We theoretically investigate the effect of anomalous quantum correlations on the light-induced frequency shift in the photoassociation spectrum of a Bose-Einstein condensate (BEC). Anomalous quantum correlations arise because, although formed from a pair of zero-momentum condensate atoms, a condensate molecule need not dissociate back to the BEC, but may just as well form a noncondensate atom pair with equal and opposite momentum, i.e., due to rogue photodissociation. The uncorrelated frequency shift of the photoassociation spectrum is to the red and linearly dependent on the laser intensity. In contrast, anomalous correlations due to rogue dissociation lead to a blueshifted photoassociation spectrum. For sufficiently low light intensities, the rogue blueshift is dominant and proportional to the squareroot of intensity.
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 simulate numerically the photodissociation of molecules into noncondensate atom pairs that accompanies photoassociation of an atomic Bose-Einstein condensate into a molecular condensate. Such rogue photodissociation sets a limit on the achievable rate of photoassociation. Given the atom density ρand mass m, the limit is approximately 6\hbarρ^{2/3}/m. At low temperatures this is a more stringent restriction than the unitary limit of scattering theory.
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…
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 …
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 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 convers…
We briefly report on zero-temperature photoassociation of a Bose-Einstein condensate, focusing on the many-body rate limit for atom-molecule conversion. An upgraded model that explicitly includes spontaneous radiative decay leads to an unanticipated shift in the position of the photoassociation resonance, which affects whether the rate (constant) maximizes or saturates, as well as the limiting value itself. A simple analytical model agrees with numerical experiments, but only for high density. Finally, an explicit comparison with the two-body unitary limit, set by the size of the condensate, f…
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
We report on the high resolution photoassociation spectroscopy of a $^{87}$Rb spin-1 Bose-Einstein condensate to the $1_\mathrm{g} (P_{3/2}) v = 152$ excited molecular states. We demonstrate the use of spin dependent photoassociation to experimentally identify the molecular states and their corresponding initial scattering channel. These identifications are in excellent agreement with the eigenvalues of a hyperfine-rotational Hamiltonian. Using the observed spectra we estimate the change in scattering length and identify photoassociation laser light frequency ranges that maximize the change in…
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…
We report the high resolution photoassociation (PA) spectroscopy of a $^{87}Rb$ Bose-Einstein condensate (BEC) to excited molecular states near the dissociation limit of $5P_{1/2} +5S_{1/2}$ by optical Bragg scattering. Since the detection of optical Bragg scattering in BEC has a high signal-noise ratio, we obtain the high resolution PA spectrum of excited molecular states in the range of $\pm1$ GHz near the dissociation limit of $5P_{1/2} +5S_{1/2}$. We compare the results with the conventional method of trap loss and show that the results agree each other very well. Many interesting phenomen…
We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate. When the magnetic field is far-off resonance, cross coupling between the two target molecules--enabled by the shared dissociation continuum--leads to an anomalous dispersive shift in the position of laser resonance, as well as unprecedented elimination and enhancement of resonant photoassociation via quantum interference. For off-resonant lasers, a dispersive shift and quantum interference appear similarly in resonant three-body Feshbach losses, except that the Feshbach node is tunable with intensity.
