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The Impact of Mesoscale Gravity Waves on Homogeneous Ice Nucleation in Cirrus Clouds

28 May 2019-Geophysical Research Letters (John Wiley & Sons, Ltd)-Vol. 46, Iss: 10, pp 5556-5565
TL;DR: In this article, the effects of mesoscale gravity waves on homogeneous aerosol freezing in midlatitude cirrus are studied by means of parcel model simulations that are driven by random vertical wind speeds constrained by balloon measurements.
Abstract: Effects of a spectrum of mesoscale gravity waves on homogeneous aerosol freezing in midlatitude cirrus are studied by means of parcel model simulations that are driven by random vertical wind speeds constrained by balloon measurements. Stochastic wave forcing with mean updraft speeds of 5–20 cm/s leads to substantial nucleated ice crystal number concentrations (ICNC) of 0.1–1 cm−3 in situations with slow large-scale cooling, which by itself would generate fewer ice crystals. The stochastic nature of wave-driven air parcel temperatures enhances ICNC even further, but the times required to reach freezing conditions unsupported by large-scale cooling may vary widely. In the presence of wave forcing, ice crystals with low ICNC (<1–10 L−1) are also generated by homogeneous freezing, albeit only rarely. Comparisons with aircraft measurements suggest significant influences of heterogeneous ice-nucleating particles and ice crystal sedimentation on ICNC, but quantifying their individual contributions remains elusive. Plain Language Summary Spontaneous freezing of airborne, water-containing particles below −38 ◦C is a fundamental pathway to form ice crystals in high-altitude cirrus clouds. This ice formation process has been well researched and was the first represented in weather forecast and climate models to advance cirrus predictions. One key characteristic is its strong dependence of the number of ice crystals formed on the cooling rate of air. Recent observations show that rapid cooling rates are generated by ubiquitous gravity waves. Here, we explore the rich suite of phenomena taking place during cirrus formation caused by a spectrum of gravity waves. We find that wave effects should be considered in future model simulations, when comparing model results with observations, and in parameterizations of cloud ice crystal formation.

Summary (2 min read)

1. Introduction

  • Mesoscale air motion variability is crucial for the nucleation of ice crystals in cirrus (see Kärcher, 2017a, and references therein).
  • Superpressure balloon (SPB) measurements at altitudes of 18–21 km directly link mesoscale vertical wind speed and the associated temperature variability to gravity waves and quantified spectral properties (Podglajen et al., 2016; Schoeberl et al., 2017).
  • Before enhancing complexity by considering effects of heterogeneous ice-nucleating particles (INPs), which are poorly constrained by field observations at cirrus temperatures (<230–235 K; Hoose & Möhler, 2012; Jensen et al., 2018), the authors focus on the more basic and much better understood homogeneous freezing process.
  • The authors evaluate statistically microphysical parcel model simulations forced with a large number of different random realizations of fluctuation time series.

2. Stochastic Simulations

  • The spectral parcel model primeice solves a large set of equations governing the temporal evolution of heat, water vapor, and supercooled/frozen water during ice nucleation and aqueous aerosol particle and ice crystal growth due to uptake of water vapor (Kärcher, 2017b).
  • 2 Geophysical Research Letters 10.1029/2019GL082437 tion between constant updraft and wave-driven vertical wind speed fluctuations, w′ , is somewhat artificial.
  • Individual w′ values are sampled randomly from a Laplacian with prescribed standard deviation 𝜎w, or, in terms of adiabatic cooling rates (𝜅), 𝜎𝜅 = 𝛤𝜎w.

3.1. Expectation Values

  • The authors performed two additional sets of simulations halving and doubling the mean vertical wind forcing of 10 cm/s. Figure 2 shows the resulting averaged ICNC, 𝜇n(w0) (expectation values).
  • The authors would expect the nucleated ICNC to approach a constant value for w0 ≪ 𝜇w, if they just looked at the mean ICNC calculated directly from the updraft speed fluctuation statistic without accounting for sink processes of the ICNC.
  • The authors call those values—shown as smooth colored curves in Figure 2—instantaneous ice numbers (equation (S4)).
  • Stronger subsidence will make cirrus formation increasingly unlikely due to the rapidly growing separation between the diminishing ice supersaturation and the homogeneous freezing threshold.
  • Preferential freezing results from the stochastic nature of the temperature fluctuations.

3.2. Comparison With Observations

  • Normalized probability density functions, dP∕dn, represent the fraction of n values that fall into a given number density bin.
  • The authors expect differences between these distributions, since the MACPEX data contain ICNCs sampled at various stages of the cirrus cloud, while the parcel simulations only consider nucleated ice crystals.
  • Regarding differences in shape, the authors note that the left (low-n) wing of the observed distribution might be affected by sample volume limitations of the measurements.
  • If the authors compute the total ICNC directly from instantaneous expectation values, they obtain 𝜇n = 0.09–0.7 cm−3 from equation (S8) for the range of mean updraft speeds prevailing during MACPEX.
  • The authors offer two explanations to account for the discrepancy in total nucleated ICNC, which is not entirely unexpected.

4. Conclusions and Outlook

  • The authors find that high updraft speed fluctuations increase total nucleated ICNC to much larger values than those calculated deterministically based solely on the probability of occurrence of the fluctuations.
  • The overall similarity of the shapes of simulated and analytical statistics suggests that wave-driven dynamical forcing and homogeneous freezing play important roles in in situ cirrus formation, inasmuch as ICNC values >10 cm−3 have been measured in cirrus.
  • When including the effects of waves, geographical, seasonal, and topographic variability in updraft speeds should be accounted for.

