Integrating in situ and satellite observations with GEOS...

Integrating in situ and satellite observations with GEOS-Chem to constrain the influence of

boreal biomass burning emissions on tropospheric oxidant chemistry

Mark Parrington, Paul Palmer (University of Edinburgh)and the BORTAS Science Team

Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS): 12 July - 3 August 2011

BORTAS sampled a wide age spectra of plumes!

Serendipity puts BORTAS in a unique position !

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0 7 14 21

Resulting perturbation to atmospheric chemistry in the troposphere.!

Composition and distribution of biomass burning outflow!

O3 production and loss within the outflow!

BORTAS addresses the science by integrating different and modelling techniques!

Resulting perturbation to atmospheric chemistry in the troposphere.!

Composition and distribution of biomass burning outflow!

O3 production and loss within the outflow!

BORTAS addresses the science by integrating different and modelling techniques!

• Wide range of biomass burning plume ages sampled by BORTAS from ground-based, in situ and satellite measurements.

• Integrated modelling approach required to fully interpret data --> high resolution GEOS-Chem and adjoint simulations nested over the North Atlantic region

Resulting perturbation to atmospheric chemistry in the troposphere.

C o m p o s i t i o n a n d distribution of biomass burning outflow

O3 production and loss within the outflow

Palmer et al., ACPD, 2013

GEOS-Chem North Atlantic nested grid• North Atlantic nested grid with boundary conditions from 2×2.5 global simulation.• Daily biomass burning emissions from FLAMBE inventory scaled down by factor of 2 (Alvarado et

al. 2010, Fisher et al. 2010, and Parrington et al. 2012).

Nested grid output at 750 hPa: 1700

UTC, 18 July 2011.

CO

40oN

45oN

50oN

55oN

60oN

80oW 60oW 40oW 20oW

50 100 150 200 [ppbv]

Ox

40oN

45oN

50oN

55oN

60oN

80oW 60oW 40oW 20oW

20 40 60 80 [ppbv]

NOy

40oN

45oN

50oN

55oN

60oN

80oW 60oW 40oW 20oW

0.00 0.75 1.50 2.25 [ppbv]

NOx

40oN

45oN

50oN

55oN

60oN

80oW 60oW 40oW 20oW

0.00 0.05 0.10 0.15 [ppbv]

CO Ox

NOy NOx

Aircraft flight track (next slide)Met. fields and

emissions available from mid-2005

through to end of 2011

GEOS-Chem vs. BORTAS aircraft measurements, 18 July 2011

199.6 199.7 199.8 199.9 200.0Time / day of year 2011

0

2

4

6

8

10

GPS

alti

tude

/ km

BORTAS flight b621: BAe-146 CO ; CTM CO

199.6 199.7 199.8 199.9 200.0Time / day of year 2011

0

100

200

300

400

500

600

700

CO /

ppbv

BORTAS flight b621: BAe-146 TECO49 O3 ; CTM O3

199.6 199.7 199.8 199.9 200.0Time / day of year 2011

0

20

40

60

80

100

120

TECO

49 O

3 / p

pb

BORTAS flight b621: BAe-146 LIF total NOy; CTM NOy

199.6 199.7 199.8 199.9 200.0Time / day of year 2011

0.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

LIF

tota

l NO

y / U

NK

NO

WN

BORTAS flight b621: BAe-146 LIF NOx ; CTM NOx

199.6 199.7 199.8 199.9 200.0Time / day of year 2011

0.0

0.1

0.2

0.3

0.4

LIF

NO

x / p

pbv

BORTAS flight b621: BAe-146 SP2 BC mass; CTM BC Hydr

199.6 199.7 199.8 199.9 200.0Time / day of year 2011

0.0

0.2

0.4

0.6

0.8

SP2

BC m

ass /

UN

KN

OW

N

Aircraft altitude CO O3

NOy NOx Black Carbon

Time / day of year 2011

GPS

altit

ude

/ km

CO /

ppb

v

O 3 /

ppb

v

NOy /

ppb

v

NOx /

ppb

v

BC m

ass

conc

entr

atio

n / μg

m-3

Evaluate O3 sensitivity to model inputs using differences between model and measurements.

