arXiv subjects

David DeMille

Publications and source records attributed to David DeMille.

At least 19 recordsLinked to original sources

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

Adiabatic passage of $^{205}$TlF with microwaves in a cryogenic beam

We present a hyperfine-resolved state preparation scheme for thallium fluoride (TlF) molecules based on microwave-driven adiabatic passage (AP) in a spatially varying electric field. This method enables efficient and robust population transfer between selected $\left|J,m_J=0\right\rangle$ hyperfine sublevels of the $X\,^1\Sigma^+_0$ ground state in a cryogenic molecular beam, a key requirement for the CeNTREX search for nuclear time-reversal symmetry violation. Two sequential stages of AP are implemented. The first transfers population from $J=0$ to $J=1$ at a local field of $173~\mathrm{V/cm}$, and the second transfers from $J=1$ to $J=2$ at $110~\mathrm{V/cm}$. Transfer efficiencies are quantified through laser-induced fluorescence, and accounting for residual population in excited rotational levels after a prior stage of rotational cooling. We achieve state transfer efficiencies of $0.92(6)$ and $1.05(5)$ for the first and second states of AP, respectively. This corresponds to a total efficiency of $0.97(8)$ for population transfer from $J=0$ to $J=2$. These results demonstrate robust and high-fidelity preparation of specific rotational/hyperfine states in TlF.

physics.atom-ph↗

arXiv2025

Simulated Laser Cooling and Magneto-Optical Trapping of Group IV Atoms

We present a scheme for laser cooling and magneto-optical trapping of the Group IV (a.k.a. Group 14 or tetrel) atoms silicon (Si), germanium (Ge), tin (Sn), and lead (Pb). These elements each possess a strong Type-II transition ($J \rightarrow J' = J-1$) between the metastable $s^2p^2 \,^3P_1$ state and the excited $s^2ps'\, ^3P_0^o$ state at an accessible laser wavelength, making them amenable to laser cooling and trapping. We focus on the application of this scheme to Sn, which has several features that make it attractive for precision measurement applications. We perform numerical simulations of atomic beam slowing, capture into a magneto-optical trap (MOT), and subsequent sub-Doppler cooling and compression in a blue-detuned MOT of Sn atoms. We also discuss a realistic experimental setup for realizing a high phase-space density sample of Sn atoms.

physics.atom-ph↗

arXiv2025

A magneto-optical trap of silver and potassium atoms

We demonstrate a dual magneto-optical trap of $^{109}$Ag and $^{39}$K. For silver, a decreasing-field Zeeman slower loads a MOT of $1.5{\times}10^8$ atoms at a temperature of 0.74(5) mK, with laser cooling occurring primarily on the $D_2$ line of $4d^{10}5s\; {}^2S_{1/2}\rightarrow 5p\; {}^2P_{3/2}$ at 328 nm. We create a novel Ag "dark spot MOT," where shelving the atoms in a dark state enhances the captured atom number by a factor of two and the lifetime by a factor of four. For potassium, we obtain $2{\times}10^8$ trapped atoms, and further cooling on the $D_1$ transition via grey molasses results in a cloud of $1.2{\times} 10^8$ atoms at 7(1) $\mu$K. We observe evidence of photoionization loss of the K MOT in the presence of Ag laser-cooling light, with implications for optimal dual species loading strategies. Our results on Ag point to simple and general laser cooling strategies for other coinage metals (Au, Cu). Furthermore, this work lays the foundation for the production of alkali-coinage metal degenerate quantum mixtures and highly polar molecules.

physics.atom-ph↗

arXiv2025

High-resolution spectroscopy of barium monofluoride: Odd isotopologues, hyperfine structure and isotope shifts

