Unitary coupled-cluster theory for the electron propagator: electron attachment and physical properties via the intermediate state representation
A scheme for the calculation of electron-attachment (EA) processes within the framework of unitary coupled-cluster (UCC) theory is presented. Analogous to the description of electron-detachment, the intermediate state representation (ISR) approach is used for the formulation and its relation to the...
Gespeichert in:
| Hauptverfasser: | , , |
|---|---|
| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
30 Jun 2025
|
| In: |
Physical chemistry, chemical physics
Year: 2025, Jahrgang: 27, Heft: 31, Pages: 16418-16427 |
| ISSN: | 1463-9084 |
| DOI: | 10.1039/D5CP01274K |
| Online-Zugang: | Verlag, kostenfrei, Volltext: https://doi.org/10.1039/D5CP01274K Verlag, kostenfrei, Volltext: https://pubs.rsc.org/en/content/articlelanding/2025/cp/d5cp01274k 
|
| Verfasserangaben: | Manuel Hodecker, Andreas Dreuw and Adrian L. Dempwolff |
MARC
| LEADER | 00000naa a2200000 c 4500 | ||
|---|---|---|---|
| 001 | 1941400752 | ||
| 003 | DE-627 | ||
| 005 | 20251117121057.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 251117s2025 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1039/D5CP01274K |2 doi | |
| 035 | |a (DE-627)1941400752 | ||
| 035 | |a (DE-599)KXP1941400752 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rda | ||
| 041 | |a eng | ||
| 084 | |a 27 |2 sdnb | ||
| 100 | 1 | |a Hodecker, Manuel |e VerfasserIn |0 (DE-588)1147707448 |0 (DE-627)1006692193 |0 (DE-576)495971871 |4 aut | |
| 245 | 1 | 0 | |a Unitary coupled-cluster theory for the electron propagator |b electron attachment and physical properties via the intermediate state representation |c Manuel Hodecker, Andreas Dreuw and Adrian L. Dempwolff |
| 264 | 1 | |c 30 Jun 2025 | |
| 300 | |b Illustrationen | ||
| 300 | |a 10 | ||
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a Computermedien |b c |2 rdamedia | ||
| 338 | |a Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Zuerst veröffentlicht: 30. Juni 2025 | ||
| 500 | |a Gesehen am 17.11.2025 | ||
| 520 | |a A scheme for the calculation of electron-attachment (EA) processes within the framework of unitary coupled-cluster (UCC) theory is presented. Analogous to the description of electron-detachment, the intermediate state representation (ISR) approach is used for the formulation and its relation to the algebraic-diagrammatic construction scheme is pointed out. Due to the UCC ansatz, the resulting equations cannot be given by closed-form expressions, but need to be approximated. Explicit working equations for two computational schemes referred to as EA-UCC2 and EA-UCC3 are given, providing electron-attachment energies and spectroscopic amplitudes of electron-attached states dominated by one-particle excitations correct through second and third order in perturbation theory, respectively. In the derivation, an expansion of the UCC transformed Hamiltonian involving Bernoulli numbers as expansion coefficients is employed. In a benchmark against full configuration interaction (FCI) results including 50 states of 21 different species, both neutral and charged, closed- and open-shell, the novel methods are characterized by mean absolute errors of 0.15 eV (EA-UCC2) and 0.10 eV (EA-UCC3). Furthermore, an approach for the computation of physical properties of electron-attached as well as electron-detached states within the UCC framework is presented. It also builds upon the ISR approach, featuring an expectation value-like formulation similar to that of the equation-of-motion coupled-cluster (EOM-CC) method or the ISR approach of the algebraic-diagrammatic construction (ADC) method. Explicit expressions for the expectation value of a general one-particle operator correct through second order in perturbation theory are given and shown to be equivalent to those of the second-order ADC/ISR procedure. | ||
