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International Symposium on Molecular Spectroscopy (ISMS)

CAVITY-ENHANCED ULTRAFAST TRANSIENT ABSORPTION SPECTROSCOPY

Yuning Chen, Thomas G. Allison, Kevin Keleher, Melanie A. R. Reber

Published Jun 16, 2014• 0 citations
Publisher

Abstract

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}

DOI
10.15278/isms.2014.mh14

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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 (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}
A high-finesse optical cavity was employed to perform highly sensitive spectroscopy of molecular oxygen at wavelengths near 763 nm. An equivalent absorption length of ∼1 km was obtained by a 26-cm-long optical cavity with a finesse of 6000. An extended cavity diode laser was frequency locked to the cavity, and pure absorption profiles were recovered by monitoring of the cavity transmission during continuous scans of the cavity resonance through O2 rotational lines, allowing a detailed investigation of the line shapes. Phase modulation of the laser at a frequency equal to the cavity free-spectral-range frequency was employed for detection of weak absorption signals inside the cavity. A minimum detectable absorption coefficient of 6.9×10-11 cm-1 Hz-1/2 was measured. Finally, a test of the symmetrization postulate in 16O nuclei was demonstrated.
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 demonstrate the generation of multiphoton quantum states of light by cavity-enhanced parametric down-conversion in the high-repetition-rate pulsed regime. An external enhancement cavity resonant with the spectral comb of modes of a mode-locked pump laser provides a coherent buildup of the pump intensity and greatly enhances the parametric gain without sacrificing its high repetition rate and comb structure. We probe the parametric gain enhancement by the conditional generation and tomographic analysis of two-photon Fock states. Besides its potential impact for efficiently generating highly nonclassical or entangled multiphoton states in many existing experimental setups, this scheme opens exciting perspectives toward the combination of quantum and comb technologies for enhanced measurements and advanced quantum computation protocols.
Abstract Measurements of ultrahigh-fidelity absorption spectra can help validate quantum theory, engineer ultracold chemistry, and remotely sense atmospheres. Recent achievements in cavity-enhanced spectroscopy using either frequency-based dispersion or time-based absorption approaches have set new records for accuracy with uncertainties at the sub-per-mil level. However, laser scanning or susceptibility to nonlinearities limits their ultimate performance. Here we present cavity buildup dispersion spectroscopy (CBDS), probing the CO molecule as an example, in which the dispersive frequency shift of a cavity resonance is encoded in the cavity’s transient response to a phase-locked non-resonant laser excitation. Beating between optical frequencies during buildup exactly localizes detuning from mode center, and thus enables single-shot dispersion measurements. CBDS can yield an accuracy limited by the chosen frequency standard and measurement duration and is currently 50 times less susceptible to detection nonlinearity compared to intensity-based methods. Moreover, CBDS is significantly faster than previous frequency-based cavity-enhanced methods. The generality of CBDS shows promise for improving fundamental research into a variety of light–matter interactions.
It is experimentally demonstrated that a narrow band continuous wave (cw) light source can be used in combination with a high-finesse optically stable cavity to perform sensitive, high-resolution direct absorption and optical rotation spectroscopy in an amazingly simple experimental setup, using ideas from the field of cavity ring down spectroscopy. Light from a scanning narrow band cw laser is coupled into the cavity via accidental coincidences of the laser frequency with the frequency of one of the multitude of modes of the cavity. The absorption and polarization rotation information is extracted from a measurement of the time-integrated light intensity leaking out of the cavity as a function of laser wavelength.