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arXiv:1906.05974 · Physical Review Letters

Observation of Interference between Resonant and Detuned stirap in the Adiabatic Creation of Na23K40 Molecules

Lan Liu, De-Chao Zhang, Huan Yang, Ya-Xiong Liu, Jue Nan, Jun Rui, Bo Zhao, Jian-Wei Pan

Published Jun 25, 2019• 38 citations

Abstract

Stimulated Raman adiabatic passage (stirap) allows efficiently transferring the populations between two discrete quantum states and has been used to prepare molecules in their rovibrational ground state. In realistic molecules, a well-resolved intermediate state is usually selected to implement the resonant stirap. Because of the complex molecular level structures, the detuned stirap always coexists with the resonant stirap and may cause unexpected interference phenomenon. However, it is generally accepted that the detuned stirap can be neglected if compared with the resonant stirap. Here we report on the first observation of interference between the resonant and detuned stirap in the adiabatic creation of ^{23}Na^{40}K ground-state molecules. The interference is identified by observing that the number of Feshbach molecules after a round-trip stirap oscillates as a function of the hold time, with a visibility of about 90%. This occurs even if the intermediate excited states are well resolved, and the single-photon detuning of the detuned stirap is about 1 order of magnitude larger than the linewidth of the excited state and the Rabi frequencies of the stirap lasers. Moreover, the observed interference indicates that if more than one hyperfine level of the ground state is populated, the stirap prepares a coherent superposition state among them, but not an incoherent mixed state. Further, the purity of the hyperfine levels of the created ground state can be quantitatively determined by the visibility of the oscillation.

DOI: 10.1103/physrevlett.122.253201

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Stimulated Raman adiabatic passage (stirap) allows efficiently transferring the populations between two discrete quantum states and has been used to prepare molecules in their rovibrational ground state. In realistic molecules, a well-resolved intermediate state is usually selected to implement the resonant stirap. Because of the complex molecular level structures, the detuned stirap always coexists with the resonant stirap and may cause unexpected interference phenomenon. However, it is generally accepted that the detuned stirap can be neglected if compared with the resonant stirap. Here we report on the first observation of interference between the resonant and detuned stirap in the adiabatic creation of ^{23}Na^{40}K ground-state molecules. The interference is identified by observing that the number of Feshbach molecules after a round-trip stirap oscillates as a function of the hold time, with a visibility of about 90%. This occurs even if the intermediate excited states are well resolved, and the single-photon detuning of the detuned stirap is about 1 order of magnitude larger than the linewidth of the excited state and the Rabi frequencies of the stirap lasers. Moreover, the observed interference indicates that if more than one hyperfine level of the ground state is populated, the stirap prepares a coherent superposition state among them, but not an incoherent mixed state. Further, the purity of the hyperfine levels of the created ground state can be quantitatively determined by the visibility of the oscillation.

Inspired by a recent experiment [Phys. Rev. Lett. 122 253201(2019)] that an unprecedented quantum interference was observed in the way of stimulated Raman adiabatic passage (STIRAP) due to the coexisting resonant- and detuned-STIRAPs, we comprehensively study this effect. Our results uncover the scheme robustness towards any external-field fluctuations coming from laser intensity noise and imperfect resonance condition, as well as the persistence of high-contrast interference pattern even when more nearby excited levels are involved. We verify that an auxiliary dynamical phase accumulated in hold time caused by the presence of the quasi-dark state in detuned-STIRAP can sensitively manipulate the visibility and frequency of the interference pattern, representing a new hallmark to measure the hyperfine energy accurately. The robust stability of the scheme comes from the intrinsic superiority embedded in the STIRAP mechanism that preserves the coherence of population transfer, which promises a remarkable performance of quantum interference in a practical implementation.

We theoretically study the generation of coherence in generalized two-level atoms with hyperfine structure by utilizing the detuning-induced stimulated Raman adiabatic passage (D-STIRAP). As expected, the degree of attainable coherence between the ground and excited states cannot be as large as that for the ideal two-level atoms without hyperfine structure. However, we find that the substantial degree of coherence can still be produced with small modulations, and the modulation period is essentially determined by the hyperfine splittings in the ground and excited states. The D-STIRAP scheme in generalized two-level atoms is sufficiently robust against the various parameters such as intensities of lasers, initial detuning, time delay between the laser pulses, and Doppler broadening. As a specific example, we show realistic results for the

{D}_{1}

transition of Na.

Inspired by a recent experiment [Phys. Rev. Letts. \textbf{122}, 253201(2019)] that an unprecedented quantum interference was observed in the way of Stimulated Raman adiabatic passage (STIRAP) due to the coexisting resonant- and detuned-STIRAPs, we comprehensively study this effect for uncovering its robustness towards the external-field fluctuations of laser noise, imperfect resonance condition as well as the excited-state decaying. We verify that, an auxiliary dynamical phase accumulated in hold time caused by the quasi-dark state can sensitively manipulate the visibility and frequency of the interference fringe, representing a new hallmark to measure the hyperfine energy accurately. The robust stability of scheme comes from the intrinsic superiority embedded in STIRAP itself, which promises a remarkable preservation of the quantum interference quality in a practical implementation.

Abstract Ultracold polar molecules represent a rapidly advancing platform at the forefront of quantum simulation, quantum computation, quantum chemistry, and precision measurement. We report an experimental investigation for improving the creation efficiency of ultracold 6Li40K ground state molecules using stimulated Raman adiabatic passage (STIRAP). We address laser amplitude/phase noise and polarization impurity to improve STIRAP efficiency. The phase noise of our two Raman lasers is suppressed effectively by extending the cavity length for the external-cavity diode lasers (ECDLs). Further, we find that even a weak polarization impurity significantly reduces the STIRAP efficiency on the single-photon resonance (Δ = 0) for 6Li40K, due to coupling to undesired molecular levels. However, STIRAP efficiencies over 90% can be achieved by increasing Δ/2π to 10 MHz, which is comparable to the excited-state scattering rate. Our work holds significance for achieving efficient STIRAP transfer in ultracold molecules with unresolved excited-state hyperfine splittings and large scattering rates.

We explore theoretically the rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) in molecular electronic states including both the rotational and the vibrational degrees of freedom, with the LiH molecule as an example. By using a pure rovibrational state as initial state, we find that, under the condition of two-photon resonance, an efficient rovibrational population transfer can be achieved via STIRAP in molecular electronic states and the desired target state can be selected by adjusting laser-pulse parameters. Besides the interested rovibrational states, however, some unwanted rovibrational states may affect population transfer process, especially while the two-photon detuning is taken into account. By inspecting the evolution process of wave packet, we can easily search these unwanted rovibrational states and study their influences. Moreover, the effect of rotational temperature on the population transfer process is discussed using thermal mixed state as initial state.

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.