The phenomenon of electronic orbital angular momentum L uncoupled from its internuclear axis has been observed in the sodium dimer using high-resolution cw optical-optical double-resonance spectroscopy. When L uncoupling occurs, the degeneracy of Lambda doubling is removed. In our experiment, the intermediate B (1)Pi(u) state of Na(2) is excited from the thermally populated ground X (1)Sigma(g) (+) state by a single-line Ar(+) laser. Then, a single-mode dye laser is used to probe the Rydberg states from the intermediate state. The signals are detected by monitoring the UV fluorescence from the triplet gerade states back to the a (3)Sigma(u) (+) state via collision energy transfer. Under our experimental resolution, the splitting of Lambda doubling in the 5 (1)Delta(g) state of Na(2) can be measured. A total of 136 rovibronic levels with ef parities have been assigned to the 5 (1)Delta(g) state. The Lambda-splitting constants deduced from these data are q(0)=0.376(90)x10(-4) cm(-1), q(v)=0.114(6)x10(-4) cm(-1), and mu=0.76(33)x10(-8) cm(-1). In general, the Lambda splitting of the Delta states is considerably smaller than that of the Pi states. However, the first-order splitting constants q(0) and q(v) reported here are larger than those in the B (1)Pi(u) state. This is due to the L uncoupling of the Rydberg states.
Doubly dressed states in a ladder-type two-photon, three-level coupling system are observed. The electromagnetically induced transparency ͑EIT͒ doublet signal is interpreted as arising from the absorption and gain components of the Mollow spectrum. The separation of the EIT doublet matches the theoretical prediction. A numerical simulation demonstrates that the Doppler velocity group may perturb the light shift from the symmetric center of the EIT doublet. The quantum nature of the EIT system significantly suppresses Doppler broadening.
The doubly excited valence (3p+3p) 2 (1)Delta(g) state of Na(2) is experimentally observed by using optical-optical double resonance spectroscopy. A single line Ar(+) laser (a total of nine lines) was used to pump the sodium dimers from thermally populated ground state X (1)Sigma(g) (+) to the intermediate B (1)Pi(u) state. Then, a single mode Ti:sapphire laser was used to probe the doubly excited 2 (1)Delta(g) state. Violet fluorescence emitted from the highly excited states (mainly 2 (3)Pi(g) or 3 (3)Pi(g) states which are transferred from 2 (1)Delta(g) state via collision) to the a (3)Sigma(u) (+) state was monitored by a filtered photomultiplier tube (PMT). A total of 582 rovibrational levels of 2 (1)Delta(g) state were observed, identified, and assigned to the vibrational and rotational quantum numbers in the range of 0< or =v< or =28 and 11< or =J< or =99, respectively. The absolute vibrational quantum number assignment was verified by comparing the totally resolved fluorescence with the calculated Franck-Condon factors between 2 (1)Delta(g) state and B (1)Pi(u) state. Dunham coefficients and Rydberg-Klein-Rees potential curve were derived from these observed quantum levels. The primary molecular constants of Na(2) 2 (1)Delta(g) state are T(e)=32 416.759(15) cm(-1), omega(e)=124.8484(36) cm(-1), B(e)=0.119 158(3) cm(-1), and R(e)=3.508 20(5) A.
This investigation clarifies the transition phenomenon between the electromagnetically induced transparency (EIT) and Raman absorption in a ladder-type system of Doppler-broadened cesium vapor. A competition window of this transition was found to be as narrow as 2 MHz defined by the probe Rabi frequency. For a weak probe, the spectrum of EIT associated with quantum interference suggests that the effect of the Doppler velocity on the spectrum is negligible. When the Rabi frequency of the probe becomes comparable with the effective decay rate, an electromagnetically induced absorption (EIA) dip emerges at the center of the power broadened EIT peak. While the Rabi frequency of the probe exceeds the effective decay rate, decoherence that is generated by the intensified probe field occurs and Raman absorption dominates the interaction process, yielding a pure absorption spectrum; the Doppler velocity plays an important role in the interaction. A theory that is based on density matrix simulation, with or without the Doppler effect, can qualitatively fit the experimental data. In this work, the coherence of atom-photon interactions is created or destroyed using the probe Rabi frequency as a decoherence source.
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