Atmospheric chemical transport models

Introduction
 The atmosphere is an extremely complex reactive system in which numerous
physical and chemical processes occur simultaneously.
 Ambient measurements give us only a glimpse of atmospheric conditions at a
particular time and location. Such measurements are often difficult to interpret
without a clear conceptual model of atmospheric processes.
 Moreover, measurements alone cannot be used directly by policymakers to
establish an effective strategy for solving air quality problems. An understanding of
individual atmospheric processes (chemistry, transport, removal, etc.) does not imply
an understanding of the system as a whole.
 Mathematical models provide the necessary framework for integration of our
understanding of individual atmospheric processes and study of their interactions.
 A combination of atmospheric measurements with atmospheric processes by
using atmospheric models is the best approach for making real progress toward
understanding the atmosphere.
 Why do we need to use atmospheric chemical
transport models?

Atmospheric chemical transport models are developed to answer the following

questions.
 What is the contribution of source A to the concentration of pollutants at site
B?
 What is the most cost-effective strategy for reducing pollutant concentrations
below an air quality standard?
 What will be the effect on air quality of the addition or the reduction of a
specific air pollutant emission flux?
 Where should one place a future source (industrial complex, freeway, etc.) to
minimize its environmental impacts?
 What will be the air quality tomorrow or the day after?
 Domains of Atmospheric models

Typical
Model Typical Domain Scale
Resolution
Microscale 200 X 200 X 100 m 5m
Urban 100 Χ 100 Χ 5 km 4 km
Regional 1000 Χ 1000 Χ 10 km 20 km
Synoptic
(continental) 3000 Χ 3000 Χ 20 km 80 km
Global 65,000 Χ 65,000 Χ 20km 5° Χ 5°

Fig. 1: Atmospheric models defined according to their spatial scale

Components of climate simulation

FSH: surface
heat flux

E: Evaporation
P: Precipitation

Trenberth, Climate
Systems Modelling
Domains of Atmospheric models (Contd.)

C(t): 0-D
C(z,t) : 1-D
C(x,z,t): 2-D
C(x,y,z,t): 3-D

C: concentration of
species

Fig. 2: Schematic depiction of (a) a box model

(zero-dimensional), (b) a column model (one-
dimensional), (c) a two-dimensional model,
and (d) a three-dimensional model
 Model types

Atmospheric models

Physical models Mathematical models

These are used to simulate

atmospheric processes by means of a
small-scale representation of the Fundamental
Fundamentalmodels
models Statistical
Statisticalmodels
models
actual system
Models based on Models based on
Ex: a small-scale replica of an urban fundamental description statistical analysis
area or a portion thereof in a wind of atmospheric physical of data
tunnel and chemical processes
Drawbacks: Problems associated with
properly duplicating the actual scales
of atmospheric motion

Fig. 3: Different types of atmospheric model

8
 Types of Atmospheric Chemical Transport Models

Atmospheric Chemical Transport Models

Lagrangian
Lagrangianmodels
models Eulerian
Eulerianmodels
models

Simulate changes in the Describe the concentrations in

chemical composition of a given an array of fixed
air parcel as it is advected in the computational cells
atmosphere

Fig. 5: Chemical transport models

 Eulerian model:

 An Eulerian modeling framework

remains fixed in space. Species enter
and leave each cell through its walls,
and the model simulates the species
concentrations at all locations as a
function of time.

Fig. 6: Schematic depiction of an Eulerian model

 Lagrangian model:

 A Lagrangian modeling framework

is one that moves with the local wind
so that there is no mass exchange
between the air parcel and its
surroundings, with the exception of
species emissions that are allowed to
enter the parcel through its base.
 The air parcel moves continuously,
Fig. 7: Schematic depiction of a Lagrangian
model so the model actually simulates
concentrations at different locations at
different times.
 Eulerian Box model
The Eulerian box enclosing a region
of atmosphere having dimensions Δx,
Δy and H(t). Hence The model is
based on the mass conservation of a
species inside a fixed Eulerian box of
volume H Δx Δy.
A mass balance for the concentration
ci of species i results in
Fig. 8: Box model framework

…………….(1)
where Qi is the mass emission rate of i (kgh-1),
Si the removal rate of i (kgh-1),
Ri, its chemical production rate (kgm- 3h-1),
c0i its background concentration,
and u the wind speed with the wind assumed to have a constant direction.
Equation (1) can be simplified by dividing with Δx Δy as,

…………………….…….(2)

where qi and si be the emission and removal rates of i per unit area (kg m - 2 h- 1)
 Eulerian Box model (Contd.)
The removal rate due to dry deposition can be described using the dry deposition
velocity of the species vd,i as
…………………………...……….(3)
and the box model governing equation assuming constant mixing height H becomes

…………….(4)

The terms on the right-hand side (RHS) of (Eq. 4) correspond to the changes in
the
concentration of i as a result of emission, chemical reaction, dry deposition, and
advection.

Term (delta x/u) is the residence time of air in box.

