We report on the dynamics of ultracold collisions induced by near-resonant frequency-chirped light. A series of identical chirped pulses, separated by a variable delay, is applied to an ultracold sample of 85Rb, and the rate of inelastic trap-loss collisions is measured. For small detunings of the chirped light below the atomic resonance, we observe that the rate of collisions induced by a given pulse can be increased by the presence of an earlier pulse. We attribute this to the enhancement of short-range collisional flux by the long-range excitation of atom pairs to an attractive molecular potential. For larger detunings and short delays, we find that a leading pulse can suppress the rate of collisions caused by a following pulse. This is due to a depletion of short-range atom pairs by the earlier pulse. Comparison of our data to classical Monte-Carlo simulations of the collisions yields reasonable agreement.
We use frequency-chirped light on the nanosecond time scale to produce ultracold $^{87}$Rb$_{2}$ molecules in the lowest triplet state via the process of photoassociation. Comparing to quantum simulations of the molecular formation, we conclude that coherent stimulated emission plays an important role and is primarily responsible for the significant difference observed between positive and negative chirps.
We describe experiments and associated quantum simulations involving the production of ultracold $^{87}$Rb$_{2}$ molecules with nanosecond pulses of frequency-chirped light. With appropriate chirp parameters, the formation is dominated by coherent processes. For a positive chirp, excited molecules are produced by photoassociation early in the chirp, then transferred into high vibrational levels of the lowest triplet state by stimulated emission later in the chirp. Generally good agreement is seen between the data and the simulations. Shaping of the chirp can lead to a significant enhancement o…
We demonstrate the ability to coherently control ultracold atomic Rb collisions using frequency-chirped light on the nanosecond time scale. For certain center frequencies of the chirp, the rate of inelastic trap-loss collisions induced by negatively chirped light is dramatically suppressed compared to the case of a positive chirp. We attribute this to a fundamental asymmetry in the system: an excited wavepacket always moves inward on the attractive molecular potential. For a positive chirp, the resonance condition moves outward in time, while for a negative chirp, it moves inward, in the same …
We have studied the effects of chirped femtosecond laser pulses on the formation of ultracold molecules in a Rb magneto-optical trap. We have found that application of chirped femtosecond pulses suppressed the formation of 85Rb-2 and 87Rb-2 lowest triplet state molecules in contrast to comparable non-chirped pulses, cw illumination, and background formation rates. Variation of the amount of chirp indicated that this suppression is coherent in nature, suggesting that coherent control is likely to be useful for manipulating the dynamics of ultracold quantum molecular gases.
We present results on coherent control of ultracold trap-loss collisions using 40 ns pulses of nonlinearly frequency-chirped light. The chirps, either positive or negative, sweep ~1 GHz in 100 ns and are centered at various detunings below the D2 line of 85Rb. At each center detuning, we compare the collisional rate constant beta for chirps that are linear in time, concave-down and concave-up. For positive chirps, we find that beta generally depends very little on the shape of the chirp. For negative chirps, however, we find that beta can be enhanced by up to 50(20)% for the case of the concav…
A semiclassical, four-level model of a nanosecond, chirped pulse interacting with all optically accessible hyperfine states in the ultracold Rb atom is analyzed aiming at population inversion within $5S_{1/2}$ electronic state. The nature of two-photon adiabatic passage performed by such a single pulse having a bandwidth smaller than the hyperfine splitting of $5S_{1/2}$ state is investigated in the framework of the dressed state picture. It is shown that two dressed states are involved in the adiabatic dynamics of population inversion. The excited state manifold appeared to play an important …
This theoretical paper investigates the formation of ground state molecules from ultracold cesium atoms in a two-color scheme. Following previous work on photoassociation with chirped picosecond pulses [Luc-Koenig et al., Phys. Rev. A {\bf 70}, 033414 (2004)], we investigate stabilization by a second (dump) pulse. By appropriately choosing the dump pulse parameters and time delay with respect to the photoassociation pulse, we show that a large number of deeply bound molecules are created in the ground triplet state. We discuss (i) broad-bandwidth dump pulses which maximize the probability to f…
We implement a 4-level semiclassical model of a single pulse interacting with the hyperfine structure in ultracold rubidium aimed at control of population dynamics and quantum state preparation. We discuss a method based on pulse chirping to achieve population inversion between hyperfine states of the 5S shell. The results may prove useful for quantum operations with ultracold atoms.
