The superposition principle and cavity ring-down spectroscopy

Lehmann, Kevin K.; Romanini, Daniele
December 1996
Journal of Chemical Physics;12/15/1996, Vol. 105 Issue 23, p10263
Academic Journal
Cavity ring-down is becoming a widely used technique in gas phase spectroscopy. It holds promise for further important extensions, which will lead to even more frequent use. However, we have found widespread confusion in the literature about the nature of coherence effects, especially when the optical cavity constituting the ring-down cell is excited with a short coherence length laser source. In this paper we use the superposition principle of optics to present a general and natural framework for describing the excitation of a ring-down cavity regardless of the relative values of the cavity ring-down time, the input pulse coherence time, or the dephasing time of absorption species inside the cavity. This analysis demonstrates that even in the impulsive limit the radiation inside a high finesse cavity can have frequency components only at the natural resonance frequencies of the cavity modes. As an immediate consequence, a sample absorption line can be detected only if it overlaps at least one of the cavity resonances. Since this point is of particular importance for high resolution applications of the technique, we have derived the same conclusion also in the time domain representation. Finally, we have predicted that it is possible to use this effect to do spectroscopy with a resolution much higher than that of the bandwidth of the excitation laser. In order to aid in the design of such experiments, expressions are derived for the temporal and spatial overlap of a Fourier transform limited input Gaussian beam with the TEMmn modes of the cavity. The expressions we derive for the spatial mode overlap coefficients are of general interest in applications where accurate mode matching to an optical cavity is required. © 1996 American Institute of Physics.


Related Articles

  • Cavity ring down spectroscopy measurements of absolute CN concentrations during flame deposition of diamond. Stolk, R. L.; ter Meulen, J. J. // Journal of Chemical Physics;11/8/2002, Vol. 117 Issue 18, p8281 

    Cavity ring down spectroscopy (CRDS) was used for measuring absolute concentration profiles of the CN (cyano) radical during oxyacetylene flame deposition of diamond. Profiles were measured for three different nitrogen additions to the flame. Novel ways for the determination of the lateral...

  • 5-ps, 10-GHz pulse generation from an all-optical semiconductor switch embedded in a ring cavity. Ueno, Yoshiyasu; Nakamura, Shigeru; Tajima, Kazuhito // Applied Physics Letters;10/15/2001, Vol. 79 Issue 16, p2520 

    We observed spontaneous generation of nearly transform-limited pulses (5 ps, 10 GHz, 1558 nm) from a semiconductor ring oscillator. This oscillator is completely different from conventional mode-locked lasers in that the pulse width is passively determined by a split delay time inside its ring...

  • Cavity ring down spectroscopy on solid C[sub 60]. Engeln, Richard; von Helden, Gert; van Roij, AndreJ.A.; Meijer, Gerard // Journal of Chemical Physics;2/1/1999, Vol. 110 Issue 5, p2732 

    Studies the cavity ring down spectroscopy on solid carbon. Measurement of the polarization rotation at a fixed wavelength; Absorption spectrum of the solid; Use of the tunable pulsed radiation from the free-electron laser for infrared experiments in Nieuwegein.

  • Infrared cavity ringdown laser absorption spectroscopy (IR-CRLAS) in low pressure flames. Scherer, J.J.; Voelkel, D.; Rakestraw, D.J. // Applied Physics B: Lasers & Optics;1997, Vol. 64 Issue 6, p699 

    We report the first application of Infrared Cavity Ringdown Laser Absorption Spectroscopy (IR-CRLAS) as a diagnostic tool for combustion chemistry studies. The high sensitivity (10[sup -5] fractional absorption) and generality of IR-CRLAS for combustion studies is demonstrated for low pressure...

  • Cavity ring-down measurements in flames using a single-mode tunable laser system. Schocker, A.; Brockhinke, A.; Bultitude, K.; Ewart, P. // Applied Physics B: Lasers & Optics;Aug2003, Vol. 77 Issue 1, p101 

    Demonstrates high-resolution pulsed cavity ring-down spectroscopy of hydroxide. Use of single-mode tunable laser; Pulse amplification of the output of a single-mode diode laser; Ring-down curves; Lineshape analysis.

  • The cavity ringdown spectrum of the visible electronic system of thiophosgene: An estimation of... Moule, D.C.; Burling, I.R.; Liu, H.; Lim, E.C. // Journal of Chemical Physics;9/15/1999, Vol. 111 Issue 11, p5027 

    Reports on the recording of the cavity ringdown (CRD) spectrum of the thiophosgene absorption system under supersonic jet conditions to obtain insights into the photophysical properties of collision-free thiophosgene. Decay of thiophosgene by the nonradiative intersystem crossing; Estimated...

  • Spontaneous emission spectra from microdroplets. Holler, Stephen; Goddard, Noel L. // Journal of Chemical Physics;4/22/1998, Vol. 108 Issue 16, p6545 

    Compares a theory interaction of excited molecules with the emission spectrum from a fluorescent microdroplet. Critical test of theory using surfactant flours on levitated microdoplets; Results in placing an excited atom/molecule near the surface of a spherical dielectric; Description of the...

  • Vibronic spectroscopy and lifetime of S[sub 1] acrolein. Paulisse, Kevin W.; Friday, Tyson O.; Graske, Margaret L.; Polik, William F. // Journal of Chemical Physics;7/1/2000, Vol. 113 Issue 1, p184 

    The S[sub 1] vibronic spectrum of acrolein (CH[sub 2]CHCHO) was obtained in a supersonic free-jet expansion using cavity ringdown spectroscopy. Comparison of room temperature and free-jet spectra was used to assign vibronic transitions. Computations using the configuration interaction-singles...

  • Pulsed cavity ring-down spectroscopy of NO and NO[sub 2] in the exhaust of a diesel engine. Evertsen, R.; Staicu, A.; Dam, N.; van Vliet, A.; ter Meulen, J.J. // Applied Physics B: Lasers & Optics;2002, Vol. 74 Issue 4/5, p465 

    The application of pulsed cavity ring-down spectroscopy has been demonstrated for the in situ quantitative determination of NO and NO[sub 2] in the exhaust of a diesel engine. NO absorption has been monitored at the transition from the Χ[sup 2] Π ground state to the A[sup 2] Σ[sup +]...


Read the Article


Sorry, but this item is not currently available from your library.

Try another library?
Sign out of this library

Other Topics