Ultrafast Science, Volume. 3, Issue 1, 0027(2023)

Rapid-Scan Nonlinear Time-Resolved Spectroscopy over Arbitrary Delay Intervals

Tobias Flöry1、*, Vinzenz Stummer1, Justinas Pupeikis2, Benjamin Willenberg2, Alexander Nussbaum-Lapping2, Edgar Kaksis1, Franco V. A. Camargo3, Martynas Barkauskas4, Christopher R. Phillips2, Ursula Keller2, Giulio Cerullo3,5, Audrius Pugžlys1,6, and Andrius Baltuška1,6
Author Affiliations
  • 1Photonics Institute, TU Wien, Vienna, Austria.
  • 2Department of Physics, ETH Zurich, Zurich, Switzerland.
  • 3Istituto di Fotonica e Nanotecnologie-CNR, Piazza Leonardo da Vinci 32, 20133 Milano, Italy.
  • 4Light Conversion Ltd., Vilnius, Lithuania.
  • 5Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano, Italy.
  • 6Center for Physical Sciences & Technology, Savanoriu  Ave. 231 LT-02300, Vilnius, Lithuania.
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    Femtosecond dual-comb lasers have revolutionized linear Fourier-domain spectroscopy by offering a rapid motion-free, precise, and accurate measurement mode with easy registration of the combs beat note in the radio frequency domain. Extensions of this technique already found application for nonlinear time-resolved spectroscopy within the energy limit available from sources operating at the full oscillator repetition rate. Here, we present a technique based on time filtering of femtosecond frequency combs by pulse gating in a laser amplifier. This gives the required boost to the pulse energy and provides the flexibility to engineer pairs of arbitrarily delayed wavelength-tunable pulses for pump–probe techniques. Using a dual-channel millijoule amplifier, we demonstrate programmable generation of both extremely short, fs, and extremely long (>ns) interpulse delays. A predetermined arbitrarily chosen interpulse delay can be directly realized in each successive amplifier shot, eliminating the massive waiting time required to alter the delay setting by means of an optomechanical line or an asynchronous scan of 2 free-running oscillators. We confirm the versatility of this delay generation method by measuring χ(2) cross-correlation and χ(3) multicomponent population recovery kinetics.

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    Tobias Flöry, Vinzenz Stummer, Justinas Pupeikis, Benjamin Willenberg, Alexander Nussbaum-Lapping, Edgar Kaksis, Franco V. A. Camargo, Martynas Barkauskas, Christopher R. Phillips, Ursula Keller, Giulio Cerullo, Audrius Pugžlys, Andrius Baltuška. Rapid-Scan Nonlinear Time-Resolved Spectroscopy over Arbitrary Delay Intervals[J]. Ultrafast Science, 2023, 3(1): 0027

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    Paper Information

    Category: Research Articles

    Received: Dec. 14, 2022

    Accepted: Mar. 29, 2023

    Published Online: Dec. 4, 2023

    The Author Email: Flöry Tobias (tobias.floery@tuwien.ac.at)

    DOI:10.34133/ultrafastscience.0027

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