In this work, we analyze the possibility of exploiting the recently demonstrated super-resonant intracavity coherent absorption effect for quantitative sensing applications. The method relies on a system of two nested resonators (ring and Fabry-Perot) which allows to increase the radiation-matter interaction pathlength by a factor proportional to the product of the two resonator’s individual finesse coefficients. In this way, it is possible to dramatically increase the interaction of intracavity radiation with a weakly absorbing sample without need of an ultra-high finesse optical cavity. Here, we propose a measurement strategy that allows to exploit the super-resonant enhancement provided by the nested-resonators system and cancel out the noise connected with the radiation source at the same time, and compare it to a conventional cavity-enhanced absorption measurement.
In this work, we analyze the possibility of exploiting the recently demonstrated super-resonant intracavity coherent absorption effect for quantitative sensing applications. The method relies on a system of two nested resonators (ring and Fabry-Perot) which allows to increase the radiation-matter interaction pathlength by a factor proportional to the product of the two resonator’s individual finesse coefficients. In this way, it is possible to dramatically increase the interaction of intracavity radiation with a weakly absorbing sample without need of an ultra-high finesse optical cavity. Here, we propose a measurement strategy that allows to exploit the super-resonant enhancement provided by the nested-resonators system and cancel out the noise connected with the radiation source at the same time, and compare it to a conventional cavity-enhanced absorption measurement.
The capability of optical resonators to extend the effective radiation-matter interaction length originates from a multipass effect, hence is intrinsically limited by the resonator's quality factor. Here, we show that this constraint can be overcome by combining the concepts of resonant interaction and coherent perfect absorption (CPA). We demonstrate and investigate super-resonant coherent absorption in a coupled Fabry-Perot (FP)/ring cavity structure. At the FP resonant wavelengths, the described phenomenon gives rise to split modes with a nearly-transparent peak and a peak whose transmission is exceptionally sensitive to the intracavity loss. For small losses, the effective interaction pathlength of these modes is proportional respectively to the ratio and the product of the individual finesse coefficients of the two resonators. The results presented extend the conventional definition of resonant absorption and point to a way of circumventing the technological limitations of ultrahigh-quality resonators in spectroscopy and optical sensing schemes.
Cavity-enhanced absorption spectroscopy is now widely used as an ultrasensitive technique in observing weak spectroscopic absorptions. Photons inside the cavity are reflected back and forth between the mirrors with reflectivities R close to one and thus (on average) exploit an absorption pathlength L that is 1/(1 − R ) longer than a single pass measurement. As suggested by the Beer-Lambert law, this increase in L results in enhanced absorbance A (given by αL with α being the absorption coefficient) which in turn favours the detection of weak absorptions. At the same time, however, only (1 − R ) of the incident light can enter the cavity [assuming that mirror transmission T is equal to (1 − R )], so that the reduction in transmitted light intensity Δ I caused by molecular absorption equates to that would be obtained if in fact no cavity were present . The enhancement in A = Δ I / I , where I is the total transmitted light intensity, achievable from CEAS therefore comes not from an increase in Δ I , but a sharp decrease in I. In this paper, we calculate the magnitudes of these two terms before and after a cavity is introduced, and aim at interpreting the sensitivity improvement offered by cavity-enhanced absorption spectroscopy from this observable-oriented (i.e. Δ I and I ) perspective. It is first shown that photon energy stored in the cavity is at best as intense as the input light source, implying that any absorbing sample within the cavity is exposed to the same or even lower light intensity after the cavity is formed. As a consequence, the intensity of the light absorbed or scattered by the sample, which corresponds to the Δ I term aforementioned, is never greater than would be the case in a single pass measurement. It is then shown that while this “numerator” term is not improved, the “denominator” term, I , is reduced considerably; therefore, the increase in contrast ratio Δ I / I is solely contributed by the attenuation of transmitted background light I and is ultimately down to the suppression of any measurement noise that is associated with it. The noise component that is most effectively suppressed is the type whose magnitude scales linearly with light intensity I , as is typical of noise caused by environmental instabilities, followed by the shot noise which scales as square root of I . No suppression is achievable for noise sources that are independent of I , a notable example being the thermal noise of a detector or of detection electronics. The usefulness of this “noise suppression” argument is that it links the sensitivity gain offered by a cavity with the property of measurement noise present in the system, and clearly suggests that the achievable sensitivity is dependent on how efficient the various noise components are “suppressed” by the cavity.
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.
We present a cavity-enhanced optical absorption measurement technique based on high-bandwidth Pound-Drever-Hall (PDH) sideband locking, which naturally provides a real-time, resonant amplitude quadrature readout that can be mapped onto the cavity’s internal loss rate. Cavity-enhancement is widely used in the detection of small signals -- an optical cavity traps photons between two highly reflective mirrors, thereby enhancing the effective path length through the absorber [Romanini et al., 2014]. Most of the available techniques, however, probe transmission signals and/or do not provide the stability required for the detection of fast signals.To ensure optimal enhancement of absorption sensitivity, probe light must be locked on resonance with the cavity. PDH locking relies on phase modulation of a laser beam, creating two sidebands on the original carrier frequency [Black, 2001]. Upon reflection from a cavity, this modulated light produces a heterodyne signal (beat note) that can be detected and demodulated. We use the phase quadrature of the beat note to lock the cavity on resonance with one of the sidebands, achieving a locking bandwidth in the MHz range that keeps cavity and probe light resonant for hours [Reinhardt et al., 2017]. Simultaneously, we monitor the amplitude quadrature, which provides a continuous, real-time, heterodyne-amplified readout of the cavity’s internal absorption. Our PDH sideband cavity-enhanced absorption readout technique (SideCAR) ensures high sensitivity without reaching saturation limits in the intracavity medium by keeping a relatively low intracavity power, since only one of the sidebands is allowed to enter the cavity, but the signal is boosted above the detector noise by heterodyne detection (using the carrier as a local oscillator).This thesis presents the theoretical formulation of the sensing technique together with the expressions for the sensitivity limit (ultimately given by the laser quantum noise), and the experimental results from a test cavity setup. Probing a proof-of-concept 5-cm-long Fabry-Perot cavity with a coupled power of 160 uW, we measure an absorption sensitivity of 7*10^(-11) cm^(-1)/sqrt(Hz) at 100 kHz (roughly the cavity bandwidth), a factor of 11 from the shot-noise limit. This technique allows the detection of small, transient signals against absorptive backgrounds with sensitivity close to the shot noise limit using a reflection-based measurement in a fairly simple setup, opening the possibility of developing new microscopic single-port real-world sensors for transients, for example using micron-scale optical fiber cavities
This paper presents a theoretical analysis of the optical properties of an optical cavity with both one- and two-photon intracavity absorption loss, without saturation. The cavity two-photon absorption loss per pass is assumed to be small, but otherwise the analysis is general. Analytical results for the cavity transmission as a function of cavity parameters, linear and two-photon intracavity loss, and detuning from resonance are derived and limiting cases discussed. Extraction of the two-photon loss from both cavity ring-down and cavity-enhanced absorption spectroscopy methods is analyzed and the predicted shot-noise limited sensitivities derived and compared. Numerical results are computed using the parameters of a recent experimental intracavity measurement of two-photon absorption of nitrous oxide. The results will be useful in the design and interpretation of cavity-enhanced, two-photon absorption spectroscopy.