NASA Atmospheric

Composition Research

Ken Jucks
Program Manager, NASA Upper Atmosphere
Research Program
Student Airborne Research Program
July 13, 2009
 What defines “Atmospheric Composition”?

✦ All the “stuff” in the atmosphere that has an impact on human lives.
❑ The basic gases involved biological and anthropogenic processes (O2,
CO2, N2O, CH4, CFCs, hydrocarbons, pollutants (NO, Ozone).
❑ The gases that are secondary products from chemistry that involves the
above gases (NO2, OH, HO2, O3,……..)
❑ Aerosols (condensed gases, dust, organic reactants, sea salt, etc.)
❑ Water in ALL it’s forms (gas, liquid, ice)!

✦ The atmospheric constituents that constrain the “radiative balance”

of the atmosphere (i.e. climate forcing)
❑ Greenhouse gases (CO2, CH4, N2O, O3, CFCs, etc.)
❑ Water in ALL it’s forms
❑ Aerosols

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 How is atmospheric research done at
NASA?
✦ Atmospheric Composition is divided up into 4 programs
❑ Upper Atmosphere Research Program
❑ Tropospheric Chemistry Program
❑ Radiation Science Program
❑ Atmospheric Chemistry Modeling and Analysis Program

✦ Research is performed along the following lines:

❑ Satellite observations of the atmosphere (Much more later)
❑ Airborne observations of the atmosphere (what you are here to learn
about!)
❑ Other “suborbital” observations of the atmosphere (sonde balloones and
LARGE high altitude balloons)
❑ Ground based observations of the atmosphere.
❑ Modeling and data analysis studies using and/or tying together ALL the
above observations.

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 Upper Atmosphere Research Program

✦ Concentrates on observations that augment the satellite

observations of ozone and the composition of the stratosphere and
upper troposphere.
✦ High altitude airplane observations of O3, CFCs, water vapor, other
source gases that can deplete ozone, and the reactive free radicals
that directly react with ozone.
✦ Higher altitude large balloon observations making similar
measurements.
✦ Ground based observations that provide the long term records of
ozone, ozone depleting substances, and reactive radicals.
✦ Other observations that “validate” the satellite observations from the
Aura satellite.
✦ Laboratory studies that help to interpret the observations from all of
the above….

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Airborne Arctic Ozone Expedition

Cloud particles Winds, P, T

N2O Gas can sample

e
nos

ay
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S-2
ay
od Q-b H 2O
erp
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da
su
riz
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NO, NOy
rlin rpo
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cen su

ClO, BrO
T-profile
Condensation nuclei
 Ozone and Chlorine
✦In 1974, Richard Stolarski and Ralph Cicerone, then at
the University of Michigan, suggest that chlorine could
also catalytically destroy ozone in the stratosphere. They
had been studying, for NASA, the possible impacts of solid
rocket propellants such as used by the Space Shuttle.

Cl + O3 -> ClO +O2

ClO + O -> Cl + O2

Net: O + O3 -> 2O2

Stolarski Cicerone
AAOE: 8/23/87 & 9/16/87 Data:
The “Smoking Gun”
2007 Aircraft Campaign in Costa Rica
 Tropical surface to stratosphere profile of
ozone-depleting bromine source gases

Decreasing levels signify

Transport through Tropical
Tropopause Layer (TTL) < 0 5 10 15 > 20
La titu de
3
15 x10 Elevated levels above 20 ppb in
upper troposphere are a sign of
convective transport.
A ltitu de (m )

10

Tropical surface sources of

short-lived organic bromine

From NASA DC-8 and WB-57 15 20 25 30

T otal O rga nic B ro m in e (pm ol/m o l)
 Probing of a tropical subvisible cirrus layer with two planes during TC4

ER-2
track

WB57 H2O rh% T (K)

alt

O3
supersat
Ice

Ice: mg/m3
ER2: Cloud Physics Lidar (upper)
WB57: In situ data (lower)
High Altitude Balloon Flights

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High Altitude Balloon Data

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Examples of photochemistry studies from balloon data

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 Advanced Global Atmospheric Gases Experiment and Affiliated
Networks

The AGAGE, and its predecessors (the Atmospheric Lifetime Experiment, ALE,
and the Global Atmospheric Gases Experiment, GAGE) have been measuring the
composition of the global atmosphere continuously since 1978.

AGAGE is distinguished
by its capability to
measure over the globe at
high frequency almost all
of the important species
in the Montreal Protocol
to protect the ozone layer
and almost all of the
significant non-CO2 gases
in the Kyoto Protocol to
mitigate climate change.

