The role of phoretic forces in providing in-cloud and below-cloud scavenging due to falling drop is reviewed by considering published papers dealing with theoretical models, laboratory and field measurements. Theoreti...The role of phoretic forces in providing in-cloud and below-cloud scavenging due to falling drop is reviewed by considering published papers dealing with theoretical models, laboratory and field measurements. Theoretical analyses agree that Brownian diffusion appears to dominate drop scavenging of aerosol with radius less than 0.1 μm, and inertial impaction dominates scavenging of aerosol with radius higher than 1 μm. Thus, there is a minimum collection efficiency for particles in the approximate range 0.1 μm - 1 μm, where phoretic forces are felt. Generally speaking, published papers report not uniform evaluations of the contribution of thermo- and diffusiophoretic forces. This disagreement is partially due to the different laboratory and field conditions, and different theoretical approaches.展开更多
This paper investigated the possibility that aerosol particles are scavenged during the first and fast diffusional growth of small ice crystals. After ice phase formation, riming, scavenging and aggregation may lead t...This paper investigated the possibility that aerosol particles are scavenged during the first and fast diffusional growth of small ice crystals. After ice phase formation, riming, scavenging and aggregation may lead to the collection of additional aerosol particles. Therefore, particles left after ice evaporation in hydrometeors, called ice residuals, may not currently be identical to ice nucleating particles. To overcome this problem, the largest ice crystals are removed during sampling in clouds and only crystals in the initial phase of growth, with diameters lower than 20 - 30 μm, are usually considered. Published papers assume that no aerosol scavenging takes place during the initial phase of growth of small ice crystals. The aim of this paper was to ascertain if this assumption is valid. Experiments were performed in a cold laboratory by considering ice crystals growing in the presence of supercooled droplets. Results showed that crystals can scavenge aerosol even in the first stage of growth. Theoretical considerations show that aerosol scavenging cannot be explained by Brownian diffusion, inertial impaction or interception processes. We suggest that the presence of aerosol in the pristine ice crystals may be due to diffusiophoretic force. During diffusive crystal growth, a flow called Stefan’s flow exists near the hydrometeor surface, driving the nearby aerosol particles towards the surface of the growing hydrometeors.展开更多
Measurements of ice crystal concentrations in mixed clouds tend to exceed ice nucleus concentrations measured in nearby clear air. This discrepancy is a source of uncertainty in climate change projections as the radia...Measurements of ice crystal concentrations in mixed clouds tend to exceed ice nucleus concentrations measured in nearby clear air. This discrepancy is a source of uncertainty in climate change projections as the radiative properties of mixed phase clouds are largely determined by their liquid and ice water content. The ice enhancement process can sometimes depend on secondary ice production, which can occur through ice crystal fracture during sublimation, cloud drop shattering during freezing or following collision with ice particles. However, the discrepancy is observed even in mixed clouds where only primary ice nucleation processes occur. Several hypotheses have been suggested for the observed discrepancies. One factor could be the existence in clouds of pockets of high vapor supersaturation formed by droplet freezing or removal of small droplets by collision with larger droplets, associated with the fact that ice crystal concentration increases with water supersaturation. However, ice crystal concentrations are usually measured at near water saturation. Additional factors could be drop freezing during evaporation and activation of droplet evaporation residues. Here we suggest that a major factor could be underestimation of the contact freezing mode as it is not measured in experimental campaigns and seldom considered in nucleation models. Laboratory experiments give only incomplete answers to the important questions concerning the contact freezing mode, e.g. what fraction of the aerosol particles that come into contact with the droplet surface results in a freezing event and what is the influence of particle type and size, air temperature and relative humidity. As supercooled droplets grow or evaporate in mixed clouds, phoretic forces should play an important role in the collision efficiency between aerosol and droplets, and consequently in contact freezing. A further question is the possibility that aerosol, usually not active in deposition or condensation/immersion freezing, can trigger ice nucleation by co展开更多
Thermophoresis and diffusiophoresis respectively refer to the directed drift of suspended particles in solutions with external thermal and chemical gradients, which have been widely used in the manipulation of mesosco...Thermophoresis and diffusiophoresis respectively refer to the directed drift of suspended particles in solutions with external thermal and chemical gradients, which have been widely used in the manipulation of mesoscopic particles. We here study a phoretic-like motion of a passive colloidal particle immersed in inhomogeneous active baths, where the thermal and chemical gradients are replaced separately by activity and concentration gradients of the active particles. By performing simulations, we show that the passive colloidal particle experiences phoretic-like forces that originate from its interactions with the inhomogeneous active fluid, and thus drifts along the gradient field, leading to an accumulation. The results are similar to the traditional phoretic effects occurring in passive colloidal suspensions, implying that the concepts of thermophoresis and diffusiophoresis could be generalized into active baths.展开更多
We simulate the self-assembly of active colloidal molecules from binary mixtures of spherical particles using a Brownian dynamics algorithm.These particles interact via phoretic interactions,which are determined by tw...We simulate the self-assembly of active colloidal molecules from binary mixtures of spherical particles using a Brownian dynamics algorithm.These particles interact via phoretic interactions,which are determined by two independently tunable parameters,surface activity and surface mobility.In systems composed of equal-size particles,we observe the formation of colloidal molecules with well-defined coordination numbers and spatial arrangement,which also display distinct dynamic functions,such as resting,translating,and rotating.By changing the size ratio to 2:1 between the two species,we further observe the formation of colloidal molecules with new structures arising from breaking the size symmetry.By tuning the mutual interactions between the smaller species via their surface mobility,we are able to control their spacing as well as the coordination number of the colloidal molecules.This study highlights the importance of tuning surface parameters and size asymmetry in controlling the structure and the active dynamics of colloidal molecules.展开更多
文摘The role of phoretic forces in providing in-cloud and below-cloud scavenging due to falling drop is reviewed by considering published papers dealing with theoretical models, laboratory and field measurements. Theoretical analyses agree that Brownian diffusion appears to dominate drop scavenging of aerosol with radius less than 0.1 μm, and inertial impaction dominates scavenging of aerosol with radius higher than 1 μm. Thus, there is a minimum collection efficiency for particles in the approximate range 0.1 μm - 1 μm, where phoretic forces are felt. Generally speaking, published papers report not uniform evaluations of the contribution of thermo- and diffusiophoretic forces. This disagreement is partially due to the different laboratory and field conditions, and different theoretical approaches.
