August 1976 T.

Gonda 233

The Growth of Small Ice Crystals in Gases

of High and Low Pressures

By Takehiko Gonda

Faculty of Science and Technology, Science University of Tokyo, Noda, Chiba, Japan
(Manuscript received 11, December 1975, in revised form 3, June 1976)

Abstract

The habit and the growth feature of small ice crystals formed in a free fall state in
high- and low-pressure helium and argon gases at the temperatures of -7 and -15* were
studied experimentally. It is found that the habit and the growth feature of small ice crystals
in the range of about 20 to 50 *m depend not only on the temperature and the degree of
supersaturation but also on the kind and the pressure of the carrier gas and the size of
crystals when small ice crystals were formed at water saturation. It is found that the
dependence of the habit of small ice crystals on temperature is more emphasized under a
high pressure but has a tendency to vanish under a low pressure. In high-pressure gas, ice
crystal shapes which have never been observed in the earth's atmospheres are found. Such
ice crystals may form in the atmospheres of Jupiter and Saturn where pressures are higher
than that of the earth.

However, the experiment was carried out only

1. Introduction
in the gases below 1 atm. So, it is difficult to
Consolidating the experimental results obtained predict the habit and the growth feature of small
by Nakaya (1954) and Hallett and Mason (1958) ice crystals grown in high-pressure gas from only
and by himself, Kobayashi (1961) considered that the investigation about those of small ice crystals
the habit of snow crystals was determined by the grown in the gas below 1 atm. Moreover, it is
temperature while the growth feature was deter- difficult to universalize the effects of the kind and
mined by the degree of supersaturation. How- the pressure of carrier gas on the habit and the
ever, Isono (1957) considered that the ice crystal growth feature of ice crystals. Therefore, the
habit was influenced by the environmental factors effects of the kind and the pressure of carrier gas
around the crystals. The environmental factors on the habit and the growth feature of small ice
around the crystals are not only the temperature crystals were studied by forming ice crystals in
and the degree of supersaturation but also the high-pressure gas. The first purpose of the pres-
diffusion field of water vapor and the field of ent study is to form small ice crystals in high
heat conduction. In the case of experiments of pressure gases with small vapor diffusivity and
van den Heuvel and Mason (1959) and Koba- to compare the obtained results with those in low
yashi (1958), the effects of the kind and the pressure gases with large vapor diffusivity. The
pressure of the carrier gas on ice crystal habit second is to examine experimentally the shapes of
did not occur. Komabayashi (1970) calculated snow crystals which may form in the atmospheres
theoretically and found that the effect of diffusion of Jupiter and Saturn as have been estimated
coefficient on the shape of ice crystals was large thermodynamically by Weidenschilling and Lewis
when the size of the ice crystal was small, but (1973).
the effect was small when the size of the crystals
became large. According to the experiment made 2. Experimental conditions for the growth of ice
by the author and Komabayashi (1971), the habit crystals
and the growth feature of small ice crystals have The high-pressure cold chamber for this study
depended markedly on the diffusion coefficient of was fully described in the previous paper (Gonda,
water vapor. 1975). Preliminary experiments to form super-
234 Journal of the Meteorological Society of Japan Vol. 54, No. 4

