arXiv subjects

Arian Jadbabaie

Publications and source records attributed to Arian Jadbabaie.

15 recordsLinked to original sources

arXiv2026

Probing $P,T$-Symmetry Violation with Optically Trapped Asymmetric Top Molecules

Searches for $P,T$-violating electromagnetic moments are among the most sensitive probes of physics beyond the Standard Model. Extending beyond current limits will benefit from molecules with fully controllable orientation at low electric fields, long coherence times, and laser coolability---all offered by asymmetric top molecules (ATMs). Exploiting the intrinsic rotational $K$-doubling in ATMs and the associated long-lived ($T_1 \gtrsim 10$ s) parity doublets afforded by $C_{2v}$ symmetry and nuclear-spin statistics, these species combine large electric polarizability with long coherence times in modest laboratory fields. We study alkaline-earth(-like) monoamides, $\mathcal{M}$--NH$_2$ ($\mathcal{M}$ = Ca, Sr, Ba, Yb, Ra), which possess favorable electronic structure for laser cooling. We perform \textit{ab initio} calculations of fine and hyperfine constants, identifying the importance of relativistic effects in the spin-rotation tensor. An effective Hamiltonian then models the rotational and hyperfine structure of the vibronic ground state, quantifying electron electric dipole moment (EDM) sensitivities and identifying feasible measurement schemes. We compute the effect of external fields and identify engineered clock transitions that suppress sensitivity to external perturbations while retaining strong EDM sensitivity, and characterize the magic trapping conditions that null differential light shifts in an optical trap. Under these conditions we project a statistical electron-EDM sensitivity over an order of magnitude beyond current best experimental limits, with further gains available from increased molecule number and coherence time. Our results establish asymmetric top molecules as a tunable platform for sensitive symmetry-violation measurements with long coherence times.

physics.atom-ph↗

arXiv2026

Production and spectroscopy of cold radioactive molecules

Molecules with heavy, radioactive nuclei promise extreme sensitivity to fundamental nuclear and particle physics. However, these nuclei are available in limited quantities, which challenges their use in precision measurements. Here we demonstrate the gas-phase synthesis, cryogenic cooling, and high-resolution laser spectroscopy of radium monohydroxide, monodeuteroxide, and monofluoride molecules ($^{226}$RaOH, $^{226}$RaOD, and $^{226}$RaF) in a tabletop apparatus by combining novel radioactive target production protocols, optically driven chemistry in a cryogenic buffer gas, and low-background spectroscopic detection methods. The molecules are cooled in the lab frame, creating conditions that are the same starting points as many current molecular precision measurement and quantum information experiments. This approach is readily applied to a wide range of species and establishes key capabilities for molecular quantum sensing of exotic nuclei.

physics.atom-ph↗

arXiv2026

Design and Performance of a Heated Gas Injector for Producing Cold Molecular Beams

We realize an injector device that supplies warm gas directly into a cryogenic environment. This injector has several advantageous features, including robustness, rigidity, simple installation, and excellent thermal isolation between a hot ($\sim$300 K) copper fill line and a cold ($<$3 K) cryogenic buffer gas cell. Less than 200 mW heat load on the cell is observed in realistic conditions of a molecular precision measurement experiment. A polyamide-imide (PAI) tube is the essential design feature. The fill line is epoxied to one end of the tube while the other end of the tube is connected to the cell via a slip-fit onto a brass nipple, realizing a complete vacuum-tight seal. PAI contracts on the brass nipple when cooled, forming a cryogenic leak-tight seal. The injector is easily (de-)mountable and rigid, with no significant displacement of the fill line relative to the cell observed during cooldown to 4 K. We characterize injector performance by flowing into the cell $\text{SF}_6$ through the hot fill line and cold $\text{He}$ buffer gas through a separate cryogenic fill line while laser ablating a barium-containing target. This produces cold BaF free radicals, detected using absorption spectroscopy. This injector design will be employed to laser cool radium-containing molecules, such as $\text{RaF}$ and $\text{RaOH}$, where leak-tight delivery of $\text{SF}_6$ and $\text{H}_2\text{O}$ reagents into a cryogenic buffer gas cell is required for scientific and safety reasons. These molecules are of particular interest for the study of symmetry-violating nuclear properties and searches for physics beyond the Standard Model.

