arXiv subjects

John L. Bohn

Publications and source records attributed to John L. Bohn.

At least 19 recordsLinked to original sources

arXiv2026

Fermi gas of polar molecules in the Pauli-blocked regime

Quantum gases of polar molecules have recently emerged as a powerful platform for exploring exotic many-body dynamics and correlated quantum behavior. To achieve the full potential of this platform, the production of deeply degenerate quantum gases of molecules in arbitrary confinement geometries is necessary. Here, we successfully evaporate fermionic KRb molecules in both 3D and quasi-2D geometries to well below their Fermi temperatures utilizing dipolar collisions. As we evaporate deeper into degeneracy in both geometries, we enter the Pauli-blocked regime with polar molecules, which we independently confirm for the first time by measuring the Pauli suppression of elastic collisions. Moreover, the Pauli suppression of collisions contributes to the limitation of our final molecular temperature to about 25% of the Fermi temperature in both geometries, particularly limiting quasi-2D evaporation where the Pauli blockade drastically reduces an otherwise large elastic to inelastic scattering ratio. This work demonstrates the production of degenerate Fermi gases of polar molecules both in a 3D harmonic trap and in mono- and bi-layer 2D configurations. Further, our work explores the fundamental limits on evaporation of molecular Fermi gases set by the Pauli-exclusion principle, which could be overcome in the future by introducing distinguishable scattering partners.

cond-mat.quant-gas↗

arXiv2026

Limits of Statistical Models of Ultracold Complex Lifetimes

The puzzle of "sticky collisions," in which molecular collision complexes exhibit unexpectedly long lifetimes, remains an unresolved mystery. A central challenge to solving this mystery is that traditional close-coupling calculations remain limited by the vast computational cost needed to take into account all the degrees of freedom involved in the collision. In this work, we propose a statistical model designed to simulate the result of full close-coupling calculations, with the goal of collecting statistics about reasonable lifetimes of collision complexes. To do so, we numerically sample resonances using random matrix theory and utilize results from quantum defect theory to calculate scattering properties and lifetimes. We find that in the limit of dense resonances, our theory agrees well with the Rice-Ramsperger-Kassel-Markus (RRKM) prediction, whereas in the limit of sparse resonances, the physics is governed by threshold behavior rather than resonant effects. By comparing these predictions to experimental results in two limits, we argue that close-coupling calculations alone may be insufficient to resolve the issue of long lifetimes.

physics.atom-ph↗

arXiv2025

CaF+CaF interactions in the ground and excited electronic states: implications for collisional losses

Accurate \textit{ab initio} potential energy surfaces are essential to understand and predict collisional outcomes in ultracold molecular systems. In this study, we explore the intermolecular interactions between two laser-cooled CaF molecules, both in their ground and excited electronic states, aiming to understand the mechanisms behind the observed collisional losses on the non-reactive, spin-polarized surface of the CaF+CaF system. Using state-of-the-art \textit{ab initio} methods, we compute twelve electronic states of the Ca$_2$F$_2$ complex within the rigid rotor approximation applied to CaF. Calculating the potential energy surfaces for the excited electronic states of Ca$_2$F$_2$ is challenging and computationally expensive. Our approach employs the multireference configuration interaction method, restricted to single and double excitations, along with a reasonably large active space to ensure the convergence in the excited states. We also compute the spin-orbit coupling between the ground state and the lowest spin-polarized triplet state, as well as the spin-spin coupling within the lowest triplet state (1) $^3\mathrm{A}'$. Additionally, we determine the electric transition dipole moments for the (1) $^3\mathrm{A}'$-(2) $^3\mathrm{A}'$ and (1) $^3\mathrm{A}'$-(1) $^3\mathrm{A}''$ transitions. Notably, we find that the lowest spin-polarized state (1) $^3\mathrm{A}'$, shifted by 1064 nm of laser light from the optical dipole trap, intersects several electronically excited states. Finally, by analyzing the potential energy surfaces, we discuss two plausible pathways that may account for the observed collisional losses on the spin-polarized surface of the CaF+CaF system.

physics.atom-ph↗

arXiv2025

Ground and excited potential energy surfaces for CaF+Ca interactions and isotope exchange reactions

