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Applied Optics

Doppler-free nonlinear absorption in ethylene by use of continuous-wave cavity ringdown spectroscopy

Christine R. Bucher, Kevin K. Lehmann, David F. Plusquellic, G. T. Fraser

Published Jun 20, 2000• 52 citations
Publisher

Abstract

We report what we believe to be the first systematic study of Doppler-free, nonlinear absorption by use of cavity ringdown spectroscopy. We have developed a variant of cavity ringdown spectroscopy for the mid-infrared region between 9 and 11 microm, exploiting the intracavity power buildup that is possible with continuous-wave lasers. The infrared source consists of a continuous-wave CO2 laser with 1-mW tunable infrared sidebands that couple into a high-finesse stable resonator. We tune the sideband frequencies to observe a saturated, Doppler-free Lamb dip in the nu7, 11(1,10) <-- 11(2,10) rovibrational transition of ethylene (C2H4). Power studies of the Lamb dip are presented to examine the intracavity effects of saturation on the Lamb-dip linewidth, the peak depth, and the broadband absorption.

DOI
10.1364/ao.39.003154

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•Jan 1, 2008•0 citations
We report what we believe to be the first systematic study of Doppler-free, nonlinear absorption by use of cavity ringdown spectroscopy. We have developed a variant of cavity ringdown spectroscopy for the mid-infrared region between 9 and 11 microm, exploiting the intracavity power buildup that is possible with continuous-wave lasers. The infrared source consists of a continuous-wave CO2 laser with 1-mW tunable infrared sidebands that couple into a high-finesse stable resonator. We tune the sideband frequencies to observe a saturated, Doppler-free Lamb dip in the nu7, 11(1,10) <-- 11(2,10) rovibrational transition of ethylene (C2H4). Power studies of the Lamb dip are presented to examine the intracavity effects of saturation on the Lamb-dip linewidth, the peak depth, and the broadband absorption.
We introduce optical feedback frequency stabilized cavity ring-down spectroscopy (OFFS-CRDS), a near-shot-noise-limited technique that combines kilohertz resolution with an absorption detection sensitivity of 5×10(-13) cm(-1) Hz(-1/2). Its distributed feedback laser source is stabilized to a highly stable V-shaped reference cavity by optical feedback and fine-tuned by means of single-sideband modulation. The stability of this narrow laser is transferred to a ring-down (RD) cavity using a new fibered Pound-Drever-Hall (PDH) locking scheme without a dedicated electro-optic phase modulator, yielding several hundred RD events per second. We demonstrate continuous coverage of more than 7 nm with a baseline noise of 5×10(-12) cm(-1) and a dynamic range spanning six decades. With its resonant intracavity light intensity on the order of 1 kW/cm2, the spectrometer was used for observing a Lamb dip in a transition of carbon dioxide involving four vibrational quanta. Saturating such a weak transition at 160 μW input power, OFFS-CRDS paves the way to Doppler-free molecular overtone spectroscopy for precision measurements of hyperfine structures and pressure shifts.
We present an ac heterodyne technique in cavity ringdown spectroscopy that permits $1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}10}$ absorption sensitivity with microwatt-level light power. Two cavity modes, one probing the empty cavity and the other probing intracavity absorption, are excited simultaneously but with their intensities temporally out of phase, with one mode decaying and the other rising. Heterodyne detection between the two modes reveals the dynamic time constants associated with the empty cavity and the additional intracavity gas absorption. The method offers a quick comparison between the on- and off-resonance information, a prerequisite to reaching the fundamental shot-noise limit. This simple and yet important improvement of cavity ringdown spectroscopy should lead to the enhanced performance of a wide range of applications.
An analytical methodology is presented to calculate spectra provided by NICE-OHMS. It is based on the solutions of the equations of motion of an open two-blocked-level system performed in the frequency domain. The polychromaticity of the impinging electromagnetic field, furthermore, trapped inside a high-finesse cavity, is a potential source of induced resonances when this field interacts with a weakly absorbing nonlinear medium. These are optimal conditions to produce the well-established hole burning. However, the radio-frequency sidebands intrinsically associated with the NICE-OHMS technique require a specific treatment for describing both absorption and optical phase shift contributions. To validate the approach, numerical simulations of two transitions of C2H2 in the near-infrared range are discussed. The Doppler broadening-free cross-sideband resonances have been clearly characterized under the regime of moderate electromagnetically induced saturation. Comparison to experimental data available [Opt. Express16, 14689 (2008)OPEXFF1094-408710.1364/OE.16.014689] allowed us to assess the eligibility of the approach.
Optical frequency standards with the reference to a narrow electronic transition of a laser-cooled collection of neutral atomic particles are becoming essential tools of research in modern precision physics experiments. In the core of a building block of an optical frequency standard is the optical continuous wave laser that has a good spectral purity of the emitted light. Such a stable optical oscillator is highly desirable in high resolution spectroscopy, if it emits in a good quality beam at a short visible wavelength. This Master thesis explores efficient techniques for building such an optical frequency source intended for use in the cooling and trapping of Calcium atoms scheme. The strong dipole transition at the blue wavelength in the atomic Calcium is needed to reduce the kinetic energy of atoms by nearly six orders of magnitude. A further reduction in the thermal energy of the laser cooled atoms is required to locate with ultra-high precision the 400 Hz narrow clock transition of the stable 40Ca isotope. The experimental methods that achieve this and approach sub-microkelvin temperature of the laser cooled bosonic isotopes of alkaline earths are inspected. The blue laser with a uniform intensity distribution in the beam is useful to maintain the trapped number of cold atoms during these experiments. The spectroscopic properties of the relative transitions in Calcium atom are also reviewed following relevant publications in the area. The constructed blue laser can be used as a primary wavelength source in the lasers network for cooling and trapping of Calcium atoms. These experiments will constitute part of the project to build an optical atom clock referenced to 40Ca narrow linewidth transition. The blue laser is constructed by generating second harmonic in a Potassium Niobate crystal, which is temperature controlled to use a type-I noncritical phase-matching of the optical nonlinear process. The power of the intracavity-generated second harmonic depends on the resonance properties of the optical resonator where this nonlinear crystal is placed. The study is aimed at characterising the designed optical resonator and the experimental parameters that describe it. The formula is derived that relates the resonance power enhancement coefficient with finesse and the power coupling contrast of a passive optical cavity. The obtained relationship is verfied during the experiments. The produced efficiency of the intracavity second harmonic generation is approx. 0.0023 mWblue/(mWred)2. The research work also examines the noise characteristics of the infrared diode laser that is used as a pump source for the intracavity generated second harmonic and determines the spectroscopic precision of the produced blue light. The frequency locking experiment is analysed using the unbalanced scheme of the polarisation stabilisation technique. The designed optical buildup cavity became a part of the unbalanced frequency discriminator in such a scheme. The results demonstrate high gain of frequency noise suppression of the stabilised laser. The unbalanced arrangement of the H}ansch-Couillaud technique has been possible due to a very low amplitude noise of semiconductor lasers.