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Communications Physics

Improving the stimulated Raman adiabatic passage efficiency for ultracold 6Li40K ground state molecules

Anbang Yang, Canming He, Xiaoyu Nie, Victor Avalos, Sofia Botsi, Sunil Kumar, Kai Dieckmann

Published Oct 10, 2025• 3 citations
Publisher

Abstract

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.

DOI
10.1038/s42005-025-02309-5

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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.
Efficient Creation of Ultracold Ground State 6Li40K^{6}\textrm{Li}^{40}\textrm{K}6Li40K Polar Molecules
We report the creation of ultracold ground state 6Li40K^{6}\textrm{Li}^{40}\textrm{K}6Li40K polar molecules with high efficiency. Starting from weakly-bound molecules state, stimulated Raman adiabatic passage (STIRAP) is adopted to coherently transfer the molecules to their singlet ro-vibrational ground state ∣X1Σ+,v=0,J=0>|\textrm{X}^{1}Σ^{+},v=0,J=0>∣X1Σ+,v=0,J=0>. By employing a singlet STIRAP pathway and low-phase-noise narrow-linewidth lasers, we observed a one-way transfer efficiency of 96(4)\,\%. Held in an optical dipole trap, the lifetime of the ground-state molecules is measured to be 5.0(3)\,ms. The large permanent dipole moment of LiK is confirmed by applying a DC electric field on the molecules and performing Stark shift spectroscopy of the ground state. With recent advances in the quantum control of collisions, our work paves the way for exploring quantum many-body physics with strongly-interacting 6Li40K^{6}\textrm{Li}^{40}\textrm{K}6Li40K molecules.
We report the creation of ultracold ground state ^{6}Li^{40}K polar molecules with high efficiency. Starting from weakly bound molecules, stimulated Raman adiabatic passage is adopted to coherently transfer the molecules to their singlet rovibrational ground state |X^{1}Σ^{+},v=0,J=0⟩. By employing a singlet stimulated Raman adiabatic passage pathway and low-phase-noise narrow-linewidth lasers, we observed a one-way transfer efficiency of 96(4)%. Held in an optical dipole trap, the lifetime of the ground state molecules is measured to be 5.0(3) ms. The large permanent dipole moment of LiK is confirmed by applying a dc electric field on the molecules and performing Stark shift spectroscopy of the ground state. With recent advances in the quantum control of collisions, our work paves the way for exploring quantum many-body physics with strongly interacting ^{6}Li^{40}K molecules.
A quantum gas of ultracold molecules, with long-range and anisotropic interactions, will enable a series of fundamental studies in physics and chemistry. In particular, samples of ground-state molecules at ultralow temperatures and high number densities will facilitate the explorations of a large number of many-body physical phenomena and applications in quantum information processing. However, due to the lack of efficiently cooling techniques such as laser cooling for atomic gases, high number densities for ultracold molecular samples are not readily attainable. Associating ultracold atoms to weakly bound dimer molecules via Feshbach resonance and subsequently transferring them to a wanted molecular ro-vibronic ground state by a stimulated Raman adiabatic passages (STIRAP) have proved to be an effective way in producing ideal ultracold molecular samples. As a typical illustration, in a recent study (2010 Nat. Phys. 6 265) Danzl et al. experimentally realized the preparation of Cs2 molecule into its ro-vibronic ground state via two different multi-level STIRAPs:one is based on a single conversion route and the others are based on a cascade-connected route (labeled by 4p-STIRAP and s-STIRAP, respectively). In this work, we present a theoretical study for these two STIRAP schemes, focusing on the differences in physical principle and realistic performance between them. On the one hand, according to the theoretical approach of quasi-dark eigenstates, we conclude that a highly efficient population transfer is achievable in both schemes. On the other hand, by systematically studying the influences of the relevant parameters, including the spontaneous decays and the detunings from the intermediate states, and the temporal sequence and the amplitude of the laser pulses, we disclose their respective advantages and weaknesses in the realistic implementation. We theoretically predict that for both schemes their maximal conversion efficiencies each can attain 0.97 as long as the spontaneous decays from the intermediate excited states are sufficiently suppressed. Yet considering the fact that the already implemented efficiency is only around 0.6 for both schemes, there is still room for optimization, e.g. using stable Rydberg energy levels in future experiment. Furthermore, the success of these two schemes can provide a new route to the controllable entanglement preparation, opening more applications in the fields of quantum logic gate and so on.
We develop a theoretical description of photoassociative stimulated Raman adiabatic passage (STIRAP) near a Feshbach resonance in a thermal atomic gas. We show that it is possible to use low-intensity laser pulses to directly excite pairs of atoms in the continuum near a Feshbach resonance and to transfer most of the atomic cloud to the lowest rovibrational level of the molecular ground state. For a broad resonance, commonly found in several mixtures of alkali atoms, our model predicts a transfer efficiency up to 97% for a given atom pair, and up to 70% when averaged over an atomic ensemble. The laser intensities and pulse durations needed for such an optimal transfer, 10 2 –10 3 W cm −2 and several microseconds, are easily achievable experimentally. A single pair of STIRAP pulses converts an estimated fraction f ∼10 −6 –10 −4 of atoms in an atomic ensemble, leading to the production of 10–1000 molecules in a large sample of 10 7 atoms. A total of ∼10 4 –10 6 pulse pairs are thus required to transfer most atoms into molecules. Such an efficiency compares with or surpasses currently available techniques for creating stable diatomic molecules, and the versatility of this approach simplifies its potential use for many molecular species.
In this paper, we carry out the non-Hermitian stimulated Raman shortcut-to-adiabatic passage (NH-STIRSAP) to create ultracold deeply-bound molecules. The open three-level molecular system is supposed to have irreversible decays out of all levels. Under the assumption of large single-photon detuning and/or strong loss rate of the excited level, the NH three-level system can be theoretically reduced to an effective two-level system. By continuously using the counter-diabatic driving of the shortcut-to-adiabaticity, an auxiliary field is produced to couple the Feshbach level with the ground level. In the numerical calculations, we firstly consider the case of decaying only from the excited level, which is the main loss of the system. Under the NH-STIRSAP, the calculations reveal that complete population transfer from the Feshbach to the ground level can occur even if the adiabatic condition is not fulfilled. Therefore, the creation efficiency of ultracold deeply-bound molecules is greatly improved. The results hold equally for counter-intuitive and intuitive time sequence of the Stokes and pump pulse. If the decays from the Feshbach and ground level are also included, the NH-STIRSAP can still restore most of that efficiency, which performs much better than typical stimulated Raman adiabatic passage. Finally, we point out that the robustness and fast transfer speed of the NH-STIRSAP facilitate the creation and detection of ultracold deeply-bound molecules.