I find the time when the sun begins to set is the BEST time to take pictures with available outdoor light. Generally that is true for all outdoor shots, but I feel that for portraits it is especially so because it gives the pictures a golden look. Everything becomes warm and pleasing.
Both images taken with a Nikon D700 and a Nikon 24-70mm f/2.8G ED-IF AF-S
f/5.0, 1/80, ISO 400

f/5.0, 1/80, ISO400
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