Impact of Cosmic Rays on Stratospheric Chlorine Chemistry and Ozone Depletion

Müller, Rolf

doi:10.1103/physrevlett.91.058502

Cited by 34 publications

(12 citation statements)

References 26 publications

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“…On the surface of amorphous solid water, the signal for e − (aq ) persists on a timescale of minutes (113) and can induce dissociative electron attachment in chlorofluorocarbons (114). This may suggest a role for hydrated electrons in atmospheric chemistry occurring on ice particles (115)(116)(117), in which the electrons are generated by cosmic rays, although this claim remains controversial (118,119).…”

Section: Photoelectron Spectroscopymentioning

confidence: 99%

The Hydrated Electron

Herbert

Coons

2017

Annu. Rev. Phys. Chem.

169

181

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Existence of a hydrated electron as a byproduct of water radiolysis was established more than 50 years ago, yet this species continues to attract significant attention due to its role in radiation chemistry, including DNA damage, and because questions persist regarding its detailed structure. This work provides an overview of what is known in regards to the structure and spectroscopy of the hydrated electron, both in liquid water and in clusters [Formula: see text], the latter of which provide model systems for how water networks accommodate an excess electron. In clusters, the existence of both surface-bound and internally bound states of the excess electron has elicited much debate, whereas in bulk water there are questions regarding how best to understand the structure of the excess electron's spin density. The energetics of the equilibrium species e(aq) and its excited states, in bulk water and at the air/water interface, are also addressed.

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Section: Photoelectron Spectroscopymentioning

confidence: 99%

The Hydrated Electron

Herbert

Coons

2017

Annu. Rev. Phys. Chem.

169

181

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“…Therefore, measures of chemical polar ozone depletion are commonly employed that rely solely on total column ozone data (e.g., Newman et al, 2004;Bodeker et al, 2005;Huck et al, 2007). Such simple measures include the average total column ozone in spring (March, NH and October, SH) poleward of 63 • , or the minimum of daily total column ozone minima over the polar cap (e.g., Newman et al, 1997;Müller, 2003;Austin et al, 2003;WMO, 2003;Eyring et al, 2006;WMO, 2007). In particular, the average March total column ozone poleward of 63…”

Section: Introductionmentioning

confidence: 99%

Simple measures of ozone depletion in the polar stratosphere

Müller¹,

Grooß²,

Lemmen³

et al. 2007

Preprint

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Abstract. We investigate the extent to which commonly considered quantities, based on total column ozone observations and simulations, are applicable as measures of ozone loss in the polar vortices. Such quantities have been used frequently in ozone assessments by the World Meteorological Organization (WMO) and to assess the performance of chemistry-climate models. The most commonly considered quantity is monthly mean column ozone poleward of a latitude of 63° in spring. For the Arctic, these monthly means were found to be insensitive to the exact choice of the latitude threshold, unlike the Antarctic where greater sensitivity was found. Choosing a threshold based on the location of the transport barrier at the vortex boundary instead of geometric latitude led to a roughly similar year-to-year variability of the monthly means, but in particular years deviations of several tens of Dobson units occurred. Moreover, the minimum of daily total ozone minima poleward of a particular latitude, another popular measure, is debatable, insofar as it relies on one single measurement or model grid point. For Arctic conditions, this minimum value occurred often in air outside polar vortex, both in the observations and in a chemistry-climate model. As a result, we recommend that the minimum of daily minima no longer be used when comparing polar ozone loss in observations and models. As a possible alternative, we suggest considering the minimum of daily average total ozone poleward of a particular equivalent latitude (or in the vortex) in spring. This definition both obviates relying on one single data point and reduces the impact of year-to-year variability in the Arctic vortex breakup on ozone loss measures. However, compact relations of such simple measures with meteorological quantities that describe the potential for polar heterogeneous chlorine activation and thus ozone loss were not found. Therefore, we argue that where possible, more sophisticated measures of chemical polar ozone loss that include additional information to disentangle the impact of transport and chemistry on ozone, should be employed.

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“…The dissociative electron transfer (DET), the equivalent of DEA in the condensed phase, from the ice to the adsorbed molecules was suggested as an additional source of halogen radicals in the stratosphere . The contribution of this process to the ozone depletion was subject of some controversy and discussion in the atmospheric community, and it probably does not play as important role in the stratosphere as suggested originally. Nevertheless, a striking enhancement of Cl − yield by several orders of magnitude was observed experimentally upon deposition of CF 2 Cl 2 on ice surface and DET from the ice to the molecule, and for other chlorofluorocarbon molecules the enhancement was measured as well .…”

Section: Examples Of Atmospheric Cluster Studiesmentioning

confidence: 99%

Section: Electron Attachmentmentioning

confidence: 99%

Mass spectrometry of aerosol particle analogues in molecular beam experiments

Fárnı́k

Lengyel

2017

Mass Spectrometry Reviews

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Nanometer-size particles such as ultrafine aerosol particles, ice nanoparticles, water nanodroplets, etc, play an important, however, not yet fully understood role in the atmospheric chemistry and physics. These species are often composed of water with admixture of other atmospherically relevant molecules. To mimic and investigate such particles in laboratory experiments, mixed water clusters with atmospherically relevant molecules can be generated in molecular beams and studied by various mass spectrometric methods. The present review demonstrates that such experiments can provide unprecedented details of reaction mechanisms, and detailed insight into the photon-, electron-, and ion-induced processes relevant to the atmospheric chemistry. After a brief outline of the molecular beam preparation, cluster properties, and ionization methods, we focus on the mixed clusters with various atmospheric molecules, such as hydrated sulfuric acid and nitric acid clusters, N O and halogen-containing molecules with water. A special attention is paid to their reactivity and solvent effects of water molecules on the observed processes.

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Impact of Cosmic Rays on Stratospheric Chlorine Chemistry and Ozone Depletion

Cited by 34 publications

References 26 publications

The Hydrated Electron

The Hydrated Electron

Simple measures of ozone depletion in the polar stratosphere

Mass spectrometry of aerosol particle analogues in molecular beam experiments

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