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In paramagnetic solids, the bulk magnetic susceptibility (BMS) contributes a part to the measured nuclear magnetic resonance (NMR) shift tensor, which depends strongly on particle shape and packing. Here, we use a Fourier-space approach to quantify BMS shifts in LiFePO4 and use the 7Li magic-angle spinning NMR spectra to directly probe the crystallite shape and size. By disentangling internal and external BMS shift contributions from the crystallite of interest and its neighbors, we show that particle shape anisotropy leaves a clear signature in the NMR line shape. Combining BMS modeling with quantum-chemical local shift parameters yields excellent agreement with experimental spectra and enables the extraction of new morphological insights, highlighting solid-state NMR as a quantitative probe of crystallite morphology in paramagnetic materials.<\/jats:p>","DOI":"10.1063\/5.0332260","type":"journal-article","created":{"date-parts":[[2026,5,22]],"date-time":"2026-05-22T10:12:57Z","timestamp":1779444777000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":1,"title":["Crystallite shape and packing of paramagnetic microcrystalline powders from the measurement and calculation of bulk magnetic susceptibility shifts in solid-state NMR"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-7168-7851","authenticated-orcid":false,"given":"Gabriel","family":"Balavoine","sequence":"first","affiliation":[{"name":"Centre de RMN \u00e0 Tr\u00e8s Haut Champs (UMR 5082, CNRS\/UCBL\/ENS de Lyon) 1 , 5 Rue de la Doua, 69100 Villeurbanne,","place":["France"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5648-4612","authenticated-orcid":false,"given":"Jos\u00e9 P.","family":"Carvalho","sequence":"additional","affiliation":[{"name":"Interdisciplinary Nanoscience Center (iNANO) and Department of Chemistry, Aarhus University 2 , Gustav Wieds Vej 14, DK-8000 Aarhus C,","place":["Denmark"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5931-2231","authenticated-orcid":false,"given":"Jonas","family":"Koppe","sequence":"additional","affiliation":[{"name":"Centre de RMN \u00e0 Tr\u00e8s Haut Champs (UMR 5082, CNRS\/UCBL\/ENS de Lyon) 1 , 5 Rue de la Doua, 69100 Villeurbanne,","place":["France"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2542-8113","authenticated-orcid":false,"given":"Andrew J.","family":"Pell","sequence":"additional","affiliation":[{"name":"Centre de RMN \u00e0 Tr\u00e8s Haut Champs (UMR 5082, CNRS\/UCBL\/ENS de Lyon) 1 , 5 Rue de la Doua, 69100 Villeurbanne,","place":["France"]},{"name":"Institut Universitaire de France (IUF) 3 , Paris 75231,","place":["France"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,5,22]]},"reference":[{"key":"2026052206125121000_c1","doi-asserted-by":"publisher","first-page":"1245","DOI":"10.1016\/j.apsusc.2015.08.017","article-title":"Influence of crystallite size and surface morphology on electrochemical properties of annealed TiO2 nanotubes","volume":"355","year":"2015","journal-title":"Appl. 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