{"paper":{"title":"Chemical Interpretation of Time-Dependent Coupled-Cluster Theory","license":"http://creativecommons.org/licenses/by/4.0/","headline":"Time-dependent coupled-cluster theory gains chemical interpretation through expansion of its wavefunctions in a Slater-determinant basis to produce time-dependent configuration weights.","cross_cats":[],"primary_cat":"physics.chem-ph","authors_text":"Aparna Krishnan, Benjamin G. Peyton, H{\\aa}kon Emil Kristiansen, T. Daniel Crawford, Thomas Bondo Pedersen","submitted_at":"2026-05-17T12:11:09Z","abstract_excerpt":"While providing a highly accurate framework for simulating laser-induced many-electron dynamics in atom and molecules, including linear and nonlinear steady-state and transient absorption spectra, time-dependent coupled-cluster theory does not offer a straightforward interpretation in chemical terms. This should be contrasted with conventional time-independent equation-of-motion coupled-cluster or frequency-dependent response models where a simple eigenvector analysis readily reveals the dominant orbital-excitation character of individual excited states. We fill this gap by expanding the left "},"claims":{"count":4,"items":[{"kind":"strongest_claim","text":"At the time-dependent coupled-cluster singles-and-doubles level of theory, we demonstrate the power of the proposed methodology by assigning valence lines in the linear absorption spectra of four ten-electron molecules (HF, H2O, NH3, and CH4) with different point-group symmetries, validating the assignment by comparison with equation-of-motion coupled-cluster singles-and-doubles theory.","source":"verdict.strongest_claim","status":"machine_extracted","claim_id":"C1","attestation":"unclaimed"},{"kind":"weakest_assumption","text":"That expanding the left and right coupled-cluster functions in the Slater-determinant basis yields configuration weights whose time evolution meaningfully corresponds to the dominant orbital-excitation character of the dynamics, rather than being an artifact of the chosen reference or truncation.","source":"verdict.weakest_assumption","status":"machine_extracted","claim_id":"C2","attestation":"unclaimed"},{"kind":"one_line_summary","text":"Introduces time-dependent configuration weights via Slater-determinant expansion of TD-CC wavefunctions to interpret dynamics and assign linear absorption peaks, demonstrated on HF, H2O, NH3, CH4 at TD-CCSD level with EOM-CCSD validation.","source":"verdict.one_line_summary","status":"machine_extracted","claim_id":"C3","attestation":"unclaimed"},{"kind":"headline","text":"Time-dependent coupled-cluster theory gains chemical interpretation through expansion of its wavefunctions in a Slater-determinant basis to produce time-dependent configuration weights.","source":"verdict.pith_extraction.headline","status":"machine_extracted","claim_id":"C4","attestation":"unclaimed"}],"snapshot_sha256":"09337daf4b764e0c1131a7e871b620fde339aaac718501cadf4a23cdafdb1584"},"source":{"id":"2605.17409","kind":"arxiv","version":1},"verdict":{"id":"0218a3ed-7dc6-4a97-8b3a-dd8c9377f464","model_set":{"reader":"grok-4.3"},"created_at":"2026-05-19T22:46:08.444715Z","strongest_claim":"At the time-dependent coupled-cluster singles-and-doubles level of theory, we demonstrate the power of the proposed methodology by assigning valence lines in the linear absorption spectra of four ten-electron molecules (HF, H2O, NH3, and CH4) with different point-group symmetries, validating the assignment by comparison with equation-of-motion coupled-cluster singles-and-doubles theory.","one_line_summary":"Introduces time-dependent configuration weights via Slater-determinant expansion of TD-CC wavefunctions to interpret dynamics and assign linear absorption peaks, demonstrated on HF, H2O, NH3, CH4 at TD-CCSD level with EOM-CCSD validation.","pipeline_version":"pith-pipeline@v0.9.0","weakest_assumption":"That expanding the left and right coupled-cluster functions in the Slater-determinant basis yields configuration weights whose time evolution meaningfully corresponds to the dominant orbital-excitation character of the dynamics, rather than being an artifact of the chosen reference or truncation.","pith_extraction_headline":"Time-dependent coupled-cluster theory gains chemical interpretation through expansion of its wavefunctions in a Slater-determinant basis to produce time-dependent configuration weights."},"integrity":{"clean":true,"summary":{"advisory":0,"critical":0,"by_detector":{},"informational":0},"endpoint":"/pith/2605.17409/integrity.json","findings":[],"available":true,"detectors_run":[{"name":"doi_title_agreement","ran_at":"2026-05-19T23:01:19.627562Z","status":"completed","version":"1.0.0","findings_count":0},{"name":"doi_compliance","ran_at":"2026-05-19T22:52:12.626296Z","status":"completed","version":"1.0.0","findings_count":0},{"name":"claim_evidence","ran_at":"2026-05-19T21:41:57.747271Z","status":"completed","version":"1.0.0","findings_count":0},{"name":"ai_meta_artifact","ran_at":"2026-05-19T21:33:23.691392Z","status":"skipped","version":"1.0.0","findings_count":0}],"snapshot_sha256":"1807f38bd89433bda9b6af73d74ebcd92e4a3a19bae88ec5b107cec559f3fc14"},"references":{"count":56,"sample":[{"doi":"","year":1967,"title":"Electronic absorption spectra and geometry of organic molecules: An application of molecular orbital theory ; Academic Press: New York, 1967","work_id":"65772057-fae4-4129-b701-ed98b4f00cce","ref_index":1,"cited_arxiv_id":"","is_internal_anchor":false},{"doi":"","year":2013,"title":"Molecular Electronic-Structure Theory ; Wiley: Chichester, 2013","work_id":"b6341efa-0570-438f-a0f4-ce7d007626a6","ref_index":2,"cited_arxiv_id":"","is_internal_anchor":false},{"doi":"","year":2015,"title":"English, N. 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