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Physical Review Letters

Measurement of Transition Dipole Moments in Lithium Dimers Using Electromagnetically Induced Transparency

J. Qi, Frank C. Spano, Teodora Kirova, Angelos Lazoudis, Jenny Magnes, L. Li, Lorenzo M. Narducci, Robert W. Field, A. M. Lyyra

Published Apr 15, 2002• 95 citations
Publisher

Abstract

We have observed electromagnetically induced transparency in a Doppler broadened molecular cascade system using fluorescence detection. We demonstrate that the power-dependent splitting of lines in the upper-level fluorescence excitation spectrum can be used as a new spectroscopic tool for the measurement of molecular transition dipole moment functions.

DOI
10.1103/physrevlett.88.173003

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The Journal of Chemical Physics•Jul 16, 2009•17 citations
We have observed electromagnetically induced transparency in a Doppler broadened molecular cascade system using fluorescence detection. We demonstrate that the power-dependent splitting of lines in the upper-level fluorescence excitation spectrum can be used as a new spectroscopic tool for the measurement of molecular transition dipole moment functions.
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.
Following our previous brief report [Phys. Rev. Lett. 88, 173003 (2002)], we report here a detailed study of electromagnetically induced transparency (EIT) and dark fluorescence in a cascade three-level diatomic lithium system using optical-optical double resonance (OODR) spectroscopy for both resonance and off resonance coupling. When a strong coupling laser couples the intermediate state $A\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{u}^{+}(v=13,J=14)$ to the upper state $G\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}_{g}(v=11,J=14)$ of 7Li2^{7}\mathrm{Li}_{2}7Li2​, the fluorescence from both $A\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{u}^{+}$ and $G\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}_{g}$ states was drastically reduced as the weak probe laser was tuned through the resonance transition between the ground state $X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{g}^{+}(v=4,J=15)$ and the excited state $A\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{u}^{+}(v=13,J=14)$. The strong coupling laser makes an optically thick medium transparent for the probe transition. In addition, the fact that fluorescence from the upper state $G\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}_{g}(v=11,J=14)$ was also dark when both lasers were tuned at resonance implies that the molecules were trapped in the ground state. We used density matrix methods to simulate the response of an open molecular three-level system to the action of a strong coupling field and a weak probe field. The analytical solutions were obtained under the steady-state condition. We have incorporated the magnetic sublevel (M)(M)(M) degeneracy of the rotational levels in the line shape analysis and report $\ensuremath{\mid}M\ensuremath{\mid}$ dependent line shape splitting. Our theoretical calculations are in excellent agreement with the observed fluorescence spectra. We show that the coherence is remarkably preserved even when the coupling field was detuned far from the resonance.
Electromagnetically induced transparency (EIT) in a molecular three-level Λ system with permanent dipole moments and undergoing m- and n-photon transitions by pump and probe lasers is investigated. Analytical expressions are derived for probe absorption spectrum and dispersion for a medium of stationary as well as thermal molecules. Contrary to the earlier study by Zhou et al. [J. Chem. Phys. 131, 034105 (2009)], we observe no amplification in 2 + 2 photon process when the sign of the difference of the permanent moments of the excited and the ground levels is reversed. Reasons for these contrasting observations are discussed. Our study shows that the permanent moments essentially damp the laser-molecule Rabi frequency to result in narrower EIT line width and larger group velocity index. These effects are further enhanced when the order of the multi-photon process is increased. The importance of the virtual mechanism is discussed by considering the special case of 2 + 1 photon EIT.
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.
Electromagnetically induced transparency in a three-level Lambda-type molecular system with nonzero permanent dipole moments is investigated. It is shown that in the (2+2)-transition processes, when the sign of d(21), the difference in permanent dipole moments of the probe transition, is positive, perfect electromagnetically induced transparency with steep normal dispersion could be obtained under specific conditions. In contrast, when the sign of d(21) is negative, surprisingly gain without inversion with steep anomalous dispersion could be attained.