The ALE/GAGE/AGAGE stations occupy

coastal & mountain sites around the world
chosen to provide accurate measurements
of trace gases whose lifetimes are long
compared to global atmospheric circulation
times.
SOGE: System for Observation of Halogenated
Greenhouse Gases in Europe
NIES: National Institute for Environmental
Studies, Japan
SNU: Seoul National University, Korea.
AGAGE WEB SITE at
http://agage.eas.gatech.edu
Tropospheric Organic Chlorine
 Network for the Detection of
Atmospheric Composition Change
Cl Time Series for 55 km, Column and Surface

Satellite Measurements:
HALOE derived Cl. The solid
black line is the UNEP baseline
scenario lagged 5.3 years.

Ground-based Remote Sensing:

Jungfraujoch Station Cl derived
from the summation of column
HCl, ClONO2, and modeled
background ClO.

Ground-based In Situ:
AGAGE data

Russell and Anderson, 2005)

 Radiation Sciences Program
Understanding Electromagnetic Radiation in the Earth System

Scientific Foci:
• Aerosols; optical properties
(microphysical and chemistry), sources,
transport, sinks, distribution
• Clouds; optical properties (cirrus particle
shape), distribution, cloud meteorology
• Aerosol – Cloud Interactions; aerosol
impact on clouds and cloud properties
• Radiative Transfer; emphasize 3D RT as
it relates to the effect of clouds on
radiative flux and remote sensing
 RSP funded tasks…

Projects typically funded in RSP:

• Analysis and modeling of satellite remote sensing and
other data (e.g., MODIS, MISR, OMI, CALIPSO,
CloudSAT, Glory, …)
• Network measurements of radiation, aerosols and
clouds for scientific investigations and satellite
calibration and validation
• Field campaigns to measure aerosols, clouds and
radiation (e.g., TC-4, ARCTAS, MACPEX, …)
• Laboratory studies to refine understanding of aerosol
and cloud properties and the processes controlling
them
 Reflectance enhancement
at cloud-free areas near clouds

Observations: 3D enhancement
Clear-sky reflectance systematically
increases near clouds

Need to understand the increase for:

•a correct interpretation of observations
•improving our knowledge of aerosol-cloud
interactions; which are a significant part of
the largest uncertainty in climate models

Possible contributors:
•More/larger aerosol (e.g., swelling)
•Undetected cloud particles
•Instrument limitations
•3D radiative processes
 AERONET-An Internationally Federated Network

• Aerosol Optical Properties Research & Enabling Project

– Program of long term systematic network measurements
– Homepage access http://aeronet.gsfc.nasa.gov/
• Mission Objectives
– Validation of satellite aerosol retrievals
– Characterization of aerosol optical properties
– Synergism with satellite observations and climate models
 The Dynamic Atmosphere:
AERONET-Defining Aerosol Optical Properties

C
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 Objective: Long-term, local - regional - worldwide aerosol and cloud profile
observations using common instrument & data processing in a federated network

Status: Goddard team + 13 Partners compose MPLNET:

12 active sites NASA LaRC
6 planned sites (in preparation) NOAA ESRL
6 proposed sites (funding dependent) Naval Research Lab - Monterey
12 short-term field campaigns Japan’s National Institute of Polar Research
1 ocean cruise (two cruises pre-dating MPLNET are available) Spain’s Instituto Nacional de Técnica Aeroespacial - INTA
4 US Universities
Accomplishments: 2 Korean Universities
• MPLNET has generated and contributed to over 30 peer reviewed 1 Taiwan University
publications since 2000. 1 Chinese University other partners pending
• Validation & algorithm development for ICESat & TOMS. CALIPSO pending.
• Cooperation with AERONET, modeling, and satellite groups led to
formulation of new Synergy Tool (online aerosol database)

active sites
field campaigns
planned sites
proposed sites

former campaign, permanent site planned
former campaign, permanent site proposed

* Most sites are co-located with AERONET

* Campaigns utilize SMART-COMMIT and/or
MAARCO platforms
* line denotes research cruise

http://mplnet.gsfc.nasa.gov
 Observations of Saharan Dust Transport

Reid et al., JGR, 2003: Puerto Rico Dust Experiment (PRIDE) in 2000

MPLNET Level 3 Data

Cabras Island Site

Aerosol & Cloud Extinction Profiles km-1

Pink dots indicate Marine Boundary Layer heights from nearby radiosonde
 Aerosol Source Plume Physical Characteristics
from MISR Space-based Multi-angle Imaging
5 5

