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Subject Areas
Carbon Cycle
Climate
Coastal Sensitivity to Sea Level Rise
Energy and Socioeconomic Systems
Land-Use and Ecosystems
Oceanic Trace Gases
Solar and Atmospheric Radiation
Trace Gas Emissions
Vegetation Response to CO2 and Climate
Fossil-Fuel CO2 Emissions
Atmospheric Trace Gas Measurements
Terrestrial Carbon Management
Carbon-14 Measurements in Atmospheric CO2 from Northern and Southern Hemisphere Sites, 1962-1993
Contributed byReidar Nydal and Knut Lövseth
Prepared byVirgene Zumbrunn* and Thomas A. Boden
*ORISE summer intern Environmental Sciences Division Publication No. 4582 Date Published: November 1996 Prepared for the
Prepared by the
DOI10.3334/CDIAC/atg.ndp057 CONTENTS
LIST OF FIGURES1. Sampling network for tropospheric 14C measurements in atmospheric CO2
LIST OF TABLES1. Summary of the tropospheric 14CO2 sampling sites
ABSTRACTNydal, R., and K. Lövseth. 1996. Carbon-14 Measurements in Atmospheric CO2 from Northern and Southern Hemisphere Sites, 1962-1993. ORNL/CDIAC-93, NDP-057. Carbon Dioxide Information Analysis Center, Oak Ridge National Laboratory, Oak Ridge, Tennessee. 67 pp. doi: 10.3334/CDIAC/atg.ndp057 In the 1960s, thermonuclear bomb tests released significant pulses of radioactive 14C into the atmosphere. This major perturbation allowed scientists to study the dynamics of the global carbon cycle by measuring and observing rates of isotopic exchange. The Radiological Dating Laboratory at the Norwegian Institute of Technology performed 14C measurements in atmospheric CO2 from 1962 to 1993 at a network of ground stations in the Northern and Southern hemispheres. These measurements were supplemented during 1965 with high-altitude (9-12.6 km) air samples collected using aircraft from the Norwegian Air Force. The resulting database, coupled with other 14C data sets, provides a greater understanding of the dynamic carbon reservoir and a crude picture of anomalous sources and sinks at different geographical latitudes. This database is outstanding for its inclusion of early 14C measurements, broad spatial coverage of sampling, consistency of sampling method, and Δ14C calculation results corrected for isotopic fractionation and radioactive decay. This database replaces previous versions published by the authors and the Radiological Dating Laboratory. Fourteen stations spanning latitudes from Spitsbergen (78°N) to Madagascar (21°S) were used for sampling during the lifetime of the Norwegian program. Some of the stations have data for only a brief period, while others have measurements through 1993. Sampling stations subject to local industrial CO2 contamination were avoided. The sites have sufficient separation to describe the latitudinal distribution of 14C in atmospheric models. The sampling procedure for all the surface (10-2400 m asl) 14C measurements in this database consisted of quantitative absorption of atmospheric CO2 in carbonate-free 0.5 N NaOH solution. The 14C measurements were made in a CO2 proportional counter and calculated (δ14C) as per mil excess above the normal 14C level defined by the US National Institute of Standards and Technology (NIST). Atmospheric 14C content is finally expressed as Δ14C, which is the relative deviation of the measured 14C activity from the NIST oxalic acid standard activity, after correction for isotopic fractionation and radioactive decay related to age. The data are organized by sampling station, and each record of the database contains the sampling dates; values for 14C excess (δ14C) relative to the NIST standard, fractionation 13C (δ13C) relative to the Pee Dee Belemnite (PDB) standard, and corrected 14C (Δ14C) excess; and the standard deviation for Δ14C. The Δ14C calculation results presented here are thus corrected for isotopic fractionation and radioactive decay, and constitute the final product of a research effort that has spanned three decades. The Δ14C station data show a sharp increase in tropospheric radiocarbon levels in the early 1960s and then a decline after