| 1. |
- Haslett, Sophie, 1988-, et al.
(author)
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Nighttime NO emissions strongly suppress chlorine and nitrate radical formation during the winter in Delhi
- 2023
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In: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:16, s. 9023-9036
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Journal article (peer-reviewed)abstract
- Atmospheric pollution in urban regions is highly influenced by oxidants due to their important role in the formation of secondary organic aerosol (SOA) and smog. These include the nitrate radical (NO3), which is typically considered a nighttime oxidant, and the chlorine radical (Cl), an extremely potent oxidant that can be released in the morning in chloride-rich environments as a result of nocturnal build-up of nitryl chloride (ClNO2). Chloride makes up a higher percentage of particulate matter in Delhi than has been observed anywhere else in the world, which results in Cl having an unusually strong influence in this city. Here, we present observations and model results revealing that atmospheric chemistry in Delhi exhibits an unusual diel cycle that is controlled by high concentrations of NO during the night. As a result of this, the formation of both NO3 and dinitrogen pentoxide (N2O5), a precursor of ClNO2 and thus Cl, are suppressed at night and increase to unusually high levels during the day. Our results indicate that a substantial reduction in nighttime NO has the potential to increase both nocturnal oxidation via NO(3 )and the production of Cl during the day.
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| 2. |
- Hofmann, Niklas, et al.
(author)
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Link between interlayer hybridization and ultrafast charge transfer in WS 2 -graphene heterostructures
- 2023
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In: 2D Materials. - 2053-1583. ; 10:3
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Journal article (peer-reviewed)abstract
- Ultrafast charge separation after photoexcitation is a common phenomenon in various van-der-Waals (vdW) heterostructures with great relevance for future applications in light harvesting and detection. Theoretical understanding of this phenomenon converges towards a coherent mechanism through charge transfer states accompanied by energy dissipation into strongly coupled phonons. The detailed microscopic pathways are material specific as they sensitively depend on the band structures of the individual layers, the relative band alignment in the heterostructure, the twist angle between the layers, and interlayer interactions resulting in hybridization. We used time- and angle-resolved photoemission spectroscopy combined with tight binding and density functional theory electronic structure calculations to investigate ultrafast charge separation and recombination in WS2-graphene vdW heterostructures. We identify several avoided crossings in the band structure and discuss their relevance for ultrafast charge transfer. We relate our own observations to existing theoretical models and propose a unified picture for ultrafast charge transfer in vdW heterostructures where band alignment and twist angle emerge as the most important control parameters.
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| 3. |
- Mishra, Suneeti, et al.
(author)
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Rapid night-time nanoparticle growth in Delhi driven by biomass-burning emissions
- 2023
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In: Nature Geoscience. - : Springer Science and Business Media LLC. - 1752-0894 .- 1752-0908. ; 16:3, s. 224-230
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Journal article (peer-reviewed)abstract
- Natural and anthropogenic biomass burning are among the major sources of particulate pollution worldwide that affects air quality, climate and human health. Delhi, one of the world’s most populated cities, experiences severe haze events caused by particulate pollution during winter, but the underlying pathways remain poorly understood. Here we observe intense and frequent nocturnal particle growth events during haze development in Delhi from measurements of aerosols and gases during January–February at the Indian Institute of Technology in Delhi. The particle growth events occur systematically despite the unfavourable condition for new-particle formation, including the lack of photochemical production of low-volatility vapours and considerable loss of vapours under extremely polluted conditions. We estimate that this process is responsible for 70% of the total particle-number concentration during haze. We identify that the condensation of primary organic vapours from biomass burning is the leading cause of the observed growth. The sharp decrease in night-time temperatures and rapid increase in biomass-burning emissions drive these primary organic vapours out of equilibrium, resulting in their condensation and the growth of nanoparticles into sizes relevant for haze formation. This high impact of primary biomass-burning emissions on night-time nanoparticle growth is unique compared with most urban locations globally, where low-volatility vapours formed through oxidation during the day drive particle growth and haze formation. As uncontrolled biomass burning for residential heating and cooking is rife in the Indo–Gangetic plain, we expect this growth mechanism to be a source of ultrafine particles, affecting the health of 5% of the world’s population and impacting the regional climate. Our work implies that regulating uncontrolled biomass-combustion emissions may help inhibit nocturnal haze formation and improve human health in India.
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