We investigate the intermolecular interactions between laser-cooled CaF and Ca, in their ground and excited electronic states, aiming to understand atom-exchange reaction pathways. Using state-of-the-art \textit{ab initio} quantum chemistry methods, we compute potential energy surfaces for nine electronic states arising from the lowest three asymptotes of Ca$_2$F trimer, within the rigid rotor approximation applied to CaF. Two-dimensional potential energy surfaces are computed for the ground state and one of the excited states. We use a combination of the coupled cluster method restricted to single, double, and perturbative triple excitations, and the multireference configuration interaction method with single and double excitations. The ground (X)~$^2\mathrm{A}'$ electronic state of the trimer is significantly deep and highly anisotropic. The excited electronic states are also strongly bound. Notably, the potential energy surface of one of the excited states, (2)~$^2\mathrm{A}'$, lies below the ground-state asymptote of the trimer. By analyzing the potential energy surfaces, we discuss atom-exchange reaction pathways involving both the ground-state interaction between CaF and Ca and the excited metastable state of Ca.

physics.atom-ph↗

arXiv2025

Collisional relaxation in shielded dipolar molecular gases

We discuss the influence of collisions on the dynamics of an ultracold gas whose constituents interact via dipolar forces. This dynamics is governed by the elastic scattering cross section of the molecules, which is to some extent under the experimentalist's control. We compare side-by-side several different situations, highlighting their similarities and differences. These situations are collisions between: 1) point dipoles; 2) electric-field-shielded polar molecules; and 3) microwave-shielded polar molecules, including the effect of microwave ellipticity.

cond-mat.quant-gas↗

arXiv2025

Theory of itinerant collisional spin dynamics in nondegenerate molecular gases

We study the fully itinerant dynamics of ultracold but nondegenerate polar molecules with a spin-$1/2$ degree of freedom encoded into two of their electric field dressed rotational states. Center of mass molecular motion is constrained to two-dimensions via tight confinement with a one-dimensional optical lattice, but remains mostly unconstrained within the plane. The pseudospins can become entangled through ultracold dipolar collisions, for which the locality of interactions is greatly relaxed by free molecular motion. At the level of single-molecule observables, collision-induced entanglement manifests as spin decoherence, for which our theoretical calculations serve well to describe recent Ramsey contrast measurements of quasi-2D confined KRb molecules at JILA [A. Carroll et al., Science 388 6745 (2025)]. In presenting a more detailed theoretical analysis of the KRb experiment, we highlight a key finding that molecular loss enhanced by particle exchange symmetry can lead to a suppression of collective spin decoherence, a mechanism with refer to as ``loss-induced quantum autoselection". We then show that by utilizing bialkali species with sufficiently large dipole moments, loss can be near completely suppressed in all collision channels via electric field tunable confinement-induced collisional shielding. The afforded collisional stability permits fully coherent spin mixing dynamics, natively realizing unitary circuit dynamics with random all-to-all connectivity and U(1) charge conservation. This work establishes a bridge between the domains of ultracold molecular collisions and many-body spin physics, ultimately proposing the use of nondegenerate bulk molecular gases as a controllable platform for nonequilibrium explorations of itinerant quantum matter.

cond-mat.quant-gas↗

arXiv2025

Quantum-State-Controlled Collisions of Ultracold Polyatomic Molecules

Collisions between ultracold calcium monohydroxide (CaOH) molecules are realized and studied. Inelastic collision rate constants are measured for CaOH prepared in ground and excited vibrational states, and the electric field dependence of these rates is measured for molecules in single quantum states of the parity-doubled bending mode. Theoretical calculations of collision rate coefficients are performed and found to agree with measured values. The lowest collisional loss rates are for states with repulsive long-range potentials that shield ultracold molecules from loss channels at short distance. These results unveil the collisional behavior of parity doublet molecules in the ultracold regime, and lay the foundation for future experiments to evaporatively cool polyatomic molecules to quantum degeneracy.

physics.atom-ph↗

arXiv2025

Observation of generalized t-J spin dynamics with tunable dipolar interactions

Long-range and anisotropic dipolar interactions profoundly modify the dynamics of particles hopping in a periodic lattice potential. We report the realization of a generalized t-J model with dipolar interactions using a system of ultracold fermionic molecules with spin encoded in the two lowest rotational states. We independently tuned the dipolar Ising and spin-exchange couplings and the molecular motion and studied their interplay on coherent spin dynamics. Using Ramsey spectroscopy, we observed and modeled interaction-driven contrast decay that depends strongly both on the strength of the anisotropy between Ising and spin-exchange couplings and on motion. This study paves the way for future exploration of kinetic spin dynamics and quantum magnetism with highly tunable molecular platforms in regimes that are challenging for existing numerical and analytical methods.

