35.
Sun, Yan; Ricci, G.; Monteverde, M.; Derkach, V.; Chanelière, T.; Aldridge, E.; Casanova, D.; Beljonne, D.; Anthony, J. E.; Chepelianskii, A. D.
Spin-Dependent Fluorescence Mediated by Antisymmetric Exchange in Triplet Exciton Pairs Journal Article
In: Phys. Rev. Lett., vol. 136, no. 21, 2026, ISSN: 1079-7114.
Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Sun2026,
title = {Spin-Dependent Fluorescence Mediated by Antisymmetric Exchange in Triplet Exciton Pairs},
author = {Yan Sun and G. Ricci and M. Monteverde and V. Derkach and T. Chanelière and E. Aldridge and D. Casanova and D. Beljonne and J. E. Anthony and A. D. Chepelianskii},
doi = {10.1103/7mt2-968k},
issn = {1079-7114},
year = {2026},
date = {2026-09-16},
journal = {Phys. Rev. Lett.},
volume = {136},
number = {21},
publisher = {American Physical Society (APS)},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
34.
Richards, Kieran D.; Wang, Wenzhao; Thielert, Philipp; Green, James D.; Hudson, John M.; Tonnelé, Claire; Casanova, David; Olivier, Yoann; Hele, Timothy J. H.; Richert, Sabine; Li, Feng; Evans, Emrys W.
Open- and Closed-ShellRoles of Sensitizer and Annihilatorin Pseudo-Single Component Mixtures for Upconversion Journal Article
In: vol. 148, no. 33, pp. 35375–35385, 2026, ISSN: 1520-5126.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Richards2026,
title = {Open- and Closed-ShellRoles of Sensitizer and Annihilatorin Pseudo-Single Component Mixtures for Upconversion},
author = {Kieran D. Richards and Wenzhao Wang and Philipp Thielert and James D. Green and John M. Hudson and Claire Tonnelé and David Casanova and Yoann Olivier and Timothy J. H. Hele and Sabine Richert and Feng Li and Emrys W. Evans},
doi = {10.1021/jacs.6c04090},
issn = {1520-5126},
year = {2026},
date = {2026-08-26},
urldate = {2026-08-26},
volume = {148},
number = {33},
pages = {35375--35385},
publisher = {American Chemical Society (ACS)},
abstract = {<jats:title>Abstract</jats:title>
<jats:p>Photochemical upconversion by annihilation of two triplet excitons to a higher-energy singlet state enables energy control of photons in optoelectronics and photonics. Upconversion initiated by a closed-shell sensitizer is limited by energy losses from singlet–triplet intersystem crossing. Here we explore open-shell organic radicals as sensitizers and their closed-shell hydrogenated analogues as annihilators in photon upconversion. The sensitizer combines optical transitions from a triphenylmethyl (TTM-1Cz) radical with energy-degenerate triplet states of an anthracene-based component (DPA) in one molecule (TTM-1Cz-DPA). The difference of one hydrogen atom in its closed-shell counterpart (HTTM-1Cz-DPA) switches the spin-optical properties to an annihilator that can mediate efficient upconversion. Red-to-blue photon upconversion by intermolecular energy transfer, from open-shell sensitizer to closed-shell annihilator, is demonstrated in solution with an apparent anti-Stokes shift higher than 0.9 eV and 7% quantum efficiency. We evaluate this mechanism against true ‘single component’ mixtures for upconversion and find that the presence of hydrogenated precursor with radicals is essential for high performance. Understanding the emergent spin-optical properties from paired open-shell and closed-shell systems enables new opportunities for energy management from the same molecular frame.</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:title>Abstract</jats:title>
<jats:p>Photochemical upconversion by annihilation of two triplet excitons to a higher-energy singlet state enables energy control of photons in optoelectronics and photonics. Upconversion initiated by a closed-shell sensitizer is limited by energy losses from singlet–triplet intersystem crossing. Here we explore open-shell organic radicals as sensitizers and their closed-shell hydrogenated analogues as annihilators in photon upconversion. The sensitizer combines optical transitions from a triphenylmethyl (TTM-1Cz) radical with energy-degenerate triplet states of an anthracene-based component (DPA) in one molecule (TTM-1Cz-DPA). The difference of one hydrogen atom in its closed-shell counterpart (HTTM-1Cz-DPA) switches the spin-optical properties to an annihilator that can mediate efficient upconversion. Red-to-blue photon upconversion by intermolecular energy transfer, from open-shell sensitizer to closed-shell annihilator, is demonstrated in solution with an apparent anti-Stokes shift higher than 0.9 eV and 7% quantum efficiency. We evaluate this mechanism against true ‘single component’ mixtures for upconversion and find that the presence of hydrogenated precursor with radicals is essential for high performance. Understanding the emergent spin-optical properties from paired open-shell and closed-shell systems enables new opportunities for energy management from the same molecular frame.</jats:p>
<jats:p>Photochemical upconversion by annihilation of two triplet excitons to a higher-energy singlet state enables energy control of photons in optoelectronics and photonics. Upconversion initiated by a closed-shell sensitizer is limited by energy losses from singlet–triplet intersystem crossing. Here we explore open-shell organic radicals as sensitizers and their closed-shell hydrogenated analogues as annihilators in photon upconversion. The sensitizer combines optical transitions from a triphenylmethyl (TTM-1Cz) radical with energy-degenerate triplet states of an anthracene-based component (DPA) in one molecule (TTM-1Cz-DPA). The difference of one hydrogen atom in its closed-shell counterpart (HTTM-1Cz-DPA) switches the spin-optical properties to an annihilator that can mediate efficient upconversion. Red-to-blue photon upconversion by intermolecular energy transfer, from open-shell sensitizer to closed-shell annihilator, is demonstrated in solution with an apparent anti-Stokes shift higher than 0.9 eV and 7% quantum efficiency. We evaluate this mechanism against true ‘single component’ mixtures for upconversion and find that the presence of hydrogenated precursor with radicals is essential for high performance. Understanding the emergent spin-optical properties from paired open-shell and closed-shell systems enables new opportunities for energy management from the same molecular frame.</jats:p>
33.
Noguchi, Hikaru; Climent, Clàudia; Tong, Ka-Ming; Yuan, Jennifer; Walsby, Charles J.; Casanova, David; Wolf, Michael O.
Elucidatingthe Mechanism of Photoinduced Sulfur MonoxideExtrusion from Dianthryl Sulfoxide Journal Article
In: Journal Of The American Chemical Society, vol. 148, no. 32, pp. 34678–34686, 2026, ISSN: 1520-5126.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Noguchi2026,
title = {Elucidatingthe Mechanism of Photoinduced Sulfur MonoxideExtrusion from Dianthryl Sulfoxide},
author = {Hikaru Noguchi and Clàudia Climent and Ka-Ming Tong and Jennifer Yuan and Charles J. Walsby and David Casanova and Michael O. Wolf},
doi = {10.1021/jacs.6c09333},
issn = {1520-5126},
year = {2026},
date = {2026-08-19},
urldate = {2026-08-19},
journal = {Journal Of The American Chemical Society},
volume = {148},
number = {32},
pages = {34678--34686},
publisher = {American Chemical Society (ACS)},
abstract = {<jats:title>Abstract</jats:title>
<jats:p>Light-induced bond cleavage reactions are powerful tools for constructing complex molecular structures under mild conditions. Among these, extrusion processes enable skeletal reorganization through the elimination of small fragments, granting access to otherwise synthetically challenging frameworks. Photoextrusion that results in the formation of carbon–carbon bonds is particularly intriguing due to the possibility of broad applicability in synthetic chemistry. 9,9′-Dianthrylsulfoxide (9-AnSO) undergoes photoinduced sulfur monoxide (SO) extrusion, resulting in C–C bond formation between the two anthracene groups. This transformation could proceed via a concerted SO elimination or stepwise radical pathway, however the excited-state dynamics remain unclear. SO-trapping and spin-trapping experiments on 9-AnSO, supported by EPR and mass spectrometry, confirm the formation of sulfinyl radicals and rule out pathways involving sulfur extrusion as S or SO2. Triplet sensitization experiments and DFT calculations support a triplet-mediated pathway, consistent with the reduced reactivity observed in the presence of oxygen. In contrast, 1,1′- and 2,2′-bridged isomers show no photochemical reactivity, demonstrating strong positional dependence of the C–S homolysis reaction. These findings provide direct evidence for a stepwise radical mechanism for SO extrusion, establish the structural features controlling photochemical C–S bond cleavage in dianthryl sulfoxides, and offer design principles for new light-responsive molecules.</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:title>Abstract</jats:title>
<jats:p>Light-induced bond cleavage reactions are powerful tools for constructing complex molecular structures under mild conditions. Among these, extrusion processes enable skeletal reorganization through the elimination of small fragments, granting access to otherwise synthetically challenging frameworks. Photoextrusion that results in the formation of carbon–carbon bonds is particularly intriguing due to the possibility of broad applicability in synthetic chemistry. 9,9′-Dianthrylsulfoxide (9-AnSO) undergoes photoinduced sulfur monoxide (SO) extrusion, resulting in C–C bond formation between the two anthracene groups. This transformation could proceed via a concerted SO elimination or stepwise radical pathway, however the excited-state dynamics remain unclear. SO-trapping and spin-trapping experiments on 9-AnSO, supported by EPR and mass spectrometry, confirm the formation of sulfinyl radicals and rule out pathways involving sulfur extrusion as S or SO2. Triplet sensitization experiments and DFT calculations support a triplet-mediated pathway, consistent with the reduced reactivity observed in the presence of oxygen. In contrast, 1,1′- and 2,2′-bridged isomers show no photochemical reactivity, demonstrating strong positional dependence of the C–S homolysis reaction. These findings provide direct evidence for a stepwise radical mechanism for SO extrusion, establish the structural features controlling photochemical C–S bond cleavage in dianthryl sulfoxides, and offer design principles for new light-responsive molecules.</jats:p>
<jats:p>Light-induced bond cleavage reactions are powerful tools for constructing complex molecular structures under mild conditions. Among these, extrusion processes enable skeletal reorganization through the elimination of small fragments, granting access to otherwise synthetically challenging frameworks. Photoextrusion that results in the formation of carbon–carbon bonds is particularly intriguing due to the possibility of broad applicability in synthetic chemistry. 9,9′-Dianthrylsulfoxide (9-AnSO) undergoes photoinduced sulfur monoxide (SO) extrusion, resulting in C–C bond formation between the two anthracene groups. This transformation could proceed via a concerted SO elimination or stepwise radical pathway, however the excited-state dynamics remain unclear. SO-trapping and spin-trapping experiments on 9-AnSO, supported by EPR and mass spectrometry, confirm the formation of sulfinyl radicals and rule out pathways involving sulfur extrusion as S or SO2. Triplet sensitization experiments and DFT calculations support a triplet-mediated pathway, consistent with the reduced reactivity observed in the presence of oxygen. In contrast, 1,1′- and 2,2′-bridged isomers show no photochemical reactivity, demonstrating strong positional dependence of the C–S homolysis reaction. These findings provide direct evidence for a stepwise radical mechanism for SO extrusion, establish the structural features controlling photochemical C–S bond cleavage in dianthryl sulfoxides, and offer design principles for new light-responsive molecules.</jats:p>
32.
