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Angle-resolved coherent wave mixing using a 4  fs ultra-broad bandwidth laser.

I P Mercer, T Witting, T Driver

    Optics Letters
    |February 16, 2017
    PubMed
    Summary

    We achieved angle-resolved coherent wave mixing with 4 fs pulses, the shortest ever used in spectroscopy. This technique reveals energy transfer dynamics in photosynthetic complexes.

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    Area of Science:

    • Ultrafast spectroscopy
    • Quantum dynamics
    • Photosynthesis research

    Background:

    • Coherent multi-dimensional spectroscopy (CMD) probes molecular dynamics.
    • Few-cycle laser pulses enable high time resolution.
    • Understanding energy transfer in light-harvesting complexes is crucial.

    Purpose of the Study:

    • To demonstrate angle-resolved coherent (ARC) wave mixing with unprecedentedly short (4 fs) laser pulses.
    • To investigate energy transfer pathways and quantum superposition states in photosynthetic complexes.
    • To explore the potential of single-laser-pulse ARC mapping.

    Main Methods:

    • Utilizing a novel laser source producing 4 fs pulses (550-1000 nm bandwidth).
    • Applying the ARC technique to study the photosynthetic low light (LL) complex from Rhodopseudomonas palustris.

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  • Analyzing population dynamics and energy transfer across 5500 cm⁻¹ (0.65 eV).

    • Main Results:

    • Achieved the shortest pulse duration (4 fs) for coherent multi-dimensional spectroscopy.
    • Observed bi-exponential population dynamics for energy transfer within the LL complex.
    • Attributed energy transfer to bacteriochlorophyll Qx transitions to the B850 pigment.
    • Demonstrated the feasibility of single-laser-pulse ARC mapping for the first time.

    Conclusions:

    • The combination of few-cycle pulses and ARC spectroscopy opens new avenues for studying quantum phenomena.
    • ARC spectroscopy provides insights into ultrafast energy transfer mechanisms in biological systems.
    • Single-laser-pulse ARC mapping offers a simplified approach for spectroscopic measurements.