Linear field-resolved spectroscopy approaching ultimate detection sensitivity

Electric-field oscillations are now experimentally accessible in the THz-to-PHz frequency range. Their measurement delivers the most comprehensive information content attainable by optical spectroscopy - if performed with high sensitivity. Yet, the trade-off between bandwidth and efficiency associated with the nonlinear mixing necessary for field sampling has so far strongly restricted sensitivity in applications such as field-resolved spectroscopy of molecular vibrations. Here, we demonstrate electric-field sampling of octave-spanning mid-infrared waves in the 18-to-39 THz (600-to-1300 cm<sup>-1</sup>) spectral region, with amplitudes ranging from the MV/cm level down to a few mV/cm. We show that employing powerful 2-µm gate pulses is key to approaching the ultimate detection limit of capturing all photons in the temporal gate, as well as providing high linearity with respect to the detected mid-infrared field. This combination of detection sensitivity, dynamic range, and linearity enables the exploitation of the full potential of emerging high-power waveform-controlled infrared sources for (non-)linear spectroscopy of solids, liquids, and gases.

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Publication Details

Journal
Optics Express
Published
2024-11-29
DOI
https://doi.org/10.1364/oe.536543
Citations
3
Primary Topic
Spectroscopy Techniques in Biomedical and Chemical Research
Type
article
Field-Weighted Citation Impact
1.99
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article

Linear field-resolved spectroscopy approaching ultimate detection sensitivity

Ernst E. Fill, Jens Limpert, Kiran Sankar Maiti, T. Butler et al.
3 citations
Optics Express
Spectroscopy Techniques in Biomedical and Chemical Research
1.99
article

Linear field-resolved spectroscopy approaching ultimate detection sensitivity

Ernst E. Fill, Jens Limpert, Kiran Sankar Maiti, T. Butler, Daniel G. Bausch, Christina Höfer, Lukas Fürst, Martin Gebhardt, Ferenc Krausz, Tobias Heuermann, Nicholas Karpowicz, Marinus Huber, Maximilian Högner, Ioachim Pupeza, Christian Gaida, Zheng Wei
article en
3 citations

Abstract

Electric-field oscillations are now experimentally accessible in the THz-to-PHz frequency range. Their measurement delivers the most comprehensive information content attainable by optical spectroscopy - if performed with high sensitivity. Yet, the trade-off between bandwidth and efficiency associated with the nonlinear mixing necessary for field sampling has so far strongly restricted sensitivity in applications such as field-resolved spectroscopy of molecular vibrations. Here, we demonstrate electric-field sampling of octave-spanning mid-infrared waves in the 18-to-39 THz (600-to-1300 cm<sup>-1</sup>) spectral region, with amplitudes ranging from the MV/cm level down to a few mV/cm. We show that employing powerful 2-µm gate pulses is key to approaching the ultimate detection limit of capturing all photons in the temporal gate, as well as providing high linearity with respect to the detected mid-infrared field. This combination of detection sensitivity, dynamic range, and linearity enables the exploitation of the full potential of emerging high-power waveform-controlled infrared sources for (non-)linear spectroscopy of solids, liquids, and gases.

Optics ExpressVol. 33(1)
Helmholtz Institute Jena (DE), University of British Columbia (CA), Leibniz Institute of Photonic Technology (DE), Graz University of Technology (AT), Max Planck Institute of Quantum Optics (DE), International Center for Transitional Justice (US), Active Fiber Systems (Germany) (DE), GfK (Germany) (DE), Friedrich Schiller University Jena (DE), Ludwig-Maximilians-Universität München (DE)
Openalex Percentile: Top 11%
Spectroscopy Techniques in Biomedical and Chemical Research
1.99
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