Cioslowski, Jerzy; Dominguez, Javier; Matito, Eduard
In: Journal of Chemical Theory and Computation, vol. 22, no. 15, pp. 7609–7623, 2026, ISSN: 1549-9626.
Abstract | Links | BibTeX | Tags: IT2067, QCD-KT
@article{Cioslowski2026,
title = {Refractory to Improvement: A Cautionary Tale of Two-ElectronDensities Computed with One-Electron Basis Sets and of Their Employmentin Quantum-Chemical Formalisms},
author = {Jerzy Cioslowski and Javier Dominguez and Eduard Matito},
doi = {10.1021/acs.jctc.6c00413},
issn = {1549-9626},
year = {2026},
date = {2026-08-11},
urldate = {2026-08-11},
journal = {Journal of Chemical Theory and Computation},
volume = {22},
number = {15},
pages = {7609--7623},
publisher = {American Chemical Society (ACS)},
abstract = {<jats:title>Abstract</jats:title>
<jats:p>A report on detailed investigations of the properties of the approximate on-top two-electron densities Φ(r⃗) computed with one-electron basis functions is presented. The key findings of these investigations, which also concern the reduced variant of Φ(r⃗), i.e.,ϕ(r→)=4Φ(r→)[ρ1(r→)]2 [where ρ1(r⃗) is the one-electron density], are as follows: 1) Φ(r⃗) converge extremely slowly to the complete basis set (CBS) limits, their errors asymptotically scaling ∼N−1/3 with the number N of basis functions (as contrasted with the ∼N−1 error scaling of the electronic energy); 2) this slow convergence results in gross inaccuracies of the approximate Φ(r⃗) computed with standard basis sets; 3) the errors in these Φ(r⃗) are, in general, refractory to reduction with standard convergence acceleration techniques such as the CBS-limit extrapolation; 4) it is essential to make a distinction between the physically meaningful genuine Φ(r⃗) (such as those produced by highly accurate calculations) and the contrived ones (such as those appearing in some variants of the Kohn–Sham formalism and in overly simplistic models) that are merely auxiliary quantities to which no physical meaning should be attached; 5) due to the presence of spurious features in the contrived Φ(r⃗), their employment in the analysis of electronic structure leads to false and misleading conclusions on chemical bonding and electron correlation; and 6) the MC-PDFT formalism suffers from a hidden “double-counting” problem, whose presence is masked for sufficiently small active spaces by its use of the contrived Φ(r⃗).</jats:p>},
keywords = {IT2067, QCD-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:title>Abstract</jats:title>
<jats:p>A report on detailed investigations of the properties of the approximate on-top two-electron densities Φ(r⃗) computed with one-electron basis functions is presented. The key findings of these investigations, which also concern the reduced variant of Φ(r⃗), i.e.,ϕ(r→)=4Φ(r→)[ρ1(r→)]2 [where ρ1(r⃗) is the one-electron density], are as follows: 1) Φ(r⃗) converge extremely slowly to the complete basis set (CBS) limits, their errors asymptotically scaling ∼N−1/3 with the number N of basis functions (as contrasted with the ∼N−1 error scaling of the electronic energy); 2) this slow convergence results in gross inaccuracies of the approximate Φ(r⃗) computed with standard basis sets; 3) the errors in these Φ(r⃗) are, in general, refractory to reduction with standard convergence acceleration techniques such as the CBS-limit extrapolation; 4) it is essential to make a distinction between the physically meaningful genuine Φ(r⃗) (such as those produced by highly accurate calculations) and the contrived ones (such as those appearing in some variants of the Kohn–Sham formalism and in overly simplistic models) that are merely auxiliary quantities to which no physical meaning should be attached; 5) due to the presence of spurious features in the contrived Φ(r⃗), their employment in the analysis of electronic structure leads to false and misleading conclusions on chemical bonding and electron correlation; and 6) the MC-PDFT formalism suffers from a hidden “double-counting” problem, whose presence is masked for sufficiently small active spaces by its use of the contrived Φ(r⃗).</jats:p>
<jats:p>A report on detailed investigations of the properties of the approximate on-top two-electron densities Φ(r⃗) computed with one-electron basis functions is presented. The key findings of these investigations, which also concern the reduced variant of Φ(r⃗), i.e.,ϕ(r→)=4Φ(r→)[ρ1(r→)]2 [where ρ1(r⃗) is the one-electron density], are as follows: 1) Φ(r⃗) converge extremely slowly to the complete basis set (CBS) limits, their errors asymptotically scaling ∼N−1/3 with the number N of basis functions (as contrasted with the ∼N−1 error scaling of the electronic energy); 2) this slow convergence results in gross inaccuracies of the approximate Φ(r⃗) computed with standard basis sets; 3) the errors in these Φ(r⃗) are, in general, refractory to reduction with standard convergence acceleration techniques such as the CBS-limit extrapolation; 4) it is essential to make a distinction between the physically meaningful genuine Φ(r⃗) (such as those produced by highly accurate calculations) and the contrived ones (such as those appearing in some variants of the Kohn–Sham formalism and in overly simplistic models) that are merely auxiliary quantities to which no physical meaning should be attached; 5) due to the presence of spurious features in the contrived Φ(r⃗), their employment in the analysis of electronic structure leads to false and misleading conclusions on chemical bonding and electron correlation; and 6) the MC-PDFT formalism suffers from a hidden “double-counting” problem, whose presence is masked for sufficiently small active spaces by its use of the contrived Φ(r⃗).</jats:p>
31.
Chuiko, Valerii; Ayers, Paul W.; Matito, Eduard
Toward more accurate natural orbital functional approximations: Including 4-index cumulant contributions Journal Article
In: The Journal of Chemical Physics, vol. 165, no. 5, 2026, ISSN: 1089-7690.
