arXiv subjects

Matthew D. Frye

Publications and source records attributed to Matthew D. Frye.

At least 19 recordsLinked to original sources

arXiv2024

Quantum control of ion-atom collisions beyond the ultracold regime

Tunable scattering resonances are crucial for controlling atomic and molecular systems. However, their use has so far been limited to ultracold temperatures. These conditions remain hard to achieve for most hybrid trapped ion-atom systems -- a prospective platform for quantum technologies and fundamental research. Here we measure inelastic collision probabilities for ${\text{Sr}^++\text{Rb}}$ and use them to calibrate a comprehensive theoretical model of ion-atom collisions. Our theoretical results, compared with experimental observations, confirm that quantum interference effects persist to the multiple-partial-wave regime, leading to the pronounced state and mass dependence of the collision rates. Using our model, we go beyond interference and identify a rich spectrum of Feshbach resonances at moderate magnetic fields with the Rb atom in its lower ($f=1$) hyperfine state, which persist at temperatures as high as 1 mK. Future observation of these predicted resonances should allow precise control of the short-range dynamics in ${\text{Sr}^+}+{\text{Rb}}$ collisions under unprecedentedly warm conditions.

physics.atom-ph↗

arXiv2024

Interactions and cold collisions of AlF in the ground and excited electronic states with He

Aluminium monofluoride (AlF) is a promising candidate for laser cooling and the production of dense ultracold molecular gases, thanks to its relatively high chemical stability and diagonal Frank-Condon factors. In this study, we examine the interactions and collisions of AlF in its $X^1\Sigma^+$, $a^3\Pi$, and $A^{1}\Pi$ electronic states with ground-state He using state-of-the-art \textit{ab initio} quantum chemistry techniques. We construct accurate potential energy surfaces (PESs) employing either the explicitly correlated coupled-cluster CCSD(T)-F12 method augmented by the CCSDT correction or the multireference configuration-interaction method for higher-excited electronic states. Subsequently, we employ these PESs in coupled-channel calculations to determine the scattering cross-sections for AlF+He collisions and bound states of the complex. We estimate the uncertainty of the calculated PESs and apply it to assess the uncertainty of the scattering results. We find a relatively low sensitivity of the cross-sections to the variation of the PESs, but the positions of shape resonances remain uncertain. The present results are relevant for further improvements and optimizations of buffer-gas cooling of AlF molecules.

physics.chem-ph↗

arXiv2024

Bose-Einstein condensation of non-ground-state caesium atoms

Bose-Einstein condensates of ultracold atoms serve as low-entropy sources for a multitude of quantum-science applications, ranging from quantum simulation and quantum many-body physics to proof-of-principle experiments in quantum metrology and quantum computing. For stability reasons, in the majority of cases the energetically lowest-lying atomic spin state is used. Here we report the Bose-Einstein condensation of caesium atoms in the Zeeman-excited mf = 2 state, realizing a non-ground-state Bose-Einstein condensate with tunable interactions and tunable loss. We identify two regions of magnetic field in which the two-body relaxation rate is low enough that condensation is possible. We characterize the phase transition and quantify the loss processes, finding unusually high three-body losses in one of the two regions. Our results open up new possibilities for the mixing of quantum-degenerate gases, for polaron and impurity physics, and in particular for the study of impurity transport in strongly correlated one-dimensional quantum wires.

cond-mat.quant-gas↗

arXiv2024

Collisions of Spin-polarized YO Molecules for Single Partial Waves

Efficient sub-Doppler laser cooling and optical trapping of YO molecules offer new opportunities to study collisional dynamics in the quantum regime. Confined in a crossed optical dipole trap, we achieve the highest phase-space density of $2.5 \times 10^{-5}$ for a bulk laser-cooled molecular sample. This sets the stage to study YO--YO collisions in the microkelvin temperature regime, and reveal state-dependent, single-partial-wave two-body collisional loss rates. We determine the partial-wave contributions to loss of specific rotational states (first excited $N=1$ and ground $N=0$) following two strategies. First, we measure the change of the collision rate in a spin mixture of $N=1$ by tuning the kinetic energy with respect to the p- and d-wave centrifugal barriers. Second, we compare loss rates between a spin mixture and a spin-polarized state in $N=0$. Using quantum defect theory with a partially absorbing boundary condition at short range, we show that the dependence on temperature for $N=1$ can be reproduced in the presence of a d-wave or f-wave resonance, and the dependence on a spin mixture for $N=0$ with a p-wave resonance.