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The Impact of Mesoscale Gravity Waves on Homogeneous
Ice Nucleation in Cirrus Clouds
B. Kärcher
1
, E. J. Jensen
2
, and U. Lohmann
3
1
DLR Oberpfaffenhofen, Institut für Physik der Atmosphäre, Wessling, Germany,
2
National Aeronautics and Space
Administration, Ames Research Center, Mountain View, CA, USA,
3
ETH Zürich, Institute of Atmospheric and Climate
Science, Zurich, Switzerland
Abstract Effects of a spectrum of mesoscale gravity waves on homogeneous aerosol freezing in
midlatitude cirrus are studied by means of parcel model simulations that are driven by random vertical
wind speeds constrained by balloon measurements. Stochastic wave forcing with mean updraft speeds of
5–20 cm/s leads to substantial nucleated ice crystal number concentrations (ICNC) of 0.1–1 cm
3
in
situations with slow large-scale cooling, which by itself would generate fewer ice crystals. The stochastic
nature of wave-driven air parcel temperatures enhances ICNC even further, but the times required to reach
freezing conditions unsupported by large-scale cooling may vary widely. In the presence of wave forcing,
ice crystals with low ICNC (<1–10 L
1
) are also generated by homogeneous freezing, albeit only rarely.
Comparisons with aircraft measurements suggest significant influences of heterogeneous ice-nucleating
particles and ice crystal sedimentation on ICNC, but quantifying their individual contributions remains
elusive.
Plain Language Summary Spontaneous freezing of airborne, water-containing particles below
38
C is a fundamental pathway to form ice crystals in high-altitude cirrus clouds. This ice formation
process has been well researched and was the first represented in weather forecast and climate models to
advance cirrus predictions. One key characteristic is its strong dependence of the number of ice crystals
formed on the cooling rate of air. Recent observations show that rapid cooling rates are generated by ubiq-
uitous gravity waves. Here, we explore the rich suite of phenomena taking place during cirrus formation
caused by a spectrum of gravity waves. We find that wave effects should be considered in future model sim-
ulations, when comparing model results with observations, and in parameterizations of cloud ice crystal
formation.
1. Introduction
Mesoscale air motion variability is crucial for the nucleation of ice crystals in cirrus (see Kärcher, 2017a,
and references therein). We refer to cirrus as upper tropospheric ice clouds that form in situ, for exam-
ple, in frontal systems. Superpressure balloon (SPB) measurements at altitudes of 18–21 km directly link
mesoscale vertical wind speed and the associated temperature variability to gravity waves and quantified
spectral properties (Podglajen et al., 2016; Schoeberl et al., 2017). Since these airborne measurement plat-
forms are advected by the wind field, properties of fluctuations derived from them are highly useful for
Lagrangian cloud studies. Dinh et al. (2016) and Jensen et al. (2016) used SPB temperature time series to
drive detailed ice nucleation simulations, focussing on the tropical tropopause layer. Kienast-Sjögren et al.
(2015)—using a Lagrangian microphysical aerosol-cloud model—investigated cirrus over a midlatitude site
combining small-scale vertical wind speeds and temperature fluctuations inferred from radiosonde sound-
ings and a high-resolution weather prediction model. Haag and Kärcher (2004) used results from a global
weather prediction model with superimposed fluctuations to study hemispheric properties of midlatitude
cirrus.
Mesoscale gravity waves are ubiquitous in the upper troposphere and lower stratosphere. SPB measure-
ments show that power spectra of their properties versus intrinsic wave frequency are typically broad and
continuous, consistent with a superposition of many waves. A spectrum of mesoscale gravity waves gener-
ates broad frequency distributions of ice crystal number concentrations (ICNC) via homogeneous freezing
of supercooled aqueous solution particles (Hoyle et al., 2005; Jensen & Pfister, 2004; Kärcher & Ström, 2003).
RESEARCH LETTER
10.1029/2019GL082437
Key Points:
We present a systematic process
study of effects of a spectrum of
gravity waves on homogeneous
ice nucleation in cirrus through
ensemble simulations
High cooling rates have
disproportionately large impact
on nucleated ice crystal number
concentrations at low background
updraft speeds
Analysis of midlatitude continental
cirrus measurements suggests impact
of heterogeneous nucleation and
sedimentation on total ice numbers
Supporting Information:
Supporting Information S1
Correspondence to:
B. rcher,
bernd.kaercher@dlr.de
Citation:
Kärcher, B., Jensen, E. J., & Lohmann,
U. (2019). The impact of mesoscale
gravity waves on homogeneous ice
nucleation in cirrus clouds.
Geophysical Research Letters, 46.
https://doi.org/10.1029/2019GL082437
Received 12 FEB 2019
Accepted 22 APR 2019
©2019. American Geophysical Union.
All Rights Reserved.
KÄRCHER ET AL. 1

