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We present spatially enhanced electric-field-induced second-harmonic (SEEFISH) generation with a chirped femtosecond beam for measurements of electric field in mesoscale confined geometries subject to destructive spurious second-harmonic generation (SHG). Spurious SHG is shown to interfere with the measured E-FISH signal coherently, and thus simple background subtraction is not sufficient for single-beam E-FISH approaches, especially in a confined system with a large surface-to-volume ratio. The results show that a chirped femtosecond beam is effective in preventing higher-order mixing and white light generation in windows near the beam focal point which further contaminates the SEEFISH signal. The successful measurements of electric field of a nanosecond dielectric barrier discharge in a test cell demonstrated that spurious SHG detected with a congruent traditional E-FISH approach can be eliminated using the SEEFISH approach. 

We report the development of a simple and sensitive two-beam hybrid femtosecond/picosecond pure rotational coherent anti-Stokes Raman scattering (fs/ps CARS) method to simultaneously measure the rotational and vibrational temperatures of diatomic molecules. Rotation–vibration non-equilibrium plays a key role in the chemistry and thermalization in low-temperature plasmas as well as thermal loading of hypersonic vehicles. This approach uses time-domain interferences between ground state and vibrationally excited N₂molecules to intentionally induce coherence beating that leads to apparent non-Boltzmann distributions in the pure rotational spectra. These distortions enable simultaneous inference of both the rotational and vibrational temperatures. Coherence beating effects were observed in single-shot fs/ps CARS measurements of a 75 Torr N₂DC glow discharge and were successfully modeled for rotational and vibrational temperature extraction. We show that this method can be more sensitive than a pure rotational fs/ps CARS approach using a spectrally narrow probe pulse. Lastly, we experimentally measured the beat frequencies via Fourier transform of the time-domain response and obtained excellent agreement with the model.