Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images
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arXiv
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| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Preprint |
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2025
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| author | Ulmer, Anatoli Ho, Phay J. Langbehn, Bruno Kuschel, Stephan Hecht, Linos Obaid, Razib Dold, Simon Driver, Taran Duris, Joseph Lin, Ming-Fu Cesar, David Franz, Paris Guo, Zhaoheng Hart, Philip A. Kamalov, Andrei Larsen, Kirk A. Li, Xiang Meyer, Michael Nakahara, Kazutaka Radloff, Robert G. Robles, River Rönnebeck, Lara Sudar, Nick Summers, Adam M. Young, Linda Walter, Peter Cryan, James Bostedt, Christoph Rupp, Daniela Marinelli, Agostino Gorkhover, Tais |
| author_facet | Ulmer, Anatoli Ho, Phay J. Langbehn, Bruno Kuschel, Stephan Hecht, Linos Obaid, Razib Dold, Simon Driver, Taran Duris, Joseph Lin, Ming-Fu Cesar, David Franz, Paris Guo, Zhaoheng Hart, Philip A. Kamalov, Andrei Larsen, Kirk A. Li, Xiang Meyer, Michael Nakahara, Kazutaka Radloff, Robert G. Robles, River Rönnebeck, Lara Sudar, Nick Summers, Adam M. Young, Linda Walter, Peter Cryan, James Bostedt, Christoph Rupp, Daniela Marinelli, Agostino Gorkhover, Tais |
| contents | The advent of isolated and intense sub-femtosecond X-ray pulses enables tracking of quantummechanical motion of electrons in molecules and solids. The combination of X-ray spectroscopy and diffraction imaging is a powerful approach to visualize non-equilibrium dynamics in systems beyond few atoms. However, extreme x-ray intensities introduce significant electronic damage, limiting material contrast and spatial resolution. Here we show that newly available intense subfemtosecond (sub-fs) x-ray FEL pulses can outrun most ionization cascades and partially reverse x-ray damage through stimulated x-ray emission in the vicinity of a resonance. In our experiment, we compared thousands of coherent x-ray diffraction patterns and simultaneously recorded ion spectra from individual Ne nanoparticles injected into the FEL focus. Our experimental results and theoretical modeling reveal that x-ray diffraction increases and the average charge state decreases in particles exposed to sub-fs pulses compared to those illuminated with 15-femtosecond pulses. Sub-fs exposures outrun most Auger decays and impact ionization processes, and enhance nonlinear effects such as stimulated emission, which cycle bound electrons between different states. These findings demonstrate that intense sub-fs x-ray FEL pulses are transformative for advancing high-resolution imaging and spectroscopy in chemical and material sciences, and open the possibilities of coherent control of the interaction between x-rays and complex specimen beyond few atoms. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2506_19394 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images Ulmer, Anatoli Ho, Phay J. Langbehn, Bruno Kuschel, Stephan Hecht, Linos Obaid, Razib Dold, Simon Driver, Taran Duris, Joseph Lin, Ming-Fu Cesar, David Franz, Paris Guo, Zhaoheng Hart, Philip A. Kamalov, Andrei Larsen, Kirk A. Li, Xiang Meyer, Michael Nakahara, Kazutaka Radloff, Robert G. Robles, River Rönnebeck, Lara Sudar, Nick Summers, Adam M. Young, Linda Walter, Peter Cryan, James Bostedt, Christoph Rupp, Daniela Marinelli, Agostino Gorkhover, Tais Optics The advent of isolated and intense sub-femtosecond X-ray pulses enables tracking of quantummechanical motion of electrons in molecules and solids. The combination of X-ray spectroscopy and diffraction imaging is a powerful approach to visualize non-equilibrium dynamics in systems beyond few atoms. However, extreme x-ray intensities introduce significant electronic damage, limiting material contrast and spatial resolution. Here we show that newly available intense subfemtosecond (sub-fs) x-ray FEL pulses can outrun most ionization cascades and partially reverse x-ray damage through stimulated x-ray emission in the vicinity of a resonance. In our experiment, we compared thousands of coherent x-ray diffraction patterns and simultaneously recorded ion spectra from individual Ne nanoparticles injected into the FEL focus. Our experimental results and theoretical modeling reveal that x-ray diffraction increases and the average charge state decreases in particles exposed to sub-fs pulses compared to those illuminated with 15-femtosecond pulses. Sub-fs exposures outrun most Auger decays and impact ionization processes, and enhance nonlinear effects such as stimulated emission, which cycle bound electrons between different states. These findings demonstrate that intense sub-fs x-ray FEL pulses are transformative for advancing high-resolution imaging and spectroscopy in chemical and material sciences, and open the possibilities of coherent control of the interaction between x-rays and complex specimen beyond few atoms. |
| title | Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images |
| topic | Optics |
| url | https://arxiv.org/abs/2506.19394 |