Rapid generation of massive thermodynamic datasets using frequency comb spectroscopy.

We demonstrate massively parallel spectroscopic measurements of 12C2H2 using an optical frequency comb. This allows for the rapid and simultaneous estimation of self-broadening and self-shifting of more than 50 optical transitions between 1512 and 1538 nm. The use of a temperature-controlled sealed gas cell allows us to measure both pressure- and temperature-mediated broadening and shifting. We present the results for the pressure-mediated self-broadening and self-shifting coefficients for 59 optical lines that make up the v1 + v3 combination band and a selection of hot bands. Our ability to measure the broadening of numerous transitions allows for the confirmation of prior work that shows that there is no measurable vibrational dependence across all acetylene bands, despite the strong dependence of the broadening coefficient on the rotational number. We also present an extensive measurement of the temperature dependence of the self-broadening for each of these 59 lines. This work shows the revolutionary power afforded by the frequency combs for rapid generation of large datasets related to thermodynamic variations of the key spectroscopic parameters of important gases.

Comb spectroscopy of CO2 produced from microbial metabolism.

We have developed a direct frequency comb spectroscopy instrument, which we have tested on Saccharomyces cerevisiae (baker's yeast) by measuring its CO2 output and production rate as we varied the environmental conditions, including the amount and type of feed sugar, the temperature, and the amount of yeast. By feeding isotopically-enhanced sugar to the yeast, we demonstrate the capability of our device to differentiate between two isotopologues of CO2, with a concentration measurement precision of 260 ppm for 12C16O2 and 175 ppm for 13C16O2. We also demonstrate the ability of our spectrometer to measure the proportion of carbon in the feed sugar converted to CO2, and estimate the amount incorporated into the yeast biomass.

Orthogonalizing the control of frequency combs for optical clockworks.

Frequency combs play a crucial supporting role for optical clocks by allowing coherent frequency division of their output signals into the electronic domain. This task requires stabilization of the comb's offset frequency and of an optical comb mode to the clock laser. However, the two actuators used to control these quantities often influence both degrees of freedom simultaneously. This non-orthogonality leads to artificial limits to the control bandwidth and unwanted noise in the comb. Here, we orthogonalize the two feedback loops with a linear combination of the measured signals in a field-programmable gate array. We demonstrate this idea using a fiber frequency comb stabilized to a clock laser at 259 THz, half the frequency of the 1S0→3P0 Yb transition. The decrease in coupling between the loops reduces the comb's optical phase noise by 20 dB. This approach could improve the performance of any comb stabilized to any optical frequency standard.

Complex direct comb spectroscopy with a virtually imaged phased array.

We demonstrate a simple interferometric technique to directly measure the complex optical transmittance over a large spectral range using a frequency-comb spectrometer based on a virtually imaged phased array. A Michelson interferometer encodes the phase deviations induced by a sample contained in one of its arms into an interferogram image. When combined with an additional image taken from each arm separately, along with a frequency-calibration image, this allows full reconstruction of the sample's optical transfer function. We demonstrate the technique with a vapor cell containing H13C14N, producing transmittance and phase spectra spanning 2.9 THz (∼23 nm) with ∼1 GHz resolution.

A quantitative mode-resolved frequency comb spectrometer.

We have developed a frequency-comb spectrometer that records 35-nm (4 THz) spectra with 2-pm (250 MHz) spectral sampling and an absolute frequency accuracy of 2 kHz. We achieve a signal-to-noise ratio of ~400 in a measurement time of 8.2 s. The spectrometer is based on a commercial frequency comb decimated by a variable-length, low-finesse Fabry Pérot filter cavity to fully resolve the comb modes as imaged by a virtually imaged phased array (VIPA), diffraction grating and near-IR camera. By tuning the cavity length, spectra derived from all unique decimated combs are acquired and then interleaved to achieve frequency sampling at the comb repetition rate of 250 MHz. We have validated the performance of the spectrometer by comparison with a previous high-precision absorption measurement of H13C14N near 1543 nm. We find excellent agreement, with deviations from the expected line centers and widths of, at most, 1 pm (125 MHz) and 3 pm (360 MHz), respectively.