Three-body Recombination Rate Research Articles

Py3BR: A software for computing atomic three-body recombination rates.

The three-body recombination reaction, or ternary association, is a termolecular reaction leading to a molecule after a three-body encounter that plays a vital role in many relevant scenarios in chemical physics. Here, we introduce the Python 3-Body Recombination program, which is dedicated to the computation of atomic three-body recombination rate coefficients. The software is based on a classical trajectory approach in hyperspherical coordinates after mapping the three-body problem as a single particle in a higher-dimensional space. This theoretical approach is fully general and applicable to any ion-atom-atom or atom-atom-atom three-body process. The predictive power of the methodology has been tested in several different experimental scenarios, reaching a good description of every system. The code structure is presented alongside examples and tests to ensure the software's capacity. In addition, the performance of the software after parallelization is shown.

Product-State Distributions of Three-Body Recombination in Zero-Collision-Energy 4He2-Alkaline-Earth-Metal Systems.

The distributions of product states after three-body recombination (TBR) of zero-collision-energy 4He2X systems, with X being 9Be, 24Mg, 40Ca, 88Sr, or 138Ba, are investigated in the hyperspherical representation by quantum mechanically solving the Schrödinger equation. It is found that the weakly bound (dimer) product states are preferentially populated for all of these cases, which could be understood from the joint effects of the lowest incident channel and the relatively long-range behavior of the corresponding nonadiabatic couplings among these lowest incident and shallow recombination channels. For the strongly bound products, since the flow is accessible in the small hyperradial region, their distributions are closely related to the behavior of the nonadiabatic couplings among the corresponding deep recombination channels. Particularly, our results indicate that the products are not always formed exclusively in the most weakly bound state when the scattering lengths among the reactants are relatively large and that there may exist a large fluctuation of the strongly bound products versus their binding energies in the universal region. In addition, the total TBR rates of these nonuniversal systems are also accounted for by the joint effects of the main adiabatic potentials and nonadiabatic couplings.

Full-dimensional quantum mechanical study of three-body recombination for cold 4He-4He-20Ne system.

The increase of the number of the two-body recombination channels strongly challenges the numerical calculation of the accurate rates for the three-body recombination (TBR) process and its reverse process, collision-induced dissociation (CID), at ultracold temperatures. By taking the 4He-4He-20Ne collision system as an example, we have obtained the rates for its TBR and CID processes involving all four recombination channels, including the two-body states 4He2 (l = 0) and 4He20Ne (l = 0, 1, 2) with l the rotational quantum number. By using the adiabatic hyperspherical method, we have considered not only total angular momentum J = 0 but also J > 0 in the ultracold collision energies (E = 0.01 - 100mK × kB). It is found that 4He2 (l = 0) is the major product after the TBR process in the ultracold limit (E ≤ 0.1mK × kB). The TBR rate into 4He2 (l = 0) is nearly one order of magnitude larger than the sum of the other three products, 4He20Ne (l = 0, 1, 2). Moreover, the CID rates for the three 4He20Ne (l = 0, 1, 2) + 4He initial states are close to each other and are smaller than that for the 4He2 (l = 0) + 20Ne initial state. Additionally, we have, for the first time, performed the channel-resolved scattering calculation that can explain the above-mentioned findings quantitatively.

Control of Dy164 Bose-Einstein condensate phases and dynamics with dipolar anisotropy

We investigate the quench dynamics of quasi-one and two dimensional dipolar Bose-Einstein condensates (dBEC) of $^{164}$Dy atoms under the influence of a fast rotating magnetic field. The magnetic field thus controls both the magnitude and sign of the dipolar potential. We account for quantum fluctuations, critical to formation of exotic quantum droplet and supersolid phases in the extended Gross-Pitaevskii formalism, which includes the so-called Lee-Huang-Yang (LHY) correction. An analytical variational ansatz allows us to obtain the phase diagrams of the superfluid and droplet phases. The crossover from the superfluid to the supersolid phase and to single and droplet arrays is probed with particle number and dipolar interaction. The dipolar strength is tuned by rotating the magnetic field with subsequent effects on phase boundaries. Following interaction quenches across the aforementioned phases, we monitor the dynamical formation of supersolid clusters or droplet lattices. We include losses due to three-body recombination over the crossover regime, where the three-body recombination rate coefficient scales with the fourth power of the scattering length ($a_s$) or the dipole length ($a_{dd}$). For fixed values of the dimensionless parameter, $\epsilon_{dd} = a_{dd}/a_s$, tuning the dipolar anisotropy leads to an enhancement of the droplet lifetimes.

