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Intracavity optogalvanic spectroscopy for radiocarbon analysis with attomole sensitivity
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Text
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Title
Intracavity optogalvanic spectroscopy for radiocarbon analysis with attomole sensitivity
Identifier
ETD_2148
Identifier
(type = hdl)
http://hdl.rutgers.edu/1782.2/rucore10002600001.ETD.000051643
Identifier
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doi:10.7282/T3736R4G
Language
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eng
Genre
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theses
Genre
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ETD doctoral
Subject
(authority = RUETD)
Topic
Applied Physics
Subject
(authority = ETD-LCSH)
Topic
Radiocarbon dating
Subject
(authority = ETD-LCSH)
Topic
Optogalvanic spectroscopy
Abstract
Carbon-14 (radiocarbon) is a naturally occurring radioactive isotope of carbon, having an extremely low natural abundance in living organisms (14C/C ~ 10-12) and a long half life of ~ 5730 years. These properties make it an ideal organic tracer for various applications
in biological, pharmaceutical and environmental sciences as well as carbon dating. Today, the state of the art radiocarbon quantitation technique is Accelerator Mass Spectrometry (AMS) which is based on ion counting using a several megavolt tandem electrostatic accelerator as a mass spectrometer. Although AMS sets the standard for high sensitivity detection, its size, cost and complexity as an analysis system, limits its wide and routine use especially in laboratory or field applications. In this thesis, a new ultrasensitive
laser based analytical technique that can quantify attomoles of 14C in submicrogram samples is demonstrated. The new system exhibits similar or better
measurement capabilities as AMS, in sensitivity (14C/C ≤ 10-15), precision (≤3%) and accuracy (≤5%). Additional advantages include non destructive analysis capability, small size, being a table top instrument, high sample throughput capability via flow processing
and the potential to be coupled to GC/LC instrumentation.
The developed Intracavity Optogalvanic Spectroscopy (ICOGS) system is based on measuring changes in electrical properties of a weakly ionized glow discharge placed inside the cavity of a periodically modulated high power (50 W) 14CO2 laser. This new configuration enabled improvement of the signal detection sensitivity by about six orders of magnitude compared to the conventional external cell optogalvanic spectroscopy
method. The signal enhancement mechanism is similar to, but with key differences from the well studied optical detection method Intracavity Absorption Spectroscopy (ICAS). Measurement capability of this new system is demonstrated with calibration curves
relative to AMS measurements with a dynamic range of more than five orders of magnitude. The systems studied exhibited saturation effects with laser power and
measurement time and also non-linearities in response with samples having enrichments greater than 12 Modern. (1 Modern = 1.10-12 14C/12C ratio.) However, standard operating procedures were developed for accurately measuring unknown samples. For a more thorough quantitative understanding of the enhancement mechanism, a physical rate equations model has been outlined.
in biological, pharmaceutical and environmental sciences as well as carbon dating. Today, the state of the art radiocarbon quantitation technique is Accelerator Mass Spectrometry (AMS) which is based on ion counting using a several megavolt tandem electrostatic accelerator as a mass spectrometer. Although AMS sets the standard for high sensitivity detection, its size, cost and complexity as an analysis system, limits its wide and routine use especially in laboratory or field applications. In this thesis, a new ultrasensitive
laser based analytical technique that can quantify attomoles of 14C in submicrogram samples is demonstrated. The new system exhibits similar or better
measurement capabilities as AMS, in sensitivity (14C/C ≤ 10-15), precision (≤3%) and accuracy (≤5%). Additional advantages include non destructive analysis capability, small size, being a table top instrument, high sample throughput capability via flow processing
and the potential to be coupled to GC/LC instrumentation.
The developed Intracavity Optogalvanic Spectroscopy (ICOGS) system is based on measuring changes in electrical properties of a weakly ionized glow discharge placed inside the cavity of a periodically modulated high power (50 W) 14CO2 laser. This new configuration enabled improvement of the signal detection sensitivity by about six orders of magnitude compared to the conventional external cell optogalvanic spectroscopy
method. The signal enhancement mechanism is similar to, but with key differences from the well studied optical detection method Intracavity Absorption Spectroscopy (ICAS). Measurement capability of this new system is demonstrated with calibration curves
relative to AMS measurements with a dynamic range of more than five orders of magnitude. The systems studied exhibited saturation effects with laser power and
measurement time and also non-linearities in response with samples having enrichments greater than 12 Modern. (1 Modern = 1.10-12 14C/12C ratio.) However, standard operating procedures were developed for accurately measuring unknown samples. For a more thorough quantitative understanding of the enhancement mechanism, a physical rate equations model has been outlined.
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electronic resource
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x, 95 p. : ill.
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Ph.D.
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Includes bibliographical references (p. 88-93)
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by Erhan Ilkmen
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Ilkmen
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Erhan
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1977
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Erhan Ilkmen
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Murnick
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Daniel
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chair
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Daniel Murnick
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Wu
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Zhen
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internal member
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Zhen Wu
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Schaden
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Martin
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Martin Schaden
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Hall
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Gene
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Gene Hall
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Barat
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Robert
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Robert Barat
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Rutgers University
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Graduate School - Newark
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2009
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2009-10
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xx
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Rutgers University Electronic Theses and Dissertations
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ETD
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Graduate School - Newark Electronic Theses and Dissertations
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rucore10002600001
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NjNbRU
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The author owns the copyright to this work.
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Copyright protected
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Open
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Permission or license
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Ilkmen
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Erhan
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Erhan Ilkmen
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Rutgers University. Graduate School - Newark
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I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
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