scholarly journals Mesoscopic surface roughness of ice crystals pervasive across a wide range of ice crystal conditions

2014 ◽  
Vol 14 (22) ◽  
pp. 12357-12371 ◽  
Author(s):  
N. B. Magee ◽  
A. Miller ◽  
M. Amaral ◽  
A. Cumiskey

Abstract. Here we show high-magnification images of hexagonal ice crystals acquired by environmental scanning electron microscopy (ESEM). Most ice crystals were grown and sublimated in the water vapor environment of an FEI-Quanta-200 ESEM, but crystals grown in a laboratory diffusion chamber were also transferred intact and imaged via ESEM. All of these images display prominent mesoscopic topography including linear striations, ridges, islands, steps, peaks, pits, and crevasses; the roughness is not observed to be confined to prism facets. The observations represent the most highly magnified images of ice surfaces yet reported and expand the range of conditions in which rough surface features are known to be conspicuous. Microscale surface topography is seen to be ubiquitously present at temperatures ranging from −10 °C to −40 °C, in supersaturated and subsaturated conditions, on all crystal facets, and irrespective of substrate. Despite the constant presence of surface roughness, the patterns of roughness are observed to be dramatically different between growing and sublimating crystals, and transferred crystals also display qualitatively different patterns of roughness. Crystals are also demonstrated to sometimes exhibit inhibited growth in moderately supersaturated conditions following exposure to near-equilibrium conditions, a phenomenon interpreted as evidence of 2-D nucleation. New knowledge about the characteristics of these features could affect the fundamental understanding of ice surfaces and their physical parameterization in the context of satellite retrievals and cloud modeling. Links to supplemental videos of ice growth and sublimation are provided.

2014 ◽  
Vol 14 (6) ◽  
pp. 8393-8418 ◽  
Author(s):  
N. B. Magee ◽  
A. Miller ◽  
M. Amaral ◽  
A. Cumiskey

Abstract. Here we show high-magnification images of hexagonal ice crystals acquired by Environmental Scanning Electron Microscopy (ESEM). Most ice crystals were grown and sublimated in the water vapor environment of an FEI-Quanta-200 ESEM, but crystals grown in a laboratory diffusion chamber were also transferred intact and imaged via ESEM. All of these images display prominent mesoscopic topography including linear striations, ridges, islands, steps, peaks, pits, and crevasses; the roughness is not observed to be confined to prism facets. The observations represent the most highly magnified images of ice surfaces yet reported and expand the range of conditions where the rough surface features are known to be conspicuous. Microscale surface topography is seen to be ubiquitously present at temperatures ranging from −10 °C to −40 °C, at super-saturated and sub-saturated conditions, on all crystal facets, and irrespective of substrate. Despite the constant presence of surface roughness, the patterns of roughness are observed to be dramatically different between growing and sublimating crystals, and transferred crystals also display qualitatively different patterns of roughness. Crystals are also demonstrated to sometimes exhibit inhibited growth in moderately supersaturated conditions following exposure to near-equilibrium conditions, a phenomena interpreted as evidence of 2-D nucleation. New knowledge of the characteristics of these features could affect the fundamental understanding of ice surfaces and their physical parameterization in the context of satellite retrievals and cloud modeling. Links to Supplement videos of ice growth and sublimation are provided.


Molecules ◽  
2021 ◽  
Vol 27 (1) ◽  
pp. 258
Author(s):  
Elzbieta Pach ◽  
Albert Verdaguer

Scanning electron microscopy (SEM) is a powerful imaging technique able to obtain astonishing images of the micro- and the nano-world. Unfortunately, the technique has been limited to vacuum conditions for many years. In the last decades, the ability to introduce water vapor into the SEM chamber and still collect the electrons by the detector, combined with the temperature control of the sample, has enabled the study of ice at nanoscale. Astounding images of hexagonal ice crystals suddenly became real. Since these first images were produced, several studies have been focusing their interest on using SEM to study ice nucleation, morphology, thaw, etc. In this paper, we want to review the different investigations devoted to this goal that have been conducted in recent years in the literature and the kind of information, beyond images, that was obtained. We focus our attention on studies trying to clarify the mechanisms of ice nucleation and those devoted to the study of ice dynamics. We also discuss these findings to elucidate the present and future of SEM applied to this field.


