Nitrogen isotopic fractionations in the low temperature (80 K) vacuum ultraviolet photodissociation of N 2
Abstract
N2 is a diatomic molecule with complex electronic structure. Interstate crossings are prominent in the high energy domain, introducing significant perturbations to the system. Nitrogen mainly photodissociates in the vacuum ultraviolet (VUV) region of the electromagnetic spectrum through both direct and indirect predissociation. Due to the complexity introduced by these perturbations, the nitrogen isotopic fractionation in N2 photodissociation is extremely hard to calculate, and an experimental approach is required. We present new data of N-isotopic fractionation in N2 photodissociation at low temperature (80 K), which shows a distinctly different15N enrichment profile compared to that at relatively higher temperatures (200 and 300 K). The new data, important to understanding the N-isotopic compositions measured in meteorites and other planetary bodies, are discussed in light of the knowledge of N2 photochemistry and calculated photoabsorption cross sections in the VUV.
- Authors:
-
- Department of Chemistry and Biochemistry, University of California, San Diego, 9500 Gilman Drive, La Jolla, California 92093-0356, USA
- Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, USA
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Aeronautics and Space Administration (NASA)
- OSTI Identifier:
- 1324841
- Alternate Identifier(s):
- OSTI ID: 1420486; OSTI ID: 1459373
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Name: Journal of Chemical Physics Journal Volume: 145 Journal Issue: 11; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 79 ASTRONOMY AND ASTROPHYSICS; photochemistry; vacuum chambers; temperature measurement; photons; photodissociation; predissociation; dissociation; meteorites; ultraviolet light; wave functions
Citation Formats
Chakraborty, Subrata, Jackson, Teresa L., Rude, Bruce, Ahmed, Musahid, and Thiemens, M. H. Nitrogen isotopic fractionations in the low temperature (80 K) vacuum ultraviolet photodissociation of N 2. United States: N. p., 2016.
Web. doi:10.1063/1.4962447.
Chakraborty, Subrata, Jackson, Teresa L., Rude, Bruce, Ahmed, Musahid, & Thiemens, M. H. Nitrogen isotopic fractionations in the low temperature (80 K) vacuum ultraviolet photodissociation of N 2. United States. https://doi.org/10.1063/1.4962447
Chakraborty, Subrata, Jackson, Teresa L., Rude, Bruce, Ahmed, Musahid, and Thiemens, M. H. Thu .
"Nitrogen isotopic fractionations in the low temperature (80 K) vacuum ultraviolet photodissociation of N 2". United States. https://doi.org/10.1063/1.4962447.
@article{osti_1324841,
title = {Nitrogen isotopic fractionations in the low temperature (80 K) vacuum ultraviolet photodissociation of N 2},
author = {Chakraborty, Subrata and Jackson, Teresa L. and Rude, Bruce and Ahmed, Musahid and Thiemens, M. H.},
abstractNote = {N2 is a diatomic molecule with complex electronic structure. Interstate crossings are prominent in the high energy domain, introducing significant perturbations to the system. Nitrogen mainly photodissociates in the vacuum ultraviolet (VUV) region of the electromagnetic spectrum through both direct and indirect predissociation. Due to the complexity introduced by these perturbations, the nitrogen isotopic fractionation in N2 photodissociation is extremely hard to calculate, and an experimental approach is required. We present new data of N-isotopic fractionation in N2 photodissociation at low temperature (80 K), which shows a distinctly different15N enrichment profile compared to that at relatively higher temperatures (200 and 300 K). The new data, important to understanding the N-isotopic compositions measured in meteorites and other planetary bodies, are discussed in light of the knowledge of N2 photochemistry and calculated photoabsorption cross sections in the VUV.},
doi = {10.1063/1.4962447},
journal = {Journal of Chemical Physics},
number = 11,
volume = 145,
place = {United States},
year = {Thu Sep 15 00:00:00 EDT 2016},
month = {Thu Sep 15 00:00:00 EDT 2016}
}
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https://doi.org/10.1063/1.4962447
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Works referenced in this record:
Pristine extraterrestrial material with unprecedented nitrogen isotopic variation
journal, June 2009
- Briani, G.; Gounelle, M.; Marrocchi, Y.
- Proceedings of the National Academy of Sciences, Vol. 106, Issue 26
Massive isotopic effect in vacuum UV photodissociation of N2 and implications for meteorite data
journal, September 2014
- Chakraborty, S.; Muskatel, B. H.; Jackson, T. L.
- Proceedings of the National Academy of Sciences, Vol. 111, Issue 41
Self-shielding in the solar nebula
journal, February 2002
- Clayton, Robert N.
- Nature, Vol. 415, Issue 6874
Source of Nitrogen Isotope Anomaly in HCN in the Atmosphere of Titan
journal, July 2007
- Liang, Mao-Chang; Heays, Alan N.; Lewis, Brenton R.
- The Astrophysical Journal, Vol. 664, Issue 2
Interstellar Chemistry Recorded in Organic Matter from Primitive Meteorites
journal, May 2006
- Busemann, H.