文摘This paper investigated the possibility that aerosol particles are scavenged during the first and fast diffusional growth of small ice crystals. After ice phase formation, riming, scavenging and aggregation may lead to the collection of additional aerosol particles. Therefore, particles left after ice evaporation in hydrometeors, called ice residuals, may not currently be identical to ice nucleating particles. To overcome this problem, the largest ice crystals are removed during sampling in clouds and only crystals in the initial phase of growth, with diameters lower than 20 - 30 μm, are usually considered. Published papers assume that no aerosol scavenging takes place during the initial phase of growth of small ice crystals. The aim of this paper was to ascertain if this assumption is valid. Experiments were performed in a cold laboratory by considering ice crystals growing in the presence of supercooled droplets. Results showed that crystals can scavenge aerosol even in the first stage of growth. Theoretical considerations show that aerosol scavenging cannot be explained by Brownian diffusion, inertial impaction or interception processes. We suggest that the presence of aerosol in the pristine ice crystals may be due to diffusiophoretic force. During diffusive crystal growth, a flow called Stefan’s flow exists near the hydrometeor surface, driving the nearby aerosol particles towards the surface of the growing hydrometeors.
文摘Measurements of ice crystal concentrations in mixed clouds tend to exceed ice nucleus concentrations measured in nearby clear air. This discrepancy is a source of uncertainty in climate change projections as the radiative properties of mixed phase clouds are largely determined by their liquid and ice water content. The ice enhancement process can sometimes depend on secondary ice production, which can occur through ice crystal fracture during sublimation, cloud drop shattering during freezing or following collision with ice particles. However, the discrepancy is observed even in mixed clouds where only primary ice nucleation processes occur. Several hypotheses have been suggested for the observed discrepancies. One factor could be the existence in clouds of pockets of high vapor supersaturation formed by droplet freezing or removal of small droplets by collision with larger droplets, associated with the fact that ice crystal concentration increases with water supersaturation. However, ice crystal concentrations are usually measured at near water saturation. Additional factors could be drop freezing during evaporation and activation of droplet evaporation residues. Here we suggest that a major factor could be underestimation of the contact freezing mode as it is not measured in experimental campaigns and seldom considered in nucleation models. Laboratory experiments give only incomplete answers to the important questions concerning the contact freezing mode, e.g. what fraction of the aerosol particles that come into contact with the droplet surface results in a freezing event and what is the influence of particle type and size, air temperature and relative humidity. As supercooled droplets grow or evaporate in mixed clouds, phoretic forces should play an important role in the collision efficiency between aerosol and droplets, and consequently in contact freezing. A further question is the possibility that aerosol, usually not active in deposition or condensation/immersion freezing, can trigger ice nucleation by co
基金Project supported by the National Natural Science Foundation of China (Grant No. 11874397)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB33000000)。
文摘Thermophoresis and diffusiophoresis respectively refer to the directed drift of suspended particles in solutions with external thermal and chemical gradients, which have been widely used in the manipulation of mesoscopic particles. We here study a phoretic-like motion of a passive colloidal particle immersed in inhomogeneous active baths, where the thermal and chemical gradients are replaced separately by activity and concentration gradients of the active particles. By performing simulations, we show that the passive colloidal particle experiences phoretic-like forces that originate from its interactions with the inhomogeneous active fluid, and thus drifts along the gradient field, leading to an accumulation. The results are similar to the traditional phoretic effects occurring in passive colloidal suspensions, implying that the concepts of thermophoresis and diffusiophoresis could be generalized into active baths.
基金the Innovation Program of Guangdong Provincial Department of Education,China(Grant No.2019KTSCX148)the Science and Technology Innovation Commission of Shenzhen(Grant No.JCYJ20170818141727254).
文摘We simulate the self-assembly of active colloidal molecules from binary mixtures of spherical particles using a Brownian dynamics algorithm.These particles interact via phoretic interactions,which are determined by two independently tunable parameters,surface activity and surface mobility.In systems composed of equal-size particles,we observe the formation of colloidal molecules with well-defined coordination numbers and spatial arrangement,which also display distinct dynamic functions,such as resting,translating,and rotating.By changing the size ratio to 2:1 between the two species,we further observe the formation of colloidal molecules with new structures arising from breaking the size symmetry.By tuning the mutual interactions between the smaller species via their surface mobility,we are able to control their spacing as well as the coordination number of the colloidal molecules.This study highlights the importance of tuning surface parameters and size asymmetry in controlling the structure and the active dynamics of colloidal molecules.
