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Register a new userBroadband calibration-free cavity-enhanced complex refractive index spectroscopy using a frequency comb
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Aleksandra Foltynowicz
Publication date
2018
fields
Physics
and research's language is
English
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We present broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), a technique for calibration-free determination of the complex refractive index of entire molecular bands via direct measurement of transmission modes of a Fabry-Perot cavity filled with the sample. The measurement of the cavity transmission spectrum is done using an optical frequency comb and a mechanical Fourier transform spectrometer with sub-nominal resolution. Molecular absorption and dispersion spectra (corresponding to the imaginary and real parts of the refractive index) are obtained from the cavity mode broadening and shift retrieved from fits of Lorentzian profiles to the individual cavity modes. This method is calibration-free because the mode broadening and shift are independent of the cavity parameters such as the length and mirror reflectivity. In this first demonstration of broadband CE-CRIS we measure simultaneously the absorption and dispersion spectra of three combination bands of CO2 in the range between 1525 nm and 1620 nm and achieve good agreement with theoretical models. This opens up for precision spectroscopy of the complex refractive index of several molecular bands simultaneously.
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Noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS) is a recently developed technique that utilizes phase modulation to obtain immunity to frequency-to-amplitude noise conversion by the cavity modes and yields high absorption sensitivity over a broad spectral range. We describe the principles of the technique and discuss possible comb-cavity matching solutions. We present a theoretical description of NICE-OFCS signals detected with a Fourier transform spectrometer (FTS), and validate the model by comparing it to experimental CO2 spectra around 1575 nm. Our system is based on an Er:fiber femtosecond laser locked to a cavity and phase-modulated at a frequency equal to a multiple of the cavity free spectral range (FSR). The NICE-OFCS signal is detected by a fast-scanning FTS equipped with a high-bandwidth commercial detector. We demonstrate a simple method of passive locking of the modulation frequency to the cavity FSR that significantly improves the long term stability of the system, allowing averaging times on the order of minutes. Using a cavity with a finesse of ~9000 we obtain absorption sensitivity of 6.4 x 10^{-11} cm^{-1} Hz^{-1/2} per spectral element, and concentration detection limit for CO2 of 450 ppb Hz^{-1/2}, determined by multiline fitting.
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 $Delta$OD $ < 1 times 10^{-9}$, extending broadband all-optical ultrafast spectroscopy techniques to dilute beams of gas-phase molecules and clusters. We describe the technical innovations behind the spectrometer and present transient absorption data on two archetypical molecular systems for excited-state intramolecular proton transfer, 1-hydroxy-2-acetonapthone and salicylideneaniline, under jet-cooled and Ar cluster conditions.
Precision laser spectroscopy is key to many developments in atomic and molecular physics and the advancement of related technologies such as atomic clocks and sensors. However, in important spectroscopic scenarios, such as astronomy and remote sensing, the light is of thermal origin and interferometric or diffractive spectrometers typically replace laser spectroscopy. In this work, we employ laser-based heterodyne radiometry to measure incoherent light sources in the near-infrared and introduce techniques for absolute frequency calibration with a laser frequency comb. Measuring the solar continuum, we obtain a signal to noise ratio that matches the prediction given by the thermal photon distribution and our systems quantum efficiency. With absolute frequency calibration we determine the center frequency of an iron line in the solar spectrum to MHz-level uncertainty in under 10 minutes, a fractional precision 1/4000 the linewidth. Additionally, we propose concepts that take advantage of refractive beam shaping to decrease pointing instabilities by nearly 100x, and of frequency comb multiplexing to increase data acquisition rates and spectral bandwidths by comparable factors. Taken together, our work brings the power of telecommunications photonics and the precision of frequency comb metrology to laser heterodyne radiometry, with implications for solar and astronomical spectroscopy, remote sensing, and precise Doppler velocimetry.
The use of relatively simple structures to achieve high performance refractive index sensors has always been urgently needed. In this work, we propose a lithography-free sensing platform based on metal-dielectric cavity, the sensitivity of our device can reach 1456700 nm/RIU for solution and 1596700 nm/RIU for solid material, and the FOM can be up to 1234500 /RIU for solution and 1900800 /RIU for solid material, which both are much higher than most sensing methods. This sensor has excellent sensing performance in both TE and TM light, and suitable for integrated microfluidic channels. Our scheme uses a multi-layers structure with a 10 nm gold film sandwiched between prism and analyte, and shows a great potential for low-cost sensing with high performance.
Context: Reliable, directly measured optical properties of astrophysical ice analogs in the infrared (IR) and terahertz (THz) range are missing. These parameters are of great importance to model the dust continuum radiative transfer in dense and cold regions, here thick ice mantles are present, and are necessary for the interpretation of future observations planned in the far-IR region. Aims: Coherent THz radiation allows direct measurement of the complex dielectric function (refractive index) of astrophysically relevant ice species in the THz range. Methods: The time-domain waveforms and the frequency-domain spectra of reference samples of CO ice, deposited at a temperature of 28.5 K and annealed to 33 K at different thicknesses, have been recorded. A new algorithm is developed to reconstruct the real and imaginary parts of the refractive index from the time-domain THz data. Results: The complex refractive index in the wavelength range of 1 mm - 150 ${mu}$m (0.3 - 2.0 THz) has been determined for the studied ice samples, and compared with available data found in the literature. Conclusions: The developed algorithm of reconstructing the real and imaginary parts of the refractive index from the time-domain THz data enables, for the first time, the determination of optical properties of astrophysical ice analogs without using the Kramers-Kronig relations. The obtained data provide a benchmark to interpret the observational data from current ground based facilities as well as future space telescope missions, and have been used to estimate the opacities of the dust grains in presence of CO ice mantles.
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