arXiv subjects

Eite Tiesinga

Publications and source records attributed to Eite Tiesinga.

At least 19 recordsLinked to original sources

arXiv2026

Quantum Scattering of Fullerene 12C60 with Rare Gas Atoms and its selection rules for rotational quenching

The discovery of the C60 fullerene opened new horizons to design carbon nanostructures with targeted electronic structure as well as transport and optical properties. For example, endohedral 12C60 molecules were proposed as candidates for functional quantum architectures to store and manipulate encased atomic and molecular qubits. Recent advances in cryogenic buffer-gas cooling and frequency-comb spectroscopy have enabled rovibrational quantum-state-resolved measurements of gas-phase 12C60, revealing rotational fine structure reflecting its high icosahedral symmetry. Here, we present a perturbative quantum description of the 12C60 molecule interacting with a buffer gas of 40Ar atoms at temperatures of order 100 K, including a detailed analysis of their electronic structure, their interaction anisotropies, and the collision-induced rotational quenching of 12C60 in its vibrational and electronic ground state. The role of the icosahedral symmetry on the collisional dynamics is emphasized leading to unusual selection rules. Finally, we compute the isotropic and anisotropic static and dynamic dipole polarizability of 12C60 in its absolute ground state in order to evaluate the long-range, van der Waals interaction between 12C60 and 40Ar.

physics.atom-ph↗

arXiv2026

Measurements of diffusion coefficients for rubidium--inert gas mixtures using coherent scattering from optically pumped population gratings

We present comprehensive determinations of the diffusion coefficients $D$ at $T=24\,\degree$C for trace amounts of naturally abundant Rb atoms in inert, naturally abundant He, Ne, N$_2$, Ar, Kr, and Xe buffer gases using a single measurement technique. We establish a spatially periodic population grating in the Rb sample using two laser beams that intersect at a small angle $\theta$ of a few milliradians. The atomic population grating decays exponentially in time due to diffusive motion induced by momentum-changing elastic collisions between Rb and buffer gas atoms or molecules, and is monitored by observing the scattered field from a read-out beam. We distinguish the contribution of diffusion from other collisional processes by measuring the characteristic $\theta^2$ dependence of the decay rate. We also measure the systematic dependence of the decay rate on the buffer gas pressure over a range of $7\,000$ Pa to $90\,000$ Pa. In this manner, we obtain diffusion coefficients at standard atmospheric pressure of $101\,325$ Pa and at a temperature of 24.0(5)~$^\circ$C. We obtain weighted averages of $0.33(5)$ cm$^2$/s, $0.214(14)$ cm$^2$/s, $0.132(7)$ cm$^2$/s, $0.123(9)$ cm$^2$/s, $0.093(9)$ cm$^2$/s, and $0.073(4)$ cm$^2$/s for Rb in He, Ne, N$_2$, Ar, Kr, and Xe, respectively. We compare this data with diffusion coefficients obtained using quantum, classical, and semi-classical theoretical methods based on the most accurate interatomic interaction potentials from the literature. Our computed diffusion coefficients based on the quantum theory agree with the experimental determinations when systematic effects are taken into account. Our measurements and modeling are relevant to the optimization of magnetometers, imaging using spin-polarized noble gases, tests of collision models based on interatomic potentials, and the development of pressure sensors.

physics.atom-ph↗

arXiv2025

Unconventional Chemical Bonding of Lanthanide-OH Molecules

We present a theoretical study of the low lying adiabatic relativistic electronic states of lanthanide monohydroxide (Ln-OH) molecules near their linear equilibrium geometries. We focus on heavy, magnetic DyOH and ErOH relevant to fundamental symmetry tests. We use a restricted-active-space self-consistent field method combined with spin-orbit coupling as well as a relativistic coupled-cluster method. In addition, electric dipole and magnetic moments are computed with the self-consistent field method. Analysis of the results from both methods shows that the dominant molecular configuration of the ground state is one where an electron from the partially filled and submerged 4f orbital of the lanthanide atom moves to the hydroxyl group, leaving the closed outer-most 6s$^2$ lone electron pair of the lanthanide atom intact in sharp contrast to the bonding in alkaline-earth monohydroxides and YbOH, where an electron from the outer-most s shell moves to the hydroxyl group. For linear molecules the projection of the total electron angular momentum on the symmetry axis is a conserved quantity with quantum number $\Omega$ and we study the polynomial $\Omega$ dependence of the energies of the ground states as well as their electric and magnetic moments. We find that the lowest energy states have $|\Omega|=15/2$ and 1/2 for DyOH and ErOH, respectively. The zero field splittings among these $\Omega$ states is approximately $hc\times 1\,000$~cm$^{-1}$. We find that the permanent dipole moments for both triatomics are fairly small at 0.23 atomic units. The magnetic moments are closely related to that of the corresponding atomic Ln$^+$ ion in an excited electronic state. We also realize that the total electron angular momentum is to good approximation conserved and has a quantum number of 15/2 for both triatomic molecules.

