Birgitta Bernhardt, Akira Ozawa, Patrick Jacquet, Marion Jacquey, Yohei Kobayashi, Thomas Udem, Ronald Holzwarth, Guy Guelachvili, Theodor W. Hänsch, Nathalie Picqué
The sensitivity of molecular fingerprinting is dramatically improved when placing the absorbing sample in a high-finesse optical cavity, thanks to the large increase of the effective path-length. As demonstrated recently, when the equidistant lines from a laser frequency comb are simultaneously injected into the cavity over a large spectral range, multiple trace-gases may be identified within a few milliseconds. Analyzing efficiently the light transmitted through the cavity however still remains challenging. Here, a novel approach, cavity-enhanced frequency comb Fourier transform spectroscopy, fully overcomes this difficulty and measures ultrasensitive, broad-bandwidth, high-resolution spectra within a few tens of $μ$s. It could be implemented from the Terahertz to the ultraviolet regions without any need for detector arrays. We recorded, within 18 $μ$s, spectra of the 1.0 $μ$m overtone bands of ammonia spanning 20 nm with 4.5 GHz resolution and a noise-equivalent-absorption at one-second-averaging per spectral element of 3 10^-12 cm^-1Hz^-1/2, thus opening a route to time-resolved spectroscopy of rapidly-evolving single-events.
We report a technique based upon the cavity ringdown method that enables to characterize the Brillouin gain coefficient directly in a laser cavity. Material gain, optical cavity parameters and lasing properties can be extracted from measurements whithin a single experiment.
Absorption spectroscopy is widely used to detect samples with spectral specificity. Here, we propose and demonstrate a method for enhancing the sensitivity of absorption spectroscopy. Exploiting multiple light scattering generated by a boron nitride (h-BN) scattering cavity, the optical path lengths of light inside a diffusive reflective cavity are significantly increased, resulting in more than ten times enhancement of sensitivity in absorption spectroscopy. We demonstrate highly sensitive spectral measurements of low concentrations of malachite green and crystal violet aqueous solutions. Bec…
We demonstrate broadband and sensitive cavity ring-down spectroscopy using a near infrared frequency comb and a time-resolved Fourier transform spectrometer. The cavity decays are measured simultaneously and spectrally sorted, leading to purely exponential decays for each spectral element. The absorption spectra of atmospheric water and carbon dioxide are retrieved and demonstrate the high frequency resolution and absorption precision of the technique. The experimental apparatus, the measurement concept and the data treatment are described. The technique benefits from the advantages of cavity …
Liquid phase sensing applications at 1550~nm are highly desirable due to widely available off-the-shelf components. Generally, liquids at 1550~nm induce a high absorption loss that limits the overall sensor's sensitivity and detection limit. One solution is to use an active fiber loop in conjunction with cavity ring down spectroscopy to overcome these absorption losses. However, the amplifier inside the fiber loop suffers from inherent gain fluctuations that limit the sensing system's overall performance. Here, we provide a novel sensor using the wavelength-scanned phase shift-cavity ring down…
Dual-comb generation from a single laser cavity provides a simple and high-performance solution to time sampling applications. We demonstrate a compact single-cavity dual-comb laser operating at gigahertz repetition rates and high repetition rate differences up to more than 100 kHz with sub-100 fs pulse duration. The single cavity approach leads to passive common noise suppression resulting in ultra-low relative timing jitter and fully resolvable comb lines in free-running operation. We showcase the laser performance with two application demonstrations: (a) time-domain spectroscopy of acetylen…
本文报道了一种新的光腔衰荡光谱方法，样品气体处于饱和吸收区。这种技术允许去耦，并同时检索空腔背景和吸收信号，通过我们开发和测试的理论模型。利用光谱应用的高灵敏度和频率精度，首次测量了自然丰度的$^{17}$ O $^{12}$ C $^{16}$ O的激发振动态的超精细结构，其精度为$10^{-11}$中的几个部分。
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 scanning5 or susceptibility to nonlinearities limits their ultimate performance. Here we present cavity buildup dispersion spectroscopy (CBDS) in which the dispersive frequency shift of a cavity resonance is encoded in the cavit…
The efficiency of the frequency conversion process at the heart of Raman heterodyne spectroscopy was improved by nearly four orders of magnitude by resonant enhancement of both the pump and signal optical fields. Our results using an erbium doped Y$_2$SiO$_5$ crystal at temperatures near 4K suggest that such an approach is promising for the quantum conversion of microwave to optical photons.