Ultracold collisions of polar OH molecules are considered in the presence of an electrostatic field. The field exerts a strong influence on both elastic and state-changing inelastic collision rate constants, leading to clear experimental signatures that should help disentangle the theory of cold molecule collisions. Based on the collision rates we discuss the prospects for evaporative cooling of electrostatically trapped OH. We also find that the scattering properties at ultralow temperatures prove to be remarkably independent of the details of the short-range interaction, owing to avoided cro…
We have studied hetero- and homonuclear excited state/ground state collisions by loading both $^{85}$Rb and $^{87}$Rb into a far off resonant trap (FORT). Because of the relatively weak confinement of the FORT, we expect the hyperfine structure of the different isotopes to play a crucial role in the collision rates. This dependence on hyperfine structure allows us to measure collisions associated with long range interatomic potentials of different structure: such as long and short ranged; or such as purely attractive, purely repulsive, or mixed attractive and repulsive. We observe significantl…
The prospects of sympathetic cooling of polar molecules with magnetically co-trapped alkali-metal atoms are generally considered poor due to strongly anisotropic atom-molecule interactions leading to large spin relaxation rates. Using rigorous quantum scattering calculations based on ab initio interaction potentials, we show that inelastic spin relaxation in low-temperature collisions of CaH(2Sigma) molecules with Li and Mg atoms occurs at a slow rate despite the strongly anisotropic interactions. This unexpected result, which we rationalize using multichannel quantum defect theory, opens up t…
We present expressions demonstrating that collisional decoherence of ultracold atoms or molecules in a coherent superposition of non-degenerate quantum states is suppressed when both the real and imaginary parts of the scattering lengths for the states in the coherent superposition are equal. We show that the rate of collisional decoherence can be enhanced or suppressed by varying an external magnetic field near a Feshbach resonance. For some resonances, the suppression is very dramatic. We propose a method for measuring the scattering length of ultracold particles in excited quantum states ex…
We demonstrate that judicious shaping of a nanosecond-time-scale frequency chirp can dramatically enhance the formation rate of ultracold $^{87}$Rb$_{2}$ molecules. Starting with ultracold $^{87}$Rb atoms, we apply pulses of frequency-chirped light to first photoassociate the atoms into excited molecules and then, later in the chirp, de-excite these molecules into a high vibrational level of the lowest triplet state, $a \, ^{3}Σ_{u}^{+}$. The enhancing chirp shape passes through the absorption and stimulated emission transitions relatively slowly, thus increasing their adiabaticity, but jumps …
Spin-polarized metastable atoms of ultracold ytterbium are trapped at high density and their inelastic collisional properties are measured. We reveal that in collisions of Yb(3P2) with Yb(1S0) there is relatively weak inelastic loss, but with a significant spin-dependence consistent with Zeeman sublevel changes as being the dominant decay process. This is in strong contrast to our observations of Yb(3P2)-Yb(3P2) collisional loss, which are, at low field, much more rapid and have essentially no spin dependence. Our results give a guideline to use the 3P2 states in many possible applications.
