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arXiv:2310.14499 · The Journal of Chemical Physics

Highly efficient creation and detection of deeply bound molecules via invariant-based inverse engineering with feasible modified drivings

Jiahui Zhang

Published Jan 8, 2024• 2 citations
arXivHTMLPDF

Abstract

Stimulated Raman Adiabatic Passage (STIRAP) and its variants, such as M-type chainwise-STIRAP, allow for efficiently transferring the populations in a multilevel system and have widely been used to prepare molecules in their rovibrational ground state. However, their transfer efficiencies are generally imperfect. The main obstacle is the presence of losses and the requirement to make the dynamics adiabatic. To this end, in the present paper, a new theoretical method is proposed for the efficient and robust creation and detection of deeply bound molecules in three-level Λ-type and five-level M-type systems via "Invariant-based shortcut-to-adiabaticity." In the regime of large detunings, we first reduce the dynamics of three- and five-level molecular systems to those of effective two- and three-level counterparts. By doing so, the major molecular losses from the excited states can be well suppressed. Consequently, the effective two-level counterpart can be directly compatible with two different "Invariant-based Inverse Engineering" protocols; the results show that both protocols give a comparable performance and have a good experimental feasibility. For the effective three-level counterpart, by considering a relation among the four incident pulses, we show that this model can be further generalized to an effective Λ-type one with the simplest resonant coupling. This generalized model permits us to borrow the "Invariant-based Inverse Engineering" protocol from a standard three-level Λ-type system to a five-level M-type system. Numerical calculations show that the weakly bound molecules can be efficiently transferred to their deeply bound states without strong laser pulses, and the stability against parameter variations is well preserved. Finally, the detection of ultracold deeply bound molecules is discussed.

DOI
10.1063/5.0183063

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Stimulated Raman Adiabatic Passage (STIRAP) and its variants, such as M-type chainwise-STIRAP, allow for efficiently transferring the populations in a multilevel system and have widely been used to prepare molecules in their rovibrational ground state. However, their transfer efficiencies are generally imperfect. The main obstacle is the presence of losses and the requirement to make the dynamics adiabatic. To this end, in the present paper, a new theoretical method is proposed for the efficient and robust creation and detection of deeply bound molecules in three-level Λ-type and five-level M-type systems via "Invariant-based shortcut-to-adiabaticity." In the regime of large detunings, we first reduce the dynamics of three- and five-level molecular systems to those of effective two- and three-level counterparts. By doing so, the major molecular losses from the excited states can be well suppressed. Consequently, the effective two-level counterpart can be directly compatible with two different "Invariant-based Inverse Engineering" protocols; the results show that both protocols give a comparable performance and have a good experimental feasibility. For the effective three-level counterpart, by considering a relation among the four incident pulses, we show that this model can be further generalized to an effective Λ-type one with the simplest resonant coupling. This generalized model permits us to borrow the "Invariant-based Inverse Engineering" protocol from a standard three-level Λ-type system to a five-level M-type system. Numerical calculations show that the weakly bound molecules can be efficiently transferred to their deeply bound states without strong laser pulses, and the stability against parameter variations is well preserved. Finally, the detection of ultracold deeply bound molecules is discussed.
Chainwise stimulated Raman adiabatic passage (C-STIRAP) in a M-type molecular system is a good alternative in creating ultracold deeply bound molecules when the typical STIRAP in a $\mathrm{\ensuremath{\Lambda}}$-type system does not work due to weak Frank-Condon factors between states. However, its creation efficiency under smooth evolution is generally low. During the process, the population in the intermediate states may decay out quickly and the strong laser pulses may induce multiphoton processes. In this paper, we find that the shortcut to adiabaticity (STA) fits very well in improving the performance of the C-STIRAP. Currently, related discussions on the so-called chainwise stimulated Raman shortcut-to-adiabatic passage (C-STIRSAP) are rare. Here, we investigate this topic under adiabatic elimination. Given a relation among the four incident pulses, it is quite interesting that the M-type system can be generalized into an effective $\mathrm{\ensuremath{\Lambda}}$-type structure with the simplest resonant coupling. Consequently, all possible methods of STA for the three-state system can be borrowed. We take the counterdiabatic driving and ``chosen path'' methods as instances to demonstrate our treatment of the molecular system. Although the chosen path method does not work well in a real three-state system if there is strong decay in the excited state, our C-STIRSAP protocol under both methods can create ultracold deeply bound molecules with high efficiency in the M-type system. The evolution time is shortened without strong laser pulses and the robustness of STA is well preserved. Finally, the detection of ultracold deeply bound molecules is discussed.
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.
In this paper, a theoretical method for the efficient creation and detection of deeply bound molecules in three-state ΛΛΛ-type and five-state M-type molecular systems is proposed. The method is based on the three-state coincident pulses technique and the generalized five-state coincident pulses technique. For the three-state system, the technique can efficiently transfer the populations from the Feshbach state to the deeply-bound state via a train of NNN pairs of resonant and coincident pump and Stokes pulses, with negligible transient populations of excited states. For the five-state system, it is found that this M-type system can be generalized into a ΛΛΛ-type structure with the simplest resonant coupling under the assumption of large one-photon detuning together with a requirement of the relation among the four incident pulses. Thereafter, this generalized model permits us to employ the reduced three-state propagator to design four coincident pulses to achieve the desired population transfer. For the numerical study, 87^{87}87Rb2_22​ is considered and, it is shown that the weakly-bound Feshbach molecules can be efficiently transferred to their deeply-bound states without strong laser pulses, and the populations of all intermediate states can be well suppressed.
The stimulated Raman adiabatic passage (STIRAP) shows an efficient technique that accurately transfers population between two discrete quantum states with the same parity, in three-level quantum systems based on adiabatic evolution. This technique has widely theoretical and experimental applications in many fields of physics, chemistry, and beyond. Here, we present a generally robust approach to speed up STIRAP with invariant-based shortcut to adiabaticity. By controlling the dynamical process, we inversely design a family of Hamiltonians that can realize fast and accurate population transfer from the first to the third level, while the systematic error is largely suppressed in general. Furthermore, a detailed trade-off relation between the population of the intermediate state and the amplitudes of Rabi frequencies in the transfer process is illustrated. These results provide an optimal route toward manipulating the evolution of three-level quantum systems in future quantum information processing.
Abstract Stimulated Raman adiabatic passage allows robust transfer between two ends of a three-state quantum system and has been employed to transfer weakly bound Feshbach molecules into their deeply bound rovibrational ground state. However, the efficient transfer remains to be explored. Here we propose a possible alternative route, based on a recently developed non-Hermitian shortcut to adiabaticity method. It is able to realize single-step transfer efficiencies up to 100% even in the presence of a decaying excited level, surpassing all the previous methods. We also prove that our scheme is robust against the external field parameter fluctuations and is expected to be applicable for abundant molecular species.
We suggest and analyze a technique for efficient and robust creation of dense ultracold molecular ensembles in their ground rovibrational state. In our approach a molecule is brought to the ground state through a series of intermediate vibrational states via a multistate chainwise stimulated Raman adiabatic passage technique. We study the influence of the intermediate states decay on the transfer process and suggest an approach that minimizes the population of these states, resulting in a maximal transfer efficiency. As an example, we analyze the formation of 87Rb2^{87}\mathrm{Rb}_{2}87Rb2​ starting from an initial Feshbach molecular state and taking into account major decay mechanisms due to inelastic atom-molecule and molecule-molecule collisions. Numerical analysis suggests a transfer efficiency >90>90%>90, even in the presence of strong collisional relaxation as are present in a high density atomic gas.