Abstract
We describe methods using frequency combs and cavities for recording two-dimensional ultrafast spectroscopy signals with high sensitivity. By coupling multiple frequency combs to modes of an optical resonator, cavity-enhanced 2D spectroscopy signals are naturally generated.
Highlights
While physicists have demonstrated exquisite control over gas-phase molecular samples [1], the optical spectroscopy that is performed on these systems is usually much less sophisticated than their solution phase counterparts, due to limitations imposed by the very small optical densities of dilute gases
Most spectroscopy in molecular beams must employ socalled “action” methods, where absorption of a photon causes a detectable change in the system, such as dissociation, ionization, or fluorescence
In a recent article [5] we described the extension of ultrasensitive direct absorption techniques to femtosecond time-resolved experiments, reporting cavity-enhanced optical measurements in a dilute molecular beam that are simultaneously ultrasensitive and ultrafast
Summary
While physicists have demonstrated exquisite control over gas-phase molecular samples [1], the optical spectroscopy that is performed on these systems is usually much less sophisticated than their solution phase counterparts, due to limitations imposed by the very small optical densities of dilute gases. In a recent article [5] we described the extension of ultrasensitive direct absorption techniques to femtosecond time-resolved experiments, reporting cavity-enhanced optical measurements in a dilute molecular beam that are simultaneously ultrasensitive and ultrafast. In this contribution, we will describe how this technology can be applied to perform ultrasensitive 2D spectroscopy. Using higher-order cavity modes, one can naturally record cavity-enhanced 2D signals by mixing three resonantly-enhanced frequency combs with carrier-envelope offset frequencies (fCEO,, fCEO,, fCEO,3) to generate a fourth resonantly enhanced frequency comb with carrierenvelope offset frequency f(3) = ±( fCEO,1 − fCEO,2)+ fCEO,. Complete details can be found in [7]
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