Abstract | Links | BibTeX | Tags: IT2067, QCD-KT
@article{Chuiko2026,
title = {Toward more accurate natural orbital functional approximations: Including 4-index cumulant contributions},
author = {Valerii Chuiko and Paul W. Ayers and Eduard Matito},
doi = {10.1063/5.0326054},
issn = {1089-7690},
year = {2026},
date = {2026-08-07},
urldate = {2026-08-07},
journal = {The Journal of Chemical Physics},
volume = {165},
number = {5},
publisher = {AIP Publishing},
abstract = {<jats:p>Accurate modeling of bond breaking remains a central challenge for reduced density matrix functional theory (RDMFT). Although some modern functionals can yield reasonably accurate dissociation energies, they often fail to reproduce key properties of the dissociated fragments, such as a vanishing fragment population covariance (also known as the delocalization index) and the correct total spin angular momentum of each fragment (local spin). In this study, we revisit the construction of natural orbital functionals by correcting the cumulant contribution produced by the PNOF5 functional. Our method enforces known contributions of the cumulant to local spin fragments and the delocalization index at the dissociation limit. We obtain the closest cumulant consistent with these physically motivated constraints and subsequently purify the corresponding one- and two-electron reduced density matrices by imposing the standard P, Q, and GN-representability conditions. The resulting functional yields improved behavior in strongly correlated regimes. Benchmarking on the dissociation of the singlet states of N2, NO+, O2, S2, and CO shows that, in the dissociation regime, the energies computed from the updated cumulant exactly reproduce the complete active space self-consistent field energies. We further analyze the limitations of the approach and identify scenarios in which the current approach performs poorly. This study provides a pathway for systematically improving natural orbital functionals to achieve reliable bond-breaking calculations within RDMFT.</jats:p>},
keywords = {IT2067, QCD-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>Accurate modeling of bond breaking remains a central challenge for reduced density matrix functional theory (RDMFT). Although some modern functionals can yield reasonably accurate dissociation energies, they often fail to reproduce key properties of the dissociated fragments, such as a vanishing fragment population covariance (also known as the delocalization index) and the correct total spin angular momentum of each fragment (local spin). In this study, we revisit the construction of natural orbital functionals by correcting the cumulant contribution produced by the PNOF5 functional. Our method enforces known contributions of the cumulant to local spin fragments and the delocalization index at the dissociation limit. We obtain the closest cumulant consistent with these physically motivated constraints and subsequently purify the corresponding one- and two-electron reduced density matrices by imposing the standard P, Q, and GN-representability conditions. The resulting functional yields improved behavior in strongly correlated regimes. Benchmarking on the dissociation of the singlet states of N2, NO+, O2, S2, and CO shows that, in the dissociation regime, the energies computed from the updated cumulant exactly reproduce the complete active space self-consistent field energies. We further analyze the limitations of the approach and identify scenarios in which the current approach performs poorly. This study provides a pathway for systematically improving natural orbital functionals to achieve reliable bond-breaking calculations within RDMFT.</jats:p>
30.
Irigoyen, Mikel; Marchand, Alice; de Pariza, Xabier Lopez; Melchin, Timo; Barquero, Aitor; Matxain, Jon M.; Sardón, Haritz; Leiza, Jose R.; Ruipérez, Fernando
In: Macromolecules, vol. 59, no. 14, pp. 8509–8521, 2026, ISSN: 1520-5835.
Abstract | Links | BibTeX | Tags: IT2067, POL-KT
@article{Irigoyen2026,
title = {Quantum-Chemical Study for Understanding the Low Incorporationof 2-Methylen-1,3-Dioxepane (MDO) in Radical Ring-Opening Copolymerizationwith Vinyl Monomers},
author = {Mikel Irigoyen and Alice Marchand and Xabier Lopez de Pariza and Timo Melchin and Aitor Barquero and Jon M. Matxain and Haritz Sardón and Jose R. Leiza and Fernando Ruipérez},
doi = {10.1021/acs.macromol.6c00681},
issn = {1520-5835},
year = {2026},
date = {2026-07-28},
urldate = {2026-07-28},
journal = {Macromolecules},
volume = {59},
number = {14},
pages = {8509--8521},
publisher = {American Chemical Society (ACS)},
abstract = {<jats:title>Abstract</jats:title>
<jats:p>Radical ring-opening polymerization (rROP) of cyclic ketene acetals (CKAs), particularly 2-methylene-1,3-dioxepane (MDO), offers a robust pathway to introduce degradable ester linkages into nondegradable vinyl backbones. However, the rational design of these materials is currently hindered by highly comonomer-dependent open-to-closed (ester vs acetal) incorporation ratios. In this study, a rigorous density functional theory (DFT) framework integrating systematic conformational sampling and implicit solvation is employed to establish a unified structure–reactivity map for MDO copolymerization across a diverse set of vinyl monomers. The computational results reveal that while MDO homopolymerization is thermodynamically driven toward quantitative ring opening due to the irreversibility of the open-chain radical, copolymerization is governed by a fine-tuned competition between the kinetic accessibility of vinyl addition and the stability of the resulting cyclic adduct. The closed-propagation barrier is primarily dictated by a SOMO–LUMO interaction, where the electronic nature and α-substitution of the comonomer modulate orbital overlap and energy. Three distinct reactivity regimes are identified: (1) high open incorporation (e.g., MDO, crotonates), where high vinyl barriers and adduct reversibility favor β-scission; (2) intermediate competition (e.g., vinyl acetate); and (3) ring-retention dominance (e.g., acrylates), where rapid vinyl addition and deep thermodynamic stabilization suppress the degradable pathway. This work provides a qualitative molecular basis for the rational selection of comonomers to maximize CKA incorporation in the open form for next-generation sustainable vinyl polymers.</jats:p>},
keywords = {IT2067, POL-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:title>Abstract</jats:title>
<jats:p>Radical ring-opening polymerization (rROP) of cyclic ketene acetals (CKAs), particularly 2-methylene-1,3-dioxepane (MDO), offers a robust pathway to introduce degradable ester linkages into nondegradable vinyl backbones. However, the rational design of these materials is currently hindered by highly comonomer-dependent open-to-closed (ester vs acetal) incorporation ratios. In this study, a rigorous density functional theory (DFT) framework integrating systematic conformational sampling and implicit solvation is employed to establish a unified structure–reactivity map for MDO copolymerization across a diverse set of vinyl monomers. The computational results reveal that while MDO homopolymerization is thermodynamically driven toward quantitative ring opening due to the irreversibility of the open-chain radical, copolymerization is governed by a fine-tuned competition between the kinetic accessibility of vinyl addition and the stability of the resulting cyclic adduct. The closed-propagation barrier is primarily dictated by a SOMO–LUMO interaction, where the electronic nature and α-substitution of the comonomer modulate orbital overlap and energy. Three distinct reactivity regimes are identified: (1) high open incorporation (e.g., MDO, crotonates), where high vinyl barriers and adduct reversibility favor β-scission; (2) intermediate competition (e.g., vinyl acetate); and (3) ring-retention dominance (e.g., acrylates), where rapid vinyl addition and deep thermodynamic stabilization suppress the degradable pathway. This work provides a qualitative molecular basis for the rational selection of comonomers to maximize CKA incorporation in the open form for next-generation sustainable vinyl polymers.</jats:p>
<jats:p>Radical ring-opening polymerization (rROP) of cyclic ketene acetals (CKAs), particularly 2-methylene-1,3-dioxepane (MDO), offers a robust pathway to introduce degradable ester linkages into nondegradable vinyl backbones. However, the rational design of these materials is currently hindered by highly comonomer-dependent open-to-closed (ester vs acetal) incorporation ratios. In this study, a rigorous density functional theory (DFT) framework integrating systematic conformational sampling and implicit solvation is employed to establish a unified structure–reactivity map for MDO copolymerization across a diverse set of vinyl monomers. The computational results reveal that while MDO homopolymerization is thermodynamically driven toward quantitative ring opening due to the irreversibility of the open-chain radical, copolymerization is governed by a fine-tuned competition between the kinetic accessibility of vinyl addition and the stability of the resulting cyclic adduct. The closed-propagation barrier is primarily dictated by a SOMO–LUMO interaction, where the electronic nature and α-substitution of the comonomer modulate orbital overlap and energy. Three distinct reactivity regimes are identified: (1) high open incorporation (e.g., MDO, crotonates), where high vinyl barriers and adduct reversibility favor β-scission; (2) intermediate competition (e.g., vinyl acetate); and (3) ring-retention dominance (e.g., acrylates), where rapid vinyl addition and deep thermodynamic stabilization suppress the degradable pathway. This work provides a qualitative molecular basis for the rational selection of comonomers to maximize CKA incorporation in the open form for next-generation sustainable vinyl polymers.</jats:p>
29.
Loizate, Mikel; Lê, Trân Ngọc Khanh; Picchio, Matias L.; Zubeltzu, Jon; Formoso, Elena; Frömbgen, Tom; Kirchner, Barbara; Tassaing, Thierry; Rezabal, Elixabete
Hydrogen-bond networks and proton transfer in choline geranate: insights from IR spectroscopy Journal Article
In: Phys. Chem. Chem. Phys., vol. 28, no. 28, pp. 17605–17614, 2026, ISSN: 1463-9084.
Abstract | Links | BibTeX | Tags: IT2067, SUS-KT
@article{Loizate2026,
title = {Hydrogen-bond networks and proton transfer in choline geranate: insights from IR spectroscopy},
author = {Mikel Loizate and Trân Ngọc Khanh Lê and Matias L. Picchio and Jon Zubeltzu and Elena Formoso and Tom Frömbgen and Barbara Kirchner and Thierry Tassaing and Elixabete Rezabal},
doi = {10.1039/d6cp01217e},
issn = {1463-9084},
year = {2026},
date = {2026-07-22},
urldate = {2026-07-22},
journal = {Phys. Chem. Chem. Phys.},
volume = {28},
number = {28},
pages = {17605--17614},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>Experiment and simulation reveal the molecular origin of proton transfer in choline–geranate, showing that transient proton exchange occurs while preserving distinct carboxylic acid and carboxylate species.</jats:p>},
keywords = {IT2067, SUS-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>Experiment and simulation reveal the molecular origin of proton transfer in choline–geranate, showing that transient proton exchange occurs while preserving distinct carboxylic acid and carboxylate species.</jats:p>
28.
Verdugo, Marta Costa; Martínez-Martínez, Virginia; Hernandez-Fernandez, Laura; Re, Francesca; Rezabal, Elixabete; Salassa, Luca
Reshaping Ru polypyridyl photochemistry with choline–geranate (CAGE) ionic liquids Journal Article
In: Chem. Commun., vol. 62, no. 55, pp. 13757–13761, 2026, ISSN: 1364-548X.
