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Optics Letters

Sub-Doppler double-resonance spectroscopy of NH_3 using a tunable-diode laser and a CO laser

W. Weber, R. W. Terhune

Published Oct 1, 1981• 15 citations
Publisher

Abstract

Results are given for a Stark-tuned double-resonance experiment, using a CO-laser pump and a diode-laser probe. The CO laser, operating on the 13-12 P(15) line at 1775.2588 cm(-1), is locked by Lamb-dip stabilization to one of the Stark components of the a(R)R(9, 9) nu(4) line of NH(3). The diode laser probes the aQ(9, 9) nu(2) line at 921.255 cm(-1), revealing a complex spectrum of sub-Doppler features, the narrowest of which are 5.3 +/- 0.3 MHz wide. As well as the resonances associated with population depletion of the common lower levels, we see line-narrowing effects that are due to two-quantum Raman-type processes and collision-induced resonances arising from state-changing collisions that preserve the molecular velocities. The zero-field a(R)R(9, 9) nu(4) line is established to be 264.1 +/- 5.0 MHz above the CO-laser line.

DOI
10.1364/ol.6.000455

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Bulletin of the American Physical Society•Jun 11, 2015•0 citations
Results are given for a Stark-tuned double-resonance experiment, using a CO-laser pump and a diode-laser probe. The CO laser, operating on the 13-12 P(15) line at 1775.2588 cm(-1), is locked by Lamb-dip stabilization to one of the Stark components of the a(R)R(9, 9) nu(4) line of NH(3). The diode laser probes the aQ(9, 9) nu(2) line at 921.255 cm(-1), revealing a complex spectrum of sub-Doppler features, the narrowest of which are 5.3 +/- 0.3 MHz wide. As well as the resonances associated with population depletion of the common lower levels, we see line-narrowing effects that are due to two-quantum Raman-type processes and collision-induced resonances arising from state-changing collisions that preserve the molecular velocities. The zero-field a(R)R(9, 9) nu(4) line is established to be 264.1 +/- 5.0 MHz above the CO-laser line.
Laser spectroscopy experiments are reported on rubidium atoms by using two or three external cavity diode lasers to study multiple resonance transitions in Λ- and V-type systems as well as on (Λ+V)-type system. Electromagnetically induced transparency (EIT) peaks having sub-natural line-widths are found on the Doppler broadened transmission backgrounds with velocity selective enhanced absorption dips. In the presence of a pump laser, probe spectrum shows enhancement of EIT signal by tuning the control laser frequency when the Λ- and V-type EIT signals are made to overlap. Theoretical analysis is carried out by solving the optical Bloch equations for five-level atomic model under Λ configuration. With the numerically simulated spectra, variation of EIT transmission peak with ground state decay rate and excited state spontaneous decay rate are investigated. Effect of pump Rabi frequency on the transmission peak is also shown.
A scheme of Doppler-free spectroscopy is experimentally demonstrated with a co-propagating control laser locking to an atomic hyperfine transition, and the differential transmission of the probe and the reference laser is detected. Crossover resonances are eliminated by selecting the class of atoms with zero velocity in the direction of beam propagation. In addition, the sub-Doppler spectrum experiences optical gain compared to the conventional saturated-absorption spectrum as a result of optical pumping.
We investigate the coherent pump?probe spectroscopy of a three-level ? system, , in the hyperfine manifold of D2 transition (852?nm) of cesium with particular reference to the sub-Doppler linewidth resonance arising from Aulter?Townes (AT) splitting and the possibility of using it for realizing a scheme for tunable atomic frequency offset locking (AFOL). We discuss here the theoretical framework for a ? system interacting with a coherent pump and probe and use it to describe the process of modulation transfer in the AT and electromagnetically induced transparency regimes. We further employ an experimental scheme consisting of a strong pump and a pair of weak probes to resolve the sub-Doppler linewidth (~8?MHz) AT resonance and study its dependence on pump intensity and detuning. In order to explore the possibility of using such a sub-Doppler linewidth resonance for AFOL, we use its first derivative signal as a frequency discriminator to stabilize the probe laser. The frequency stability of the probe is characterized by means of error signal analysis. This study reveals that while the frequency stability of the AT locked laser is limited by the pump laser, the tuning range of the offset frequency lock can cover the entire Doppler profile and its immediate neighbourhood, thereby providing a simple and cost effective alternative to the external modulator. The study described in this paper contributes to the discussion on the subtle link between dressed state spectroscopy and AFOL, which is relevant for developing a master?slave-type laser system in the domain of coherent photon?atom interaction.
An ongoing spectroscopic investigation of atomic rubidium utilizes a two-photon, single-laser excitation process. Transitions accessible with our tunable laser include 5P1/2 (F ′ ) ← 5S1/2 (F) and 5P3/2 (F ′ ) ← 5S1/2 (F). The laser is split into a pump and probe beam to allow for Doppler-free measurements of transitions between hyperfine levels. The pump and probe beams are overlapped in a counter-propagating geometry and the laser frequency scans over a transition. Absorption, fluorescence and polarization spectroscopy techniques are applied to this basic experimental setup. The temperature of the vapor cell and the power of the pump and probe beams have been varied to explore line broadening effects and signal-to-noise of each technique. This humble setup will hopefully grow into a more robust experimental arrangement in which double resonance, two-laser excitations are used to explore hyperfine state changing collisions between rubidium atoms and noble gas atoms. Rb-noble gas collisions can transfer population between hyperfine levels, such as 5P3/2 (F ′ = 3) Collision ←− 5P3/2 (F ′ = 2), and the probe beam couples 7S1/2 (F ′′ = 2) ← 5P3/2 (F ′ = 3). Polarization spectroscopy signal depends on the rate of population transfer due to the collision as well as maintaining the orientation created by the pump laser. Fluorescence spectroscopy relies only on transfer of population due to the collision. Comparison of these techniques yields information regarding the change of the magnetic sublevels, mF , during hyperfine state changing collisions.