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arXiv:2607.00583 · The Journal of Physical Chemistry Letters

Open Quantum Systems Driven by Chirped Pulses: Quantized versus Semiclassical Fields and the Validity of the Rotating-Wave Approximation

Justin Zhengjie Tan, Frank Großmann, Yiying Yan, Maxim Gelin, Yang Zhao

quant-phSubmitted Jul 1, 2026• Announced Jul 2, 2026• 1 citation
arXivHTMLPDF

Abstract

Population transfer via chirped rapid adiabatic passage is studied using open quantum and semiclassical models, with and without the rotating-wave approximation. A time-dependent variational approach based on the multiple-Davydov D$_2$ trial state is employed to simulate the quantum models with an arbitrary finite mean photon number. We examine the accuracy of both the semiclassical field description and the rotating-wave approximation. Robust population transfer is identified over a wide parameter regime controlled by the laser spectral chirp and is found to be insensitive to the spin--phonon coupling strength, Gaussian pulse area, and energy gap of the two-level system.

DOI
10.1021/acs.jpclett.6c01634

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Population transfer via chirped rapid adiabatic passage is studied using open quantum and semiclassical models, with and without the rotating-wave approximation. A time-dependent variational approach based on the multiple-Davydov D2_22​ trial state is employed to simulate the quantum models with an arbitrary finite mean photon number. We examine the accuracy of both the semiclassical field description and the rotating-wave approximation. Robust population transfer is identified over a wide parameter regime controlled by the laser spectral chirp and is found to be insensitive to the spin--phonon coupling strength, Gaussian pulse area, and energy gap of the two-level system.
We investigate the problem of population transfer in a two-states system driven by an external electromagnetic field featuring a few cycles, until the extreme limit of two or one cycle. Taking the physical constraint of zero-area total field into account, we determine strategies leading to ultrahigh-fidelity population transfer despite the failure of the rotating wave approximation. We specifically implement adiabatic passage based on adiabatic Floquet theory for a number of cycles as low as 2.5 cycles, finding and making the dynamics follow an adiabatic trajectory connecting the initial and targeted states. Nonadiabatic strategies with shaped or chirped pulses, extending the π-pulse regime to two- or single-cycle pulses, are also derived.
The ultrafast particle population transfer in a ■-type three-level atomic system driven by linearly polarized chirped Gauss femtosecond laser pulse is investigated by using numerical solution of the Schrdinger equation without the rotating wave approximation(RWA).It is shown that the population transfer is mainly determined by the Rabi frequency(intensity) of the driving laser field and chirp rate,and the ratio of two dipole moments and the pulse width also have obvious effect on the population transfer.By choosing suitable values of the above parameters,nearly complete population transfer(99.6%) can be realized.
Abstract We have proposed and demonstrated a fast and robust method of population transfer between two quantum states using a quadratically chirped laser source. Numerically solving the time-dependent Schrödinger equation, transition probabilities have been obtained and the condition of the adiabatic passage is investigated. In this scheme, the wavelength of a laser source is quadratically swept in time to arbitrarily engineer the transition probabilities. The results show that complete and robust population transfer could be achieved by appropriate adjusting of the system parameters including the laser chirping parameter, the center frequency, and the coupling strength. Using this method, the time of the complete transition could be drastically decreased compared to the incorporation of the traditional linearly chirped laser.
In the physics literature it is common to see the rotating wave approximation and the adiabatic approximation used to justify the use of chirped pulses for two-level quantum systems driven by one external field, in particular when the resonance frequency of the system is not known precisely. Both approximations need relatively long time and are essentially based on averaging theory of dynamical systems. Unfortunately, the two approximations cannot be done independently since, in a sense, the two time scales interact. The purpose of this paper is to study how the cascade of the two approximations can be justified and how large becomes the final time as the fidelity goes to one, while preserving the robustness of the adiabatic strategy. Our main result gives a precise quantification of the uncertainty interval of the resonance frequency for which the strategy works. We believe that this result, beside its mathematical interest, could be useful in experimental situations.
This paper considers population transfer between eigenstates of a finite quantum ladder controlled by a classical electric field. Using an appropriate change of variables, we show that this setting can be set in the framework of adiabatic passage, which is known to facilitate ensemble control of quantum systems. Building on this insight, we present a mathematical proof of robustness for a control protocol—chirped pulse—practised by experimentalists to drive an ensemble of quantum systems from the ground state to the most excited state. We then propose new adiabatic control protocols using a single chirped and amplitude-shaped pulse, to robustly perform any permutation of eigenstate populations, on an ensemble of systems with unknown coupling strengths. These adiabatic control protocols are illustrated by simulations on a four-level ladder.