cooled water fog in the chamber were carried out within 2 minutes after the seeding had been about
2 to 3 times before the actual measurements were 115% respect to ice at the temperature of -15*.
done. The vapor pressure in the chamber reached The reasons why helium and argon gases were
to above 90% with respect to ice when this ope- used in this experiment are as follows. The first
ration was done. At the temperature of -15*, is because the vapor diffusivity and the thermal
water vapor was supplied for about 8 to 10 conductivity of helium gas are largely different
minutes in the gas at 1 atm and about 15 minutes from those of argon gas. The second is because
in the gases at high- and low-pressures. After a a great deal of helium and argon gases may exist
stirrer was rotated for about 10 seconds, the small in the planetary atmospheres. Physical constants
amount of silver iodide smoke was supplied in of these gases are shown in Tables 1 and 2. It is
the chamber. Then, small ice crystals were form- understood from these tables that the coefficient
ed in dense supercooled water fog, that is, at of viscosity of helium and argon gases is not
water saturation. The fact that the vapor pres- largely different. Therefore, the fall velocity of
sure in the chamber was maintained at water an ice crystal of a given size in helium is nearly
saturation for about 2 minutes was confirmed by equal to that in argon. The mean size of ice
the detection method described below. At first, crystals formed in helium gas under atmospheric
the chamber was filled with dense fog for 2 to 3 pressure at -15* and at water saturation was
minutes after the seeding. Secondly, both super- about 50*m. As both the crystal size and the
cooled water droplets and ice crystals fallen on a fall velocity are small, ice crystals fell approxi-
glass plate did not evaporate for a long time. mately according to Stoke's law. In order to ex-
Thirdly, it was confirmed by the use of a hygro- clude ice crystals which may have been formed
meter that the vapor pressure in the chamber below water saturation, only the ice crystals
fallen within 2 minutes after the seeding were
Table 1. Physical constants of helium chosen to study the habit and the growth feature
gas at 0* as a function of of ice crystals.
pressure (Hirschfelder et al,
1966). 3. Variation of the growth feature of small ice
crystals formed in helium with pressure
Microphotographs of ice crystals which were
formed with the highest frequency in helium gas
at -7 and -15* at water saturation are shown
in Fig. 1 and the frequency of their occurrences
is shown in Fig. 2. At the pressures higher than
10 atm at -7*, as shown in these figures, the
predominant growth feature of ice crystals form-
ed in the gas were deeply hollowed prisms which
had grown preferentially along the c-axis (sheath-
like crystals) and slim needle-like crystals with
small projections from each corner of the prisms.
Table 2. Physical constants of argon Ice crystals formed predominantly in the gas with
gas at 0°C as a function of pressure lower than 5 atm but higher than 1 atm
pressure (Hirschfelder et al, at -7* were prisms with skeletal structures. At
1966).
pressures lower than 1 atm prisms with no
skeletal structures were formed with the highest
frequency in the gas. At pressures higher than
5 atm, needles were formed with a relatively
small frequency at -7*. At the normal and
lower pressures, needles were not present.
Ice crystals formed predominantly in the gas
with pressure higher than 5 atm at -15* and
at water saturation were thin plane crystals with
dendritic development at both the top and the
bottom of a center prism (double plate). The
frequency with which these crystals were formed
August 1976 T. Gonda 235

Fig. 1 Ice crystals formed predominantly in helium gas

at various pressures at -7 (left column) and -15*
(right column).

Fig. 2 The statistical frequency of the growth feature

of ice crystals formed in helium gas at various
pressures at -7 and -15*.

increases with increasing pressure of the gas. thick single plates with no skeletal structures. As
Generally speaking, the interior structures at the can be seen in Fig. 2, the growth feature of ice
central part of the ice crystals formed in high- crystals formed at -7 and -15* depends on the

pressure helium are very complicated. On the pressure of the gas.

other hand, the interior structures at the edges The size of ice crystals with each growth fea-
or the corners of these crystals are comparatively ture formed in helium at -15* is plotted against
simple. The predominant growth feature of ice the vapor diffusivity in Fig. 3. It can be seen from
crystals formed in the gas lower than 1 atm at the figure that the size of ice crystals with each
-15* and at water saturation was solid plates . growth feature increases with increasing vapor
These crystals were not double plates but very diffusivity. In the figure, the size of the dendrite
236 Journal of the Meteorological Society of Japan Vol. 54, No. 4

gases at -7 and -15* and at water saturation

are shown in Fig. 4, and the frequency of their
occurrences is shown in Fig. 5. It can be seen
in these figures that prisms were formed pre-
dominantly at all pressures of argon gas at -7*
and at water saturation, but hollow prisms were
formed predominantly in high-pressure argon
gas. On the other hand, solid prisms were formed
predominantly at pressures lower than 1 atm. At
the normal pressure, needles were formed in
argon at -7*. This is different from the case
of helium.
The predominant growth feature of ice crystals
Fig. 3 The size of ice crystals with each formed in argon gas higher than 5 atm at -15*
growth feature formed in helium was thin plane crystals with dendritic develop-
gas at -7* versus the vapor dif- ment at both the top and the bottom of a center
fusivity.
prism. The predominant growth features of ice
crystals formed in low-pressure argon at -15*
is the largest, that of the stellar is medium and and at water saturation were skeleton plate and
that of the skeleton plate is the smallest at smaller solid plate. The growth features of ice crystals
vapor diffusivity at -15*. formed in high- and low-pressure argon at -15*
Next, the size of the stellar is the largest, that have nearly the same feature as those of helium
of skeleton plate is medium and that of the solid at -15*. However, in argon gas at normal pres-
sure at -15*, dendrite was formed with a small
plate is the smallest at larger vapor diffusivity at
-15* . The facts shown in the figure mean that frequency at 1 atm while no dendrite was seen
the growth feature of small ice crystals depends in helium gas at normal pressure. No solid plate
not only on the pressure of the carrier gas but was formed in argon at normal pressure, while
also on the size of crystals. it was observed in helium with a small frequency
at -15*. It can be understood from these ex-
4. Variation of the growth feature of small ice
perimental results at -7 and -15* that the
crystals formed in argon with pressure
growth features of ice crystals formed in argon
Ice crystals predominantly formed in argon are a little different from those in helium.

