggest that size effects on freezing may be more important than the degree of ammoniation of the sulfate compound.