Super-resolution stimulated X-ray Raman spectroscopy
(2025) In Nature 643(8072). p.662-668- Abstract
Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing1,2, self-induced transparency3 and stimulated X-ray Raman scattering (SXRS)4. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies5,6. However, experimental observations of SXRS to date4,7,8 have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited... (More)
Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing1,2, self-induced transparency3 and stimulated X-ray Raman scattering (SXRS)4. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies5,6. However, experimental observations of SXRS to date4,7,8 have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited joint energy–time resolution of 0.1 eV–40 fs. We used a new covariance analysis between statistically spiky broadband incident X-ray and scattered X-ray Raman pulses. Using 18,000 single shots, we beat not only the incident (about 8 eV) bandwidth but also the approximately 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy9. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and a broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. This stochastic SXRS approach represents a first step towards tracking elementary events that determine chemical outcomes10.
(Less)
- author
- organization
- publishing date
- 2025-07
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Nature
- volume
- 643
- issue
- 8072
- pages
- 7 pages
- publisher
- Nature Publishing Group
- external identifiers
-
- scopus:105010711106
- pmid:40670638
- ISSN
- 0028-0836
- DOI
- 10.1038/s41586-025-09214-5
- language
- English
- LU publication?
- yes
- id
- 21666031-1f22-488a-8927-cb7b51f9da65
- date added to LUP
- 2025-12-12 12:01:18
- date last changed
- 2025-12-13 03:00:09
@article{21666031-1f22-488a-8927-cb7b51f9da65,
abstract = {{<p>Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing<sup>1,2</sup>, self-induced transparency<sup>3</sup> and stimulated X-ray Raman scattering (SXRS)<sup>4</sup>. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies<sup>5,6</sup>. However, experimental observations of SXRS to date<sup>4,7,8</sup> have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited joint energy–time resolution of 0.1 eV–40 fs. We used a new covariance analysis between statistically spiky broadband incident X-ray and scattered X-ray Raman pulses. Using 18,000 single shots, we beat not only the incident (about 8 eV) bandwidth but also the approximately 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy<sup>9</sup>. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and a broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. This stochastic SXRS approach represents a first step towards tracking elementary events that determine chemical outcomes<sup>10</sup>.</p>}},
author = {{Li, Kai and Ott, Christian and Agåker, Marcus and Ho, Phay J. and Doumy, Gilles and Magunia, Alexander and Rebholz, Marc and Simon, Marc and Mazza, Tommaso and De Fanis, Alberto and Baumann, Thomas M. and Montano, Jacobo and Rennhack, Nils and Usenko, Sergey and Ovcharenko, Yevheniy and Chordiya, Kalyani and Cheng, Lan and Rubensson, Jan Erik and Meyer, Michael and Pfeifer, Thomas and Gaarde, Mette B. and Young, Linda}},
issn = {{0028-0836}},
language = {{eng}},
number = {{8072}},
pages = {{662--668}},
publisher = {{Nature Publishing Group}},
series = {{Nature}},
title = {{Super-resolution stimulated X-ray Raman spectroscopy}},
url = {{http://dx.doi.org/10.1038/s41586-025-09214-5}},
doi = {{10.1038/s41586-025-09214-5}},
volume = {{643}},
year = {{2025}},
}