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arXiv:cond-mat/0108121 · Physical Review A

Photoassociative frequency shift in a quantum degenerate gas

Jordan M. Gerton, Brian J. Frew, Randall G. Hulet

Published Oct 15, 2001• 44 citations
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Abstract

A light-induced frequency shift is observed in single-photon photoassociative spectra of magnetically trapped, quantum degenerate ${}^{7}\mathrm{Li}.$ The shift is a manifestation of the coupling between the threshold continuum scattering states and discrete bound levels in the excited-state molecular potential induced by the photoassociation laser. The frequency shift is observed to be linear in the laser intensity with a measured proportionality constant that is in good agreement with theoretical predictions. This phenomenon has important implications for a scheme to alter the interactions between atoms in a Bose-Einstein condensate using photoassociation resonances.

DOI
10.1103/physreva.64.053410

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A light-induced frequency shift is observed in single-photon photoassociative spectra of magnetically trapped, quantum degenerate 7Li.{}^{7}\mathrm{Li}.7Li. The shift is a manifestation of the coupling between the threshold continuum scattering states and discrete bound levels in the excited-state molecular potential induced by the photoassociation laser. The frequency shift is observed to be linear in the laser intensity with a measured proportionality constant that is in good agreement with theoretical predictions. This phenomenon has important implications for a scheme to alter the interactions between atoms in a Bose-Einstein condensate using photoassociation resonances.
An experiment studying the effects of photoassociation in a quantum degenerate gas of 7Li bosons has been performed in a permanent magnet trap. A saturation in the one-photon photoassociation rate and a shift in the resonance due to the applied light field from the 2S 1/2 ground state to the 2P1/2 v ' = 83 excited molecular vibrational state have been measured and compared with theory. Limitations in the ability of the permanent magnet apparatus to study photoassociation in a Bose-Einstein condensate have prompted the development of a magneto-optical trap and an electro-magnetic trap. These new traps will assist in the process of creating a large BEC where the effects of photoassociation will be studied.
We observe light-induced frequency shifts in one-color photoassociative spectra of magnetically trapped 4 He* atoms in the metastable 2 3 S 1 state. A pair of ultracold spin-polarized 2 3 S 1 helium atoms is excited into a molecular bound state in the purely long-range 0 u + potential connected to the 2 3 S 1 -2 3 P 0 asymptote. The shift arises from the optical coupling of the molecular excited bound state with the scattering states and the bound states of two colliding 2 3 S 1 atoms. We measure the frequency-shifts for several ro-vibrational levels in the 0 u + potential and find a linear dependence on the photoassociation laser intensity. Comparison with a theoretical analysis provides a good indication for the s -wave scattering length a of the quintet ( 5 Σ g + ) potential, a = 7.2 ± 0.6 nm, which is significantly lower than most previous results obtained by non-spectroscopic methods.
Molecular spectroscopy is used to probe a quantum degenerate gas of 7Li atoms. Several effects are investigated using both single-color and two-color (Raman) photoassociative spectroscopy. An unusual spectral shift with laser intensity is observed for single-color photoassociation and the intensity dependence agrees with theoretical predictions. Additionally, the prospects for altering the interactions between ground-state atoms is investigated for both the single-color and Raman schemes. The single-color scheme is found to be impractical experimentally (although feasible theoretically) while the Raman scheme may be experimentally feasible as well. The Raman spectra display an interesting lineshape which is found to reflect the rate for inelastic collisions involving ground-state molecules (produced via the Raman process) as well as the attractive mean-field interactions between atoms in the condensate. Under certain circumstances, a dispersive Raman lineshape is observed which may be due to coherence properties of both the condensate and the thermal gas. Additionally, the Raman lineshape appears to reflect the kinetic time scale for thermal atoms to enter the condensate via elastic collisions. The Raman technique is applied to studies of the condensate growth and collapse dynamics caused by attractive interactions between condensate atoms, and enables the first direct observations of this phenomenon.
Herein, we report on the experimental observations and a quantitative determination of the laser-induced frequency shift (LIFS) in the photoassociation (PA) spectra of spinor Bose-Einstein condensate of sodium. Our investigations revealed a nonlinear dependence of the LIFS on the intensity of PA laser. By developing a model within the quadratic Stark effect, we simulate the experimental results via a theoretical model that confirms the former. The experimental observations and the theoretical analysis can further improve the accuracy of investigations on important molecular properties and on preparation of specific molecular states, with possible applications in various key fields.
We measure the effect of a magnetic Feshbach resonance (FR) on the rate and light-induced frequency shift of a photoassociation resonance in ultracold 7Li. The photoassociation-induced loss-rate coefficient K_{p} depends strongly on magnetic field, varying by more than a factor of 10;{4} for fields near the FR. At sufficiently high laser intensities, K_{p} for a thermal gas decreases with increasing intensity, while saturation is observed for the first time in a Bose-Einstein condensate. The frequency shift is also strongly field dependent and exhibits an anomalous blueshift for fields just below the FR.
The rate of photoassociation (PA) determines how quickly molecules form from atoms illuminated by a resonant laser pulse. Knowledge of limits of this molecular formation rate provide a fundamental component on the maximum rate that a tightly bound ground state molecular Bose-Einstein condensate (BEC) could be formed using a two-photon transition. This molecular synthesis represents the beginning of a new era of ultracold quantum chemistry. The available Feshbach resonance in this system is an indispensable tool to increase the molecular formation rate due to PA in the anticipation of revealing these fundamental rate limits. While the rate saturates in a thermal gas, no evidence of saturation has yet been observed in a BEC. A loss of atoms due to a PA pulse tuned to the v " = 83 excited state molecular vibrational level provides the measurement of the PA rate. The rate varies by several orders of magnitude either by tuning the magnetic field near a Feshbach resonance or by adjusting the PA intensity. We measure the PA rate at magnetic fields between 550-900 Gauss in a BEC and a thermal gas, which is near the Feshbach resonance at 736 Gauss. The rapidly changing rate near the Feshbach resonance reflects the overlap between the ground state and the excited state wavefunctions. We present the first quantitative measurement of the PA rate near a Feshbach resonance. We measure the magnetic field dependence of the molecular resonance position near the Feshbach resonance. We introduce the first observation of a positive energy shift associated with photoassociation. The measured energy shift asymptotically diverges as it approaches the Feshbach resonance and agrees qualitatively with described theory at all magnetic fields. We observe intensity dependent saturation in the PA rate in a thermal gas and the measurements qualitatively agree with a unitarity limited rate. The first conclusive evidence for a suppression of the PA rate occurs for intensities above the saturation intensity. We report the first observed saturation of the PA rate in a BEC. Three separate theories present possible mechanisms for the observed saturation.