the majority of nuclear tests came to an end on August 5, 1963 (Test Ban Treaty). The sharp peaks in tropospheric radiocarbon in the early 1960s are more pronounced in the Northern Hemisphere, reflecting the location of most atomic weapons tests. The measurements show large seasonal variations in the Δ14C level during the early 1960s mainly as a result of springtime transport of bomb Δ14C from the stratosphere. During the 1970s, the seasonal variations are smaller and due partly to seasonal variations in CO2 from fossil-fuel emissions. The rate of decrease of atmospheric radiocarbon provides a check on the exchange constants of the atmosphere and ocean. This report and all data it describes are available from the Carbon Dioxide Information Analysis Center (CDIAC) without charge. The Nydal and Lövseth atmospheric 14C database comprises 21 data files totaling 0.2 megabytes in size. The following report describes the sampling methods and analysis. In addition, the report includes a complete discussion of CDIAC's data-processing efforts, the contents and format of the data files, and a reprint of a Nydal and Lövseth journal article. PART 1: OVERVIEW1. NAME OF THE NUMERIC DATA PACKAGECarbon-14 Measurements in Atmospheric CO2 from Northern and Southern Hemisphere Sites, 1962-1993 2. PRINCIPAL INVESTIGATORSReidar Nydal and Knut LövsethRadiological Dating Laboratory The Norwegian Institute of Technology Trondheim, Norway 3. KEYWORDSRadiocarbon, 14C, atmospheric CO2, quantitative NaOH absorption, carbon isotopes, bomb 14C, Δ14C, δ14C, δ13C, troposphere, stratosphere, aircraft sampling 4. BACKGROUND INFORMATIONAtmospheric carbon dioxide (CO2) contains, besides 12C (~99%), small amounts of the carbon isotopes 13C and 14C. Only 14C is radioactive with a half-life of 5730 years. In the atmosphere, 14C occurs principally as 14CO2 and is usually produced by nuclear reactions between cosmic ray neutrons and the nitrogen atoms of the air (Libby 1952). Solar (heliomagnetic), geomagnetic, and ocean forcing all play a role in atmospheric 14CO2 (Stuiver and Braziunas 1993). Before nuclear bomb testing during the 1950s and early 1960s, radiocarbon levels in the atmosphere had been in decline. Suess (1955) demonstrated that forests grown between 1930 and 1950 had Δ14C values 20-40 per mil below those of pre-1890 woods as a result of anthropogenic 14C-free CO2 emissions since the Industrial Revolution. Nuclear bomb testing has since swamped the "Suess Effect(1)." After a series of atomic weapons tests were conducted at higher northern latitudes, notably Novaya Zemlya in the former Soviet Union, scientists at the Radiological Dating Laboratory in Norway seized the opportunity to conduct CO2 sampling to trace the distribution and flux of bomb 14C with funding support from the Norwegian Research Council. In the early 1960s, several ground sampling sites were established in Norway. These Norwegian study sites gradually expanded to a global network of 14 stations spanning latitudes from Spitsbergen (78°N) to Madagascar (21°S) (Fig. 1; Table 1). Sites possibly contaminated by local CO2 sources were avoided. Additional sites were chosen to improve spatial coverage so that the distribution of radiocarbon could be characterized with respect to latitude. During 1965 the ground-level measurements were supplemented with measurements made on air samples collected from the lower stratosphere (9000-12600 m) using aircraft from the Norwegian Air Force. This data document provides the surface 14C measurements made by the Radiological Dating Laboratory at this global sampling network and the high-altitude measurements made during 1965. The Δ14C data presented here are corrected for isotopic fractionation and radioactive decay, and constitute the final product of a research effort that has spanned three decades. The earliest measurements date back to 1962, and a few sites have data through 1993. Earlier versions of this database have been presented by Nydal (1966, 1968, 1993), Nydal and Lövseth (1983), and Nydal et al. (1971).
