If the cpu is consistently running at 80c or higher a better cooler might not be a bad idea. Typically a 212 evo is fine for mild overclocking but 4.6ghz is more at the upper end and more of a scenario for a more adequate cooler. You can try tightening the center knurled screw under the heatsink fins to try and increase contact pressure a bit to see if that helps. Otherwise despite being a good cooler for the money/design, it's still just a 4 heat pipe single fan cooler with a rating to handle up to 180w tdp.
My cpu runs a bit cooler at 4.6ghz with slightly higher vcore (1.284v) but it's being cooled by a dark rock pro 3. It has 7 heatpipes, 2 fans and is rated to 250w tdp. It tops out around 80-81c under p95 stress testing and in the mid/high 60's in games. 99% of the time even under full load it's under 70-75c.
I've got another 4690k with a mild overclock at 4.2ghz running lower temps, lower vcore with a 212 evo. That was before the cryorig h7 was released, had it been available I would have opted for that cooler.
It's also hard to get definitive temps from a stress test like real bench. It's good for a multicomponent full system stress test but due to the varied nature of all the tests the temps are erratic and all over the place. Try prime95 v26.6 with small fft's enabled for a steady state load to get an idea of your thermals. Ideally there wouldn't be more than a 10c spread between any two cores but there's no hard or fast rule or guarantee that there won't be more.
As it is the temps are showing a variation of only 12c overall and the times where you saw 80c on one core and only 65c on the fourth could have been during one of those moments where core one (0) was being stressed harder than the 4th core. That's typical of a normal real working load but why it's important to use something that places even steady load like p95.
http://www.tomshardware.com/forum/id-1800828/intel-temperature-guide.html