- Science, Vol. 312, Issue 5774
Oscillator strengths and line widths of dipole-allowed transitions in N214 between 89.7 and 93.5nm
journal, March 2008
- Stark, G.; Lewis, B. R.; Heays, A. N.
- The Journal of Chemical Physics, Vol. 128, Issue 11
Production of N+∗ from N2 + hv: Effective EUV emission yields from laboratory and dayglow data
journal, August 1991
- Meier, R. R.; Samson, James A. R.; Chung, Y.
- Planetary and Space Science, Vol. 39, Issue 8
Extreme ultraviolet laser excitation of isotopic molecular nitrogen: The dipole-allowed spectrum of 15N2 and 14N15N
journal, August 2003
- Sprengers, J. P.; Ubachs, W.; Baldwin, K. G. H.
- The Journal of Chemical Physics, Vol. 119, Issue 6
Oscillator strength and linewidth measurements of dipole-allowed transitions in N214 between 93.5 and 99.5nm
journal, December 2005
- Stark, G.; Huber, K. P.; Yoshino, K.
- The Journal of Chemical Physics, Vol. 123, Issue 21
A 15N-Poor Isotopic Composition for the Solar System As Shown by Genesis Solar Wind Samples
journal, June 2011
- Marty, B.; Chaussidon, M.; Wiens, R. C.
- Science, Vol. 332, Issue 6037
Isotope-selective photodissociation of ozone molecules induced by infrared laser irradiation
journal, April 2008
- Kuze, Hiroaki; Sato, Tetsuya; Kambe, Takashi
- Chemical Physics Letters, Vol. 455, Issue 4-6
Nitrogen abundances and isotopic compositions in stony meteorites
journal, February 1978
- Kung, Chun-Chan; Clayton, Robert N.
- Earth and Planetary Science Letters, Vol. 38, Issue 2
Ultrafast Predissociation Mechanism of the 1 Π u States of 14 N 2 and Its Isotopomers upon Attosecond Excitation from the Ground State
journal, August 2012
- Muskatel, B. H.; Remacle, F.; Levine, R. D.
- The Journal of Physical Chemistry A, Vol. 116, Issue 46
Structure and predissociation of the 3pσuD Σ3u+ Rydberg state of N2: First extreme-ultraviolet and new near-infrared observations, with coupled-channels analysis
journal, November 2008
- Lewis, B. R.; Baldwin, K. G. H.; Heays, A. N.
- The Journal of Chemical Physics, Vol. 129, Issue 20
Mass-Independent Oxygen Isotopic Partitioning During Gas-Phase SiO2 Formation
journal, October 2013
- Chakraborty, S.; Yanchulova, P.; Thiemens, M. H.
- Science, Vol. 342, Issue 6157
Compositional differences in enstatite chondrites based on carbon and nitrogen stable isotope measurements
journal, December 1986
- Grady, Monica M.; Wright, I. P.; Carr, L. P.
- Geochimica et Cosmochimica Acta, Vol. 50, Issue 12
Photodissociation of interstellar N 2
journal, June 2013
- Li, X.; Heays, A. N.; Visser, R.
- Astronomy & Astrophysics, Vol. 555
Isotopic Compositions of Cometary Matter Returned by Stardust
journal, December 2006
- McKeegan, K. D.; Aleon, J.; Bradley, J.
- Science, Vol. 314, Issue 5806
The Physical Chemistry of Mass-Independent Isotope Effects and Their Observation in Nature
journal, May 2012
- Thiemens, Mark H.; Chakraborty, Subrata; Dominguez, Gerardo
- Annual Review of Physical Chemistry, Vol. 63, Issue 1
Experimental verification of strong rotational dependence of fluorescence and predissociation yield in the b 1 Π u ( v = 1) level of 14 N 2
journal, January 2012
- Wu, C. Y. Robert; Judge, D. L.; Tsai, M. -H.
- The Journal of Chemical Physics, Vol. 136, Issue 4
Predissociative decay of the c′41Σu+, v = 0 state of N2
journal, April 1997
- Ubachs, W.
- Chemical Physics Letters, Vol. 268, Issue 1-2
Isotope selective photodissociation of N 2 by the interstellar radiation field and cosmic rays
journal, February 2014
- Heays, Alan N.; Visser, Ruud; Gredel, Roland
- Astronomy & Astrophysics, Vol. 562
High-resolution Fourier-transform extreme ultraviolet photoabsorption spectroscopy of 14 N 15 N
journal, December 2011
- Heays, A. N.; Dickenson, G. D.; Salumbides, E. J.
- The Journal of Chemical Physics, Vol. 135, Issue 24
On the strong and selective isotope effect in the UV excitation of N2 with implications toward the nebula and Martian atmosphere
journal, March 2011
- Muskatel, B. H.; Remacle, F.; Thiemens, M. H.
