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Addendum: Sub-Doppler optical-optical double-resonance spectroscopy using a cavity-enhanced frequency comb probe

Vinicius Silva Oliveira, Isak Silander, Lucile Rutkowski, Grzegorz Soboń, Ove Axner, Kevin K. Lehmann, Aleksandra Foltynowicz

Published Jan 1, 2024• 0 citations
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We demonstrate a Doppler thermometer based on direct optical frequency comb spectroscopy of an 85^{85}85Rb vapor with a chirped electro-optic frequency comb (EOFC). The direct EOFC Doppler thermometer is accurate to within its approximately 1 K statistical uncertainty. We experimentally compare direct EOFC spectroscopy with conventional Doppler spectroscopy using a single-frequency, step-scanned laser probe. Our results show that direct EOFC spectroscopy mitigates transit-induced optical pumping distortion of the atomic lineshape, which is the dominant systematic temperature shift in alkali atom Doppler thermometry. Optical Bloch equation simulations of conventional and direct EOFC Doppler spectroscopy confirm that EOFC spectroscopy can use higher optical power to reduce statistical noise without optical pumping distortion. Our results indicate that EOFC Doppler thermometry is a promising approach to realizing a primary thermometer with size and measurement rate sufficient for applications including pharmaceutical manufacturing and nuclear waste monitoring.
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}
We study resonantly enhanced cascaded two-photon transitions in Doppler-broadened rubidium vapor, induced by an optical frequency comb. Cascaded two-step excitation of atoms from the ground state 5SSS1/2{}_{1/2}1/2​ to the final 5DDD5/2{}_{5/2}5/2​ state via an intermediate 5PPP3/2{}_{3/2}3/2​ state as well as the influence of the frequency comb repetition rate on the two-photon fluorescence signal have been investigated. It is shown that the careful choice of fR{f}_{R}fR​ leads to enhancement of the two-photon signal with considerable increase of the final 5D5/25{D}_{5/2}5D5/2​-state population due to velocity-selective double resonance. Since the double-resonance condition for two different rubidium isotopes is fulfilled for different fR{f}_{R}fR​, the possibility of isotope-selective two-photon excitation is explored. The dependence of the two-photon signal on external magnetic field values and different repetition rates of the optical frequency comb is also investigated.