arXiv subjects

Alexander Frenett

Publications and source records attributed to Alexander Frenett.

9 recordsLinked to original sources

arXiv2026

Photon Cycling and Laser Cooling of an Asymmetric Top Molecule

We realize two-dimensional magnetically-assisted Sisyphus laser cooling of an asymmetric top molecule (ATM), calcium monoamide (CaNH$_2$). Vibrational state closure is achieved with $41.1 \pm 6.3$ photons scatters using optical pumping of the $X[3_1]$ state. Photon-cycling measurements show good agreement with branching ratios determined by dispersed fluorescence spectroscopy. Rotational closure is maintained by driving the $X[1_{11}] \to A [0_{00}]$ transition. The observed absence of additional state leakage channels broadens the scope of molecular laser cooling to include ATMs, which are the most general geometric class of molecules and possess the richest internal structure. Future applications of quantum controlled ATMs include new quantum information platforms and searches for physics beyond the Standard Model.

physics.atom-ph↗

arXiv2026

Optical cycling on thorium monoxide (ThO) for an improved test of fundamental symmetries

Optical cycling refers to repeated excitation and spontaneous emission on an electronic transition in an atom or molecule. Optical cycling in molecules can enable a wide range of quantum control and readout techniques, but unfortunately it has only been demonstrated on a small class of alkali-like or alkaline-earth-like molecules. Thorium monoxide (ThO), a molecule used in one of the most precise permanent electron electric dipole moment (eEDM) searches (ACME [1]), does not fall into this category. In this work, we demonstrate the first optical cycling on this non-conventional class over a range of experimental parameter space, including laser intensity, polarization switching rate, and interaction time. We show that both the $J = 1, 2$ rotational levels of ThO molecule are capable of cycling $11(2)$ photons on average with a single laser, at $1.9(6) \times 10^{6}~\mathrm{s}^{-1}$ and $2.3(7)\times 10^6~\mathrm{s}^{-1}$ scattering rate, respectively, before population is lost to other vibronic levels. We outline a scheme to apply this demonstrated optical cycling in an ACME-style eEDM measurement, improving the detection efficiency by over fourfold compared to non-cycling fluorescence detection. This would lead to over a twofold enhancement in the statistical sensitivity of the eEDM search. This optical cycling scheme can be further extended to scatter about 100 photons, which would enable a wider range of quantum control and sensing using ThO molecules. [1] V. Andreev, D. G. Ang, D. DeMille, J. M. Doyle, G. Gabrielse, J. Haefner, N. R. Hutzler, Z. Lasner, C. Meisenhelder, B. R. O`Leary, C. D. Panda, A. D. West, E. P. West, and X. Wu, Nature 562, 355 (2018).

physics.atom-ph↗

arXiv2024

Magneto-optical trapping of a heavy polyatomic molecule for precision measurement

We report a magneto-optical trap of strontium monohydroxide (SrOH) containing 2000(600) molecules at a temperature of 1.2(3) mK. The lifetime is 91(9) ms, which is limited by decay to optically unaddressed vibrational states. This provides the foundation for future sub-Doppler cooling and optical trapping of SrOH, a polyatomic molecule suited for precision searches for physics beyond the Standard Model including new CP violating particles and ultralight dark matter. We also identify important features in this system that guide cooling and trapping of complex and heavy polyatomic molecules into the ultracold regime.

physics.atom-ph↗

arXiv2024

Vibrational Branching Ratios for Laser-Cooling of Nonlinear Strontium-Containing Molecules

The vibrational branching ratios from the lowest excited electronic state for $\textrm{SrOCH}_3$, $\textrm{SrNH}_2$, and $\textrm{SrSH}$ are measured at the $< 0.1\%$ level. Spectra are obtained by driving the $\tilde{X} - \tilde{A}$ transitions and dispersing the fluorescence on a grating spectrometer. We also perform $\textit{ab initio}$ calculations for the energies of vibrational levels relevant for laser cooling, as well as branching ratios to support the interpretations of all molecular spectra. Symmetry group analysis is applied in conjunction with our data to study rotational closure in these molecules. These analyses indicate favorable prospects for laser cooling $\textrm{SrNH}_2$ and other similar alkaline-earth(-like) amides for future beyond the Standard Model physics searches using polyatomic molecules with long-lived parity doublets.

