Fabian Munkes, Matthew H Rayment, Alexander Trachtmann, Florian Anschütz, Ettore Eder, Philipp Hengel, Yannick Schellander, Patrick Schalberger, Norbert Fruehauf, Jens Anders, Robert Löw, Tilman Pfau, Stephen D Hogan, Harald Kübler
{"title":"High-Resolution Continuous-Wave Laser Spectroscopy of Long-Lived Rydberg States in NO.","authors":"Fabian Munkes, Matthew H Rayment, Alexander Trachtmann, Florian Anschütz, Ettore Eder, Philipp Hengel, Yannick Schellander, Patrick Schalberger, Norbert Fruehauf, Jens Anders, Robert Löw, Tilman Pfau, Stephen D Hogan, Harald Kübler","doi":"10.1021/acs.jpclett.4c02002","DOIUrl":null,"url":null,"abstract":"<p><p>High-resolution continuous-wave (cw) laser spectroscopy of nitric oxide (NO) molecules has been performed to study and characterize the energy-level structure of and effects of electric fields on the high Rydberg states. The experiments were carried out with molecules flowing through a room temperature gas cell. Rydberg-state photoexcitation was implemented using the resonance enhanced <math><mrow><mo>(</mo><mi>n</mi><mi>l</mi><mo>)</mo></mrow><msup><mrow><mi>X</mi></mrow><mrow><mo>+</mo></mrow></msup><mmultiscripts><mrow><msup><mrow><mtext> </mtext><mi>Σ</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow><mprescripts></mprescripts><none></none><mrow><mn>1</mn></mrow></mmultiscripts><mo>←</mo><mi>H</mi><mmultiscripts><mrow><msup><mrow><mtext> </mtext><mi>Σ</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow><mprescripts></mprescripts><none></none><mrow><mn>2</mn></mrow></mmultiscripts><mo>←</mo><mi>A</mi><mmultiscripts><mrow><msup><mrow><mtext> </mtext><mi>Σ</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow><mprescripts></mprescripts><none></none><mrow><mn>2</mn></mrow></mmultiscripts><mo>←</mo><mi>X</mi><mmultiscripts><mrow><msub><mrow><mi>Π</mi></mrow><mrow><mn>3</mn><mo>/</mo><mn>2</mn></mrow></msub></mrow><mprescripts></mprescripts><none></none><mrow><mn>2</mn></mrow></mmultiscripts></math> three-color three-photon excitation scheme. Excited molecules were detected by high-sensitivity optogalvanic methods. Detailed measurements were made of Rydberg states with principal quantum numbers <i>n</i> = 22 and 32 in the series converging to the lowest rotational and vibrational state of the NO<sup>+</sup> cation. The experimental data were compared with the results of numerical calculations which provided insight into the orbital angular momentum character of the intermediate H <sup>2</sup>Σ<sup>+</sup> state, improved determinations of the <i>n</i>f and <i>n</i>g quantum defects, a bound on the magnitude of the <i>n</i>h quantum defect, and information on the decay rates of the <i>n</i>f and <i>n</i>g Rydberg states. These measurements represent a step-change in laser spectroscopic studies of high Rydberg states in small atmospheric molecules. They open opportunities for more detailed studies of slow decay processes of Rydberg NO molecules confined in electrostatic traps, the synthesis of ultralong range Rydberg bimolecules, and the development of optical methods for trace gas detection.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8000,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c02002","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/10/1 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
High-resolution continuous-wave (cw) laser spectroscopy of nitric oxide (NO) molecules has been performed to study and characterize the energy-level structure of and effects of electric fields on the high Rydberg states. The experiments were carried out with molecules flowing through a room temperature gas cell. Rydberg-state photoexcitation was implemented using the resonance enhanced three-color three-photon excitation scheme. Excited molecules were detected by high-sensitivity optogalvanic methods. Detailed measurements were made of Rydberg states with principal quantum numbers n = 22 and 32 in the series converging to the lowest rotational and vibrational state of the NO+ cation. The experimental data were compared with the results of numerical calculations which provided insight into the orbital angular momentum character of the intermediate H 2Σ+ state, improved determinations of the nf and ng quantum defects, a bound on the magnitude of the nh quantum defect, and information on the decay rates of the nf and ng Rydberg states. These measurements represent a step-change in laser spectroscopic studies of high Rydberg states in small atmospheric molecules. They open opportunities for more detailed studies of slow decay processes of Rydberg NO molecules confined in electrostatic traps, the synthesis of ultralong range Rydberg bimolecules, and the development of optical methods for trace gas detection.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.