physics.atom-ph↗

arXiv2026

Non-destructive cavity readout of molecules for precision measurements

We propose a non-destructive method to measure the population of molecules in a selected rotational-hyperfine state by coupling them to a high-finesse optical cavity. In contrast to traditional techniques, our approach enables fast (less than 1 ms) repeated measurements with reduced heating and losses, and with precision below the standard quantum limit. The method is particularly advantageous for radioactive molecules, systems of high interest for symmetry violation searches, for which production and sample size are limited, and repeated interrogation is essential for improved sensitivity.

physics.atom-ph↗

arXiv2025

Engineered Molecular Clock Transitions for Symmetry Violation Searches

Heavy polar molecules are sensitive probes of physics Beyond the Standard Model. However, uncontrolled external electromagnetic fields pose challenges to achieving precise and accurate measurements. Minimizing susceptibility to these fields is therefore critical and has played an important role in all precision experiments of this type. Here we devise and demonstrate clock transitions engineered to realize robust symmetry violation searches in the polyatomic molecule YbOH. Sensitivities to external fields can be suppressed by orders-of-magnitude while preserving high sensitivity to the electron electric dipole moment (eEDM). We perform Ramsey measurements on these clock transitions and observe suppression of electric and magnetic sensitivities by at least a factor of 700 and 200, respectively, and demonstrate the robustness of their spin coherence against large electromagnetic field fluctuations. We further identify and employ selected quantum states to make sensitive measurements of external magnetic and electric fields, another critical feature for highly accurate measurements. This approach of molecular engineering is broadly applicable to diverse molecular species and states, including those with complex nuclei and those that are compatible with state-of-the-art cooling and trapping techniques, thereby offering the potential to significantly improve experimental sensitivity to a wide range of New Physics while expanding the chemical design space for molecular quantum science.

physics.atom-ph↗

arXiv2025

Prospects for measuring the electron's electric dipole moment with polyatomic molecules in an optical lattice

We present the conceptual design of an experiment to measure the electron's electric dipole moment (eEDM) using $^{138}$BaOH molecules in an optical lattice. The BaOH molecule is laser-coolable and highly sensitive to the eEDM, making it an attractive candidate for such a precision measurement, and capturing it in an optical lattice offers potentially very long coherence times. We study possibilities and limitations of this approach, identify the most crucial limiting factors and ways to overcome them. The proposed apparatus can reach a statistical error of $10^{-30}\,e\,$cm by measuring spin precession on a total number of $5 \times 10^9$ molecules over a span of 120 days.

physics.atom-ph↗

arXiv2023

Engineering field-insensitive molecular clock transitions for symmetry violation searches

Molecules are a powerful platform to probe fundamental symmetry violations beyond the Standard Model, as they offer both large amplification factors and robustness against systematic errors. As experimental sensitivities improve, it is important to develop new methods to suppress sensitivity to external electromagnetic fields, as limits on the ability to control these fields are a major experimental concern. Here we show that sensitivity to both external magnetic and electric fields can be simultaneously suppressed using engineered radio frequency, microwave, or two-photon transitions that maintain large amplification of CP-violating effects. By performing a clock measurement on these transitions, CP-violating observables including the electron electric dipole moment, nuclear Schiff moment, and magnetic quadrupole moment can be measured with suppression of external field sensitivity of $\gtrsim$100 generically, and even more in many cases. Furthermore, the method is compatible with traditional Ramsey measurements, offers internal co-magnetometry, and is useful for systems with large angular momentum commonly present in molecular searches for nuclear CP-violation.

physics.atom-ph↗

arXiv2023

Quantum-Enhanced Metrology for Molecular Symmetry Violation using Decoherence-Free Subspaces

We propose a method to measure time-reversal symmetry violation in molecules that overcomes the standard quantum limit while leveraging decoherence-free subspaces to mitigate sensitivity to classical noise. The protocol does not require an external electric field, and the entangled states have no first-order sensitivity to static electromagnetic fields as they involve superpositions with zero average lab-frame projection of spins and dipoles. This protocol can be applied with trapped neutral or ionic species, and can be implemented using methods which have been demonstrated experimentally.

