Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Photoassociation: From a quasicontinuum model to coherent matter optics

Matthew Mackie

Published Oct 1, 1999• 1 citation
OpenAlex

Abstract

We consider the process of photoassociation (PA) that occurs when a pair of colliding atoms interacts with a photon, thereby making a transition from the two-atom continuum to a bound molecular state. Such free-bound transitions are described by quantizing the molecule's dissociation continuum, and coupling each of these quasicontinuum (QC) levels to a similarly discrete molecular level. The correct free-atom results are recovered no later than at the end of a given calculation by taking the limit as the QC spacing tends to zero. From the quasicontinuum model, we are led to adapt the few-level and second-quantization methods of photon optics to analyze free-bound transitions. In particular, we establish the PA density parameter as nearly identical to the phase-space parameter as a Bose-Einstein condensate (BEC), illustrate the near-unit efficiency of one- and two-color photoassociation of a BEC, and develop coherent atom-molecule transitions as the matter optics version of second-harmonic generated photons. ^

Related papers

Quasicontinuum modeling of photoassociation

Matt Mackie, Juha Javanainen

We analyze photoassociation theoretically by treating the dissociation continuum of a molecule as a quasicontinuum (QC) of discrete states. In this manner, free-bound transitions are reduced to a few-level problem. The correct continuum limit is deduced from an explicit analysis of the density of QC states. Besides giving the usual photoassociation rate, the QC model facilitates the analysis of the steady-state molecular yield. Moreover, complications such as velocity redistribution and line broadening due to atom-atom collisions may be treated basically in the same way as in connection with the customary two-level atom. Next we adapt the standard three-level quantum optics to describe free-bound-bound photoassociation for both continuous-wave and pulsed two-color excitation. For a quantum degenerate gas of atoms, a proper two-photon resonant scheme may transform atoms to ground state molecules with near-unit efficiency even in the presence of spontaneous losses from the intermediate state.

Physical Review A•Oct 1, 1999•53 citations

Theory of coherent photoassociation of a Bose-Einstein condensate

Marijan Koštrun, Matt Mackie, Robin Côté +1 more

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). The 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 the field theory for atoms and molecules is used to demonstrate that, in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of density fluctuations. Experimental complications, including spontaneous emission and unwanted ``rogue'' photodissociation from a photoassociated molecule, are analyzed. A two-color Raman scheme is studied as a method to set up an effective two-mode scheme with reduced spontaneous-emission losses. We discuss photoassociation rates and photoassociation Rabi frequencies for high-lying vibrational states in alkali dimers both on the basis of molecular-structure calculations, and by comparing with an experiment [Wynar et al., Science 287, 1016 (2000)].

arXiv:physics/0006066•Physical Review A•Nov 15, 2000•86 citations

Theory of atom-molecule Bose-Einstein condensate

Marijan Koštrun

A study of coherent photoassociation is presented for the case of an atomic Bose-Einstein condensate. It is shown that the phenomenon is analogous to coherent optical transient in a few-level system, with a difference that the participating levels have Bose enhanced populations. A second-quantized Hamiltonian in momentum and position representation is developed to describe photoassociation. A classical version of the field theory for atoms and molecules is used to demonstrate that in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of the density fluctuations. ^ A simple mean-field model of atom-molecule Bose-Einstein condensate is constructed and it is shown that in the model there is no collapse, irrespective of the sign of the effective atom-atom scattering length. The properties of the two most important eigenstates, the ground state and the twin state, are determined for different values of the system parameters δ and K, the detuning and the atom-molecule coupling, respectively. It is shown that in a coupled atom-molecule system a collapse is replaced by a dynamical instability. The lines in the parameter space where these instabilities occur are in fact fractures where the underlying eigenstates discontinuously change. The features of instability are in good qualitative agreement with the experimental observations of collapse. ^

•Jan 1, 2002•1 citation

Manipulating Quantum States of Molecules Created via Photoassociation of Bose-Einstein Condensates

Xiaoting Zhou, Xiong-Jun Liu, Hui Jing +2 more

We show the quantum state transfer technique in two-color photoassociation (PA) of a Bose-Einstein condensate, where a quantized field is used to couple the free-bound transition from atom state to excited molecular state. Under the weak excitation condition, we find that quantum states of the quantized field can be transferred to the created molecular condensate. The feasibility of this technique is confirmed by considering the atomic and molecular decays discovered in the current PA experiments. The present results allow us to manipulate quantum states of molecules in the photoassociation of a Bose-Einstein condensate.

arXiv:quant-ph/0701080•Jan 14, 2007•0 citations

Probability of photoassociation from a quasicontinuum approach

Juha Javanainen, Matt Mackie

We examine photoassociation by using a quasicontinuum to describe the colliding atoms. The quasicontinuum system is analyzed using methods adapted from the theory of laser spectroscopy and quantum optics, and a continuum limit is then taken. In a degenerate gas the equilibrium probability of photoassociation may be close to unity. In the continuum limit, for a thermal atomic sample, the stimulated Raman adiabatic passage (STIRAP) mechanism cannot be employed to eliminate unwanted spontaneous transitions.

