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Exploring Time-Domain Femtosecond Rotational Coherent Raman Scattering for Diagnostics

Raveesh, Meena LU ; Hosseinnia, Ali LU orcid ; Padhiary, Abhijit ; Wei, Xiangyu ; Kornienko, Vassily LU ; Kristensson, Elias LU ; Ehn, Andreas LU ; Peterson, Brian ; Linne, Mark LU and Bood, Joakim LU (2025) In Journal of Raman Spectroscopy 56(8). p.666-672
Abstract

The diagnostic potential of femtosecond (fs) rotational coherent Raman scattering (RCRS) in the time domain is initially investigated. While RCRS concepts in the spectral domain obtain species selectivity and temperature sensitivity by resolving the spectral shape, mainly reflecting the Boltzmann-distributed, rotational populations of the Raman-active molecules present, the current time-domain fs-RCRS technique resolves the temporal shape of rotational revival signatures, which are influenced both by the population distributions and centrifugal distortion. Experiments in air and pure nitrogen are reported revealing temperature sensitivity in the recorded fs-RCRS temporal scans. A theoretical model can predict experimental data with good... (More)

The diagnostic potential of femtosecond (fs) rotational coherent Raman scattering (RCRS) in the time domain is initially investigated. While RCRS concepts in the spectral domain obtain species selectivity and temperature sensitivity by resolving the spectral shape, mainly reflecting the Boltzmann-distributed, rotational populations of the Raman-active molecules present, the current time-domain fs-RCRS technique resolves the temporal shape of rotational revival signatures, which are influenced both by the population distributions and centrifugal distortion. Experiments in air and pure nitrogen are reported revealing temperature sensitivity in the recorded fs-RCRS temporal scans. A theoretical model can predict experimental data with good agreement for temporal scans recorded in air at room temperature and pure nitrogen at 293, 400, and 580 K. Theoretical results show that a dual-probe configuration could provide temperature sensitivity that increases with increasing temperature, that is, directly opposite to the temperature dependence of the sensitivity in spectrally resolved RCRS, which is essentially flat beyond 1500 K. This result suggests that time-domain fs-RCRS could be a useful tool for single-shot thermometry in reactive flow environments, potentially providing improved sensitivity at high temperatures compared to spectral-domain RCRS techniques. Another major benefit with the time-domain fs-RCRS technique is that it only requires a single fs laser source.

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author
; ; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
rotational-CARS, temperature sensitivity, time-domain fs-RCRS, ultrafast diagnostics
in
Journal of Raman Spectroscopy
volume
56
issue
8
pages
7 pages
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:105000476423
ISSN
0377-0486
DOI
10.1002/jrs.6801
language
English
LU publication?
yes
id
96dc8453-a8f3-45b4-b4cc-22600867759f
date added to LUP
2025-09-11 11:42:41
date last changed
2025-10-14 09:07:45
@article{96dc8453-a8f3-45b4-b4cc-22600867759f,
  abstract     = {{<p>The diagnostic potential of femtosecond (fs) rotational coherent Raman scattering (RCRS) in the time domain is initially investigated. While RCRS concepts in the spectral domain obtain species selectivity and temperature sensitivity by resolving the spectral shape, mainly reflecting the Boltzmann-distributed, rotational populations of the Raman-active molecules present, the current time-domain fs-RCRS technique resolves the temporal shape of rotational revival signatures, which are influenced both by the population distributions and centrifugal distortion. Experiments in air and pure nitrogen are reported revealing temperature sensitivity in the recorded fs-RCRS temporal scans. A theoretical model can predict experimental data with good agreement for temporal scans recorded in air at room temperature and pure nitrogen at 293, 400, and 580 K. Theoretical results show that a dual-probe configuration could provide temperature sensitivity that increases with increasing temperature, that is, directly opposite to the temperature dependence of the sensitivity in spectrally resolved RCRS, which is essentially flat beyond 1500 K. This result suggests that time-domain fs-RCRS could be a useful tool for single-shot thermometry in reactive flow environments, potentially providing improved sensitivity at high temperatures compared to spectral-domain RCRS techniques. Another major benefit with the time-domain fs-RCRS technique is that it only requires a single fs laser source.</p>}},
  author       = {{Raveesh, Meena and Hosseinnia, Ali and Padhiary, Abhijit and Wei, Xiangyu and Kornienko, Vassily and Kristensson, Elias and Ehn, Andreas and Peterson, Brian and Linne, Mark and Bood, Joakim}},
  issn         = {{0377-0486}},
  keywords     = {{rotational-CARS; temperature sensitivity; time-domain fs-RCRS; ultrafast diagnostics}},
  language     = {{eng}},
  number       = {{8}},
  pages        = {{666--672}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Journal of Raman Spectroscopy}},
  title        = {{Exploring Time-Domain Femtosecond Rotational Coherent Raman Scattering for Diagnostics}},
  url          = {{http://dx.doi.org/10.1002/jrs.6801}},
  doi          = {{10.1002/jrs.6801}},
  volume       = {{56}},
  year         = {{2025}},
}