Search arXiv⌕ Search
Home/Archive/arXiv

arXiv · 2503.13838

Narrowline Laser Cooling and Spectroscopy of Molecules via Stark States

Kameron Mehling·Justin J. Burau·Logan E. Hillberry·Mengjie Chen·Parul Aggarwal·Lan Cheng·Jun Ye·Simon Scheidegger
View original source ↗Read source document ↗Export metadata ↓

Abstract

The electronic energy level structure of yttrium monoxide (YO) provides a long-lived, low-lying $^{2}Δ$ state ideal for high-precision molecular spectroscopy, narrowline laser cooling at the single photon-recoil limit, and studying dipolar physics with unprecedented interaction strength. High-resolution laser spectroscopy of ultracold laser-cooled YO molecules is used to study the Stark effect in the A$^{\prime}\,^{2}Δ_{3/2}\,J=3/2$ state. An immediate onset of the linear Stark effect is observed in the presence of weak applied electric fields due to the near degenerate $Λ$-doublet and the large electric dipole moment. By applying a small electric field the Stark insensitive state is spectroscopically isolated and the absolute transition frequency to the X$\,^2Σ^+$ electronic ground state is determined with a fractional frequency uncertainty of 9 $\times$ 10$^{-12}$. This electric field control is necessary to implement a quasi-closed photon cycling scheme that preserves parity. With this scheme the first narrowline laser cooling of a molecules is demonstrated, reducing the temperature of sub-Doppler cooled YO in two dimensions.

Explore related subjects

physics.atom-ph

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

Kameron Mehling, Justin J. Burau, Logan E. Hillberry, Mengjie Chen, Parul Aggarwal, Lan Cheng, Jun Ye, Simon Scheidegger. 2025-11-13. Narrowline Laser Cooling and Spectroscopy of Molecules via Stark States. https://doi.org/10.1103/9v1s-d6bd

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

arXiv2026

State-Dependent Diffusion and Spectra of Strongly Driven Thermal Atoms

We propose a state-dependent diffusion model for strongly driven thermal-atom spectra. Starting from the trajectory-dependent internal-state evolution of individual atoms, we derive a closed spatial equation for the local density-matrix field using a velocity-moment expansion. Measurements of an $^{85}$Rb atomic-filter transmission spectrum agree well with the model up to a maximum Gaussian peak intensity of $1.27\times10^{3}$ W/cm$^2$, approaching six orders of magnitude above the $^{85}$Rb D2-line saturation intensity. Counterintuitively, the model reveals an anomalous optical-pumping pathway in which intense light transfers atoms from nominally dark states into bright states. Hyperfine Paschen--Back splitting selectively enhances this anomalous pathway while suppressing conventional optical pumping, allowing the filter to maintain approximately 97$\%$ transmission at the highest intensity studied. This work provides a framework for controlling strongly driven atomic ensembles and designing saturation-resistant atomic optical devices.

physics.atom-ph↗
arXiv2026

Interactions and excitation blockade of Rydberg macrodimers

We present a theoretical study of interactions between Rydberg macrodimers, molecular bound states of Rydberg atoms, and the largest known neutral homonuclear diatomic molecules. Accounting for the large number of molecular interaction channels from four interacting Rydberg atoms, we show that macrodimer-macrodimer interactions are anisotropic and similar in strength and range to atomic-state Rydberg interactions. Our analysis reveals the presence of two-atom, three-atom, and four-atom contributions in the bimolecular system, and elucidates how these interactions are rooted in the underlying atomic Rydberg-state couplings. Our calculations of the excitation blockade between macrodimers are in reasonable agreement with experimentally observed signals, and pave the way for the exploration of optically controlled collective quantum dynamics in molecular systems.

physics.atom-ph↗
arXiv2026

Non-orthogonal extension of Graspg - dynamic electron correlation for large and compact active spaces

Accurate relativistic multiconfiguration calculations of correlation-sensitive atomic properties are often limited by the rapid growth of configuration state function expansions when a single common orthonormal orbital basis is used. In this work, a partitioned correlation function interaction (PCFI) method is developed for relativistic atomic structure calculations. The correlation space is separated into physically motivated components, which are optimized independently with correlation-specific orbital sets. The interactions between configuration spaces constructed from mutually non-orthogonal orbital sets are evaluated using biorthonormal transformations, allowing different correlation effects to be combined in a compact final interaction calculation. Full details of the method are provided, emphasizing its connection to configuration state function generators (CSFGs), which significantly reduce the time required to construct the Hamiltonian matrix in conventional RCI calculations. Applications to the neutral Li, Be, and Al atoms are presented for energy levels, mass shifts and hyperfine structure constants. Compared with conventional relativistic configuration interaction (RCI) calculations that rely on a single orbital basis, PCFI produces more compact and predictable convergence patterns for both total and transition energies. It also offers greater stability for correlation-sensitive properties such as specific mass shifts and hyperfine constants. By using property-oriented partitions, PCFI captures core-polarization effects more effectively, thereby reducing the oscillatory behavior often observed in standard RCI approaches. Overall, the results demonstrate that PCFI provides a promising and computationally efficient framework for accurate relativistic multiconfiguration calculations of correlation-dependent atomic properties.

physics.atom-ph↗