Abstract | Links | BibTeX | Tags: IT2067, SUS-KT
@article{CostaVerdugo2026,
title = {Reshaping Ru polypyridyl photochemistry with choline–geranate (CAGE) ionic liquids},
author = {Marta Costa Verdugo and Virginia Martínez-Martínez and Laura Hernandez-Fernandez and Francesca Re and Elixabete Rezabal and Luca Salassa},
doi = {10.1039/d6cc02290a},
issn = {1364-548X},
year = {2026},
date = {2026-07-16},
urldate = {2026-07-16},
journal = {Chem. Commun.},
volume = {62},
number = {55},
pages = {13757--13761},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>Choline–geranate (CAGE) ionic liquids are emerging as powerful topical delivery media, yet their impact on the photochemistry of metal-based phototherapeutics remains unexplored.</jats:p>},
keywords = {IT2067, SUS-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>Choline–geranate (CAGE) ionic liquids are emerging as powerful topical delivery media, yet their impact on the photochemistry of metal-based phototherapeutics remains unexplored.</jats:p>
27.
Lew-Yee, Juan Felipe Huan; Rezabal, Elixabete; Lopez, Xabier; Piris, Mario; Mercero, Jose M.
A Python-Based Module for Exploring Machine Learning-Inspired Optimization Algorithms Using Quantum Chemistry Journal Article
In: J. Chem. Educ., vol. 103, no. 7, pp. 3929–3937, 2026, ISSN: 1938-1328.
Links | BibTeX | Tags: IT2067, MatCat-KT, NOFT
@article{Lew-Yee2026b,
title = {A Python-Based Module for Exploring Machine Learning-Inspired Optimization Algorithms Using Quantum Chemistry},
author = {Juan Felipe Huan Lew-Yee and Elixabete Rezabal and Xabier Lopez and Mario Piris and Jose M. Mercero},
doi = {10.1021/acs.jchemed.5c01470},
issn = {1938-1328},
year = {2026},
date = {2026-07-14},
urldate = {2026-07-14},
journal = {J. Chem. Educ.},
volume = {103},
number = {7},
pages = {3929--3937},
publisher = {American Chemical Society (ACS)},
keywords = {IT2067, MatCat-KT, NOFT},
pubstate = {published},
tppubtype = {article}
}
26.
Chithra, Sree; Pigot, Corentin; Tonnelé, Claire; Redman, Ashley J.; Richert, Sabine; Casanova, David; Gray, Victor
Electron transfer from singlet fission dimers: possibilities and limitations Journal Article
In: Chem. Sci., vol. 17, no. 26, pp. 12970–12980, 2026, ISSN: 2041-6539.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Chithra2026,
title = {Electron transfer from singlet fission dimers: possibilities and limitations},
author = {Sree Chithra and Corentin Pigot and Claire Tonnelé and Ashley J. Redman and Sabine Richert and David Casanova and Victor Gray},
doi = {10.1039/d6sc00259e},
issn = {2041-6539},
year = {2026},
date = {2026-07-08},
urldate = {2026-07-08},
journal = {Chem. Sci.},
volume = {17},
number = {26},
pages = {12970--12980},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>
The singlet/triplet pair equilibrium in tetracene dimers can drive singlet‑like electron transfer but inevitably yields only one long-lived T
<jats:sub>1</jats:sub>
, limiting diffusion-controlled ET efficiencies from free triplets to <100% yield.
</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>
The singlet/triplet pair equilibrium in tetracene dimers can drive singlet‑like electron transfer but inevitably yields only one long-lived T
<jats:sub>1</jats:sub>
, limiting diffusion-controlled ET efficiencies from free triplets to <100% yield.
</jats:p>
The singlet/triplet pair equilibrium in tetracene dimers can drive singlet‑like electron transfer but inevitably yields only one long-lived T
<jats:sub>1</jats:sub>
, limiting diffusion-controlled ET efficiencies from free triplets to <100% yield.
</jats:p>
25.
Wu, Yifan; Wang, Bipeng; Chaudhary, Mohit; Casanova, David; Prezhdo, Oleg V.
Efficient Nonadiabatic Molecular Dynamics with Machine Learning Hamiltonian Interpolation Journal Article
In: J. Phys. Chem. Lett., vol. 17, no. 26, pp. 7328–7335, 2026, ISSN: 1948-7185.
Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Wu2026,
title = {Efficient Nonadiabatic Molecular Dynamics with Machine Learning Hamiltonian Interpolation},
author = {Yifan Wu and Bipeng Wang and Mohit Chaudhary and David Casanova and Oleg V. Prezhdo},
doi = {10.1021/acs.jpclett.6c01666},
issn = {1948-7185},
year = {2026},
date = {2026-07-02},
urldate = {2026-07-02},
journal = {J. Phys. Chem. Lett.},
volume = {17},
number = {26},
pages = {7328--7335},
publisher = {American Chemical Society (ACS)},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
24.
Churchill, Olivia; Martin, Robert; Lockyer, Selena J.; Whitehead, George F. S.; Timco, Grigore A.; Collison, David; McInnes, Eric J. L.; Reta, Daniel; Schnack, Jürgen; Winpenny, Richard E. P.
A new {Cr10Ni4} seahorse featuring an oxalate ligand Journal Article
In: Inorganic Chemistry Communications, vol. 190, 2026, ISSN: 1387-7003.
Links | BibTeX | Tags: IT2067, MoMag-KT
@article{Churchill2026,
title = {A new {Cr10Ni4} seahorse featuring an oxalate ligand},
author = {Olivia Churchill and Robert Martin and Selena J. Lockyer and George F.S. Whitehead and Grigore A. Timco and David Collison and Eric J.L. McInnes and Daniel Reta and Jürgen Schnack and Richard E.P. Winpenny},
doi = {10.1016/j.inoche.2026.116828},
issn = {1387-7003},
year = {2026},
date = {2026-06-26},
journal = {Inorganic Chemistry Communications},
volume = {190},
publisher = {Elsevier BV},
keywords = {IT2067, MoMag-KT},
pubstate = {published},
tppubtype = {article}
}
23.
Teotonico, Jacopo; Ruipérez, Fernando; Ballard, Nicholas
In: Polym. Chem., vol. 17, no. 23, pp. 2479–2490, 2026, ISSN: 1759-9962.
Abstract | Links | BibTeX | Tags: IT2067, POL-KT
@article{Teotonico2026,
title = {Dynamic exchange in vinylogous urethane vitrimers: computational and experimental approaches to screen structure–property relationships of dynamic bonds},
author = {Jacopo Teotonico and Fernando Ruipérez and Nicholas Ballard},
doi = {10.1039/d6py00217j},
issn = {1759-9962},
year = {2026},
date = {2026-06-16},
urldate = {2026-06-16},
journal = {Polym. Chem.},
volume = {17},
number = {23},
pages = {2479--2490},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>Computational and experimental screening of vinylogous urethane vitrimers reveals how substituents tune dynamic bond exchange. DFT is combined with NMR experiments to link molecular structure to stress relaxation, enabling tailored performance.</jats:p>},
keywords = {IT2067, POL-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>Computational and experimental screening of vinylogous urethane vitrimers reveals how substituents tune dynamic bond exchange. DFT is combined with NMR experiments to link molecular structure to stress relaxation, enabling tailored performance.</jats:p>
22.
Jiménez-García, Juan Carlos; López-Gallego, Fernando; López, Xabier; Sancho, David De
MartiniSurf: Automated Simulations of Surface-Immobilized Biomolecular Systems with Martini Journal Article
In: J. Chem. Inf. Model., 2026, ISSN: 1549-960X.
Links | BibTeX | Tags: Bio-KT, IT2067
@article{Jiménez-García2026b,
title = {MartiniSurf: Automated Simulations of Surface-Immobilized Biomolecular Systems with Martini},
author = {Juan Carlos Jiménez-García and Fernando López-Gallego and Xabier López and David De Sancho},
doi = {10.1021/acs.jcim.6c00953},
issn = {1549-960X},
year = {2026},
date = {2026-06-16},
urldate = {2026-06-16},
journal = {J. Chem. Inf. Model.},
publisher = {American Chemical Society (ACS)},
keywords = {Bio-KT, IT2067},
pubstate = {published},
tppubtype = {article}
}
21.
Santamaría, Guillermo; Siddi, Francesco; Carreras, Abel; Dettori, Riccardo; Simoncelli, Michele; Melis, Claudio; Casanova, David; Beljonne, David
Anharmonic Effects Revealed by Temperature-Dependent Phonon Lifetimes and Thermal Conductivities in a π-Conjugated Molecular Crystal Journal Article
In: J. Chem. Theory Comput., vol. 22, no. 11, pp. 5742–5751, 2026, ISSN: 1549-9626.
Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Santamaría2026,
title = {Anharmonic Effects Revealed by Temperature-Dependent Phonon Lifetimes and Thermal Conductivities in a π-Conjugated Molecular Crystal},
author = {Guillermo Santamaría and Francesco Siddi and Abel Carreras and Riccardo Dettori and Michele Simoncelli and Claudio Melis and David Casanova and David Beljonne},
doi = {10.1021/acs.jctc.6c00412},
issn = {1549-9626},
year = {2026},
date = {2026-06-09},
urldate = {2026-06-09},
journal = {J. Chem. Theory Comput.},
volume = {22},
number = {11},
pages = {5742--5751},
publisher = {American Chemical Society (ACS)},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
20.
Loirette-Pelous, Aurelian; Boto, Roberto A.; Aizpurua, Javier; Esteban, Ruben
Addressing Intramolecular Vibrational Redistribution in a Single Molecule through Pump and Probe Surface-Enhanced Vibrational Spectroscopy Journal Article
In: ACS Photonics, vol. 13, no. 11, pp. 3088–3101, 2026, ISSN: 2330-4022.
@article{Loirette-Pelous2026,
title = {Addressing Intramolecular Vibrational Redistribution in a Single Molecule through Pump and Probe Surface-Enhanced Vibrational Spectroscopy},
author = {Aurelian Loirette-Pelous and Roberto A. Boto and Javier Aizpurua and Ruben Esteban},
doi = {10.1021/acsphotonics.6c00030},
issn = {2330-4022},
year = {2026},
date = {2026-06-03},
urldate = {2026-06-03},
journal = {ACS Photonics},
volume = {13},
number = {11},
pages = {3088--3101},
publisher = {American Chemical Society (ACS)},
keywords = {IT2067},
pubstate = {published},
tppubtype = {article}
}
19.
Armentia, Lydia; López, Xabier; Sancho, David De
Molecular determinants of arginine versus lysine cation–π interactions in biomolecular condensates Journal Article Forthcoming
In: Commun Chem, vol. 9, no. 1, Forthcoming, ISSN: 2399-3669.
Links | BibTeX | Tags: Bio-KT, IT2067
@article{Armentia2026,
title = {Molecular determinants of arginine versus lysine cation–π interactions in biomolecular condensates},
author = {Lydia Armentia and Xabier López and David De Sancho},
doi = {10.1038/s42004-026-02075-7},
issn = {2399-3669},
year = {2026},
date = {2026-05-26},
journal = {Commun Chem},
volume = {9},
number = {1},
publisher = {Springer Science and Business Media LLC},
keywords = {Bio-KT, IT2067},
pubstate = {forthcoming},
tppubtype = {article}
}
18.
Hannan, Robert J.; Vondran, Alexandria M.; Cho, Sunghwan; Hanson, Kerry M.; Tonnelé, Claire; Casanova, David; Bardeen, Christopher J.; Bahamonde, Ana
Photochemical reduction of aryl chlorides, bromides, and iodides via ternary EDA complexes with guanidine bases Journal Article
In: Chem. Sci., vol. 17, no. 17, pp. 8486–8492, 2026, ISSN: 2041-6539.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Hannan2026b,
title = {Photochemical reduction of aryl chlorides, bromides, and iodides \textit{via} ternary EDA complexes with guanidine bases},
author = {Robert J. Hannan and Alexandria M. Vondran and Sunghwan Cho and Kerry M. Hanson and Claire Tonnelé and David Casanova and Christopher J. Bardeen and Ana Bahamonde},
doi = {10.1039/d6sc00251j},
issn = {2041-6539},
year = {2026},
date = {2026-05-06},
urldate = {2026-05-06},
journal = {Chem. Sci.},
volume = {17},
number = {17},
pages = {8486--8492},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>
Commercially available TBD was found to be an effective photoreductant for a variety of aryl halides. The reactivity is proposed to proceed
<jats:italic>via</jats:italic>
formation of a ternary EDA complex composed of two TBD molecules and one aryl halide.
</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>
Commercially available TBD was found to be an effective photoreductant for a variety of aryl halides. The reactivity is proposed to proceed
<jats:italic>via</jats:italic>
formation of a ternary EDA complex composed of two TBD molecules and one aryl halide.
</jats:p>
Commercially available TBD was found to be an effective photoreductant for a variety of aryl halides. The reactivity is proposed to proceed
<jats:italic>via</jats:italic>
formation of a ternary EDA complex composed of two TBD molecules and one aryl halide.
</jats:p>
17.
Gastearena, Xuban; Ruipérez, Fernando; Barroso-Bujans, Fabienne; Lam, Anabel; Matxain, Jon M.
In: Polymer, vol. 350, no. 129792, 2026, ISSN: 0032-3861.
Links | BibTeX | Tags: IT2067, POL-KT
@article{Gastearena2026,
title = {An insight into the monomeric isomerism in the polymerization of glycidol with B(C6F5)3: A DFT study of the initiation, propagation and cyclization steps},
author = {Xuban Gastearena and Fernando Ruipérez and Fabienne Barroso-Bujans and Anabel Lam and Jon M. Matxain},
doi = {10.1016/j.polymer.2026.129792},
issn = {0032-3861},
year = {2026},
date = {2026-04-02},
urldate = {2026-04-02},
journal = {Polymer},
volume = {350},
number = {129792},
publisher = {Elsevier BV},
keywords = {IT2067, POL-KT},
pubstate = {published},
tppubtype = {article}
}
16.
Kanavos, Ioannis; Nakahata, Douglas H.; Barrett, Madeleine S.; dos Santos, Ancély F.; Zubiria-Ulacia, Maria; Pieslinger, German E.; da Silva Teixeira, Ana Beatriz; Medeiros, Isadora; Rocha, Clarissa Ribeiro Reily; Eberle, Jonas; Lobinski, Ryszard; Matxain, Jon Mattin; Hall, Matthew D.; Angeli, José P. Friedmann; Arnér, Elias S. J.; Ronga, Luisa; de Paiva, Raphael E. F.
What lies beyond thioredoxin reductase? Cyclometallated gold compounds reveal Sec selectivity in glutathione peroxidases Journal Article
In: Free Radical Biology and Medicine, vol. 247, pp. 139–156, 2026, ISSN: 0891-5849.
Links | BibTeX | Tags: IT2067, POL-KT
@article{Kanavos2026,
title = {What lies beyond thioredoxin reductase? Cyclometallated gold compounds reveal Sec selectivity in glutathione peroxidases},
author = {Ioannis Kanavos and Douglas H. Nakahata and Madeleine S. Barrett and Ancély F. dos Santos and Maria Zubiria-Ulacia and German E. Pieslinger and Ana Beatriz da Silva Teixeira and Isadora Medeiros and Clarissa Ribeiro Reily Rocha and Jonas Eberle and Ryszard Lobinski and Jon Mattin Matxain and Matthew D. Hall and José P. Friedmann Angeli and Elias S.J. Arnér and Luisa Ronga and Raphael E.F. de Paiva},
doi = {10.1016/j.freeradbiomed.2026.02.007},
issn = {0891-5849},
year = {2026},
date = {2026-04-01},
journal = {Free Radical Biology and Medicine},
volume = {247},
pages = {139--156},
publisher = {Elsevier BV},
keywords = {IT2067, POL-KT},
pubstate = {published},
tppubtype = {article}
}
15.
Rodriguez, Alba; Formoso, Elena; Knudsen, Birgitta R.; Tesauro, Cinzia; Fuertes, Maria; Alonso, Concepcion
In: ChemMedChem, vol. 21, no. 5, 2026, ISSN: 1860-7187.
Abstract | Links | BibTeX | Tags: Bio-KT, IT2067
@article{Rodriguez2026,
title = {Synthesis, Biological Evaluation, and Theoretical Study of Indenoquinolinylphosphine Oxide Derivatives as Topoisomerase 1 Inhibitors and Antiproliferative Agents},
author = {Alba Rodriguez and Elena Formoso and Birgitta R. Knudsen and Cinzia Tesauro and Maria Fuertes and Concepcion Alonso},
doi = {10.1002/cmdc.202500751},
issn = {1860-7187},
year = {2026},
date = {2026-03-13},
urldate = {2026-03-13},
journal = {ChemMedChem},
volume = {21},
number = {5},
publisher = {Wiley},
abstract = {<jats:p>
The topoisomerase 1 (TOP1) enzymatic inhibition and antiproliferative activity of phosphorated indenoquinoline derivatives were investigated. First, the preparation of new hybrid quinoline and tetrahydroquinoline structures with a phosphine oxide group was performed by a two‐step Povarov type [4 + 2]‐cycloaddition reaction between the corresponding phosphorated aldimines with indene in the presence of BF
<jats:sub>3</jats:sub>
·Et
<jats:sub>2</jats:sub>
O, affording corresponding 1,2,3,4‐tetrahydroindeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>9</jats:bold>
, 7H‐indeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>10</jats:bold>
and 7‐oxoindeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>11</jats:bold>
with good yields. The synthesized derivatives were evaluated as TOP1 inhibitors, showing that some derivatives (
<jats:bold>9f</jats:bold>
,
<jats:bold>9g</jats:bold>
,
<jats:bold>9l</jats:bold>
, and
<jats:bold>11m</jats:bold>
) show better or similar activity to the reference compound (CPT) at 1 min. The synthesized derivatives were screened for their antiproliferative activity in different cancerous cell lines, and all of them present a higher selective cytotoxicity in the human lung adenocarcinoma cell line (A549), than in the others. In contrast, almost none of the synthesized phosphorated compounds exhibited antiproliferative activity toward nonmalignant lung fibroblasts MCR5. These results suggest that phosphine oxide‐substituted quinoline derivatives have important properties as TOP1 inhibitors and show an interesting cytotoxicity against six different cancerous cell lines.