physics.atom-ph↗

arXiv2022

Zeeman-Sisyphus Deceleration for Heavy Molecules with Perturbed Excited-State Structure

We demonstrate and characterize Zeeman-Sisyphus (ZS) deceleration of a beam of ytterbium monohydroxide (YbOH). Our method uses a combination of large magnetic fields ($\sim$ 2.5 T) and optical spin-flip transitions to decelerate molecules while scattering only $\sim$ 10 photons per molecule. We study the challenges associated with the presence of internal molecular perturbations among the excited electronic states and discuss the methods used to overcome these challenges, including a modified ZS decelerator using microwave and optical transitions.

physics.atom-ph↗

arXiv2022

Zeeman-Sisyphus Deceleration of Molecular Beams

We present a robust, continuous molecular decelerator that employs high magnetic fields and few optical pumping steps. CaOH molecules are slowed, accumulating at low velocities in a range sufficient for loading both magnetic and magneto-optical traps. During the slowing, the molecules scatter only 7 photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.

physics.atom-ph↗

arXiv2020

Observation and laser spectroscopy of ytterbium monomethoxide, YbOCH$_3$

We describe a laser spectroscopic study of ytterbium monomethoxide, YbOCH$_3$, a species of interest to searches for time-reversal symmetry violation using laser-cooled molecules. We report measurements of vibrational structure in the $\tilde{X}$ and $\tilde{A}$ states, vibrational branching ratios for several components of the $\tilde{A}$ state, and radiative lifetimes of low-lying electronic states. $\textit{Ab initio}$ calculations are used to aid the assignment of vibronic emission bands and provide insight into the electronic and vibrational structure. Our results demonstrate that rapid optical cycling is feasible for YbOCH$_3$, opening a path to orders-of-magnitude increased sensitivity in future measurements of P- and/or T-violating physics.

physics.atom-ph↗

arXiv2019

Laser-Cooled Polyatomic Molecules for Improved Electron Electric Dipole Moment Searches

Doppler and Sisyphus cooling of $^{174}$YbOH are achieved and studied. This polyatomic molecule has high sensitivity to physics beyond the Standard Model and represents a new class of species for future high-precision probes of new T-violating physics. The transverse temperature of the YbOH beam is reduced by nearly two orders of magnitude to $< 600 \, μ$K and the phase-space density is increased by a factor of $>6$ via Sisyphus cooling. We develop a full numerical model of the laser cooling of YbOH and find excellent agreement with the data. We project that laser cooling and magneto-optical trapping of long-lived samples of YbOH molecules are within reach and these will allow a high sensitivity probe of the electric dipole moment (EDM) of the electron. The approach demonstrated here is easily generalized to other isotopologues of YbOH that have enhanced sensitivity to other symmetry-violating electromagnetic moments.

physics.atom-ph↗

arXiv2018

Two-photon vibrational transitions in ${\rm O}_2^+$ as probes of variation of the proton-to-electron mass ratio

Vibrational overtones in deeply bound molecules are sensitive probes for variation of the proton-to-electron mass ratio $μ$. In nonpolar molecules, these overtones may be driven as two-photon transitions. Here, we present procedures for experiments with ${\rm O}_2^+$, including state-preparation through photoionization, a two-photon probe, and detection. We calculate transition dipole moments between all $X\,^2Π_g$ vibrational levels and those of the $A\,^2Π_u$ excited electronic state. Using these dipole moments, we calculate two-photon transition rates and AC-Stark-shift systematics for the overtones. We estimate other systematic effects and statistical precision. Two-photon vibrational transitions in ${\rm O}_2^+$ provide multiple routes to improved searches for $μ$ variation.

physics.atom-ph↗