Abstract Polyatomic molecules have been identified as sensitive probes of charge-parity violating and parity violating physics beyond the Standard Model (BSM). For example, many linear triatomic molecules are both laser-coolable and have parity doublets in the ground electronic state arising from the bending vibration, both features that can greatly aid BSM searches. Understanding the state is a crucial prerequisite to precision measurements with linear polyatomic molecules. Here, we characterize the fundamental bending vibration of YbOH using high-resolution optical spectroscopy on the nominally forbidden transition at 588 nm. We assign 39 transitions originating from the lowest rotational levels of the state, and accurately model the state’s structure with an effective Hamiltonian using best-fit parameters. Additionally, we perform Stark and Zeeman spectroscopy on the state and fit the molecule-frame dipole moment to Dand the effective electrong-factor to . Further, we use an empirical model to explain observed anomalous line intensities in terms of interference from spin–orbit and vibronic perturbations in the excited state. Our work is an essential step toward searches for BSM physics in YbOH and other linear polyatomic molecules.
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Computation of the expectation value of the spin operator S^2 for the spin-flip Bethe–Salpeter equation
Abstract Spin-flip (SF) methods applied to excited-state approaches like the Bethe–Salpeter equation allow access to the excitation energies of open-shell systems, such as molecules and defects in solids. The eigenstates of these solutions, however, are generally not eigenstates of the spin operator . Even for simple cases where the excitation vector is expected to be, for example, a triplet state, the value of may be found to differ from 2.00; this difference is called ‘spin contamination’. The expectation values must be computed for each excitation vector, to assist with the characterization of the particular excitation and to determine the amount of spin contamination of the state. Our aim is to provide for the first time in the SF methods literature a comprehensive resource on the derivation of the formulas for as well as its computational implementation. After a brief discussion of the theory of the SF Bethe–Salpeter equation (BSE) and some examples further illustrating the need for calculating , we present the derivation for the general equation for computing with the eigenvectors from an SF-BSE calculation, how it is implemented in a Python script, and timing information on how this calculation scales with the size of the SF-BSE Hamiltonian.
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- Award ID(s):
- 2144317
- PAR ID:
- 10509064
- Publisher / Repository:
- Institute of Physics Publishing
- Date Published:
- Journal Name:
- Electronic Structure
- Volume:
- 6
- Issue:
- 2
- ISSN:
- 2516-1075
- Page Range / eLocation ID:
- 027001
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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