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TOWARDS THE ULTIMATE OPTICAL DETECTION SENSITIVITY: NEW SPECTROSCOPIC OPPORTUNITIES- AND A ZILLION NEW WAVELENGTH/FREQUENCY STANDARDS

J. L. Hall

Published Jan 1, 1996• 0 citations
OpenAlex

Abstract

High sensitivity detection of quantum absorption is demonstrated at a sensitivity of $1 \\times 10^{11}$ integrated absorption, in 1 sec, using 10 mTorr total gas pressure. Achieving highly sensitive detection relies on simple basic principles: 1) The molecule-generated electric field in the forward direction (the "darkness wave") is most precious, and contains the maximum available information. It is the physical manifestation of the -$alpha^{*}$L term appearing when beer#### absorption law is expanded for low opacity, 2) After generating the molecular signal, the detected unabsorbed light sets the "shotnoise" measurement floor. We use an optical transmission cavity for the gas cell, since the high internal "build-up" field will elicit a strong molecular "darkness wave", for a given transmitted de light on the detector, A more conventional explanation of Gavity Enhancement would be the extension of the effective cell length by the factor finesse $^{*}2/\\pi.3$) To avoid excess low-frequency noise, such small signals should be measured by ac methods, comparing on-resonant and off-resonant cases in quick succession. 4) By SIMULTANEOUSLY obtaining and subtracting these cases, one provides a siginal channel with NO OUTPUT unless there is a resonance. This is conveniently accomplished by using the FM detection method with the optical heterodyne sidebands and carrier being transmitted through the cavity via adjacent axial orders 5). A remarkable property of this configuration, when the modulation frequency= cavity mode spacing, is the suppression of ANY detection of laser frequency noise with the transmitted light. We can refer to this property as (laser FM-) noise-Immune detection. This enables profitable use of cavity finesse in the range above 10,000, without a nois penalty, Altogether, we refer to this new spectroscopy as Noise-Immune, Cavity-Enhanced, Optical Heterodyne Molecular spectroscopy, i.e. "NICE OHMS". We have measured excellent saturated dispersion signals from HCCH in the band near 790 mm ($\\nu_{1} + 3 \\nu_{3}$), and recently, using a Nd:YAG source, from the HCCD P(5) line ($\\nu_{2} + 3 \\nu_{3}$) at 1064 mm. The saturation peaks broaden from the transit limit of 270 kHz near zero pressure at the rate 34.7 kHz/m Torr. We observe interesting narrow linwidths 8-fold below the transit limit, basically using optical selection of slow molecules by low power and pressure (2 mW and 2 m Torr). The absolute frequency is measurred to be 281, 635,363,960 MHz $\\pm 45$ kHz.

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Cavity-enhanced absorption sensing based on Pound-Drever-Hall sideband locking

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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

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CAVITY-ENHANCED ULTRAFAST TRANSIENT ABSORPTION SPECTROSCOPY

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We introduce cavity enhanced ultrafast transient absorption spectroscopy, which employs frequency combs and high-finesse optical cavities. % The schematic of apparatus is shown in Figure 1. Sub-100 fs pulses with a repetition rate of 90 MHz are generated by a home-built Ytterbium fiber laser. The amplified light has a power up to 10 W, which is used to pump an optical parametric oscillator, followed by second-harmonic generation(SHG) that converts the wavelength from near-IR to visible. A pump comb at 530 nm is separately generated by SHG. Both pump and probe combs are coupled into high-finesse cavities. Compared to the conventional transient absorption spectroscopy method, the detection sensitivity can be improved by a factor of $\left(\frac{\mathcal{F}}{\pi} \right)^2 \sim 10^5$, where $\mathcal{F}$ is the finesse of cavity. This ultrasensitive technology enables the direct all-optical dynamics study in molecular beams. We will apply the cavity enhanced ultrafast transient absorption spectroscopy to investigate the dynamics of visible chromophores and then extend the wavelength to mid-IR to study vibrational dynamics of small hydrogen-bonded clusters. %\begin{wrapfigure}{I}{1\textwidth} % \centering % \includegraphics[width = 0.7\textwidth]{CETAS_details.eps} %\caption{Schematic of cavity enhanced ultrafast transient absorption spectroscopy apparatus. An amplified fiber laser frequency comb is converted to visible light and pump and probe combs are coupled to high-finesse optical resonators. Transmission of the probe light is measured.} %\end{wrapfigure}

