Evaluating the Role of Aerosol Mixing State

in Cloud Droplet Nucleation

using a new activation parameterization

Daniel Rothenberg and Chien Wang

Massachusetts Institute of Technology
Department of Earth, Atmospheric, and Planetary Sciences
Program in Atmospheres, Oceans, and Climate

December 11, 2013

EAPS
Department of
Earth, Atmospheric,
and Planetary Sciences

Rothenberg/Wang (MIT)

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The Mixing State Problem

How do you represent mixtures of aerosols in GCMs/CRMs?

Uniform, homogeneous composition

particles
Rothenberg/Wang (MIT)

Different populations of chemically

homogeneous particles
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The Mixing State Problem

Real aerosol populations are

chemically and physically
heterogeneous

Different particles with varying

optical and microphysical
properties

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The Mixing State Problem

Real aerosol populations are

chemically and physically
heterogeneous

Different particles with varying

optical and microphysical
properties

Important to capture this

diversity in order to resolve
anthropogenic aerosol
effects on clouds/climate!

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Example Effect: Droplet Nucelation

Put aerosols in an updraft...
adiabatic cooling

supersaturated environment

condensational growth of
aerosol/droplets

bifurcate aerosol into cloud droplets

(activation) and haze

Droplet nucleation
simulated with
detailed parcel model

cloud droplets

Critical factor - Smax (function of

temperature, updraft speed, aerosol
properties)

haze

How does the aerosol mixing state

contribute to potential droplet
activation?
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Error in Droplet Nucleation due to

Internal Mixing Assumption
45000

Original - internal mixture

Decomposed
mixed - internal
sulfate - external
carbon - external

40000

nN (rp ) (cm3 )

35000
30000
25000

20000
15000

()

10000
5000
0
104

103

102

rp (m)

101

100

104

103

Nucleated Droplet Count Error

(internal - external)

carbon

102

rp (m)

gamma

0.8
0.6
0.4
0.2
sulfate
internal

0.2

0.4

Rothenberg/Wang (MIT)

alpha

0.6

0.8

250
200
150
100
50
0
-50
-100
-150
-200
-250

101

100

Internal mixture of
carbon/sulfate
decompose into spectrum
of mixtures preserving
number and mass of each
species
Error in predicted droplet
number from 1 m/s updraft,
explicitly computed with
detailed parcel model
+100% error when mostly
carbon - important for
downwind of intense biomass
burning/industrial emissions?

external
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MARC = a Multimode, 2-Moment, and Mixing-state-resolving!

Model of Aerosols for Research of Climate!
Log-normal distribution, 2 prognostic moments (Q, N) + BIM & OIM, prescribed !

Aging (surface preparation)

Coagulation)

Growth

Radiation

Meteorology
Clouds

sp

on

su

ati

-re

cle

ap

Nu

Ev

en
s
gaseous oxidation e

Condensation
(Kim et al., JGR, 2008)

aqueous oxidation
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Droplet Nucleation / Activation Parameterization

Smax - the Activation Equation
From parcel theory, can derive (Ghan et al, 2011)
1/2
tmax
Z
dN
r (tact ) + 2G
dSc
Sdt
dSc

V
4w
=
GSmax

S
Zmax

tact

Need assumptions,
1
2
3

aerosol modes have bulk properties (e.g. hygroscopicity)

instantaneous particle growth in equilibrium with relative humidity
activation instantly happens when particle sees critical S (Kohler Theory)

Basic equation underlying parameterizations used in GCMs/CRMs to predict

droplet nucleation
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Droplet Nucleation Errors in CESM+MARC

Error, predicted droplet nucleation (ARG - explicit)
1/cm3, Avg: -36.8 (-597.9 -0.3)
60N
30N
0
30S
60S
180W

120W

60W

60E

120E

180E

Error, predicted droplet nucleation (FN - explicit)

1/cm3, Avg: -5.2 (-360.7 26.1)
60N
30N
0
30S
60S
180W

120W

60W

Rothenberg/Wang (MIT)

60E

120E

240
160
80
0
80
160
240

180E

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240
160
80
0
80
160
240

Severe underprediction in
areas with high carbonaceous
aerosol loading

Exactly in regions most

important for anthropogenic
aerosol effects

Need to better parameterize

mixing state / competition
effects on droplet nucleation

Parameterizations:
ARG - Abdul-Razzak and Ghan, 2000
FN - Fountoukis and Nenes, 2005
explicit - numerical parcel model
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Polynomial Chaos Expansion of Parcel Model

Polynomial emulator of full-complexity model
Computationally-cheap (produce/run), accurate distribution of modeled response

Updraft speed,
temperature, pressure,
aerosol properties

Detailed Parcel Model

Smax

Rothenberg/Wang (MIT)

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Polynomial Chaos Expansion of Parcel Model

Polynomial emulator of full-complexity model
Computationally-cheap (produce/run), accurate distribution of modeled response
Produce sets of
model runs based
on PDFs of input
parameters

