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arXiv:2510.22875 · Physical Review A

Control of valence-electron motion in Xe cations using the stimulated-Raman-adiabatic-passage technique

Miguel A. Alarcón, Karl Hauser, Nikolay V. Golubev

Published Dec 18, 2025• 2 citations

Abstract

This work theoretically investigates possibilities of using the Stimulated Raman Adiabatic Passage (STIRAP) and its variants to control a coherent superposition of quantum states. We present a generalization of the so-called fractional STIRAP (f-STIRAP), demonstrating precise control over the mixing ratio of quantum states in the wave packet. In contrast to conventional f-STIRAP, designed to drive a system from an eigenstate into a coherent superposition, our scheme enables arbitrary control over the composition of an already existing superposition state. We demonstrate that an approximate version of this technique -- where analytically designed laser pulses with composite envelopes are replaced by simple Gaussian pulses -- achieves comparable performance in controlling the dynamics of the wave packet. A limiting case of this scheme, utilizing two pulses with identical Gaussian envelopes and tuned delay and relative phase, is also explored, revealing experimentally accessible pathways for manipulating quantum coherence. We apply our developed techniques to control the ultrafast charge migration in the spin-orbit split ground electronic states of xenon cation via intermediate valence- and core-excited states. Finally, we propose concrete experimental realizations of the developed control schemes in combination with attosecond transient absorption spectroscopy as a method to probe the system.

DOI: 10.1103/2k75-h2pm

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We discuss the properties of a simple and robust scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states - fractional stimulated Raman adiabatic passage (fractional STIRAP) - first proposed by Marte et al (1991 Phys. Rev. A 44 R4118). As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, here the two pulses terminate simultaneously, while maintaining a constant ratio of amplitudes. We extend earlier research and suggest a realization of this scheme with two smoothly varying delayed laser pulses (which can be derived from a single laser), the parameters of the created superposition being controlled by the polarization of the delayed pulse. Furthermore, we provide simple analytic estimates of the robustness of this process against variations in the laser intensity, laser frequency and pulse delay. Finally, we discuss an extension to multistate systems which provides a possibility for creating coherent superpositions of more than two states.

We discuss a simple scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states. The technique, which we call fractional stimulated Raman adiabatic passage ({\it f-STIRAP}), is based upon (incomplete) adiabatic population transfer between an initial state

ψ_1

and state

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through an intermediate state

ψ_2

. As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, the two pulses terminate simultaneously while maintaining a constant ratio of amplitudes. The independence of f-STIRAP from details of pulse shape and pulse area makes it the analog of conventional STIRAP in the creation of coherent superpositions of states. We suggest a smooth realization of f-STIRAP which requires only two laser pulses (which can be derived from a single laser) and at the same time ensures the automatic fulfillment of the asymptotic conditions at early and late times. Furthermore, we provide simple analytic estimates of the robustness of f-STIRAP against variations in the pulse intensity, the pulse delay, and the intermediate-state detuning, and discuss its possible extension to multistate systems.

We introduce a high-fidelity technique for coherent control of three-state quantum systems, which combines two popular control tools---stimulated Raman adiabatic passage (STIRAP) and composite pulses. By using composite sequences of pairs of partly delayed pulses with appropriate phases, the nonadiabatic transitions, which prevent STIRAP from reaching unit fidelity, can be canceled to an arbitrary order by destructive interference, and therefore, the technique can be made arbitrarily accurate. The composite phases are given by simple analytic formulas, and they are universal for they do not depend on the specific pulse shapes, the pulse delay, and the pulse areas.

Coherent manipulation of quantum states is of crucial importance in accurate control of a quantum system. A fundamental goal is coherently transferring the population of a desired state with near-unit fidelity. For this purpose, we theoretically demonstrate a novel coherent double-stimulated Raman adiabatic passage (STIRAP) in a three-level Λ-type system for realizing the switch of unequal initial preparations on two ground states. This operation uses a single optical pulse sequence accomplishing both bright-STIRAP and dark-STIRAP processes, in which the intermediate-level detuning and the pulse delay must be given an optimal adjustment. Besides, owing to the imperfection of double-STIRAP transition, the sensitivity of the switch fidelity with respect to the spontaneous loss from the intermediate state, to the pulse amplitude and to the population difference, is also discussed. This work suggests a simple and experimentally feasible all-optical approach to switch a superposition quantum state, serving as one-step closer to the goal of coherent manipulation of quantum systems.

Stimulated Raman adiabatic passage (STIRAP) is a widely-used technique of coherent state-to-state manipulation for many applications in physics, chemistry, and beyond. The adiabatic evolution of the state involved in STIRAP, called adiabatic passage, guarantees its robustness against control errors, but also leads to problems of low efficiency and decoherence. Here we propose and experimentally demonstrate an alternative approach, termed stimulated Raman "user-defined" passage (STIRUP), where a parameterized state is employed for constructing desired evolutions to replace the adiabatic passage in STIRAP. The user-defined passages can be flexibly designed for optimizing different objectives for different tasks, e.g. minimizing leakage error. To experimentally benchmark its performance, we apply STIRUP to the task of coherent state transfer in a superconducting Xmon qutrit. We found that STIRUP completed the transfer more then four times faster than STIRAP with enhanced robustness, and achieved a fidelity of 99.5%, which is the highest among all recent experiments based on STIRAP and its variants. In practice, STIRUP differs from STIRAP only in the design of driving pulses; therefore, most existing applications of STIRAP can be readily implemented with STIRUP.

The rovibrational dynamics of an extended ladder stimulated Raman adiabatic passage (STIRAP) system through permanent dipole moment transitions is investigated theoretically using the time-dependent quantum-wave-packet method for the ground electronic state of the HF molecule. The calculated results show that nearly 100

%

of the population can be transferred to the target state through (1+2), (1+3), and (2+2) STIRAP schemes. By choosing a suitable excitation pathway, the effects of the background states on the final population of the target state can be removed. For the multiphoton STIRAP process, the one-photon overtone pump scheme is more efficient than the two-photon pump scheme in controlling the population transfer to the target state.