</jats:p>},
keywords = {Bio-KT, IT2067},
pubstate = {published},
tppubtype = {article}
}
<jats:p>
The topoisomerase 1 (TOP1) enzymatic inhibition and antiproliferative activity of phosphorated indenoquinoline derivatives were investigated. First, the preparation of new hybrid quinoline and tetrahydroquinoline structures with a phosphine oxide group was performed by a two‐step Povarov type [4 + 2]‐cycloaddition reaction between the corresponding phosphorated aldimines with indene in the presence of BF
<jats:sub>3</jats:sub>
·Et
<jats:sub>2</jats:sub>
O, affording corresponding 1,2,3,4‐tetrahydroindeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>9</jats:bold>
, 7H‐indeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>10</jats:bold>
and 7‐oxoindeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>11</jats:bold>
with good yields. The synthesized derivatives were evaluated as TOP1 inhibitors, showing that some derivatives (
<jats:bold>9f</jats:bold>
,
<jats:bold>9g</jats:bold>
,
<jats:bold>9l</jats:bold>
, and
<jats:bold>11m</jats:bold>
) show better or similar activity to the reference compound (CPT) at 1 min. The synthesized derivatives were screened for their antiproliferative activity in different cancerous cell lines, and all of them present a higher selective cytotoxicity in the human lung adenocarcinoma cell line (A549), than in the others. In contrast, almost none of the synthesized phosphorated compounds exhibited antiproliferative activity toward nonmalignant lung fibroblasts MCR5. These results suggest that phosphine oxide‐substituted quinoline derivatives have important properties as TOP1 inhibitors and show an interesting cytotoxicity against six different cancerous cell lines.
</jats:p>
The topoisomerase 1 (TOP1) enzymatic inhibition and antiproliferative activity of phosphorated indenoquinoline derivatives were investigated. First, the preparation of new hybrid quinoline and tetrahydroquinoline structures with a phosphine oxide group was performed by a two‐step Povarov type [4 + 2]‐cycloaddition reaction between the corresponding phosphorated aldimines with indene in the presence of BF
<jats:sub>3</jats:sub>
·Et
<jats:sub>2</jats:sub>
O, affording corresponding 1,2,3,4‐tetrahydroindeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>9</jats:bold>
, 7H‐indeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>10</jats:bold>
and 7‐oxoindeno[2,1‐c]quinolinylphosphine oxides
<jats:bold>11</jats:bold>
with good yields. The synthesized derivatives were evaluated as TOP1 inhibitors, showing that some derivatives (
<jats:bold>9f</jats:bold>
,
<jats:bold>9g</jats:bold>
,
<jats:bold>9l</jats:bold>
, and
<jats:bold>11m</jats:bold>
) show better or similar activity to the reference compound (CPT) at 1 min. The synthesized derivatives were screened for their antiproliferative activity in different cancerous cell lines, and all of them present a higher selective cytotoxicity in the human lung adenocarcinoma cell line (A549), than in the others. In contrast, almost none of the synthesized phosphorated compounds exhibited antiproliferative activity toward nonmalignant lung fibroblasts MCR5. These results suggest that phosphine oxide‐substituted quinoline derivatives have important properties as TOP1 inhibitors and show an interesting cytotoxicity against six different cancerous cell lines.
</jats:p>
14.
Toldo, Josene M.; Staab, Jakob K.; Matito, Eduard; Foroutan-Nejad, Cina; Ottosson, Henrik
Deciphering the molecular origin of the 19.3 eV electronic excitation energy of H 3 + Journal Article
In: Chem. Sci., vol. 17, no. 10, pp. 5029–5037, 2026, ISSN: 2041-6539.
Links | BibTeX | Tags: IT2067, QCD-KT
@article{Toldo2026,
title = {Deciphering the molecular origin of the 19.3 eV electronic excitation energy of H _{3} ^{+}},
author = {Josene M. Toldo and Jakob K. Staab and Eduard Matito and Cina Foroutan-Nejad and Henrik Ottosson},
doi = {10.1039/d5sc09067a},
issn = {2041-6539},
year = {2026},
date = {2026-03-11},
urldate = {2026-03-11},
journal = {Chem. Sci.},
volume = {17},
number = {10},
pages = {5029--5037},
publisher = {Royal Society of Chemistry (RSC)},
keywords = {IT2067, QCD-KT},
pubstate = {published},
tppubtype = {article}
}
13.
Owona, Josianne; Goto, Selom J.; Truflandier, Lionel; Tonnelé, Claire; Castet, Frédéric
In: Phys. Chem. Chem. Phys., vol. 28, no. 10, pp. 6636–6648, 2026, ISSN: 1463-9084.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Owona2026,
title = {Pressure- and aggregation-induced modulation of linear and nonlinear optical properties in a push–pull chromophore: insights from computational modelling},
author = {Josianne Owona and Selom J. Goto and Lionel Truflandier and Claire Tonnelé and Frédéric Castet},
doi = {10.1039/d5cp04030b},
issn = {1463-9084},
year = {2026},
date = {2026-03-11},
urldate = {2026-03-11},
journal = {Phys. Chem. Chem. Phys.},
volume = {28},
number = {10},
pages = {6636--6648},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>We report a theoretical investigation of the structural and optical responses of a molecular crystal based on a push–pull chromophore subjected to increasing isotropic pressure ranging from 1 to 30 kbar.</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>We report a theoretical investigation of the structural and optical responses of a molecular crystal based on a push–pull chromophore subjected to increasing isotropic pressure ranging from 1 to 30 kbar.</jats:p>
12.
Mitxelena, Ion; Lew-Yee, Juan Felipe Huan; Piris, Mario
5- and 6-Membered Rings: A Natural Orbital Functional Study Journal Article
In: Journal of Chemical Theory and Computation, vol. 22, iss. 6, pp. 2799-2807, 2026.
Abstract | Links | BibTeX | Tags: IT2067, NOFT
@article{nokey,
title = {5- and 6-Membered Rings: A Natural Orbital Functional Study},
author = {Ion Mitxelena and Juan Felipe Huan Lew-Yee and Mario Piris},
doi = {https://doi.org/10.1021/acs.jctc.5c01861},
year = {2026},
date = {2026-03-05},
urldate = {2026-03-05},
journal = {Journal of Chemical Theory and Computation},
volume = {22},
issue = {6},
pages = {2799-2807},
abstract = {The Global Natural Orbital Functional (GNOF) provides a straightforward approach to capture most electron correlation effects without needing perturbative corrections or limited active spaces selection. In this work, we evaluate both the original GNOF and its modified variant, GNOFm, on a set of twelve 5- and 6-membered molecular rings, systems characterized primarily by dynamic correlation. This reference set is vital as it comprises essential substructures of more complex molecules. We report complete-basis-set limit correlation energies for GNOF, GNOFm, and the benchmark CCSD(T) method. Across the Dunning basis sets, both functionals deliver a balanced and accurate description of the molecular set, with GNOFm showing small but systematic improvements while preserving the overall robustness of the original formulation. These results confirm the reliability of the GNOF family and its ability to capture dynamic correlation effects.},
keywords = {IT2067, NOFT},
pubstate = {published},
tppubtype = {article}
}
The Global Natural Orbital Functional (GNOF) provides a straightforward approach to capture most electron correlation effects without needing perturbative corrections or limited active spaces selection. In this work, we evaluate both the original GNOF and its modified variant, GNOFm, on a set of twelve 5- and 6-membered molecular rings, systems characterized primarily by dynamic correlation. This reference set is vital as it comprises essential substructures of more complex molecules. We report complete-basis-set limit correlation energies for GNOF, GNOFm, and the benchmark CCSD(T) method. Across the Dunning basis sets, both functionals deliver a balanced and accurate description of the molecular set, with GNOFm showing small but systematic improvements while preserving the overall robustness of the original formulation. These results confirm the reliability of the GNOF family and its ability to capture dynamic correlation effects.
11.
Luna, Emelin; Olazabal, Ion; de Somer, Tobias; Nachtergaele, Pieter; Lopez, Xabier; Ximenis, Marta; de Meester, Steven; Sardon, Haritz
Solvent switch strategy to facilitate the downstream process of chemical recycling of plastics Journal Article
In: Resources, Conservation and Recycling, vol. 226, 2026, ISSN: 0921-3449.
Links | BibTeX | Tags: Bio-KT, IT2067
@article{Luna2026b,
title = {Solvent switch strategy to facilitate the downstream process of chemical recycling of plastics},
author = {Emelin Luna and Ion Olazabal and Tobias de Somer and Pieter Nachtergaele and Xabier Lopez and Marta Ximenis and Steven de Meester and Haritz Sardon},
doi = {10.1016/j.resconrec.2025.108686},
issn = {0921-3449},
year = {2026},
date = {2026-02-23},
journal = {Resources, Conservation and Recycling},
volume = {226},
publisher = {Elsevier BV},
keywords = {Bio-KT, IT2067},
pubstate = {published},
tppubtype = {article}
}
10.