4
4
3 3
2 2

MISR nadir view
1 0.0 0.6 1.2 0.0 1.2 2.4 0 5000 10,000
Oregon wildfire Sept 04 2003 Smoke & bkgd aerosol amount ~Particle Size Smoke Plume Height

P1 P2 P3 P4 P5

MISR Stereo­Derived Smoke Plume Height histograms for five patches, plus model­derived atmospheric stability profile
From: R. Kahn et al. JGR
• Wildfire smoke plumes tend to concentrate in layers of high relative atmospheric stability. 
2007
layers of high relative atmospheric stability
• With buoyancy from a fire or volcano, they can reach stable layers 
fire or volcano above the boundary layer.
above the boundary layer
• The MISR plume height measurements can be used in models that predict aerosol transport.
in models that predict aerosol transport
• The GEOS­CHEM Modeling group at Harvard (J. Logan et al) is investigating this application. 
GEOS­CHEM Modeling
 CALIPSO Observations – All 3 Lidar Channels
9 June 2006

Desert Cirrus Biomass

dust smoke
Altitude, km

Fire locations in southern

Africa from MODIS
10 June 2006
Altitude, km
Altitude, km

56.71 47.85 39.92 31.94 23.93 15.90 7.81 -0.23 -8.28 -16.31 -24.33 -32.32 -40.27
32.16 28.57 25.78 23.46 21.42 19.55 17.77 16.05 14.23 12.56 10.69 8.64 6.30
 MODIS Aerosol Products View the Global
Aerosol System in an Entirely New Way
• Quantitatively calculate intercontinental transport of dust (Kaufman et al.,
2005) or pollution (Yu et al. in preparation)
• Observationally-based estimate of aerosol direct radiative effect (Remer and
Kaufman, 2006; Yu et al., 2006; Bellouin et al.2005; Chung et al., 2005)
• Observationally-based estimate of oceanic aerosol anthropogenic component
or direct forcing (Kaufman et al. 2006)
• Tool for operational air quality forecasts (Al Saadi et al. 2005)
 Glory Instruments Measure Important
Parameters for Understanding Climate
Understanding climate variability and change requires measuring:
• Aerosol Properties - optical thickness (±/2), size (explicit),
shape (new), and refractive index (new)
• Total Solar Irradiance
APS Provides:
Determination of the global distribution of natural and
anthropogenic aerosols and clouds with accuracy and
coverage sufficient for significantly improved quantification of
direct and indirect aerosol climate effects:
 Uncertainty in the effect of aerosols on global warming
accounts for roughly 40 percent of the uncertainty in the
radiative forcing function.
 Retrieval of aerosol particle microphysical properties by
inverting multi-angle and multi-spectral radiance and
polarization measurements will significantly extend the
information content concerning aerosols from multi-spectral
instruments such as MODIS and MISR. TIM Provides:
Continued measurement of the Total Solar Irradiance to determine
the Sun’s direct and indirect effect on the Earth’s climate.
 Total Solar Irradiance with precision of 10 ppm and accuracy of
100 ppm are needed to understand the role of the sun in climate
change and to understand the astrophysics of the nearest star to
the Earth.
 Glory Will Increase Our Understanding of
the Earth’s Energy Budget
Effective climate forcings (W/m2) (1880–2003)

Direct/Indirect Aerosol Effects Hansen et al., Science

warming

Are Large and Uncertain 308, 1431–1435 (2005)

cooling

Overlap of TIM Measurements

Enables Long-term Record
ARCTAS measurements enable fundamentally improved
prediction of Cloud Condensation Nuclei (CCN) in biomass
burning smoke plumes

Before:

10-X underprediction of CCN indicates

large fraction of organics are water
soluble

Analysis of ARCTAS measurements is showing that organic carbon contributes

significantly to the CCN activity of fresh biomass burning plumes and that
quantifying the water soluble (organic/inorganic) carbon fraction is fundamental
to improved prediction of CCN.
Such improvement in CCN closure theory is critical to reducing uncertainty in
prediction of aerosol indirect effects on climate, particularly given expected
changes in biomass burning.
 Atmospheric Chemistry Modeling and Analysis Program

Modeling studies using NASA satellite data.

Modeling and analysis of NASA ground, airborne, and balloon

data sets.

Model development to improve atmosphere and climate change

prediction.

All of these studies are to advance the knowledge of the

fundamental processes of the atmosphere and it’s interaction with
the rest of the Earth Climate system.

