{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T12:53:43Z","timestamp":1792068823219,"version":"4.4.0"},"reference-count":38,"publisher":"American Chemical Society (ACS)","issue":"41","license":[{"start":{"date-parts":[[2026,10,5]],"date-time":"2026-10-05T00:00:00Z","timestamp":1791158400000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"name":"German Research Council (DFG)","award":["EXC 2033  390677874  RESOLV"],"award-info":[{"award-number":["EXC 2033  390677874  RESOLV"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,10,15]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>The lowest-frequency Raman mode of water, observed through depolarized light scattering or optical Kerr effect techniques, is routinely used to track dynamic changes of interfacial water near ions or biomolecules. Despite this broad importance, its microscopic origin and relation to dielectric relaxation remains debated since decades\u2500with conflicting interpretations even for pure water. To resolve this controversy, we first accurately compute the Raman spectrum down to a few GHz based on ab initio simulations. Second, we introduce detailed decomposition analyses down to the dynamics of nuclei and electrons to reveal that the rotational and translational contributions are equally important. Third, strong negative orientational cross-correlations as well as internal field effects are found to modify the rotational component in very distinct ways. Overall, our analysis down to the electronic structure level provides an unexpectedly complex mechanistic scenario that fully resolves the long-standing debate concerning the lowest-frequency Raman mode of water and its relation to the dielectric spectrum.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02937","type":"journal-article","created":{"date-parts":[[2026,10,5]],"date-time":"2026-10-05T11:02:20Z","timestamp":1791198140000},"page":"11816-11821","source":"Crossref","is-referenced-by-count":0,"title":["Resolving the\nNature of the Lowest-Frequency Raman\nMode of Liquid Water"],"prefix":"10.1021","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9331-5172","authenticated-orcid":true,"given":"Florian","family":"Pabst","sequence":"first","affiliation":[{"name":"SISAA \u2212 Scuola Internazionale Superiore di Studi Avanzati , ,","place":["Trieste, Italy, 34136"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Harald","family":"Forbert","sequence":"additional","affiliation":[{"name":"Ruhr-Universita\u0308t Bochum , , ,","place":["Bochum, Germany, 44780"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dominik","family":"Marx","sequence":"additional","affiliation":[{"name":"Ruhr-Universita\u0308t Bochum , , ,","place":["Bochum, Germany, 44780"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,5]]},"reference":[{"key":"2026101508211294800_cit1","doi-asserted-by":"publisher","first-page":"278","DOI":"10.1038\/122278a0","article-title":"Molecular Spectra in\nthe Extreme Infra-Red","volume":"122","author":"Raman","year":"1928","journal-title":"Nature"},{"key":"2026101508211294800_cit2","doi-asserted-by":"publisher","first-page":"882","DOI":"10.1038\/122882b0","article-title":"Rotation of Molecules\nInduced by Light","volume":"122","author":"Raman","year":"1928","journal-title":"Nature"},{"key":"2026101508211294800_cit3","doi-asserted-by":"publisher","first-page":"303","DOI":"10.1103\/PhysRev.188.303","article-title":"Intermolecular Light Scattering in\nLiquids","volume":"188","author":"McTague","year":"1969","journal-title":"Phys. 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Lett."},{"key":"2026101508211294800_cit23","volume-title":"Dynamic Light Scattering\nwith Applications to Chemistry, Biology, and Physics (Courier Corporation","author":"Berne","year":"2000"},{"key":"2026101508211294800_cit24","doi-asserted-by":"publisher","first-page":"3973","DOI":"10.1063\/1.1774986","article-title":"Quantum Corrections\nto Classical Time-Correlation Functions: Hydrogen Bonding and Anharmonic\nFloppy Modes","volume":"121","author":"Ram\u0131rez","year":"2004","journal-title":"J. Chem. Phys."},{"key":"2026101508211294800_cit25","doi-asserted-by":"publisher","first-page":"1419","DOI":"10.1103\/RevModPhys.84.1419","article-title":"Maximally\nLocalized Wannier Functions: Theory and Applications","volume":"84","author":"Marzari","year":"2012","journal-title":"Rev. Mod. Phys."},{"key":"2026101508211294800_cit26","doi-asserted-by":"publisher","first-page":"4124","DOI":"10.1021\/ct4005307","article-title":"Raman Spectra of Liquid\nWater from Ab Initio Molecular Dynamics: Vibrational Signatures of\nCharge Fluctuations in the Hydrogen Bond Network","volume":"9","author":"Wan","year":"2013","journal-title":"J. Chem. Theory Comput.h"},{"key":"2026101508211294800_cit27","doi-asserted-by":"publisher","first-page":"345","DOI":"10.1002\/cphc.201800923","article-title":"Understanding\nLocal-Field Correction\nFactors in the Framework of the Onsager- Bo\u0308ttcher Model","volume":"20","author":"Aubret","year":"2019","journal-title":"ChemPhysChem"},{"key":"2026101508211294800_cit28","doi-asserted-by":"publisher","first-page":"244501","DOI":"10.1063\/5.0133511","article-title":"On the Intensity\nof Light Scattered by Molecular Liquids\n- Comparison of Experiment and Quantum Chemical Calculations","volume":"157","author":"Pabst","year":"2022","journal-title":"J. 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Phys."},{"key":"2026101508211294800_cit37","doi-asserted-by":"publisher","first-page":"12063","DOI":"10.1021\/ja202272k","article-title":"Extended Frequency\nRange Depolarized Light Scattering\nStudy of N-Acetyl-Leucine-Methylamide\u2013Water Solutions","volume":"133","author":"Perticaroli","year":"2011","journal-title":"J. Am. Chem. Soc."},{"key":"2026101508211294800_cit38","doi-asserted-by":"publisher","first-page":"142602","DOI":"10.1016\/j.cplett.2025.142602","article-title":"A Fresh Perspective on Water Dynamics\nin Aqueous Lithium Chloride Solutions","volume":"885","author":"Zei\u00dfler","year":"2026","journal-title":"Chem.\nPhys. 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