| 700 | 1 | |a Dreuw, Andreas |d 1972- |e VerfasserIn |0 (DE-588)1060214598 |0 (DE-627)799305626 |0 (DE-576)416304974 |4 aut | |
| 700 | 1 | |a Dempwolff, Adrian |e VerfasserIn |0 (DE-588)119179024X |0 (DE-627)1670258432 |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t Physical chemistry, chemical physics |d Cambridge : RSC Publ., 1999 |g 27(2025), 31, Seite 16418-16427 |h Online-Ressource |w (DE-627)270125175 |w (DE-600)1476244-4 |w (DE-576)080160328 |x 1463-9084 |7 nnas |a Unitary coupled-cluster theory for the electron propagator electron attachment and physical properties via the intermediate state representation |
| 773 | 1 | 8 | |g volume:27 |g year:2025 |g number:31 |g pages:16418-16427 |g extent:10 |a Unitary coupled-cluster theory for the electron propagator electron attachment and physical properties via the intermediate state representation |
| 856 | 4 | 0 | |u https://doi.org/10.1039/D5CP01274K |x Verlag |x Resolving-System |z kostenfrei |3 Volltext |
| 856 | 4 | 0 | |u https://pubs.rsc.org/en/content/articlelanding/2025/cp/d5cp01274k |x Verlag |z kostenfrei |3 Volltext |
| 951 | |a AR | ||
| 992 | |a 20251117 | ||
| 993 | |a Article | ||
| 994 | |a 2025 | ||
| 998 | |g 119179024X |a Dempwolff, Adrian |m 119179024X:Dempwolff, Adrian |d 700000 |d 708000 |e 700000PD119179024X |e 708000PD119179024X |k 0/700000/ |k 1/700000/708000/ |p 3 |y j | ||
| 998 | |g 1060214598 |a Dreuw, Andreas |m 1060214598:Dreuw, Andreas |d 700000 |d 708000 |e 700000PD1060214598 |e 708000PD1060214598 |k 0/700000/ |k 1/700000/708000/ |p 2 | ||
| 999 | |a KXP-PPN1941400752 |e 4807878778 | ||
| BIB | |a Y | ||
| SER | |a journal | ||
| JSO | |a {"origin":[{"dateIssuedDisp":"30 Jun 2025","dateIssuedKey":"2025"}],"relHost":[{"note":["Gesehen am 20.02.24"],"pubHistory":["1.1999 -"],"part":{"year":"2025","volume":"27","text":"27(2025), 31, Seite 16418-16427","issue":"31","pages":"16418-16427","extent":"10"},"language":["eng"],"titleAlt":[{"title":"PCCP"}],"disp":"Unitary coupled-cluster theory for the electron propagator electron attachment and physical properties via the intermediate state representationPhysical chemistry, chemical physics","type":{"media":"Online-Ressource","bibl":"periodical"},"corporate":[{"display":"Royal Society of Chemistry","role":"isb"}],"recId":"270125175","name":{"displayForm":["RSC, Royal Society of Chemistry"]},"origin":[{"publisherPlace":"Cambridge","dateIssuedKey":"1999","dateIssuedDisp":"1999-","publisher":"RSC Publ."}],"physDesc":[{"extent":"Online-Ressource"}],"id":{"zdb":["1476244-4"],"eki":["270125175"],"issn":["1463-9084"]},"title":[{"title":"Physical chemistry, chemical physics","subtitle":"PCCP ; a journal of European chemical societies","title_sort":"Physical chemistry, chemical physics"}]}],"physDesc":[{"noteIll":"Illustrationen","extent":"10 S."}],"id":{"doi":["10.1039/D5CP01274K"],"eki":["1941400752"]},"title":[{"title_sort":"Unitary coupled-cluster theory for the electron propagator","subtitle":"electron attachment and physical properties via the intermediate state representation","title":"Unitary coupled-cluster theory for the electron propagator"}],"type":{"bibl":"article-journal","media":"Online-Ressource"},"note":["Zuerst veröffentlicht: 30. Juni 2025","Gesehen am 17.11.2025"],"recId":"1941400752","person":[{"display":"Hodecker, Manuel","given":"Manuel","role":"aut","family":"Hodecker"},{"role":"aut","family":"Dreuw","display":"Dreuw, Andreas","given":"Andreas"},{"display":"Dempwolff, Adrian","given":"Adrian","role":"aut","family":"Dempwolff"}],"language":["eng"],"name":{"displayForm":["Manuel Hodecker, Andreas Dreuw and Adrian L. Dempwolff"]}} | ||
| SRT | |a HODECKERMAUNITARYCOU3020 | ||