 Entrainment

 Up to this point it has been assumed that the height of the mixing layer
that defines the vertical extent of the box remains constant.
 Actually, the mixing height varies diurnally with low values during the
nighttime and higher values during the daytime.
 When the mixing height decreases, there is no direct change in the
concentration ci inside the mixed layer. As the mixing height decreases, air
originally inside the box is left aloft above the box. Surface sources and sinks
will have a more significant effect as the box will be smaller.
 If the mixing height increases, the box entrains air from the layer above.
This entrainment and subsequent dilution will change the concentration c i,
and this process should be explicitly included in the model.
 This dilution rate will depend on the concentration of the species aloft, c ia.
 Entrainment (Contd.)
Assume that at a given moment the box has a height H, a concentration c i,
and the concentration above it is c ai. If after time Δt, the box height increases
to H + ΔH and the concentration of i to c i + Δci then a mass balance for i
gives
………………………(5)

which, after neglecting the second-order term Δc i ΔH, simplifies to

……………………………................(6)

Dividing by Δt and taking the limit Δt 0 , (25.11) becomes

………………………………………(7)

The entrainment term given by (Eq. 7) should be included in the box model
only if the mixing height is increasing. Summarizing, the entraining Eulerian
box model equations are

……………..…(8)

……(9)
 Lagrangian Box Model

 The Eulerian box model considers the entire airshed is assumed to be

well mixed within the box. So no spatial resolution within the box.
 This weakness can be circumvented by selecting as the modeling
framework a much smaller box that is allowed to move with the wind in the
airshed (Figure 7). This box extends vertically up to the mixing height,
while its horizontal dimensions can be selected arbitrarily.
 This model simulates advection of an air parcel over the airshed, its
subsequent movement and collection of emissions, the buildup of primary
and secondary species, and finally its exit from the airshed.
 The major assumption of the Lagrangian box model is that there is no
horizontal dispersion; that is, material in the box is not removed by mixing
and dilution with the surrounding air.
 Lagrangian Box Model (Contd.)
The mass balance for the Lagrangian box is identical to (Eq. 8) and (Eq. 9)
with the exception that the advection terms are absent

………………………..…(10)

………………(11)
 Numerical solution to chemical transport models
 As it is very complicated to solve the governing equation of the model as a whole,
therefore the numerical techniques by means of operators are used to solve the
equation.
 Chemical transport models solve chemical species equations of the general form

…(12)

Advection Cloud processes Aerosol Emission rate

processes

Diffusion Dry deposition Net production from

gas-phase reactions
A Advection operator
D Diffusion operator
C Cloud operator
G Gas-phase chemistry operator
P Aerosol operator
S Source/sink operator
 Numerical solution to chemical transport models (Contd.)

 Operator splitting: Operator splitting is the most popular technique for the
solution of Eq. 12.
 Instead of solving the full equation at once, the problem is solved by applying
each process operator individually and then couple the various changes resulting
from the separate partial calculations.
 Diffusion
From the numerical point of view, the diffusion operator that solves

 It is probably the simplest to deal with of those involved in the full

atmospheric diffusion equation.
 Because of its physical nature, diffusion tends to smooth out gradients and
lend overall stability to the physical processes. Most typical finite difference or
finite element procedures are quite adequate for solving diffusion-type
operator problems.
 Advection
Advection problems are more difficult to solve numerically than the diffusion
problems. The advection operator included in

The one dimensional advection equation with constant velocity u

becomes
 LMDz INCA model (Outline)

Initial
Initialstate
state SST
SST

General 3 min Physics (radiation,

circulation (nudging) 30 min ……) 2D
3D

6 hour
15 min
ECMWF
Tracer
Tracerphysics
physics
(Convection,
(Convection,
Large
Largescale
scale
Planetary
Planetaryboundary
boundary
advection
advection
layer)
layer)

Fig. 9: Outline of LMDz INCA model

 LMDz INCA model (Overview)

Simulation
Simulationofofaerosol
aerosolcycle
cycle Direct
Directmodel
modeloutput
output
Transport
Transport Mass
Massconcentration
concentration
Microphysics
Microphysics Particle
Particleproperties
properties
Water
Wateruptake
uptake Deposition
Deposition
Removal
Removalprocess
process

Global
Globalemission
emission Derived
Derivedparameters,
parameters,
Spatial
Spatialdistribution
distribution model
modelvalidation:
validation:
Temporal
Temporaldistribution
distribution Optical
Opticaldepth
depth
Particle
Particleproperties
properties Radiative
Radiativeforcing
forcing

Fig. 10: An overview of LMDz INCA model

 Atmospheric Lifetime of
species

Board teaching done for the topic and gave class notes.

See page 22 to 27 of Seinfeld-pandis; mixing of species and its

atmospheric lifetime to see if it is well-mixed in atmospheric layer or
has gradient in distribution.
 Aerosol optical properties and
radiative forcing calculations

Board teaching done for the topic and gave class notes.

Beer-Lambert law, Mie theory. See also slides of chapter 6