arXiv subjects

Robin Côté

Publications and source records attributed to Robin Côté.

At least 19 recordsLinked to original sources

arXiv2026

Strategic Plan for Neutral Atom Quantum Computation

We present a strategic plan for neutral atom quantum computation, bringing together hardware development and theory advancements to achieve the goal of practical quantum advantage. The concept of practical quantum advantage is defined, along with how to verify claims of advantage, and approaches to designing quantum algorithms that deliver practical advantage. Future directions for neutral atom quantum processor hardware are described: scaling-up system size, Qubit encodings and atomic platforms, going further below threshold with neutral-atom logical-qubit performance, continuous reloading of qubits, and fast readout. We also explore opportunities for scalable integrated photonic control technologies. Alongside hardware advancements, new developments in quantum error correction and compilation of quantum circuits are proposed. Finally, we examine the opportunity of networking multiple neutral atom quantum processors together to perform distributed quantum computing and overcome possible limitations of a single system.

quant-ph↗

arXiv2023

Charge Transfer via Temporary Bonds in $C_{60} + C_{60}^+$ Molecular Collisions

We present a theoretical description of resonant charge transfer in collisions of nano-particles, specifically for $C_{60} + C_{60}^+$ collisions. We predict that transient bonds between colliding fullerenes can significantly extend the interaction time, allowing for a greater probability of charge transfer. In our model, the dumbbell-shaped $(C_{60}-C_{60})^+$ quasi-molecule, that is temporarily formed during the collision, is described as a dynamic system of 120 zero-range potentials. Using this model, we calculate the exchange interaction between colliding fullerenes and subsequently determine the corresponding charge transfer cross sections at different collision velocities. Our results have been verified with data obtained from quantum molecular dynamics simulations of the fullerene collisions. The presented theoretical model provides a description of the experimental data on the $C_{60} + C_{60}^+ $ resonant charge transfer collision through the inclusion of the temporary formation of dumbbell-shaped fullerene molecules at low collision velocities.

physics.chem-ph↗

arXiv2023

Inner Energy Relaxation and Growth of Nano-Size Particles

In this study, molecular dynamics simulations were conducted to investigate the relaxation of the internal energy in nano-sized particles and its impact on the nucleation of atomic clusters. Quantum-mechanical potentials were utilized to analyze the growth and collision relaxation of the internal energy of Ar$_n$H$^+$ clusters in a metastable Ar gas. The results revealed that small nano-clusters are formed in highly excited rotational-vibrational states, and the relaxation of internal energy and growth of these nascent clusters are concurrent processes with a strong mutual influence. Under non-equilibrium growth conditions, the relaxation of internal energy can delay the cluster growth process. The rates of cluster growth and internal energy relaxation were found to be influenced by energy-transfer collisions between cluster particles and free Ar atoms of the bath gas. Furthermore, the non-equilibrium growth and internal energy relaxation of small nano-clusters were found to depend on the structure of the cluster's atomic shells. An ensemble of molecular dynamics simulations were conducted to investigate the growth, time-evolution of kinetic and total energies of Ar$_n$H$^+$ clusters with specified $n \leq 11$, and the results were explained by collisional relaxation processes described by the Boltzmann equation. Finally, the general relationship between the rates of internal energy relaxation and non-equilibrium growth of nano-particles is discussed.

physics.atm-clus↗

arXiv2022

Model of Charge Transfer Collisions Between $C_{60}$ and Slow Ions

A semi-classical model describing the charge transfer collisions of $C_{60}$ fullerene with different slow ions has been developed to explain available experimental data. This data reveals multiple Breit-Wigner like peaks in the cross sections, with subsequent peaks of reactive cross sections decreasing in magnitude. Calculations of the charge transfer probabilities and cross sections for quasi-resonant and reactive collisions have been performed using semi-empirical potentials of interaction between fullerenes and ion projectiles. All computations have been carried out with realistic wave functions for $C_{60}$'s valence electrons derived from the simplified jellium model. The quality of these electron wave functions have been successfully verified by comparing theoretical calculations and experimental data on the small angle cross sections of resonant $C_{60}+ C_{60}^+$ collisions. Using the semi-empirical potentials to describe resonant scattering phenomena in $C_{60}$ collisions with ions and Landau-Zener charge transfer theory, we calculated theoretical cross sections for various $C_{60}$ charge transfer and fragmentation reactions which agree with experiments.