Laser-driven ionization mechanisms of aluminum for single particle aerosol mass spectrometry

Single particle aerosol mass spectrometry (SPAMS), an analytical technique for measuring the size and composition of individual micron-scale particles, is capable of analyzing atmospheric pollutants and bioaerosols much more efficiently and with more detail than conventional methods which require the collection of particles onto filters for analysis in the laboratory. Despite SPAMS’ demonstrated capabilities, the primary mechanisms of ionization are not fully understood, which creates challenges in optimizing and interpreting SPAMS signals. In this paper, we present a well-stirred reactor model for the reactions involved with the laser-induced vaporization and ionization of an individual particle. The SPAMS conditions modeled in this paper include a 248 nm laser which is pulsed for 8 ns to vaporize and ionize each particle in vacuum. The ionization of 1 μm, spherical Al particles was studied by approximating them with a 0-dimensional plasma chemistry model. The primary mechanism of absorption of the 248 nm photons was pressure-broadened direct photoexcitation to Al(y2D). Atoms in this highly excited state then undergo superelastic collisions with electrons, heating the electrons and populating the lower energy excited states. We found that the primary ionization mechanism is electron impact ionization of various excited state Al atoms, especially Al(y2D). Because the gas expands rapidly into vacuum, its temperature decreases rapidly. The rate of three-body recombination (e− + e− + Al+ → Al + e−) increases at low temperature, and most of the electrons and ions produced recombine within several μs of the laser pulse. The importance of the direct photoexcitation indicates that the relative peak heights of different elements in SPAMS mass spectra may be sensitive to the available photoexcitation transitions. The effects of laser intensity, particle diameter, and expansion dynamics are also discussed.

Modeling of a 43 GHz microplasma within a photonic crystal

The electron density (ne) and argon metastable density (1s5) of a 43GHz microplasma are obtained using the zero-dimensional plasma kinetics solver (ZDPlasKin®) for an incident power of 160 and 1000mW and argon pressures of 10–600Torr (1.3×103 to 8.0×104Pa). These simulations are compared with previously published experimental data. To determine the self-consistent electric field in the modeled plasma, the three-dimensional millimeter wave fields are computed as a function of electron density using ANSYS EM19.2, HFSS®. This electromagnetic field model is coupled to ZDPlasKin such that any increase in the simulated plasma density correctly attenuates the simulated electric field within the microplasma. The electron density is found to be sensitive to argon gas temperature, so a two-zone temperature model was needed to obtain agreement with experimental measurements. The temperature in the central core of the microplasma was determined by a previous experimental study. That temperature was used as an input to the model for the simulation of volume recombination losses. The outer regions of the microplasma are assumed to be in equilibrium with the walls (300K). This second temperature was used in the model to determine diffusion losses. The modeled electron and metastable densities are of the order 1020 and 1018m−3, respectively. This is in good agreement with those measured experimentally as long as the two-zone temperature model is used. In the absence of a hot gas core, the modeled three-body recombination rates are excessive and the simulation severely under-predicts the electron density and over-estimates the metastable density. We conclude that the millimeter wave microplasma has a hot core (2500K at 600Torr) that rarifies the argon gas and effectively reduces three-body recombination. This allows one to achieve high electron density on the order of 1020m−3 with only 100mW of wave power.

Low-Field Feshbach Resonances and Three-Body Losses in a Fermionic Quantum Gas of 161Dy

We report on the high-resolution Feshbach spectroscopy on a degenerate, spin-polarized Fermi gas of 161Dy atoms, measuring three-body recombination losses at a low magnetic field. For field strengths up to 1 G, we identify as much as 44 resonance features and observe the plateaus of very low losses. For four selected typical resonances, we study the dependence of the threebody recombination rate coefficient on the magnetic resonance detuning and on the temperature. We observe a strong suppression of losses with decreasing temperature already for small detunings from the resonance. The characterization of complex behavior of the three-body losses of fermionic 161Dy is important for future applications of this peculiar species in research on atomic quantum gases.

