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Effects of Urban-Influenced

Thunderstorms on Atmospheric
Chemistry

Kenneth E. Pickering
Department of Meteorology
University of Maryland

HEAT Planning Workshop


March 15, 2004
Outline

• Background – chemical measurements,


modeling for deep convection, urban
plumes, lightning NOx
• HEAT – proposed objectives,
measurements, modeling strategies
• Possible activities
Effects of Deep Convection
- Venting of boundary layer pollution
- Transport of NOx, NMHCs, CO, and HOx precursors to
upper troposphere
- Downward transport of cleaner air
- Transported pollutants allow efficient ozone production in
upper troposphere
- Results in enhanced upper tropospheric ozone production
over broad regions
- Increased potential for intercontinental transport
- Enhanced radiative forcing by ozone
Effects of Deep Convection
- Lightning production of NO
- Perturbation of photolysis rates
- Effective wet scavenging of soluble species
- Incorporation of pollution aerosols into precipitation
processes
- Nucleation of particles in convective outflow

- In remote regions low values of O3 and NOx are


transported to upper troposphere
- Larger values of these species tranported to PBL where
they can more readily be destroyed
Aircraft Measurements of Trace Gas Redistribution
in Oklahoma PRESTORM June 15, 1985 MCC

CO

O3

Dickerson et al., 1987, Science


Pickering et al., 1990
Pickering et al., 1990
Kansas-Oklahoma Squall Line Cell

Goddard Cumulus Ensemble (GCE) Model with offline tracer transport


June 10-11 PRESTORM Initial Conditions

Altitude CO (ppbv) O3 (ppbv) NOx (pptv)


0-1.75 km 150 (245) 28 (64) 900 (2950)
1.75-2.5 135 28 607
2.5-5.0 106 35 280
5.0-8.1 67 43 97
8.1-10.3 76 60 218
10.3-trop. 65 75 308

Urban BL values in parentheses Pickering et al. (1992)


Representative of ~45 km downwind of Oklahoma City
Vertically-averaged Ozone Production in
Cloud Outflow
June 10-11 PRESTORM (4-15 km)
Cloud-
Undisturbed Processed
Rural air 2.7 5.7 - 6.2
Urban plume 2.7 9.4 - 9.9

Values in ppbv/day Pickering et al. (1992)


LW Radiative Forcing - Clouds LW Radiative Forcing - Clear
The effect of thunderstorms on local O3 can be
remarkable even at periphery of storm.
On the third day of a high O3 episode (June 24-26 1998), a line of
thunderstorms passed just north of the Fair Hill, MD monitor.
Production of NO by Lightning
- Global production estimates range from
2 to 20 Tg N/yr due to uncertainty in global flash rate and in
the production per flash
- Global flash rate estimated from OTD satellite measurement
~44 flashes/s (Christian et al., 2003)
- Production per flash estimated from analysis of NO spikes in
aircraft measurements, cloud-scale chemical transport
modeling, or mass flux techniques
- Cloud-scale chemical transport models represent lightning
either through explicit electrophysics or use of
observed/parameterized flashes
- Models addressing other important questions: production per
CG flash vs. production per IC flash; vertical distribution of
lightning NOx at storm dissipation
July 12, 1996 STERAO-A Storm – NE Colorado
Cloud-scale Chemical Model Results - July 12, 1996
Transport Only – No chemistry or NO from Lightning

DeCaria et al., 2000


CG: 460 CG: 460
IC:46 IC: 345
Moles NO
Per Flash

CG: 460 CG: 460


IC: 460
IC: 690

Model-simulated vs. Measured NOx Profiles


For Four Lightning NO Production Scenarios
DeCaria et al. (2000)

22
Ozone Production for 24 hours Following Storm

42 x 42 km anvil region Entire model domain


EULINOX - July 21, 1998

a. b.
(Huntrieser et al., 2002).
1630 UTC 1653 UTC

Original Cell
Cell
Splitting

1734 UTC 1803 UTC


Multicellular

Supercell

(Höller et al., 2000).


PCG = PIC = 250 moles/flash
gives best agreement with Falcon
measurements at 8.5 km of mean
NOx ~ 3 ppbv
With 3 ppbv NOx in UT, ozone
production is less efficient than in
STERAO-A case with ~1.2 ppbv

Max. ΔP(O3) ~4 ppbv versus


~10 ppbv in STERAO-A case
HEAT Objectives
Characterize and quantify convective
transport of urban pollution from BL to UT

Quantify lightning production of NOx

Examine effects on UT chemistry (e.g., O3,


HOx production)
Objective 1 – Convective Transport
• Study transport and fate of urban pollutants
• Examine relative importance of convective
motions, scavenging, and chemistry
• Measurements required – vertical profiles of
chemical mixing ratios before, during and after
storm (CO, NO, NOx, NOy, O3, SO2, HOx, HC,
peroxides, aldehydes, acetone, aerosols)
• Characterize inflow, outflow, and storm core (?)
• U. of WY King Air – low level inflow, outflow
• WMI Lear Jet – anvil outflow
• Chemical analysis of precip from mesonet
• CO, CO2 as tracers of air motion in storm
Objective 2: Production of Lightning NOx
• Quantify amount of NO produced per flash, per
meter of flash channel, per thunderstorm, by
different storm types
• Quantify amount produced by an IC flash vs. that
produced by a CG flash and by different
components of a flash
• Measurements required – NO, NOx, NOy in low
level inflow/outflow, in anvil outflow, and in
storm core (?). Channel lengths and distributions
from lightning mapping system, CG flashes from
NLDN
• Analysis of flash and aircraft NO spike meas.;
chemical transport modeling; mass flux analysis
Objective 3: Effects on UT Chemistry
• Examine effects of combination of pollution and
lightning NOx on UT O3 and HOx chemistry
• Quantify relative contributions of boundary layer
and lightning NOx to UT NOx mixing ratios
• Chemical transport modeling required
• To verify these models, chemical measurements
needed in convective outflow plumes hours to
days downstream
Possible Post-Mission Analysis and
Modeling Activities
• Analysis of relationships between flash data and
observed NO spikes
• Cloud-resolving model simulations of chemical
transport, wet scavenging, lightning NO
production (parameterized, explicit); comparisons
with measurements and between models
• Tests of convective transport and lightning
parameterizations in regional models; calculation
of downstream ozone production