Imaging collective quantum fluctuations of the structure of a complex molecule

• 成果类型: Article
• 署名作者: Richard, Benoit; Boll, Rebecca; Banerjee, Sourav; Schaefer, Julia M.; Jurek, Zoltan; Kastirke, Gregor; Fehre, Kilian; Schoeffler, Markus S.; Anders, Nils; Baumann, Thomas M.; Eckart, Sebastian; Erk, Benjamin; De Fanis, Alberto; Doerner, Reinhard; Grundmann, Sven; Grychtol, Patrik; Hofmann, Max; Ilchen, Markus; Kircher, Max; Kubicek, Katharina; Kunitski, Maksim; Li, Xiang; Mazza, Tommaso; Meister, Severin; Melzer, Niklas; Montano, Jacobo; Music, Valerija; Ovcharenko, Yevheniy; Passow, Christopher; Pier, Andreas; Rennhack, Nils; Rist, Jonas; Rivas, Daniel E.; Rolles, Daniel; Schlichting, Ilme; Schmidt, Lothar Ph. H.; Schmidt, Philipp; Trabert, Daniel; Trinter, Florian; Wagner, Rene; Walter, Peter; Ziolkowski, Pawel; Rudenko, Artem; Meyer, Michael; Santra, Robin; Inhester, Ludger; Jahnke, Till
• 署名单位: Helmholtz Association; Deutsches Elektronen-Synchrotron (DESY); University of Hamburg; University of Hamburg; European XFEL; University of Hamburg; Goethe University Frankfurt; Helmholtz Association; GSI Helmholtz-Center for Heavy Ion Research; Helmholtz Association; Deutsches Elektronen-Synchrotron (DESY); Kansas State University; Stanford University; United States Department of Energy (DOE); SLAC National Accelerator Laboratory; Max Planck Society; Universitat Kassel; Universitat Kassel; Max Planck Society; Max Planck Society; Fritz Haber Institute of the Max Planck Society
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-9509
• DOI: 10.1126/science.adu2637
• 发表日期: 2025-08-07
• 页码: 650-654
• 关键词: basis-sets; DYNAMICS; motion; ion

摘要

Because of the Heisenberg uncertainty principle, the structure of a molecule fluctuates about its mean geometry, even in the ground state. Observing this fundamental quantum effect experimentally-particularly, revealing the collective nature of the structural quantum fluctuations-remains an unmet challenge for complex molecules. In this work, we achieved this for an 11-atom molecule by inducing its Coulomb explosion with an x-ray free-electron laser. We show that the structural fluctuations manifest themselves in correlated variations of ion momenta obtained through coincident detection of the atomic fragments from individual molecules. Our analysis scheme allows extracting these variations, despite our measurements covering only a fraction of the full 33-dimensional momentum space, thereby establishing a general approach for extracting information on high-dimensional structural dynamics using Coulomb explosion.