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[Fe(pic)3]Cl2·EtOH (pic = 2-picolylamine) is a spin-crossover compound that can be converted from the low-spin state to the high-spin state at temperatures below the thermal transition temperature by way of light irradiation in the visible part of the electromagnetic spectrum. For this compound, the question regarding the quantum efficiency of this photoconversion process and its possible dependence on irradiation intensity gave rise to some controversy. The experimental results presented in this paper demonstrate that the quantum efficiency of the photoconversion at 11 K is on the order of unity, with no noticeable dependence on irradiation intensity. It does, however, depend to some extent on the fraction of complexes already converted to the high-spin state. ENACHESCU, Cristian, OETLIKER, Ulrich, HAUSER, Andreas. Photoexcitation in the Spin-Crossover Compound [Fe(pic)3]Cl2·EtOH (pic = 2-Picolylamine). Journal of Physica