The puzzling hyper-fine structure and an accurate equilibrium geometry of succinic anhydride
An accurate semiexperimental equilibrium structure of succinic anhydride has been determined from a combination of experiment and theory. The cm-wave and mm-wave rotational spectra of succinic anhydride, 3,4-dihydrofuran-2,5-dione, were recorded in a pulsed supersonic jet using Fourier-transform mic...
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| Published in | Physical chemistry chemical physics : PCCP Vol. 22; no. 9; pp. 5170 - 5177 |
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| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
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England
Royal Society of Chemistry
04.03.2020
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| Abstract | An accurate semiexperimental equilibrium structure of succinic anhydride has been determined from a combination of experiment and theory. The cm-wave and mm-wave rotational spectra of succinic anhydride, 3,4-dihydrofuran-2,5-dione, were recorded in a pulsed supersonic jet using Fourier-transform microwave spectroscopy and in a free-jet using mm-wave absorption spectroscopy. Many lines in the cm-wave spectrum show fine structure and after eliminating all other possibilities the origin of this fine structure is determined to be from spin-spin interaction. Accurate rotational and quartic centrifugal distortion constants are determined. Assignments of 13C and 18O singly substituted isotopologues in natural abundance were used to obtain a substitution geometry for the heavy atoms of succinic anhydride. Theoretical approaches permitted the calculation of a Born-Oppenheimer ab initio structure and the determination of a semiexperimental equilibrium structure in which computed rovibrational corrections were utilized to convert vibrational ground state rotational constants into equilibrium constants. The agreement between the semiexperimental structure and the Born-Oppenheimer ab initio structure is excellent. Succinic anhydride has been shown to have a planar heavy atom equilibrium structure with the effects of a large amplitude vibration apparent in the resultant rotational constants. |
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| AbstractList | An accurate semiexperimental equilibrium structure of succinic anhydride has been determined from a combination of experiment and theory. The cm-wave and mm-wave rotational spectra of succinic anhydride, 3,4-dihydrofuran-2,5-dione, were recorded in a pulsed supersonic jet using Fourier-transform microwave spectroscopy and in a free-jet using mm-wave absorption spectroscopy. Many lines in the cm-wave spectrum show fine structure and after eliminating all other possibilities the origin of this fine structure is determined to be from spin-spin interaction. Accurate rotational and quartic centrifugal distortion constants are determined. Assignments of 13C and 18O singly substituted isotopologues in natural abundance were used to obtain a substitution geometry for the heavy atoms of succinic anhydride. Theoretical approaches permitted the calculation of a Born-Oppenheimer ab initio structure and the determination of a semiexperimental equilibrium structure in which computed rovibrational corrections were utilized to convert vibrational ground state rotational constants into equilibrium constants. The agreement between the semiexperimental structure and the Born-Oppenheimer ab initio structure is excellent. Succinic anhydride has been shown to have a planar heavy atom equilibrium structure with the effects of a large amplitude vibration apparent in the resultant rotational constants. An accurate semiexperimental equilibrium structure of succinic anhydride has been determined from a combination of experiment and theory. The cm-wave and mm-wave rotational spectra of succinic anhydride, 3,4-dihydrofuran-2,5-dione, were recorded in a pulsed supersonic jet using Fourier-transform microwave spectroscopy and in a free-jet using mm-wave absorption spectroscopy. Many lines in the cm-wave spectrum show fine structure and after eliminating all other possibilities the origin of this fine structure is determined to be from spin–spin interaction. Accurate rotational and quartic centrifugal distortion constants are determined. Assignments of 13 C and 18 O singly substituted isotopologues in natural abundance were used to obtain a substitution geometry for the heavy atoms of succinic anhydride. Theoretical approaches permitted the calculation of a Born–Oppenheimer ab initio structure and the determination of a semiexperimental equilibrium structure in which computed rovibrational corrections were utilized to convert vibrational ground state rotational constants into equilibrium constants. The agreement between the semiexperimental structure and the Born–Oppenheimer ab initio structure is excellent. Succinic anhydride has been shown to have a planar heavy atom equilibrium structure with the effects of a large amplitude vibration apparent in the resultant rotational constants. |
| Author | Vogt, Natalja Godfrey, Peter D McNaughton, Don Grabow, Jens-Uwe Demaison, Jean Obenchain, Daniel A Jahn, Michaela K Nair, K P Rajappan |
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| Cites_doi | 10.1021/jp067278j 10.1039/C4CP05905K 10.1063/1.4895904 10.1007/s11224-015-0654-0 10.1063/1.1136443 10.1016/0022-2860(95)08844-L 10.1063/1.2039347 10.1039/C6CP07487A 10.1007/s11224-009-9434-z 10.1016/j.jms.2016.06.001 10.1021/jp9040327 10.3891/acta.chem.scand.27-1101 10.1016/j.jms.2011.03.027 10.1007/s11224-010-9714-7 10.1107/S0365110X65004243 10.1016/0022-2852(91)90393-O 10.1016/0022-2860(88)80283-7 10.1063/1.443297 10.1021/jp963765v 10.1063/1.1147553 10.1063/1.4929999 10.1021/jp8089177 10.1016/j.jms.2018.03.003 10.1016/j.molstruc.2010.02.037 |
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| SubjectTerms | Anhydrides Chemical equilibrium Equilibrium Fine structure Fourier transforms Millimeter waves Rotational spectra Rotational states Spectrum analysis |
| Title | The puzzling hyper-fine structure and an accurate equilibrium geometry of succinic anhydride |
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