The cross section of a given process fundamentally quantifies the probability for that given process to occur. In the quantum regime of low energies, the cross section can vary strongly with collision energy due to quantum effects. Here, we report on a method to directly measure the atom-ion collisional cross section in the energy range of 0.2-12 mK$\cdot$ k$_B$, by shuttling ultracold atoms trapped in an optical-lattice across a radio-frequency trapped ion. In this method, the average number of atom-ion collisions per experiment is below one such that the energy resolution is not limited by t…
We discuss the production of ultracold molecules in their electronic ground state by photoassociation employing electronically excited states with ion-pair character and strong spin-orbit interaction. A short photoassociation laser pulse drives a non-resonant three-photon transition for alkali atoms colliding in their lowest triplet state. The excited state wave packet is transferred to the ground electronic state by a second laser pulse, driving a resonant two-photon transition. After analyzing the transition matrix elements governing the stabilization step, we discuss the efficiency of popul…
We report on calculations of the elastic cross section and thermalization rate for collision between two maximally spin-polarized chromium atoms in the cold and ultracold regimes, relevant to buffer-gas and magneto-optical cooling of chromium atoms. We calculate ab initio potential energy curves for Cr2 and the van der Waals coefficient C6, and construct interaction potentials between two colliding Cr atoms. We explore the effect of shape resonances on elastic cross section, and find that they dramatically affect the thermalization rate. Our calculated value for the s-wave scattering length is…
We determine the inter-species s-wave triplet scattering length a3 for all K-Rb isotopic mixtures by measuring the cross-section for collisions between 41K and 87Rb in different temperature regimes. The positive value a3=+163(+57,-12)a0 ensures the stability of binary 41K-87Rb Bose-Einstein condensates. For the fermion-boson mixture 40K-87Rb we obtain a large and negative scattering length which implies an efficient sympathetic cooling of the fermionic species down to the degenerate regime.
Elastic and inelastic properties of weakly bound s- and p-wave molecules of fermionic atoms that collide with a third atom are investigated. Analysis of calculated collisional properties of s-wave dimers of fermions in different spin states permit us to compare and highlight the physical mechanisms that determine the stability of s-wave and p-wave molecules. In contrast to s-wave molecules, the collisional properties of p-wave molecules are found to be largely insensitive to variations of the p-wave scattering length and that these collisions will usually result in short molecular lifetimes. W…
Photoassociation of ultracold atoms induced by chirped picosecond pulses is analyzed in a non-perturbative treatment by following the wavepackets dynamics on the ground and excited surfaces. The initial state is described by a Boltzmann distribution of continuum scattering states. The chosen example is photoassociation of cesium atoms at temperature T=54 $μK$ from the $a^3 Σ_u^+(6s,6s)$ continuum to bound levels in the external well of the $0_g^-(6s+6p_{3/2})$ potential. We study how the modification of the pulse characteristics (carrier frequency, duration, linear chirp rate and intensity) ca…
Collision cross sections and rate constants between two ground- state oxygen molecules are investigated theoretically at translational energies below $\sim 1$K and in zero magnetic field. We present calculations for elastic and spin- changing inelastic collision rates for different isotopic combinations of oxygen atoms as a prelude to understanding their collisional stability in ultracold magnetic traps. A numerical analysis has been made in the framework of a rigid- rotor model that accounts fully for the singlet, triplet, and quintet potential energy surfaces in this system. The results offe…
We present a comprehensive collection of ultracold three-body collisions properties near overlapping Feshbach resonances. Our results incorporate variations of all scattering lengths and demonstrate novel collisional behavior, such as atom-molecule interference effects. Taking advantage of the unique ways in which these collisions reflect Efimov physics, new pathways to control atomic and molecular losses open up. Further, we show that overlapping resonances can greatly improve the chances of observing multiple Efimov features in an ultracold quantum gas for nearly any system.
