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A Multimodal Wide-Field Fourier-Transform Raman Microscope
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Set-up for broadband Fourier-transform multidimensional electronic spectroscopy.

A Al Haddad, A Chauvet, J Ojeda

    Optics Letters
    |February 14, 2015
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    We developed a compact 2D Fourier transform setup using an argon-filled hollow core fiber laser. This system achieves sub-10-fs pulses and resolves ground-state vibrational coherences in Rhodamine 101.

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    Area of Science:

    • Ultrafast spectroscopy
    • Nonlinear optics
    • Physical chemistry

    Background:

    • 2D Fourier transform (2DFT) spectroscopy is a powerful technique for analyzing molecular dynamics.
    • Achieving stable, ultra-broadband light sources is crucial for high-resolution 2DFT measurements.
    • Characterizing ultrafast vibrational coherences provides insights into molecular structure and function.

    Purpose of the Study:

    • To develop a compact and passively phase-stabilized ultra-broadband 2D Fourier transform setup.
    • To generate sub-10-femtosecond pulses for high-resolution spectroscopic analysis.
    • To investigate the nonlinear optical response and vibrational dynamics of Rhodamine 101.

    Main Methods:

    • Utilized an amplified Ti:Al2O3 laser to pump an argon-filled hollow core fiber, generating an ultra-broadband light source (420-900 nm).
    • Employed a deformable mirror-based pulse shaper to achieve sub-10-femtosecond pulse durations.
    • Performed 2D Fourier transform spectroscopy on Rhodamine 101 to probe its nonlinear response.

    Main Results:

    • Successfully generated an ultra-broadband light source spanning 420-900 nm with sub-10-fs pulses.
    • Resolved vibrational coherences with a 150 fs period in the ground state of Rhodamine 101.
    • Demonstrated the capability of the compact setup for detailed molecular dynamics studies.

    Conclusions:

    • The developed compact 2D Fourier transform setup offers a stable and efficient platform for ultrafast spectroscopy.
    • The system enables high-resolution probing of molecular vibrational coherences.
    • This work advances the tools available for studying complex molecular systems.