physics.atom-ph↗

arXiv2024

Spin--spin interaction and magnetic Feshbach resonances in collisions of high-spin atoms with closed-shell atoms

We investigate interactions and ultracold collisions of high-spin but spherical atoms with closed-shell atoms, focussing on the example of Cr with Yb. Such a combination has only one potential energy curve but gives rise to a substantial intra-atomic spin--spin interaction, which causes Feshbach resonances due to rotationally excited states. We find such resonances are guaranteed below 250 G and can reach widths of 10s of G in favorable circumstances. We study the effect of hyperfine structure, which can create additional wide resonances at low fields. Finally, we consider isotopic substitution and show that for any realistic potential it is very likely at least one combination of commonly used isotopes will have resonances with experimentally favorable properties. Thus, this is a promising system for both molecule formation and studying quantum mixtures including dipolar species.

physics.atom-ph↗

arXiv2023

Shielding collisions of ultracold CaF molecules with static electric fields

We study collisions of ultracold CaF molecules in strong static electric fields. These fields allow the creation of long-range barriers in the interaction potential, effectively preventing the molecules from reaching the short-range region where inelastic and other loss processes are likely to occur. We carry out coupled-channel calculations of rate coefficients for elastic scattering and loss. We develop an efficient procedure for including energetically well-separated rotor functions in the basis set via a Van Vleck transformation. We show that shielding is particularly efficient for CaF and allows the rate of two-body loss processes to be reduced by a factor of $10^7$ or more at a field of 23 kV/cm. The loss rates remain low over a substantial range of fields. Electron and nuclear spins cause strong additional loss in some small ranges of field, but have little effect elsewhere. These results pave the way for evaporative cooling of CaF towards quantum degeneracy.

quant-ph↗

arXiv2023

Long-range states and Feshbach resonances in collisions between ultracold alkali-metal diatomic molecules and atoms

We consider the long-range states expected for complexes formed from an alkali-metal diatomic molecule in a singlet state and an alkali-metal atom. We explore the structure of the Hamiltonian for such systems, and the couplings between the six angular momenta that are present. We consider the patterns and densities of the long-range states, and the terms in the Hamiltonian that can cause Feshbach resonances when the states cross threshold as a function of magnetic field. We present a case study of $^{40}$K$^{87}$Rb+$^{87}$Rb. We show multiple types of resonance due to long-range states with rotational and/or hyperfine excitation, and consider the likelihood of them existing at low to moderate magnetic fields.

physics.atom-ph↗

arXiv2023

Magnetic Feshbach resonances between atoms in $^2$S and $^3$P$_0$ states: mechanisms and dependence on atomic properties

Magnetically tunable Feshbach resonances exist in ultracold collisions between atoms in $^2$S and $^3$P$_0$ states, such as an alkali-metal atom colliding with Yb or Sr in a clock state. We investigate the mechanisms of these resonances and identify the terms in the collision Hamiltonian responsible for them. They involve indirect coupling between the open and closed channels, via intermediate channels involving atoms in $^3$P$_1$ states. The resonance widths are generally proportional to the square of the magnetic field and are strongly enhanced when the magnitude of the background scattering length is large. For any given pair of atoms, the scattering length can be tuned discretely by choosing different isotopes of the $^3$P$_0$ atom. For each combination of an alkali-metal atom and either Yb or Sr, we consider the prospects of finding an isotopic combination that has both a large background scattering length and resonances at high but experimentally accessible field. We conclude that $^{87}$Rb+Yb, Cs+Yb and $^{85}$Rb+Sr are particularly promising combinations.