We have studied the formation of ultracold RbSr molecules with laser pulses. After discussing the advantages of the Mott insulator phase for the control with pulses, we present two classes of strategies. The first class involves two electronic states. Two extensions of stimulated Raman adiabatic passage (STIRAP) for multi-level transitions are used : alternating STIRAP (A-STIRAP) and straddle STIRAP (S-STIRAP). Both transfer dynamics are modeled and compared. The second class of strategies involves only the electronic ground state and uses infrared (IR)/TeraHertz (THz) pulses. The chemical bon…
Understanding the sources of losses and chemical reactions of ultracold alkali-metal molecules is among the critical elements needed for their application in precision measurements and quantum technologies. Recent experiments with nonreactive systems have reported unexpectedly large loss rates, posing a challenge for theoretical explanation. Here, we examine the dynamics of intermediate four-atom complexes formed in bimolecular collisions. We calculate the nuclear spin--rotation, spin--spin, and quadrupole coupling constants for bialkali tetramers using ab intio quantum-chemical methods. We sh…
We optimize a collision-induced cooling process for ultracold atoms in the nondegenerate regime. It makes use of a Feshbach resonance, instead of rf radiation in evaporative cooling, to selectively expel hot atoms from a trap. Using functional minimization we analytically show that for the optimal cooling process the resonance energy must be tuned such that it linearly follows the temperature. Here, optimal cooling is defined as maximizing the phase-space density after a fixed cooling duration. The analytical results are confirmed by numerical Monte-Carlo simulations. In order to simulate more…
We report our experimental results on the collisional physics between non-S-state atoms (ytterbium (Yb), effectively a two-electron system, in the metastable ${}^3\mathrm{P}_2$ state) and S-state atoms (lithium (Li), an alkali metal, in the ground state). At low magnetic fields, by measuring inelastic interspecies collisional losses in the double quantum degenerate mixture we reveal the strong dependence of the inelastic losses on the internal spin states of both species and suppressed losses in stretched state configurations. Increasing the magnetic field up to 800 G we further investigate th…
We present a scheme to embed molecular anions in a gas of ultracold rubidium atoms as a route towards the preparation of cold molecular ions by collisional cooling with ultracold atoms. Associative detachment as an important loss process in collisions between OH- molecules and rubidium atoms is studied. The density distribution of trapped negative ions in the multipole radiofrequency trap is measured by photodetachment tomography, which allows us to derive absolute rate coefficients for the process. We define a regime where translational and internal cooling of molecular ions embedded into the…
We present investigations of the formation rate and collisional stability of lithium Feshbach molecules in an ultracold three-component mixture composed of two resonantly interacting fermionic 6-Li spin states and bosonic 174-Yb. We observe long molecule lifetimes (> 100 ms) even in the presence of a large ytterbium bath and extract reaction rate coefficients of the system. We find good collisional stability of the mixture in the unitary regime, opening new possibilities for studies and probes of strongly interacting quantum gases in contact with a bath species.
The Fano effect (U. Fano, Phys. Rev. \textbf{15},1866 (1961) shows that an inelastic scattering process can be suppressed when the output channel (OC) is coupled to an isolated bound state. In this paper we investigate the application of this effect for the suppression of two-body collisional losses of ultracold atoms. The Fano effect is originally derived via a first-order perturbation treatment for coupling between the incident channel (IC) and the OC. We generalize the Fano effect to systems with arbitrarily strong IC--OC couplings. We analytically prove that, in a system with one IC and on…
We study the behavior of the Eisenbud-Wigner collisional time delay around Feshbach resonances in cold and ultracold atomic and molecular collisions. We carry out coupled-channels scattering calculations on ultracold Rb and Cs collisions. In the low-energy limit, the time delay is proportional to the scattering length, so exhibits a pole as a function of applied field. At high energy, it exhibits a Lorentzian peak as a function of either energy or field. For narrow resonances, the crossover between these two regimes occurs at an energy proportional to the square of the resonance strength param…
We report measurement of the inelastic and elastic collision rates for ^{88}Sr atoms in the (5s5p)^3P_0 state in a crossed-beam optical dipole trap. This is the first measurement of ultracold collision properties of a ^3P_0 level in an alkaline-earth atom or atom with similar electronic structure. Since the (5s5p)^3P_0 state is the lowest level of the triplet manifold, large loss rates indicate the importance of principle-quantum-number-changing collisions at short range. We also provide an estimate of the collisional loss rates for the (5s5p){^3P_2} state.