cond-mat.quant-gas↗

arXiv2024

Confinement-induced field-linked states of ultracold polar molecules

We predict the existence of stable bound states between pairs of ultracold diatomic molecules with the aid of a static electric field and 1D harmonic confinement. We focus on collisions of NaK-NaK identical fermions, for which we find that currently achievable experimental parameters allow the observation of these confinement-induced field-linked bound states as scattering resonances. The bound state is highly stable with lifetimes estimated to be tens of seconds long. With the diatomic molecules bound at distances a fraction of the dipolar length scale, these complexes allow for explorations of polyatomic chemistry and Fermi gas superfluid pairing.

physics.atom-ph↗

arXiv2024

Simulations of evaporation to deep Fermi degeneracy in microwave-shielded molecules

In the quest toward realizing novel quantum matter in ultracold molecular gases, we perform a numerical study of evaporative cooling in ultracold gases of microwave-shielded polar fermionic molecules. Our Monte Carlo simulations incorporate accurate two-body elastic and inelastic scattering cross sections, realistic modeling of the optical dipole trap, and the influence of Pauli blocking at low temperatures. The simulations are benchmarked against data from evaporation studies performed with ultracold NaK molecules, showing excellent agreement. We further explore the prospects for optimizing the evaporation efficiency by varying the ramp rate and duration of the evaporation trajectory. Our simulation shows that it is possible to reach $< 10\%$ of the Fermi temperature under optimal conditions even in the presence of two-body molecular losses.

cond-mat.quant-gas↗

arXiv2024

Hyperfine-to-rotational energy transfer in ultracold atom-molecule collisions

Energy transfer between different mechanical degrees of freedom in atom-molecule collisions has been widely studied and largely understood. However, systems involving spins remain less explored, especially with a state-to-state precision. Here, we directly observed the energy transfer from atomic hyperfine to molecular rotation in the $^{87}$Rb ($|F_a,M_{F_a}\rangle = |2,2\rangle$) + $^{40}$K$^{87}$Rb (in the rovibronic ground state $N=0$) $\longrightarrow$ Rb ($ |1,1\rangle$) + KRb ($N=0,1,2$) exothermic collision. We probed the quantum states of the collision products using resonance-enhanced multi-photon ionization followed by time-of-flight mass spectrometry. We also carried out state-of-the-art quantum scattering calculations, which rigorously take into account the coupling between the spin and rotational degrees of freedom at short range, and assume that the KRb monomer can be treated as a rigid rotor moving on a single potential energy surface. The calculated product rotational state distribution deviates from the observations even after extensive tuning of the atom-molecule potential energy surface, suggesting that vibrational degrees of freedom and conical intersections play an important part in ultracold Rb + KRb collisions. Additionally, our ab initio calculations indicate that spin-rotation coupling is dramatically enhanced near a conical intersection, which is energetically accessible at short range. The observations confirm that spin is coupled to mechanical rotation at short range and establish a benchmark for future theoretical studies.

physics.atom-ph↗

arXiv2023

Prospects for thermalization of microwave-shielded ultracold molecules

We study anisotropic thermalization in dilute gases of microwave shielded polar molecular fermions. For collision energies above the threshold regime, we find that thermalization is suppressed due to a strong preference for forward scattering and a reduction in total cross section with energy, significantly reducing the efficiency of evaporative cooling. We perform close-coupling calculations on the effective potential energy surface derived by Deng et al. [Phys. Rev. Lett. 130, 183001 (2023)], to obtain accurate 2-body elastic differential cross sections across a range of collision energies. We use Gaussian process regression to obtain a global representation of the differential cross section, over a wide range of collision angles and energies. The route to equilibrium is then analyzed with cross-dimensional rethermalization experiments, quantified by a measure of collisional efficiency toward achieving thermalization.