physics.atom-ph↗

arXiv2022

Observation of magnetic Feshbach resonances between Cs and ${}^{173}$Yb

We report the first observation of magnetic Feshbach resonances between ${}^{173}$Yb and $^{133}$Cs. In a mixture of Cs atoms prepared in the $(f=3, m_f=3)$ state and unpolarized fermionic ${}^{173}$Yb we observe resonant atom loss due to two sets of magnetic Feshbach resonances around 622~G and 702~G. Resonances for individual Yb nuclear spin components $m_{i,\mathrm{Yb}}$ are split by its interaction with the Cs electronic spin, which also provides the main coupling mechanism for the observed resonances. The observed splittings and relative resonance strengths are in good agreement with theoretical predictions from coupled-channel calculations.

physics.atom-ph↗

arXiv2022

Feshbach resonances and molecule formation in ultracold mixtures of Rb and Yb($^3$P) atoms

We have investigated magnetically tunable Feshbach resonances in ultracold collisions of Rb with Yb in its metastable $^3$P$_2$ and $^3$P$_0$ states, using coupled-channel scattering and bound-state calculations. For the $^3$P$_2$ state, we find sharp resonances when both atoms are in their lowest Zeeman sublevels. However, these resonances are decayed by inelastic processes that produce Yb atoms in $^3$P$_1$ and $^3$P$_0$ states. The molecules that might be produced by magnetoassociation at the $^3$P$_2$ thresholds can decay by similar pathways and would have lifetimes no more than a few microseconds. For the $^3$P$_0$ state, by contrast, there are resonances that are promising for magnetoassociation. There are resonances due to both rotating and non-rotating molecular states that are significantly stronger than the analogous resonances for Yb($^1$S). The ones due to rotating states are denser in magnetic field; in contrast to Yb($^1$S), they exist even for bosonic isotopes of Yb($^3$P$_0$).

physics.atom-ph↗

arXiv2021

Magnetic Feshbach resonances in collisions of $^{23}$Na$^{40}$K with $^{40}$K

We present measurements of more than 80 magnetic Feshbach resonances in collisions of ultracold $^{23}$Na$^{40}$K with $^{40}$K. We assign quantum numbers to a group of low-field resonances and show that they are due to long-range states of the triatomic complex in which the quantum numbers of the separated atom and molecule are approximately preserved. The resonant states are not members of chaotic bath of short-range states. Similar resonances are expected to be a common feature of alkali-metal diatom + atom systems.

physics.atom-ph↗

arXiv2021

Complexes formed in collisions between ultracold alkali-metal diatomic molecules and atoms

We explore the properties of 3-atom complexes of alkali-metal diatomic molecules with alkali-metal atoms, which may be formed in ultracold collisions. We estimate the densities of vibrational states at the energy of atom-diatom collisions, and find values ranging from 2.2 to 350~K$^{-1}$. However, this density does not account for electronic near-degeneracy or electron and nuclear spins. We consider the fine and hyperfine structure expected for such complexes. The Fermi contact interaction between electron and nuclear spins can cause spin exchange between atomic and molecular spins. It can drive inelastic collisions, with resonances of three distinct types, each with a characteristic width and peak height in the inelastic rate coefficient. Some of these resonances are broad enough to overlap and produce a background loss rate that is approximately proportional to the number of outgoing inelastic channels. Spin exchange can increase the density of states from which laser-induced loss may occur.

physics.atom-ph↗

arXiv2021

Molecule-molecule and atom-molecule collisions with ultracold RbCs molecules

Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes or to laser-free decay pathways. For atom-molecule mixtures, RbCs+Rb and RbCs+Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom-molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.

