Double-modulation electro-optic sampling for pump-and-probe ultrafast correlation measurements

We describe a novel electro-optic double-modulation (DM) sampling technique for ultrafast transient spectroscopy, which is characterized by a superior signal-to-noise ratio compared to that of a regular single-modulation technique. DM is achieved by a combined effect of a radio-frequency modulation, which eliminates most of the low-frequency noise, and an audio-frequency modulation, which makes use of a high-performance, low-frequency lock-in amplifier. The DM sensitivity is comparable to that of the more sophisticated schemes involving electrical mixing and the $\mathrm{A–B}$ noise reduction method. We show that the DM technique offers superior performance in two-beam transient pump-and-probe correlation measurements compared to the regular single frequency modulation technique and is an ideal scheme for three-beam picosecond correlation measurements.