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Journal of Physics B Atomic Molecular and Optical Physics

The Autler-Townes splitting in uranium observed with pulsed lasers

P. Thornton Greenland, D. N. Travis, D J H Wort

Published Mar 28, 1991• 14 citations
Publisher

Abstract

The authors describe measurements of the Autler-Townes splitting in optical transitions in uranium using pulsed lasers in a double optical resonance experiment. These measurements give absolute values for transition strengths. Although the resolution of the experiments is insufficient to show explicitly either the magnetic degeneracy of the levels, or the quantum mechanical oscillations which arise from the pulse shape, theoretical analysis shows that both these effects contribute significantly to the observed lineshapes. Separate experiments in which a third laser was used to ionize the uranium through an autoionizing level were also performed and a fit to the ion yield as a function of laser intensities provides confirmation of the coupling strengths derived from the double optical resonance experiments.

DOI
10.1088/0953-4075/24/6/017

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Journal of Physics B Atomic and Molecular Physics•May 14, 1987•1 citation
The authors describe measurements of the Autler-Townes splitting in optical transitions in uranium using pulsed lasers in a double optical resonance experiment. These measurements give absolute values for transition strengths. Although the resolution of the experiments is insufficient to show explicitly either the magnetic degeneracy of the levels, or the quantum mechanical oscillations which arise from the pulse shape, theoretical analysis shows that both these effects contribute significantly to the observed lineshapes. Separate experiments in which a third laser was used to ionize the uranium through an autoionizing level were also performed and a fit to the ion yield as a function of laser intensities provides confirmation of the coupling strengths derived from the double optical resonance experiments.
Autler–Townes (AT) splitting has been experimentally observed in the optical transition between the zero-point levels of S 1 and S 0 for supersonically cooled 2-methoxythiophenol, 2-fluorothiophenol, and 2-chlorothiophenol. This is the first experimental observation of the light-dressed quantum states of polyatomic molecules ( N > 3) in the electronic transition. In the resonance-enhanced ionization process involving the optically coupled states, if Rabi cycling is ensured within the nanosecond laser pulse, AT splitting is clearly observed for the open system for which the excited-state lifetime is shorter than hundreds of picoseconds. Semiclassical optical Bloch equations and a dressed-atom approach based on the three-level atomic model describe the experiment quite well, giving deep insights into the light–matter interaction in polyatomic molecular systems.
In recent years, coherent effects in atomic and molecular systems have been studied extensively, especially in several new classes of effects, such as lasing without inversion (LWI), electromagnetically induced transparency (EIT), coherent population trapping (CPT), AC Stark effect and Autler-Townes (AT) splitting in multilevel systems. The AC stark effect and Autler-Townes splitting in molecules have only been investigated recently. We demonstrate AC stark effect and Autler-Townes (AT) splitting in a lithium molecule using cw multi-photon spectroscopy. The excited upper level of the G1PigG^{1}\\Pi_{g}G1Pig​ is prepared by the optical-optical double resonance (OODR) excitation. The OODR line is split in the presence of a third coupling laser, which couples the upper level to an another intermediate level when the coupling laser is on or near resonance transition. The AT line shape consists of the superposition of ∣MJ∣|M_{J}|∣MJ​∣ components which have been resolved for G1Pig(v=12,J=3,f)G^{1}\\Pi_{g}(v=12, J=3,f)G1Pig​(v=12,J=3,f). We find that the AT splittingis linearly proportional to ∣MJ∣|M_{J}|∣MJ​∣, which allows the excitation of molecules with a selected ∣MJ∣|M_{J}|∣MJ​∣ level. The AC Stark shift of the OODR line is observed when the coupling laser is detuned from the resonance transition.
The dependence of the optical Autler-Townes effect on laser field phase fluctuations describable by a two-dimensional Markovian process (phase-diffusion model with a non-Lorentzian line shape) is investigated experimentally in atomic sodium. An intense cw laser tuned to near resonance with the 3S1/2{3\mathrm{S}}_{1/2}3S1/2​(F=2,MF{\mathrm{M}}_{\mathrm{F}}MF​=2)\ensuremath{\rightarrow}3P3/2{3\mathrm{P}}_{3/2}3P3/2​(F=3,MF{\mathrm{M}}_{\mathrm{F}}MF​=3) transition was frequency modulated to generate phase fluctuations with the desired characteristics. A weak probe laser coupling to the 4D5/2{D}_{5/2}D5/2​(F=4, MF{M}_{F}MF​=4) state was used to obtain the double-peaked optical Autler-Townes absorption profiles in order to investigate their dependencies on band shape, bandwidth, intensity, and detuning of the intense fluctuating laser field. Reversals of the peak-height asymmetry and reversion to normal asymmetry with increased detuning were observed and measured. Quantitative studies of the spectral widths and splittings of the peaks are also reported. Measured absorption profiles are in excellent agreement with calculations based on previous theoretical work.
Some features of the optical Autler-Townes effect as observed in Doppler-broadened three-level systems, including the physical significance of the observed line splitting, the conditions for the observation of the doublet, the doublet separation and the detuning effects, are discussed in this paper. A graphical illustration of the phenomenon, based on a search for on-resonance velocity groups, is proposed which allows a complete qualitative discussion of the effect and shows that the observed doublet is not really a splitting of the resonance as for the atom at rest but rather corresponds to a frequency hole where the laser probe does not see any resonant velocity group. The method is applied to real three-level systems of neon as typical cases. A semi-classical density-matrix calculation is performed numerically and definitely confirms the results of the qualitative graphical discussion ; furthermore it shows that, for many experimental situations, the first order approximation is inadequate. The observation of the Autler-Townes doublet in a new experiment using two dye lasers is reported. The experimental results and that of one of our previous experiments are compared with the theoretical predictions ; the agreement is quite satisfactory.