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Coherent correlation imaging for resolving fluctuating states of matter

Klose, Christopher; Büttner, Felix; Hu, Wen; Mazzoli, Claudio; Litzius, Kai; Battistelli, Riccardo; Zayko, Sergey; Lemesh, Ivan; Bartell, Jason M.; Huang, Mantao; Günther, Christian M.; Schneider, Michael; Barbour, Andi; Wilkins, Stuart B.; Beach, Geoffrey S. D.; Eisebitt, Stefan; Pfau, Bastian

Fluctuations and stochastic transitions are ubiquitous in nanometre-scale systems, especially in the presence of disorder. However, their direct observation has so far been impeded by a seemingly fundamental, signal-limited compromise between spatial and temporal resolution. Here we develop coherent correlation imaging (CCI) to overcome this dilemma. Our method begins by classifying recorded camera frames in Fourier space. Contrast and spatial resolution emerge by averaging selectively over same-state frames. Temporal resolution down to the acquisition time of a single frame arises independently from an exceptionally low misclassification rate, which we achieve by combining a correlation-based similarity metric1,2 with a modified, iterative hierarchical clustering algorithm3,4. We apply CCI to study previously inaccessible magnetic fluctuations in a highly degenerate magnetic stripe domain state with nanometre-scale resolution. We uncover an intricate network of transitions between more than 30 discrete states. Our spatiotemporal data enable us to reconstruct the pinning energy landscape and to thereby explain the dynamics observed on a microscopic level. CCI massively expands the potential of emerging high-coherence X-ray sources and paves the way for addressing large fundamental questions such as the contribution of pinning5,6,7,8 and topology9,10,11,12 in phase transitions and the role of spin and charge order fluctuations in high-temperature superconductivity13,14.
Published in: Nature, 10.1038/s41586-022-05537-9, Springer Nature