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Precision molecular spectroscopy provides a sensitive detection method for ultralight bosonic dark matter. This wavelike dark matter couples to the Standard Model fundamental constants, modulates the frequencies of the molecular transitions and of the resonances of the optical cavities, and brings oscillations in the laser absorption spectroscopy signals. Spectroscopy experiments with differential detection methods approach the fundamental limitation imposed by quantum noise in photodetection. The use of squeezed light in spectroscopy is addressed here to circumvent this limitation. An experimental setup is proposed for the interrogation of an acetylene transition at 1542 nm with a bright squeezed light field and a homodyne detection scheme. This approach enables measurements using the squeezed quadrature, ensures broadband sensitivity, demonstrates robustness to moderate losses, and provides improved constraints for the couplings of the ultralight bosonic dark matter to the Standard Model in the radiofrequency range.

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The Noise-Immune Cavity-Enhanced Optical Heterodyne Molecular Spectrometry (NICE-OHMS) is a modern technique renowned for its ultimate sensitivity, because it combines long equivalent absorption length provided by a high finesse cavity, and a detection theoretically limited by the sole photon-shot-noise. One fallout of the high finesse is the possibility to accumulating strong intracavity electromagnetic fields (EMF). Under this condition, molecular transitions can be easy saturated giving rise to the usual Lamb dips (or hole burning). However, the unusual shape of the basically trichromatic EMF (due to the RF lateral sidebands) induces nonlinear couplings, i.e., new crossover transitions. An analytical methodology will be presented to calculate spectra provided by NICE-OHMS experiments. It is based on the solutions of the equations of motion of an open two-blocked-level system performed in the frequency-domain (optically thin medium). Knowing the transition dipole moment, the NICE-OHMS signals (``absorption-like'' and ``dispersion-like'') can be simulated by integration over the Doppler shifts and by paying attention to the molecular Zeeman sublevels and to the EMF polarizationfootnote{J. Opt. Soc. Am. B 32, 838 (2015)}. The approach has been validated by discussion experimental data obtained on two transitions of ${rm C_{2}H_{2}}$ in the near-infrared under moderated saturationfootnote{Optics Express 16, 14689 (2008)}. One of the applications of the saturated absorption is to be able to simultaneously determine the transition intensity and the density number while only one these 2 quantities can only be assessed in nonlinear absorption.

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Understanding the sensitivity of cavity-enhanced absorption spectroscopy: pathlength enhancement versus noise suppression

Bin Ouyang, Roderic L. Jones

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.

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Jun Ye, J. L. Hall

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.