Physical Review A•Aug 1, 1998•64 citations

Bose-Stimulated Raman Adiabatic Passage in Photoassociation

Matt Mackie, Ryan Kowalski, Juha Javanainen

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 raises an interest because STIRAP has been predicted to be absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. Nevertheless, we find that 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 efficiency.

arXiv:physics/9909060•Physical Review Letters•Apr 24, 2000•160 citations
We consider the process of photoassociation (PA) that occurs when a pair of colliding atoms interacts with a photon, thereby making a transition from the two-atom continuum to a bound molecular state. Such free-bound transitions are described by quantizing the molecule's dissociation continuum, and coupling each of these quasicontinuum (QC) levels to a similarly discrete molecular level. The correct free-atom results are recovered no later than at the end of a given calculation by taking the limit as the QC spacing tends to zero. From the quasicontinuum model, we are led to adapt the few-level and second-quantization methods of photon optics to analyze free-bound transitions. In particular, we establish the PA density parameter as nearly identical to the phase-space parameter as a Bose-Einstein condensate (BEC), illustrate the near-unit efficiency of one- and two-color photoassociation of a BEC, and develop coherent atom-molecule transitions as the matter optics version of second-harmonic generated photons. ^
We analyze photoassociation theoretically by treating the dissociation continuum of a molecule as a quasicontinuum (QC) of discrete states. In this manner, free-bound transitions are reduced to a few-level problem. The correct continuum limit is deduced from an explicit analysis of the density of QC states. Besides giving the usual photoassociation rate, the QC model facilitates the analysis of the steady-state molecular yield. Moreover, complications such as velocity redistribution and line broadening due to atom-atom collisions may be treated basically in the same way as in connection with the customary two-level atom. Next we adapt the standard three-level quantum optics to describe free-bound-bound photoassociation for both continuous-wave and pulsed two-color excitation. For a quantum degenerate gas of atoms, a proper two-photon resonant scheme may transform atoms to ground state molecules with near-unit efficiency even in the presence of spontaneous losses from the intermediate state.
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). The 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 the field theory for atoms and molecules is used to demonstrate that, in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of density fluctuations. Experimental complications, including spontaneous emission and unwanted ``rogue'' photodissociation from a photoassociated molecule, are analyzed. A two-color Raman scheme is studied as a method to set up an effective two-mode scheme with reduced spontaneous-emission losses. We discuss photoassociation rates and photoassociation Rabi frequencies for high-lying vibrational states in alkali dimers both on the basis of molecular-structure calculations, and by comparing with an experiment [Wynar et al., Science 287, 1016 (2000)].
A study of coherent photoassociation is presented for the case of an atomic Bose-Einstein condensate. It is shown that the phenomenon is analogous to coherent optical transient in a few-level system, with a difference that the participating levels have Bose enhanced populations. A second-quantized Hamiltonian in momentum and position representation is developed to describe photoassociation. A classical version of the field theory for atoms and molecules is used to demonstrate that in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of the density fluctuations. ^ A simple mean-field model of atom-molecule Bose-Einstein condensate is constructed and it is shown that in the model there is no collapse, irrespective of the sign of the effective atom-atom scattering length. The properties of the two most important eigenstates, the ground state and the twin state, are determined for different values of the system parameters δ and K, the detuning and the atom-molecule coupling, respectively. It is shown that in a coupled atom-molecule system a collapse is replaced by a dynamical instability. The lines in the parameter space where these instabilities occur are in fact fractures where the underlying eigenstates discontinuously change. The features of instability are in good qualitative agreement with the experimental observations of collapse. ^
We show the quantum state transfer technique in two-color photoassociation (PA) of a Bose-Einstein condensate, where a quantized field is used to couple the free-bound transition from atom state to excited molecular state. Under the weak excitation condition, we find that quantum states of the quantized field can be transferred to the created molecular condensate. The feasibility of this technique is confirmed by considering the atomic and molecular decays discovered in the current PA experiments. The present results allow us to manipulate quantum states of molecules in the photoassociation of a Bose-Einstein condensate.
We examine photoassociation by using a quasicontinuum to describe the colliding atoms. The quasicontinuum system is analyzed using methods adapted from the theory of laser spectroscopy and quantum optics, and a continuum limit is then taken. In a degenerate gas the equilibrium probability of photoassociation may be close to unity. In the continuum limit, for a thermal atomic sample, the stimulated Raman adiabatic passage (STIRAP) mechanism cannot be employed to eliminate unwanted spontaneous transitions.
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 raises an interest because STIRAP has been predicted to be absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. Nevertheless, we find that 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 efficiency.