physics.atom-ph↗

arXiv2023

Optical cycling in polyatomic molecules with complex hyperfine structure

We have developed and demonstrated a scheme to achieve rotationally-closed photon cycling in polyatomic molecules with complex hyperfine structure and sensitivity to hadronic symmetry violation, specifically $^{171}$YbOH and $^{173}$YbOH. We calculate rotational branching ratios for spontaneous decay and identify repumping schemes which use electro-optical modulators (EOMs) to address the hyperfine structure. We demonstrate our scheme by cycling photons in a molecular beam and verify that we have achieved rotationally-closed cycling by measuring optical pumping into unaddressed vibrational states. Our work makes progress along the path toward utilizing photon cycling for state preparation, readout, and laser cooling in precision measurements of polyatomic molecules with complex hyperfine structure.

physics.atom-ph↗

arXiv2023

Direct measurement of high-lying vibrational repumping transitions for molecular laser cooling

Molecular laser cooling and trapping requires addressing all spontaneous decays to excited vibrational states that occur at the $\gtrsim 10^{-4} - 10^{-5}$ level, which is accomplished by driving repumping transitions out of these states. However, the transitions must first be identified spectroscopically at high-resolution. A typical approach is to prepare molecules in excited vibrational states via optical cycling and pumping, which requires multiple high-power lasers. Here, we demonstrate a general method to perform this spectroscopy without the need for optical cycling. We produce molecules in excited vibrational states by using optically-driven chemical reactions in a cryogenic buffer gas cell, and implement frequency-modulated absorption to perform direct, sensitive, high-resolution spectroscopy. We demonstrate this technique by measuring the spectrum of the $\tilde{A}^2Π_{1/2}(1,0,0)-\tilde{X}^2Σ^+(3,0,0)$ band in $^{174}$YbOH. We identify the specific vibrational repump transitions needed for photon cycling, and combine our data with previous measurements of the $\tilde{A}^2Π_{1/2}(1,0,0)-\tilde{X}^2Σ^+(0,0,0)$ band to determine all of the relevant spectral constants of the $\tilde{X}^2Σ^+(3,0,0)$ state. This technique achieves high signal-to-noise, can be further improved to measure increasingly high-lying vibrational states, and is applicable to other molecular species favorable for laser cooling.

physics.atom-ph↗

arXiv2023

Quantum Control of Trapped Polyatomic Molecules for eEDM Searches

Ultracold polyatomic molecules are promising candidates for experiments in quantum science, quantum sensing, ultracold chemistry, and precision measurements of physics beyond the Standard Model. A key, yet unrealized, requirement of these experiments is the ability to achieve full quantum control over the complex internal structure of the molecules. Here, we establish coherent control of individual quantum states in a polyatomic molecule, calcium monohydroxide (CaOH), and use these techniques to demonstrate a method for searching for the electron electric dipole moment (eEDM). Optically trapped, ultracold CaOH molecules are prepared in a single quantum state, polarized in an electric field, and coherently transferred into an eEDM sensitive state where an electron spin precession measurement is performed. To extend the coherence time of the measurement, we utilize eEDM sensitive states with tunable, near-zero magnetic field sensitivity. The spin precession coherence time is limited by AC Stark shifts and uncontrolled magnetic fields. These results establish a path for eEDM searches with trapped polyatomic molecules, towards orders-of-magnitude improved experimental sensitivity to time-reversal-violating physics.

physics.atom-ph↗

arXiv2023

Characterizing the Fundamental Bending Vibration of a Linear Polyatomic Molecule for Symmetry Violation Searches