Geophysical Research Letters 10.1029/2019GL082437
The random nature of wave perturbations motivates the use of probabilistic methods to describe them. Pro-
cess models have studied aspects of homogeneous freezing using randomized small-scale dynamical forcing
(Dinh et al., 2016; Hoyle et al., 2005; Murphy, 2014; Shi & Liu, 2016).
Faithful applications of cirrus parameterizations in cloud schemes of large-scale models require sound rep-
resentations of unresolved cooling rates (Lohmann & Kärcher, 2002). While the attribution of ice nucleation
mechanisms in cirrus clouds in global climate models is challenging (Dietlicher et al., 2018; Gasparini et al.,
2018) and such models have already begun to parameterize the impact of unresolved gravity waves on cirrus
formation (Penner et al., 2018), it is important to explore this issue systematically on the process level as a
prerequisite to improving ice nucleation parameterizations (Barahona & Nenes, 2008; Kärcher & Lohmann,
2002).
Before enhancing complexity by considering effects of heterogeneous ice-nucleating particles (INPs), which
are poorly constrained by field observations at cirrus temperatures (<230–235 K; Hoose & Möhler, 2012;
Jensen et al., 2018), we focus on the more basic and much better understood homogeneous freezing process.
Field measurements leave little doubt that homogeneous freezing of supercooled aerosol particles is active
in cirrus and responsible for at least the generation of the rightmost tail (
>0.5 cm
3
) of probability distribu-
tions of ICNC. The main factor limiting INP effects is their low upper tropospheric number concentration
(
<0.1 cm
3
; DeMott et al., 2010), which makes them inefficient in suppressing homogeneous freezing in
the presence of sufficiently large vertical wind speeds (DeMott et al., 1997). Nonetheless, potent INPs are
capable of modulating or, if sufficiently abundant, dominating cirrus properties according to global model
simulations (Gettelman et al., 2012; Kuebbeler et al., 2014; Penner et al., 2018; Shi & Liu, 2016; Zhou &
Penner, 2014).
We explore systematically the homogeneous freezing process in midlatitude cirrus clouds due to gravity
wave-driven fluctuations of vertical wind speed consistent with Lagrangian SPB measurements. The pre-
scribed wave perturbations represent conditions away from strong local wave sources such as elevated
mountain ridges or deep convective clouds. We evaluate statistically microphysical parcel model simula-
tions forced with a large number of different random realizations of fluctuation time series. We compare our
results with data taken during an extensive airborne field campaign, allowing us to extend previous findings
on factors controlling midlatitude cirrus cloud formation (Jensen et al., 2013). We describe the stochastic
ice nucleation simulations in section 2, analyze the results of tens of thousands of them and compare them
to aircraft observations in section 3, and conclude our work in section 4.
2. Stochastic Simulations
The spectral parcel model prime solves a large set of equations governing the temporal evolution of heat,
water vapor, and supercooled/frozen water during ice nucleation and aqueous aerosol particle and ice crystal
growth due to uptake of water vapor (Kärcher, 2017b). We consider ambient conditions above ice but below
water saturation, where ice crystals can form homogeneously by freezing of liquid solution droplets.
Air parcel temperature, T, is adiabatically perturbed by random vertical wind speed fluctuations, w
. These
fluctuations are superimposed onto a constant updraft speed, w
0
0, driving ice microphysics in the
absence of wave-driven variability. Its prescribed value may be thought of as representative for synoptic
conditions (w
0
< 10 cm/s), orographic forcing (10–100 cm/s and sometimes exceeding 1 m/s), or pertur-
bations induced by convection (
>1 m/s). Values of w
0
greater than 1–10 m/s are found in the detrainment
zones of deep convective clouds, where homogeneous ice formation involves aerosol particles that have
been activated into cloud droplets prior to or along with freezing at temperatures 233–238 K. Presumably,
at these conditions, vertical wind speed fluctuations have different statistical properties (e.g., mean values,
variances, and power spectral densities) than those caused by gravity waves, so the findings reported here
are not directly applicable to such cases. Background wind speeds of (fractions of) millimeters per second
are found in the tropical tropopause layer, where T is lower (<200 K) than in midlatitudes studied here.
A decomposition of updraft speeds has also been employed by Spichtinger and Krämer (2013), represent-
ing fluctuations by a monochromatic sinusodial wave. Investigating the impact of wave phase at which ice
nucleation sets in, Jensen et al. (2010) showed that a spectrum of waves with random phases leads to broad
ICNC distributions. Since the constant updraft w
0
introduced here refers to the large-scale vertical wind
speeds resolved in global models, only the range w
0
< 1–10 c/s is relevant. For higher w
0
values, the separa-
KÄRCHER ET AL. 2