Fig. 4 Ice crystals formed predominantly in argon gas

at various pressures at -7 (left column) and -15*
(right column).
August 1976 T. Gonda 237

Fig. 5 The statistical frequency of the growth feature of

ice crystals formed in argon gas at various pres-
sures at -7 and -15*.

increases. This means that the habit as well as

5. Variation of the habit of small ice crystals the growth feature of small ice crystals depends
with pressure on the pressure of the carrier gas.
Fig. 6 shows the mean values of the ratio of As seen in the figure, the relationship between
the lengths along the c- and a-axes of small ice the values of c/ a in argon and the vapor dif-
crystals formed in helium (open circles) and argon fusivity is nearly the same tendency as that in
(solid circles) at -7 and -15* plotted against helium. However, the values of c/ a in argon
the vapor diffusivity. As seen in the figure, the are closer to unity than those in helium at the
smaller the vapor diffusivity is, the further the same vapor diffusivity.
values of c/a of ice crystals in helium at -7 and
-15* deviate from unity. That is, the smaller 6. Discussions
the vapor diffusivity is, the more the dependence
The habit and the growth feature of snow
of the habit on the temperature is enhanced.
crystals with size above about 1 mm can not be
Meanwhile, the dependence of the habit on tem-
compared simply with those of small ice crystals
perature almost vanishes as the vapor diffusivity whose sizes are below about 50 *m because the
habit and the growth feature depend on the size
of crystals. However, in order to clarify physical
meanings of experimental results, let us dare to
compare the habit and the growth feature of snow
crystals with those of small ice crystals. It is well
known that when the supersaturation over ice is
small, short solid prisms and thick solid plates
with no skeletal structures form in the case of
snow crystals at -7 and -15*, respectively.
When the supersaturation over ice is large,
needles, long prisms, sheath-type crystals, thin
Fig. 6 The mean values of the ratio of
plates and complicated dendrites form in the case
the lengths along the c- and the
of snow crystals. In the case of small ice crystals,
a- axes of ice crystals at -7 and
-15* versus the vapor diffu- in helium and argon gases at normal pressure no

sivity (open circles: in helium complicated dendritec structures are observed, nor

gas, solid circles: in argon gas). sheath-like crystals are observed. No needles are
 238 Journal of the Meteorological Society of Japan Vol. 54, No. 4

observed under the same condition. On the con-the gas having larger thermal conductivity when
trary, in high-pressure helium and argon gases, the vapor diffusivity is constant. The details of
slim needle-like crystals, sheath-like crystals, thin physical meanings of obtained results will be de-
complicated dendrites with the secondary armsscribed in other paper.
and thin stellar-type crystals are observed on According to the thermodynamical calculations
small ice crystals below about 50 *m. When the by Weidenschilling and Lewis (1973), it was
vapor diffusivity increases, the size of the ice speculated that ice clouds formed in the mixture
crystals increases and the growth features of the of hydrogen and helium of about 20 atmat-15*
crystals are more simplified. in the jupiter's atmospheres. Moreover, it was
That is, short solid
prisms and thick solid plates form at a large speculated that ice clouds formed in the saturn's
vapor diffusivity. atmospheres of the mixture of hydrogen and
Fig. 7 illustrates the schematic diagram of the helium of about 15 atm at -15*. The shapes
habit and the growth feature of the small ice of ice crystals which may grow in these planetary
crystals formed in the present experiment versus atmospheres at high pressure may be of dendritic
the temperature and the vapor diffusivity. It can structures with secondary branches even at the
be seen from the figure that the dependence of same size which allows only solid plate growth
the habit on temperature is more pronounced at in the earth's atmosphere. Especially, the small
a smaller vapor diffusivity, while less at a larger dendrites may be double plates whose size at the
vapor diffusivity. The schematic diagram of the top of a center prism is largely different from
habit and the growth feature of small ice crystals the size at the bottom. Therefore, it is supposed
grown at -7 and -15* versus the vapor dif- that the central part of small ice crystals growing
fusivity and the thermal conductivity are shown
in Figs. 8(a) and (b), respectively. In Fig. 8(a),
the skeleton column forms predominantly in
helium at -7* when the vapor diffusivity is
about 0.9 cm2 •sec-1. On the other hand, the solid
column of which the axial ratio c/a is close to
unity forms predominantly in argon at -7* at
the same vapor diffusivity. In Fig . 8(b), the
skeleton plate forms predominantly in helium at
-15* when the vapor diffusivity is about
0.9 cm2 •sec-1. Meanwhile, the solid plate of which
the axial ratio c/ a is close to unity forms pre-
dominantly in argon at -15* at the same vapor
diffusivity. The observations described above
mean that the habit and the growth feature of
ice crystals grown in the gas having smaller ther-
mal conductivity is more simplified than those in

