A system is described in which a real molecular state is tuned into and out of resonance with the intermediate level of a two-photon transition, by the laser-induced ac-Stark effect. Two narrow-band CO2 wave-guide lasers are utilized to induce rovibrational transitions in the ν3 ladder of SF6. A weak probe laser monitors the absorption for the [Formula: see text] two-photon transition. Simultaneously, a strong pump laser is in resonance with the [Formula: see text] one-photon transition. The ac-Stark splitting is observed and quantum interferences between two-photon amplitudes involving different intermediate states occur. It is demonstrated that destructive interference allows suppression of the two-photon excitation for an appropriate pump laser power. Simulations based on the Dressed State Picture and the optical Bloch equations show a satisfactory agreement with the experiment.
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
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∣ components which have been resolved for
G1Pig(v=12,J=3,f). We find that the AT splittingis linearly proportional to
∣MJ∣, which allows the excitation of molecules with a selected
∣MJ∣ level. The AC Stark shift of the OODR line is observed when the coupling laser is detuned from the resonance transition.
A semiclassical treatment is given for the serial, near-resonant interaction of three waves in seven equivalent four-level atomic or molecular systems. Explicit equations are presented for the complex susceptibilties for the three waves, valid for $t\ensuremath{\gg}{T}_{2}$, which contain implicit ac Stark-shift and -splitting information, and can be separated into one-, two-, and three-photon contributions. For the case of a weak third or terminal wave, equations for the degree of ac Stark shifting and splitting are found and indicate that the three-photon or triple-resonance contribution is immune to the optical Stark effect if the remaining two waves are tuned to at least two-photon resonance conditions. The conditions for Doppler-free triple resonance are outlined, and it is shown that an equivalent ac Stark broadening may exist but may also be minimized by an appropriate choice of field intensities.