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  • Open Access

Spatial Phase Coherence in Femtosecond Coherent Raman Scattering

Ali Hosseinnia1,2,*, Michele Marrocco3,†, Francesco Vergari3,4, Meena Raveesh5, Sebastian Riewer1, Ashutosh Jena1, Abhishek Kushwaha1, Francesco Mazza1, Mark Linne6 et al.

Joakim Bood5 and Isaac Boxx1

  • *Contact author: ali.hosseinnia@list.lu
  • †Contact author: michele.marrocco@enea.it
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Phys. Rev. Lett. 136, 163801 – Published 22 April, 2026

DOI: https://doi.org/10.1103/r98z-7bwj

Abstract

Conventional femtosecond coherent laser spectroscopy predominantly focuses on the temporal phase coherence through time- or frequency-resolved methods. In this Letter, we suggest an alternative experimental framework based on spatial phase coherence. The intrinsic spectral dispersion of wave vectors in femtosecond pulses and sample dimensions exceeding the laser wavelength creates a compelling basis to establish spatial phase coherence as a novel approach to femtosecond laser spectroscopy. Using rotational Raman coherence in air as a case study, we analyze the transverse spatial distribution of the third-order signal generated by the rotational wave packet. Our findings reveal apparent temporal shifts and distortions in time-resolved signals that arise in conventional measurements lacking sensitivity to spatial phase coherence. Moreover, we demonstrate that spatial phase coherence can serve as a useful tool for thermometric applications, showcasing its sensitivity to temperature variations. These discoveries open new avenues in femtosecond laser spectroscopy, including an alternative single-shot detection scheme, a new form of Raman coherence imaging, and molecular species quantification during overlapping fractional revivals.

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Phys. Rev. Lett. 136, 163801– Published 22 April, 2026
  • Received 7 February 2025
  • Revised 11 June 2025
  • Accepted 17 March 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

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