Physical Review A•May 17, 2000•52 citations
High sensitivity detection of quantum absorption is demonstrated at a sensitivity of 1times10111 \\times 10^{11}1times1011 integrated absorption, in 1 sec, using 10 mTorr total gas pressure. Achieving highly sensitive detection relies on simple basic principles: 1) The molecule-generated electric field in the forward direction (the "darkness wave") is most precious, and contains the maximum available information. It is the physical manifestation of the -alpha∗alpha^{*}alpha∗L term appearing when beer#### absorption law is expanded for low opacity, 2) After generating the molecular signal, the detected unabsorbed light sets the "shotnoise" measurement floor. We use an optical transmission cavity for the gas cell, since the high internal "build-up" field will elicit a strong molecular "darkness wave", for a given transmitted de light on the detector, A more conventional explanation of Gavity Enhancement would be the extension of the effective cell length by the factor finesse ∗2/pi.3^{*}2/\\pi.3∗2/pi.3) To avoid excess low-frequency noise, such small signals should be measured by ac methods, comparing on-resonant and off-resonant cases in quick succession. 4) By SIMULTANEOUSLY obtaining and subtracting these cases, one provides a siginal channel with NO OUTPUT unless there is a resonance. This is conveniently accomplished by using the FM detection method with the optical heterodyne sidebands and carrier being transmitted through the cavity via adjacent axial orders 5). A remarkable property of this configuration, when the modulation frequency= cavity mode spacing, is the suppression of ANY detection of laser frequency noise with the transmitted light. We can refer to this property as (laser FM-) noise-Immune detection. This enables profitable use of cavity finesse in the range above 10,000, without a nois penalty, Altogether, we refer to this new spectroscopy as Noise-Immune, Cavity-Enhanced, Optical Heterodyne Molecular spectroscopy, i.e. "NICE OHMS". We have measured excellent saturated dispersion signals from HCCH in the band near 790 mm (nu1+3nu3\\nu_{1} + 3 \\nu_{3}nu1​+3nu3​), and recently, using a Nd:YAG source, from the HCCD P(5) line (nu2+3nu3\\nu_{2} + 3 \\nu_{3}nu2​+3nu3​) at 1064 mm. The saturation peaks broaden from the transit limit of 270 kHz near zero pressure at the rate 34.7 kHz/m Torr. We observe interesting narrow linwidths 8-fold below the transit limit, basically using optical selection of slow molecules by low power and pressure (2 mW and 2 m Torr). The absolute frequency is measurred to be 281, 635,363,960 MHz pm45\\pm 45pm45 kHz.
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
We introduce cavity enhanced ultrafast transient absorption spectroscopy, which employs frequency combs and high-finesse optical cavities. % The schematic of apparatus is shown in Figure 1. Sub-100 fs pulses with a repetition rate of 90 MHz are generated by a home-built Ytterbium fiber laser. The amplified light has a power up to 10 W, which is used to pump an optical parametric oscillator, followed by second-harmonic generation(SHG) that converts the wavelength from near-IR to visible. A pump comb at 530 nm is separately generated by SHG. Both pump and probe combs are coupled into high-finesse cavities. Compared to the conventional transient absorption spectroscopy method, the detection sensitivity can be improved by a factor of (Fπ)2∼105\left(\frac{\mathcal{F}}{\pi} \right)^2 \sim 10^5(πF​)2∼105, where F\mathcal{F}F is the finesse of cavity. This ultrasensitive technology enables the direct all-optical dynamics study in molecular beams. We will apply the cavity enhanced ultrafast transient absorption spectroscopy to investigate the dynamics of visible chromophores and then extend the wavelength to mid-IR to study vibrational dynamics of small hydrogen-bonded clusters. %\begin{wrapfigure}{I}{1\textwidth} % \centering % \includegraphics[width = 0.7\textwidth]{CETAS_details.eps} %\caption{Schematic of cavity enhanced ultrafast transient absorption spectroscopy apparatus. An amplified fiber laser frequency comb is converted to visible light and pump and probe combs are coupled to high-finesse optical resonators. Transmission of the probe light is measured.} %\end{wrapfigure}
Precision molecular spectroscopy provides a sensitive detection method for ultralight bosonic dark matter. This wavelike dark matter couples to the Standard Model fundamental constants, modulates the frequencies of the molecular transitions and of the resonances of the optical cavities, and brings oscillations in the laser absorption spectroscopy signals. Spectroscopy experiments with differential detection methods approach the fundamental limitation imposed by quantum noise in photodetection. The use of squeezed light in spectroscopy is addressed here to circumvent this limitation. An experimental setup is proposed for the interrogation of an acetylene transition at 1542 nm with a bright squeezed light field and a homodyne detection scheme. This approach enables measurements using the squeezed quadrature, ensures broadband sensitivity, demonstrates robustness to moderate losses, and provides improved constraints for the couplings of the ultralight bosonic dark matter to the Standard Model in the radiofrequency range.
The Noise-Immune Cavity-Enhanced Optical Heterodyne Molecular Spectrometry (NICE-OHMS) is a modern technique renowned for its ultimate sensitivity, because it combines long equivalent absorption length provided by a high finesse cavity, and a detection theoretically limited by the sole photon-shot-noise. One fallout of the high finesse is the possibility to accumulating strong intracavity electromagnetic fields (EMF). Under this condition, molecular transitions can be easy saturated giving rise to the usual Lamb dips (or hole burning). However, the unusual shape of the basically trichromatic EMF (due to the RF lateral sidebands) induces nonlinear couplings, i.e., new crossover transitions. An analytical methodology will be presented to calculate spectra provided by NICE-OHMS experiments. It is based on the solutions of the equations of motion of an open two-blocked-level system performed in the frequency-domain (optically thin medium). Knowing the transition dipole moment, the NICE-OHMS signals (``absorption-like'' and ``dispersion-like'') can be simulated by integration over the Doppler shifts and by paying attention to the molecular Zeeman sublevels and to the EMF polarizationfootnote{J. Opt. Soc. Am. B 32, 838 (2015)}. The approach has been validated by discussion experimental data obtained on two transitions of rmC2H2{rm C_{2}H_{2}}rmC2​H2​ in the near-infrared under moderated saturationfootnote{Optics Express 16, 14689 (2008)}. One of the applications of the saturated absorption is to be able to simultaneously determine the transition intensity and the density number while only one these 2 quantities can only be assessed in nonlinear absorption.
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.
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.