Experimental studies with ultracold atoms have enabled major breakthroughs in understanding three-body physics, historically a fundamental yet challenging problem. This is because the interactions among ultracold atoms can be precisely varied using magnetically tunable scattering resonances known as Feshbach resonances. The collisions of ultracold atoms have been discovered to have many universal aspects near the unitarity limit. Away from this limit, many quantum states are expected to be active during a three-body collision, making the collisional observables practically unpredictable. Here …
We report measurement of inelastic loss in dense and cold metastable ytterbium (Yb[$^3P_2$]). Use of an optical far-off-resonance trap enables us to trap atoms in all magnetic sublevels, removing multichannel collisional trap loss from the system. Trapped samples of Yb[$^3P_2$] are produced at a density of 2$\times10^{13}$ cm$^{-3}$ and temperature of 2 $μ$K. We observe rapid two-body trap loss of Yb[$^3P_2$] and measure the inelastic collision rate constant 1.0(3)$\times10^{-11}$ cm$^3$s$^{-1}$. The existence of the fine-structure changing collisions between atoms in the $^3P_2$ state is stro…
This theoretical paper presents numerical calculations for photoassociation of ultracold cesium atoms with a chirped laser pulse and detailed analysis of the results. In contrast with earlier work, the initial state is represented by a stationary continuum wavefunction. In the chosen example, it is shown that an important population transfer is achieved to $\approx 15$ vibrational levels in the vicinity of the v=98 bound level in the external well of the $0_g^-(6s+6p_{3/2})$ potential. Such levels lie in the energy range swept by the instantaneous frequency of the pulse, thus defining a ``phot…
Ultra-cold collisions of spin-polarized 24Mg,40Ca, and 88Sr in the metastable 3P2 excited state are investigated. We calculate the long-range interaction potentials and estimate the scattering length and the collisional loss rate as a function of magnetic field. The estimates are based on molecular potentials between 3P2 alkaline-earth atoms obtained from ab initio atomic and molecular structure calculations. The scattering lengths show resonance behavior due to the appearance of a molecular bound state in a purely long-range interaction potential and are positive for magnetic fields below 50 …
We develop a collisional formalism adapted for the dynamics of ultracold dipolar particles in a confined geometry and in fields tilted relative to the confinement axis. Using tesseral harmonics instead of the usual spherical harmonics to expand the scattering wavefunction, we recover a good quantum number $ξ= \pm 1$ which is conserved during the collision. We derive the general expression of the dipole-dipole interaction in this convenient basis set as a function of the polar and azimuthal angles of the fields. We apply the formalism to the collision of fermionic and bosonic polar KRb molecule…
The collisional stability of ultracold polar molecules in electrostatic traps is considered. Rate constants for collisions that drive molecules from weak-field-seeking to strong-field-seeking states are estimated using a simple model. The rates are found to be quite large, of order 10^{-12} - 10^{-10} cm^3/sec, and moreover to grow rapidly in an externally applied electric field. It is argued that these results are generic for polar molecules, and that therefore polar molecules should be trapped by other than electrostatic means.
We experimentally demonstrate cooling of trapped ions by collisions with co-trapped, higher mass neutral atoms. It is shown that the lighter $^{39}$K$^{+}$ ions, created by ionizing $^{39}$K atoms in a magneto-optical trap (MOT), when trapped in an ion trap and subsequently allowed to cool by collisions with ultracold, heavier $^{85}$Rb atoms in a MOT, exhibit a longer trap lifetime than without the localized $^{85}$Rb MOT atoms. A similar cooling of trapped $^{85}$Rb$^{+}$ ions by ultracold $^{133}$Cs atoms in a MOT is also demonstrated in a different experimental configuration to validate th…
We study ultracold three-body collisions of bosons and fermions when the interatomic interaction is tuned near a narrow Feshbach resonance. We show that the width of the resonance has a substantial impact on the collisional properties of ultracold gases in the strongly interacting regime. We obtain numerical and analytical results that allow us to identify universal features related to the resonance width. For narrow resonances, we have found a suppression of all inelastic processes in boson systems leading to deeply bound states and an enhancement for fermion systems.
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 lo…
Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photo-excitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecu…
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 gro…
We report on deviations beyond the Born-Oppenheimer approximation in the potassium inter-atomic potentials. Identifying three up-to-now unknown $d$-wave Feshbach resonances, we significantly improve the understanding of the $^{39}$K inter-atomic potentials. Combining these observations with the most recent data on known inter- and intra-isotope Feshbach resonances, we show that Born-Oppenheimer corrections can be determined from atomic collisional properties alone and that significant differences between the homo- and heteronuclear case appear.
