We theoretically examine Raman photoassociation of a Bose-Einstein condensate, revisiting stimulated Raman adiabatic passage (STIRAP). Due to collisional mean-field shifts, efficient molecular conversion requires strong coupling and low density, either of which can bring about rogue photodissociation to noncondensate modes. We demonstrate explicitly that rogue transitions are negligible for low excited-state fractions and photodissociation that is slower than the STIRAP timescale. Moreover, we derive a reduced-parameter model of collisions, and thereby find that a gain in the molecular conversion efficiency can be obtained by adjusting the atom-atom scattering length with off-resonant magnetoassociation. This gain saturates when the atom-atom scattering length is tuned to a specific fraction of either the molecule-molecule or atom-molecule scattering length. We conclude that a fully-optimized STIRAP scheme may offer the best chance for achieving coherent conversion from an atomic to a molecular condensate with photoassociation.
We analyze coherent two-color photoassociation of a Bose-Einstein condensate, focusing on stimulated Raman adiabatic passage (STIRAP) in free-bound-bound transitions from atoms to molecules. This problem is of particular interest since STIRAP is predicted to be necessarily absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. However, Bose-stimulation enhances the free-bound dipole matrix element for an atomic condensate, and photoassociative STIRAP turns out to be a viable mechanism for converting an atomic condensate to a molecular condensate with near-unit …
The influence of intense electromagnetic wave on photoassociation is investigated. The quantum-mechanical problem of the stimulated transition is considered. The probabilities for stimulated production of mesic atoms in states with large principal quantum numbers are calculated.
We discuss the role of Bose enhancement of the dipole matrix element in photoassociation, using stimulated Raman adiabatic passage as an example. In a nondegenerate gas the time scale for coherent optical transients tends to infinity in the thermodynamic limit, whereas Bose enhancement keeps this time scale finite in a condensate. Coherent transients are therefore absent in photoassociation of a thermal nondegenerate gas, but are feasible if the gas is a condensate.
We theoretically investigate Raman photoassociation of a degenerate Bose-Fermi mixture of atoms and the subsequent prospect for anomalous (Cooper) pairing between atoms and molecules. Stable fermionic molecules are created via free-bound-bound stimulated Raman adiabatic passage which, in contrast to purely bosonic systems, can occur in spite of collisions. With the leftover atomic condensate to enhance intrafermion interactions, the superfluid transition to atom-molecule Cooper pairs occurs at a temperature that is roughly an order of magnitude below what is currently feasible.
We study coherent photoassociation, phenomena analogous to coherent optical transients in few-level systems, which may take place in photoassociation of an atomic Bose-Einstein condensate but not in a nondegenerate gas. We develop a second-quantized Hamiltonian to describe photoassociation, and apply the Hamiltonian both in the momentum representation and in the position representation (field theory). Solution of the two-mode problem including only one mode each for the atomic and molecular condensates displays analogs of Rabi oscillations and rapid adiabatic passage. A classical version of th…
Collective two-color photoassociation of a freely-interacting 87Rb Bose-Einstein condensate is theoretically examined, focusing on stimulated Raman adiabatic passage (STIRAP) from an atomic to a stable molecular condensate. In particular, Drummond et al. [Phys. Rev. A 65, 063619 (2002); cond-mat/0110578] have predicted that particle-particle interactions can limit the efficiency of collective atom-molecule STIRAP, and that optimizing the laser parameters can partially overcome this limitation. We suggest that the molecular conversion efficiency can be further improved by treating the initial c…
We have produced ultracold, polar RbCs* molecules via photoassociation in a laser-cooled mixture of Rb and Cs atoms. Using a model of the RbCs* molecular interaction which reproduces the observed rovibrational structure, we infer decay rates in our experiments into deeply bound singlet ground state RbCs vibrational levels as high as 5 x 10^5 s^-1 per level. Population in such deeply bound levels could be efficiently transferred to the vibrational ground state using a single stimulated Raman transition, opening the possibility to create large samples of stable, ultracold polar molecules.
Photoassociation and the Feshbach resonance are, in principle, feasible means for creating a molecular Bose-Einstein condensate from an already-quantum-degenerate gas of atoms; however, mean-field shifts and irreversible decay place practical constraints on the efficient delivery of stable molecules using either mechanism alone. We therefore propose Feshbach-stimulated Raman photoproduction, i.e., a combination of magnetic and optical methods, as a viable means to collectively convert degenerate atoms into a stable molecular condensate with near-unit efficiency.
