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With silicone the proper way is to first wipe the surfaces clean with acetone. Then apply a thick bead of silicone making sure it sticks to both surfaces with no gaps (very important), doesn't need to look pretty. After that you spray it with soapy water which prevents it from sticking where you don't want it to and then use a wet/soapy popsicle stick (or a dedicated tool) to scrape off the excess. After that you can spray it again and super gently pull your finger over it to smooth it out. Should come out looking something like this.
I've gotten good results doing caulking like this aswell but some people say that acrylic caulk may react with the water/soap and you should instead use a dedicated tooling agent.