We investigate the ultracold reaction dynamics of magnetically trapped NH($X ^3Σ^-$) radicals using rigorous quantum scattering calculations involving three coupled potential energy surfaces. We find that the reactive NH + NH cross section is driven by a short-ranged collisional mechanism, and its magnitude is only weakly dependent on magnetic field strength. Unlike most ultracold reactions observed so far, the NH + NH scattering dynamics is non-universal. Our results indicate that chemical reactions can cause more trap loss than spin-inelastic NH + NH collisions, making molecular evaporative …
At ultracold temperatures, the Pauli exclusion principle suppresses collisions between identical fermions. This has motivated the development of atomic clocks using fermionic isotopes. However, by probing an optical clock transition with thousands of lattice-confined, ultracold fermionic Sr atoms, we have observed density-dependent collisional frequency shifts. These collision effects have been measured systematically and are supported by a theoretical description attributing them to inhomogeneities in the probe excitation process that render the atoms distinguishable. This work has also yield…
We report Ramsey spectroscopy on the clock states of individual Cs impurities immersed in an ultracold Rb bath. We record both the interaction-driven phase evolution and the decay of fringe contrast of the Ramsey interference signal to obtain information about bath density or temperature nondestructively. The Ramsey fringe is modified by a differential shift of the collisional energy when the two Cs states superposed interact with the Rb bath. This differential shift is directly affected by the mean gas density and the details of the Rb-Cs interspecies scattering length, affecting the phase ev…
We study collisional rethermalization in ultracold dipolar thermal gases, made intricate by their anisotropic differential cross sections. Theoretical methods are provided to derive the number of collisions per rethermalization, which for dipolar gases, is highly dependent on the dipole alignment axis. These methods are formulated to be easily applied in experimental contexts, even reducing to analytic expressions if the route to thermal equilibrium is governed by short-time dynamics. In the analytic case, collisional rethermalization is fully characterized by the dipole magnitude and orientat…
In plasmas at very low temperatures formation of neutral atoms is dominated by collisional three-body recombination, owing to the strong ~ T^(-9/2) scaling of the corresponding recombination rate with the electron temperature T. While this law is well established at high temperatures, the unphysical divergence as T -> 0 clearly suggest a breakdown in the low-temperature regime. Here, we present a combined molecular dynamics-Monte-Carlo study of electron-ion recombination over a wide range of temperatures and densities. Our results reproduce the known behavior of the recombination rate at high …
While ion heating by elastic electron-ion collisions may be neglected for a description of the evolution of freely expanding ultracold neutral plasmas, the situation is different in scenarios where the ions are laser-cooled during the system evolution. We show that electron-ion collisions in laser-cooled plasmas influence the ionic temperature, decreasing the degree of correlation obtainable in such systems. However, taking into account the collisions increases the ion temperature much less than what would be estimated based on static plasma clouds neglecting the plasma expansion. The latter l…
Collisional resonances are an important tool which has been used to modify interactions in ultracold gases, for realizing novel Hamiltonians in quantum simulations, for creating molecules from atomic gases and for controlling chemical reactions. So far, such resonances have been observed for atom-atom collisions, atom-molecule collisions and collisions between Feshbach molecules which are very weakly bound. Whether such resonances exist for ultracold ground state molecules has been debated due to the possibly high density of states and/or rapid decay of the resonant complex. Here we report a v…
Several mechanisms by which an external electromagnetic field influences the temperature of a plasma are studied analytically and specialized to the system of an ultracold plasma (UCP) driven by a uniform radio frequency (RF) field. Heating through collisional absorption is reviewed and applied to UCPs. Furthermore, it is shown that the RF field modifies the three body recombination process by ionizing electrons from intermediate high-lying Rydberg states and upshifting the continuum threshold, resulting in a suppression of three body recombination. Heating through collisionless absorption ass…
We introduce a combined molecular dynamics (MD) and quantum trajectories (QT) code to simulate the effects of near-resonant optical fields on state-vector evolution and particle motion in a collisional system. In contrast to collisionless systems, in which the quantum dynamics of multi-level, laser-driven particles with spontaneous emission can be described with the optical Bloch equations (OBEs), particle velocities in sufficiently collisional systems change on timescales comparable to those of the laser-induced, quantum-state dynamics. These transient velocity changes can cause the time-aver…