Updraft speed,
temperature, pressure,
aerosol properties

Detailed Parcel Model

Polynomial Chaos
Expansion

Smax

Save response
function(s)

Rothenberg/Wang (MIT)

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Polynomial Chaos Expansion of Parcel Model

Polynomial emulator of full-complexity model
Computationally-cheap (produce/run), accurate distribution of modeled response
Produce sets of
model runs based
on PDFs of input
parameters

Updraft speed,
temperature, pressure,
aerosol properties

Detailed Parcel Model

Polynomial Chaos
Expansion

Numerical
quadrature to
compute
coefficients of
orthogonal
basis
functions

Smax

Save response
function(s)

Rothenberg/Wang (MIT)

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Parcel Model
Emulator

December 11, 2013

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Supersaturation (%)

104

103

SM1
SM2
SM3
SM4
SM5

Supersaturation (Polynomial Chaos)

Droplet Concentration, cm3 (Polynomial Chaos)

Emulation Results - Single Mode Aerosol

102

101 1
10

0.8
0.7
0.6
0.5
0.4
0.3
0.2
0.1
0.0 -2
10

102

103

10-2

10-3

104

Droplet Concentration, cm3 (Detailed Parcel Model)

SM1
SM2
SM3
SM4
SM5

ARG
FN
parcel
pce

Aerosols (SMi ) from Nenes and Seinfeld, 2003

10-3

10-2

Supersaturation (Detailed Parcel Model)

TOP: Emulator well-calibrated except

for large number concentrations of
small particles (SM5)
LEFT: Reproduces non-linear response
in Smax due to important variables

10-1

100

Updraft Speed (m/s)

Rothenberg/Wang (MIT)

101
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Supersaturation (%)

104

103

SM1
SM2
SM3
SM4
SM5

Supersaturation (Polynomial Chaos)

Droplet Concentration, cm3 (Polynomial Chaos)

Emulation Results - Single Mode Aerosol

102

101 1
10

0.8
0.7
0.6
0.5
0.4
0.3
0.2
0.1
0.0 -2
10

102

103

10-2

10-3

104

Droplet Concentration, cm3 (Detailed Parcel Model)

SM1
SM2
SM3
SM4
SM5

ARG
FN
parcel
pce

Aerosols (SMi ) from Nenes and Seinfeld, 2003

10-3

10-2

Supersaturation (Detailed Parcel Model)

TOP: Emulator well-calibrated except

for large number concentrations of
small particles (SM5)
LEFT: Reproduces non-linear response
in Smax due to important variables
Next step - extend to multiple aerosol
modes
10-1

100

Updraft Speed (m/s)

Rothenberg/Wang (MIT)

101
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Conclusions/Summary

Resolving some degree of the mixing state of heterogeneous aerosol calculations

will change the potential for droplet nucleation and calculated cloud droplet burden.
Existing parameterizations for global models may not be well-calibrated for the
complexity and diversity of aerosol populations predicted from mixing-state resolving
models.

Rothenberg/Wang (MIT)

AGU Fall 2013

December 11, 2013

11 / 12

Conclusions/Summary

Resolving some degree of the mixing state of heterogeneous aerosol calculations

will change the potential for droplet nucleation and calculated cloud droplet burden.
Existing parameterizations for global models may not be well-calibrated for the
complexity and diversity of aerosol populations predicted from mixing-state resolving
models.
Biases in physics calculations due to complex mixing state must be addressed to
accurately simulate anthropogneic aerosol effects on clouds and climate.

Rothenberg/Wang (MIT)

AGU Fall 2013

December 11, 2013

11 / 12

Conclusions/Summary

Resolving some degree of the mixing state of heterogeneous aerosol calculations

will change the potential for droplet nucleation and calculated cloud droplet burden.
Existing parameterizations for global models may not be well-calibrated for the
complexity and diversity of aerosol populations predicted from mixing-state resolving
models.
Biases in physics calculations due to complex mixing state must be addressed to
accurately simulate anthropogneic aerosol effects on clouds and climate.
Polynomial Chaos and other advanced statistical techniques could help produce
efficient activation parameterizations specifically tuned for applications in GCMs and
CRMs.

Rothenberg/Wang (MIT)

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December 11, 2013

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Acknowledgments

This material is based upon work supported by the National Science Foundation
Graduate Research fellowship under NSF Grant No. 1122374

We would also like to thank Steve Ghan (PNNL) for providing a reference parcel model
and code for his activation scheme; Rotem Bar-Or and Alex Avramov (MIT) for helping
run the CESM+MARC and for helpful discussion; Dan Czizco, Ron Prinn, and Paul
OGorman (MIT) for feedback and comments while preparing portions of this work for
the MIT PAOC General Examination.
Coupled CESM+MARC runs performed using the NCAR Yellowstone supercomputer.

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