physics.chem-ph↗

arXiv2021

Photoassociation of ultracold long-range polyatomic molecules

We explore the feasibility of optically forming long-range tetratomic and larger polyatomic molecules in their ground electronic state from ultracold pairs of polar molecules aligned by external fields. Depending on the relative orientation of the interacting diatomic molecules, we find that a tetratomic can be formed either as a weakly bound complex in a very extended halo state or as a pure long-range molecule composed of collinear or nearly-collinear diatomic molecules. The latter is a novel type of tetratomic molecule comprised of two diatomic molecules bound at long intermolecular range and predicted to be stable in cold and ultracold regimes. Our numerical studies were conducted for ultracold KRb and RbCs, resulting in production of (KRb)$_2$ and (RbCs)$_2$ complexes, respectively. Based on universal properties of long-range interactions between polar molecules, we identify triatomic and tetratomic linear polar molecules with favorable ratio of dipole and quadrupole moments for which the apporach could be generalized to form polyatomic molecules.

physics.atom-ph↗

arXiv2019

Reaction blockading in charged-neutral excited-state chemistry at low collision energy

We study an excited atom-polar molecular ion chemical reaction (Ca$^*$ + BaCl$^+$) at low temperature by utilizing a hybrid atom-ion trapping system. The reaction rate and product branching fractions are measured and compared to model calculations as a function of both atomic quantum state and collision energy. At the lowest collision energy we find that the chemical dynamics dramatically differ from capture theory predictions and are primarily dictated by the radiative lifetime of the atomic quantum state instead of the underlying excited-state interaction potential. We provide a simple rule for calculating at what temperature this regime, where the collision complex lifetime is longer than the radiative lifetime of the quantum state, is reached. This effect, which greatly suppresses the reactivity of short-lived excited states, provides a means for directly probing reaction range. It also naturally suppresses unwanted chemical reactions in hybrid trapping experiments, allowing longer molecular ion coherence and interrogation times.

physics.chem-ph↗

arXiv2018

Signature of the $s$-wave regime high above ultralow temperatures

Physical processes involving charge transfer, spin exchange, or excitation exchange often occur in conditions of resonant scattering. We show that the $s$-wave contribution can be used to obtain a good approximation for the full cross section. This approximation is found to be valid for a wide range of scattering energies, including high above the Wigner regime, where many partial waves contribute. We derive an analytical expression for the exchange cross section and demonstrate its relationship to the Langevin cross section. We give examples for resonant charge transfer as well as spin-flip and excitation exchange. Our approximation can be used to gain information about the $s$-wave regime from data obtained at much higher temperatures, which would be advantageous for systems where the ultracold quantum regime is not easily reachable.

physics.atom-ph↗

arXiv2017

Synthesis of mixed hypermetallic oxide BaOCa$^+$ from laser-cooled reagents in an atom-ion hybrid trap

Hypermetallic alkaline earth (M) oxides of formula MOM have been studied under plasma conditions that preclude insight into their formation mechanism. We present here the application of emerging techniques in ultracold physics to the synthesis of a mixed hypermetallic oxide, BaOCa$^+$. These methods, augmented by high-level electronic structure calculations, permit detailed investigation of the bonding and structure, as well as the mechanism of its formation via the barrierless reaction of Ca $(^3P_J)$ with BaOCH$_{3}^+$. Further investigations of the reaction kinetics as a function of collision energy over the range 0.005 K to 30 K and of individual Ca fine-structure levels compare favorably with calculations based on long-range capture theory.