5. SAMPLING AND CALCULATIONAll ground-level air samples represented in this database were collected by dynamic quantitative absorption of atmospheric CO2 in carbonate-free 0.5 N sodium hydroxide (NaOH) solution. During the collection process, a dish of NaOH was exposed to the air for 4 to 7 days. Following exposure, the samples were treated with hydrochloric acid to regenerate the carbon dioxide. After a purification procedure, the CO2 was analyzed in a proportional counter to assess 14C content. Typically, a counter has gas volumes of 1-2 L and operates at 2 atm pressure. Until 1981 a counting time of 2 days (48 hours) was often used (Nydal and Lövseth 1983), but a counting time of 4 days was used later in order to obtain higher precision. High-altitude samples were collected in the Trondheim area during 1965 using aircraft from the Norwegian Air Force. Flights originated from Örlandet Airport and covered a region bounded by 62-65°N and 6-10°E, at altitudes of 9000-12600 m. Samples were collected using a filter with a 1.4 kg molecular sieve that absorbs CO2 from the penetrating air. The filter container was placed under the wing of the plane and opened and closed with electrically-operated shutters at both ends. With the plane traveling at a speed of approximately 900 km/hr the filter shutters were opened 15 minutes to allow sufficient amounts of CO2 to be absorbed. After determination of the 14C content in a proportional counter, the δ14C values were calculated as per mil excess above the normal 14C level defined by the National Institute of Standards and Technology (NIST, formerly the US National Bureau of Standards). Atmospheric 14C content is finally expressed as Δ14C, which is the relative deviation of the measured 14C activity from the NIST oxalic acid standard activity, after correction for isotopic mass fractionation and radioactive decay related to age (Stuiver and Polach 1977). Δ14C is expressed in per mil (not as a percentage) and calculated using the following two steps:
In step 1, the 14C excess (Δ14) is only corrected for isotopic mass fractionation. δ14C represents the uncorrected (for decay) 14C relative to the NIST standard and δ13C represents the deviation in the 13C/12C ratio relative to the Pee Dee Belemnite (Pee Dee River, South Carolina) standard. The 13C/12C ratio was measured by mass spectrometry. By themselves, the δ13C values represent data that are highly influenced by fractionation in NaOH in the absorbing dish. In the earlier presentation of the 14C data from the Radiological Dating Laboratory only step 1 was used, and the decay of the NIST 14C reference standard after 1950 was not taken into account (Nydal and Lövseth 1983). Applying the approximate formula in step 2, where λ is 1/8267 years (T/ln2 where T is the 5730 year half-life of 14C) and t is the year of sampling, this small decay (2-5 per mil) has now been applied to all the Δ14C data appearing in this database. For a further discussion of the sampling methods and each sampling site, please see the reprint of Nydal and Lövseth (1983) in Appendix B. For additional information on the high-altitude sampling, see Hagemann et al. (1965), Nydal (1966), and Nydal and Lövseth (1983). For additional information on the sampling sites, radiocarbon standards, and carbon isotope measurements, see Nydal (1966, 1968), Craig (1961), and Levin et al. (1980). 6. APPLICATIONS OF THE DATAThese measurements were originally made to assess potential human health risks from radioactive fallout in the atmosphere. Fortunately it was also recognized that the radioactive isotopes already injected into the atmosphere could be useful tracers in geophysical research. These 14C measurements document the time lag of isotopic sea-air exchange and chronicle a long-term decline in Δ14CO2 at Northern and Southern hemisphere sites. These measurements complement other radiocarbon data sets (Broecker and Olson 1959; Levin et al. 1985, 1995; Manning et al. 1990; Olsson 1993) and support the pronounced twentieth-century Δ14C reduction reported by Stuiver and Quay (1981) due to 14C-free carbon dioxide released by fossil-fuel combustion. This data set is unique for its inclusion of measurements in the early 1960s that trace the bomb 14C released by a series of nuclear tests. All measurements at the global network of sites were taken by dynamic quantitative absorption of CO2 in NaOH solution. This consistency in sampling technique over a period of three decades is valuable to researchers and modelers. The Δ14C tropospheric data show a sharp increase in tropospheric radiocarbon levels in the early 1960s and then a decline after the majority of nuclear tests came to an end on August 5, 1963 through the Test Ban Treaty. The sharp peaks in tropospheric radiocarbon in the early 1960s are more pronounced in the Northern Hemisphere, reflecting the location of most atomic weapons tests. The measurements show large seasonal variations in the Δ14C level in the early 1960s, mainly as a result of springtime transport of bomb 14C from the stratosphere (Fig. 2). During the 1970s, the seasonal variations are smaller and are partly due to seasonal variations in CO2 from fossil-fuel emissions. The rate of decrease of atmospheric radiocarbon provides a check on the exchange constants of the atmosphere and ocean. 