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The method is applied to (R)-propylene oxide as a benchmark system, comparing infinite-dilution conditions with highly concentrated solutions in water and carbon tetrachloride. The calculated VCD spectra show very good agreement with experimental data and only weak concentration dependence. However, analysis of the excitonic eigenstates reveals the formation of transient, thermally populated excitonic clusters characterized by delocalized vibrational excitations and widely dispersed rotatory strengths. The equilibrium distribution and free-energy profile of these clusters are characterized, providing microscopic insights into excitonic effects in VCD spectra of soft condensed-phase systems.<\/jats:p>","DOI":"10.1063\/5.0326643","type":"journal-article","created":{"date-parts":[[2026,5,22]],"date-time":"2026-05-22T10:12:43Z","timestamp":1779444763000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Theoretical-computational modeling of the vibrational chirality of interacting chromophores: VCD signal and equilibrium properties of excitonic\n                    <i>clusters<\/i>"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9488-0536","authenticated-orcid":false,"given":"Andrea","family":"Amadei","sequence":"first","affiliation":[{"name":"Department of Chemical and Technological Sciences, University of Rome \u201cTor Vergata,\u201d 1 Via della Ricerca Scientifica, I-00185 Rome,","place":["Italy"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2959-0158","authenticated-orcid":false,"given":"Massimiliano","family":"Aschi","sequence":"additional","affiliation":[{"name":"Department of Physical and Chemical Sciences, University of L\u2019Aquila 2 , Via Vetoio (Coppito 1), L\u2019Aquila 67010,","place":["Italy"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,5,22]]},"reference":[{"key":"2026052206123816700_c1","doi-asserted-by":"publisher","first-page":"3381","DOI":"10.1021\/acs.chemrev.9b00636","article-title":"Structure of condensed phase peptides: Insights from vibrational circular dichroism and Raman optical activity techniques","volume":"120","year":"2020","journal-title":"Chem. 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