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 $\tilde{X} {}^2Σ^+ (010)$ state arising from the bending vibration, both features that can greatly aid BSM searches. Understanding the $\tilde{X} {}^2Σ^+ (010)$ state is a crucial prerequisite to precision measurements with linear polyatomic molecules. Here, we characterize fundamental bending vibration of ${}^{174}$YbOH using high-resolution optical spectroscopy on the nominally forbidden $\tilde{X} {}^2Σ^+ (010) \rightarrow \tilde{A} {}^2Π_{1/2} (000)$ transition at 588 nm. We assign 39 transitions originating from the lowest rotational levels of the $\tilde{X} {}^2Σ^+ (010)$ 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 $\tilde{X} {}^2Σ^+ (010)$ state and fit the molecule-frame dipole moment to $D_\mathrm{mol}=2.16(1)$ D and the effective electron $g$-factor to $g_S=2.07(2)$. 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 $\tilde{A} {}^2Π_{1/2} (000)$ state. Our work is an essential step toward searches for BSM physics in YbOH and other linear polyatomic molecules.

physics.atom-ph↗

arXiv2021

Fine and hyperfine interactions in $^{171}$YbOH and $^{173}$YbOH

The odd isotopologues of ytterbium monohydroxide, $^{171,173}$YbOH, have been identified as promising molecules in which to measure parity (P) and time reversal (T) violating physics. Here we characterize the $\tilde{A}^{2}Π_{1/2}(0,0,0)-\tilde{X}^2Σ^+(0,0,0)$ band near 577 nm for these odd isotopologues. Both laser-induced fluorescence (LIF) excitation spectra of a supersonic molecular beam sample and absorption spectra of a cryogenic buffer-gas cooled sample were recorded. Additionally, a novel spectroscopic technique based on laser-enhanced chemical reactions is demonstrated and utilized in the absorption measurements. This technique is especially powerful for disentangling congested spectra. An effective Hamiltonian model is used to extract the fine and hyperfine parameters for the $\tilde{A}^{2}Π_{1/2}(0,0,0)$ and $\tilde{X}^2Σ^+(0,0,0)$ states. A comparison of the determined $\tilde{X}^2Σ^+(0,0,0)$ hyperfine parameters with recently predicted values (M. Denis, et al., J. Chem. Phys. $\bf{152}$, 084303 (2020), K. Gaul and R. Berger, Phys. Rev. A $\bf{101}$, 012508 (2020), J. Liu et al., J. Chem. Phys. $\bf{154}$, 064110 (2021)) is made. The measured hyperfine parameters provide experimental confirmation of the computational methods used to compute the P,T-violating coupling constants $W_d$ and $W_M$, which correlate P,T-violating physics to P,T-violating energy shifts in the molecule. The dependence of the fine and hyperfine parameters of the $\tilde{A}^{2}Π_{1/2}(0,0,0)$ and $\tilde{X}^2Σ^+(0,0,0)$ states for all isotopologues of YbOH are discussed and a comparison to isoelectronic YbF is made.

physics.atom-ph↗

arXiv2019

Enhanced Yield from a Cryogenic Buffer Gas Beam Source via Excited State Chemistry

We use narrow-band laser excitation of Yb to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the Standard Model (BSM). By exciting atomic Yb to the metastable $^3$P$_1$ state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment (eEDM) and nuclear magnetic quadrupole moment (NMQM) experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment. Additionally, our calculations compare reaction pathways of Yb($^3$P) with the reactants H$_2$O and H$_2$O$_2$. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics.

physics.atom-ph↗

arXiv2018

A large-diameter cryogenic rotation stage for half-wave plate polarization modulation on the POLARBEAR-2 experiment

We describe the design of a cryogenic rotation stage (CRS) for use with the cryogenic half-wave plate (CHWP) polarization modulator on the POLARBEAR-2b and POLARBEAR-2c (PB2b/c) cosmic microwave background (CMB) experiments, the second and third installments of the Simons Array. Rapid modulation of the CMB polarization signal using a CHWP suppresses 1/f contamination due to atmospheric turbulence and allows a single polarimeter to measure both polarization states, mitigating systematic effects that arise when differencing orthogonal detectors. To modulate the full detector array while avoiding excess photon loading due to thermal emission, the CHWP must have a clear-aperture diameter of > 450 mm and be cooled to < 100 K. We have designed a 454-mm-clear-aperture, < 65 K CRS using a superconducting magnetic bearing driven by a synchronous magnetic motor. We present the specifications for the CRS, its interfacing to the PB2b/c receiver cryostat, its performance in a stand-alone test, and plans for future work.

astro-ph.IM↗