Geophysical Research Letters 10.1029/2019GL082437
tion between constant updraft and wave-driven vertical wind speed fluctuations, w
, is somewhat artificial.
Outside of convection, waves are the only source of updraft speeds in excess of
10 cm/s and even smaller
values associated with synoptic and planetary waves.
The wave forcing employed here accounts for the observed, double exponential (Laplacian) shape of the
vertical wind speed statistic, L(w
)=exp(−|w
|𝜇
w
)∕(2𝜇
w
). This distribution has zero mean, and 𝜇
w
is
the mean value taken over the one-sided (updraft) statistic, relating to the standard deviation,
𝜎
w
, via
𝜇
w
2
0
w
L(w
)dw
= 𝜎
w
2. The Laplacian approximately fits Lagrangian measurements (Podglajen
et al., 2016) and is used to generate fluctuation time series, w
(t), one for each nucleation simulation. The
vertical wind speed fluctuations are autocorrelated over a time t
c
= 2.8 min. Therefore, they are defined
only at discrete times (multiples of t
c
) and were approximated by stair steps for numerical integration. The
power spectrum of w
is flat (Figure 1 in Podglajen et al., 2016), meaning that all wave frequencies up to
the Brunt-Väisälä frequency—an upper limit constraining gravity wave propagation—are included in the
forcing with equal weight.
The temperature fluctuations, T
, that result from the wind forcing are obtained by advancing the stochastic
differential equation DT
Dt =−𝛤 w
, where DDt denotes the Lagrangian (material) time derivative and
𝛤 0.01 K/m is the dry adiabatic lapse rate. Individual w
values are sampled randomly from a Laplacian
with prescribed standard deviation
𝜎
w
, or, in terms of adiabatic cooling rates (𝜅), 𝜎
𝜅
= 𝛤𝜎
w
. This approach
replicates the first-order autoregressive model to represent T
(t) as proposed by Podglajen et al. (2016) based
on the underlying w
measurements. In prime, DT
Dt is added to adiabatic and diabatic temperature
tendencies, related to w
0
and latent heat exchange, respectively. Based on previous observational evidence,
we choose a cooling rate standard deviation 𝜎
𝜅
= 5 K/hr as a baseline value at cirrus levels. Cooling rate
fluctuations do not vary significantly with altitude within few kilometers around the tropopause (Podglajen
et al., 2016).
Figure 1 shows results from parcel model simulations, each initialized at T
0
= 221 K (air pressure 300 hPa)
and ice saturation ratio S
0
= 1.3. These values are slightly above (3 K for T
0
) and below (0.2 for S
0
) the
values at freezing and were chosen such that mesoscale temperature variations are capable of triggering
homogeneous freezing and within reasonable time scales (few hours). The initial total number density, mean
dry radius, and geometric standard deviation of lognormally distributed aerosol particles were 500 cm
3
,
20 nm, and 1.5, respectively. We do not vary aerosol parameters, because the dependence of n on them is
much weaker than on w (Kärcher & Lohmann, 2002; Kay & Wood, 2008; Liu & Shi, 2018). Time steps used in
the simulations are variable, 𝛿t [s]=1∕(w
0
+ |w
|)[cms], resolving individual freezing events. In addition,
we imposed t
c
as an upper limit time step to capture each vertical wind speed fluctuation.
With n indicating the number concentration of nucleated ice crystals, the circles in Figure 1 represent all
{n, w
0
} data points resulting from an ensemble of 10, 000 simulations. Each simulation was started with a
random choice for w
0
and a different w
(t)-realization (given 𝜎
𝜅
= 5 K/hr or 𝜇
w
10 cm/s) and terminated
once the nucleated ice crystal number mixing ratio assumed a constant value after the first freezing event.
The quenching of supersaturation right after freezing makes subsequent nucleation events unlikely, except
in cases with very low n; therefore, the restriction of our analysis to first nucleation events is not problematic.
Statistics of first freezing times are presented in the supporting information.
The simulations capture the dependence of nucleated ICNC on the homogeneous freezing temperature, T
,
which is, however, very weak. We note that across all the cases discussed here, T
*
218 K with very little
scatter (
±0.25 K), corresponding to a narrow range of ice saturation ratios, S
1.5 ± 0.02, characteristic for
homogeneous freezing events (Kärcher & Jensen, 2017). Examining the full upper tropospheric temperature
range would reveal significant variations of T
and nucleated ICNC.
The data points in Figure 1 exhibit considerable scatter for w
0
< 10–20 cm/s, about 15% lie below n =
10
3
cm
3
. These nonpersistent cooling events have been termed temperature limited by Dinh et al. (2016).
Most of these low-n events are generated when w
changes its sign before the freezing event is completed.
They happen to occur since the wave-driven vertical wind speed fluctuations contain high-frequency con-
tributions associated with time scales of 5–10 min, comparable to the duration of homogeneous freezing
events (minutes; Jensen et al., 2016). The fraction of nonpersistent cooling events would be lower without
restricting the analysis to first freezing times.
KÄRCHER ET AL. 3

Geophysical Research Letters 10.1029/2019GL082437
Figure 1. Number concentration, n, of homogeneously nucleated ice crystals versus background updraft speed, w
0
,
from ensemble simulations (circles). In each case, gravity wave-induced vertical wind speed fluctuations driving ice
microphysics in the parcel simulations were randomly sampled from a Laplacian distribution with a mean value of
updraft speed (standard deviation of cooling rate) fluctuations
𝜇
w
= 10 cm/s (𝜎
𝜅
5 K/hr) added to the constant w
0
.
The arrow points to an excessively high concentration generated by an exceptionally large updraft fluctuation. The
curve was obtained from simulations without fluctuations.
The scatter of n in a given narrow w
0
-range decreases progressively with increasing w
0
. The curve obtained
from simulations without fluctuations follows a power law dependence, as expected from cloud physical
theory (Kärcher & Lohmann, 2002): n(w)=n
1
[(w
0
+ w
)∕w
1
]
𝛼
, where n
1
is the nucleated ICNC at a given
T and w = w
1
. A good fit at T = 218 K is obtained for n
1
= 0.185 cm
3
, w
1
= 10 cm/s, and 𝛼 = 32
(Figure 1). The data collapse onto this curve beyond w
0
= 1 m/s, showing that w
0
governs ice formation
for w
0
≫𝜇
w
(deterministic regime). By contrast, ice formation is entirely controlled by the fluctuations
for w
0
≪𝜇
w
(fluctuation-dominated regime). In the deterministic regime, nonpersistent cooling events no
longer occur; we do not discuss this regime any further with
𝜇
w
= 5 20 cm/s, as we are concerned with
nonconvective (in situ) ice formation, where values w
0
< 10 cm/s prevail.
The arrow highlights a very rare data point indicating
400 ice crystals per cubic centimeter of air. In this
case, one single freezing event caused by an updraft speed fluctuation of 16.7 m/s (10 𝜎
w
) depleted about
80% of the available aerosol particles. Fluctuation amplitudes of comparable magnitude are captured by the
non-Gaussian statistic, L(w
). The probability of occurrence of such a value is exp(−10
2)≈10
6
. This
means that in a sample of 10, 000 data points, there is a 1% chance of encountering such an event. Filling
the gap between the outlier and the majority of the other data points in Figure 1 requires a much larger
number of simulations.
3. Analysis of Nucleated ICNC
3.1. Expectation Values
We performed two additional sets of simulations halving and doubling the mean vertical wind forcing of
10 cm/s. We calculated in each case moving averages of n over 75 w
0
data points from the full {n, w
0
} data
sets. Figure 2 shows the resulting averaged ICNC,
𝜇
n
(w
0
) (expectation values). As expected from the above,
the nucleated concentrations converge showing decreasing scatter as w
0
enters the deterministic regime.
KÄRCHER ET AL. 4