2006 ◽  
Vol 63 (5) ◽  
pp. 1513-1525 ◽  
Author(s):  
Valery Shcherbakov ◽  
Jean-François Gayet ◽  
Brad Baker ◽  
Paul Lawson

Abstract During the South Pole Ice Crystal Experiment, angular scattering intensities (ASIs) of single ice crystals formed in natural conditions were measured for the first time with the polar nephelometer instrument. The microphysical properties of the ice crystals were simultaneously obtained with a cloud particle imager. The observations of the scattering properties of numerous ice crystals reveal high variability of the ASIs in terms of magnitude and distribution over scattering angles. To interpret observed ASI features, lookup tables were computed with a modified ray tracing code, which takes into account the optical geometry of the polar nephelometer. The numerical simulations consider a wide range of input parameters for the description of the ice crystal properties (particle orientation, aspect ratio, surface roughness, and internal inclusions). A new model of surface roughness, which assumes the Weibull statistics, was proposed. The simulations reproduce the overwhelming majority of the observed ASIs features and trace very well the quasi-specular reflection from crystal facets. The discrepancies observed between the model and the experimental data correspond to the rays, which pass through the ice crystal and are scattered toward the backward angles. This feature may be attributed to the internal structure of the ice crystals that should be considered in modeling refinements.


2016 ◽  
Vol 9 (8) ◽  
pp. 3817-3836 ◽  
Author(s):  
Naruki Hiranuma ◽  
Ottmar Möhler ◽  
Gourihar Kulkarni ◽  
Martin Schnaiter ◽  
Steffen Vogt ◽  
...  

Abstract. Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters (< 5 µm). Here, for the first time we describe a development of an ice-selecting PCVI (IS-PCVI) to separate ice in controlled mixed-phase cloud system based on the particle inertia with the cut-off diameter  ≥  10 µm. We also present its laboratory application demonstrating the use of the impactor under a wide range of temperature and humidity conditions. The computational fluid dynamics simulations were initially carried out to guide the design of the IS-PCVI. After fabrication, a series of validation laboratory experiments were performed coupled with the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) expansion cloud simulation chamber. In the AIDA chamber, test aerosol particles were exposed to the ice supersaturation conditions (i.e., RHice > 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter  ≥  10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of  ~ 10–30 µm in diameter with small inadvertent intrusion (~  5 %) of unwanted particles.


2017 ◽  
Vol 10 (12) ◽  
pp. 4639-4657 ◽  
Author(s):  
Jake Zenker ◽  
Kristen N. Collier ◽  
Guanglang Xu ◽  
Ping Yang ◽  
Ezra J. T. Levin ◽  
...  

Abstract. We have developed a new method to determine ice nucleating particle (INP) concentrations observed by the Texas A&amp;M University continuous flow diffusion chamber (CFDC) under a wide range of operating conditions. In this study, we evaluate differences in particle optical properties detected by the Cloud and Aerosol Spectrometer with POLarization (CASPOL) to differentiate between ice crystals, droplets, and aerosols. The depolarization signal from the CASPOL instrument is used to determine the occurrence of water droplet breakthrough (WDBT) conditions in the CFDC. The standard procedure for determining INP concentration is to count all particles that have grown beyond a nominal size cutoff as ice crystals. During WDBT this procedure overestimates INP concentration, because large droplets are miscounted as ice crystals. Here we design a new analysis method based on depolarization ratio that can extend the range of operating conditions of the CFDC. The method agrees reasonably well with the traditional method under non-WDBT conditions with a mean percent error of ±32.1 %. Additionally, a comparison with the Colorado State University CFDC shows that the new analysis method can be used reliably during WDBT conditions.


