Rotational level spacings in HD from vibrational saturation spectroscopy

F. M.J. Cozijn; M. L. Diouf; V. Hermann; E. J. Salumbides; M. Schlösser; W. Ubachs

doi:10.1103/PhysRevA.105.062823

Rotational level spacings in HD from vibrational saturation spectroscopy

F. M.J. Cozijn, M. L. Diouf, V. Hermann, E. J. Salumbides, M. Schlösser, W. Ubachs

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Abstract

The R(1), R(3), and P(3) rovibrational transitions in the (2-0) overtone band of the HD molecule are measured in Doppler-free saturation using the technique of NICE-OHMS spectroscopy. For the P(3) line, hitherto not observed in saturation, we report a frequency of 203821936805(60) kHz. The dispersive line shapes observed in the three spectra show strong correlations, allowing for extraction of accurate information on rotational level spacings. This leads to level spacings of Δ(J=3)-(J=1)=13283245098(30) kHz in the v=0 ground state and Δ(J=4)-(J=2)=16882368179(20) kHz in the v=2 excited vibration in HD. These results show that experimental values for the rotational spacings are consistently larger than those obtained with advanced ab initio theoretical calculations at 1.5σ, where the uncertainty is determined by theory. The same holds for the vibrational transitions where systematic deviations of 1.7-1.9σ are consistently found for the five lines accurately measured in the (2-0) band.

Original language	English
Article number	062823
Pages (from-to)	1-8
Number of pages	8
Journal	Physical Review A
Volume	105
Issue number	6
Early online date	28 Jun 2022
DOIs	https://doi.org/10.1103/PhysRevA.105.062823
Publication status	Published - Jun 2022

Bibliographical note

Funding Information:
The authors thank IHM van Stokkum (VUA) for fruitful discussions on the data analysis. The research was funded via the Access Program of Laserlab-Europe (Grants No. 654148 and No. 871124), a European Union Horizon 2020 research and innovation program. Financial support from the European Research Council (ERC-Advanced Grant No. 670168) and from the Netherlands Organisation for Scientific Research (NWO), via the Program “The Mysterious Size of the Proton,” is gratefully acknowledged. M.S. wants to thank the Baden-Württemberg Foundation for the generous support of this work within the Elite-Postdoc-Fellowship.

Publisher Copyright:
© 2022 American Physical Society.

Funding

The authors thank IHM van Stokkum (VUA) for fruitful discussions on the data analysis. The research was funded via the Access Program of Laserlab-Europe (Grants No. 654148 and No. 871124), a European Union Horizon 2020 research and innovation program. Financial support from the European Research Council (ERC-Advanced Grant No. 670168) and from the Netherlands Organisation for Scientific Research (NWO), via the Program “The Mysterious Size of the Proton,” is gratefully acknowledged. M.S. wants to thank the Baden-Württemberg Foundation for the generous support of this work within the Elite-Postdoc-Fellowship.

Funders	Funder number
ERC-Advanced
Baden-Württemberg Stiftung
Horizon 2020 Framework Programme	670168
European Research Council
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
Horizon 2020

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10.1103/PhysRevA.105.062823

Rotational level spacings in HD from vibrational saturation spectroscopyFinal published version, 1.37 MBLicence: Article 25fa Dutch Copyright Act

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title = "Rotational level spacings in HD from vibrational saturation spectroscopy",

abstract = "The R(1), R(3), and P(3) rovibrational transitions in the (2-0) overtone band of the HD molecule are measured in Doppler-free saturation using the technique of NICE-OHMS spectroscopy. For the P(3) line, hitherto not observed in saturation, we report a frequency of 203821936805(60) kHz. The dispersive line shapes observed in the three spectra show strong correlations, allowing for extraction of accurate information on rotational level spacings. This leads to level spacings of Δ(J=3)-(J=1)=13283245098(30) kHz in the v=0 ground state and Δ(J=4)-(J=2)=16882368179(20) kHz in the v=2 excited vibration in HD. These results show that experimental values for the rotational spacings are consistently larger than those obtained with advanced ab initio theoretical calculations at 1.5σ, where the uncertainty is determined by theory. The same holds for the vibrational transitions where systematic deviations of 1.7-1.9σ are consistently found for the five lines accurately measured in the (2-0) band.",

author = "Cozijn, {F. M.J.} and Diouf, {M. L.} and V. Hermann and Salumbides, {E. J.} and M. Schl{\"o}sser and W. Ubachs",

note = "Funding Information: The authors thank IHM van Stokkum (VUA) for fruitful discussions on the data analysis. The research was funded via the Access Program of Laserlab-Europe (Grants No. 654148 and No. 871124), a European Union Horizon 2020 research and innovation program. Financial support from the European Research Council (ERC-Advanced Grant No. 670168) and from the Netherlands Organisation for Scientific Research (NWO), via the Program “The Mysterious Size of the Proton,” is gratefully acknowledged. M.S. wants to thank the Baden-W{\"u}rttemberg Foundation for the generous support of this work within the Elite-Postdoc-Fellowship. Publisher Copyright: {\textcopyright} 2022 American Physical Society.",

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AU - Salumbides, E. J.

AU - Schlösser, M.

AU - Ubachs, W.

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N2 - The R(1), R(3), and P(3) rovibrational transitions in the (2-0) overtone band of the HD molecule are measured in Doppler-free saturation using the technique of NICE-OHMS spectroscopy. For the P(3) line, hitherto not observed in saturation, we report a frequency of 203821936805(60) kHz. The dispersive line shapes observed in the three spectra show strong correlations, allowing for extraction of accurate information on rotational level spacings. This leads to level spacings of Δ(J=3)-(J=1)=13283245098(30) kHz in the v=0 ground state and Δ(J=4)-(J=2)=16882368179(20) kHz in the v=2 excited vibration in HD. These results show that experimental values for the rotational spacings are consistently larger than those obtained with advanced ab initio theoretical calculations at 1.5σ, where the uncertainty is determined by theory. The same holds for the vibrational transitions where systematic deviations of 1.7-1.9σ are consistently found for the five lines accurately measured in the (2-0) band.

AB - The R(1), R(3), and P(3) rovibrational transitions in the (2-0) overtone band of the HD molecule are measured in Doppler-free saturation using the technique of NICE-OHMS spectroscopy. For the P(3) line, hitherto not observed in saturation, we report a frequency of 203821936805(60) kHz. The dispersive line shapes observed in the three spectra show strong correlations, allowing for extraction of accurate information on rotational level spacings. This leads to level spacings of Δ(J=3)-(J=1)=13283245098(30) kHz in the v=0 ground state and Δ(J=4)-(J=2)=16882368179(20) kHz in the v=2 excited vibration in HD. These results show that experimental values for the rotational spacings are consistently larger than those obtained with advanced ab initio theoretical calculations at 1.5σ, where the uncertainty is determined by theory. The same holds for the vibrational transitions where systematic deviations of 1.7-1.9σ are consistently found for the five lines accurately measured in the (2-0) band.

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Rotational level spacings in HD from vibrational saturation spectroscopy

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