Jiménez-García, Juan Carlos; Zeballos, Nicoll; López-Gallego, Fernando; López, Xabier; Sancho, David De
Mechanistic Determinants of Oriented Enzyme Immobilization from Martini Simulations Journal Article
In: J. Phys. Chem. Lett., vol. 17, no. 7, pp. 2094–2102, 2026, ISSN: 1948-7185.
Links | BibTeX | Tags: Bio-KT, IT2067
@article{Jiménez-García2026,
title = {Mechanistic Determinants of Oriented Enzyme Immobilization from Martini Simulations},
author = {Juan Carlos Jiménez-García and Nicoll Zeballos and Fernando López-Gallego and Xabier López and David De Sancho},
doi = {10.1021/acs.jpclett.5c03753},
issn = {1948-7185},
year = {2026},
date = {2026-02-19},
urldate = {2026-02-19},
journal = {J. Phys. Chem. Lett.},
volume = {17},
number = {7},
pages = {2094--2102},
publisher = {American Chemical Society (ACS)},
keywords = {Bio-KT, IT2067},
pubstate = {published},
tppubtype = {article}
}
9.
Lew-Yee, Juan Felipe Huan; Mitxelena, Ion; del Campo, Jorge M.; Piris, Mario
DoNOF 2.0: A modern open-source electronic structure program for natural orbital functionals Journal Article
In: The Journal of Chemical Physics, vol. 164, iss. 7, pp. 072501, 2026, ISSN: 1089-7690.
Abstract | Links | BibTeX | Tags: IT2067, NOFT
@article{Lew-Yee2026,
title = {DoNOF 2.0: A modern open-source electronic structure program for natural orbital functionals},
author = {Juan Felipe Huan Lew-Yee and Ion Mitxelena and Jorge M. del Campo and Mario Piris},
doi = {10.1063/5.0316927},
issn = {1089-7690},
year = {2026},
date = {2026-02-18},
urldate = {2026-02-18},
journal = {The Journal of Chemical Physics},
volume = {164},
issue = {7},
pages = {072501},
publisher = {AIP Publishing},
abstract = {In this work, we present the second version of the Donostia natural orbital functional software, an open-source program for natural orbital functional calculations. The new release incorporates improved optimization algorithms, capabilities for excited-state computations, support for ab initio molecular dynamics, and integration with the libcint library. DoNOF 2.0 also extends its property toolbox by enabling the evaluation of nonlinear optical responses, including static polarizabilities and higher-order hyperpolarizabilities via a finite-field Romberg–Richardson scheme.},
keywords = {IT2067, NOFT},
pubstate = {published},
tppubtype = {article}
}
In this work, we present the second version of the Donostia natural orbital functional software, an open-source program for natural orbital functional calculations. The new release incorporates improved optimization algorithms, capabilities for excited-state computations, support for ab initio molecular dynamics, and integration with the libcint library. DoNOF 2.0 also extends its property toolbox by enabling the evaluation of nonlinear optical responses, including static polarizabilities and higher-order hyperpolarizabilities via a finite-field Romberg–Richardson scheme.
8.
Calvo, Unai; Matxain, Jon M.; Egurrola, Jose Javier; Burgoa, Aizeti; Ruipérez, Fernando
Polymer-metal oxide interfaces in XHNBR/PA6 blends: computational insights toward sustainable crosslinking Journal Article
In: RSC Adv., vol. 16, no. 10, pp. 9167–9179, 2026, ISSN: 2046-2069.
Abstract | Links | BibTeX | Tags: IT2067, POL-KT
@article{Calvo2026,
title = {Polymer-metal oxide interfaces in XHNBR/PA6 blends: computational insights toward sustainable crosslinking},
author = {Unai Calvo and Jon M. Matxain and Jose Javier Egurrola and Aizeti Burgoa and Fernando Ruipérez},
doi = {10.1039/d5ra09279e},
issn = {2046-2069},
year = {2026},
date = {2026-02-11},
journal = {RSC Adv.},
volume = {16},
number = {10},
pages = {9167--9179},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {Polyamide 6 (PA6) is a high-performance thermoplastic widely used in engineering applications, while carboxylated hydrogenated nitrile rubber (XHNBR) provides viscoelastic damping and reactive carboxyl groups for crosslinking with metal oxides. },
keywords = {IT2067, POL-KT},
pubstate = {published},
tppubtype = {article}
}
7.
Rodriguez-Jimenez, Jose Aaron; Calupitan, Jan Patrick; Casanova, David
Electronic structure origins of radical character in triangular fused acenes: sextet stabilization vs. antiaromaticity release Journal Article
In: ORGANIC CHEMISTRY FRONTIERS, vol. 13, no. 3, pp. 794-802, 2026.
Links | BibTeX | Tags: IT2067, MolEles-KT
@article{WOS:001629880400001,
title = {Electronic structure origins of radical character in triangular fused
acenes: sextet stabilization vs. antiaromaticity release},
author = {Jose Aaron Rodriguez-Jimenez and Jan Patrick Calupitan and David Casanova},
doi = {10.1039/d5qo01343g},
year = {2026},
date = {2026-02-01},
journal = {ORGANIC CHEMISTRY FRONTIERS},
volume = {13},
number = {3},
pages = {794-802},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
6.
Carreras, Abel; Orús, Román; Casanova, David
Limitations of quantum hardware for molecular energy estimation using VQE Journal Article
In: Phys. Chem. Chem. Phys., vol. 28, no. 4, pp. 2834–2846, 2026, ISSN: 1463-9084.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Carreras2026,
title = {Limitations of quantum hardware for molecular energy estimation using VQE},
author = {Abel Carreras and Román Orús and David Casanova},
doi = {10.1039/d5cp03907j},
issn = {1463-9084},
year = {2026},
date = {2026-01-28},
urldate = {2026-01-28},
journal = {Phys. Chem. Chem. Phys.},
volume = {28},
number = {4},
pages = {2834--2846},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {<jats:p>In this study, we investigate the performance of VQE algorithms implemented on current quantum hardware for determining molecular ground-state energies, focusing on the adaptive derivative-assembled pseudo-Trotter ansatz VQE (ADAPT-VQE).</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:p>In this study, we investigate the performance of VQE algorithms implemented on current quantum hardware for determining molecular ground-state energies, focusing on the adaptive derivative-assembled pseudo-Trotter ansatz VQE (ADAPT-VQE).</jats:p>
5.
Omist, Alicia; Casanova, David
Spin-Permutation Diabatization: A General Framework for Spin Localization and Exchange Coupling Journal Article
In: J. Chem. Theory Comput., vol. 22, no. 2, pp. 963–971, 2026, ISSN: 1549-9626.
Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Omist2026,
title = {Spin-Permutation Diabatization: A General Framework for Spin Localization and Exchange Coupling},
author = {Alicia Omist and David Casanova},
doi = {10.1021/acs.jctc.5c01904},
issn = {1549-9626},
year = {2026},
date = {2026-01-27},
urldate = {2026-01-27},
journal = {J. Chem. Theory Comput.},
volume = {22},
number = {2},
pages = {963--971},
publisher = {American Chemical Society (ACS)},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
4.
Merino, Santos; Villar, Alberto; Díez-Ahedo, Ruth; Gárate, Eider; Amenabar, Iban; Gay, Ralph; Espina, Jorge; Zapata-Herrera, Mario; Boto, Roberto A.; Aizpurua, Javier
Acrylamide molecule detection by surface-enhanced infrared absorption spectroscopy using resonant nanoantennas Journal Article
In: Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, vol. 345, 2026, ISSN: 1386-1425.
@article{Merino2026,
title = {Acrylamide molecule detection by surface-enhanced infrared absorption spectroscopy using resonant nanoantennas},
author = {Santos Merino and Alberto Villar and Ruth Díez-Ahedo and Eider Gárate and Iban Amenabar and Ralph Gay and Jorge Espina and Mario Zapata-Herrera and Roberto A. Boto and Javier Aizpurua},
doi = {10.1016/j.saa.2025.126772},
issn = {1386-1425},
year = {2026},
date = {2026-01-15},
journal = {Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy},
volume = {345},
publisher = {Elsevier BV},
keywords = {IT2067},
pubstate = {published},
tppubtype = {article}
}
3.
Guimarães, Amanda R.; Ballesteros, Óscar R.; Rivilla, Iván; Olaizola, Irene; Odriozola-Gimeno, Mikel; de Cózar, Abel; de Sancho, David; Lopez, Xabier; Banales, Jesus M.; Cossío, Fernando P.
Computational Analysis of a Next-Generation Platinum-Based Chemotherapies that Induce DNA Double-Strand Breaks Journal Article
In: J. Chem. Inf. Model., vol. 66, no. 1, pp. 668–683, 2026, ISSN: 1549-960X.
@article{Guimarães2025,
title = {Computational Analysis of a Next-Generation Platinum-Based Chemotherapies that Induce DNA Double-Strand Breaks},
author = {Amanda R. Guimarães and Óscar R. Ballesteros and Iván Rivilla and Irene Olaizola and Mikel Odriozola-Gimeno and Abel de Cózar and David de Sancho and Xabier Lopez and Jesus M. Banales and Fernando P. Cossío},
doi = {10.1021/acs.jcim.5c01654},
issn = {1549-960X},
year = {2026},
date = {2026-01-12},
urldate = {2026-01-12},
journal = {J. Chem. Inf. Model.},
volume = {66},
number = {1},
pages = {668--683},
publisher = {American Chemical Society (ACS)},
keywords = {IT2067},
pubstate = {published},
tppubtype = {article}
}
2.