7. DATA LIMITATIONS AND RESTRICTIONSPlease note that the δ13C values provided in this database are not representative of atmospheric values. In this database the 13C data serve as guides to the 14C measurements and were used to calculate corrected 14C. It should also be noted that the 13C/C12 ratio was not measured for every sample. In these instances where the 13C/C12 ratio was not measured, a mean value is given for δ13C and identified by a flag code. These mean values were calculated from 20-40 ground-level measurements or 4 high-altitude measurements. 8. REFERENCES
9. DATA-PROCESSING ACTIVITIES AND QUALITY ASSURANCE CHECKS PERFORMED BY CDIACCDIAC is committed to the quality assurance (QA) of data before distribution. In order to provide scientists and researchers with high-quality data, CDIAC reviews the data it receives for consistent formatting, completeness, reasonableness, and accuracy. Each review involvesprogramming that is specific to the needs of each data set. These efforts are indicative of CDIAC's mission to provide the international scientific community with high-quality, well-documented data. DATA-PROCESSING CDIAC obtained the Nydal and Lövseth database as an electronic-mail message from Reidar Nydal. CDIAC staff edited the message and created the ASCII data files for each site. Working copies of the files were created and processed in the following ways: 1. The original ASCII files were reformatted into a consistent format and combined in a single file with data from all sites. 2. Both SAS® and FORTRAN 77 codes were written and are available to the user for reading any of the ASCII data files. QA CHECKS 1. Each file was checked to ensure formatting consistency and to confirm the absence of missing data entries. 2. Checks were performed to confirm the uniqueness of each laboratory reference code and to ensure that sampling intervals were formatted consistently. 3. Mean, minimum, and maximum values for δ14C, δ13C, and corrected Δ14C data at each site were calculated and assessed for reasonableness. 4. All δ14C, δ13C, and corrected Δ14C measurements were plotted and assessed for reasonableness. 5. Any inconsistencies or suspect measurements were reported to and addressed by the investigators before the data set was released. SAS® is the registered trademark of SAS Institute, Inc., Cary, North Carolina, 27511, USA. 10. HOW TO OBTAIN THE DATA AND DOCUMENTATIONThe Nydal and Lövseth database is available in machine-readable form from CDIAC without charge. The database may also be downloaded from CDIAC's anonymous File Transfer Protocol (FTP) site, by using the address, login instructions, and FTP commands listed below. In addition, the database is available on 9-track magnetic tape, 8-mm tape, or IBM- or Macintosh-formatted floppy diskettes. For tape requests, please include preferred tape specifications (i.e., 1600 or 6250 BPI for 9-track tapes and 8200 or 8500 format for 8-mm tapes, labeled or nonlabeled, ASCII or EBCDIC characters, variable or fixed-record lengths). Requests without tape specifications will be filled on 9-track, 6250 BPI, nonlabeled tapes with file attributes shown in Sect. 11. This documentation is available only from CDIAC. Electronic versions of the documentation are available via the World Wide Web from CDIAC's home page (http://cdiac.esd.ornl.gov). Requests for printed copies of the documentation should be addressed to World Data Center-A for Atmospheric Trace Gases Oak Ridge National Laboratory Post Office Box 2008 Oak Ridge, TN 37831-6290, USA The tapes, diskettes, and documentation may also be ordered by telephone, facsimile, or electronic mail: Telephone: (865) 574-3645 or (865) 574-0390 FTP access: ftp cdiac.esd.ornl.gov (or 128.219.24.36) Enter anonymous at the userid prompt NOTE: When using these radiocarbon data in a presentation or publication, PLEASE acknowledge the principal investigators, Reidar Nydal and Knut Lövseth, and the Norwegian Institute of Technology! PART 2: CONTENT AND FORMAT OF DATA FILES11. LISTING OF FILES PROVIDEDThe following is a list of the files that compose the Nydal and Lövseth atmospheric carbon isotope database and that are distributed by CDIAC along with this documentation. These files are available on a variety of media (see Sect. 10, "How To Obtain the Data and Documentation"). This listing has been tailored to reflect a 9-track magnetic tape request. The record formats, block sizes, and record lengths shown are the defaults for those not specifying these parameters when requesting machine-readable data files on 9-track magnetic tape. The default tape density, labeling, and characters are 6250 BPI, nonlabeled, and ASCII, respectively.