Barium monofluoride (BaF) is a promising molecular species for precision tests of fundamental symmetries and interactions. We present a combined theoretical and experimental study of BaF spectra and isotope shifts, focusing in particular on the poorly understood odd isotopologues 137BaF and 135BaF. By comparing state-of-the-art ab initio calculations with high-resolution fluorescence and absorption spectroscopy data, we provide a benchmark for electronic structure theory and disentangle the hyperfine and rovibrational spectra of the five most abundant isotopologues, from 138BaF to 134BaF. The comprehensive knowledge gained enables a King plot analysis of the isotope shifts that reveals the odd-even staggering of the barium nuclear charge radii. It also paths the way for improved laser cooling of rare BaF isotopologues and crucially supports future measurements of nuclear anapole and Schiff moments.

physics.atom-ph↗

arXiv2025

A cryogenic buffer gas beam source with in-situ ablation target replacement

The design and performance of a cryogenic buffer gas beam (CBGB) source with a load-lock system is presented. The ACME III electron electric dipole moment (eEDM) search experiment uses this source to produce a beam of cold, slow thorium monoxide (ThO) molecules. A key feature of the apparatus is its capability to replace ablation targets without interrupting vacuum or cryogenic conditions, increasing the average signal in the eEDM search. The source produces approximately $1.3 \times 10^{11}$ ground-state ThO molecules per pulse, with a rotational temperature of $4.8$ K, molecular beam solid angle of $0.31$ sr, and forward velocity of $200$ m/s. These parameters match the performance of traditional sources that require time-consuming thermal cycles for target replacement. A long-term yield improvement of about 40% is achieved when the load-lock system is used to replace targets biweekly.

physics.atom-ph↗

arXiv2025

Rotational-hyperfine cooling of $^{205}$TlF in a cryogenic beam

The aim of CeNTREX (Cold Molecule Nuclear Time-Reversal Experiment) is to search for time-reversal symmetry violation in the thallium nucleus, by measuring the Schiff moment of $^{205}$Tl in the polar molecule thallium fluoride (TlF). CeNTREX uses a cryogenic beam of TlF with a rotational temperature of 6.3(2) K. This results in population spread over dozens of rotational and hyperfine sublevels of TlF, while only a single level is useful for the Schiff moment measurement. Here we present a protocol for cooling the rotational and hyperfine degrees of freedom in the CeNTREX beam, transferring the majority of the Boltzmann distribution into a single rotational and hyperfine sublevel by using a single ultraviolet laser and a pair of microwave beams. We achieve a factor of $20.1(4)$ gain in the population of the $J=0$, $F=0$ hyperfine sublevel of the TlF ground state.

physics.atom-ph↗

arXiv2023

Electroweak Nuclear Properties from Single Molecular Ions in a Penning Trap

We present a novel technique to probe electroweak nuclear properties by measuring parity violation (PV) in single molecular ions in a Penning trap. The trap's strong magnetic field Zeeman shifts opposite-parity rotational and hyperfine molecular states into near degeneracy. The weak interaction-induced mixing between these degenerate states can be larger than in atoms by more than twelve orders of magnitude, thereby vastly amplifying PV effects. The single molecule sensitivity would be suitable for applications to nuclei across the nuclear chart, including rare and unstable nuclei.

physics.atom-ph↗

arXiv2023

High density loading and collisional loss of laser cooled molecules in an optical trap

We report optical trapping of laser-cooled molecules at sufficient density to observe molecule-molecule collisions for the first time in a bulk gas. SrF molecules from a red-detuned magneto-optical trap (MOT) are compressed and cooled in a blue-detuned MOT. Roughly 30% of these molecules are loaded into an optical dipole trap with peak number density $n_0 \approx 3\times 10^{10} \text{ cm}^{-3}$ and temperature $T\approx40$ $\mu$K. We observe two-body loss with rate coefficient $\beta = 2.7^{+1.2}_{-0.8}\times 10^{-10} \text{ cm}^3 \text{ s}^{-1}$. Achieving this density and temperature opens a path to evaporative cooling towards quantum degeneracy of laser-cooled molecules.

