introduction

1
LNOx Influence on Upper Tropospheric Ozone Lihua Wang 1 , Mike Newchurch 1 , Arastoo Biazar 1 , Williams Koshak 2 , Xiong Liu 3 1 Univ. of Alabama in Huntsville, 2 NASA/MSFC, 3 SAO&UMBC Introduction Lightning is a particularly significant NO x source (LNO x ) in the middle and upper troposphere where NO x is long-lived, typically at more dilute concentrations, and consequently more efficient at producing ozone than in the boundary layer where the majority of NO x is emitted. Currently, the CMAQ model does not count for NO x emission from lightning. However, it's important to quantify the effect of LNO x on tropospheric ozone concentration in order to make our model simulation more realistic, particularly in regions/periods with frequent lightning events. In this study, we will apply the National Lightning Detection Network (NLDN) lightning data as an extra NO x emission sources to the CMAQ model and then quantify the contributions of LNO x to tropospheric ozone. These quantitative values will be useful for parameterization in future modeling studies. NLDN The U.S. National Lightning Detection Network (NLDN) has been providing real-time, continental-scale information on cloud-to-ground (CG) lightning since 1989 (Cummins et al., 1998). After its most-recent system-wide upgrade in 2002, the CG flash detection efficiency (DE) has been improved into the range of 90-95% throughout the continental U.S. (Cummins et al., 2006). Parameterization We adjust CG flash counts for NLDN detection efficiency (DE) of ~95%. Scale up the CG flash counts to total flashes using a fixed IC:CG ratio value (3) which is close to the Boccippio et al. (2001) 4-yr mean IC:CG ratio value (2.94). Assume each flash produces 500 moles of NOx; 75% of LNOx as LNO and 25% as LNO 2 . Vertically distribute LNO x amounts into 39 layers of CMAQ model according to the mid-latitude continental profile specified in Pickering et al. (1998). D aily N O x em ission overC M AQ domain 0 5E+14 1E+15 2E+15 2E+15 3E+15 3E+15 4E+15 4E+15 7/14 7/19 7/24 7/29 8/3 8/8 8/13 8/18 8/23 8/28 9/2 9/7 Date NOx em ission (m olecules/cm 2/day) NO 2 em ission forCN TRL NO em ission forCN TRL LN O 2 LN O LNO x versus Total N O x em ission 0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.35 0.40 0.45 7/14 7/19 7/24 7/29 8/3 8/8 8/13 8/18 8/23 8/28 9/2 9/7 Date Ratio ofLNOx/total NOx em ission (a) (b) Figure 1. (a) Daily NO x emissions (molecules/cm2/day) over CMAQ domain for the CNTRL run as well as LNO x emission. (b) Ratio of daily LNO x production versus daily total NO x emission (including LNO x ). •Two model runs are made: •CNTRL: NOx emission only from the boundary layer; •CNTRL_LNOx: NOx emission from the boundary layer and lightning. (Both runs use pre-defined boundary conditions that may not represent the real atmosphere well) Figure 2. NO 2 emission during 0 GMT ~ 24 GMT, (a) July 29, 2006; (b) July 30, 2006. Upper left: NO 2 emission from CNTRL; Upper right: NO 2 emission for CNTRL_LNO x ; Bottom: LNO 2 . LNO x influenc e Figure 3. NO 2 column from OMI and CMAQ model. Upper: OMI tropospheric (left) and total (right) NO 2 column. Bottom: Tropospheric NO 2 at 19:00 GMT, from two CMAQ simulations: CNTRL (left) and CNTRL_LNO x (right). The CMAQ tropospheric NO 2 is calculated based on the tropopause pressure from OMI O 3 data. Figure 4. Tropopause pressure field from OMI O 3 data. CMAQ tropospheric columns of NO 2 and O 3 are calculated according to these pressures. Blank areas indicate failure of obtaining tropopause pressure from OMI O 3 data set. Ozone enhancemen t due to LNO x Ozone enhancement due to LNO x LNO x influence on CMAQ O 3 (compared with OMI O 3 ) (19:00 GMT, 7/30/2006) (19:00 GMT, 8/10/2006) Figure 5. Tropospheric ozone column from OMI and CMAQ model (CNTRL and CNTRL_LNO x runs). Evaluating LNO x influence on Ozone Prediction using ozonesonde measurements (Aug. 2006) Overall influence Not influenced Improved Significantly improved Figure 6. LNO x influenced O 3 at IONS06 stations. Three groups are divided Three groups are divided : Not influenced: Kelowna(26), Bratt’s Lake(28), Trinidad Head(29) Improved: Table Mountain(25), Holtsville(10), Boulder(27), Egbert(15), Paradox(5), Yarmouth(13), Walsingham(19), Narragansett(27) Significantly improved: Socorro(25), Houston(16), Ron Brown(23), Huntsville(29), Valparaiso(5), Beltsville(9), Wallops Island(10) Note: Digits indicate number of ozonesonde measurements within 15:00 ~ 23:00 GMT at each station. Consistent with Cooper et al., 2009 Figure 8. Monthly average location of a 20-day passive LNO x tracer that has been allowed to decay with a 4-day e-folding lifetime, indicating the regions where LNO x would most likely be found, as well as the regions where ozone production would most likely occur, for July through September 2006. Figure 9: Median filtered tropospheric ozone (FTO 3 ) mixing ratios during August 2006 at all 14 IONS06 measurement sites between 10 and 11 km. FTO 3 is the measured ozone within the troposphere with the model calculated stratospheric ozone contribution removed. Details on the methodology are given by Cooper et al. [2007]. Figure adapted from Cooper et al. [2007]. Figure 7. Mean normalized bias when model predicted O 3 (CNTRL and LNO x runs) and OMI O 3 are evaluated by ozonesonde measurements. Conclusions We estimate total lightning NO x amount from NLDN CG flashes based on a set of assumptions (DE~95%, IC:CG ratio ~ 3, LNO x production rate ~ 500 moles N per flash), and put them into 39 CMAQ model layers according to Pickering’s vertical distribution profile. LNO x contributes 27% to total NO x emission during July 15 ~ Sept. 7, 2006. Model prediction shows significant enhancement in upper tropospheric ozone concentration due to lightning-produced NO x above southeastern and eastern U.S. Kelown a Bratt’s Lake Trinidad Head Table MountainHoltvil le Socorro Boulder Housto n Huntsvil le Valparai so Walsingham Egbert Paradox Yarmouth Narragansett Beltsvi lle Wallops Island Research vessel Ron Brown LNO x impacts on model NO 2 prediction Contact info: Lihua Wang [email protected] The 90 th American Meteorological Society Annual Meeting, 17-21 January 2010 - Atlanta, GA NO 2 emission modified by LNO x Averaged during entire period: ~ 27%