physics.atom-ph↗

arXiv2024

On the effect of "glancing" collisions in the cold atom vacuum standard

We theoretically investigate the effect of ``glancing" collisions on the ultra-high vacuum (UHV) pressure readings of the cold atom vacuum standard (CAVS), based on either ultracold $^7$Li or $^{87}$Rb atoms. Here, glancing collisions are those collisions between ultracold atoms and room-temperature background atoms or molecules in the vacuum that do not impart enough kinetic energy to eject an ultracold atom from its trap. Our model is wholly probabilistic and shows that the number of the ultracold atoms remaining in the trap as a function of time is non-exponential. We update the recent results of a comparison between a traditional pressure standard -- a combined flowmeter and dynamic expansion system -- to the CAVS [D.S. Barker, et al., arXiv:2302.12143] to reflect the results of our model. We find that the effect of glancing collisions shifts the theoretical predictions of the total loss rate coefficients for $^7$Li colliding with noble gases or N$_2$ by up to $0.6$ %. Likewise, we find that in the limit of zero trap depth the experimentally extracted loss rate coefficients for $^{87}$Rb colliding with noble gases or N$_2$ shift by as much as 2.2 %.

physics.atom-ph↗

arXiv2024

CODATA Recommended Values of the Fundamental Physical Constants: 2022

We report the 2022 self-consistent values of constants and conversion factors of physics and chemistry recommended by the Committee on Data of the International Science Council (CODATA). The recommended values can also be found at physics.nist.gov/constants. The values are based on a least-squares adjustment that takes into account all theoretical and experimental data available through 31 December 2022. A discussion of the major improvements as well as inconsistencies within the data is given.

hep-ph↗

arXiv2024

Rotational magic conditions for ultracold molecules in the presence of Raman and Rayleigh scattering

Molecules have vibrational, rotational, spin-orbit and hyperfine degrees of freedom or quantum states, each of which responds in a unique fashion to external electromagnetic radiation. The control over superpositions of these quantum states is key to coherent manipulation of molecules. For example, the better the coherence time the longer quantum simulations can last. The important quantity for controlling an ultracold molecule with laser light is its complex-valued molecular dynamic polarizability. Its real part determines the tweezer or trapping potential as felt by the molecule, while its imaginary part limits the coherence time. Here, our study shows that efficient trapping of a molecule in its vibrational ground state can be achieved by selecting a laser frequency with a detuning on the order of tens of GHz relative to an electric-dipole-forbidden molecular transition. Close proximity to this nearly forbidden transition allows to create a sufficiently deep trapping potential for multiple rotational states without sacrificing coherence times among these states from Raman and Rayleigh scattering. In fact, we demonstrate that magic trapping conditions for multiple rotational states of the ultracold $^{23}$Na$^{87}$Rb polar molecule can be created.

quant-ph↗

arXiv2024

Monte-Carlo simulations of the capture and cooling of alkali-metal atoms by a supersonic helium jet

We present three-dimensional Monte-Carlo simulations of the capture of 1000 K $^7$Li or 500 K $^{87}$Rb atoms by a continuous supersonic $^4$He jet and show that intense alkali-metal beams form with narrow transverse and longitudinal velocity distributions. The nozzle creating the $^4$He jet is held at approximately 4 K. These conditions are similar to those in the cold $^7$Li source developed by some of us as described in [Phy. Rev. A 107, 013302 (2023)]. The simulations use differential cross-sections obtained from quantum scattering calculations of $^7$Li or $^{87}$Rb atoms with $^4$He atoms for relative collision energies between $k\times 1$ mK to $k\times 3000$ K, where $k$ is the Boltzmann constant. For collision energies larger than $\approx k\times 4$ K the collisions favor forward scattering, deflecting the $^7$Li or $^{87}$Rb atoms by no more than a few degrees. From the simulations, we find that about 1$\%$ of the lithium atoms are captured into the $^4$He jet, resulting in a lithium beam with a most probable velocity of about $210$ m/s and number densities on the order of $10^{8}$ cm$^{-3}$. Simulations predict narrow yet asymmetric velocity distributions which are verified by comparing to fluorescence measurements of the seeded $^7$Li atoms. We find agreement between simulated and experimentally measured seeded $^7$Li densities to be better than 50$\%$ across a range of $^4$He flow rates. We make predictions for capture efficiency and cooling of $^{87}$Rb by a supersonic $^4$He jet. The capture efficiency for $^{87}$Rb is expected to be similar to $^7$Li.