physics.atom-ph↗

arXiv2023

Opportunities for Fundamental Physics Research with Radioactive Molecules

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this manuscript, we review the scientific case for studying radioactive molecules, discuss recent atomic, molecular, nuclear, astrophysical, and chemical advances which provide the foundation for their study, describe the facilities where these species are and will be produced, and provide an outlook for the future of this nascent field.

nucl-ex↗

arXiv2022

Using parity-nonconserving spin-spin coupling to measure the Tl nuclear anapole moment in a TlF molecular beam

An experiment utilizing a TlF molecular beam is being developed by the CeNTREX collaboration to search for hadronic interactions that violate both time-reversal (T) and parity (P) invariance. Here we propose to use the same beam to look for a T-invariance conserving but P-nonconserving (PNC) effect induced by the anapole moment of the Tl nucleus, via a vector coupling of the two nuclear spins in TlF. To measure the nuclear anapole moment, the dc electric and magnetic fields in CeNTREX are replaced by rf fields resonant with a nuclear spin flip transition. We adapt the relativistic coupled cluster method in a combination with relativistic density functional theory for the calculation of the molecular PNC spin-spin vector coupling constant that links the experimental signal with the anapole moment. The value of the P-conserving spin-spin coupling constant calculated within the same approach is found to be in good agreement with available experimental data.

physics.atom-ph↗

arXiv2022

Towards improved loading, cooling, and trapping of molecules in magneto-optical traps

Recent experiments have demonstrated direct cooling and trapping of diatomic and triatomic molecules in magneto-optical traps (MOTs). However, even the best molecular MOTs to date still have density $10^{-5}$ times smaller than in typical atomic MOTs. The main limiting factors are: (i) inefficiencies in slowing molecules to velocities low enough to be captured by the MOT, (ii) low MOT capture velocities, and (iii) limits on density within the MOT resulting from sub-Doppler heating~[J. A. Devlin and M. R. Tarbutt, Phys. Rev. A \textbf{90}, 063415 (2018)]. All of these are consequences of the need to drive `Type-II' optical cycling transitions, where dark states appear in Zeeman sublevels, in order to avoid rotational branching. We present simulations demonstrating ways to mitigate each of these limitations. This should pave the way towards loading molecules into conservative traps with sufficiently high density and number to evaporatively cool them to quantum degeneracy.

physics.atom-ph↗

arXiv2022

Electrostatic focusing of cold and heavy molecules for the ACME electron EDM search

The current best upper limit for electron electric dipole moment (EDM), $|d_e|<1.1\times10^{-29}\,$e$\cdot$cm ($90$% confidence), was set by the ACME collaboration in 2018. The ACME experiment uses a spin-precession measurement in a cold beam of ThO molecules to detect $d_e$. An improvement in statistical uncertainty would be possible with more efficient use of molecules from the cryogenic buffer gas beam source. Here, we demonstrate electrostatic focusing of the ThO beam with a hexapole lens. This results in a factor of $16$ enhancement in the molecular flux detectable downstream, in a beamline similar to that built for the next generation of ACME. We also demonstrate an upgraded rotational cooling scheme that increases the ground state population by $3.5$ times compared to no cooling, consistent with expectations and a factor of $1.4$ larger than previously in ACME. When combined with other demonstrated improvements, we project over an order of magnitude improvement in statistical sensitivity for the next generation ACME electron EDM search.

physics.atom-ph↗

arXiv2022

Measurement of the H$^3Δ_1$ Radiative Lifetime in ThO

The best limit on the electron electric dipole moment (eEDM) comes from the ACME II experiment [Nature \textbf{562} (2018), 355-360] which probes physics beyond the Standard Model at energy scales well above 1 TeV. ACME II measured the eEDM by monitoring electron spin precession in a cold beam of the metastable H$^3Δ_1$ state of thorium monoxide (ThO) molecules, with an observation time $τ\approx 1$ ms for each molecule. We report here a new measurement of the lifetime of the ThO (H$^3Δ_1$) state, $τ_H = 4.2\pm 0.5$ ms. Using an apparatus within which $τ\approx τ_H$ will enable a substantial reduction in uncertainty of an eEDM measurement.