2016 ◽  
Vol 113 (7) ◽  
pp. 1749-1753 ◽  
Author(s):  
Harutoshi Asakawa ◽  
Gen Sazaki ◽  
Ken Nagashima ◽  
Shunichi Nakatsubo ◽  
Yoshinori Furukawa

Surfaces of ice are covered with thin liquid water layers, called quasi-liquid layers (QLLs), even below their melting point (0 °C), which govern a wide variety of phenomena in nature. We recently found that two types of QLL phases appear that exhibit different morphologies (droplets and thin layers) [Sazaki G. et al. (2012) Proc Natl Acad Sci USA 109(4):1052−1055]. However, revealing the thermodynamic stabilities of QLLs remains a longstanding elusive problem. Here we show that both types of QLLs are metastable phases that appear only if the water vapor pressure is higher than a certain critical supersaturation. We directly visualized the QLLs on ice crystal surfaces by advanced optical microscopy, which can detect 0.37-nm-thick elementary steps on ice crystal surfaces. At a certain fixed temperature, as the water vapor pressure decreased, thin-layer QLLs first disappeared, and then droplet QLLs vanished next, although elementary steps of ice crystals were still growing. These results clearly demonstrate that both types of QLLs are kinetically formed, not by the melting of ice surfaces, but by the deposition of supersaturated water vapor on ice surfaces. To our knowledge, this is the first experimental evidence that supersaturation of water vapor plays a crucially important role in the formation of QLLs.


2016 ◽  
Author(s):  
Naruki Hiranuma ◽  
Ottmar Möhler ◽  
Gourihar Kulkarni ◽  
Martin Schnaiter ◽  
Steffen Vogt ◽  
...  

Abstract. Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large size cloud hydrometeors is difficult mainly due to its small cut-size diameters (< 5 µm). Here, for the first time we describe a development of an ice-selecting PCVI (IS-PCVI) to separate ice in the controlled mixed-phase cloud system based on the particle inertia with the cut-off diameter > 10 µm. We also present its laboratory application demonstrating the use of the impactor under a wide range of temperature and humidity conditions. The computational fluid dynamics (CFD) simulations were initially carried out to guide the design of the IS-PCVI. After fabrication, a series of validation laboratory experiments were performed coupled with the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) expansion cloud simulation chamber. In the AIDA chamber, test aerosol particles were exposed to the ice supersaturation conditions (i.e., RHice > 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of size ≥ 10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of ~ 10–30 µm in diameter with small inadvertent intrusion (~ 5 %) of unwanted particles.


2010 ◽  
Vol 10 (6) ◽  
pp. 2927-2935 ◽  
Author(s):  
W. C. Pfalzgraff ◽  
R. M. Hulscher ◽  
S. P. Neshyba

Abstract. We present the first clearly resolved observations of surfaces of growing and ablating hexagonal ice crystals using variable-pressure scanning electron microscopy. The ice surface develops trans-prismatic strands, separated from one another by distances of 5–10 μm. The strands are present at a wide range of supersaturations, but are most pronounced at temperatures near the frost point. Pyramidal facets consistent with Miller-Bravais indices of 1011, and possibly also 2021, are associated with ice growth under these conditions. A molecular-dynamics model of a free-standing ice Ih nanocolumn containing 8400 water molecules does not develop trans-prismatic strands, suggesting these features originate at larger spatial or temporal scales. The possible relevance of these surface features to cirrus ice is discussed.


2017 ◽  
Author(s):  
Jake Zenker ◽  
Kristen N. Collier ◽  
Guanglang Xu ◽  
Ping Yang ◽  
Ezra J. T. Levin ◽  
...  

Abstract. We have developed a new method to determine ice nucleating particle (INP) concentrations observed by a Continuous Flow Diffusion Chamber (CFDC) under a wide range of operating conditions. In this study, we evaluate differences in particle optical properties detected by the Cloud and Aerosol Spectrometer with POLarization (CASPOL) to differentiate between ice crystals, droplets, and aerosols. The depolarization signal from the CASPOL instrument is used to determine the occurrence of water droplet breakthrough (WDBT) conditions in the CFDC, under which traditional determination of ice nucleating particle concentrations by size discrimination fails. To overcome the challenge of WDBT, we design a new analysis method using depolarization ratio that can extend the range of operating conditions of the CFDC. The method agrees reasonably well with the traditional method under non-WDBT conditions with a mean percent error of ±32.1 %. Additionally, a comparison with the Colorado State University (CSU) CFDC shows that the new analysis method can be used reliably during WDBT conditions.


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