Phase stable, shot-to-shot measurement of third- and fifth-order two-quantum correlation spectra using a pulse shaper in the pump-probe geometry

使用泵浦探测几何中的脉冲整形器对三阶和五阶双量子相关光谱进行相位稳定的逐次测量

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作者:Kieran M Farrell, Martin T Zanni

Abstract

We demonstrate the first phase stable measurement of a third-order 2Q spectrum using a pulse shaper in the pump-probe geometry. This measurement was achieved by permuting the time-ordering of the pump pulses, thus rearranging the signal pathways that are emitted in the probe direction. The third-order 2Q spectrum is self-heterodyned by the probe pulse. Using this method, one can interconvert between a 1Q experiment and a 2Q experiment by simply reprogramming a pulse shaper or delay stage. We also measure a fifth-order absorptive 2Q spectrum in the pump-probe geometry, which contains similar information as a third-order experiment but does not suffer from dispersive line shapes. To do so, we introduce methods to minimize saturation-induced artifacts of the pulse shaper, improving fifth-order signals. These techniques add new capabilities for 2D spectrometers that use pulse shapers in the pump-probe beam geometry.

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