Scattering hypervolume of fermions in two dimensions

We define the three-body scattering hypervolume ${D}_{F}$ for identical spin-polarized fermions in two dimensions by considering the wave function of three such fermions colliding at zero energy and zero orbital angular momentum. We derive the asymptotic expansions of such a wave function when three fermions are far apart or one pair and the third fermion are far apart, and ${D}_{F}$ appears in the coefficients of such expansions. For weak-interaction potentials, we derive an approximate formula of ${D}_{F}$ by using the Born expansion. We then study the shift of energy of three such fermions in a large periodic area due to ${D}_{F}$. This shift is proportional to ${D}_{F}$ times the square of the area of the triangle formed by the momenta of the fermions. We also calculate the shifts of energy and of pressure of spin-polarized two-dimensional Fermi gases due to a nonzero ${D}_{F}$ and the three-body recombination rate of spin-polarized ultracold atomic Fermi gases in two dimensions.

Ultracold state-to-state chemistry for three-body recombination in realistic 3He2-alkaline-earth-metal systems.

The ultracold state-to-state chemistry for three-body recombination (TBR) in realistic systems has recently been experimentally investigated with full quantum state resolution. However, many detected phenomena remain challenging to be explored and explained from the theoretical viewpoints because this generally requires computational powers beyond state of the art. Here, the product-state distributions after TBR of 3He2-alkaline-earth-metal systems, i.e., after the processes of 3He + 3He + X → 3HeX + 3He with X being 9Be, 24Mg, 40Ca, 88Sr, or 138Ba, in the zero-collision-energy limit are theoretically studied. Two propensity rules for the distribution of the products found in current experiments have been checked, and the mechanism underlying these product-state distributions is explored. Particularly, two main intriguing transition pathways are identified, which may be responsible for the nonlinear distribution of the products vs their respective rotational quantum number. In addition, the TBR rates of these systems are also influenced by details of the interaction potential and relevant nonadiabatic couplings.

Three-Body Recombination of Cold 3He–3He–T− System

The atom-atom-anion three-body recombination (TBR) and collision induced dissociation (CID) processes of the 3He–3He–T− system at ultracold temperatures are investigated by solving the Schrödinger equation in the adiabatic hyperspherical representation. The variations of the TBR and CID rates with the collision energies in the ultracold temperatures are obtained. It is found that the JΠ = 1− symmetry dominates the TBR and CID processes in most of the considered collision energy range. The rate of TBR (CID) into (from) the l = 1 anion is larger than those for the l = 0 and l = 2 anions, with the l representing the rotational quantum number of 3HeT−. This can be understood via the nonadiabatic couplings among the different channels.

Full-dimensional quantum mechanical study of He3+He3+X− → He3+He3X−(X=HorD)

The atom-atom-anion three-body recombination (TBR) of $^{3}\mathrm{He}+^{3}\mathrm{He}+{X}^{\ensuremath{-}}$($X=\mathrm{H}\phantom{\rule{4pt}{0ex}}\text{or}\phantom{\rule{4pt}{0ex}}\mathrm{D}$) systems at ultracold temperatures ($T=0.01\ensuremath{\sim}100$ mK) are studied by solving the Schr\"odinger equation in the adiabatic hyperspherical representation. It is found that for each system, $^{3}\mathrm{He}+^{3}\mathrm{He}+{\mathrm{H}}^{\ensuremath{-}}$ or $^{3}\mathrm{He}+^{3}\mathrm{He}+{\mathrm{D}}^{\ensuremath{-}}$, the ${J}^{\mathrm{\ensuremath{\Pi}}}={1}^{\ensuremath{-}}$ symmetry dominates the TBR process, and the rates of TBR into $l=1\phantom{\rule{4pt}{0ex}}^{3}\mathrm{He}{X}^{\ensuremath{-}}$ molecular anions are roughly three times as large as than that into $l=0\phantom{\rule{4pt}{0ex}}^{3}\mathrm{He}{X}^{\ensuremath{-}}$ molecular anions for $T\ensuremath{\in}[0.01,10]$ mK, where $l$ denotes the two-body rotational quantum number. In addition, for a given product state, the TBR rates of the $^{3}\mathrm{He}{+}^{3}\mathrm{He}+{\mathrm{H}}^{\ensuremath{-}}$ system are larger than that of the $^{3}\mathrm{He}+^{3}\mathrm{He}+{\mathrm{D}}^{\ensuremath{-}}$ system by roughly two orders of magnitude which could be ascribed to the major nonadiabatic couplings between the entrance and recombination channels.