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Not influenced Improved Significantly improved. Overall influence. Bratt’s Lake. Kelowna. Egbert. Paradox. Yarmouth. Valparaiso. Trinidad Head. Boulder. Narragansett. Walsingham. Beltsville. Wallops Island. LNO x influence. Socorro. Huntsville. - PowerPoint PPT Presentation

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Page 1: Introduction

LNOx Influence on Upper Tropospheric OzoneLihua Wang1, Mike Newchurch1, Arastoo Biazar1, Williams Koshak2, Xiong Liu3

1Univ. of Alabama in Huntsville, 2NASA/MSFC, 3SAO&UMBC

Introduction

Lightning is a particularly significant NOx source (LNOx) in the middle and upper troposphere where NOx is long-lived, typically at more dilute concentrations, and consequently more efficient at producing ozone than in the boundary layer where the majority of NOx is emitted.

Currently, the CMAQ model does not count for NOx emission from lightning.

However, it's important to quantify the effect of LNOx on tropospheric ozone concentration in order to make our model simulation more realistic, particularly in regions/periods with frequent lightning events.

In this study, we will apply the National Lightning Detection Network (NLDN) lightning data as an extra NOx emission sources to the CMAQ model and then quantify the contributions of LNOx to tropospheric ozone. These quantitative values will be useful for parameterization in future modeling studies.

NLDN

The U.S. National Lightning Detection Network (NLDN) has been providing real-time, continental-scale information on cloud-to-ground (CG) lightning since 1989 (Cummins et al., 1998). After its most-recent system-wide upgrade in 2002, the CG flash detection efficiency (DE) has been improved into the range of 90-95% throughout the continental U.S. (Cummins et al., 2006).

Parameterization

We adjust CG flash counts for NLDN detection efficiency (DE) of ~95%.

Scale up the CG flash counts to total flashes using a fixed IC:CG ratio value (3) which is close to the Boccippio et al. (2001) 4-yr mean IC:CG ratio value (2.94).

Assume each flash produces 500 moles of NOx; 75% of LNOx as LNO and 25% as LNO2.

Vertically distribute LNOx amounts into 39 layers of CMAQ model according to the mid-latitude continental profile specified in Pickering et al. (1998).

