Photoelectron Spectroscopy and Theoretical Studies of PCSe − , AsCS − , AsCSe − , and NCSe − : Insights into the Electronic Structures of the Whole Family of ECX − Anions (E=N, P, As; X=O, S, Se)

Yuan, Qinqin; Tambornino, Frank; Hinz, Alexander; Borden, Weston Thatcher; Goicoechea, Jose M.; Chen, Bo; Wang, Xue‐Bin

doi:10.1002/ange.201906904

Title: Photoelectron Spectroscopy and Theoretical Studies of PCSe ⁻ , AsCS ⁻ , AsCSe ⁻ , and NCSe ⁻ : Insights into the Electronic Structures of the Whole Family of ECX ⁻ Anions (E=N, P, As; X=O, S, Se)

Abstract

Abstract The newly synthesized phosphorus‐ and arsenic‐containing analogues of the thio‐ and seleno‐cyanate anions, PCSe ⁻ , AsCS ⁻ , and AsCSe ⁻ , as well as the known ion NCSe ⁻ were investigated in the gas phase by negative‐ion photoelectron spectroscopy (NIPES), velocity‐map imaging (VMI) spectroscopy, and quantum‐chemical computations. The electron affinities (EA), spin–orbit (SO) splittings, and “symmetric”/“asymmetric” stretching frequencies of the neutral radicals ECX ^. (E=N, P, As; X=S, Se), generated by electron detachment from the corresponding anions, were obtained from the spectra. The calculated EAs, SO splittings, and vibrational frequencies are in excellent agreement with the experimental measurements. These newly obtained values, when combined with those previously determined for the lighter analogues, show interesting trends on descending the pnictogen and chalcogen series. These trends are rationalized based on electronegativity arguments, the electron distributions in the HOMOs, and NBO/NRT analyses.

Authors:

Yuan, Qinqin ^[1]; Tambornino, Frank ^[2]; Hinz, Alexander ^[3]; Borden, Weston Thatcher ^[4]; Goicoechea, Jose M. ^[5]; Chen, Bo ^[6];

^[1]

Physical Sciences Division Pacific Northwest National Laboratory 902 Battelle Boulevard, P. O. Box 999, MS K8-88 Richland WA 99352 USA
Department of Chemistry University of Oxford Chemistry Research Laboratory 12 Mansfield Road Oxford OX1 3TA UK, Fachbereich Chemie Philipps-Universität Marburg Hans-Meerwein-Strasse 4 35043 Marburg Germany
Karlsruhe Institut of Technology (KIT) Institute for Inorganic Chemistry (AOC) Engesserstraße 15, Geb. 30.45 76131 Karlsruhe Germany
Department of Chemistry and the Center for Advanced Scientific Computing and Modeling University of North Texas 1155 Union Circle, #305070 Denton TX 76203-5070 USA
Department of Chemistry University of Oxford Chemistry Research Laboratory 12 Mansfield Road Oxford OX1 3TA UK
Department of Chemistry Pennsylvania State University University Park PA 16801 USA

Publication Date:: Wed Sep 04 00:00:00 EDT 2019

Sponsoring Org.:: USDOE

OSTI Identifier:: 1560282

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie

Additional Journal Information:: Journal Name: Angewandte Chemie Journal Volume: 131 Journal Issue: 42; Journal ID: ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Yuan, Qinqin, Tambornino, Frank, Hinz, Alexander, Borden, Weston Thatcher, Goicoechea, Jose M., Chen, Bo, and Wang, Xue‐Bin. Photoelectron Spectroscopy and Theoretical Studies of PCSe − , AsCS − , AsCSe − , and NCSe − : Insights into the Electronic Structures of the Whole Family of ECX − Anions (E=N, P, As; X=O, S, Se).  Germany: N. p., 2019. 
Web.  doi:10.1002/ange.201906904.

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                    Yuan, Qinqin, Tambornino, Frank, Hinz, Alexander, Borden, Weston Thatcher, Goicoechea, Jose M., Chen, Bo, & Wang, Xue‐Bin. Photoelectron Spectroscopy and Theoretical Studies of PCSe − , AsCS − , AsCSe − , and NCSe − : Insights into the Electronic Structures of the Whole Family of ECX − Anions (E=N, P, As; X=O, S, Se).  Germany.  https://doi.org/10.1002/ange.201906904

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                    Yuan, Qinqin, Tambornino, Frank, Hinz, Alexander, Borden, Weston Thatcher, Goicoechea, Jose M., Chen, Bo, and Wang, Xue‐Bin. Wed .  
"Photoelectron Spectroscopy and Theoretical Studies of PCSe − , AsCS − , AsCSe − , and NCSe − : Insights into the Electronic Structures of the Whole Family of ECX − Anions (E=N, P, As; X=O, S, Se)".  Germany.  https://doi.org/10.1002/ange.201906904.

