Magnetic gaps in organic tri-radicals: From a simple model to accurate estimates
| العنوان: | Magnetic gaps in organic tri-radicals: From a simple model to accurate estimates |
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| المؤلفون: | Vincenzo Barone, Ivo Cacelli, Alessandro Ferretti, Giacomo Prampolini |
| المساهمون: | Barone, Vincenzo, Cacelli, Ivo, Ferretti, Alessandro, Prampolini, Giacomo |
| المصدر: | The Journal of chemical physics 146 (2017). doi:10.1063/1.4977598 info:cnr-pdr/source/autori:Barone V.; Cacelli I.; Ferretti A.; Prampolini G./titolo:Magnetic gaps in organic tri-radicals: From a simple model to accurate estimates/doi:10.1063%2F1.4977598/rivista:The Journal of chemical physics/anno:2017/pagina_da:/pagina_a:/intervallo_pagine:/volume:146 |
| سنة النشر: | 2017 |
| مصطلحات موضوعية: | Physics, 010304 chemical physics, Hubbard model, Physical and Theoretical Chemistry, Polyradicals, Band gap, General Physics and Astronomy, Electronic structure, Configuration interaction, 010402 general chemistry, 01 natural sciences, Quantum chemistry, 0104 chemical sciences, symbols.namesake, Quantum mechanics, 0103 physical sciences, symbols, Statistical physics, organic tri-radicals, Physical and Theoretical Chemistry, Ground state, Hamiltonian (quantum mechanics), Quantum, Polyradicals |
| الوصف: | The calculation of the energy gap between the magnetic states of organic poly-radicals still represents a challenging playground for quantum chemistry, and high-level techniques are required to obtain accurate estimates. On these grounds, the aim of the present study is twofold. From the one side, it shows that, thanks to recent algorithmic and technical improvements, we are able to compute reliable quantum mechanical results for the systems of current fundamental and technological interest. From the other side, proper parameterization of a simple Hubbard Hamiltonian allows for a sound rationalization of magnetic gaps in terms of basic physical effects, unraveling the role played by electron delocalization, Coulomb repulsion, and effective exchange in tuning the magnetic character of the ground state. As case studies, we have chosen three prototypical organic tri-radicals, namely, 1,3,5-trimethylenebenzene, 1,3,5-tridehydrobenzene, and 1,2,3-tridehydrobenzene, which differ either for geometric or electronic structure. After discussing the differences among the three species and their consequences on the magnetic properties in terms of the simple model mentioned above, accurate and reliable values for the energy gap between the lowest quartet and doublet states are computed by means of the so-called difference dedicated configuration interaction (DDCI) technique, and the final results are discussed and compared to both available experimental and computational estimates. |
| تدمد: | 1089-7690 |
| DOI: | 10.1063/1.4977598 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::47e1ee21f60e70576f24e32351e1e8d5 https://pubmed.ncbi.nlm.nih.gov/28298126 |
| Rights: | OPEN |
| رقم الانضمام: | edsair.doi.dedup.....47e1ee21f60e70576f24e32351e1e8d5 |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 10897690 |
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| DOI: | 10.1063/1.4977598 |