physics.atom-ph↗

arXiv2023

Accurate measurement of the loss rate of cold atoms due to background gas collisions for the quantum-based cold atom vacuum standard

We present measurements of thermalized collisional rate coefficients for ultra-cold $^7$Li and $^{87}$Rb colliding with room-temperature He, Ne, N$_2$, Ar, Kr, and Xe. In our experiments, a combined flowmeter and dynamic expansion system, a vacuum metrology standard, is used to set a known number density for the room-temperature background gas in the vicinity of the magnetically trapped $^7$Li or $^{87}$Rb clouds. Each collision with a background atom or molecule removes a $^7$Li or $^{87}$Rb atom from its trap and the change in the atom loss rate with background gas density is used to determine the thermalized loss rate coefficients with fractional standard uncertainties better than 1.6 % for $^7$Li and 2.7 % for $^{87}$Rb. We find consistency -- a degree of equivalence of less than one -- between the measurements and recent quantum-scattering calculations of the loss rate coefficients [J. Klos and E. Tiesinga, J. Chem. Phys. 158, 014308 (2023)], with the exception of the loss rate coefficient for both $^7$Li and $^{87}$Rb colliding with Ar. Nevertheless, the agreement between theory and experiment for all other studied systems provides validation that a quantum-based measurement of vacuum pressure using cold atoms also serves as a primary standard for vacuum pressure, which we refer to as the cold-atom vacuum standard.

physics.atom-ph↗

arXiv2023

Quantum Control of Atom-Ion Charge Exchange via Light-induced Conical Intersections

Conical intersections are crossing points or lines between two or more adiabatic electronic potential energy surfaces in the multi-dimensional coordinate space of colliding atoms and molecules. Conical intersections and corresponding non-adiabatic coupling can greatly affect molecular dynamics and chemical properties. In this paper, we predict significant or measurable non-adiabatic effects in an ultracold atom-ion charge-exchange reaction in the presence of laser-induced conical intersections (LICIs). We investigate the fundamental physics of these LICIs on molecular reactivity under unique conditions: those of relatively low laser intensity of $10^8$ W/cm$^2$ and ultracold temperatures below 1 mK. We predict irregular interference effects in the charge-exchange rate coefficients between K and Ca$^+$ as functions of laser frequency. These irregularities occur in our system due to the presence of two LICIs. To further elucidate the role of the LICIs on the reaction dynamics, we compare these rate coefficients with those computed for a system where the CIs have been ``removed''. In the laser frequency window, where conical interactions are present, the difference in rate coefficients can be as large as $10^{-9}$ cm$^3$/s.

physics.atom-ph↗

arXiv2022

Comparison of two multiplexed portable cold-atom vacuum standards

We compare the vacuum measured by two portable cold-atom vacuum standards (pCAVS) based on ultracold $^7$Li atoms. The pCAVS are quantum-based standards that use a priori scattering calculations to convert a measured loss rate of cold atoms from a conservative trap into a background gas pressure. Our pCAVS devices share the same laser system and measure the vacuum concurrently. The two pCAVS together detected a leak with a rate on the order of $10^{-6}$ Pa L/s. After fixing the leak, the pCAVS measured a pressure of about 40 nPa with 2.6 % uncertainty. The two pCAVS agree within their uncertainties, even when swapping some of their component parts. Operation of the pCAVS was found to cause some additional outgassing, on the order of $10^{-8}$ Pa L/s, which can be mitigated in the future by better thermal management.

