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Optics Express

Energy efficient method for two-photon population transfer with near-resonant chirped pulses

Carles Serrat, Jens Biegert

Published Nov 13, 2008• 10 citations
Publisher

Abstract

We investigate a method for complete population inversion in three level systems through pi-pulse bichromatic two-photon coherent excitation and study the dependence on the chirp of the laser pulses. We observe that the population inversion does not monotonously decrease with increasing the time-bandwidth product, and that the excitation depends on the sign of the chirp of the individual pulses. Our results evidence a strategy for coherent population transfer which is energetically superior to adiabatic methods and opens the door for real-world applications, since it alleviates the need for challenging generation of transform-limited pulses at arbitrary wavelengths.

DOI
10.1364/oe.16.019667

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Europhysics Letters (EPL)•Oct 24, 2025•1 citation
We investigate a method for complete population inversion in three level systems through pi-pulse bichromatic two-photon coherent excitation and study the dependence on the chirp of the laser pulses. We observe that the population inversion does not monotonously decrease with increasing the time-bandwidth product, and that the excitation depends on the sign of the chirp of the individual pulses. Our results evidence a strategy for coherent population transfer which is energetically superior to adiabatic methods and opens the door for real-world applications, since it alleviates the need for challenging generation of transform-limited pulses at arbitrary wavelengths.
We investigate a method for creating complete population inversion in a three level system by using bichromatic two‐photon coherent excitations with laser pulses, and study the dependence of the optimal population transfer on the chirp of the pulses. We observe that the population inversion does not monotonously decrease with increasing the time‐bandwidth product, and that the excitation depends on the sign of the chirp of the individual pulses. Our results, which evidence a worthwhile strategy for coherent population transfer in three level systems, are particularized to the level structure of atomic sodium, with regard to applications in bichromatic mesospheric guide stars.
Adiabatic passage induced by chirped laser pulses in three-level $\ensuremath{\Lambda}$ systems is investigated. Two different strategies for efficient population transfer (equal and opposite sign of the chirp) are analyzed. The role of detuning, crucial for the attempt to reduce the population of the intermediate state, is demonstrated. The scheme of adiabatic passage by laser pulses with chirps of different sign is not symmetric with respect to the sign of the one-photon detuning. Blue detuning results in a smaller transient population of the intermediate state than does red detuning. The results are explained on the basis of dressed states. Numerical results for a fully off-resonant adiabatic passage scheme, based on two pulses with the same sign of the chirps, are also considered. The robustness of the schemes in terms of the Rabi frequency, chirp rate, detuning, and time delay of the pulses is explored.
Detailed theoretical analysis and numerical simulation indicate that nearly complete electronic population inversion of molecular systems can be achieved with intense positively chirped broadband laser pulses. To provide a simple physical picture, a two-level model is used to examine the condition for the so-called π pulses and a four-level model is designed to demonstrate for molecular systems the correlation between the sign of the chirp and the excited state population. The proposed molecular π pulse is the combined result of vibrational coherence in the femtosecond regime and adiabatic inversion in the picosecond regime. Numerical results for a displaced oscillator, for LiH and for I2, show that the proposed molecular π pulse scheme is robust with respect to changes in field parameters such as the linear positive chirp rate, field intensity, bandwidth, and carrier frequency, and is stable with respect to thermal and condensed phase conditions including molecular rotation, rovibronic coupling, and electronic dephasing.
We propose a scheme for coherent control of population transfer and arbitrary superpositions of quantum states by a single-chirped laser pulse in a Λ-type excited-doublet four-level system. It is shown that selective, efficient, and robust population transfer from the initial state to the target states (excited or ground) can be achieved via chirped adiabatic passage when the pulse bandwidth is smaller than about 1/10 of the energy separations between the excited-doublet levels and between the ground states. Moreover, arbitrary coherent superpositions between the excited-doublet states, or between the higher ground state and either of the excited-doublet states, can be created by appropriately tuning the chirp rate and detuning the laser field. The proposed flexible method of coherent control of population transfer and arbitrary superpositions between the initially unpopulated states requires only a single pulse, and is robust against variations in the laser parameters, which has potential applications in quantum information processing.
We present a numerical solution for complete population inversion in a four-level ladder system obtained by using a full π-pulse illumination scheme with resonant ultrashort phase-locked Gaussian laser pulses. We find that a set of pulse areas such as √3π , √2π , and √3π completely inverts the four-level system considering identical effective dipole coupling coefficients. The solution is consistent provided the involved electric fields are not too strong and it is amply accurate also in the case of diverse transition dipole moments. We study the effect of detuning and chirp of the laser pulses on the complete population inversion using the level structure of atomic sodium interacting with ps and fs pulses as an example. Our result opens the door for multiple applications such as efficient ultrashort pulse lasing in the UV or the engineering of quantum states for quantum computing.
Abstract This study demonstrates complete adiabatic population transfer in a closed three-level atomic system using chirped laser pulses. By satisfying the three-photon resonance condition, we effectively mitigate the first-order Doppler effect. Under the assumption of weak coupling between the stable levels, we show that relative phase fluctuations of the lasers exert a negligible influence on the population dynamics during the transfer process. A comprehensive analysis of the system parameters is conducted to determine the optimal conditions for achieving 100% population transfer while minimizing the excited state population