Search NASA⌕ Search
Home/Archive/DOE OSTI

DOE OSTI · 3023002

Imaging Three-Dimensional Molecular Structure and Dynamics with Multiparticle Covariance and Cumulant Coulomb Explosion Analysis

Cheng, Chuan [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)]·Kumagai, Yoshiaki [Nara Women’s University (Japan)]·Nagaya, Kiyonobu [Kyoto University (Japan)]·Gejo, Tatsuo [University of Hyogo (Japan)]·Harries, James [QST, Hyogo (Japan); Japan Synchrotron Radiation Research Institute, Hyogo (Japan)]·Burt, Michael [University of Oxford (United Kingdom); Trent University, ON (Canada)] (ORCID:0000000273178649)·Brouard, Mark [University of Oxford (United Kingdom)] (ORCID:0000000334210850)·Duley, Avijit [Kansas State University, Manhattan, KS (United States)]·Hockett, Paul [National Research Council of Canada, Ottawa, ON (Canada)]·McManus, Joseph W. [University of Oxford (United Kingdom)] (ORCID:0000000279112042)·Minns, Russell S. [University of Southampton (United Kingdom)] (ORCID:0000000167752977)·Mondal, Subhendu [Haldia Institute of Technology (India)] (ORCID:0000000309270421)·Owada, Shigeki [RIKEN SPring-8 Center, Hyogo (Japan)]·Razmus, Weronika [University of Southampton (United Kingdom)]·Rolles, Daniel [Kansas State University, Manhattan, KS (United States)] (ORCID:0000000239653477)·Sato, Takahiro [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)]·Thompson, Henry J. [University of Southampton (United Kingdom)] (ORCID:0009000727182229)·Venkatachalam, Anbu S. [Kansas State University, Manhattan, KS (United States)] (ORCID:0000000252066955)·Warne, Emily M. [University of Oxford (United Kingdom)] (ORCID:0000000212056939)·Walmsley, Tiffany [University of Oxford (United Kingdom)] (ORCID:0000000214465904)·Yagi, Mana [University of Hyogo (Japan)]·Bucksbaum, Philip [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)]·Allum, Felix [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000280448969)·Forbes, Ruaridh [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); University of California, Davis, CA (United States)] (ORCID:0000000320975991)
View original source ↗Read source document ↗Export metadata ↓

Abstract

Coulomb explosion imaging (CEI) provides a direct means of imaging molecular geometry by correlating fragment ion momenta following the fragmentation of a molecular polycation. Here, we demonstrate the use of three-body covariance and four-body cumulant analysis to extract three-dimensional (3D) structural information from the X-ray-induced Coulomb explosion of tert-butyl iodide (C4H9I). Site-selective ionization at the iodine 4d edge with intense femtosecond soft X-ray pulses from an X-ray free-electron laser (XFEL) enables rapid charge buildup and molecular breakup. By correlating ionic fragments in the molecular frame, we isolate complete dissociation channels and reveal subtle structural changes, such as umbrella-type motion of the branched alkyl chain, during the ionization process. Comparison with point-charge simulations of the Coulomb explosion shows close agreement, validating the approach. Furthermore, these results establish covariance/cumulant mapping as a powerful strategy for imaging complex three-dimensional molecular structures and point the way toward time-resolved CEI using both XFEL and tabletop sources for capturing ultrafast structural dynamics.

