An Investigation of Photo‐ and Pressure‐Induced Effects in a Pair of Isostructural Two‐Dimensional Spin‐Crossover Framework Materials
Identifieur interne : 003E54 ( Main/Exploration ); précédent : 003E53; suivant : 003E55An Investigation of Photo‐ and Pressure‐Induced Effects in a Pair of Isostructural Two‐Dimensional Spin‐Crossover Framework Materials
Auteurs : Natasha F. Sciortino [Australie] ; Suzanne M. Neville [Australie] ; Cédric Desplanches [France] ; Jean-François Létard [France] ; Victor Martinez [Espagne] ; José Antonio Real [Espagne] ; Boujemaa Moubaraki [Australie] ; Keith S. Murray [Australie] ; Cameron J. Kepert [Australie]Source :
- Chemistry – A European Journal [ 0947-6539 ] ; 2014-06-10.
Abstract
Two new isostructural iron(II) spin‐crossover (SCO) framework (SCOF) materials of the type [Fe(dpms)2(NCX)2] (dpms=4,4′‐dipyridylmethyl sulfide; X=S (SCOF‐6(S)), X=Se (SCOF‐6(Se))) have been synthesized. The 2D framework materials consist of undulating and interpenetrated rhomboid (4,4) nets. SCOF‐6(S) displays an incomplete SCO transition with only approximately 30 % conversion of high‐spin (HS) to low‐spin iron(II) sites over the temperature range 300–4 K (T1/2=75 K). In contrast, the NCSe− analogue, SCOF‐6(Se), displays a complete SCO transition (T1/2=135 K). Photomagnetic characterizations reveal quantitative light‐ induced excited spin‐state trapping (LIESST) of metastable HS iron(II) sites at 10 K. The temperature at which the photoinduced stored information is erased is 58 and 50 K for SCOF‐6(S) and SCOF‐6(Se), respectively. Variable‐pressure magnetic measurements were performed on SCOF‐6(S), revealing that with increasing pressure both the T1/2 value and the extent of spin conversion are increased; with pressures exceeding 5.2 kbar a complete thermal transition is achieved. This study confirms that kinetic trapping effects are responsible for hindering a complete thermally induced spin transition in SCOF‐6(S) at ambient pressure due to an interplay between close T1/2 and T(LIESST) values.
Url:
DOI: 10.1002/chem.201400367
Affiliations:
- Australie, Espagne, France
- Aquitaine, Nouvelle-Aquitaine, Nouvelle-Galles du Sud
- Bordeaux, Sydney
- Université Bordeaux I, Université de Bordeaux, Université de Sydney
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The 2D framework materials consist of undulating and interpenetrated rhomboid (4,4) nets. SCOF‐6(S) displays an incomplete SCO transition with only approximately 30 % conversion of high‐spin (HS) to low‐spin iron(II) sites over the temperature range 300–4 K (T1/2=75 K). In contrast, the NCSe− analogue, SCOF‐6(Se), displays a complete SCO transition (T1/2=135 K). Photomagnetic characterizations reveal quantitative light‐ induced excited spin‐state trapping (LIESST) of metastable HS iron(II) sites at 10 K. The temperature at which the photoinduced stored information is erased is 58 and 50 K for SCOF‐6(S) and SCOF‐6(Se), respectively. Variable‐pressure magnetic measurements were performed on SCOF‐6(S), revealing that with increasing pressure both the T1/2 value and the extent of spin conversion are increased; with pressures exceeding 5.2 kbar a complete thermal transition is achieved. This study confirms that kinetic trapping effects are responsible for hindering a complete thermally induced spin transition in SCOF‐6(S) at ambient pressure due to an interplay between close T1/2 and T(LIESST) values.</div></front></TEI><affiliations><list><country><li>Australie</li><li>Espagne</li><li>France</li></country><region><li>Aquitaine</li><li>Nouvelle-Aquitaine</li><li>Nouvelle-Galles du Sud</li></region><settlement><li>Bordeaux</li><li>Sydney</li></settlement><orgName><li>Université Bordeaux I</li><li>Université de Bordeaux</li><li>Université de Sydney</li></orgName></list><tree><country name="Australie"><region name="Nouvelle-Galles du Sud"><name sortKey="Sciortino, Natasha F" sort="Sciortino, Natasha F" uniqKey="Sciortino N" first="Natasha F." last="Sciortino">Natasha F. Sciortino</name></region><name sortKey="Kepert, Cameron J" sort="Kepert, Cameron J" uniqKey="Kepert C" first="Cameron J." last="Kepert">Cameron J. Kepert</name><name sortKey="Kepert, Cameron J" sort="Kepert, Cameron J" uniqKey="Kepert C" first="Cameron J." last="Kepert">Cameron J. Kepert</name><name sortKey="Kepert, Cameron J" sort="Kepert, Cameron J" uniqKey="Kepert C" first="Cameron J." last="Kepert">Cameron J. Kepert</name><name sortKey="Moubaraki, Boujemaa" sort="Moubaraki, Boujemaa" uniqKey="Moubaraki B" first="Boujemaa" last="Moubaraki">Boujemaa Moubaraki</name><name sortKey="Murray, Keith S" sort="Murray, Keith S" uniqKey="Murray K" first="Keith S." last="Murray">Keith S. Murray</name><name sortKey="Neville, Suzanne M" sort="Neville, Suzanne M" uniqKey="Neville S" first="Suzanne M." last="Neville">Suzanne M. 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