Resonant Coupling in the Heteronuclear Alkali Dimers for Direct Photoassociative Formation of X(0,0) Ultracold Molecules

Stwalley, William C.; Banerjee, Jayita; Bellos, Michael; Carollo, Ryan; Recore, Matthew; Mastroianni, Michael

doi:10.1021/jp901803f

Cited by 42 publications

(39 citation statements)

References 31 publications

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“…This process provides continuous production and accumulation of the absolute ground state molecules without complicated transfer techniques. Finally the observation of suitable pairs of resonantly coupled states for KRb, together with related observations in LiCs, NaCs and RbCs, inspires confidence that similar pathways can be found for other heteronulcear molecules as predicted in [15].…”

Section: Discussionsupporting

confidence: 71%

“…Such states occur if there is a strong resonant coupling between specific vibrational levels of two appropriate excited electronic states. This phenomenon has been observed in Rb 2 [12], Cs 2 [13], RbCs [14] and is theoretically predicted for many heteronuclear dimers [15]. In NaCs [10], this phenomenon is believed to lead the formation of molecules in the rovibronic ground state.…”

Section: Introductionmentioning

confidence: 51%

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Direct photoassociative formation of ultracold KRb molecules in the lowest vibrational levels of the electronic ground state

et al. 2012

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We report continuous direct photoassociative formation of ultracold KRb molecules in the lowest vibrational levels (v ′′ = 0 − 10) of the electronic ground state (X 1 Σ + ), starting from 39 K and 85 Rb atoms in a magneto-optical trap. The process exploits a newfound resonant coupling between the 2(1), v ′ = 165 and 4(1), v ′ = 61 levels, which exhibit an almost equal admixture of the uncoupled eigenstates. The production rate of the X 1 Σ + (v ′′ =0) level is estimated to be 5 × 10 3 molecules/sec.

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Section: Discussionsupporting

confidence: 71%

Section: Introductionmentioning

confidence: 51%

Direct photoassociative formation of ultracold KRb molecules in the lowest vibrational levels of the electronic ground state

et al. 2012

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“…The most spectacular experimental achievements on ultracold dipolar molecular gases have been performed on KRb molecules [8,9,11,19] which motivated a wealth of theoretical investigations on this species [17,[20][21][22][23]. An * maxence.lepers@u-psud.fr accurate description of long-range interactions involving the other heteronuclear alkali diatoms is strongly needed since they draw rising attention [24][25][26][27][28][29][30][31][32]. Considering two identical polar molecules at large distances R (in atomic units 1 a.u.…”

Section: Introductionmentioning

confidence: 99%

Long-range interactions between polar alkali-metal diatoms in external electric fields

et al. 2013

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We computed the long-range interactions between two identical polar bialkali molecules in their rovibronic ground level, for all ten species involving Li, Na, K, Rb and Cs, using accurate quantum chemistry results combined with available spectroscopic data. Huge van der Waals interaction is found for eight species in free space. The competition of the van der Waals interaction with the dipole-dipole interaction induced by an external electric field parallel or perpendicular to the intermolecular axis is investigated by varying the electric field magnitude and the intermolecular distance. Our calculations predict a regime with the mutual orientation of the two molecules but with no preferential direction in the laboratory frame. A mechanism for the stimulated one-photon radiative association of a pair of ultracold polar molecules into ultracold tetramers is proposed, which would open the way towards the optical manipulation of ultracold polyatomic molecules.

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“…The resonance coupling of the B(1) 1 Π and 2 1 Π states of KRb (see, Fig. 1) is found to be a promising pathway for direct photoassociative formation of the X(0, 0) ultracold molecules 5 . The rigorous multi-channel modeling of the laser formation of vibrationally cold KRb molecules has been accomplished in Ref.…”

Section: Introductionmentioning

confidence: 98%

Twofold diabatization of the KRb(1–2)Π1complex in the framework ofab initioand deperturbation approaches

2016

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The twofold diabatization of the KRb (1 ∼ 2) We performed a diabatization of the mutually perturbed 1 1 Π and 2 1 Π states of KRb based on both electronic structure calculation and direct coupled-channel deperturbation analysis of experimental energies. The potential energy curves (PECs) of the diabatic states and their scalar coupling were constructed from the ab initio adiabatic PECs by analytically integrating the radial ψ ad 1 |∂/∂R|ψ ad 2 matrix element obtained by a finite-difference method. The diabatic potentials and electronic coupling function were refined by the least squares fitting of the rovibronic termvalues of the 1 1 Π ∼ 2 1 Π complex. The empirical PECs combined with the coupling function as well as the diabatized spin-orbit coupling and transition dipole matrix elements are useful for further deperturbation treatment of both singlet and triplet states manifold. I. INTRODUCTIONThe accurate representation of the interacting electronic states plays a key role in understanding the detailed mechanism of the photo and collisionally induced chemical reactions. The singlet-triplet levels of alkali metal dimers serve as an intermediate state in the two step optical transformation of the weakly bound atomic pairs into the absolute ground X 1 Σ + (v = 0, J = 0) molecular state 1,2 . To suppress the undesired spontaneous transitions to the low-lying states a coherent stimulated Raman adiabatic passage 3 (STIRAP) is often used.The photoassociative production and trapping of ultracold KRb molecules has been performed 4 . The resonance coupling of the B(1) 1 Π and 2 1 Π states of KRb (see, Fig. 1) is found to be a promising pathway for direct photoassociative formation of the X(0, 0) ultracold molecules 5 . The rigorous multi-channel modeling of the laser formation of vibrationally cold KRb molecules has been accomplished in Ref. 6 9,10 to the lowest X(0, 0) level through the B 1 Π ∼ c 3 Σ + levels located near the second dissociation threshold.A comprehensive review of modern spectroscopic studies of the KRb electronic states can be found in the ebook 12 . The mutually perturbed 1 1 Π and 2 1 Π states converging to the second K(4 2 S)+Rb(5 2 P) and third K(4 2 P)+Rb(5 2 S) dissociation thresholds were investigated 13,14 using Doppler-free optical-optical double resonance polarization spectroscopy (OODRPS). In the sub- 15,16 included in the present CC deperturbation analysis. The inset enlarges the region in the vicinity of the crossing point of V1(R) and V2(R) diabatic PECs.The adiabatic potentials, permanent and transition dipole moments for the radially coupled 1 1 Π and 2 1 Π states were first ab initio calculated in Refs 19 and 20. The comprehensive set of non-relativistic PECs, permanent and transition dipole moments for the ground and excited states of KRb are available 11,21-25 as well. The SOC effect has been included into ab initio calculations in Refs. 6,11,24,and 26. Among other alkali diatomics, the KRb molecule stands out because of the high density of the electronic states belonging to both...

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Resonant Coupling in the Heteronuclear Alkali Dimers for Direct Photoassociative Formation of X(0,0) Ultracold Molecules

Cited by 42 publications

References 31 publications

Direct photoassociative formation of ultracold KRb molecules in the lowest vibrational levels of the electronic ground state

Direct photoassociative formation of ultracold KRb molecules in the lowest vibrational levels of the electronic ground state

Long-range interactions between polar alkali-metal diatoms in external electric fields

Twofold diabatization of the KRb(1–2)Π1complex in the framework ofab initioand deperturbation approaches

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