cond-mat.quant-gas↗

arXiv2023

Merging Dipolar Supersolids in a Double-Well Potential

We theoretically investigate the merging behaviour of two identical supersolids through dipolar Bose-Einstein condensates confined within a double-well potential. By adiabatically tuning the barrier height and the spacing between the two wells for specific trap aspect ratios, the two supersolids move toward each other and lead to the emergence of a variety of ground state phases, including a supersolid state, a macrodroplet state, a ring state, and a labyrinth state. We construct a phase diagram that characterizes various states seen during the merging transition. Further, we calculate the force required to pull the two portions of the gas apart, finding that the merged supersolids act like a deformable plastic material. Our work paves the way for future studies of layer structure in dipolar supersolids and the interaction between them in experiments.

cond-mat.quant-gas↗

arXiv2023

Probability distributions of atomic scattering lengths

The probability distribution of the real and imaginary parts of atomic scattering lengths $a$ are derived, in a two-channel model that allows for inelastic scattering to occur. While the real part of $a$ remains Cauchy-distributed, as predicted for single channel scattering in the classic work of Gribakin and Flambaum, the imaginary part of $a$ is seen to be strongly peaked near zero. Two-body inelastic scattering rates may therefore be smaller in general than a naive estimate would suggest.

physics.atom-ph↗

arXiv2023

Viscous damping in weltering motion of trapped hydrodynamic dipolar Fermi gases

We consider collective motion and damping of dipolar Fermi gases in the hydrodynamic regime. We investigate the trajectories of collective oscillations -- here dubbed ``weltering'' motions -- in cross-dimensional rethermalization experiments via Monte Carlo simulations, where we find stark differences from the dilute regime. These observations are interpreted within a semi-empirical theory of viscous hydrodynamics for gases confined to anisotropic harmonic potentials. The derived equations of motion provide a simple effective theory that show favorable agreement with full numerical solutions. To do so, the theory must carefully account for the size and shape of the effective volume within which the gas' behavior is hydrodynamic. Although formulated for dipolar molecules, our theoretical framework retains a flexibility to accommodate arbitrary elastic cross sections.

cond-mat.quant-gas↗

arXiv2023

Electro-association of ultracold dipolar molecules into tetramer field-linked states

The presence of electric or microwave fields can modify the long-range forces between ultracold dipolar molecules in such a way as to engineer weakly-bound states of molecule pairs. These so-called field-linked states [Avdeenkov et al., Phys. Rev. Lett. 90, 043006 (2003), Lassablière et al., Phys. Rev. Lett. 121, 163402 (2018)], in which the separation between the two bound molecules can be orders of magnitude larger than the molecules themselves, have been observed as resonances in scattering experiments [Chen et al., Nature 614, 59 (2023)]. Here, we propose to use them as tools for the assembly of weakly-bound tetramer molecules, by means of ramping an electric field, the electric-field analog of magneto-association in atoms. This ability would present new possibilities for constructing ultracold polyatomic molecules.

physics.atom-ph↗

arXiv2023

Sticking lifetime of ultracold CaF molecules in triplet interactions

A six-dimensional potential energy surface is constructed for the spin-polarized triplet state of CaF-CaF by \textit{ab initio} calculations at the CCSD(T) level of theory, followed by Gaussian process interpolation. The potential is utilized to calculate the density of states for this bi alkaline-earth-halogen system where we find the value 0.038 $μ$K$^{-1}$, implying a mean resonance spacing of 26 $μ$K in the collision complex. This value implies an associated Rice-Ramsperger-Kassel-Marcus lifetime of 18 $μ$s, thus predicting long-lived complexes in collisions at ultracold temperatures.

physics.atom-ph↗

arXiv2023

Out-of-Time-Order-Correlator for van der Waals potential

The quantum-to-classical correspondence is often quantified in dynamics by a quantity referred to as the out-of-time-order correlator (OTOC). In chaotic systems, the OTOC is expected to grow exponentially at early time, characteristic of a Lyapunov exponent, however, exponential growth can also occur for integrable systems. Here we investigate the OTOC for realistic diatomic molecular potentials in one degree of freedom, finding that the OTOC can grow exponentially near the dissociation energy of the moelcule. Further, this dynamics is tied to the classical dynamics of the atoms at the outer classical turning point of the potential. These results should serve to guide and interpret dynamical chaos in more complex molecules.

quant-ph↗