Abstract
The optical response of the fluorescent molecule IR144 in solution is probed by pairs of collinear pulses with intensity just above the linear dependence using two different pulse shaping methods. The first approach mimics a Michelson interferometer, while the second approach, known as multiple independent comb shaping (MICS), eliminates spectral interference. The comparison of interfering and non-interfering pulses reveals that linear interference between the pulses leads to the loss of experimental information at early delay times. In both cases, the delay between the pulses is controlled with attosecond resolution and the sample fluorescence and stimulated emission are monitored simultaneously. An out-of-phase behavior is observed for fluorescence and stimulated emission, with the fluorescence signal having a minimum at zero time delay. Experimental findings are modeled using a two-level system with relaxation that closely matches the phase difference between fluorescence and stimulated emission and the relative intensities of the measured effects.
Highlights
The optical response of molecules in solution to a pulse of light has been the subject of numerous studies [1, 2] that have evolved with technology from the microsecond to the femtosecond timescale
When two collinear identical pulses, such as those generated by a Michelson interferometer, are scanned in time, they optically interfere, causing different amplitude modulation of the laser spectrum at different delay times
High-order phase distortions introduced by the optics in the laser system as well as by the setup are compensated by the multiphoton intrapulse interference phase scan (MIIPS) [4] software resulting in 35 fs transform limited (TL) pulses at the sample
Summary
The optical response of molecules in solution to a pulse of light has been the subject of numerous studies [1, 2] that have evolved with technology from the microsecond to the femtosecond timescale. The optical response of the fluorescent molecule IR144 in solution is probed by pairs of collinear pulses with intensity just above the linear dependence using two different pulse shaping methods. The comparison of interfering and non-interfering pulses reveals that experimental information can be lost at early delay times because of linear interference between the pulses.
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