Spatial and temporal dynamics of atmospheric pollutants in

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Spatial and temporal dynamics of atmospheric pollutants in London, UK. Carole Helfter, Eiko Nemitz,

Spatial and temporal dynamics of atmospheric pollutants in London, UK. Carole Helfter, Eiko Nemitz, Chiara Di Marco, Ben Langford, Neil Mullinger, Ute Skiba • To provide a top-down validation of bottom-up emission inventories • (i) emissions of CO, CO 2 and aromatic VOCs are well captured by atmospheric inventories; • (ii) NOx and CH 4 are underestimated.

Long-term Measurements in London Anemometer & sampling inlet Timeline of Measurements • 2006 -

Long-term Measurements in London Anemometer & sampling inlet Timeline of Measurements • 2006 - CO 2/CO/VOC Fluxes (campaign) • 2007 - PM 1 Aerosol Fluxes (campaign) • 2011 – Continuous EC fluxes of CO 2/CO/CH 4/H 2 O • 2012 -2013 - NOx and O 3 fluxes • 2014 – N 2 O fluxes (Campaign) • 2015 – N 2 O fluxes Instrument location Sampling height 190 m above street level

The BT Tower – Flux Footprint 90 th percentile 10 th percentile Flux Footprint

The BT Tower – Flux Footprint 90 th percentile 10 th percentile Flux Footprint §. Central London §Footprint 180 km 2. § Mean building height 12 m. § Typically 2 -4 km from the tower (6 km to North). § N-NW: Mainly residential. § E & W: gradient commercial – residential. § SE – SW: heavily built-up, commercial. § Footprint entrains Thames river SE of tower

Flux Inventory Measurements Top-down Validation of Emission Inventories: GHGs Annual budgets: Excellent agreement between

Flux Inventory Measurements Top-down Validation of Emission Inventories: GHGs Annual budgets: Excellent agreement between measurements and inventory (CO and CO 2) Large spatial variability and seasonality observed for all 3 gases but discrepancy between measured and inventory CH 4 budget. What CH 4 source(s) is the inventory missing/ underestimating? Perhaps biogenic?

Top-down Validation of Emission Inventories: NOx West Footprint • Urban parkland • Lower traffic

Top-down Validation of Emission Inventories: NOx West Footprint • Urban parkland • Lower traffic density • Traffic < NOx source East Footprint • Fewer green areas • Higher traffic density • Traffic > NOx source Lee, J. D. et al. : Environ. Sci. Technol. 49, 1025 -1034, 2015.

Top-down Validation of Emission Inventories: VOCs Temporal Trends Acetaldehyde Isoprene Comparison with NAEI Benzene

Top-down Validation of Emission Inventories: VOCs Temporal Trends Acetaldehyde Isoprene Comparison with NAEI Benzene Flux Measurements Fluxes and concentrations highest in August and September (coupled to light and air temperature). VOC [t km-2 yr-1] National Atmospheric Emission Inventory (NAEI) Fluxes: low seasonality (50% -90% emissions attributed to traffic). Boundary layer height or advection explains winter increase in concentrations. Langford, B. et al. : Atmos. Chem. Phys. , 10, 627 -645, 2010. Valach, A. et al. : Atmos. Chem. Phys. , 15, 7777– 7796, 2015.