We show that the highly excited rovibrational spectra of a diatomic molecule and the closely related slow atomic collision processes contain more systematics and require less parameters to characterize than the Rydberg spectrum of an atom. In the case of a single channel, for example, we show that a single short-range parameter gives a complete description of slow collisions for practically all angular momenta, and covers an energy range of hundreds of millikelvins. The same parameter also describes the highly excited rovibrational spectra in the threshold region, including states of different angular momenta. Sample applications and predictions of the theory are discussed, including comparisons with experiment.
Algebraic Determination of Spectral Characteristics of Rovibrational States of Diatomic Molecules. I. Diagram Technique for Determination of Vibrational Dependences of Matrix Elements
Algebraic Determination of Spectral Characteristics of Rovibrational States of Diatomic Molecules. II. Analysis of the Vibration-Rotation Interaction by Means of the Factorization Method
Following the first principles the elements of the analytic theory of potential curves for diatomic molecules (diatomics) are presented. It is based on matching the perturbation theory at small internuclear distances $R$ and multipole expansion at large distances, modified by instanton-induced trans-series for homonuclear case, with addition of the phenomenologically described equilibrium configuration, if exists. It leads to a new class of (generalized) meromorphic potentials (modified by exponential terms) with difference in degrees of polynomials in numerator and denominator equal to 4 (6) …
We report a direct measurement of the 0-1 R(0) vibrational transition frequency in ground-state hydrogen deuteride (HD) using infrared-ultraviolet double resonance spectroscopy in a molecular beam. Ground-state molecules are vibrationally excited using a frequency comb referenced continuous-wave infrared laser, and the excited molecules are detected via state-selective ionization with a pulsed ultraviolet laser. We determine an absolute transition frequency of 111 448 815 477(13) kHz. The 0.12 parts-per-billion (ppb) uncertainty is limited primarily by the residual first-order Doppler shift.
The H$_2$+H$_2$ system has long been considered as a benchmark system for ro-vibrational energy transfer in bimolecular collisions. However, most studies thus far have focused on collisions involving H$_2$ molecules in the ground vibrational level or in the first excited vibrational state. While H$_2$+H$_2$/HD collisions have received wide attention due to the important role they play in astrophysics, D$_2$+D$_2$ collisions have received much less attention. Recently, Zhou et al. [Nat. Chem. 4 658 (2022)] examined stereodynamic aspects of rotational energy transfer in collisions of two aligned…
Accurate photodissociation cross sections have been computed for transitions from the X $^1Σ^+$ ground electronic state of CS to six low-lying excited electronic states. New ab initio potential curves and transition dipole moment functions have been obtained for these computations using the multi-reference configuration interaction approach with the Davidson correction (MRCI+Q) and aug-cc-pV6Z basis sets. State-resolved cross sections have been computed for transitions from nearly the full range of rovibrational levels of the X $^1Σ^+$ state and for photon wavelengths ranging from 500 $\textÅ$…
Interatomic potentials, electric properties, and spectroscopy of the ground and excited states of the Rb_2 molecule: Ab initio calculations and effect of a non-resonant field
Effect of the avoided crossing on the rovibrational energy levels, resonances, and predissociation lifetimes within the ground and first excited electronic states of lithium fluoride
Triatomic molecule RaOH combines the advantages of laser-coolability and the spectrum with close opposite-parity doublets. This makes it a promising candidate for experimental study of the $\mathcal{P}$,$\mathcal{T}$-violation. Previous studies concentrated on the calculations for different geometries without the averaging over the rovibrational wave function and stressed the possibility that the dependence of the $\mathcal{P}$, $\mathcal{T}$ parameters on the bond angle may significantly alter the observed value. We obtain the rovibrational wave functions of RaOH in the ground electronic stat…
We demonstrate the coherent creation of a single NaCs molecule in its rotational, vibrational, and electronic (rovibronic) ground state in an optical tweezer. Starting with a weakly bound Feshbach molecule, we locate a two-photon transition via the $|{c^3Σ,v'=26}\rangle$ excited state and drive coherent Rabi oscillations between the Feshbach state and a single hyperfine level of the NaCs rovibronic ground state $|{X^1Σ,v''=0,N''=0}\rangle$ with a binding energy of $D_0 = h \times 147038.30(2)$ GHz. We measure a lifetime of $3.4\pm1.6$ s for the rovibronic ground-state molecule, which possesses…
We report on the fragmentation dynamics of triply charged, diatomic, molecular ions of NO and CO. Dissociative fragmentation after multiple ionization of NO and CO is studied under the impact of 200 keV proton beam using recoil-ion momentum spectrometer. Kinetic Energy Release distributions (KERDs) for various fragmentation channels were obtained. We have also calculated the potential energy curves (PECs) for ground and several excited states of NO^{3+} and CO^{3+} molecular ion. The obtained KERDs are discussed in the background of the calculated PECs as well as the simple Coulomb excitation …
Characterising molecules for fundamental physics: an accurate spectroscopic model of methyltrioxorhenium derived from new infrared and millimetre-wave measurements
Spectroscopy of the Hyperfine Structure of HD$^+$ in Rotationally Excited States with 10-ppb Uncertainty
ASML；Laboratoire Kastler Brossel, Sorbonne Université, CNRS, ENS-PSL Research University, Collège de France（卡斯勒-布罗塞尔实验室，索邦大学，法国国家科学研究中心，巴黎文理研究大学，法兰西学院）；LaserLaB, Department of Physics and Astronomy, Vrije Universiteit Amsterdam（激光实验室，阿姆斯特丹自由大学物理与天文系）；Science Institute and Faculty of Physical Sciences, University of Iceland（冰岛大学理学院和物理科学学院）
We report a detailed molecular spectroscopy study on the lowest excited electronic states of $^{23}\rm{Na}^{87}\rm{Rb}$ for producing ultracold $^{23}\rm{Na}^{87}\rm{Rb}$ molecules in the electronic, rovibrational and hyperfine ground state. Starting from weakly-bound Feshbach molecules, a series of vibrational levels of the $A^{1}Σ^{+}-b^{3}Π$ coupled excited states were investigated. After resolving, modeling and interpreting the hyperfine structure of several lines, we successfully identified a long-lived level resulting from the accidental hyperfine coupling between the $0^+$ and $0^-$ com…
