TY - JOUR U1 - Wissenschaftlicher Artikel A1 - Harouna-Mayer, Sani Y. A1 - Klemeyer, Lars A1 - Zito, Cecilia A. A1 - Bielecki, Johan A1 - Cheng, Xuemei A1 - Derelli, Davide A1 - Estillore, Armando D. A1 - Gröne, Tjark L. R. A1 - Haas, Lukas V. A1 - Letrun, Romain A1 - Kim, Chan A1 - Koliyadu, Jayanath C. P. A1 - Mall, Abhishek A1 - Mazumder, Parichita A1 - Melo, Diogo V. M. A1 - Round, Adam R. A1 - Samanta, Amit K. A1 - Sarma, Abhisakh A1 - Shen, Zhou A1 - Sun, Xiao A1 - Vagovic, Patrik A1 - Wollweber, Tamme A1 - Bean, Richard A1 - Küpper, Jochen A1 - Chapman, Henry N. A1 - Koziej, Dorota A1 - Ayyer, Kartik T1 - Single-Particle X‑ray Scattering Reveals a High Local Supersaturation of Precursors as the Origin of CoO Assembly Formation JF - The Journal of Physical Chemistry Letters N2 - Single-particle small-angle X-ray scattering (SP-SAXS) at X-ray free electron lasers (XFELs) enables quantitative analysis of morphological heterogeneity that is fundamentally inaccessible to ensemble-averaged in situ techniques. By recording diffraction snapshots from isolated particles, SP-SAXS resolves low-contrast, less abundant, or transient species within heterogeneous particle populations that would otherwise remain hidden to conventional X-ray techniques. We demonstrate this unique capability by investigating the solvothermal formation of CoO nanocrystal assemblies from a Co­(acac)3 precursor in benzyl alcohol. The single-particle data revealed amorphous, uniform-density Co­(acac)2 spheres as transient intermediates that directly crystallize into cavernous CoO nanocrystal assemblies, explaining why CoO forms as hierarchical aggregates rather than as isolated nanocrystals. These results establish SP-SAXS as a uniquely powerful framework for uncovering nonclassical nanoparticle formation pathways hidden in ensemble measurements. AB - Single-particle small-angle X-ray scattering (SP-SAXS) at X-ray free electron lasers (XFELs) enables quantitative analysis of morphological heterogeneity that is fundamentally inaccessible to ensemble-averaged in situ techniques. By recording diffraction snapshots from isolated particles, SP-SAXS resolves low-contrast, less abundant, or transient species within heterogeneous particle populations that would otherwise remain hidden to conventional X-ray techniques. We demonstrate this unique capability by investigating the solvothermal formation of CoO nanocrystal assemblies from a Co­(acac)3 precursor in benzyl alcohol. The single-particle data revealed amorphous, uniform-density Co­(acac)2 spheres as transient intermediates that directly crystallize into cavernous CoO nanocrystal assemblies, explaining why CoO forms as hierarchical aggregates rather than as isolated nanocrystals. These results establish SP-SAXS as a uniquely powerful framework for uncovering nonclassical nanoparticle formation pathways hidden in ensemble measurements. Y1 - 2026 SN - 1948-7185 SS - 1948-7185 UN - https://nbn-resolving.org/urn:nbn:de:hbz:kob7-26672 U6 - https://doi.org/10.1021/acs.jpclett.6c00191 DO - https://doi.org/10.1021/acs.jpclett.6c00191 VL - 17 IS - 23 SP - 6418 EP - 6424 S1 - 7 PB - American Chemical Society ER -