physics.atom-ph↗

arXiv2017

Charge transfer in ultracold gases via Feshbach resonances

We investigate the prospects of controlling charge-exchange in ultracold collisions of heteroisotopic combinations of atoms and ions of the same element. The treatment, readily applicable to alkali or alkanine-earth metals, is illustrated in the process $^9$Be$^{+}$ + $^{10}$Be $\leftrightarrow$ $^{9}$Be + $^{10}$Be$^{+}$, which exhibits favorable electronic, nuclear, and hyperfine structure. Feshbach resonances are obtained from quantum scattering calculations in a standard coupled-channel formalism with non-BO terms originating from the nuclear kinetic operator. Near a narrow resonance predicted at 322 G, we find the charge-exchange rate coefficient to rise from practically zero to values larger than $10^{-12}$ cm$^3$/s. Our results suggest controllable charge-exchange reactions between different isotopes of suitable atom-ion pairs with potential applications to quantum systems engineered to study charge diffusion in trapped cold atom-ion mixtures and emulate many-body physics.

physics.atom-ph↗

arXiv2016

Production of NaCa$^+$ molecular ions in the ground state from cold atom-ion mixtures by photoassociation via an intermediate state

We present a theoretical analysis of optical pathways for formation of cold Ca($^1$S)Na$^+$($^1$S) molecular ions via an intermediate state. The formation schemes are based on ab initio potential energy curves and transition dipole moments calculated using effective-core-potential methods of quantum chemistry. In the proposed approach, starting from a mixture of cold trapped Ca$^+$ ions immersed into an ultracold gas of Na atoms, (NaCa)$^+$ molecular ions are photoassociated in the excited E$^{1}Σ^+$ electronic state and allowed to spontaneously decay either to the ground electronic state or an intermediate state from which the population is transferred to the ground state via an additional optical excitation. By analyzing all possible pathways, we find that the efficiency of a two-photon scheme, via either B$^{1}Σ^+$ or C$^{1}Σ^+$ potential, is sufficient to produce significant quantities of ground state (NaCa)$^+$ molecular ions. A single-step process results in lower formation rates that would require either a high density sample or a very intense photoassociation laser to be viable.

physics.atom-ph↗

arXiv2014

Rydberg Electrons in a Bose-Einstein Condensate

We investigate a hybrid system composed of ultracold Rydberg atoms immersed in an atomic Bose-Einstein condensate (BEC). The coupling between the Rydberg electrons and BEC atoms leads to the excitation of phonons, the exchange of which induces Yukawa interaction between Rydberg atoms. Due to the small electron mass, the effective charge associated with this quasi-particle-mediated interaction can be large, while its range is equal to the healing length of the BEC, which can be tuned by adjusting the scattering length of the BEC atoms. We find that for small healing lengths, the distortion of the BEC can "image" the wave function density of the Rydberg electron, while large healing lengths induce an attractive Yukawa potential between the two Rydberg atoms that can form a new type of ultra-long-range molecule. We discuss both cases for a realistic system.

cond-mat.quant-gas↗

arXiv2014

Ab initio potential curves for the X $^2Σ_u^+$, A $^2Π_u$ and B $^2Σ_g^+$ states of Ca$_{2}^+$

We report \textit{ab initio} calculations of the X $^2 Σ_{u}^+$, A $^2Π_u$ and B $^2 Σ_{g}^+$ states of the Ca$_{2}^+$ dimer. All electron CAS+MRCI calculations are performed for the X $^2 Σ_{u}^+$ and B $^2 Σ_{g}^+$ states, while valence CAS+MRCI calculations using an effective core potential are used to describe the A $^2Π_u$ state. A double well is found in the B $^2 Σ_{g}^+$ state. Spectroscopic constants, vibrational levels, transition moments and radiative lifetimes are calculated for the most abundant isotope of calcium ($^{40}$Ca). The static dipole and quadrupole polarizabilities, and the leading order van der Waals coefficients are also calculated for all three states.

physics.chem-ph↗

arXiv2014

Photoassociation of ultracold molecules near a Feshbach resonance as a probe of the electron-proton mass ratio variation

We show that the photoassociation (PA) rate of ultracold diatomic molecules in the vicinity of a Feshbach resonance could be used to probe variations of the electron-to-proton mass ratio $β= m_e/m_p$, a quantity related to other fundamental constants via the $Λ_{\mathrm{QCD}}$ scale. The PA rate exhibits two features near a Feshbach resonance, a minimum and a maximum, which are very sensitive to the details of the interactions and the exact mass of the system. The effect and detection threshold are illustrated in the formation rates of ultracold Li$_2$ and LiNa molecules by performing coupled-channel calculations in an external magnetic field. We find that the PA rate is particularly sensitive near narrow Feshbach resonances in heavy molecules, where it might be possible to detect relative variability of $β$ on the order of $10^{-15}-10^{-16}$. We also use a two-channel model to derive a proportionality relation between the variation of the PA rate and $β$ applicable to diatomic molecules.