Explore related subjects

ImagingIonizationMolecular imagingX-rays

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

Cheng, Chuan [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Kumagai, Yoshiaki [Nara Women’s University (Japan)], Nagaya, Kiyonobu [Kyoto University (Japan)], Gejo, Tatsuo [University of Hyogo (Japan)], Harries, James [QST, Hyogo (Japan); Japan Synchrotron Radiation Research Institute, Hyogo (Japan)], Burt, Michael [University of Oxford (United Kingdom); Trent University, ON (Canada)] (ORCID:0000000273178649), Brouard, Mark [University of Oxford (United Kingdom)] (ORCID:0000000334210850), Duley, Avijit [Kansas State University, Manhattan, KS (United States)], Hockett, Paul [National Research Council of Canada, Ottawa, ON (Canada)], McManus, Joseph W. [University of Oxford (United Kingdom)] (ORCID:0000000279112042), Minns, Russell S. [University of Southampton (United Kingdom)] (ORCID:0000000167752977), Mondal, Subhendu [Haldia Institute of Technology (India)] (ORCID:0000000309270421), Owada, Shigeki [RIKEN SPring-8 Center, Hyogo (Japan)], Razmus, Weronika [University of Southampton (United Kingdom)], Rolles, Daniel [Kansas State University, Manhattan, KS (United States)] (ORCID:0000000239653477), Sato, Takahiro [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Thompson, Henry J. [University of Southampton (United Kingdom)] (ORCID:0009000727182229), Venkatachalam, Anbu S. [Kansas State University, Manhattan, KS (United States)] (ORCID:0000000252066955), Warne, Emily M. [University of Oxford (United Kingdom)] (ORCID:0000000212056939), Walmsley, Tiffany [University of Oxford (United Kingdom)] (ORCID:0000000214465904), Yagi, Mana [University of Hyogo (Japan)], Bucksbaum, Philip [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Allum, Felix [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000280448969), Forbes, Ruaridh [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); University of California, Davis, CA (United States)] (ORCID:0000000320975991). 2026-03-10. Imaging Three-Dimensional Molecular Structure and Dynamics with Multiparticle Covariance and Cumulant Coulomb Explosion Analysis. https://doi.org/10.1021/acs.jpclett.6c00162

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related reports

DOE OSTI2025

Electrically Reconfigurable Liquid Metal Nanophotonic Platform for Color Display and Imaging

Dynamically tunable optical materials and device architectures are essential for future photonic technologies, yet conventional solid metals lack the intrinsic tunability required for advanced functionalities. Gallium-based liquid metals (LMs) present an appealing alternative thanks to their distinctive mechanical and optical properties; however, their practical integration in tunable photonic elements remains largely unexplored. Here, in this study, an electrochemically controlled nanophotonic platform is demonstrated that integrates a dynamically reconfigurable LM ground plane with gold nanoantenna arrays within a microfluidic system, enabling precise and reversible modulation of optical resonances across the visible to mid-infrared spectral ranges. By employing moderate operational voltages (1.5–3.0 V), real-time tuning of high-resolution structural color patterns is achieved through nanoscale control of the interfacial gap between the LM and Au nanoantennas. This innovative platform facilitates electrically programmable, high-contrast color patterns suitable for dynamic optical displays, secure anti-counterfeiting labels, and imaging applications. Additionally, this platform enables tunable mid-infrared spectral responses, which may be utilized for chemical and biological sensing applications. This versatile integrated LM-based nanophotonic platform opens new paths toward multifunctional, actively tunable/reconfigurable photonic device and system technologies.

Imaging↗
DOE OSTI2023

Electron Microscopy Studies of Soft Nanomaterials

This review highlights recent efforts on applying electron microscopy (EM) to soft (including biological) nanomaterials. We will show how developments of both the hardware and software of EM have enabled new insights into the formation, assembly, and functioning (e.g., energy conversion and storage, phonon/photon modulation) of these materials by providing shape, size, phase, structural, and chemical information at the nanometer or higher spatial resolution. Specifically, we first discuss standard real-space two-dimensional imaging and analytical techniques which are offered conveniently by microscopes without special holders or advanced beam technology. The discussion is then extended to recent advancements, including visualizing three-dimensional morphology of soft nanomaterials using electron tomography and its variations, identifying local structure and strain by electron diffraction, and recording motions and transformation by in situ EM. On these advancements, we cover state-of-the-art technologies designed for overcoming the technical barriers for EM to characterize soft materials as well as representative application examples. Here, the even more recent integration of machine learning and its impacts on EM are also discussed in detail. With our perspectives of future opportunities offered at the end, we expect this review to inspire and stimulate more efforts in developing and utilizing EM-based characterization methods for soft nanomaterials at the atomic to nanometer length scales in academic research and industrial applications.

Imaging↗
NASA NTRS2019

Advanced Optical Techniques for Sensing and Imaging in Harsh Environments

Advances in aircraft propulsion technologies require new techniques for performance evaluation of aircraft components and subsystems as well as reliable in-flight control and health management. Those components and subsystems operate in harsh environments and for a proper operation these environments should be constantly monitored to obtain the designed performance of the engine. Optical techniques due to their immunity to electromagnetic radiation, chemical stability, and other unique features pose to meet the ever increasing requirements of the industry.The presentation will address applications of advanced optical techniques for both for sensing and imaging. In the process we will address fiber optics Bragg temperature sensors that were developed at NASA Glenn Research Center and tested at NASA Armstrong Flight Research Center as well as other advanced techniques for sensing and imaging in harsh environments. The presentation will also include discussion on various applications of presented techniques and proposed directions for future development.

Imaging↗