Broadband 2D electronic spectrometer using white light and pulse shaping: noise and signal evaluation at 1 and 100...

We have developed a broad bandwidth two-dimensional electronic spectrometer that operates shot-to-shot at repetition rates up to 100 kHz using an acousto-optic pulse shaper. It is called a two-dimensional white-light (2D-WL) spectrometer because the input is white-light supercontinuum. Methods for 100 kHz data collection are studied to understand how laser noise is incorporated into 2D spectra during measurement. At 100 kHz, shot-to-shot scanning of the delays and phases of the pulses in the pulse sequence produces a 2D spectrum 13-times faster and with the same signal-to-noise as using mechanical stages and a chopper. Comparing 100 to 1 kHz repetition rates, data acquisition time is decreased by a factor of 200, which is beyond the improvement expected by the repetition rates alone due to reduction in 1/f noise. These improvements arise because shot-to-shot readout and modulation of the pulse train at 100 kHz enables the electronic coherences to be measured faster than the decay in correlation between laser intensities. Using white light supercontinuum for the pump and probe pulses produces high signal-to-noise spectra on samples with optical densities <0.1 within a few minutes of averaging and an instrument response time of <46 fs thereby demonstrating that that simple broadband continuum sources, although weak, are sufficient to create high quality 2D spectra with >200 nm bandwidth.