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Simulation of Carbonyl Sulfide (COS) to better understand the urban biosphere signal

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Simulation of Carbonyl Sulfide (COS) to better understand the urban biosphere signal

Background

Currently, anthropogenic CO2emissions over urban regions can be calculated in several ways: 1) bottom-up approaches (or inventories) based on energy consumption within city limits and emission factors that depend on type of fuel and processes, 2) using14CO2as tracer for fossil CO2, and 3) subtracting the biosphere signal from observation (measured) CO2data. All of these approaches have their limitations. Given the immense amount of time and resources needed to develop inventories (1), generic emission factors and data assumptions are often used which result in a high degree of uncertainty. Additionally, temporal extrapolation and spatial redistribution lead to further uncertainties. Albeit14CO2is an ideal tracer for fossil CO2because14C is entirely lost to radioactive decay in fossil fuels, the high costs and technological requirements of radio isotope measurements make method (2) hardly reproducible in the long term and high frequency required to monitor urban emissions. There are many biosphere models that can be used to determine the biosphere signal to apply method (3), but it is not always clear which one has the best approximation of net ecosystem exchange (NEE) and the differences are significant.

Gara Villalba

1,2

, Xavier Gabarrell

1

, Elliott Campbell

2

1

Dept. of Chemical, Biological and Environmental Engineering, Autonomous University of Barcelona, Spain (Gara.Villalba@uab.es)

2

Sierra Nevada Research Institute and School of Engineering, UC Merced, California

Abstract

We suggest that COS can be used to determine which ecosystem model best represents the biosphere signal. Just like CO2, COS is taken up by photosynthesis but is not given off in respiration and can thus be used as a trace gas to estimate GPP. We begin with COS surface fluxes provided by SiB and CASA, regridded to lower resolution using NDVI values, for a 9, 3, and 1 km-resolution domain over the Bay Area of San Francisco and part of the San Joaquin Valley. Simulations using the atmospheric model WRF provide the meteorological data, which along with the COS fluxes, are used to run the transport model STEM over a 20-day period in March 2015. Simulations of COS mixing ratio based on the various surface flux models are compared to observed data available from several locations. The model that best represents COS uptake consequently also provides the most accurate simulation of CO2biosphere signal, and can be used to estimate fossil fuel CO2emissions.

Methods

3 nested domains are centered over the city of Livermore, CA.

Resolutions: d01 9km, d02 3km, and d03 1km.

Model

WRF

Model version: 3.7.1 (August 13, 2015) Simulation period: March 5-25 2015 PBL scheme: Mellor-Yamada-Janjic (Eta) TKE

Land surface model: NOAH

Cumulus: Grell-Devenyi ensemble scheme STEM Sulfur Transport. dEposition Model

Calculations:

Where:

1.84: LRU (Stimler et al 2012)

1.1: average ambient [COS]/[CO2] ratio from INTEX/NA experiment (Blake et al 2004)

Domain Calculating COS surface fluxes based on NDVI

𝑁𝐷𝑉𝐼 𝑣𝑎𝑙𝑢𝑒 𝑓𝑜𝑟 1 𝑁𝐷𝑉𝐼 𝑝𝑖𝑥𝑒𝑙 𝑁𝐷𝑉𝐼 𝑣𝑎𝑙𝑢𝑒 𝑓𝑜𝑟 𝑒𝑛𝑡𝑖𝑟𝑒 𝑆𝑇𝐸𝑀 𝑑𝑜𝑚𝑎𝑖𝑛 𝑆𝑖𝐵 𝐶𝑂𝑆 𝑓𝑙𝑢𝑥 𝑣𝑎𝑙𝑢𝑒

(entire STEM domain) 𝐶𝑂𝑆 𝑓𝑙𝑢𝑥 𝑣𝑎𝑙𝑢𝑒 𝑓𝑜𝑟 1 𝑝𝑖𝑥𝑒𝑙

SiB surface flux 1.25º x 1.0º MODIS NDVI 1km or 250 m

X =

Using STEM to determine COS mixing ratios

Surface flux and drawdown (difference between 450 ppt and simulated COS surface concentrations) is shown below on left for a typical day reflecting mean flow conditions, north-westerly winds, significant drawdown over the continent and less drawdown over the ocean. The model also showed some synoptic events in which continental air is brought to the ocean, and is brought back to the land again, showing atypical drawdowns such as is shown below on the right.

Results

✓NOAA Sutro tower measurements in San Francisco (Montzka JGR, 2007) are on average upwind from study area of Livermore and provides background COS and CO2mixing ratios (average of 505 ppt and 405 ppm, respectively, for study period).

✓Seasonal variations are about 10-15%, and are similar to previous studies).

✓Synoptic variation during study period shown in zoomed-in box, is about 10%.

✓COS measurements are taken twice daily, not every day (15 measurements during study period).

✓Sandia location.

✓505 ppt background included.

✓Amplitude: approx 20 ppt

✓Wave: 24-hour variation, min 450, 461 ppt and max 503, 500 ppt, for SiB and CASA respectively.

✓Synoptic event happening on 3/21 after which COS concentrations rise by 20 ppt.

Potential continental influence until 21, after which marine air (less plant influence) seems more prominent.

✓CO2background value of 405 ppm.

✓modeled total CO2 underestimates observed CO2, suggesting higher fossil CO2than determined by Vulcan inventories.

✓better model results during marine influence.

✓highest concentrations of total CO2occur in early am, confirming other studies (Feng et al.,ACF, 2016).

✓Modeled COS mixing ratios are high at night (up to 503 ppt), then start to drop late morning/noon, reaching lowest values between 12:00 and 16:00 (down to 460 ppt for CASA and 450 for SiB).

✓Model results are not in phase with observations, by about 10 hours during continental influence (before March 20th), and by about 5 hours during marine influence (after March 21st). We found this discrepancy between observed and modeled results in another COS study of the Redwoods in California, and are presently working on tweaking STEM to improve mixing ratio calculations.

✓Mean wind speed at z=1 (Sandia tower at 13 meters).

✓Similar patterns and phases.

Acknowledgements:This work is possible thanks to Marie Sklodowska Curie grant 653950 UrbanCO2Flux, financed by the European Commission Horizon 2020, as well as UCOP Lab Fee.

300 320 340 360 380 400 420 440

300 350 400 450 500 550 600 650 700 750

CO2 ppm

COS ppt

Local time in Livermore, CA

Observed concentrations at Sutro Tower SUTRO COS Sutro CO2

Study period

350 400 450 500 550 600

COS mixing ratio ppt SANDIA observed SUTRO observed

0 200 400 600 800 1000 1200 1400 1600

150 200 250 300 350 400 450 500 550 600

meters

COS mixing ratio ppt

Local time at Livermore, CA

COS STEM runs with MODIS method

SiB STEM ppt observed Sandia ppt CASA STEM ppt PBLH m spin up

✓ Observed is highest in the middle of the day coinciding with deepest boundary layer, which has a greater effect on the mixing ratio (due to increased mixing) than the capture of COS by photosynthesis.

These findings are coherent with previous studies of forested areas.

330 360 390 420 450 480

ppm

Local time in Livermore, CA

CO2mixing ratio ppm total CO2 observed Sandia Vulcan CO2

TOTAL CO2= CO2 background+ CO2 respiration+ CO2 fossil– CO2 GEE

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