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Spatial Phase Coherence in Femtosecond Coherent Raman Scattering

Hosseinnia, Ali LU orcid ; Marrocco, Michele LU ; Vergari, Francesco ; Raveesh, Meena LU ; Riewer, Sebastian ; Jena, Ashutosh ; Kushwaha, Abhishek ; Mazza, Francesco ; Linne, Mark LU and Bood, Joakim LU , et al. (2026) In Physical Review Letters 136(16).
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... (More)

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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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review Letters
volume
136
issue
16
article number
163801
publisher
American Physical Society
external identifiers
  • pmid:42113151
  • scopus:105036489820
ISSN
0031-9007
DOI
10.1103/r98z-7bwj
language
English
LU publication?
yes
id
fbf654db-3a59-4201-b740-3b9cdc3ae849
date added to LUP
2026-05-21 14:43:47
date last changed
2026-06-18 17:03:27
@article{fbf654db-3a59-4201-b740-3b9cdc3ae849,
  abstract     = {{<p>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.</p>}},
  author       = {{Hosseinnia, Ali and Marrocco, Michele and Vergari, Francesco and Raveesh, Meena and Riewer, Sebastian and Jena, Ashutosh and Kushwaha, Abhishek and Mazza, Francesco and Linne, Mark and Bood, Joakim and Boxx, Isaac}},
  issn         = {{0031-9007}},
  language     = {{eng}},
  number       = {{16}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review Letters}},
  title        = {{Spatial Phase Coherence in Femtosecond Coherent Raman Scattering}},
  url          = {{http://dx.doi.org/10.1103/r98z-7bwj}},
  doi          = {{10.1103/r98z-7bwj}},
  volume       = {{136}},
  year         = {{2026}},
}