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@article{osti_1560282,

  title        = {Photoelectron Spectroscopy and Theoretical Studies of PCSe − , AsCS − , AsCSe − , and NCSe − : Insights into the Electronic Structures of the Whole Family of ECX − Anions (E=N, P, As; X=O, S, Se)},

  author       = {Yuan, Qinqin and Tambornino, Frank and Hinz, Alexander and Borden, Weston Thatcher and Goicoechea, Jose M. and Chen, Bo and Wang, Xue‐Bin},

  abstractNote = {Abstract The newly synthesized phosphorus‐ and arsenic‐containing analogues of the thio‐ and seleno‐cyanate anions, PCSe − , AsCS − , and AsCSe − , as well as the known ion NCSe − were investigated in the gas phase by negative‐ion photoelectron spectroscopy (NIPES), velocity‐map imaging (VMI) spectroscopy, and quantum‐chemical computations. The electron affinities (EA), spin–orbit (SO) splittings, and “symmetric”/“asymmetric” stretching frequencies of the neutral radicals ECX . (E=N, P, As; X=S, Se), generated by electron detachment from the corresponding anions, were obtained from the spectra. The calculated EAs, SO splittings, and vibrational frequencies are in excellent agreement with the experimental measurements. These newly obtained values, when combined with those previously determined for the lighter analogues, show interesting trends on descending the pnictogen and chalcogen series. These trends are rationalized based on electronegativity arguments, the electron distributions in the HOMOs, and NBO/NRT analyses.},

  doi          = {10.1002/ange.201906904},

  journal      = {Angewandte Chemie},

  number       = 42,

  volume       = 131,

  place        = {Germany},

  year         = {Wed Sep 04 00:00:00 EDT 2019},

  month        = {Wed Sep 04 00:00:00 EDT 2019}

}

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Title: Photoelectron Spectroscopy and Theoretical Studies of PCSe − , AsCS − , AsCSe − , and NCSe − : Insights into the Electronic Structures of the Whole Family of ECX − Anions (E=N, P, As; X=O, S, Se)

Abstract

Citation Formats

Acyl- und Alkylidenphosphane. XXXIII. Lithoxy-methylidenphosphan � DME und -methylidinphosphan � 2 DME ? Synthese und Struktur journal, June 1992

The 2-Phosphaethynolate Anion: A Convenient Synthesis and [2+2] Cycloaddition Chemistry journal, August 2013

Eine monoanionische Arsenid-Quelle: Decarbonylierung des 2-Arsaethinolat-Anions bei der Reaktion mit Stannylenen journal, November 2016

Phosphanierung von Kohlenmonoxid: eine einfache Synthese von Natriumphosphaethinolat (NaOCP) journal, July 2011

The 2-Arsaethynolate Anion: Synthesis and Reactivity Towards Heteroallenes journal, April 2016

Uranium and thorium complexes of the phosphaethynolate ion journal, January 2015

2-Phospha- and 2-Arsaethynolates - Versatile Building Blocks in Modern Synthetic Chemistry: 2-Phospha- and 2-Arsaethynolates - Versatile Building Blocks in Modern Synthetic Chemistry journal, May 2018

Performance of dynamically weighted multiconfiguration self-consistent field and spin-orbit coupling calculations of diatomic molecules of Group 14 elements journal, January 2011

Alkylidinphosphane und -arsane. I [P ? C?S]?[Li(dme)3]+ - Synthese und Struktur journal, March 1994

A General Synthesis of Phosphorus‐ and Arsenic‐Containing Analogues of the Thio‐ and Seleno‐cyanate Anions journal, June 2018

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The 2-Arsaethynolate Anion: Synthesis and Reactivity Towards Heteroallenes journal, April 2016

A Monoanionic Arsenide Source: Decarbonylation of the 2-Arsaethynolate Anion upon Reaction with Bulky Stannylenes journal, November 2016

Unexpected Photodegradation of a Phosphaketenyl-Substituted Germyliumylidene Borate Complex journal, March 2017

The 2-Phosphaethynolate Anion: A Convenient Synthesis and [2+2] Cycloaddition Chemistry journal, August 2013

HPCO-A Phosphorus-Containing Analogue of Isocyanic Acid journal, March 2017

Ambient-Temperature Synthesis of 2-Phosphathioethynolate, PCS - , and the Ligand Properties of ECX - (E = N, P; X = O, S) : Ambient-Temperature Synthesis of 2-Phosphathioethynolate journal, November 2015

Photoelectron spectroscopy of CN − , NCO − , and NCS − journal, January 1993

Spectroscopic Characterization, Computational Investigation, and Comparisons of ECX – (E = As, P, and N; X = S and O) Anions journal, June 2017

Synthesis and Characterization of Terminal [Re(XCO)(CO) 2 (triphos)] (X=N, P): Isocyanate versus Phosphaethynolate Complexes journal, September 2012

HPCO-A Phosphorus-Containing Analogue of Isocyanic Acid journal, March 2017

Phosphination of Carbon Monoxide: A Simple Synthesis of Sodium Phosphaethynolate (NaOCP) journal, July 2011