Geophysical Research Letters 10.1029/2019GL082437
Figure 2. Mean ice crystal number concentration, 𝜇
n
,versusw
0
from ensemble simulations for three cases
𝜎
𝜅
= 2.5, 5, 10 K/hr (red, magenta, and blue), or 𝜇
w
5, 10, 20 cm/s (𝜎
w
7.5, 15, 30 cm/s, respectively. The black
curve is obtained from simulations without fluctuations, where ice forms at w
0
. For comparison, the colored smooth
curves mark the mean nucleated concentrations calculated analytically from the updraft speed statistic. The left panel
highlights the transition of simulated
𝜇
n
to vanishing background cooling (w
0
0).
A surprising feature is the increase of 𝜇
n
for low w
0
that is most pronounced for larger forcing. We would
expect the nucleated ICNC to approach a constant value for w
0
≪𝜇
w
, if we just looked at the mean ICNC
calculated directly from the updraft speed fluctuation statistic without accounting for sink processes of the
ICNC. We call those values—shown as smooth colored curves in Figure 2—instantaneous ice numbers
(equation (S4)).
High cooling rates have a greater chance than low cooling rates to reach freezing thresholds,
{T
, S
}, giving
them a large statistical weight despite their lower abundance in the updraft distribution. For example, at T
already close close to T
, while a small cooling rate might not suffice to reach T
, a high cooling rate might
well trigger freezing. This effect (coined preferential freezing) is stronger the larger
𝜇
w
and significantly
increases
𝜇
n
as w
0
diminishes. With increasing w
0
pushing the parcel faster close to freezing conditions,
low cooling rate fluctuations have an increasing chance to nucleate ice as well. The contribution of the
fluctuations to w is dwarfed by w
0
for w
0
≫𝜇
w
.
This said, we still expect
𝜇
n
to saturate in the limit w
0
0, at which point the air parcels undergo a pure
random temperature (supersaturation) walk unsupported by a constant baseline cooling. The left panel in
Figure 2 extends the simulations to lower w
0
and indeed shows the expected behavior as w
0
0. An imme-
diate implication is that freezing is also possible for slightly negative w
0
causing a background warming.
However, stronger subsidence will make cirrus formation increasingly unlikely due to the rapidly growing
separation between the diminishing ice supersaturation and the homogeneous freezing threshold.
Preferential freezing results from the stochastic nature of the temperature fluctuations. It is absent in esti-
mates of instantaneous values of nucleated ICNC (colored curves), or when the updraft statistic is equal to, or
approaches, a monodisperse distribution. Apart from this, preferential freezing does not depend on the exact
functional form of w
statistic, as long as it has a finite second moment. Times at which freezing conditions
are met along a stochastic air parcel trajectory vary widely depending on the actual mesoscale temperature
evolution and hence on how far initial conditions {S
0
, T
0
} are away from {S
, T
} (Figure S3). These times
KÄRCHER ET AL. 5

Citations
More filters
01 May 2013
TL;DR: In this paper, the composition of the residual particles within cirrus crystals after the ice was sublimated was determined in situ, showing that mineral dust and metallic particles are the dominant sources of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent.
Abstract: Formation of cirrus clouds depends on the availability of ice nuclei to begin condensation of atmospheric water vapor. Although it is known that only a small fraction of atmospheric aerosols are efficient ice nuclei, the critical ingredients that make those aerosols so effective have not been established. We have determined in situ the composition of the residual particles within cirrus crystals after the ice was sublimated. Our results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent. Further, composition analysis combined with relative humidity measurements suggests that heterogeneous freezing was the dominant formation mechanism of these clouds.

44 citations

Journal ArticleDOI
TL;DR: In this article, the authors make use of long-duration balloon observations to devise a probabilistic model describing mesoscale temperature uctuations (MTF) away from strong wave sources and show that MTF are subject to damping at a rate near the Coriolis frequency when the vertical wind speed fluctuations are autocorrelated over a fraction of a Brunt Väisälä period.
Abstract: Ubiquitous mesoscale gravity waves generate high cooling rates important for cirrus formation. We make use of long‐duration balloon observations to devise a probabilistic model describing mesoscale temperature uctuations (MTF) away from strong wave sources. We define background conditions based on observed probability distributions of temperature and underlying vertical wind speed fluctuations. We show theoretically that MTF are subject to damping at a rate near the Coriolis frequency when the vertical wind speed fluctuations are autocorrelated over a fraction of a Brunt‐Väisälä period. We find that for background wave activity, a decrease in temperature of 1K translates into cooling rate standard deviations and mean updraft speeds of 4–8Kh and ≈ 10–20 cms, respectively, depending on latitude and stratification. We introduce an effective Coriolis frequency to generate cooling rates in equatorial regions consistent with balloon data. Above ice saturation, MTF are large enough to affect ice crystal nucleation. Our results help constrain uncertainty in aerosol‐cirrus interactions, provide insights to better meet challenges in comparing measurement data with model simulations, and support the development of cutting‐edge ice cloud schemes in global models. Plain Language Summary: The limited scientific understanding of pure ice clouds (cirrus)—and therefore the difficulty to account for them inmodels—causes substantial uncertainty in climate projections. Two research issues important for cirrus formation continue to form a roadblock on the path of scientific progress: the dynamical forcing driving cirrus ice crystal formation and the ice‐forming properties of solid atmospheric particles. Long‐duration balloons floating in the high atmosphere have quantified key properties of gravity waves that generate vertical air motions (cooling rates) crucial for ice formation in cirrus. Only when occurrence and magnitude of cooling rates are well understood can effects of different solid and liquid ice‐forming particles during cirrus formation be predicted with confidence. Blending insights obtained from the research balloon measurements with theoretical methods developed in statistical physics, our study elaborates on the dynamical forcing issue by devising a model that represents air parcel cooling rates on a probabilistic basis. We thereby hope to contribute significantly to a comprehensive process understanding and, ultimately, to removing one of the roadblocks in cloud research.