Model Ox sensitivity to NOx emissions sources

Biomass burning

35oN40oN45oN50oN55oN60oN65oN70oN75oN

120oW 90oW 60oW 30oW

Lightning



Anthropogenic



Aircraft + Biofuel + Soil



0.0 1.0 2.0 [×10-4]

Biomass Burning Lightning

Anthropogenic Aircraft/biofuel/soil

Recall: the adjoint model provides a computationally efficient calculation of the sensitivity of the output of a model to its inputs through the partial derivatives.

July 2011 adjoint sensitivity of model Ox at

3 ozonesonde launch sites in Maritime Canada (▲) to North American

continental NOx emissions sources.

Sensitivity to biomass burning emissions smaller

than to anthropogenic sources but distinct

geographical distribution.

(dJ/dOx)/max(dJdOx)

35oN

40oN

45oN

50oN

55oN

60oN

65oN


-0.00 0.50 1.00

(dJ/dNOx)/max(dJdOx)

35oN

40oN

45oN

50oN

55oN

60oN

65oN


-2.71e-05 1.86e-03 3.75e-03

4D-variational assimilation of BORTAS aircraft O3 measurements

Cost function defined at each model chemistry time-step:

Normalised gradient of cost function with respect to initial model concentrations of Ox and NOx shows sensitivity along air mass trajectory upwind from measurements:

Difference between model and measured mixing ratio Sobs = representativeness error (50%)

+ measurement error (~5%)

Control vector defined as initial model tracer concentrations

= mean aircraft O3 “observation operator”

∂J/∂[NOx]apriori, 750-500 hPa average∂J/∂[Ox]apriori, 750-500 hPa average

(dJ/dOx)/max(dJdOx)

35oN

40oN

45oN

50oN

55oN

60oN

65oN


-0.00 0.50 1.00

(dJ/dNOx)/max(dJdOx)

35oN

40oN

45oN

50oN

55oN

60oN

65oN


-2.71e-05 1.86e-03 3.75e-03

4D-variational assimilation of BORTAS aircraft O3 measurements

Cost function defined at each model chemistry time-step:

Normalised gradient of cost function with respect to initial model concentrations of Ox and NOx shows sensitivity along air mass trajectory upwind from measurements:

Difference between model and measured mixing ratio Sobs = representativeness error (50%)

+ measurement error (~5%)

Control vector defined as initial model tracer concentrations

= mean aircraft O3 “observation operator”

∂J/∂[NOx]apriori, 750-500 hPa average∂J/∂[Ox]apriori, 750-500 hPa average

45

60

!!!!!!!!!!!!!!!!!!!!!!!!!

3000 4000 5000 6000

5000

NOAA HYSPLIT MODEL Backward trajectories ending at 1800 UTC 18 Jul 11

GDAS Meteorological Data

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Job ID: 11186 Job Start: Wed May 8 15:19:23 UTC 2013 Source 1 lat.: 44.812000 lon.: -64.525000 height: 5000 m AGL Trajectory Direction: Backward Duration: 24 hrs Vertical Motion Calculation Method: Model Vertical Velocity Meteorology: 0000Z 15 Jul 2011 - GDAS1

NA

TI

ON

AL

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NI C

AND A TMOS PHERI C

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noaa

Summary• The BORTAS measurement campaign in the summer of 2011

sampled biomass burning smoke plumes with a wide range of ages.• measurements of key tracers associated with biomass burning made

from variety of ground-based, airborne, and satellite instruments.

• http://www.atmos-chem-phys-discuss.net/special_issue165.html

• GEOS-Chem nested grid for North Atlantic region links transport of biomass burning plumes between North America and Europe.

• Adjoint sensitivity calculations indicate model O3 sensitivity to precursor emissions and distributions.

Next steps• Assimilate BORTAS aircraft measurements into North Atlantic

nested grid to constrain model oxidant chemistry and scale-up measurements to evaluate broader regional impact.

• Assimilate satellite observations over the BORTAS campaign period to test consistency between different measurements of biomass burning outflow.

Integrating in situ and satellite observations with GEOS...

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