Daily NOx emission over CMAQ domain

0

5E+14

1E+15

2E+15

2E+15

3E+15

3E+15

4E+15

4E+15

7/14 7/19 7/24 7/29 8/3 8/8 8/13 8/18 8/23 8/28 9/2 9/7

Date

NO

x em

issi

on (m

olec

ules

/cm

2/da

y)

NO2 emission for CNTRL NO emission for CNTRL LNO2 LNO

LNOx versus Total NOx emission

0.00

0.05

0.10

0.15

0.20

0.25

0.30

0.35

0.40

0.45

7/14 7/19 7/24 7/29 8/3 8/8 8/13 8/18 8/23 8/28 9/2 9/7

Date

Rat

io o

f LN

Ox/

tota

l NO

x em

issi

on

(a) (b)

Figure 1. (a) Daily NOx emissions (molecules/cm2/day) over CMAQ domain for the CNTRL run as well as LNOx emission. (b) Ratio of daily LNOx production versus daily total NOx emission (including LNOx).

•Two model runs are made:

•CNTRL: NOx emission only from the boundary layer;•CNTRL_LNOx: NOx emission from the boundary layer and lightning.

(Both runs use pre-defined boundary conditions that may not represent the real atmosphere well)

Figure 2. NO2 emission during 0 GMT ~ 24 GMT, (a) July 29, 2006; (b) July 30, 2006. Upper left: NO2 emission from CNTRL; Upper right: NO2 emission for CNTRL_LNOx; Bottom: LNO2.

LNOx influence

Figure 3. NO2 column from OMI and CMAQ model. Upper: OMI tropospheric (left) and total (right) NO2

column. Bottom: Tropospheric NO2 at 19:00 GMT, from two CMAQ simulations: CNTRL (left) and CNTRL_LNOx (right). The CMAQ tropospheric NO2 is calculated based on the tropopause pressure from OMI O3 data.

Figure 4. Tropopause pressure field from OMI O3 data.CMAQ tropospheric columns of NO2 and O3 are calculated according to these pressures. Blank areas indicate failure of obtaining tropopause pressure from OMI O3 data set.

Ozone enhancement due to LNOx

Ozone enhancement due to LNOx

LNOx influence on CMAQ O3 (compared with OMI O3)

(19:00 GMT, 7/30/2006) (19:00 GMT, 8/10/2006)

Figure 5. Tropospheric ozone column from OMI and CMAQ model (CNTRL and CNTRL_LNOx runs).

Evaluating LNOx influence on Ozone Prediction using ozonesonde measurements (Aug. 2006)

Overall influence Not influenced Improved Significantly improved

Figure 6. LNOx influenced O3 at IONS06 stations.

Three groups are dividedThree groups are divided:

Not influenced: Kelowna(26), Bratt’s Lake(28), Trinidad Head(29)

Improved: Table Mountain(25), Holtsville(10), Boulder(27), Egbert(15), Paradox(5), Yarmouth(13), Walsingham(19), Narragansett(27)

Significantly improved: Socorro(25), Houston(16), Ron Brown(23), Huntsville(29), Valparaiso(5), Beltsville(9), Wallops Island(10)

Note: Digits indicate number of ozonesonde measurements within 15:00 ~ 23:00 GMT at each station.

Consistent with Cooper et al., 2009

Figure 8. Monthly average location of a 20-day passive LNOx tracer that has been allowed to decay with a 4-day e-folding lifetime, indicating the regions where LNOx would most likely be found, as well as the regions where ozone production would most likely occur, for July through September 2006.

Figure 9: Median filtered tropospheric ozone (FTO3) mixing ratios during August 2006 at all 14 IONS06 measurement sites between 10 and 11 km. FTO3 is the measured ozone within the troposphere with the model calculated stratospheric ozone contribution removed. Details on the methodology are given by Cooper et al. [2007]. Figure adapted from Cooper et al. [2007].

Figure 7. Mean normalized bias when model predicted O3 (CNTRL and LNOx runs) and OMI O3 are evaluated by ozonesonde measurements.

Conclusions

We estimate total lightning NOx amount from NLDN CG flashes based on a set of assumptions (DE~95%, IC:CG ratio ~ 3, LNOx production rate ~ 500 moles N per flash), and put them into 39 CMAQ model layers according to Pickering’s vertical distribution profile.

LNOx contributes 27% to total NOx emission during July 15 ~ Sept. 7, 2006.

Model prediction shows significant enhancement in upper tropospheric ozone concentration due to lightning-produced NOx above southeastern and eastern U.S.

Kelowna Bratt’s Lake

Trinidad Head

Table MountainHoltville

Socorro

Boulder

Houston

Huntsville

ValparaisoWalsingham

EgbertParadoxYarmouth

Narragansett

BeltsvilleWallops Island

Research vessel Ron Brown

LNOx impacts on model NO2 prediction

Contact info: Lihua Wang [email protected] 90th American Meteorological Society Annual Meeting, 17-21 January 2010 - Atlanta, GA

NO2 emission modified by LNOx

Averaged during entire period: ~ 27%