physics.atom-ph↗

arXiv2021

Prospects for assembling ultracold radioactive molecules from laser-cooled atoms

Molecules with unstable isotopes often contain heavy and deformed nuclei and thus possess a high sensitivity to parity-violating effects, such as Schiff moments. Currently the best limits on Schiff moments are set with diamagnetic atoms. Polar molecules with quantum-enhanced sensing capabilities, however, can offer better sensitivity. In this work, we consider the prototypical 223Fr107Ag molecule, as the octupole deformation of the unstable 223Fr francium nucleus amplifies the nuclear Schiff moment of the molecule by two orders of magnitude relative to that of spherical nuclei and as the silver atom has a large electronegativity. To develop a competitive experimental platform based on molecular quantum systems, 223Fr atoms and 107Ag atoms have to be brought together at ultracold temperatures. That is, we explore the prospects of forming 223Fr107Ag from laser-cooled Fr and Ag atoms. We have performed fully relativistic electronic-structure calculations of ground and excited states of FrAg that account for the strong spin-dependent relativistic effects of Fr and the strong ionic bond to Ag. In addition, we predict the nearest-neighbor densities of magnetic-field Feshbach resonances in ultracold 223Fr+107Ag collisions with coupled-channel calculations. These resonances can be used for magneto-association into ultracold, weakly-bound FrAg. We also determine the conditions for creating 223Fr107Ag molecules in their absolute ground state from these weakly-bound dimers via stimulated Raman adiabatic passage using our calculations of the relativistic transition electronic dipole moments.

quant-ph↗

arXiv2021

Relativistic aspects of orbital and magnetic anisotropies in the chemical bonding and structure of lanthanide molecules

The electronic structure of magnetic lanthanide atoms is fascinating from a fundamental perspective. They have electrons in a submerged open 4f shell lying beneath a filled 6s shell with strong relativistic correlations leading to a large magnetic moment and large electronic orbital angular momentum. This large angular momentum leads to strong anisotropies, i. e. orientation dependencies, in their mutual interactions. The long-ranged molecular anisotropies are crucial for proposals to use ultracold lanthanide atoms in spin-based quantum computers, the realization of exotic states in correlated matter, and the simulation of orbitronics found in magnetic technologies. Short-ranged interactions and bond formation among these atomic species have thus far not been well characterized. Efficient relativistic computations are required. Here, for the first time we theoretically determine the electronic and ro-vibrational states of heavy homonuclear lanthanide Er2 and Tm2 molecules by applying state-of-the-art relativistic methods. In spite of the complexity of their internal structure, we were able to obtain reliable spin-orbit and correlation-induced splittings between the 91 Er2 and 36 Tm2 electronic potentials dissociating to two ground-state atoms. A tensor analysis allows us to expand the potentials between the atoms in terms of a sum of seven spin-spin tensor operators simplifying future research. The strengths of the tensor operators as functions of atom separation are presented and relationships among the strengths, derived from the dispersive long-range interactions, are explained. Finally, low-lying spectroscopically relevant ro-vibrational energy levels are computed with coupled-channels calculations and analyzed.

quant-ph↗

arXiv2019

Feshbach resonances in $p$-wave three-body recombination within Fermi-Fermi mixtures of open-shell $^6$Li and closed-shell $^{173}$Yb atoms

We report on observations and modeling of interspecies magnetic Feshbach resonances in dilute ultracold mixtures of open-shell alkali-metal $^6$Li and closed-shell $^{173}$Yb atoms with temperatures just above quantum degeneracy for both fermionic species. Resonances are located by detecting magnetic-field-dependent atom loss due to three-body recombination. We resolve closely-located resonances that originate from a weak separation-dependent hyperfine coupling between the electronic spin of $^6$Li and the nuclear spin of $^{173}$Yb, and confirm their magnetic field spacing by ab initio electronic-structure calculations. Through quantitative comparisons of theoretical atom-loss profiles and experimental data at various temperatures between 1 $μ$K and 20 $μ$K, we show that three-body recombination in fermionic mixtures has a $p$-wave Wigner threshold behavior leading to characteristic asymmetric loss profiles. Such resonances can be applied towards the formation of ultracold doublet ground-state molecules and quantum simulation of superfluid $p$-wave pairing.