Fig. 8 Schematic diagram of the habit

and the growth feature of small
Fig. 7 Schematic diagram of the habit ice crystals with respect to the
and the growth feature of small vapor diffusivity and the thermal
ice crystals with respect to the conductivity.
temperature and the vapor dif- (a) at -7°C
fusivity. (b) at -15°C
 August 1976 T. Gonda 239

in these planetary atmospheres is very complicat-

Acknowledgements
ed and the interior structures of the edges and
The author wishes to express his deep thanks
corners of the crystals are simple.
to Prof. M. Komabayashi, Meteorological college
7. Conclusion of Japan Meteorological Agency for reading of
the manuscript and many helpful suggestions and
Small ice crystals were grown in high-pressure
continuing discussions and encouragement. The
gases of 15 atm. The habit and the growth fea-
ture of the ice crystals were studied by means of author is also deeply indebted to Prof. K. Isono,
Nagoya University for helpful advice and en-
photomicrographs. Ice crystals grown in high-
couragement during the course of this work.
pressure gases had very complicated shapes which
had never been found in the earth's atmosphere.
References
The experiments of the growth of ice crystals in
high- and low-pressure gases were carried out by Gonda, T. and M. Komabayashi, 1971: Skeletal and
dendritic structures of ice crystals as a function
the use of the same cold chamber and the ob-
of thermal conductivity and vapor diffusivity. J.
tained results are follows.
Meteor. Soc. Japan, 49, 32-42.
It has been found that the earlier conclusion Gonda, T., 1975: A high-pressure cold chamber for
that the habit and the growth feature of ice the study of ice crystal growth in compressed
crystals do not depend on the kind and the pres- gases. J. Meteor. Soc. Japan, 53, 322-327.
sure of the carrier gas but on the temperature Hallett, J., and B. J. Mason, 1958: The influence of
and supersaturation (van den Heuvel and Mason, temperature and supersaturation on the habit of
1959) does not apply to ice crystals smaller than ice crystals grown from the vapor. Proc. Roy.
50 *m. The habit and the growth feature of Soc. A, 247, 440-453.
Hirschf elder, J. 0., C. F. Curtiss and R. B. Bird,
small ice crystals in the range of about 20 to
1966: Molecular theory of gases and liquids. The
50 *m depend not only on the temperature and
3rd edition, John Wiley.
supersaturation but also on the kind and the pres-
Isono, K., 1957: On the growth of ice crystals in
sure of the carrier gas and the size of crystals the air. J. Meteor. Soc. Japan, 75th Ann. Vol.,
in the case of ice crystals formed at water satura- 31-37.
tion. It has been found that the dependence of Kobayashi, T., 1958: On the habit of snow crystals
the habit of small ice crystals on temperature is artificially produced at low pressure. J. Meteor.
more enhanced at a high-pressure but have a Soc. Japan, 36, 193-208.
tendency to vanish at a low-pressure. Moreover, it 1961: The growth of snow crystals at low
has been found that the habit and the growth supersaturation. Phil. Mag., 6, 1363-1370.
Komabayashi, M., 1970: Shape instability of crystals
feature of ice crystals grown in the gas having
of ice, carbon dioxide and ammonia grown in a
smaller thermal conductivity is more simplified
cold chamber. J. Meteor. Soc. Japan, 48, 270-
than those in the gas having larger thermal con-
286.
ductivity when the vapor diffusivity is constant. Nakaya, U., 1954: Snow crystals, natural and arti-
The temperature and the pressure used in this ficial. Harvard Univ. Press, 248-252.
experiment are nearly equal to those of the Van den Heuvel, A. P, and B. J. Mason, 1959:
formation of ice clouds which may exist in the Habit of ice crystals grown in hydrogen, carbon
atmospheres of Jupiter and Saturn. Therefore, dioxide and air at reduced pressure. Nature , 185,
the shapes of ice crystals obtained by this experi- 519-520.
Weidenschilling, S. T. and J. S. Lewis, 1973: Atmos-
ment may be usable for the study of the clouds
pheric and cloud structures of the Jovian planets.
of Jupiter and Saturn. Icarus, 20, 465-476.
240 Journal of the Meteorological Society of Japan Vol. 54, No. 4