physics.atom-ph↗

arXiv2022

Electric dipole moments and the search for new physics

Static electric dipole moments of nondegenerate systems probe mass scales for physics beyond the Standard Model well beyond those reached directly at high energy colliders. Discrimination between different physics models, however, requires complementary searches in atomic-molecular-and-optical, nuclear and particle physics. In this report, we discuss the current status and prospects in the near future for a compelling suite of such experiments, along with developments needed in the encompassing theoretical framework.

hep-ph↗

arXiv2021

Theoretical Aspects of Radium-Containing Molecules Amenable to Assembly from Laser-Cooled Atoms for New Physics Searches

We explore the possibilities for a next-generation electron-electric-dipole-moment experiment using ultracold heteronuclear diatomic molecules assembled from a combination of radium and another laser-coolable atom. In particular, we calculate their ground state structure and their sensitivity to parity- and time-reversal (${\cal{P,T}}$) violating physics arising from flavor-diagonal charge-parity (${\cal{CP}}$) violation. Among these species, the largest ${\cal{P,T}}$-violating molecular interaction constants -- associated for example with the electron electric dipole moment -- are obtained for the combination of radium (Ra) and silver (Ag) atoms. A mechanism for explaining this finding is proposed. We go on to discuss the prospects for an electron EDM search using ultracold, assembled, optically trapped RaAg molecules, and argue that this system is particularly promising for rapid future progress in the search for new sources of ${\cal{CP}}$ violation.

physics.atom-ph↗

arXiv2021

Frequency-doubled Nd:YAG MOPA laser system with programmable rectangular pulses up to 200 microseconds

A compact frequency-doubled diode-pumped Nd:YAG master-oscillator power-amplifier laser system with programmable microsecond pulse length has been developed. Analog pulse shaping of the output from a single-frequency continuous-wave Nd:YAG oscillator, and subsequent amplification, allowed the generation of rectangular pulses with pulse lengths on the order of the Nd:YAG fluorescence lifetime. Temporally flat-top pulses of 1064 nm light with 520 mJ pulse energy, 2.6 kW peak power, and 200 $μ$s duration, with linewidth below 10 kHz, were obtained at a repetition rate of 2 Hz. Second harmonic generation in a LBO crystal yielded pulses of 262 mJ and 1.3 kW peak power at 532 nm. The peak power can be maintained within 2.9% over the duration of the laser pulse, and long-term intensity stability of 1.1% was observed. The spatially flat-top beam at 1064 nm used in the amplifier is converted to a Gaussian beam at 532 nm with beam quality factor $M^2=1.41(14)$ during the second harmonic generation. This system has potential as a pump source for Ti:sapphire, dye, or optical parametric amplifiers to generate tunable high-power single-frequency radiation for applications in precision measurements and laser slowing.

physics.optics↗

arXiv2021

Polarization Enhanced Deep Optical Dipole Trapping of $Λ$-cooled Polar Molecules

We demonstrate loading of SrF molecules into an optical dipole trap (ODT) via in-trap $Λ$-cooling. We find that this cooling can be optimized by a proper choice of relative ODT and $Λ$ beam polarizations. In this optimized configuration, we observe molecules with temperatures as low as 14(1) $μ$K in traps with depths up to 570 $μ$K. With optimized parameters, we transfer $\!\sim\!5$% of molecules from our radio-frequency magneto-optical trap into the ODT, at a density of $\sim\!2\times 10^{9}$ cm$^{-3}$, a phase space density of $\sim\!2\times 10^{-7}$, and with a trap lifetime of $\!\sim\!1$ s.

physics.atom-ph↗