20 citations


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  • ...Note, however, that our scheme currently does not include mesoscale gravity waves and might therefore underestimate updraft velocities and ICNC from homogeneous nucleation (Haag & Kärcher, 2004; Jensen et al., 2016; Kärcher et al., 2019; Kärcher & Podglajen, 2019; Schoeberl et al., 2015)....

    [...]

Journal ArticleDOI
TL;DR: In this article, the horizontal spectrum of vertical velocity w is less well known compared to horizontal motion w. Here, w spectra are related to the atmospheric dynamics w and are used for atmospheric modeling.
Abstract: Vertical motions are fundamental for atmospheric dynamics. Compared to horizontal motions, the horizontal spectrum of vertical velocity w is less well known. Here, w spectra are related to ...

18 citations

Journal ArticleDOI
17 Jun 2021
TL;DR: In this article, the authors used a high-resolution cirrus column model to investigate how aircraft-emitted soot particles, released after ice crystals sublimate at the end of the lifetime of contrails and contrail cirrus, perturb the formation of cirrus.
Abstract: Fully accounting for the climate impact of aviation requires a process-level understanding of the impact of aircraft soot particle emissions on the formation of ice clouds. Assessing this impact with the help of global climate models remains elusive and direct observations are lacking. Here we use a high-resolution cirrus column model to investigate how aircraft-emitted soot particles, released after ice crystals sublimate at the end of the lifetime of contrails and contrail cirrus, perturb the formation of cirrus. By allying cloud simulations with a measurement-based description of soot-induced ice formation, we find that only a small fraction (<1%) of the soot particles succeeds in forming cloud ice alongside homogeneous freezing of liquid aerosol droplets. Thus, soot-perturbed and homogeneously-formed cirrus fundamentally do not differ in optical depth. Our results imply that climate model estimates of global radiative forcing from interactions between aircraft soot and large-scale cirrus may be overestimates. The improved scientific understanding reported here provides a process-based underpinning for improved climate model parametrizations and targeted field observations. Only a small part of aircraft-soot–cirrus interactions succeeds in forming cloud ice, according to simulations with a numerical cirrus cloud model. This suggests that radiative forcing from aircraft soot may have been overestimated.

14 citations

References
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Journal ArticleDOI
TL;DR: In this paper, numerical simulations and airborne measurements are used to evaluate the impact of physical processes on synoptically forced, midlatitude cirrus ice concentrations, and the agreement within a factor of 2 between ice concentrations measured with independent techniques (replicators and optical imaging probes) provides confidence in the accuracy of the in situ measurements.
Abstract: [1] Numerical simulations and airborne measurements are used to evaluate the impact of physical processes on synoptically forced, midlatitude cirrus ice concentrations. The agreement within a factor of 2 between ice concentrations measured with independent techniques (replicators and optical imaging probes) provides confidence in the accuracy of the in situ measurements. We use a computationally efficient modeling approach that incorporates the key cirrus physical processes, such that thousands of cloud cases can be simulated and the model results can be statistically compared with observations. One-dimensional simulations with detailed treatments of cloud microphysical processes are driven by temperatures and vertical winds extracted from meteorological analyses. Small-scale temperature and vertical wind perturbations associated with mesoscale waves are superimposed on the analysis fields. We find that in simulations with only homogeneous freezing nucleation, ice concentration statistics are very sensitive to the specified mesoscale wave vertical wind perturbations. With the frequency distribution of vertical winds adjusted to agree with aircraft observations, we obtain good agreement between the simulated and observed ice concentration frequency distributions. Both the observations and simulations indicate that relatively high ice concentrations (≥1000 L−1) occur rarely in these clouds (less than 1% of the time). Simulations including both homogeneous and heterogeneous nucleation indicate that even with moderate concentrations of ice nuclei (20 L−1), heterogeneous nucleation is an important ice production process, particularly for relatively low ice concentrations and warm temperatures. With enhanced ice nuclei concentrations (100 L−1), heterogeneous nucleation dominates ice production in the model. We find that it is critically important to include the impact of sedimentation on the evolution of ice concentrations when comparing model results with observations. Ice crystal collection efficiencies are poorly constrained at low temperatures, and we find that aggregation can significantly reduce ice concentrations. Sensitivity tests indicate that neither the agreement between observed and simulated ice crystal statistics nor the sensitivities indicated by the simulations are significantly affected by model assumptions such as the time periods simulated, geographic domain covered, trajectory paths calculated, or ice crystal habit assumed.

62 citations


"The Impact of Mesoscale Gravity Wav..." refers background or methods or result in this paper

  • ...More importantly, differences between measured and simulated ICNC statistics are consistent with the potential importance of ice crystal sedimentation and INP in cirrus as observed during an aircraft campaign over the continental United States....

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  • ...In Figure 3, we compare simulation results for n dP∕dn and instantaneous statistics that do not account for preferential freezing (equation (S7)) with data taken during the Midlatitude Cirrus Properties Experiment (MACPEX), an airborne field campaign that focused on synoptically forced midlatitude cirrus clouds over the south central United States (Jensen et al., 2013)....

