IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-38873-z.html
   My bibliography  Save this article

Direct observation of coherence transfer and rotational-to-vibrational energy exchange in optically centrifuged CO2 super-rotors

Author

Listed:
  • Timothy Y. Chen

    (Sandia National Laboratories
    Applied Materials, Inc.)

  • Scott A. Steinmetz

    (Sandia National Laboratories)

  • Brian D. Patterson

    (Sandia National Laboratories)

  • Ahren W. Jasper

    (Argonne National Laboratory)

  • Christopher J. Kliewer

    (Sandia National Laboratories)

Abstract

Optical centrifuges are laser-based molecular traps that can rotationally accelerate molecules to energies rivalling or exceeding molecular bond energies. Here we report time and frequency-resolved ultrafast coherent Raman measurements of optically centrifuged CO2 at 380 Torr spun to energies beyond its bond dissociation energy of 5.5 eV (Jmax = 364, Erot = 6.14 eV, Erot/kB = 71, 200 K). The entire rotational ladder from J = 24 to J = 364 was resolved simultaneously which enabled a more accurate measurement of the centrifugal distortion constants for CO2. Remarkably, coherence transfer was directly observed, and time-resolved, during the field-free relaxation of the trap as rotational energy flowed into bending-mode vibrational excitation. Vibrationally excited CO2 (ν2 > 3) was observed in the time-resolved spectra to populate after 3 mean collision times as a result of rotational-to-vibrational (R-V) energy transfer. Trajectory simulations show an optimal range of J for R-V energy transfer. Dephasing rates for molecules rotating up to 5.5 times during one collision were quantified. Very slow decays of the vibrational hot band rotational coherences suggest that they are sustained by coherence transfer and line mixing.

Suggested Citation

  • Timothy Y. Chen & Scott A. Steinmetz & Brian D. Patterson & Ahren W. Jasper & Christopher J. Kliewer, 2023. "Direct observation of coherence transfer and rotational-to-vibrational energy exchange in optically centrifuged CO2 super-rotors," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38873-z
    DOI: 10.1038/s41467-023-38873-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-38873-z
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-023-38873-z?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Ivan O. Antonov & Patrick R. Stollenwerk & Sruthi Venkataramanababu & Ana P. Lima Batista & Antonio G. S. Oliveira-Filho & Brian C. Odom, 2021. "Precisely spun super rotors," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Sruthi Venkataramanababu & Anyang Li & Ivan O. Antonov & James B. Dragan & Patrick R. Stollenwerk & Hua Guo & Brian C. Odom, 2023. "Enhancing reactivity of SiO+ ions by controlled excitation to extreme rotational states," Nature Communications, Nature, vol. 14(1), pages 1-7, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38873-z. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.