What time of day do you think is the best time to take natural light photos?
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depends upon the subject. Around sunset and sunrise are called "the golden hour" because most people like that "feel". Of course, that time varies depending upon where you are and what season it is.
Facetious answer: any time you're getting paid for it! Sensible answer: entirely depends on the kind of look you want. Like Vasco says golden hour (aka Magic Hour) has a very pretty, almost ethereal look. The film "Heaven's Gate" shot extensively during magic hour. Also depends on the time of year and your geographic location. I live in the UK and I love late afternoon sunlight in the winter. Long shadows, golden/apricot-y colour, simply gorgeous. Bear in mind that if shooting around noon in the summer when the sun is directly overhead is very unflattering to faces. Movies shooting in these conditions (like most westerns) use a large overhead silk to soften the light on actors faces. Or you can place your subject under shade. Ultimately, your best bet is to take test photos at different times of the day (or even the year if you have that luxury) and learn how it looks in all these conditions. Hope that rather lengthy answer helps!
Sunrise, sunset, after sunset are all great for people plus things. Also good for cars on flat terrain ( desert / beach). Scenic shots and architecture can be good - or bad - any time of day. Depends on perspective and how the shadows fall. Overcast days change it all- so do fog. High noon especially summer is best avoided for people, unless you LIKE the wedding scene in The Godfather .... Raccoon eye shadows will be unattractive. All this assumes you have no grip package to silk / reflect / modify existing light.
There is a reason so any commercials shoot outside at sunrise and sunset. The golden low hard light makes everything look great.
The time of day depends on color temperature & mood your trying to set. 1000 - 1400 or indoor lighting for regular day shots with no particular mood, sunrise & sunset for romance or awakening, dusk & dawn for a sense of urgency, darkness for suspense or horror.
The final hours before the sun goes down? Or so I've heard.