physics.atom-ph↗

arXiv2021

Collisions in a dual-species magneto-optical trap of molecules and atoms

We study inelastic collisions between CaF molecules and $^{87}$Rb atoms in a dual-species magneto-optical trap. The presence of atoms increases the loss rate of molecules from the trap. By measuring the loss rates and density distributions, we determine a collisional loss rate coefficient $k_{2} = (1.43 \pm 0.29) \times 10^{-10}$ cm$^{3}$/s at a temperature of 2.4 mK. We show that this is not substantially changed by light-induced collisions or by varying the populations of excited-state atoms and molecules. The observed loss rate is close to the universal rate expected in the presence of fast loss at short range, and can be explained by rotation-changing collisions in the ground electronic state.

physics.atom-ph↗

arXiv2021

Collisions Between Ultracold Molecules and Atoms in a Magnetic Trap

We prepare mixtures of ultracold CaF molecules and Rb atoms in a magnetic trap and study their inelastic collisions. When the atoms are prepared in the spin-stretched state and the molecules in the spin-stretched component of the first rotationally excited state, they collide inelastically with a rate coefficient of $k_2 = (6.6 \pm 1.5) \times 10^{-11}$ cm$^{3}$/s at temperatures near 100~$μ$K. We attribute this to rotation-changing collisions. When the molecules are in the ground rotational state we see no inelastic loss and set an upper bound on the spin relaxation rate coefficient of $k_2 < 5.8 \times 10^{-12}$ cm$^{3}$/s with 95% confidence. We compare these measurements to the results of a single-channel loss model based on quantum defect theory. The comparison suggests a short-range loss parameter close to unity for rotationally excited molecules, but below 0.04 for molecules in the rotational ground state.

physics.atom-ph↗

arXiv2020

Observation of Efimov Universality across a Non-Universal Feshbach Resonance in \textsuperscript{39}K

We study three-atom inelastic scattering in ultracold \textsuperscript{39}K near a Feshbach resonance of intermediate coupling strength. The non-universal character of such resonance leads to an abnormally large Efimov absolute length scale and a relatively small effective range $r_e$, allowing the features of the \textsuperscript{39}K Efimov spectrum to be better isolated from the short-range physics. Meticulous characterization of and correction for finite temperature effects ensure high accuracy on the measurements of these features at large-magnitude scattering lengths. For a single Feshbach resonance, we unambiguously locate four distinct features in the Efimov structure. Three of these features form ratios that obey the Efimov universal scaling to within 10\%, while the fourth feature, occurring at a value of scattering length closest to $r_e$, instead deviates from the universal value.

cond-mat.quant-gas↗

arXiv2020

Prospects of forming high-spin polar molecules from ultracold atoms

We have investigated Feshbach resonances in collisions of high-spin atoms such as Er and Dy with closed-shell atoms such as Sr and Yb, using coupled-channel scattering and bound-state calculations. We consider both low-anisotropy and high-anisotropy limits. In both regimes we find many resonances with a wide variety of widths. The wider resonances are suitable for tuning interatomic interactions, while some of the narrower resonances are highly suitable for magnetoassociation to form high-spin molecules. These molecules might be transferred to short-range states, where they would have large magnetic moments and electric dipole moments that can be induced with very low electric fields. The results offer the opportunity to study mixed quantum gases where one species is dipolar and the other is not, and open up important prospects for a new field of ultracold high-spin polar molecules.

physics.atom-ph↗

arXiv2020

Sticky collisions of ultracold RbCs molecules

Understanding and controlling collisions is crucial to the burgeoning field of ultracold molecules. All experiments so far have observed fast loss of molecules from the trap. However, the dominant mechanism for collisional loss is not well understood when there are no allowed 2-body loss processes. Here we experimentally investigate collisional losses of nonreactive ultracold RbCs molecules, and compare our findings with the sticky collision hypothesis that pairs of molecules form long-lived collision complexes. We demonstrate that loss of molecules occupying their rotational and hyperfine ground state is best described by second-order rate equations, consistent with the expectation for complex-mediated collisions, but that the rate is lower than the limit of universal loss. The loss is insensitive to magnetic field but increases for excited rotational states. We demonstrate that dipolar effects lead to significantly faster loss for an incoherent mixture of rotational states.

cond-mat.quant-gas↗