We report on two-photon photoassociation (PA) spectroscopy of ultracold heteronuclear LiRb molecules. This is used to determine the binding energies of the loosely bound levels of the electronic ground singlet and the lowest triplet states of LiRb. We observe strong two-photon PA lines with power broadened line widths greater than 20 GHz at relatively low laser intensity of 30 W/cm$^{2}$. The implication of this observation on direct atom to molecule conversion using stimulated Raman adiabatic passage (STIRAP) is discussed and the prospect for electronic ground state molecule production is the…
We report on a resonantly coupled 2(1) - 4 (1) photoassociation resonance in LiRb. This pair of states displays interesting decay physics that hint at interference-like effects caused by two different decay paths. We observe decay to predominantly $X \ ^1Σ^+ \ v=43$, with significant numbers of molecules produced in $X \ ^1Σ^+ \ v=2$ - 12. This photoassociation resonance also produces $\sim$300 $X \ ^1Σ^+ \ v=0 \ J=0$ molecules/second. Finally, we identify a stimulated Raman adiabatic passage transfer pathway from $v=43$ to $v=0$ that has the potential to produce up to $2 \times 10^5$ LiRb mol…
We theoretically study saturation effects induced by an external static electric field on photoassociation (PA) of a heteronuclear atom pair. A static electric field influences scattering wave-function of two heteronuclear atoms as described in [D. Chakraborty, J. Hazra and B. Deb, J. Phys. B. {\bf 44} 095201 (2011)]. For certain values of electric field strengths there exist anisotropic resonances in ground state scattering leading to a large modification of scattering wave-function at short and intermediate separations where photoassociative Franck-Condon overlap is significant. Photoassocia…
We produce ${^{84}\mathrm{Sr}_2}$ molecules using Bose-enhanced Raman photoassociation. We apply the stimulated Raman adiabatic passage (STIRAP) technique on a Bose-Einstein condensate (BEC) to produce more than $8 \times 10^3$ ultracold molecules. This chemical reaction is only made possible because of the Bose enhancement of the optical transition dipole moment between the initial atomic state and an intermediate molecular state. We study the effect of Bose enhancement by measuring the transition Rabi frequency in a BEC and by comparing it with measurements for two atoms in sites of a Mott i…
The Stimulated Raman Adiabatic Passage (STIRAP) procedure is a robust and complete population transfer method which have various application in chemistry and atomic physics. Here, we study the effects of one-photon detuning, transition time, pulse width, and pulse delay parameters on the population transfer via STIRAP and b-STIRAP techniques. Moreover, the impact of the field amplitude which decreases the population transfer has been analyzed and it is shown that in b-STIRAP, the robustness of the complete transition can be improved by decreasing the field amplitude in the single-photon resona…
We report the achievement of stimulated Raman adiabatic passage (STIRAP) in the microwave frequency range between internal states of a Bose-Einstein condensate (BEC) magnetically trapped in the vicinity of an atom chip. The STIRAP protocol used in this experiment is robust to external perturbations as it is an adiabatic transfer, and power-efficient as it involves only resonant (or quasi-resonant) processes. Taking into account the effect of losses and collisions in a non-linear Bloch equations model, we show that the maximum transfer efficiency is obtained for non-zero values of the one- and …
We present an analytic description of the effects of dephasing processes on stimulated Raman adiabatic passage in a tripod quantum system. To this end, we develop an effective two-level model. Our analysis makes use of the adiabatic approximation in the weak dephasing regime. An effective master equation for a two-level system formed by two dark states is derived, where analytic solutions are obtained by utilizing the Demkov-Kunike model. From these, it is found that the fidelity for the final coherent superposition state decreases exponentially for increasing dephasing rates. Depending on the…
The space-time method is applied to a model system-the Simple Harmonic Oscillator in a laser field to simulate the Stimulated Raman Adiabatic Passage (STIRAP) process. The Space-Time method is a computational theory first introduced by Weatherford et. al. to solve Time-Dependent Systems with one boundary value and applied to electron spin system with invariant Hamiltonian [Journal of Molecular Structure {\bf 592} 47]. The implementation in the present work provides an efficient and general way to solve the Time-Dependent Schr{ö}dinger Equation and can be applied to multi-state systems. The alg…
We study two-photon excitation of Rydberg states of atoms under stimulated adiabatic passage with delayed laser pulses. We find that the combination of strong interaction between the atoms in Rydberg state and the spontaneous decay of the intermediate exited atomic state leads to the Rydberg excitation of precisely one atom within the atomic ensemble. The quantum Zeno effect offers a lucid interpretation of this result: the Rydberg blocked atoms repetitively scattering photons effectively monitor a randomly excited atom which therefore remains in the Rydberg state. This system can be used for …
We implement high-efficiency coherent excitation to a Rydberg state using stimulated Raman adiabatic passage in a cold atom electron and ion source. We achieve an efficiency of 60% averaged over the laser excitation volume with a peak efficiency of 82%, a 1.6 times improvement relative to incoherent pulsed-laser excitation. Using pulsed electric field ionization of the Rydberg atoms we create electron bunches with durations of 250 ps. High-efficiency excitation will increase source brightness, crucial for ultrafast electron diffraction experiments, and coherent excitation to high-lying Rydberg…
