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  1. Abstract We report on the development of a highly sensitive electric field induced second harmonic generation diagnostic setup capable of measuring electric field strengths as low as 1 V cm 1 at the picosecond time scale under atmospheric pressure conditions. This unprecedented sensitivity is achieved through passive homodyne detection, which utilizes stray signals generated by an optical component in the beam path. Our detection limit of 0.3–0.5 V cm 1 represents an improvement of over 2–3 orders of magnitude compared to previous reports (100–1000 V cm 1 ) in the literature. Additionally, we demonstrate sensitivity to the polarity of the electric field. Experimental results are corroborated by simulations of the 400 ps time-resolved homodyne process, offering deeper insights into the enhanced detection capabilities and the system’s ability to resolve the field sign. 
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  2. We report on the experimental observation of non-resonant, second-order optical sum-frequency generation (SFG) in five different atomic and molecular gases. The measured signal is attributed to a SFG process by characterizing its intensity scaling and its polarization behavior. We show that the electric quadrupole mechanism cannot explain the observed trends and suggest a mechanism based on symmetry breaking along the incident beam path arising from laser-induced species ground state number density gradients. Our results demonstrate that the SFG is about four orders of magnitude stronger than the third-harmonic generation (THG) and independent from any externally applied electric fields. These features make this method suitable for gas number density measurements at the picosecond time scale in reactive flows and plasmas. 
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