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A pump–probe study of the photoassociation of cold rubidium molecules

Jovana S. Petrovic, David J. McCabe, Duncan G. England, Hugo E. L. Martay, Melissa E. Friedman, Alexander J. Dicks, Emiliya Dimova, Ian A. Walmsley

Published Jan 1, 2009• 5 citations
Publisher

Abstract

The dynamics of the excited state during the photoassociation of cold molecules from cold rubidium atoms is studied in a series of pump-probe experiments. Dipole transitions similar to those of the atoms are observed in the molecular signal. While such behaviour is characteristic of the long-range molecules, the photoassociation of bound molecules is confirmed in additional experiments. The pump-probe signal observed on a 250 ps time scale did not, however, reveal wavepacket oscillations predicted by theory. This result is discussed using numerical simulations of photoassociation and a modification to the current experiments that could lead to the detection of wavepacket dynamics is suggested.

DOI
10.1039/b818494a

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The dynamics of the excited state during the photoassociation of cold molecules from cold rubidium atoms is studied in a series of pump-probe experiments. Dipole transitions similar to those of the atoms are observed in the molecular signal. While such behaviour is characteristic of the long-range molecules, the photoassociation of bound molecules is confirmed in additional experiments. The pump-probe signal observed on a 250 ps time scale did not, however, reveal wavepacket oscillations predicted by theory. This result is discussed using numerical simulations of photoassociation and a modification to the current experiments that could lead to the detection of wavepacket dynamics is suggested.
The establishment of robust laser-cooling techniques for the formation of ultracold atoms has provided a test-bed for low-temperature science, with scattering events changing character from incoherent thermal interactions to coherent quantum mechanical events. A natural extension is the pursuit of ultracold molecules in prescribed low-energy internal states. Atomic cooling techniques, however, do not generalize to the molecular regime due to the complex energy-level structure afforded by its extra degrees of motion. An indirect approach to ultracold molecule formation - photoassociation using ultrafast laser pulses - is the focus of this thesis. A broadband field associates atom pairs into a localized molecular wavepacket that evolves within the attractive excited-state potential. A suitably timed dump pulse may thus be applied to stabilize population into deeply bound ground vibrational states. This strategy may be generalized to any species whose spectroscopy matches the pulse spectrum, and offers a coherent population transfer scheme that does not require precise knowledge of the system. This thesis presents experiments using high-energy photoassociation pulses applied to ultracold rubidium atoms. The pulses quench the background ground-state molecular population but form bound dimers within the excited state. A pump-probe experiment was designed to chart the excited-state dynamics; however, the oscillations predicted by theoretical calculations were not evident in the molecular signal. The nature of the dynamics is expected to be strongly dependent on the initial state of the atom pairs addressed by the ultrafast pulse: a bound molecular population provides an additional candidate to free atoms. A spectroscopic measurement characterizes these bound molecules and identifies their formation mechanism. A subsequent experiment provides evidence that the predominant contributor to the pump-probe signal is the unbound initial population. The consequences with regard to both the observation of excited-state dynamics and the subsequent application of a dump pulse are discussed.
The complexity of ultrafast molecular photoionization presents an obstacle to the modeling of pump-probe experiments. Here, a simple optimized model of atomic rubidium is combined with a molecular dynamics model to predict quantitatively the results of a pump-probe experiment in which long-range rubidium dimers are first excited, then ionized after a variable delay. The method is illustrated by the outline of two proposed feasible experiments and the calculation of their outcomes. Both of these proposals use Feshbach 87Rb^{87}\mathrm{Rb}87Rb2{}_{2}2​ molecules. We show that long-range molecular pump-probe experiments should observe spin-orbit precession given a suitable pump pulse, and that the associated high-frequency beat signal in the ionization probability decays after a few tens of picoseconds. If the molecule was to be excited to only a single fine-structure state, then a low-frequency oscillation in the internuclear separation would be detectable through the time-dependent ionization cross section, giving a mechanism that would enable observation of coherent vibrational motion in this molecule.
Pump-probe experiments are performed in which cold colliding Na atoms are photoassociated to form Na2{\mathrm{Na}}_{2}Na2​ molecules, and subsequently ionized. The experiments are performed in a regime where the pulsed photoassociation to an intermediate potential takes place at long range, and to several electronic, vibrational, and rotational states. A probe pulse then produces an ionization signal by further exciting these molecules to autoionizing doubly excited states. The time dependence of the ion signal shows a dramatic flux-enhancement effect on a nanosecond time scale due to the motion on the intermediate potentials. This time dependence can be viewed as monitoring the inward motion and dephasing of a population wave packet formed at long range.
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the spectral cut position to the asymptotic transition frequency of the rubidium D1 or D2 lines, respectively. Measurements of the molecular photoassociation signal as a function of the pulse energy reveal a non-linear dependence and indicate a non-perturbative excitation process. Chirping the association laser pulse allowed us to change the phase of the coherent transients. Furthermore, a signature for molecules in the electronic ground state is found, which is attributed to molecule formation by femtosecond photoassociation followed by spontaneous decay. In a subsequent article [A. Merli et al., submitted] quantum mechanical calculations are presented, which compare well with the experimental data and reveal further details about the observed coherent transient dynamics.
The expansion of laser cooling capabilities from the atomic to the molecular regime has proven challenging due to the lack of availability of an equivalent closed-loop cooling cycle within the rich molecular internal energy level structure. An enticing solution is the application of ultrafast coherent control techniques to ultracold molecule generation. Unlike continuous-wave photoassociation techniques, the use of broadband 'pump' and 'dump' pulses offers the opportunity to access deeply bound vibrational states. Unlike alternative vibrational cooling strategies such as stimulated Raman adiabatic passage or incoherent optical cycling, this approach preserves coherence and does not require a detailed knowledge of the system spectroscopy. We report on pump-probe experiments investigating the dynamical evolution of bound excited-state Rb2dimers after photoassociation. Learning about these dynamics is an important step towards efficient pump-dump formation of deeply bound ground-state molecules. Based on a spectroscopic measurement of the initial state occupied by the interacting atom pairs, we provide evidence that background triplet molecules preassociated by the trapping lasers, additionally to unbound scattering atom pairs, may play an important role in photoassociation dynamics.
An experimental pump-probe study of the photoassociative creation of translationally ultracold rubidium molecules is presented together with numerical simulations of the process. The formation of loosely bound excited-state dimers is observed as a first step toward a fully coherent pump-dump approach to the stabilization of Rb2{\text{Rb}}_{2}Rb2​ into its lowest ground vibrational states. The population that contributes to the pump-probe process is characterized and found to be distinct from a background population of preassociated molecules.