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…
Quantum degenerate molecules represent a new paradigm for fundamental studies and practical applications. Association of already quantum degenerate atoms into molecules provides a crucial shortcut around the difficulty of cooling molecules to ultracold temperatures. Whereas association can be induced with either laser or magnetic fields, photoassociation requires impractical laser intensity to overcome poor overlap between the atom pair and molecular wavefunctions, and experiments are currently restricted to magnetoassociation. Here we model realistic production of a quantum degenerate gas of …
We demonstrate coherent one-color photoassociation of a Bose-Einstein condensate, which results in Rabi oscillations between atomic and molecular condensates. We attain atom-molecule Rabi frequencies that are comparable to decoherence rates by driving photoassociation of atoms in an $^{88}$Sr condensate to a weakly-bound level of the metastable $^{1}S_{0}+^{3}P_{1}$ molecular potential, which has a long lifetime and large Franck-Condon overlap integral with the ground scattering state. Transient shifts and broadenings of the excitation spectrum are clearly seen at short times, and they create …
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…
Cold quantum gases, when acted upon by electromagnetic fields, can give rise to samples where isolated atoms coexist with dimers or trimers, which raises the question of the interactions between these various constituents. Here we perform microwave photoassociation in a degenerate gas of $^{87}$Rb atoms to create weakly-bound dimers in their electronic ground state. From the density-induced shift of the photoassociation line, we measure the atom-dimer scattering length for the two least-bound states of the molecular potential. We also determine the complete energy diagram of one hyperfine mani…
Coherent control of reactants remains a longstanding challenge in quantum chemistry. In particular, we have studied laser-induced molecular formation (photoassociation) in a Raman-dressed spin-orbit-coupled 87Rb Bose-Einstein condensate, whose spin quantum state is a superposition of multiple bare spin components. In contrast to the notably different photoassociation-induced fractional atom losses observed for the bare spin components of a statistical mixture, a superposition state with a comparable spin composition displays the same fractional loss on every spin component. We interpret this a…
We show theoretically that it is possible to optically control collective spin-exchange processes in spinor Bose condensates through virtual photoassociation. The interplay between optically induced spin exchange and spin-dependent collisions provides a flexible tool for the control of atomic spin dynamics, including enhanced or inhibited quantum spin oscillations, the optically-induced ferromagnetic-to-antiferromagnetic transition, and coherent matter-wave spin conversion.
We theoretically examine the neutral atom-molecule analogue of the anomalous quantum correlations between degenerate electrons, i.e., Cooper pairs, that are responsible for superconductivity. Based on rogue dissociation of triatomic molecules (trimers) into opposite-momentum pairs of atoms and diatomic molecules (dimers) via a photoassociation or Feshbach resonance, we find a superfluid transition to a Bose-Einstein condensate of trimers dressed by atom-dimer Cooper pairs, at a critical temperature in reach of present ultracold technology.
We demonsatrate an all optical technique to evaporatively produce sodium Bose-Einstein condensates (BEC). We use a crossed-dipole trap formed from light near 1060 nm, and a simple ramp of the intensity to force evaporation. In addition, we introduce photoassociation as diagnostic of the trap loading process, and show that it can be used to detect the onset of Bose-Einstein condensation. Finally, we demonstrate the straightforward production of multiple traps with condensates using this technique, and that some control over the spinor state of the BEC is achieved by positioning the trap as well…
We discuss the dynamics of an atomic Bose-Einstein condensate when pairs of atoms are converted into molecules by single-color photoassociation. Three main regimes are found and it is shown that they can be understood on the basis of time-dependent two-body theory. In particular, the so-called rogue dissociation regime [Phys. Rev. Lett., 88, 090403 (2002)], which has a density-dependent limit on the photoassociation rate, is identified with a transient regime of the two-atom dynamics exhibiting universal properties. Finally, we illustrate how these regimes could be explored by photoassociating…
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 theoretically examine two-color photoassociation of a Bose-Einstein condensate, focusing on the role of rogue decoherence in the formation of macroscopic atom-molecule superpositions. Rogue dissociation occurs when two zero-momentum condensate atoms are photoassociated into a molecule, which then dissociates into a pair of atoms of equal-and-opposite momentum, instead of dissociating back to the zero-momentum condensate. As a source of decoherence that may damp quantum correlations in the condensates, rogue dissociation is an obstacle to the formation of a macroscopic atom-molecule superpos…
We develop the idea of manipulating the scattering length $a$ in low-temperature atomic gases by using nearly resonant light. As found, if the incident light is close to resonance with one of the bound $p$ levels of electronically excited molecule, then virtual radiative transitions of a pair of interacting atoms to this level can significantly change the value and even reverse the sign of $a$. The decay of the gas due to photon recoil, resulting from the scattering of light by single atoms, and due to photoassociation can be minimized by selecting the frequency detuning and the Rabi frequency…