Scattering hypervolume of spin-polarized fermions

We analyze the collision of three identical spin-polarized fermions at zero collision energy, assuming arbitrary finite-range potentials, and define the corresponding three-body scattering hypervolume ${D}_{F}$. The scattering hypervolume $D$ was first defined for identical bosons in 2008. It is the three-body analog of the two-body scattering length. We solve the three-body Schr\"odinger equation asymptotically when the three fermions are far apart or one pair and the third fermion are far apart, deriving two asymptotic expansions of the wave function. Unlike the case of bosons for which $D$ has the dimension of length to the fourth power, here the ${D}_{F}$ we define has the dimension of length to the eighth power. We then analyze the interaction energy of three such fermions with momenta $\ensuremath{\hbar}{\mathbf{k}}_{1}$, $\ensuremath{\hbar}{\mathbf{k}}_{2}$, and $\ensuremath{\hbar}{\mathbf{k}}_{3}$ in a large periodic cubic box. The energy shift due to ${D}_{F}$ is proportional to ${D}_{F}/{\mathrm{\ensuremath{\Omega}}}^{2}$, where $\mathrm{\ensuremath{\Omega}}$ is the volume of the box. We also calculate the shifts of energy and pressure of spin-polarized Fermi gases due to a nonzero ${D}_{F}$ and the three-body recombination rate of spin-polarized ultracold atomic Fermi gases at finite temperatures.

Classical threshold law for the formation of van der Waals molecules.

We study the role of pairwise long-range interactions in the formation of van der Waals molecules through direct three-body recombination processes A + B + B → AB + B, based on a classical trajectory method in hyperspherical coordinates developed in our earlier works [J. Pérez-Ríos et al., J. Chem. Phys. 140, 044307 (2014); M. Mirahmadi and J. Pérez-Ríos, J. Chem. Phys. 154, 034305 (2021)]. In particular, we find the effective long-range potential in hyperspherical coordinates with an exact expression in terms of dispersion coefficients of pairwise potentials. Exploiting this relation, we derive a classical threshold law for the total cross section and the three-body recombination rate yielding an analytical expression for the three-body recombination rate as a function of the pairwise long-range coefficients of the involved partners.

Three-body recombination near the d -wave resonance in ultracold Rb85−Rb87 mixtures

In this study, we investigate the three-body recombination (TBR) rates on both sides of the interspecies $d$-wave Feshbach resonance in the $^{85}\mathrm{Rb}$ -$^{87}\mathrm{Rb}\ensuremath{-}^{87}\mathrm{Rb}$ system using the $R$-matrix propagation method in the hyperspherical coordinate frame. Our calculations are based on the Lennard-Jones model potential for the Rb-Rb interaction. Two different mechanisms of recombination-rate enhancement for positive and negative $^{85}\mathrm{Rb}$ -$^{87}\mathrm{Rb} d$-wave scattering lengths are analyzed. On the positive-scattering-length side, recombination-rate enhancement occurs due to the existence of three-body shape resonance, while on the negative-scattering-length side, the coupling between the lowest entrance channel and the highest recombination channel is crucial to the appearance of the enhancement. In addition, our study shows that the intraspecies interaction has a significant role in determining the emergence of recombination-rate enhancements. Compared to the case in which the three pairwise interactions are in $d$-wave resonance, when the $^{87}\mathrm{Rb}\ensuremath{-}^{87}\mathrm{Rb}$ interaction is near the $d$-wave resonance, the values of the interspecies scattering length that produce the recombination enhancement shift. In particular, when the $^{87}\mathrm{Rb}\ensuremath{-}^{87}\mathrm{Rb}$ interaction is away from the $d$-wave resonance, the enhancement disappears on the side with negative interspecies scattering length.

Three-body recombination calculations with a two-body mapped grid method

We investigate the prospects of combining a standard momentum space approach for ultracold three-body scattering with efficient coordinate space schemes to solve the underlying two-body problem. In many of those schemes the two-body problem is numerically restricted up to a finite interparticle distance $r_\mathrm{b}$. We analyze effects of this two-body restriction on the two- and three-body level using pairwise square-well potentials that allow for analytic two-body solutions and more realistic Lennard-Jones van der Waals potentials to model atomic interactions. We find that the two-body $t$-operator converges exponentially in $r_\mathrm{b}$ for the square-well interaction. Setting $r_\mathrm{b}$ to 2000 times the range of the interaction, the three-body recombination rate can be determined accurately up to a few percent when the magnitude of the scattering length is small compared to $r_\mathrm{b}$, while the position of the lowest Efimov features is accurate up to the percent level. In addition we find that with the introduction of a momentum cut-off, it is possible to determine the three-body parameter in good approximation even for deep van der Waals potentials.

On the formation of van der Waals complexes through three-body recombination.