- Proceedings of the National Academy of Sciences, Vol. 108, Issue 15
The Mass-Independent Fractionation of Oxygen: A Novel Isotope Effect and Its Possible Cosmochemical Implications
journal, March 1983
- Thiemens, M. H.; Heidenreich, J. E.
- Science, Vol. 219, Issue 4588
Isotopic variation of experimental lifetimes for the lowest Πu1 states of N2
journal, April 2005
- Sprengers, J. P.; Ubachs, W.; Baldwin, K. G. H.
- The Journal of Chemical Physics, Vol. 122, Issue 14
Nonadiabatic representations of the 1 Σ + u and 1 Π u states of the N 2 molecule
journal, September 1983
- Stahel, D.; Leoni, M.; Dressler, K.
- The Journal of Chemical Physics, Vol. 79, Issue 6
Predissociation mechanism for the lowest Πu1 states of N2
journal, April 2005
- Lewis, B. R.; Gibson, S. T.; Zhang, W.
- The Journal of Chemical Physics, Vol. 122, Issue 14
Comparison between predissociation mechanisms in two isoelectronic molecules: CO and N 2
journal, June 2007
- Lefebvre-Brion, H.; Lewis, B. R.
- Molecular Physics, Vol. 105, Issue 11-12
Dipole-allowed excited states of N2: Potential energy curves, vibrational analysis, and absorption intensities
journal, October 2001
- Spelsberg, Dirk; Meyer, Wilfried
- The Journal of Chemical Physics, Vol. 115, Issue 14
Lifetime and predissociation yield of 14N2 b 1Πu(v=1)
journal, May 2004
- Sprengers, J. P.; Ubachs, W.; Johansson, A.
- The Journal of Chemical Physics, Vol. 120, Issue 19
Optical observation of the 3sσgFΠu3 Rydberg state of N2
journal, October 2005
- Sprengers, J. P.; Reinhold, E.; Ubachs, W.
- The Journal of Chemical Physics, Vol. 123, Issue 14
Nitrogen isotope variations in the Solar System
journal, June 2015
- Füri, Evelyn; Marty, Bernard
- Nature Geoscience, Vol. 8, Issue 7
Lifetime and predissociation yield of N214bΠu1(v=1) revisited: Effects of rotation
journal, December 2005
- Lewis, B. R.; Gibson, S. T.; Sprengers, J. P.
- The Journal of Chemical Physics, Vol. 123, Issue 23
Carbon, hydrogen and nitrogen in carbonaceous chondrites: Abundances and isotopic compositions in bulk samples
journal, August 1985
- Kerridge, John F.
- Geochimica et Cosmochimica Acta, Vol. 49, Issue 8
A coupled-channel model of the Π3u states of N2: Structure and interactions of the 3sσgF3 Π3u and 3pπuG3 Π3u Rydberg states
journal, October 2008
- Lewis, B. R.; Heays, A. N.; Gibson, S. T.
- The Journal of Chemical Physics, Vol. 129, Issue 16
Performance of the vacuum ultraviolet high-resolution and high-flux beamline for chemical dynamics studies at the Advanced Light Source
journal, May 1997
- Heimann, P. A.; Koike, M.; Hsu, C. W.
- Review of Scientific Instruments, Vol. 68, Issue 5
Interactions of the 3pπucΠu1(v=2) Rydberg-complex member in isotopic N2
journal, April 2008
- Vieitez, M. O.; Ivanov, T. I.; de Lange, C. A.
- The Journal of Chemical Physics, Vol. 128, Issue 13
Kinetic nitrogen isotope fractionation associated with thermal decomposition of NH3: Experimental results and potential applications to trace the origin of N2 in natural gas and hydrothermal systems
journal, October 2009
- Li, Long; Cartigny, Pierre; Ader, Magali
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 20
Works referencing / citing this record:
Use of Isotope Effects To Understand the Present and Past of the Atmosphere and Climate and Track the Origin of Life
journal, February 2019
- Thiemens, Mark H.; Lin, Mang
- Angewandte Chemie, Vol. 131, Issue 21
Use of Isotope Effects To Understand the Present and Past of the Atmosphere and Climate and Track the Origin of Life
journal, May 2019
- Thiemens, Mark H.; Lin, Mang
- Angewandte Chemie International Edition, Vol. 58, Issue 21
Time resolved mechanism of the isotope selectivity in the ultrafast light induced dissociation in N 2
journal, September 2019
- Komarova, Ksenia G.; Remacle, Francoise; Levine, R. D.
- The Journal of Chemical Physics, Vol. 151, Issue 11
Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N 2
journal, May 2018
- Ajay, Jayanth S.; Komarova, Ksenia G.; Remacle, Francoise
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 23
The discovery of chemically produced mass independent isotope effects: The physical chemistry basis and applications to the early solar system, planetary atmospheres, and the origin of life: Acceptance Speech of the Leonard Medal July 2017
journal, October 2018
- Thiemens, Mark H.
- Meteoritics & Planetary Science, Vol. 54, Issue 1