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  • ...It is possible that high-n events are underrepresented in the data set, since they happen to be rather localized and more easily missed by the probing aircraft (Jensen et al., 2013)....

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  • ...…statistics that do not account for preferential freezing (equation (S7)) with data taken during the Midlatitude Cirrus Properties Experiment (MACPEX), an airborne field campaign that focused on synoptically forced midlatitude cirrus clouds over the south central United States (Jensen et al., 2013)....

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  • ...We compare our results with data taken during an extensive airborne field campaign, allowing us to extend previous findings on factors controlling midlatitude cirrus cloud formation (Jensen et al., 2013)....

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Journal ArticleDOI
TL;DR: In this article, the authors predict aerosol sensitivity in clouds formed by homogeneous freezing using timescales for the generation and depletion of water vapor, using adiabatic parcel modeling to constrain αi ≥ 0.1 for small ice crystals forming at high ice supersaturation.
Abstract: [1] Using timescales for the generation and depletion of water vapor, we predict aerosol sensitivity in clouds formed by homogeneous freezing. Our timescale analysis explains why aerosol sensitivity increases dramatically with ice deposition coefficients (αi) ≪ 0.1, and also why aerosol sensitivity increases as vertical velocity increases, temperature decreases, aerosol number decreases, and aerosol size decreases. We combine existing in-situ observations with adiabatic parcel modeling to constrain αi ≥ 0.1 for small ice crystals forming at high ice supersaturations. Two important implications for understanding and modeling upper tropospheric water vapor budgets emerge from our results: 1) aerosol sensitivity can be appreciable at low temperatures and moderate updrafts (∼5 cm/s) in the upper tropical troposphere, 2) reconciling our results with recent laboratory measurements supports theory that αi increases with ice supersaturation and/or decreases with ice crystal size.

61 citations


"The Impact of Mesoscale Gravity Wav..." refers background in this paper

  • ...We do not vary aerosol parameters, because the dependence of n on them is much weaker than on w (Kärcher & Lohmann, 2002; Kay & Wood, 2008; Liu & Shi, 2018)....

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  • ...Outside of convection, waves are the only source of updraft speeds in excess of ≈10 cm/s and even smaller values associated with synoptic and planetary waves. The wave forcing employed here accounts for the observed, double exponential (Laplacian) shape of the vertical wind speed statistic, L(w′) = exp(−|w|∕μw)∕(2μw). This distribution has zero mean, and μw is the mean value taken over the one-sided (updraft) statistic, relating to the standard deviation, σw, via μw ≡ 2 ∫ ∞ 0 w ′L(w′)dw′ = σw∕ √ 2. The Laplacian approximately fits Lagrangian measurements (Podglajen et al., 2016) and is used to generate fluctuation time series, w (t), one for each nucleation simulation. The vertical wind speed fluctuations are autocorrelated over a time tc = 2.8 min. Therefore, they are defined only at discrete times (multiples of tc) and were approximated by stair steps for numerical integration. The power spectrum of w is flat (Figure 1 in Podglajen et al., 2016), meaning that all wave frequencies up to the Brunt-Väisälä frequency—an upper limit constraining gravity wave propagation—are included in the forcing with equal weight. The temperature fluctuations, T , that result from the wind forcing are obtained by advancing the stochastic differential equation DT ∕Dt = −Γw , where D∕Dt denotes the Lagrangian (material) time derivative and Γ ≈ 0.01 K/m is the dry adiabatic lapse rate. Individual w values are sampled randomly from a Laplacian with prescribed standard deviation σw, or, in terms of adiabatic cooling rates (κ), σκ = Γσw. This approach replicates the first-order autoregressive model to represent T (t) as proposed by Podglajen et al. (2016) based on the underlying w measurements....

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Journal ArticleDOI
TL;DR: In this paper, a new multiple-mode ice microphysical scheme was applied to the general circulation model ECHAM5-HAM to analyze the competition between homogeneous freezing of solution droplets, deposition nucleation of pure dust particles, and immersion freezing of coated and pre-existing ice.
Abstract: . In order to study aerosol–cloud interactions in cirrus clouds, we apply a new multiple-mode ice microphysical scheme to the general circulation model ECHAM5-HAM. The multiple-mode ice microphysical scheme allows for analysis of the competition between homogeneous freezing of solution droplets, deposition nucleation of pure dust particles, and immersion freezing of coated dust particles and pre-existing ice. We base the freezing efficiencies of coated and pure dust particles on the most recent laboratory data. The effect of pre-existing ice, which has been neglected in previous ice nucleation parameterizations, is to deplete water vapour by depositional growth and thus prevent homogeneous and heterogeneous freezing from occurring. As a first step, we extensively tested the model and validated the results against in situ measurements from various aircraft campaigns. The results compare well with observations; properties such as ice crystal size and number concentration as well as supersaturation are predicted within the observational spread. We find that heterogeneous nucleation on mineral dust particles and the consideration of pre-existing ice in the nucleation process may lead to significant effects: globally, ice crystal number and mass are reduced by 10 and 5%, whereas the ice crystals' size is increased by 3%. The reductions in ice crystal number are most pronounced in the tropics and mid-latitudes in the Northern Hemisphere. While changes in the microphysical and radiative properties of cirrus clouds in the tropics are mostly driven by considering pre-existing ice, changes in the northern hemispheric mid-latitudes mainly result from heterogeneous nucleation. The so-called negative Twomey effect in cirrus clouds is represented in ECHAM5-HAM. The net change in the radiation budget is −0.94 W m−2, implying that both heterogeneous nucleation on dust and pre-existing ice have the potential to modulate cirrus properties in climate simulations and thus should be considered in future studies.