Optical properties of ensembles of three-level quantum emitters coupled to plasmonic systems are investigated employing a self-consistent model. It is shown that stimulated Raman adiabatic passage (STIRAP) technique can be successfully adopted to control optical properties of hybrid materials with collective effects present and playing an important role in light-matter interactions. We consider a core-shell nanowire comprised of a silver core and a shell of coupled quantum emitters and utilize STIRAP scheme to control scattering efficiency of such a system in a frequency and spatial dependent …
Coherent manipulation of quantum states is of crucial importance in accurate control of a quantum system. A fundamental goal is coherently transferring the population of a desired state with near-unit fidelity. For this propose, we theoretically demonstrate a novel coherent double-stimulated Raman adiabatic passage (STIRAP) in a three-level $Λ$-type system for realizing the switch of unequal initial preparations on two ground states. This operation uses single optical pulse sequence accomplishing both bright-STIRAP and dark-STIRAP process, in which the intermediate-level detuning and the pulse…
State-of-the-art {\em ab initio} techniques have been applied to compute the potential energy curves for the SrYb molecule in the Born-Oppenheimer approximation for the ground state and first fifteen excited singlet and triplet states within the coupled-cluster framework. The leading long-range coefficients describing the dispersion interactions at large interatomic distances are also reported. The electric transition dipole moments have been obtained as the first residue of the polarization propagator computed with the linear response coupled-cluster method restricted to single and double exc…
We show theoretically that it is possible to form a cold molecular ion from a pair of colliding atom and ion at low energy by photoassociative two-photon Raman processes. We explore the possibility of stimulated Raman adiabatic passage (STIRAP) from the continuum of ion-atom scattering states to an ionic molecular state. We provide physical conditions under which coherent population transfer is possible in stimulated Raman photoassociation. Our results are important for experimental realization of PA in ion-atom cold collisions.
Adiabatic passage techniques, used to drive a system from one quantum state into another, find widespread application in physics and chemistry. We focus on techniques to spatially transport a quantum amplitude over a strongly coupled system, such as STImulated Raman Adiabatic Passage (STIRAP) and Coherent Tunnelling by Adiabatic Passage (CTAP). Previous results were shown to work on certain graphs, such as linear chains, square and triangular lattices, and branched chains. We prove that similar protocols work much more generally, in a large class of (semi-)bipartite graphs. In particular, unde…
We survey results on the creation of heteronuclear Fermi molecules by tuning a degenerate Bose-Fermi mixture into the neighborhood of an association resonance, either photoassociation or Feshbach, as well as the subsequent prospects for Cooper-like pairing between atoms and molecules. In the simplest case of only one molecular state, corresponding to either a Feshbach resonance or one-color photoassociation, the system displays Rabi oscillations and rapid adiabatic passage between a Bose-Fermi mixture of atoms and fermionic molecules. For two-color photoassociation, the system admits stimulate…
In the Comment by M. Mackie \textit{et al.} [arXiv: physics/0212111 v.4], the authors suggest that the molecular conversion efficiency in atom-molecule STIRAP can be improved by lowering the initial atomic density, which in turn requires longer pulse durations to maintain adiabaticity. Apart from the fact that the mean-field approximation becomes questionable at low densities, we point out that a low-density strategy with longer pulses has several problems. It generally requires higher pulse energies, and increases radiative losses. We also show that even within the approximations used in the …
Studies on the interactions between an alkali atom and an alkaline earth ion at low energy are important in the field of cold chemistry. In this paper we, extensively, study the structure, interactions, and dynamics of (MgCs)$^+$ molecular ion. We use an ab initio approach based on the formalism of non-empirical pseudo-potential for Mg$^{2+}$ and Cs$^+$ cores, large Gaussian basis sets and full valence configuration interaction. In this context, the (MgCs)$^+$ cation is treated as an effective two-electron system. Potential energy curves and their spectroscopic constants for the ground and the…
We study the many-body dynamics of stimulated Raman adiabatic passage in the presence of on-site interactions. In the classical mean-field limit, explored in Phys. Rev. Lett. {\bf 121}, 250405 (2018), interaction-induced chaos leads to the breakdown of adiabaticity under the quasi-static variation of the parameters, thus producing {\em low} sweep rate boundaries on efficient population transfer. We show that for the corresponding many-body system, alternative quantum pathways from the initial to the target state, open up at even slower sweep rates. These quantum detours avoid the chaotic class…
We report on the direct conversion of laser-cooled 41K and 87Rb atoms into ultracold 41K87Rb molecules in the rovibrational ground state via photoassociation followed by stimulated Raman adiabatic passage. High-resolution spectroscopy based on the coherent transfer revealed the hyperfine structure of weakly bound molecules in an unexplored region. Our results show that a rovibrationally pure sample of ultracold ground-state molecules is achieved via the all-optical association of laser-cooled atoms, opening possibilities to coherently manipulate a wide variety of molecules.