aFixed-block record format. ®SAS is the registered trademark of SAS Institute, Inc., Cary, North Carolina, 27511, USA. 12. FILE DESCRIPTIONSThis section describes the content and format of each of the 21 files that compose this numeric data package (NDP) and the Nydal and Lövseth atmospheric carbon isotope database. DATA FILES This NDP consists of the following 21 files:
DATA FILE FORMATS (*.ASC) This NDP contains 15 data files that provide 1619 estimates of δ14C, δ13C, and Δ14C in atmospheric CO2 from 14 locations. The period of record differs by station. The earliest measurements were made in 1962, and the latest estimates are from 1993. Most stations have records only for the 1960s. All of the data files have the same format and none contain missing values. Some δ13C values are flagged as mean values; users are urged to pay attention to these flags before analyzing or interpreting the corresponding values. Each file is sorted by sample collection date and may be read with the following FORTRAN 77 code:
The following SAS® input statement may also be used to read these files:
Stated in tabular form, the contents include the following:
where
DATA FILE FORMAT (STRAT.DAT) This NDP contains one data file that provides eleven estimates of δ14C, δ13C, and Δ14C in atmospheric CO2 from the low stratosphere during 1965. High-altitude samples were collected in the Trondheim area using aircraft from the Norwegian Air Force. Flights originated from Örlandet Airport and covered the region bounded by 62-65°N and 6-10°E, at altitudes of 9000-12600 m. Samples were collected using a filter with a 1.4 kg molecular sieve that absorbs CO2 from the penetrating air. The filter container was placed under the wing of the plane and opened and closed with electrically-operated shutters at both ends. With the plane traveling at a speed of approximately 900 km/hr the filter shutters were opened 15 minutes to allow sufficient amounts of CO2 to be absorbed. The file may be read with the following FORTRAN 77 code:
The following SAS® input statement may also be used to read this file:
Stated in tabular form, the contents include the following:
where
13. LISTING OF THE FORTRAN 77 DATA RETRIEVAL PROGRAMSThe following is a listing of the FORTRAN 77 data retrieval code (ndp057.for) written by the preparers to read and print any of the files containing the station 14C data.
The following is a listing of the FORTRAN 77 data retrieval code (strat.for) written by the preparers to read and print the file containing the stratospheric 14C data.
14. LISTING OF THE SAS® DATA RETRIEVAL PROGRAMSThe following is a listing of the SAS® data retrieval code (ndp057.sas) written by the preparers to read and print any of the files containing the station 14C data.
The following is a listing of the SAS® data retrieval code (strat.sas) written by the preparers to read and print the file containing the stratospheric 14C data.
15. PARTIAL LISTING OF DATA FILESThe following presents a partial listing of one (nydal.asc) of the 15 data files that contain the station 14C data. This file is identical in format to all data files containing the station 14C data. The first 25 lines of the file nydal.asc are as follows:
The last 25 lines of the file nydal.asc are as follows:
The following is a complete listing of the data file (strat.dat) containing the stratospheric 14C data.
16. VERIFICATION OF DATA TRANSPORTThe data files contained in this NDP may be read with the FORTRAN 77 or SAS® data retrieval programs provided. To verify that the data have been correctly transported to their systems, users should generate some or all of the statistics presented in Tables 2 and 3. These tables present simple summary statistics for the file that contains data from all 14 sites (i.e., file nydal.asc) and the file that contains the stratospheric 14C measurements (i.e., file strat.dat). If the statistics generated by the user differ from those presented here, the data files may have been corrupted in transport. These statistics are presented only as a tool to ensure proper reading of the data files. They are not to be construed as summaries of the data sets.
APPENDIX AFIGURES SHOWING TROPOSPHERIC AND Fig. A-1. Corrected 14C measurements from air samples collected at Kapp Linné, Fruholmen, Gråkallen, and Vassfjellet Fig. A-2. Corrected 14C measurements from air samples collected at Lindesnes, Norway;
APPENDIX BREPRINTS OF PERTINENT LITERATURE Tracing Bomb 14C in the Atmosphere 1962-1980, by R. Nydal and K. Lövseth, 1983. Journal of Geophysical Research 88:3621-42.The copyright permission kindly extended to the Carbon Dioxide Information Analysis Center by the American Geophysical Union did not include reprinting in the electronic form, only printed matter. |
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