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    Arbitrary-Detuning ASynchronous OPtical Sampling (AD-ASOPS) enables multiscale pump-probe spectroscopy across picosecond to millisecond timescales. This straightforward method is accurate, validated against spectral interferometry.

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    Area of Science:

    • Spectroscopy
    • Ultrafast Dynamics
    • Optical Physics

    Background:

    • Pump-probe spectroscopy is crucial for studying ultrafast phenomena.
    • Existing methods often face limitations in timescale accessibility.
    • Independent free-running oscillators present challenges in precise time-delay control.

    Purpose of the Study:

    • To introduce and validate Arbitrary-Detuning ASynchronous OPtical Sampling (AD-ASOPS) for multiscale pump-probe spectroscopy.
    • To demonstrate the straightforward implementation of AD-ASOPS using pre-existing femtosecond amplifiers.
    • To assess the accuracy and reliability of the AD-ASOPS technique across a wide range of time delays.

    Main Methods:

    • Development and implementation of the Arbitrary-Detuning ASynchronous OPtical Sampling (AD-ASOPS) technique.
    • Utilizing pre-existing femtosecond amplifiers seeded by independent free-running oscillators.
    • Comparative analysis against spectral interferometry for delay accuracy validation.

    Main Results:

    • AD-ASOPS successfully enables pump-probe spectroscopy with time delays from picoseconds to milliseconds.
    • The method is easily implemented on existing femtosecond amplifier setups.
    • Accuracy was confirmed, with delay computation standard deviations ranging from 0.31 to 1.7 ps.

    Conclusions:

    • AD-ASOPS offers a versatile and accessible approach for multiscale spectroscopic investigations.
    • The technique overcomes limitations in timescale coverage for pump-probe experiments.
    • AD-ASOPS provides reliable and accurate time-delay measurements for diverse experimental conditions.