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent \textit{ab-initio} calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold $^{87}$Rb$^{84}$Sr bosonic molecules. First, we have studied the formation by photoassociation followed by spontaneous emission. The photoassociation rates to levels belonging to electronic states converging to the $^{87}$Rb$(5s\,^2S)$+$^{84}$Sr($5s5p\,^3P_{0,1,2}$) …
We theoretically examine the creation of a Fermi-degenerate gas of molecules via a photoassociation or Feshbach resonance applied to a degenerate Bose-Fermi mixture of atoms. This problem raises an interest because, unlike bosons, fermions in general do not behave cooperatively, so that the collective conversion of, say, two million atoms into one million molecules is not to be expected. Nevertheless, we find that the coupled Fermi system displays collective Rabi-like oscillations and adiabatic passage between atoms and molecules, thereby mimicking Bose-Einstein statistics. Cooperative associa…
We review methods for coherently controlling Rydberg quantum states of atomic ensembles using Adiabatic Rapid Passage and Stimulated Raman Adiabatic Passage. These methods are commonly used for population inversion in simple two-level and three-level systems. We show that adiabatic techniques allow us to control population and phase dynamics of complex entangled states of mesoscopic atomic ensembles for quantum information processing with Rydberg atoms. We also propose several schemes of single-qubit and two-qubit gates based on adiabatic passage, Rydberg blockade and Förster resonances in Ryd…
We present schemes for geometric phase compensation in adiabatic passage which can be used for the implementation of quantum logic gates with atomic ensembles consisting of an arbitrary number of strongly interacting atoms. Protocols using double sequences of stimulated Raman adiabatic passage (STIRAP) or adiabatic rapid passage (ARP) pulses are analyzed. Switching the sign of the detuning between two STIRAP sequences, or inverting the phase between two ARP pulses, provides state transfer with well defined amplitude and phase independent of atom number in the Rydberg blockade regime. Using the…
Spatial adiabatic passage processes for ultracold atoms trapped in tunnel-coupled cylindrically symmetric concentric potentials are investigated. Specifically, we discuss the matter-wave analogue of the rapid adiabatic passage (RAP) technique for a high fidelity and robust loading of a single atom into a harmonic ring potential from a harmonic trap, and for its transport between two concentric rings. We also consider a system of three concentric rings and investigate the transport of a single atom between the innermost and the outermost rings making use of the matter-wave analogue of the stimu…
We investigate theoretically the application of Sawtooth Wave Adiabatic Passage (SWAP) in a 1D magneto-optical trap (MOT). As opposed to related methods that have been previously discussed, our approach utilizes repeated cycles of stimulated absorption and emission processes to achieve both trapping and cooling, thereby reducing the adverse effects that arise from photon scattering. Specifically, we demonstrate this method's ability to cool, slow, and trap particles with fewer spontaneously emitted photons, higher forces and in less time when compared to a traditional MOT scheme that utilizes …
We present an analysis of the stimulated Raman adiabatic passage processes based on the methods of differential geometry. The present work was inspired by an excellent article by Bruce W. Shore et al. (R. G. Unanyan, B. W. Shore, and K. Bergmann Phys. Rev. A \textbf{59}, 2910 (1999)). We demonstrate how a purely geometric interpretation of the adiabatic passage in quantum tripod systems as a Riemannian parallel transport of the dark state vector along the Bloch sphere allows describing the evolution of the system for a given sequence of Stokes, pump and control laser excitation pulses. In comb…
Experiments with cold ion-atom mixtures have recently opened the way for the production and application of ultracold molecular ions. Here, in a comparative study, we theoretically investigate ground and several excited electronic states and prospects for the formation of molecular ions composed of a calcium ion and an alkali-metal atom: CaAlk$^{+}$ (Alk=Li, Na, K, Rb, Cs). We use a quantum chemistry approach based on non-empirical pseudopotential, operatorial core-valence correlation, large Gaussian basis sets, and full configuration interaction method for valence electrons. Adiabatic potentia…
