Characterization of gas-phase thorium nitride

Le, Anh T.; Nakhate, Sanjay G.; Nguyen, Duc-Trung; Steimle, Timothy C.; Heaven, Michael C.

doi:10.1063/1.5089136

Characterization of gas-phase thorium nitride

Journal Article · Tue Apr 09 00:00:00 EDT 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5089136· OSTI ID:1609350

Le, Anh T. ^[1]; ^[2]; Nguyen, Duc-Trung ^[2]; ^[2]; ^[3]

Arizona State Univ., Tempe, AZ (United States); DOE/OSTI
Arizona State Univ., Tempe, AZ (United States)
Emory Univ., Atlanta, GA (United States)

In this work, properties of gas-phase thorium nitride, ThN, have been experimentally determined from a combined optical and microwave spectroscopic study. An intense band near 555 nm has been assigned as the [18.0]1.5–X²Σ⁺ (0,0) transition and recorded at high resolution in the presence of static electric and magnetic fields. The observed optical Stark shifts were analyzed to determine permanent electric dipole moments, $$\vec{μ}_{el}$$ for the [18.0]1.5 and X²Σ⁺ states of 4.38 ± 0.02D and 5.11 ± 0.09D, respectively. Zeeman shifts were used to determine the magnetic g-factors. The pure rotational spectrum was recorded using a separated field optical pump/probe microwave repopulation scheme and analyzed to determine the bond length and ¹⁴N magnetic hyperfine and nuclear electric quadrupole parameters. A molecular orbital correlation diagram and ligand field electronic structure models are used to provide a qualitative interpretation of the electronic state ordering, magneto- and electro-static properties, and hyperfine interactions. Electronic structure calculations for the X²Σ⁺ state were performed, and results were compared with observations. Observed trends in $$\vec{μ}_{el}$$ for the ThX (X = N, S, O, F, and Cl) series are discussed.

View Accepted Manuscript (DOE)

Research Organization:: Arizona State Univ., Tempe, AZ (United States); Emory Univ., Atlanta, GA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: FG02-01ER15153; SC0018241

OSTI ID:: 1609350

Alternate ID(s):: OSTI ID: 1505883

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 14 Vol. 150; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (32)