Manjanath, Aaditya; Casanova, David; Sahara, Ryoji; Hsu, Chao‐Ping
Localized Molecular Orbitals for Single Excitation Theories Journal Article
In: J Comput Chem, vol. 47, no. 1, 2026, ISSN: 1096-987X.
Abstract | Links | BibTeX | Tags: IT2067, MolEles-KT
@article{Manjanath2025,
title = {Localized Molecular Orbitals for Single Excitation Theories},
author = {Aaditya Manjanath and David Casanova and Ryoji Sahara and Chao‐Ping Hsu},
doi = {10.1002/jcc.70293},
issn = {1096-987X},
year = {2026},
date = {2026-01-05},
urldate = {2026-01-05},
journal = {J Comput Chem},
volume = {47},
number = {1},
publisher = {Wiley},
abstract = {<jats:title>ABSTRACT</jats:title>
<jats:p>Excited states of systems composed of linked fragments or stacked molecules are important for understanding their optoelectronic properties. These states, when projected to individual fragments, are either local (LEs) or charge transfer excitons (CTEs). However, the canonical molecular orbitals (CMOs) obtained from a typical calculation tend to delocalize, which makes the subsequent analysis of excited states cumbersome. In this work, we report a simple approach to address this problem by employing localized molecular orbitals (LMOs) as linear combinations of the CMOs in the occupied and virtual subspaces separately after a self‐consistent field calculation. This separated linear combination ensures that configuration interaction singles (CIS), random phase approximation (RPA), and their corresponding density functional theory (DFT) counterparts [Tamm‐Dancoff approximation time‐dependent DFT (TDA‐TDDFT) and TDDFT] calculations with LMOs are mathematically equivalent to those performed with CMOs. We performed tests on simple symmetric and asymmetric dimer systems and found that the excited states are numerically identical in excitation energies and transition moments for both LMOs and CMOs, except for very few states that are only found in either LMO or CMO (in symmetric cases). The LMO basis makes both qualitative and quantitative analyses of the excited states much more accessible, as the extent of LE and CTE contributions can be easily defined. Consequently, this simple yet robust approach can be useful for characterizing excitons in multichromophoric systems and in condensed phases, which is useful when studying problems pertaining to electron/excitation energy transfer processes.</jats:p>},
keywords = {IT2067, MolEles-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:title>ABSTRACT</jats:title>
<jats:p>Excited states of systems composed of linked fragments or stacked molecules are important for understanding their optoelectronic properties. These states, when projected to individual fragments, are either local (LEs) or charge transfer excitons (CTEs). However, the canonical molecular orbitals (CMOs) obtained from a typical calculation tend to delocalize, which makes the subsequent analysis of excited states cumbersome. In this work, we report a simple approach to address this problem by employing localized molecular orbitals (LMOs) as linear combinations of the CMOs in the occupied and virtual subspaces separately after a self‐consistent field calculation. This separated linear combination ensures that configuration interaction singles (CIS), random phase approximation (RPA), and their corresponding density functional theory (DFT) counterparts [Tamm‐Dancoff approximation time‐dependent DFT (TDA‐TDDFT) and TDDFT] calculations with LMOs are mathematically equivalent to those performed with CMOs. We performed tests on simple symmetric and asymmetric dimer systems and found that the excited states are numerically identical in excitation energies and transition moments for both LMOs and CMOs, except for very few states that are only found in either LMO or CMO (in symmetric cases). The LMO basis makes both qualitative and quantitative analyses of the excited states much more accessible, as the extent of LE and CTE contributions can be easily defined. Consequently, this simple yet robust approach can be useful for characterizing excitons in multichromophoric systems and in condensed phases, which is useful when studying problems pertaining to electron/excitation energy transfer processes.</jats:p>
<jats:p>Excited states of systems composed of linked fragments or stacked molecules are important for understanding their optoelectronic properties. These states, when projected to individual fragments, are either local (LEs) or charge transfer excitons (CTEs). However, the canonical molecular orbitals (CMOs) obtained from a typical calculation tend to delocalize, which makes the subsequent analysis of excited states cumbersome. In this work, we report a simple approach to address this problem by employing localized molecular orbitals (LMOs) as linear combinations of the CMOs in the occupied and virtual subspaces separately after a self‐consistent field calculation. This separated linear combination ensures that configuration interaction singles (CIS), random phase approximation (RPA), and their corresponding density functional theory (DFT) counterparts [Tamm‐Dancoff approximation time‐dependent DFT (TDA‐TDDFT) and TDDFT] calculations with LMOs are mathematically equivalent to those performed with CMOs. We performed tests on simple symmetric and asymmetric dimer systems and found that the excited states are numerically identical in excitation energies and transition moments for both LMOs and CMOs, except for very few states that are only found in either LMO or CMO (in symmetric cases). The LMO basis makes both qualitative and quantitative analyses of the excited states much more accessible, as the extent of LE and CTE contributions can be easily defined. Consequently, this simple yet robust approach can be useful for characterizing excitons in multichromophoric systems and in condensed phases, which is useful when studying problems pertaining to electron/excitation energy transfer processes.</jats:p>
1.
Ding, Lexin; Matito, Eduard; Schilling, Christian
Chemical bonding concepts emerge naturally from maximally entangled atomic orbitals Journal Article
In: Nat Commun, vol. 17, no. 1, 0000, ISSN: 2041-1723.
Abstract | Links | BibTeX | Tags: IT2067, QCD-KT
@article{Ding2026,
title = {Chemical bonding concepts emerge naturally from maximally entangled atomic orbitals},
author = {Lexin Ding and Eduard Matito and Christian Schilling},
doi = {10.1038/s41467-026-73527-w},
issn = {2041-1723},
journal = {Nat Commun},
volume = {17},
number = {1},
publisher = {Springer Science and Business Media LLC},
abstract = {<jats:title>Abstract</jats:title>
<jats:p>Chemical bonding is a nonlocal phenomenon that binds atoms into molecules. Its ubiquitous presence in chemistry, however, stands in stark contrast to its ambiguous definition and the lack of a universal perspective for its understanding. In this work, we rationalize and characterize chemical bonding through the lens of an equally nonlocal concept from quantum information, the orbital entanglement. We introduce the maximally entangled atomic orbitals (MEAOs) whose entanglement pattern is shown to recover both Lewis (two-center) and beyond-Lewis (multicenter) structures, with multipartite entanglement serving as a comprehensive index of bond strength. Our unifying framework for bonding analyses is effective not only for equilibrium geometries but also for transition states in chemical reactions and complex phenomena such as aromaticity. It also has the potential to elevate the Hilbert space atomic partitioning to match the prevalent real-space partitioning in the theory of atoms in molecules. Accordingly, our work provides a new framework for understanding fuzzy chemical concepts using rigorous, quantitative descriptors from quantum information.</jats:p>},
keywords = {IT2067, QCD-KT},
pubstate = {published},
tppubtype = {article}
}
<jats:title>Abstract</jats:title>
<jats:p>Chemical bonding is a nonlocal phenomenon that binds atoms into molecules. Its ubiquitous presence in chemistry, however, stands in stark contrast to its ambiguous definition and the lack of a universal perspective for its understanding. In this work, we rationalize and characterize chemical bonding through the lens of an equally nonlocal concept from quantum information, the orbital entanglement. We introduce the maximally entangled atomic orbitals (MEAOs) whose entanglement pattern is shown to recover both Lewis (two-center) and beyond-Lewis (multicenter) structures, with multipartite entanglement serving as a comprehensive index of bond strength. Our unifying framework for bonding analyses is effective not only for equilibrium geometries but also for transition states in chemical reactions and complex phenomena such as aromaticity. It also has the potential to elevate the Hilbert space atomic partitioning to match the prevalent real-space partitioning in the theory of atoms in molecules. Accordingly, our work provides a new framework for understanding fuzzy chemical concepts using rigorous, quantitative descriptors from quantum information.</jats:p>
<jats:p>Chemical bonding is a nonlocal phenomenon that binds atoms into molecules. Its ubiquitous presence in chemistry, however, stands in stark contrast to its ambiguous definition and the lack of a universal perspective for its understanding. In this work, we rationalize and characterize chemical bonding through the lens of an equally nonlocal concept from quantum information, the orbital entanglement. We introduce the maximally entangled atomic orbitals (MEAOs) whose entanglement pattern is shown to recover both Lewis (two-center) and beyond-Lewis (multicenter) structures, with multipartite entanglement serving as a comprehensive index of bond strength. Our unifying framework for bonding analyses is effective not only for equilibrium geometries but also for transition states in chemical reactions and complex phenomena such as aromaticity. It also has the potential to elevate the Hilbert space atomic partitioning to match the prevalent real-space partitioning in the theory of atoms in molecules. Accordingly, our work provides a new framework for understanding fuzzy chemical concepts using rigorous, quantitative descriptors from quantum information.</jats:p>