physics.atom-ph↗

arXiv2018

Observation of bound state self-interaction in a nano-eV atom collider

Quantum mechanical scattering resonances for colliding particles occur when a continuum scattering state couples to a discrete bound state between them. The coupling also causes the bound state to interact with itself via the continuum and leads to a shift in the bound state energy, but, lacking knowledge of the bare bound state energy, measuring this self-energy via the resonance position has remained elusive. Here, we report on the direct observation of self-interaction by using a nano-eV atom collider to track the position of a magnetically-tunable Feshbach resonance through a parameter space spanned by energy and magnetic field. Our system of potassium and rubidium atoms displays a strongly non-monotonic resonance trajectory with an exceptionally large self-interaction energy arising from an interplay between the Feshbach bound state and a different, virtual bound state at a fixed energy near threshold.

cond-mat.quant-gas↗

arXiv2018

Orbital quantum magnetism in spin dynamics of strongly interacting magnetic lanthanide atoms

Laser cooled lanthanide atoms are ideal candidates with which to study strong and unconventional quantum magnetism with exotic phases. Here, we use state-of-the-art closed-coupling simulations to model quantum magnetism for pairs of ultracold spin-6 erbium lanthanide atoms placed in a deep optical lattice. In contrast to the widely used single-channel Hubbard model description of atoms and molecules in an optical lattice, we focus on the single-site multi-channel spin evolution due to spin-dependent contact, anisotropic van der Waals, and dipolar forces. This has allowed us to identify the leading mechanism, orbital anisotropy, that governs molecular spin dynamics among erbium atoms. The large magnetic moment and combined orbital angular momentum of the 4f-shell electrons are responsible for these strong anisotropic interactions and unconventional quantum magnetism. Multi-channel simulations of magnetic Cr atoms under similar trapping conditions show that their spin-evolution is controlled by spin-dependent contact interactions that are distinct in nature from the orbital anisotropy in Er. The role of an external magnetic field and the aspect ratio of the lattice site on spin dynamics is also investigated.

physics.atom-ph↗

arXiv2018

A semiclassical theory of phase-space dynamics of interacting bosons

We study the phase-space representation of dynamics of bosons in the semiclassical regime where the occupation number of the modes is large. To this end, we employ the van Vleck-Gutzwiller propagator to obtain an approximation for the Green's function of the Wigner distribution. The semiclassical analysis incorporates interference of classical paths and reduces to the truncated Wigner approximation (TWA) when the interference is ignored. Furthermore, we identify the Ehrenfest time after which the TWA fails. As a case study, we consider a single-mode quantum nonlinear oscillator, which displays collapse and revival of observables. We analytically show that the interference of classical paths leads to revivals, an effect that is not reproduced by the TWA or a perturbative analysis.

cond-mat.quant-gas↗

arXiv2018

Fractal Universality in Near-Threshold Magnetic Lanthanide Dimers

Ergodic quantum systems are often quite alike, whereas nonergodic, fractal systems are unique and display characteristic properties. We explore one of these fractal systems, weakly bound dysprosium lanthanide molecules, in an external magnetic field. As recently shown, colliding ultracold magnetic dysprosium atoms display a soft chaotic behavior with a small degree of disorder. We broaden this classification by investigating the generalized inverse participation ratio and fractal dimensions for large sets of molecular wave functions. Our exact close-coupling simulations reveal a dynamic phase transition from partially localized states to totally delocalized states and universality in its distribution by increasing the magnetic field strength to only a hundred Gauss (or 10 mT). Finally, we prove the existence of nonergodic delocalized phase in the system and explain the violation of ergodicity by strong coupling between near-threshold molecular states and the nearby continuum.

cond-mat.dis-nn↗

arXiv2018

Development of a new UHV/XHV pressure standard (cold atom vacuum standard)

The National Institute of Standards and Technology has recently begun a program to develop a primary pressure standard that is based on ultra-cold atoms, covering a pressure range of 1 x 10-6 to 1 x 10-10 Pa and possibly lower. These pressures correspond to the entire ultra-high vacuum range and extend into the extreme-high vacuum. This cold-atom vacuum standard (CAVS) is both a primary standard and absolute sensor of vacuum. The CAVS is based on the loss of cold, sensor atoms (such as the alkali-metal lithium) from a magnetic trap due to collisions with the background gas (primarily H2) in the vacuum. The pressure is determined from a thermally-averaged collision cross section, which is a fundamental atomic property, and the measured loss rate. The CAVS is primary because it will use collision cross sections determined from ab initio calculations for the Li + H2 system. Primary traceability is transferred to other systems of interest using sensitivity coefficients.

physics.app-ph↗