Unexpected Photodegradation of a Phosphaketenyl-Substituted Germyliumylidene Borate Complex journal, March 2017

Gaussian basis sets for use in correlated molecular calculations. X. The atoms aluminum through argon revisited journal, June 2001

Isolation of Au-, Co-η 1 PCO and Cu-η 2 PCO complexes, conversion of an Ir–η 1 PCO complex into a dimetalladiphosphene, and an interaction-free PCO anion journal, January 2016

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Phosphinecarboxamide: A Phosphorus-Containing Analogue of Urea and Stable Primary Phosphine journal, December 2013

Title: Photoelectron Spectroscopy and Theoretical Studies of PCSe ⁻ , AsCS ⁻ , AsCSe ⁻ , and NCSe ⁻ : Insights into the Electronic Structures of the Whole Family of ECX ⁻ Anions (E=N, P, As; X=O, S, Se)

Acyl- und Alkylidenphosphane. XXXIII. Lithoxy-methylidenphosphan � DME und -methylidinphosphan � 2 DME ? Synthese und Struktur
journal, June 1992

The 2-Phosphaethynolate Anion: A Convenient Synthesis and [2+2] Cycloaddition Chemistry
journal, August 2013

Eine monoanionische Arsenid-Quelle: Decarbonylierung des 2-Arsaethinolat-Anions bei der Reaktion mit Stannylenen
journal, November 2016

Phosphanierung von Kohlenmonoxid: eine einfache Synthese von Natriumphosphaethinolat (NaOCP)
journal, July 2011

The 2-Arsaethynolate Anion: Synthesis and Reactivity Towards Heteroallenes
journal, April 2016

Uranium and thorium complexes of the phosphaethynolate ion
journal, January 2015

2-Phospha- and 2-Arsaethynolates - Versatile Building Blocks in Modern Synthetic Chemistry: 2-Phospha- and 2-Arsaethynolates - Versatile Building Blocks in Modern Synthetic Chemistry
journal, May 2018

Performance of dynamically weighted multiconfiguration self-consistent field and spin-orbit coupling calculations of diatomic molecules of Group 14 elements
journal, January 2011

Alkylidinphosphane und -arsane. I [P ? C?S]?[Li(dme)3]+ - Synthese und Struktur
journal, March 1994

A General Synthesis of Phosphorus‐ and Arsenic‐Containing Analogues of the Thio‐ and Seleno‐cyanate Anions
journal, June 2018

Cyclo-oligomerization of isocyanates with Na(PH ₂ ) or Na(OCP) as “P ⁻ ” anion sources
journal, January 2015

The 2-Arsaethynolate Anion: Synthesis and Reactivity Towards Heteroallenes
journal, April 2016

A Monoanionic Arsenide Source: Decarbonylation of the 2-Arsaethynolate Anion upon Reaction with Bulky Stannylenes
journal, November 2016

Unexpected Photodegradation of a Phosphaketenyl-Substituted Germyliumylidene Borate Complex
journal, March 2017

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journal, August 2013

HPCO-A Phosphorus-Containing Analogue of Isocyanic Acid
journal, March 2017

Ambient-Temperature Synthesis of 2-Phosphathioethynolate, PCS ^- , and the Ligand Properties of ECX ^- (E = N, P; X = O, S) : Ambient-Temperature Synthesis of 2-Phosphathioethynolate
journal, November 2015

Photoelectron spectroscopy of CN ⁻ , NCO ⁻ , and NCS ⁻
journal, January 1993

Spectroscopic Characterization, Computational Investigation, and Comparisons of ECX ^– (E = As, P, and N; X = S and O) Anions
journal, June 2017

Synthesis and Characterization of Terminal [Re(XCO)(CO) ₂ (triphos)] (X=N, P): Isocyanate versus Phosphaethynolate Complexes
journal, September 2012

HPCO-A Phosphorus-Containing Analogue of Isocyanic Acid
journal, March 2017

Phosphination of Carbon Monoxide: A Simple Synthesis of Sodium Phosphaethynolate (NaOCP)
journal, July 2011

Unexpected Photodegradation of a Phosphaketenyl-Substituted Germyliumylidene Borate Complex
journal, March 2017

Gaussian basis sets for use in correlated molecular calculations. X. The atoms aluminum through argon revisited
journal, June 2001

Isolation of Au-, Co-η ¹ PCO and Cu-η ² PCO complexes, conversion of an Ir–η ¹ PCO complex into a dimetalladiphosphene, and an interaction-free PCO anion
journal, January 2016

Isolation of a Heavier Cyclobutadiene Analogue: 2,4-Digerma-1,3-diphosphacyclobutadiene
journal, May 2016

A General Synthesis of Phosphorus- and Arsenic-Containing Analogues of the Thio- and Seleno-cyanate Anions
journal, June 2018

Phosphinecarboxamide: A Phosphorus-Containing Analogue of Urea and Stable Primary Phosphine
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