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Here, we apply Bayesian free-energy model selection to compare Gaussian models with different numbers of components for a coherent anti-Stokes Raman scattering (CARS)-derived spontaneous-Raman-equivalent Im[\u03c7(3)] spectrum. When applied to the amide I spectrum of a drug-treated binucleated human mammary epithelial cell (HMEC), the four-component model showed the lowest Bayesian free energy and the highest posterior model probability of 72.4% among the tested candidate models. In a separate dataset from an untreated mononucleated HMEC, Bayesian free energy exhibited internal minima at K = 3 for the amide I region and K = 6 for the CH stretching region, whereas RSS decreased monotonically with increasing model complexity in both cases. This workflow reduces user-dependent bias and improves the reproducibility of spectral decomposition in single-cell CARS analysis when the likelihood, prior ranges, candidate models, and preprocessing procedures are explicitly specified.<\/jats:p>","DOI":"10.1063\/5.0334971","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T10:40:10Z","timestamp":1790851210000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Bayesian free-energy model selection for amide I band decomposition in multiplex coherent anti-Stokes Raman scattering (CARS) microscopy"],"prefix":"10.1063","volume":"165","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-3613-9878","authenticated-orcid":false,"given":"Koki","family":"Ota","sequence":"first","affiliation":[{"name":"Graduate School of Science and Technology, Keio University 1 , 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kyosuke","family":"Tanaka","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Faculty of Science, Kyushu University 2 , 744, Motooka, Nishi-ku, Fukuoka 819-0395,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6153-2137","authenticated-orcid":false,"given":"Yuichi","family":"Yokoyama","sequence":"additional","affiliation":[{"name":"Japan Synchrotron Radiation Research Institute (JASRI) 3 , 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shigeo","family":"Ishibashi","sequence":"additional","affiliation":[{"name":"Department of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba 4 , 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6739-2948","authenticated-orcid":false,"given":"Akihito","family":"Inoko","sequence":"additional","affiliation":[{"name":"Department of Pathology, Aichi Medical University School of Medicine 5 , 1-1 Yazakokarimata, Nagakute, Aichi 480-1195,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7603-2194","authenticated-orcid":false,"given":"Ryo","family":"Suzuki","sequence":"additional","affiliation":[{"name":"Graduate School of Science and Technology, Keio University 1 , 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7625-6665","authenticated-orcid":false,"given":"Masaichiro","family":"Mizumaki","sequence":"additional","affiliation":[{"name":"Department of Physics, Faculty of Science, Kumamoto University 6 , 2-39-1 Kurokami, Chuo-ku, Kumamoto 860-8555,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3682-7627","authenticated-orcid":false,"given":"Hideaki","family":"Kano","sequence":"additional","affiliation":[{"name":"Graduate School of Science and Technology, Keio University 1 , 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,10,1]]},"reference":[{"issue":"6264","key":"2026100106400216800_c1","doi-asserted-by":"publisher","first-page":"aaa8870","DOI":"10.1126\/science.aaa8870","article-title":"Vibrational spectroscopic imaging of living systems: An emerging platform for biology and medicine","volume":"350","year":"2015","journal-title":"Science"},{"key":"2026100106400216800_c2","doi-asserted-by":"publisher","first-page":"77","DOI":"10.1146\/annurev-physchem-040412-110103","article-title":"Biomolecular imaging with coherent nonlinear vibrational microscopy","volume":"64","year":"2013","journal-title":"Annu. 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