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Atmospheric Methane Isotope Records Covering the Holocene Period

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Atmospheric Methane Isotope Records Covering the Holocene Period Quaternary Science Reviews 29 (2010) 213–221 Contents lists available at ScienceDirect Quaternary Science Reviews journal homepage: www.elsevier.com/locate/quascirev Atmospheric methane isotope records covering the Holocene period Todd Sowers The Earth and Environmental Systems Institute, Penn State University, 317B EESB Building, University Park, PA 16802, United States article info abstract Article history: 13 12 d13 d Records of the C/ C( CH4) and the D/H ( DCH4 ) ratio of atmospheric methane were recovered from Received 15 January 2009 13 the GISP II ice core covering the last 11,000 years. All totaled, 76 samples were analyzed for d CH4 and 65 Received in revised form d adjacent samples for DCH between 86 and 1696 m below surface (mbs) providing a temporal resolution 22 May 2009 4 that is better than one pair of isotope samples every 200 years. The d13CH record exhibits a decreasing Accepted 27 May 2009 4 trend throughout the Holocene beginning at À46.4& at 11,000 years BP (BP defined as 1950 AD ¼ 11 ka), 13 and decreasing to À48.4& at 1 ka. The 2& d CH4 drop is likely to be a combination of increased CH4 emissions from Arctic lake ecosystems and an increase in the ratio of C3/C4 plants in wetlands where CH4 is emitted. The C3/C4 ratio increase is the result of increasing CO2 values throughout the Holocene combined with the activation of high NH ecosystems that are predominantly C3 type. d The DCH record over the early-mid Holocene shows a slightly decreasing trend that would be pre- 4 d dicted by increased CH4 emissions from Arctic lakes. Between 4 ka and 1 ka, DCH4 values increase by 13 w20& while d CH4 values remain effectively constant. There are at least two plausible explanations for & d this 20 DCH4 shift. First, a dramatic shift in CH4 emissions from higher latitudes to the tropics could 13 account for the observed shift though the lack of a corresponding d CH4 shift is difficult to reconcile. d d Secondly, a gradual release of marine clathrates with enriched DCH4 values explains both the DCH4 and 13 d CH4 records over this period. Ó 2009 Elsevier Ltd. All rights reserved. 1. Introduction The strong coupling between circum-N. Atlantic climate and CH4 variations does not, however, hold during the Holocene (Fig. 1). Atmospheric CH4 records illustrate variability on numerous High-resolution CH4 records covering the Holocene show moder- timescales. The longest record from the EPICA project covering the ately high CH4 values (w700 ppb) during the Pre Boreal period last 800,000 years (800 kyr) document low CH4 values (w350 ppb) (9.5–11 kyr before present, 9.5–11 ka). Between 9.5 and 5.5 ka, CH4 during the coldest parts of the glacial periods and relatively high drops gradually to w580 ppb before it slowly rises to preindustrial (600–700 ppb) values during warm interglacial periods (Spahni values (w700 ppb) by 1 ka (1000 AD). Finally, the last 200 years et al., 2005; Loulergue et al., 2008). Embedded within the normal show a dramatic CH4 doubling due to increased anthropogenic glacial/interglacial cycle, CH4 variations have a significant amount emissions making CH4 the second most important long-lived of variability associated with the 20 kyr precession bandwidth that greenhouse gas in the atmosphere today (Forster et al., 2007). The is attributed to a monsoonal influence on tropical wetland CH4 ‘‘bowl’’ shaped CH4 curve during the Holocene is disconnected from emissions (Chappellaz et al., 1990; Brook et al., 1996). Furthermore, the stable temperature records that dominate the circum N. 18 millennial scale CH4 fluctuations appear to be tightly coupled with Atlantic as illustrated by the isotopic temperature (d Oice) record Dansgaard/Oeschger climate oscillations during glacial periods from GISP II in Fig. 1. with higher CH4 values associated with warmer interstadial periods Three prominent hypotheses have been put forth to explain the (Chappellaz et al., 1993). The strong coupling between atmospheric Holocene CH4 record. The Ruddiman hypothesis posits that early CH4 values and Greenland temperatures has been interpreted to civilizations began to influence atmospheric CH4 levels beginning imply a strong teleconnection between circum-N. Atlantic climate about 5 ka (Ruddiman, 2003). The basis for this hypothesis is the and the global hydrologic cycle (Chappellaz et al., 1993; Brook et al., strong coupling between CH4 and NH insolation as modulated by 1996). Asian–African monsoons (Loulergue et al., 2008). The hypothesis has been supported by the correlation between decreasing NH insolation and CH4 concentrations during previous interglacial E-mail address: [email protected] periods (with the exception of marine isotope stage 11) (Ruddiman 0277-3791/$ – see front matter Ó 2009 Elsevier Ltd. All rights