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Here we report the encapsulation of formaldehyde inside C<jats:sub>60<\/jats:sub> by molecular surgery, yielding the supermolecular complex CH<jats:sub>2<\/jats:sub>O@C<jats:sub>60<\/jats:sub>, despite the 4.4\u2009\u00c5 van der Waals length of CH<jats:sub>2<\/jats:sub>O exceeding the 3.7\u2009\u00c5 internal diameter of C<jats:sub>60<\/jats:sub>. The presence of CH<jats:sub>2<\/jats:sub>O significantly reduces the cage HOMO-LUMO gap. Nuclear spin-spin couplings are observed between the fullerene host and the formaldehyde guest. The rapid spin-lattice relaxation of the formaldehyde <jats:sup>13<\/jats:sup>C nuclei is attributed to a dominant spin-rotation mechanism. Despite being squeezed so tightly, the encapsulated formaldehyde molecules rotate freely about their long axes even at cryogenic temperatures, allowing observation of the ortho-to-para spin isomer conversion by infrared spectroscopy. The particle in a box nature of the system is demonstrated by the observation of two quantised translational modes in the cryogenic THz spectra.<\/jats:p>","DOI":"10.1038\/s41467-024-46886-5","type":"journal-article","created":{"date-parts":[[2024,3,21]],"date-time":"2024-03-21T09:01:37Z","timestamp":1711011697000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["Squeezing formaldehyde into C60 fullerene"],"prefix":"10.1038","volume":"15","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3603-722X","authenticated-orcid":false,"given":"Vijyesh K.","family":"Vyas","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"George R.","family":"Bacanu","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0767-8263","authenticated-orcid":false,"given":"Murari","family":"Soundararajan","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Elizabeth S.","family":"Marsden","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tanzeeha","family":"Jafari","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anna","family":"Shugai","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0585-0843","authenticated-orcid":false,"given":"Mark E.","family":"Light","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5827-9495","authenticated-orcid":false,"given":"Urmas","family":"Nagel","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6165-8290","authenticated-orcid":false,"given":"Toomas","family":"R\u00f5\u00f5m","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9878-1180","authenticated-orcid":false,"given":"Malcolm H.","family":"Levitt","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9891-5502","authenticated-orcid":false,"given":"Richard J.","family":"Whitby","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2024,3,21]]},"reference":[{"key":"46886_CR1","doi-asserted-by":"publisher","first-page":"162","DOI":"10.1038\/318162a0","volume":"318","author":"HW Kroto","year":"1985","unstructured":"Kroto, H. 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