高 圧 気体 及 び低 圧 気体 中 に於 け る
氷 晶の成長

権 田 武 彦
東京理科大学理工学部
-7*と-15*の 温 度 で ヘ リ ウム とア ル ゴ ンの 高圧 気 体 中 と低 圧 気 体 中 で 成 長 した 氷 晶 の 晶 相 と成 長 型 が 実 験
的 に 調 べ られ た 。 そ の結 果,約20*mか ら50*mま で の 氷 晶 の 晶 相 と成 長 型 は,水 飽 和 の下 で は,温 度 と過飽 和 度
の み で は な く,気 体 の種 類 と圧 力,更 に 結 晶 の大 き さに も依 存 す る事 が わ か った 。-7*の 下 で 成 長 す る氷 晶 は,高
圧 気 体 中 即 ち 水 蒸気 の拡 散 係数 の小 さ い 領域 で は,晶 相 の温 度 依 存 性 が一 層 強調 され,氷 晶 は,C軸 方向に優先的に
成 長 し,同 時 に 氷 晶 の 角又 は縁 が優 先 的 に成 長 し,成 長 型 は,復 雑 化す る。 即 ち,高 圧 気 体 中 で成 長 す る 氷 晶 は,細
い さや 状 結 晶 又 は,針 状 結 晶 が卓 越 す る 。一 方,低 圧 気 体 中 即 ち,水 蒸気 の拡 散 係数 の 大 きい 領域 で は,晶 相 の 温 度
依 存 性 が 消え て,軸 比 が1に 近 づ き,同 時 に,氷 晶 の角 又 は 縁 で の優 先 的 成 長 も消え て成 長 型 は,単 純 化 す る。 即 ち
低 圧 気 体 中 で 成 長 す る 氷 晶 は,a軸 とC軸 の軸 比 が1に 近 い 無 垢 の 結 晶 で あ る。
15*で 成 長 す る 氷 晶 は,高 圧 気体 中 で は,-7*の 場 合 と同 様 に,晶 相-の 温 度 依 存 性 が 一 層 強 調 され,氷 晶
は,a軸 方 向 に優 先 的 に 成 長 し,同 時 に成 長 型 も復 雑化 す る。 即 ち,-15*の 高 圧 気 体 中 で 成 長 す る氷 晶 は,第2
枝 を 持 っ,つ づ み 型 の 薄 い 樹 枝 状 結 晶 又 は 第2枝 を 持 つ 薄 い 六 花 状 結 晶 が 卓 越 す る。一 方,低 圧 気体 中 で は,一7*
の場 合 と同 様 に,晶 相 の 温 度 依 存 性 が 消え,同 時 に 成 長 型 も単 純 化 す る。 即ち,-15*の 低 圧 気 体 中 で 成 長 す る氷
晶は,軸 比 が1に 近 い 無 垢 の 結 晶 で あ る。
ヘ リ ウ ム と ア ル ゴ ソ気 体 中 で 成 長 した 氷 晶 を 比 べ て み る と,そ の晶 相 と成 長 型 の形 成 頻 度 が,少 し異 る事 が わ か っ
た 。 高 圧 気 体 中 で 成 長 した 氷 晶 の中 に は,地 球 よ りも大 気 圧 の高 い 木 星 や 土 星 の大 気 中 で 成 長 して い る と思 わ れ る結

晶が み つ か った 。