Dual Comb Spectroscopy

List of publications Conference contribution

Coherent Raman spectro-imaging with laser frequency combs

Optical spectroscopy and imaging of microscopic samples have opened up a wide range of applications throughout the physical, chemical, and biological sciences. High chemical specificity may be achieved by directly interrogating the fundamental or low-lying vibrational energy levels of the compound molecules. Amongst the available prevailing label-free techniques, coherent Raman scattering has the distinguishing features of high spatial resolution down to 200 nm and three-dimensional sectioning. However, combining fast imaging speed and identification of multiple - and possibly unexpected- compounds remains challenging: existing high spectral resolution schemes require long measurement times to achieve broad spectral spans. Here we overcome this difficulty and introduce a novel concept of coherent anti-Stokes Raman scattering (CARS) spectro-imaging with two laser frequency combs. We illustrate the power of our technique with high resolution (4 cm-1) Raman spectra spanning more than 1200 cm-1 recorded within less than 15 microseconds. Furthermore, hyperspectral images combining high spectral (10 cm-1) and spatial (2 micrometers) resolutions are acquired at a rate of 50 pixels per second. Real-time multiplex accessing of hyperspectral images may dramatically expand the range of applications of nonlinear microscopy.Comment: 8 pages, 3 figure

Broadband near-ultraviolet dual comb spectroscopy

The highly energetic photons of ultraviolet light drive electronic and rovibronic transitions in all molecular species. This radiation is thus a prime tool for strongly selective spectroscopic fingerprinting and real-time environmental monitoring if broad spectral coverage, short acquisition times and high spectral resolution is achieved - requirements that are in mutual competition in traditional applications. As a novel approach with intrinsic potency in all three aspects, here we introduce ultraviolet dual comb spectroscopy using two broadband ultraviolet frequency combs centered at 871 THz and covering a spectral bandwidth of 35.7 THz. Within a 100 us acquisition time window, we obtain rotational state-resolved absorption spectra of formaldehyde, a prototype molecule with high relevance for laser spectroscopy and environmental sciences. This is the first realization of broadband dual comb spectroscopy in the ultraviolet spectral region and a pioneering tool to allow for real-time monitoring of rovibronic transitions.Comment: 17 pages, 10 figure

Ultraviolet dual comb spectroscopy: a roadmap

Dual Comb Spectroscopy proved its versatile capabilities in molecular fingerprinting in different spectral regions, but not yet in the ultraviolet (UV). Unlocking this spectral window would expand fingerprinting to the electronic energy structure of matter.This will access the prime triggers of photo-chemical reactions with unprecedented spectral resolution. In this research article, we discuss the milestones marking the way to the first UV dual comb spectrometer. We present experimental and simulated studies towards UV dual comb spectroscopy, directly applied to planned absorption measurements of formaldehyde (centered at 343 nm, 3.6 eV) and argon (80 nm, 16 eV). This will enable an unparalleled relative resolution of up to $10^{-9}$ - with a table-top UV source surpassing any synchrotron linked spectrometer by at least two and any grating-based UV spectrometer by up to six orders of magnitude

Cavity-enhanced dual-comb spectroscopy

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 µs. It could be implemented from the Terahertz to the ultraviolet regions without any need for detector arrays. We recorded, within 18 µs, spectra of the 1.0 µm 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