Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction

The ultrafast spontaneous electron-density fluctuation dynamics in molecules is studied theoretically by off-resonant multiple X-ray diffraction events. The time- and wavevector-resolved photon-coincidence signals give an image of electron-density fluctuations expressed through the four-point correlation function of the charge density in momentum space. A Fourier transform of the signal provides a real-space image of the multipoint charge-density correlation functions, which reveal snapshots of the evolving electron density in between the diffraction events. The proposed technique is illustrated by ab initio simulations of the momentum- and real-space inelastic scattering signals from a linear cyanotetracetylene molecule.

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Publication Date:
NSF-PAR ID:
10082159
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
116
Issue:
2
Page Range or eLocation-ID:
p. 395-400
ISSN:
0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Charge density waves (CDWs) in the cuprate high-temperature superconductors have evoked much interest, yet their typical short-range nature has raised questions regarding the role of disorder. Here we report a resonant X-ray diffraction study of ZrTe$${}_{3}$$${}_{3}$, a model CDW system, with focus on the influence of disorder. Near the CDW transition temperature, we observe two independent signals that arise concomitantly, only to become clearly separated in momentum while developing very different correlation lengths in the well-ordered state that is reached at a distinctly lower temperature. Anomalously slow dynamics of mesoscopic charge domains are further found near the transition temperature, in spite of the expected strong thermal fluctuations. Our observations signify the presence of distinct experimental fingerprints of pristine and disorder-perturbed CDWs. We discuss the latter also in the context of Friedel oscillations, which we argue might promote CDW formation via a self-amplifying process.