In this work, we show that van der Waals molecules X-RG (where RG is the rare gas atom) may be created through direct three-body recombination collisions, i.e., X + RG + RG → X-RG + RG. In particular, the three-body recombination rate at temperatures relevant for buffer gas cell experiments is calculated via a classical trajectory method in hyperspherical coordinates [Pérez-Ríos et al., J. Chem. Phys. 140, 044307 (2014)]. As a result, it is found that the formation of van der Waals molecules in buffer gas cells (1 K ≲ T ≲ 10 K) is dominated by the long-range tail (distances larger than the LeRoy radius) of the X-RG interaction. For higher temperatures, the short-range region of the potential becomes more significant. Moreover, we notice that the rate of formation of van der Walls molecules is of the same order of the magnitude independent of the chemical properties of X. As a consequence, almost any X-RG molecule may be created and observed in a buffer gas cell under proper conditions.

Investigation of a Collisional Radiative Model for Laser-Produced Plasmas

Plasmas of a variety of types can be described by the collisional radiative (CR) model developed by Colombant and Tonan. From the CR model, the ion distribution of a plasma at a given electron temperature and density can be found. This information is useful for further simulations, and due to this, the employment of a suitable CR model is important. Specifically, ionization bottlenecks, where there are enhanced populations of certain charge states, can be seen in these ion distributions, which in some applications are important in maintaining large amounts of a specific ion. The present work was done by implementing an accepted CR model, proposed by Colombant and Tonon, in Python and investigating the effects of variations in the ionization energy and outermost electron subshell occupancy term on the positions of ionization bottlenecks. Laser Produced Plasmas created using a Nd:YAG laser with an electron density of ∼ne = 1021 cm−3 were the focus of this work. Plots of the collisional ionization, radiative recombination, and three-body recombination rate coefficients as well as the ion distribution and peak fractional ion population for various elements were examined. From these results, it is evident that using ionization energies from the NIST database and removing the orbital occupancy term in the CR model produced results with ionization bottlenecks in expected locations.

Effect of dielectronic recombination on charge-state distribution in laser-produced plasma based on steady-state collisional-radiative models

Armed with four different steady-state collisional-radiative (CR) models, we investigated the effect of dielectronic recombination (DR) on the charge-state distribution in laser-produced silicon plasma. To assess this effect, we performed a series of temporally resolved spectra of highly charged Si ions in the extreme ultraviolet region. Ab initio calculations of the DR rate coefficients were done for Si6+–Si4+ ions. We also analyzed the evolution of the collisional ionization, radiative recombination, three-body recombination, photo-ionization, and DR rate coefficients as a function of electron temperature. The electron temperature and electron density for different delay times were obtained by comparing the normalized experimental and simulated spectra. The ion fraction and average charge state from the four different CR models were also obtained. The results indicate that the DR process has a greater influence in the stage of plasma evolution that cannot be neglected in plasma diagnoses.

Three-body losses of a polarized Fermi gas near a p -wave Feshbach resonance in effective field theory

We study three-body recombination of fully spin-polarized ${}^6$Li atoms that are interacting resonantly in relative p-waves. Motivated by a recent experiment, we focus on negative scattering volumes where three atoms recombine into a deep dimer and another atom. We calculate the three-body recombination rate using a Faddeev equation derived from effective field theory. In particular, we study the magnetic field and temperature dependences of the loss rate and use the recombination data to determine the effective range of the p-wave atom-atom interaction. We also predict the existence of a shallow three-body bound state that manifests itself as a prominent feature in the energy-dependent three-body recombination rate.

Three-dimensional chemical non-equilibrium simulation of an argon transferred arc with cross-flow

A three-dimensional chemical non-equilibrium plasma simulation is performed to investigate the plasma characteristics of a high-intensity argon transferred arc exposed to cross-flow. The model is validated by comparison with experimental data from the literature, and reasonable agreement is obtained for the calculated electron temperature distributions. The simulation results indicate that the interactions of the cross gas flow with the plasma column have a significant influence on the distributions of the electric field close to the anode surface. At a high cross-flow rate, corresponding changes to the distributions of current density and Joule heating occur, leading to a high electron temperature zone stretching upstream of the arc attachment region. By examining the chemical reaction processes near the anode surface, it is found that the rate of electron-impact ionization of excited atoms and the three-body recombination rate are comparable at the positions in the upstream region close to the anode surface where the electron temperature is high, so the electron density does not increase in this region. Compared to the case without cross gas flow, the heavy-species temperature distribution becomes more constricted at a large cross-flow rate, and the energy loss due to the convective cooling makes the temperature gradients steeper on the side facing the cross-flow.