TY - JOUR
T1 - Cu-based metalorganic systems
T2 - An ab initio study of the electronic structure
AU - Salguero, L. Andrea
AU - Jeschke, Harald O.
AU - Rahaman, Badiur
AU - Saha-Dasgupta, Tanusri
AU - Buchsbaum, Christian
AU - Schmidt, Martin U.
AU - Valentí, Roser
PY - 2007/2/13
Y1 - 2007/2/13
N2 - Within a first principles framework, we study the electronic structure of the recently synthesized polymeric coordination compound Cu(II)-2,5-bis(pyrazol- 1-yl)-1,4-dihydroxybenzene (CuCCP), which has been suggested to be a good realization of a Heisenberg spin-1/2 chain with antiferromagnetic coupling. By using a combination of classical with ab initio quantum mechanical methods, we design on the computer reliable modified structures of CuCCP aimed at studying effects of Cu-Cu coupling strength variations on this spin-1/2 system. For this purpose, we performed two types of modifications on CuCCP. In one case, we replaced H in the linker by (i) an electron donating group (NH 2) and (ii) an electron withdrawing group (CN), while the other modification consisted of adding H 2O and NH 3 molecules in the structure which change the local coordination of the Cu(II) ions. With the Nth order muffin tin orbital (NMTO) downfolding method, we provide a quantitative analysis of the modified electronic structure and the nature of the Cu-Cu interaction paths in these new structures and discuss its implications for the underlying microscopic model.
AB - Within a first principles framework, we study the electronic structure of the recently synthesized polymeric coordination compound Cu(II)-2,5-bis(pyrazol- 1-yl)-1,4-dihydroxybenzene (CuCCP), which has been suggested to be a good realization of a Heisenberg spin-1/2 chain with antiferromagnetic coupling. By using a combination of classical with ab initio quantum mechanical methods, we design on the computer reliable modified structures of CuCCP aimed at studying effects of Cu-Cu coupling strength variations on this spin-1/2 system. For this purpose, we performed two types of modifications on CuCCP. In one case, we replaced H in the linker by (i) an electron donating group (NH 2) and (ii) an electron withdrawing group (CN), while the other modification consisted of adding H 2O and NH 3 molecules in the structure which change the local coordination of the Cu(II) ions. With the Nth order muffin tin orbital (NMTO) downfolding method, we provide a quantitative analysis of the modified electronic structure and the nature of the Cu-Cu interaction paths in these new structures and discuss its implications for the underlying microscopic model.
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U2 - 10.1088/1367-2630/9/1/001
DO - 10.1088/1367-2630/9/1/001
M3 - Article
AN - SCOPUS:33847048183
VL - 9
JO - New Journal of Physics
JF - New Journal of Physics
SN - 1367-2630
M1 - A26
ER -