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Physical Review A

Progress toward full optical control of ultracold-molecule formation: Role of scattering Feshbach resonances

R. Lefèbvre, Osman Atabek

Published Jun 15, 2020• 4 citations
Publisher

Abstract

Feshbach resonances play a major role in translationally cold-molecule preparation. In this context, their laser control is of crucial importance. This work is devoted to the depiction of some basic mechanisms of such a control using intense, short laser pulses and referring to nonlinear multiphoton processes. Our goal is to adiabatically transport a Feshbach resonance onto a zero-width resonance, the characteristics of which have already been discussed in the literature. Three processes are then addressed: (i) during the rise of the pulse and its plateau, the preparation of a so-called laser bound molecule (LBM) still stable, but structurally different from the standard chemically bound molecule; (ii) during the pulse switching off, an adiabatic transport of this LBM on a very few excited vibrational levels, and (iii) concomitantly, a filtration strategy to photodissociate all these levels except one, giving thus rise to but a single field-free excited vibrational state. With or without an eventual stimulated Raman adiabatic passage technique to bring all the population to the ground rovibrational state, this opens an alternate for a full optical control of ultracold-molecule formation. The illustrative example, offering the potentiality to be transposed to other diatomics, is ${\mathrm{H}}_{2}^{+}$.

DOI
10.1103/physreva.101.063406

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Feshbach resonances play a major role in translationally cold-molecule preparation. In this context, their laser control is of crucial importance. This work is devoted to the depiction of some basic mechanisms of such a control using intense, short laser pulses and referring to nonlinear multiphoton processes. Our goal is to adiabatically transport a Feshbach resonance onto a zero-width resonance, the characteristics of which have already been discussed in the literature. Three processes are then addressed: (i) during the rise of the pulse and its plateau, the preparation of a so-called laser bound molecule (LBM) still stable, but structurally different from the standard chemically bound molecule; (ii) during the pulse switching off, an adiabatic transport of this LBM on a very few excited vibrational levels, and (iii) concomitantly, a filtration strategy to photodissociate all these levels except one, giving thus rise to but a single field-free excited vibrational state. With or without an eventual stimulated Raman adiabatic passage technique to bring all the population to the ground rovibrational state, this opens an alternate for a full optical control of ultracold-molecule formation. The illustrative example, offering the potentiality to be transposed to other diatomics, is H2+{\mathrm{H}}_{2}^{+}H2+​.
In molecular photodissociation, some specific combinations of laser parameters (wavelength and intensity) lead to unexpected zero-width resonances (ZWRs) with, in principle, infinite lifetimes. Their potential to induce basic quenching mechanisms has recently been devised in the laser control of vibrational cooling through filtration strategies [O. Atabek et al., Phys. Rev. A 87, 031403(R) (2013)]. A full quantum adiabatic control theory based on the adiabatic Floquet Hamiltonian is developed to show how a laser pulse could be envelope-shaped and frequency-chirped so as to protect a given initial vibrational state against dissociation, taking advantage of its continuous transport on the corresponding ZWR all along the pulse duration. As compared with previous control scenarios that actually suffered from nonadiabatic contamination, drastically different and much more efficient filtration goals are achieved. A semiclassical analysis helps us to find and interpret a complete map of ZWRs in the laser parameter plane. In addition, the choice of a given ZWR path, among the complete series identified by the semiclassical approach, turns out to be crucial for the cooling scheme, targeting a single vibrational state population left at the end of the pulse, while all others have almost completely decayed. The illustrative example, which has the potential to be transposed to other diatomics, is Na2{\mathrm{Na}}_{2}Na2​ prepared by photoassociation in vibrationally hot but translationally and rotationally cold states.
Abstract We investigate theoretically the formation of an ultracold CsYb molecule in the absolute ground state by full optical control. The laser-assisted self-induced Feshbach resonance takes place when the trap state in the optical lattice is coupled with a rovibrational state of the ground electronic state. The Feshbach molecule is formed in the resonant rovibrational state via an adiabatic population transfer by ramping the frequency of a chirped pulse. Two schemes are designed to prepare the absolute ground-state molecule starting from the Feshbach molecule: a pump–dump scheme controlled by short pulses and a stimulated-Raman-adiabatic-passage (STIRAP) scheme steered by long pulses. The probabilities of converting the Feshbach molecule to the absolute ground state molecule by using the pump–dump and the STIRAP schemes are 16% and 99%, respectively.
In recent experiments on ultracold matter, molecules have been produced from ultracold atoms by photoassociation, Feshbach resonances, and three-body recombination. The created molecules are translationally cold, but vibrationally highly excited. This will eventually lead them to be lost from the trap due to collisions. We propose shaped laser pulses to transfer these highly excited molecules to their ground vibrational level. Optimal control theory is employed to find the light field that will carry out this task with minimum intensity. We present results for the sodium dimer. The final target can be reached to within 9999%99 provided the initial guess field is physically motivated. We find that the optimal fields contain the transition frequencies required by a good Franck-Condon pumping scheme. The analysis identifies the ranges of intensity and pulse duration which are able to achieve this task before any other competing processes take place. Such a scheme could produce stable ultracold molecular samples or even stable molecular Bose-Einstein condensates.
We propose a type of Feshbach resonance occurring when two different ultracold atoms in their ground state undergo an sss-wave collision in the presence of a laser. The collisional levels of the atom pair are coupled by the laser to a rovibrational molecular level of the same electronic ground state: We name it a laser-assisted self-induced Feshbach resonance. This mechanism, valid for all heteronuclear quantum gas mixtures, is analyzed on the example of ultracold 87Rb^{87}\mathrm{Rb}87Rb and 84Sr^{84}\mathrm{Sr}84Sr atoms for which the resonant laser frequency falls in the subterahertz range. The interspecies scattering length can be controlled with the laser frequency and intensity without atom loss. Moreover, chirping slowly, the frequency allows for the adiabatic formation of ultracold 87Rb84Sr^{87}\mathrm{Rb}\phantom{\rule{0.16em}{0ex}}^{84}\mathrm{Sr}87Rb84Sr molecules in a manner very similar to a magnetic Feshbach resonance. A stimulated Raman adiabatic passage follows for stabilizing the molecules in their rovibronic ground state.
We have studied the formation of ultracold RbSr molecules with laser pulses. After discussing the advantages of the Mott insulator phase for the control with pulses, we present two classes of strategies. The first class involves two electronic states. Two extensions of stimulated Raman adiabatic passage (STIRAP) for multilevel transitions are used: alternating STIRAP (A-STIRAP) and straddle STIRAP (S-STIRAP). Both transfer dynamics are modeled and compared. The second class of strategies involves only the electronic ground state and uses infrared (IR) and terahertz (THz) pulses. The molecular bond is first created by the application of a THz chirped pulse or $\ensuremath{\pi}$-pulse. Subsequently, the molecules are transferred to their rovibrational ground level using IR pulses. For this last step, different optimized pulse sequences that were obtained through optimal control techniques have been studied. The relative merits of these strategies in terms of efficiency and robustness are discussed with respect to the experimental feasibility based on present laser technologies.
One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.