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The Journal of Chemical Physics

Perspective: Stimulated Raman adiabatic passage: The status after 25 years

Klaas Bergmann, Nikolay V. Vitanov, Bruce W. Shore

Published May 1, 2015• 194 citations
Publisher

Abstract

The first presentation of the STIRAP (stimulated Raman adiabatic passage) technique with proper theoretical foundation and convincing experimental data appeared 25 years ago, in the May 1st, 1990 issue of The Journal of Chemical Physics. By now, the STIRAP concept has been successfully applied in many different fields of physics, chemistry, and beyond. In this article, we comment briefly on the initial motivation of the work, namely, the study of reaction dynamics of vibrationally excited small molecules, and how this initial idea led to the documented success. We proceed by providing a brief discussion of the physics of STIRAP and how the method was developed over the years, before discussing a few examples from the amazingly wide range of applications which STIRAP now enjoys, with the aim to stimulate further use of the concept. Finally, we mention some promising future directions.

DOI
10.1063/1.4916903

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The first presentation of the STIRAP (stimulated Raman adiabatic passage) technique with proper theoretical foundation and convincing experimental data appeared 25 years ago, in the May 1st, 1990 issue of The Journal of Chemical Physics. By now, the STIRAP concept has been successfully applied in many different fields of physics, chemistry, and beyond. In this article, we comment briefly on the initial motivation of the work, namely, the study of reaction dynamics of vibrationally excited small molecules, and how this initial idea led to the documented success. We proceed by providing a brief discussion of the physics of STIRAP and how the method was developed over the years, before discussing a few examples from the amazingly wide range of applications which STIRAP now enjoys, with the aim to stimulate further use of the concept. Finally, we mention some promising future directions.
The procedure of stimulated-Raman adiabatic passage (STIRAP), one of many well-established techniques for quantum-state manipulation, finds widespread application in chemistry, physics, and information processing. Numerous reviews discuss these applications, the history of its development, and some of the underlying physics. This tutorial supplies material useful as background for the STIRAP reviews as well as related techniques for adiabatic manipulation of quantum structures, with emphasis on the theory and simulation rather than on experimental results. It particularly emphasizes the picturing of behavior in various abstract vector spaces, wherein torque equations offer intuition about adiabatic changes. Appendices provide brief explanations of related coherent-excitation topics and useful evaluations of relative strengths of coherent transitions—the Rabi frequencies—involving Zeeman sublevels.
Abstract STIRAP (stimulated Raman adiabatic passage) is a powerful laser-based method, usually involving two photons, for efficient and selective transfer of populations between quantum states. A particularly interesting feature is the fact that the coupling between the initial and the final quantum states is via an intermediate state, even though the lifetime of the latter can be much shorter than the interaction time with the laser radiation. Nevertheless, spontaneous emission from the intermediate state is prevented by quantum interference. Maintaining the coherence between the initial and final state throughout the transfer process is crucial. STIRAP was initially developed with applications in chemical dynamics in mind. That is why the original paper of 1990 was published in The Journal of Chemical Physics . However, from about the year 2000, the unique capabilities of STIRAP and its robustness with respect to small variations in some experimental parameters stimulated many researchers to apply the scheme to a variety of other fields of physics. The successes of these efforts are documented in this collection of articles. In Part A the experimental success of STIRAP in manipulating or controlling molecules, photons, ions or even quantum systems in a solid-state environment is documented. After a brief introduction to the basic physics of STIRAP, the central role of the method in the formation of ultracold molecules is discussed, followed by a presentation of how precision experiments (measurement of the upper limit of the electric dipole moment of the electron or detecting the consequences of parity violation in chiral molecules) or chemical dynamics studies at ultralow temperatures benefit from STIRAP. Next comes the STIRAP-based control of photons in cavities followed by a group of three contributions which highlight the potential of the STIRAP concept in classical physics by presenting data on the transfer of waves (photonic, magnonic and phononic) between respective waveguides. The works on ions or ion strings discuss options for applications, e.g. in quantum information. Finally, the success of STIRAP in the controlled manipulation of quantum states in solid-state systems, which are usually hostile towards coherent processes, is presented, dealing with data storage in rare-earth ion doped crystals and in nitrogen vacancy (NV) centers or even in superconducting quantum circuits. The works on ions and those involving solid-state systems emphasize the relevance of the results for quantum information protocols. Part B deals with theoretical work, including further concepts relevant to quantum information or invoking STIRAP for the manipulation of matter waves. The subsequent articles discuss the experiments underway to demonstrate the potential of STIRAP for populating otherwise inaccessible high-lying Rydberg states of molecules, or controlling and cooling the translational motion of particles in a molecular beam or the polarization of angular-momentum states. The series of articles concludes with a more speculative application of STIRAP in nuclear physics, which, if suitable radiation fields become available, could lead to spectacular results.
This paper begins with the premise that stimulated Raman adiabatic passage (STIRAP) from one state to another by coupling to an intermediate state necessarily requires some population of that intermediate state. The usual view of the process depends on having no population in the intermediate state, but a simple argument from the time-dependent Schr\"odinger equation shows that such adiabatic transfer cannot occur. From another perspective, removing the time dependence of the Hamiltonian by making the rotating frame transformation cancels the optical frequency oscillations but does not account for the envelopes of the pulses commonly used for STIRAP. By assuming a small but finite intermediate state amplitude ${\ensuremath{\varepsilon}}_{1}$ in the wave function, the propagator for the evolution between initial and final states is derived. Applying the propagator to the initial state produces a single compact formula for the final intermediate-state population that is readily evaluated for an arbitrary choice of laser pulse parameters. Several plots for various experimental conditions show that under the conditions normally used for STIRAP experiments the effects are typically a few percent or less, but in the end this effect puts an ultimate limit on total efficiency.
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 stimulated Raman adiabatic passage (STIRAP) through permanent dipole moment transitions are investigated theoretically using a time-dependent quantum wave packet method for the ground electronic state of an HF molecule. The two basic STIRAP processes, $\ensuremath{\Lambda}$ and ladder systems, are simulated. The calculated results show that nearly 100100%100 of the population can be transferred to the target state. Besides the interested transitions, the pulses can induce other transitions which affect the dynamics of STIRAP. The final populations of the initial and target states depend on delay time.