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 GMI Reproduces Ozone Observations in
both the Stratosphere and Troposphere

GMI simulated ozone reproduces daily features The seasonal cycle variability of Aura
seen by Aura’s Microwave Limb Sounder (MLS) in MLS O3 (shaded) is nearly matched
the Lower Stratosphere. by GMI (red cross-hatched) for 2005.
Mean O3 values track each other
faithfully (black, MLS; red GMI).
OMI - MLS
90
60 75
30
DU

0
DU

-30 GMI zonal mean column of Tropospheric ozone

Latitude

-60
0
-90 nearly matches the Aura Tropospheric column,
2005 GMI
90
75
(i.e., the difference between the OMI total ozone
60
30 column and the stratospheric ozone column
DU

0 from MLS).
DU

-30
-60
0
-90
J FJ FM MA AM MJ J JJ A
A SS OO NN D D
 Ozone Hole Recovery
✦ Antarctic ozone depletion (the
“ozone hole”) is caused by
human-produced chlorine and
bromine gases. International 550
regulation of these gases Sep. 2006
should lead to ozone recovery.
330
✦ A parametric model of the
ozone hole area has been
developed based on satellite,
ground, and aircraft 110
observations of ozone and
chlorine and bromine species. Sep. 2002

✦ This model suggests that the

ozone hole area will begin to
decrease in 2023 and will be
fully recovered to 1980’s levels
by 2070.

✦ Recent occurrences of
particularly small (2002) or
large (2006) ozone holes are
not indicative of a long-term
trend.
 Polar chlorine and ozone chemistry
 Recent laboratory measurements have raised questions about one of the crucial steps
in the chlorine-catalyzed loss of ozone in the polar stratosphere (new Pope et al.
measured ClO dimer photolysis cross sections)
 When the newly-measured values are used chemistry transport models, abundances
of reactive chlorine (ClO) and depletion of ozone are severely underestimated
compared to observations by MLS
 Simulated chlorine
deactivation is
delayed, with modeled
HCl much lower than
observed at the end of
winter
 MLS data are a key
observation
component of SPARC
initiative on polar
ozone loss

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[Santee et al., 2008, JGR]
 HIRDLS Cloud Extinction
April 2007 Northern Winter 2006
cloud occurrence cloud extinction

Thin clouds are difficult to detect from space. The first

comprehensive climatology of thin clouds has been
developed with the HIRDLS limb viewing IR radiometer.
• Tropical thin cirrus are important in controlling climate
change and water vapor in the the stratosphere.
• Polar Stratospheric Clouds (PSCs) are key players in
spring polar ozone depletion.
HIRDLS, Steve Massie NCAR • Comparisons with MLS relative humidity (RHI) and
35 CALIPSO backscatter show good agreement.
 Combining OMI and MODIS allows for:
- better estimates of aerosol height
- better estimates of aerosol absorption
- ability to characterize aerosol
absorption.

The combination of OMI/MODIS data

enables the determination of single
scattering albedo at 388 nm over 3 dust
regions during Jan 2006 with less certainty
than before combining sensors

0.89 0.86

0.92

Satheesh et al., (2009) JGR

 Koren et al. (2008) Science Davidi et al., (submitted to
ACP)

AOD=0.2

AIRS Temperature
Cloud fraction

1000 mb
925 mb

All data 850 mb

Aerosol optical depth 700 mb

0 0.1 0.2 0.3 0.4 0.5
0.6 MODIS AOD
Combining MODIS aerosol and cloud data with AIRS temperature profiles
leads to a semi-quantitative understanding of aerosol-cloud interactions

At low AOD, increasing aerosol In upper boundary layer (850 mb)

increases cloud fraction via a increasing aerosol increases temp
microphysical pathway (absorption)
At high AOD, increasing aerosol At surface (1000 mb) increasing aerosol
decreases cloud fraction via a decreases temperature (mostly from
radiative pathway. increasing cloudiness through
microphysical pathway.)

Note turning point at AOD =

 HIRDLS Cloud Extinction
April 2007 Northern Winter 2006
cloud occurrence cloud extinction

Thin clouds are difficult to detect from space. The first

comprehensive climatology of thin clouds has been
developed with the HIRDLS limb viewing IR radiometer.
• Tropical thin cirrus are important in controlling climate
change and water vapor in the the stratosphere.
• Polar Stratospheric Clouds (PSCs) are key players in
spring polar ozone depletion.
HIRDLS, Steve Massie NCAR • Comparisons with MLS relative humidity (RHI) and
38 CALIPSO backscatter show good agreement.