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Résumé
The linear (χ(1)) and second-order nonlinear (χ(2)) optical properties of metal-organic frameworks (MOFs) have been evaluated and interpreted by employing the combined local field theory/charge embedding approach. Three MOFs have been selected, the isostructural bis{4-[2-(4-pyridyl)ethenyl]benzoato}-zinc(II) (PEB-Zn) and bis{4-[2-(4-pyridyl)ethenyl]benzoato}-cadmium(II) (PEB-Cd) and bis{4-[3-(4-pyridyl)ethenyl]benzoato}-cadmium(II) (PEB′-Cd). The simulations, employing the Møller-Plesset second-order perturbation theory level to describe the ion properties, conclude that (i) χ(2) of PEB-Zn (∼60 pm/V at 1064 nm) is about 10% larger than that of PEB-Cd, (ii) χ(2) of PEB′-Cd attains 100 pm/V at 1064 nm [i.e., twice more than that of PEB-Cd or an amplitude similar to that of the 4-(N,N-dimethylamino)-3-acetamidonitrobenzene (DAN) molecular crystal] and (iii) the change of crystal structure accompanying an increase of temperature from 173 to 298 K leads to a decrease of χ(2) by ca. 10%. For the isostructural PEB-Zn and PEB-Cd, the outcome of Kurtz-Perry SHG powder method has been simulated as a function of the grain size, demonstrating that differences between the two MOFs only show up for room temperature structures. A value of 1.29 was estimated for the PEB-Zn/PEB-Cd contrast ratio, in qualitative agreement with experiment (1.16). This work opens the way toward a theoretically based design of MOFs with outstanding second-order nonlinear optical responses. (Graph Presented).
langue originale | Anglais |
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Pages (de - à) | 6741-6749 |
Nombre de pages | 9 |
journal | Journal of Physical Chemistry C: Nanomaterials and interfaces |
Volume | 120 |
Numéro de publication | 12 |
Les DOIs | |
Etat de la publication | Publié - 31 mars 2016 |
Empreinte digitale
Examiner les sujets de recherche de « Second-Order Nonlinear Optical Susceptibilities of Metal-Organic Frameworks Using a Combined Local Field Theory/Charge Embedding Electrostatic Scheme ». Ensemble, ils forment une empreinte digitale unique.Projets
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PAI n°P7/05 - FS2: Systèmes supramoléculaires fonctionnels (PAI P7/05)
CHAMPAGNE, B., De Vos, D., Van der Auweraer, M., Jérôme, C., Lazzaroni, R., Marin, G., Jonas, A., Du Prez, F., Vanderzande, D., Van Tendeloo, G., Van Speybroeck, V., NENON, S. & STAELENS, N.
1/04/12 → 30/09/17
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Plateforme Technologique Calcul Intensif
Benoît Champagne (!!Manager)
Plateforme technologique Calcul intensifEquipement/installations: Plateforme technolgique