physics.atom-ph↗

arXiv2013

Feshbach-optimized photoassociation of ultracold $^6$Li$^{87}$Rb molecules with short pulses

Two-color photoassociation of ground state $^6$Li$^{87}$Rb molecules via the $\mathrm{B}^1Π$ electronic state using short pulses near a magnetic Feshbach resonance is studied theoretically. A near-resonant magnetic field is applied to mix the hyperfine singlet and triplet components of the initial wave function and enhance the photoassociation rate, before the population is transferred to the ground state by a second pulse. We show that an increase of up to three orders of magnitude in the absolute number of molecules produced is attainable for deeply bound vibrational levels. This technique can be generalized to other molecules with accessible magnetic Feshbach resonances.

physics.atom-ph↗

arXiv2013

Associative detachment of rubidium hydroxide

We performed calculations of the optimized structure, harmonic vibrational frequencies and dissociation energies of RbOH and its anion, and investigate the interactions between Rb and OH$^-$ leading to possible associative detachment pathways. The electron affinity of RbOH was computed to be 0.2890 eV, with a bond energy of Rb+OH$^-$ half that of Rb+OH. To determine other possible charge loss pathways, the Rb+OH and Rb+OH$^-$ dissociation curves were computed using couple cluster methods along all possible collisional angles. An adiabatic curve crossing between the neutral and charged molecule was found at the inner wall of the molecular potential curve for linear geometries. Associative detachment rates were estimated using the Langevin ion capture cross-section for hydroxide. We find for $v\ge 2$ an associative detachment rate of $>2\times 10^{-9}$ cm$^3$s$^{-1}$, while for $v=0$ and 1 no appreciable rate exists. This strong dependence on vibrational level suggests the ability to control the associative detachment rate directly.

physics.chem-ph↗

arXiv2013

Rubidium Rydberg linear macrotrimers

We investigate the interaction between three rubidium atoms in highly excited ($58p$) Rydberg states lying along a common axis and calculate the potential energy surfaces (PES) between the three atoms. We find that three-body long-range potential wells exist in some of these surfaces, indicating the existence of very extended bound states that we label \textit{macrotrimers}. We calculate the lowest vibrational eigenmodes and the resulting energy levels and show that the corresponding vibrational periods are rapid enough to be detected spectroscopically.

physics.atom-ph↗

arXiv2012

Long range forces between polar alkali diatoms aligned by external electric fields

Long range electrostatic, induction and dispersion coefficients including terms of order $R^{-8}$ have been calculated by the sum over states method using time dependent density functional theory. We also computed electrostatic moments and static polarizabilities of the individual diatoms up to the octopole order using coupled cluster and density functional theory. The laboratory-frame transformed electrostatic moments and van der Waals coefficients corresponding to the alignment of the diatomic molecules were found. We use this transformation to obtain the coupling induced by an external DC electric field, and present values for all XY combinations of like polar alkali diatomic molecules with atoms from Li to Cs. Analytic solutions to the dressed-state laboratory-frame electrostatic moments and long range intermolecular potentials are also given for the DC low-field limit.

physics.chem-ph↗

arXiv2012

Controllable binding of polar molecules and meta-stability of 1-D gases with attractive dipole forces

We explore one-dimensional (1-D) samples of ultracold polar molecules with attractive dipole-dipole interactions and show the existence of a repulsive barrier due to a strong quadrupole interaction between molecules. This barrier can stabilize a gas of ultracold KRb molecules and even lead to long-range wells supporting bound states between molecules. The properties of these wells can be controlled by external electric fields, allowing the formation of long polymer-like chains of KRb, and studies of quantum phase transitions by varying the effective interaction between molecules. We discuss the generalization of those results to other systems.

physics.chem-ph↗