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Trends in N<sub>2</sub>O and SF<sub>6</sub> mole fractions in archived air samples from Cape Meares, Oregon (USA), 1978–1996
oleh: T. C. Rolfe, A. L. Rice
Format: | Article |
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Diterbitkan: | Copernicus Publications 2019-07-01 |
Deskripsi
<p>Quantifying historical trends in atmospheric greenhouse gases (GHGs) is important to understanding changes in their budgets and for climate modeling, which simulates historic and projects future climate. Archived samples analyzed using updated measurement techniques and calibration scales can reduce uncertainties in historic records of GHG mole fractions and their trends in time. Here, we present historical measurements of two important GHGs, nitrous oxide (<span class="inline-formula">N<sub>2</sub>O</span>) and sulfur hexafluoride (<span class="inline-formula">SF<sub>6</sub></span>), collected at the midlatitude Northern Hemisphere station Cape Meares, Oregon (USA, 45.5<span class="inline-formula"><sup>∘</sup></span> N, 124<span class="inline-formula"><sup>∘</sup></span> W), between 1978 and 1996 in archived air samples from the Oregon Health and Science University – Portland State University (OHSU–PSU) air archive. <span class="inline-formula">N<sub>2</sub>O</span> is the third most important anthropogenically forced GHG behind carbon dioxide (<span class="inline-formula">CO<sub>2</sub></span>) and methane (<span class="inline-formula">CH<sub>4</sub></span>). <span class="inline-formula">SF<sub>6</sub></span> has a low abundance in the atmosphere, but is one of the most powerful GHGs known. Measurements of atmospheric <span class="inline-formula">N<sub>2</sub>O</span> made during this period are available for select locations, but before mid-1990 they have larger uncertainties than more recent periods due to advancements made in gas chromatography (GC) methods. Few atmospheric <span class="inline-formula">SF<sub>6</sub></span> measurements exist pre-1990, particularly in the Northern Hemisphere. The GC system used to measure <span class="inline-formula">N<sub>2</sub>O</span> and <span class="inline-formula">SF<sub>6</sub></span> mixing ratios in this work is designed to be fully automated, and is capable of running up to 15 samples per batch. Measurement precision (1<span class="inline-formula"><i>σ</i></span>) of <span class="inline-formula">N<sub>2</sub>O</span> and <span class="inline-formula">SF<sub>6</sub></span> is 0.16 % and 1.1 %, respectively (evaluated at 328.7 ppb and 8.8 ppt). Samples were corrected for detector response nonlinearity when measured against our reference standard, with the corrections determined to be 0.14 ppb ppb<span class="inline-formula"><sup>−1</sup></span> in <span class="inline-formula">N<sub>2</sub>O</span> and 0.03 ppt ppt<span class="inline-formula"><sup>−1</sup></span> in <span class="inline-formula">SF<sub>6</sub></span>. The mixing ratio of <span class="inline-formula">N<sub>2</sub>O</span> in archived samples is found to be <span class="inline-formula">301.5±0.3</span> ppb in 1980 and rises to <span class="inline-formula">313.5±0.3</span> ppb in 1996. The average growth rate over this period is <span class="inline-formula">0.78±0.03</span> ppb yr<span class="inline-formula"><sup>−1</sup></span> (95 % CI). The seasonal amplitude is statistically robust, with a maximum anomaly of 0.3 ppb near April and a minimum near November of <span class="inline-formula">−0.4</span> ppb. Measurements of <span class="inline-formula">N<sub>2</sub>O</span> match well with previously reported values for Cape Meares and other comparable locations. The mixing ratio of <span class="inline-formula">SF<sub>6</sub></span> in analyzed samples is found to be <span class="inline-formula">0.85±0.03</span> ppt in 1980 and rises to <span class="inline-formula">3.83±0.03</span> ppt in 1996. The average growth rate over this period is <span class="inline-formula">0.17±0.01</span> ppt yr<span class="inline-formula"><sup>−1</sup></span> (95 % CI). The seasonality is statistically robust and has an annual peak amplitude of 0.04 ppt near January and a minimum amplitude of <span class="inline-formula">−0.03</span> ppt near July. These are unique <span class="inline-formula">SF<sub>6</sub></span> results from this site and represent a significant increase in the <span class="inline-formula">SF<sub>6</sub></span> data available during the 1980s and early 1990s. The mixing ratio and growth rate of <span class="inline-formula">SF<sub>6</sub></span> measured compares well to other Northern Hemisphere measurements over this period. From these <span class="inline-formula">N<sub>2</sub>O</span> and <span class="inline-formula">SF<sub>6</sub></span> measurements, we conclude that sample integrity is generally robust in the OHSU-PSU air archive for <span class="inline-formula">N<sub>2</sub>O</span> and <span class="inline-formula">SF<sub>6</sub></span>.</p>