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arXiv:quant-ph/0508110

The Role of Doppler Broadening in Electromagnetically Induced Transparency and Autler-Townes Splitting in Open Molecular Systems

Angelos Lazoudis, Ergin H. Ahmed, L. Li, Teodora Kirova, Peng Qi, Annie Hansson, Jenny Magnes, Frank C. Spano, A. M. Lyyra

Published Aug 15, 2005• 0 citations
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Abstract

We describe in this Letter how inhomogeneous line broadening affects the Autler-Townes (AT) splitting in a three level open molecular cascade system. For moderate Rabi frequencies in the range of 300 to 500 MHz the fluorescence line shape from the uppermost level |3> in this system depends strongly on the frequency ratio of the two laser fields. However, the fluorescence spectrum of the intermediate level |2> appears as expected. We provide a description of the conditions for optimally resolved AT splitting in terms of the probe laser/coupling field frequency ratio and laser propagation geometry based on our theoretical analysis of the Doppler integral. This is important for applications such as molecular angular momentum alignment as well as for the measurement of the transition dipole moment matrix element.

DOI
10.48550/arxiv.quant-ph/0508110

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Wavelength dependence of coherently induced transparency in a Doppler-broadened cascade medium

Sara Shepherd, David J. Fulton, Malcolm H. Dunn

The effect of changing the coupling laser transition, and hence the wavelength, on the coherently induced transparency seen by a probe beam in a Doppler-broadened cascade electromagnetically induced transparency (EIT) configuration is studied experimentally and theoretically. The transparency of the vapor is shown to be an effect not just of EIT, but of the varying Autler-Townes splitting for each velocity group within the vapor. Consequently, the best overall transparency for Rabi splittings less than the Doppler width is not at the position of matched coupling and probe wavelengths, but for coupling wavelengths less than that of the probe. \textcopyright{} 1996 The American Physical Society.

Physical Review A•Dec 1, 1996•81 citations
We describe in this Letter how inhomogeneous line broadening affects the Autler-Townes (AT) splitting in a three level open molecular cascade system. For moderate Rabi frequencies in the range of 300 to 500 MHz the fluorescence line shape from the uppermost level |3> in this system depends strongly on the frequency ratio of the two laser fields. However, the fluorescence spectrum of the intermediate level |2> appears as expected. We provide a description of the conditions for optimally resolved AT splitting in terms of the probe laser/coupling field frequency ratio and laser propagation geometry based on our theoretical analysis of the Doppler integral. This is important for applications such as molecular angular momentum alignment as well as for the measurement of the transition dipole moment matrix element.
We have investigated the effects of inhomogeneous Doppler line broadening on the Autler-Townes (AT) splitting in a three-level open molecular cascade system. For moderate Rabi frequencies in the range of 300−−600MHz300--600\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}300−−600MHz, the fluorescence line shape from the uppermost level \ensuremath{\mid}3⟩ in this system depends strongly on the wave-number ratio of the two laser fields. However, the fluorescence spectrum of the intermediate level \ensuremath{\mid}2⟩ appears as expected. We provide a description of the conditions for optimally resolved AT splitting in terms of the ratio of the probe and coupling laser wave numbers, and the laser propagation geometry based on our theoretical analysis of the Doppler integral. The low threshold Rabi frequency region for Autler-Townes splitting is important for high-resolution Autler-Townes spectroscopy since the laser E-field amplitudes are modest in continuous-wave laser experiments.
Theoretical analysis of the Autler-Townes splitting pattern in a three-level cascade excitation of a Doppler-broadened sample reveals that the observed Autler-Townes splitting is not only a function of the coupling-laser Rabi frequency, as in the homogeneously broadened case, but can also strongly depend on the wavenumber ratio of the coupling and probe lasers. Utilizing a steady-state density matrix formalism, we derive exact expressions for the populations of the intermediate and upper levels for a homogeneously broadened system. In the limit of a weak probe field, analytical expressions for Doppler-broadened excitation spectra from the intermediate and upper levels are derived. Using these expressions, we investigate the critical role of Doppler broadening on the observation of Autler-Townes splitting and its asymptotic behavior as a function of the coupling Rabi frequency for counterpropagating and copropagating configurations for different wavenumber ratios of the lasers.
We study the relationship between electromagnetically-induced transparency(EIT) and Autler–Townes(AT) splitting in a cascade three-level Doppler-broadened system. By comparing the absorption spectrum with the fluorescence excitation spectrum, it is found that for a Doppler-broadened system, EIT resonance cannot be explained as the result of quantum interference, unlike the case of a homogeneously broadened system. Instead, the macroscopic polarization interference plays an important role in determining the spectra of EIT and AT splitting, which can be explained within the same framework when being detected by the absorption spectra.
Abstract We utilize an electromagnetically induced transparency (EIT) of a three-level cascade system involving Rydberg state in a room-temperature cell, formed with a cesium 6S1/2–6P3/2–66S1/2 scheme, to investigate the Autler–Townes (AT) splitting resulting from a 15.21-GHz radio-frequency (RF) field that couples the | 66 S 1 / 2 〉 → | 65 P 1 / 2 〉 Rydberg transition. The radio-frequency electric field induced AT splitting, γ AT, is defined as the peak-to-peak distance of an EIT-AT spectrum. The dependence of AT splitting γ AT on the probe and coupling Rabi frequency, Ωp and Ωc, is investigated. It is found that the EIT-AT splitting strongly depends on the EIT linewidth that is related to the probe and coupling Rabi frequency in a weak RF-field regime. Using a narrow linewidth EIT spectrum would decrease the uncertainty of the RF field measurements. This work provides new experimental evidence for the theoretical framework in [J. Appl. Phys. 121, 233106 (2017)].
We propose a general theoretical scheme to investigate the crossover from electromagnetically induced transparency (EIT) to Autler–Townes splitting (ATS) in open ladder-type atomic and molecular systems with Doppler broadening. We show that when the wavenumber ratio kc/kp≈−1, EIT, ATS, and EIT-ATS crossover exist for both ladder-I and ladder-II systems, where kc (kp) is the wavenumber of control (probe) field. Furthermore, when kc/kp is far from −1, EIT can occur, but ATS is destroyed if the upper state of the ladder-I system is a Rydberg state. In addition, ATS exists but EIT is not possible if the control field used to couple the two lower states of the ladder-II system is a microwave field. The theoretical scheme developed here can be applied to atoms, molecules, and other systems (including Na2 molecules, and Rydberg atoms), and the results obtained may have practical applications in optical information processing and transformation.
The effect of changing the coupling laser transition, and hence the wavelength, on the coherently induced transparency seen by a probe beam in a Doppler-broadened cascade electromagnetically induced transparency (EIT) configuration is studied experimentally and theoretically. The transparency of the vapor is shown to be an effect not just of EIT, but of the varying Autler-Townes splitting for each velocity group within the vapor. Consequently, the best overall transparency for Rabi splittings less than the Doppler width is not at the position of matched coupling and probe wavelengths, but for coupling wavelengths less than that of the probe. \textcopyright{} 1996 The American Physical Society.