reserved. doi:10.1016/j.quascirev.2009.05.023 214 T. Sowers / Quaternary Science Reviews 29 (2010) 213–221 -34 -36 18 Oice (‰ SMOW) -38 GRIPCH4 ice O -40 Taylor DomeCH4 18 GISPCH4 900 Dome CCH4 Chappellaz 1997 800 Brook 2000 CH 700 4 (ppb) 600 500 400 50 (ppb) 4 40 30 N-S CH 0 2 4 6 8 10 12 Calendar Age (ka) Fig. 1. Methane concentration records covering the Holocene. The upper curve is the isotopic temperature record from GISP II (Grootes et al., 1993). The middle curves are methane concentration records from GRIP (Blunier et al., 1995), Taylor Dome (Brook et al., 2000), GISP II (Brook et al., 1996), Dome C (Flu¨ ckiger et al., 2002). The bottom portion of the figure illustrates the interpolar CH4 gradient (IPG) from (Chappellaz et al., 1997), and (Brook et al., 2000). and Thomson, 2001). Early rice agricultural practices (excessive weighted balance of all sources and sinks and their characteristic flooding) yielded higher per capita CH4 emissions than today such isotope effects. Atmospheric CH4 changes can thus be the result of that even though world population was extremely low, humans changes in sources, sinks or some combination of the two. CH4 actually had a progressively higher impact on atmospheric CH4 isotope records from ice cores, therefore, provide fundamental loadings between 5 ka and the present. Ruddiman suggests that the boundary conditions for assessing the cause of observed concen- decline in the interpolar CH4 gradient (IPG) between 4 ka and 0.8 ka tration variations. For example, atmospheric CH4 levels increased supports his hypothesis because the population increases during from 450 to 600 ppb near the end of the Younger Dryas period w d13 d this period were centered on the equator, causing the reduced IPG 11.5 ka. CH4 and DCH4 records covering this transition show in the late Holocene. no discernable trends associated with the increased CH4 values Another prominent hypothesis put forward to explain the (Schaefer et al., 2006; Sowers, 2006; Fischer et al., 2008). While Holocene CH4 record points to changes in tropical wetland emis- there are many plausible explanations for the lack of an isotope sions as the primary driving force (Chappellaz et al., 1997). Under signature accompanying this particular concentration increase, the this hypothesis, the broad CH4 minimum at 5 ka is driven by lower most straightforward explanation maintains a constant proportion tropical CH4 emissions while, the IPG record is primarily driven by of both emissions and sinks, while global sources increase relative d moderate changes in tropical emissions along with more subtle to the sink terms. Moreover, the lack of a substantial DCH4 increase changes in NH wetland emissions. Because tropical wetlands are by during this period ruled out a massive clathrate destablization far the largest natural source of CH4 and clearly tied to NH insola- event as the cause of the concentration increase (Sowers, 2006). tion via the monsoons, small changes in the hydrologic cycle in the Important information pertaining to the latitudinal sources of tropics can yield large changes in atmospheric CH4 loading over CH4 can be derived from the interpolar CH4 gradient (IPG). Because very short time periods. the primary CH4 sink (tropospheric OH radicals) is uniformly The third set of ideas put forth to explain the concentration history distributed about the equator, the N–S CH4 IPG is a qualitative involves changes in the sink term for atmospheric CH4. The concen- measure of N–S source distribution. Continuous atmospheric CH4 tration of CH4 in the atmosphere is always controlled by the balance measurements throughout the globe today illustrate the prepon- between the sources and sinks. Thus, the decreasing concentration derance of NH CH4 sources that yield IPG estimates for the last two trend in the early to mid part of the Holocene could be the result of an decades between 125 and 145 ppb (Dlugokencky et al., 2003). increase in the rate at which CH4 is removed from the atmosphere as Historical IPG estimates can be reconstructed from ice cores by opposed to a decrease in the sources. Present day estimates of the analyzing CH4 in Greenland and Antarctic ice core samples that primary CH4 sinks suggest tropospheric OH radicals account for 88% were occluded at the same time. The accuracy of these paleoIPG of total while soils and stratospheric destruction make up5% and 7%of estimates depends on how well the two ice core timescales can be total (Reeburgh, 2004). Tropospheric OH radicals are also the primary established and the analytical uncertainties associated with the sink for volatile organic compounds (VOCs) and CO. As such, changes CH4 measurements (Da¨llenbach et al., 2000). There are two studies in the atmospheric loading of these entities will have an impact on the that have attempted to reconstruct Holocene IPG values from ice lifetime of atmospheric CH4 that is independent of the CH4 sources. cores. Chappellaz et al.
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