Cobalt Prussian blue analogues (Na x Co[Fe(CN)6] y ; x ∼ 4 y − 3 ) whose valences are close to Co 3 + and Fe 2 + show characteristic phase transitions triggered by cooperative charge transfer (CT) from Fe 2 + to Co 3 + . Here, we extended the cooperative CT to the entire region of sodium concentration ( 0 ≤ x ≤ 4 y − 2 ). We systematically investigated (1) upper ( T c u ) and lower ( T c l ) critical temperature, (2) variation of the [ Fe 2 + (CN)6] 4 − ([ Fe 3 + (CN)6] 3 − ) concentration, and (3) spectral weight ( I ET ) due to electron transfer from Fe 2 + to Co 3 + of thin films of Na x Co[Fe(CN)6]0.82 against x. In a wide x region from 0.00 to 0.57, we observed first-order phase transition triggered by the cooperative CT. The extended CT model reproduces the x-dependent behavior of the [FeII(CN)6] 4 − ([FeIII(CN)6] 3 − ) concentration and I ET , except for the high-x region above x ∼ 0.9 .
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