Bottom-up analysis of rovibrational helical dichroism Hrast, Mateja Koutentakis, Georgios Maslov, Mikhail ; https://orcid.org/0000-0003-4074-2570 Lemeshko, Mikhail ; https://orcid.org/0000-0002-6990-7802 ddc:530 We present a general theoretical framework for helical dichroism (HD), establishing an explicit link between chiral resolution and orbital angular momentum (OAM) exchange in light–matter interaction. Tracing microscopic mechanisms of the OAM transfer, we derive rotational selection rules, which establish that HD emerges only from the spin–orbit coupling of light, even for beams without the far-field OAM. Our findings refine the conditions for observing HD, provide a tool to re-examine the outcome of prior experiments, and guide future designs for chiral sensing with structured light. American Physical Society 2026 info:eu-repo/semantics/article doc-type:article text http://purl.org/coar/resource_type/c_2df8fbb1 https://research-explorer.ista.ac.at/record/21149 https://research-explorer.ista.ac.at/download/21149/21210 Hrast M, Koutentakis G, Maslov M, Lemeshko M. Bottom-up analysis of rovibrational helical dichroism. <i>Physical Review Letters</i>. 2026;136(5). doi:<a href="https://doi.org/10.1103/fkf1-1jml">10.1103/fkf1-1jml</a> eng info:eu-repo/semantics/altIdentifier/doi/10.1103/fkf1-1jml info:eu-repo/semantics/altIdentifier/issn/0031-9007 info:eu-repo/semantics/altIdentifier/e-issn/1079-7114 info:eu-repo/semantics/altIdentifier/arxiv/2505.16393 info:eu-repo/semantics/openAccess