F-Block N-Heterocyclic Carbene Complexes Arnold, Polly L.; Liddle, Stephen T. ChemInform, Vol. 38, Issue 2 https://doi.org/10.1002/chin.200702227	journal	January 2007
The Pure Rotational Spectrum of the Actinide-Containing Compound Thorium Monoxide. Dewberry, Christopher T.; Etchison, Kerry C.; Cooke, Stephen A. ChemInform, Vol. 38, Issue 45 https://doi.org/10.1002/chin.200745002	journal	November 2007
Relativistic Hamiltonians for Chemistry: A Primer Saue, Trond ChemPhysChem, Vol. 12, Issue 17 https://doi.org/10.1002/cphc.201100682	journal	November 2011
The ORCA program system: The ORCA program system Neese, Frank Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 1 https://doi.org/10.1002/wcms.81	journal	June 2011
Molpro: a general-purpose quantum chemistry program package: Molpro Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2 https://doi.org/10.1002/wcms.82	journal	July 2011
Progress in molecular uranium-nitride chemistry King, David M.; Liddle, Stephen T. Coordination Chemistry Reviews, Vol. 266-267 https://doi.org/10.1016/j.ccr.2013.06.013	journal	May 2014
The pure rotational spectrum of thorium monosulfide, ThS Steimle, Timothy C.; Zhang, Ruohan; Heaven, Michael C. Chemical Physics Letters, Vol. 639 https://doi.org/10.1016/j.cplett.2015.09.048	journal	October 2015
Comparison of the T1 and D1 diagnostics for electronic structure theory: a new definition for the open-shell D1 diagnostic Lee, Timothy J. Chemical Physics Letters, Vol. 372, Issue 3-4 https://doi.org/10.1016/s0009-2614(03)00435-4	journal	April 2003
Rotational Spectroscopy of Diatomic Molecules Brown, John M.; Carrington, Alan https://doi.org/10.1017/CBO9780511814808	book	January 2003
Optical Stark and Zeeman Spectroscopy of Thorium Fluoride (ThF) and Thorium Chloride (ThCl) Nguyen, Duc-Trung; Steimle, Timothy; Linton, Colan The Journal of Physical Chemistry A, Vol. 123, Issue 7 https://doi.org/10.1021/acs.jpca.8b11853	journal	November 2018
Mixed Imidazolin-2-iminato–Cp* Thorium(IV) Complexes: Synthesis and Reactivity Toward Oxygen-Containing Substrates Karmel, Isabell S. R.; Fridman, Natalia; Tamm, Matthias Organometallics, Vol. 34, Issue 12 https://doi.org/10.1021/acs.organomet.5b00273	journal	June 2015
Relativistic effects in structural chemistry Pyykko, Pekka Chemical Reviews, Vol. 88, Issue 3 https://doi.org/10.1021/cr00085a006	journal	May 1988
Recent Developments in Synthesis and Structural Chemistry of Nonaqueous Actinide Complexes Jones, Matthew B.; Gaunt, Andrew J. Chemical Reviews, Vol. 113, Issue 2 https://doi.org/10.1021/cr300198m	journal	October 2012
Complexation and Extraction of Trivalent Actinides and Lanthanides by Triazinylpyridine N -Donor Ligands Panak, Petra J.; Geist, Andreas Chemical Reviews, Vol. 113, Issue 2 https://doi.org/10.1021/cr3003399	journal	October 2012
F-Block N-Heterocyclic Carbene Complexes Arnold, Polly L.; Casely, Ian J. Chemical Reviews, Vol. 109, Issue 8 https://doi.org/10.1021/cr8005203	journal	August 2009
Coordination Chemistry with f-Element Complexes for an Improved Understanding of Factors That Contribute to Extraction Selectivity Gorden, Anne E. V.; DeVore, Michael A.; Maynard, Branson A. Inorganic Chemistry, Vol. 52, Issue 7 https://doi.org/10.1021/ic300887p	journal	June 2012
Two-Dimensional Fluorescence (Excitation/Emission) Spectroscopy as a Probe of Complex Chemical Environments Reilly, Neil J.; Schmidt, Timothy W.; Kable, Scott H. The Journal of Physical Chemistry A, Vol. 110, Issue 45 https://doi.org/10.1021/jp064411z	journal	November 2006
Spectroscopy and Structure of the Simplest Actinide Bonds Heaven, Michael C.; Barker, Beau J.; Antonov, Ivan O. The Journal of Physical Chemistry A, Vol. 118, Issue 46 https://doi.org/10.1021/jp507283n	journal	October 2014
F-block N-heterocyclic carbene complexes Arnold, Polly L.; Liddle, Stephen T. Chemical Communications, Issue 38 https://doi.org/10.1039/b606829d	journal	January 2006
The pure rotational spectrum of the actinide-containing compound thorium monoxide Dewberry, Christopher T.; Etchison, Kerry C.; Cooke, Stephen A. Physical Chemistry Chemical Physics, Vol. 9, Issue 35 https://doi.org/10.1039/b709343h	journal	January 2007
Metal–metal bonds in f-element chemistry Liddle, Stephen T.; Mills, David P. Dalton Transactions, Issue 29 https://doi.org/10.1039/b904318g	journal	January 2009
Recent developments in actinide–ligand multiple bonding Hayton, Trevor W. Chemical Communications, Vol. 49, Issue 29 https://doi.org/10.1039/c3cc39053e	journal	January 2013
The interpretation of molecular magnetic hyperfine interactions Fitzpatrick, James A. J.; Manby, Frederick R.; Western, Colin M. The Journal of Chemical Physics, Vol. 122, Issue 8 https://doi.org/10.1063/1.1851501	journal	February 2005
Two dimensional laser induced fluorescence spectroscopy: A powerful technique for elucidating rovibronic structure in electronic transitions of polyatomic molecules Gascooke, Jason R.; Alexander, Ula N.; Lawrance, Warren D. The Journal of Chemical Physics, Vol. 134, Issue 18 https://doi.org/10.1063/1.3578174	journal	May 2011
Spectroscopic investigations of ThF and ThF ⁺ Barker, Beau J.; Antonov, Ivan O.; Heaven, Michael C. The Journal of Chemical Physics, Vol. 136, Issue 10 https://doi.org/10.1063/1.3691301	journal	March 2012
The route to high accuracy in ab initio calculations of Cu quadrupole-coupling constants Cheng, Lan; Stopkowicz, Stella; Stanton, John F. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4767767	journal	December 2012
Resonant two-photon ionization spectroscopy of jet-cooled UN: Determination of the ground state Matthew, Daniel J.; Morse, Michael D. The Journal of Chemical Physics, Vol. 138, Issue 18 https://doi.org/10.1063/1.4803472	journal	May 2013
The permanent electric dipole moment of thorium sulfide, ThS Le, Anh; Heaven, Michael C.; Steimle, Timothy C. The Journal of Chemical Physics, Vol. 140, Issue 2 https://doi.org/10.1063/1.4861045	journal	January 2014
The hyperfine structure of ¹²⁹ I ₂ and ₁₂₇ I ₁₂₉ in the B band system Salumbides, E. J.; Eikema, K. S. E.; Ubachs, W. Molecular Physics, Vol. 104, Issue 16-17 https://doi.org/10.1080/00268970600747696	journal	August 2006
Branching ratios and radiative lifetimes of the U , L , and I states of thorium oxide Kokkin, Damian L.; Steimle, Timothy C.; DeMille, David Physical Review A, Vol. 90, Issue 6 https://doi.org/10.1103/physreva.90.062503	journal	December 2014
Characterization of the I ( \| Ω \| = 1 ) – X 1 Σ + ( 0 , 0 ) band of thorium oxide Kokkin, Damian L.; Steimle, Timothy C.; DeMille, David Physical Review A, Vol. 91, Issue 4 https://doi.org/10.1103/physreva.91.042508	journal	April 2015
f-Element-metal bond chemistry Patel, Dipti; Liddle, Stephen T. Reviews in Inorganic Chemistry, Vol. 32, Issue 1 https://doi.org/10.1515/revic.2012.0001	journal	January 2012

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