There's a simple three-step process I use
1: Think about when you'll be free to talk for a while.
2: Check if that's a good time to call
3: Call when you say you will with a few ideas for what to do
"I'll give you a call tomorrow night, is that a good time for you?"
"If I call you on Tuesday around noon, will you have time to talk?"
"I'm working on a big project for a client and won't have any free time until Thursday. Is Thursday afternoon a good time to call you?"
Being specific makes it clear that you're genuinely interested and following through establishes that you're reliable enough to do what you say you'll do. I'd take those two factors over an arbitrary balance between desperation and aloofness any day.
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