We present a complex-valued electric field model for experimentally observed cavity transmission in coherent cavity-enhanced (CE) multiplexed spectroscopy (i.e., dual-comb spectroscopy, DCS). The transmission model for CE-DCS differs from that previously derived for Fourier-transform CE direct frequency comb spectroscopy [Foltynowicz et al., Appl. Phys. B 110, 163-175 (2013)] by the treatment of the local oscillator which, in the case of CE-DCS, does not interact with the enhancement cavity. Validation is performed by measurements of complex-valued near-infrared spectra of CO and CO$_2$ by an …
The achievable instrument sensitivity is a critical parameter for the continued development of THz applications. Techniques such as Cavity-Enhanced Techniques and Cavity Ring Down Spectroscopy have not yet been employed at THz frequency due to the difficulties to construct a high finesse Fabry-Pérot cavity. Here, we describe such a THz resonator based on a low-loss oversized corrugated waveguide with highly reflective photonic mirrors obtaining a finesse above 3000 around 620 GHz. These components enable a Fabry-Perot THz Absorption Spectrometer with an equivalent interaction length of one kil…
Vertical external-cavity surface-emitting lasers (VECSELs) augmented by intra-cavity nonlinear optical frequency conversion have emerged as an attractive light source of ultraviolet to visible light for demanding scientific applications, relative to other laser technologies. They offer high power, low phase noise, wide frequency tunability, and excellent beam quality in a simple and inexpensive system architecture. Here, we characterize the frequency stability of an intra-cavity frequency-doubled VECSEL with 690 mW of output power at 475 nm using the delayed self-heterodyne technique and direc…
Broadband ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D spectroscopy, are widely used to study molecular dynamics. However, these techniques are typically restricted to optically thick samples, such as solids and liquid solutions. In this article we discuss a cavity-enhanced ultrafast transient absorption spectrometer covering almost the entire visible range with a detection limit of $Δ$OD $ < 1 \times 10^{-9}$, extending broadband all-optical ultrafast spectroscopy techniques to dilute beams of gas-phase molecules and clusters. We describe the techni…
Mode-resolved dual-comb spectroscopy (DCS) is an emerging spectroscopic tool with the potential to simultaneously achieve a broad spectral coverage and ultrahigh spectral resolution in terahertz (THz) spectroscopy. However, the need for two independently stabilized ultrafast lasers significantly hampers the potential application of DCS techniques. In this article, we demonstrate mode-resolved DCS in the THz region based on a free-running single-cavity dual-comb fiber laser with adaptive sampling. Low-pressure spectroscopy of acetonitrile gas with absorption features approaching the Doppler lim…
Advances in high-resolution laser spectroscopy have enabled many scientific breakthroughs in physics, chemistry, biology and astronomy. Optical frequency combs have pushed measurement limits with ultrahigh-frequency accuracy and fast-measurement speed while tunable diode laser spectroscopy is used in scenarios that require high power and continuous spectral coverage. Despite these advantages of tunable diode laser spectroscopy, it is challenging to precisely determine the instantaneous frequency of the laser because of fluctuations in the scan speed. Here we demonstrate a simple spectroscopy s…
We report on the coupling of the emission from a single europium-doped nanocrystal to a fiber-based microcavity under cryogenic conditions. As a first step, we study the sample properties and observe a strong correlation between emission lifetime and brightness, as well as a lifetime reduction for nanocrystals embedded in a polymer film. This is explained by differences in the local density of states. We furthermore quantify the scattering loss of a nanocrystal inside the cavity and use this to deduce the crystal size. Finally, by resonantly coupling the cavity to a selected transition, we per…
One way of optically monitoring molecule concentrations is to utilise the high sensitivity of the transmission and reflection rates of Fabry-Perot cavities to changes of their optical properties. Up to now, intrinsic and extrinsic Fabry-Perot cavity sensors have been considered with analytes either being placed inside the resonator or coupled to evanescent fields on the outside. Here we show that Fabry-Perot cavities can also be used to monitor molecule concentrations non-invasively and remotely, since the reflection of light from the target molecules back into the Fabry-Perot cavity adds upwa…
Optical cavities can enhance and control light-matter interactions. This has recently been extended to the nanoscale, and with single emitter strong coupling regime even at room temperature using plasmonic nano-cavities with deep sub-diffraction-limited mode volumes. However, with emitters in static nano-cavities, this limits the ability to tune coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) spectroscopy, imaging, and control. Based on a nano-cavity formed between a scanning plasmonic antenna-tip and the substrate, by …
Efficient quantum memory is of paramount importance for long-distance quantum communications, as well as for complex large-scale computing architectures. We investigate the capability of Er$^{3+}$:Y$_2$SiO$_5$ crystal to serve as a quantum memory for the travelling microwave photons by employing techniques developed for dense optical ensembles. In our efforts to do so, we have performed high-resolution microwave spectroscopy of Er$^{3+}$:Y$_2$SiO$_5$, where we identified electronic spin as well as hyperfine transitions. Furthermore, we have explored spectral hole burning technique and studied …
We report the most accurate measurement of the position of the weak quadrupole S(2) 2-0 line in D$_2$. The spectra were collected with a frequency-stabilized cavity ring-down spectrometer (FS-CRDS) with an ultra-high finesse optical cavity ($\mathcal{F}$ = 637 000) and operating in the frequency-agile, rapid scanning spectroscopy (FARS) mode. Despite working in the Doppler-limited regime, we reached 40 kHz of statistical uncertainty and 161 kHz of absolute accuracy, achieving the highest accuracy for homonuclear isotopologues of molecular hydrogen. The accuracy of our measurement corresponds t…