60 citations


"The Impact of Mesoscale Gravity Wav..." refers background in this paper

  • ...Nonetheless, potent INPs are capable of modulating or, if sufficiently abundant, dominating cirrus properties according to global model simulations (Gettelman et al., 2012; Kuebbeler et al., 2014; Penner et al., 2018; Shi & Liu, 2016; Zhou & Penner, 2014)....

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Journal ArticleDOI
TL;DR: In this paper, the impact of high-frequency fluctuations of temperature on homogeneous nucleation of ice crystals in the vicinity of the tropical tropopause was investigated using a bin microphysics scheme for air parcels.
Abstract: . The impact of high-frequency fluctuations of temperature on homogeneous nucleation of ice crystals in the vicinity of the tropical tropopause is investigated using a bin microphysics scheme for air parcels. The imposed temperature fluctuations come from measurements during isopycnic balloon flights near the tropical tropopause. The balloons collected data at high frequency, guaranteeing that gravity wave signals are well resolved. With the observed temperature time series, the numerical simulations with homogeneous freezing show a full range of ice number concentration (INC) as previously observed in the tropical upper troposphere. In particular, a low INC may be obtained if the gravity wave perturbations produce a non-persistent cooling rate (even with large magnitude) such that the absolute change in temperature remains small during nucleation. This result is explained analytically by a dependence of the INC on the absolute drop in temperature (and not on the cooling rate). This work suggests that homogeneous ice nucleation is not necessarily inconsistent with observations of low INCs.

55 citations


"The Impact of Mesoscale Gravity Wav..." refers background or methods in this paper

  • ...Process models have studied aspects of homogeneous freezing using randomized small-scale dynamical forcing (Dinh et al., 2016; Hoyle et al., 2005; Murphy, 2014; Shi & Liu, 2016)....

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  • ...These nonpersistent cooling events have been termed temperature limited by Dinh et al. (2016)....

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  • ...Dinh et al. (2016) and Jensen et al. (2016) used SPB temperature time series to drive detailed ice nucleation simulations, focussing on the tropical tropopause layer....

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Journal ArticleDOI
TL;DR: In this article, the authors used the coupled Community Atmosphere Model version 5.2 (CAM5)/IMPACT model to estimate the climate impacts of aircraft soot acting as heterogeneous ice nuclei (IN) in large-scale cirrus clouds.
Abstract: The indirect effect of aircraft soot on cirrus clouds is subject to large uncertainties due to uncertainty in the effectiveness of aircraft soot acting as heterogeneous ice nuclei (IN) and the complexity caused by background ice nucleation, which introduces two major competing ice nucleation mechanisms: homogeneous freezing that generally produces more abundant ice particles and heterogeneous nucleation that generally produces fewer ice particles. In this paper, we used the coupled Community Atmosphere Model version 5.2 (CAM5)/IMPACT model to estimate the climate impacts of aircraft soot acting as IN in large-scale cirrus clouds. We assume that only the aircraft soot particles that are preactivated in persistent contrail cirrus clouds are efficient IN. Further, we assume that these particles lose their ability to act as efficient IN when they become coated with three monolayers of sulfate. We varied the background number concentration of sulfate aerosols allowed to act as homogeneous ice nucleation sites as well as the dust concentrations that act as heterogeneous ice nuclei to examine the sensitivity of the forcing by aircraft soot to the background atmosphere. The global average effect can range from a high negative (cooling) rate, −0.35 W m−2, for the high sulfate/low dust case to a positive (warming) rate, +0.09 W m−2, for the low sulfate/low dust case (default CAM5 setup) when approximately 0.6% of total aviation soot acts as IN. The net negative forcing is caused by the addition of IN to a background atmosphere that is dominated by homogeneous nucleation (mainly in the tropic Indian Ocean, Central America, and North Atlantic Ocean). The forcings can be all positive, about +0.11 to +0.21 W m−2, when the background atmosphere is dominated by pure heterogeneous ice nucleation.

54 citations

Frequently Asked Questions (2)
Q1. What are the contributions in "The impact of mesoscale gravity waves on homogeneous ice nucleation in cirrus clouds" ?

Effects of a spectrum of mesoscale gravity waves on homogeneous aerosol freezing in midlatitude cirrus are studied by means of parcel model simulations that are driven by random vertical wind speeds constrained by balloon measurements. This ice formation process has been well researched and was the first represented in weather forecast and climate models to advance cirrus predictions. The authors find that wave effects should be considered in future model simulations, when comparing model results with observations, and in parameterizations of cloud ice crystal formation. The stochastic nature of wave-driven air parcel temperatures enhances ICNC even further, but the times required to reach freezing conditions unsupported by large-scale cooling may vary widely. Comparisons with aircraft measurements suggest significant influences of heterogeneous ice-nucleating particles and ice crystal sedimentation on ICNC, but quantifying their individual contributions remains elusive. 

Given the rather long times required for stochastic trajectories to trigger freezing even in air that is already ice supersaturated, future studies should investigate in which situations large-scale cooling, local relative humidity, and INP conditions are most relevant for atmospheric applications. While the effect of such damping is unimportant for the present study, its effect on first freezing times for less ice supersaturated initial conditions and weak or absent large-scale forcing should be studied in future work. The overall similarity of the shapes of simulated and analytical statistics suggests that wave-driven dynamical forcing and homogeneous freezing play important roles in in situ cirrus formation, inasmuch as ICNC values > 10 cm−3 have been measured in cirrus. More importantly, differences between measured and simulated ICNC statistics are consistent with the potential importance of ice crystal sedimentation and INP in cirrus as observed during an aircraft campaign over the continental United States.