Here's my thoughts and personal experience. I don't know how I'm supposed to format this for clarity... but here we go.
Cooling and Possible Heat Savings
The cooler definitely explains a lot. That is your personal preference though. Since you're running it 100% 24/7 it would still be loud with a liquid setup if you don't have adequate A/C in the room. The heat has to go somewhere. You're basically just limiting the setup by dB, which is limiting stability by heat/wattage.
You could be getting errors from too much heat from the Memory. I'm not sure what kit your using, I thought I saw it in the thread somewhere, but I don't see it now. I feel like 1.5v should not be needed for 3600mhz, that is really going to depend on your Memory kit though. I think memory starts throwing errors at 50c. You can get something like HWiNFO64 to monitor all kinds of parameters of the system, including Memory. Although I think monitoring software sometimes messes with Ryzen Master (or vice-versa?) last time I checked since they poll on the same sensors.
You can probably save some CPU heat/wattage headroom by turning down that Vsoc voltage. Have you tested Vsoc at 1.1 or 1.12? It won't save much at idle, but it will be by a significant amount at load. I am not gaining any stability by using 1.2 vs 1.1 on the newest BIOS w/ Agesa 1.2.0.7. If you end up saving a lot of heat from turning down Vsoc you may be able to increase your CPU clocks, raising Vcore if needed since you would now have more heat headroom.
The same actually goes for your Vcore, it seems you've done your fiddling, but if you don't actually throw any errors with less voltage, you might as well turn the Vcore down more too.
FYI, if you update BIOS, you will want to test all of your new limits and stability since it's pretty common to have performance changes with updated BIOS.
Side note about Gear Down Mode (GDM)
Memory has a setting called Gear Down Mode (GDM), GearDownEn in Ryzen Master from your initial picture. This setting will raise certain odd numbered timings, your CL15, to an even number, CL16. So I'm not sure if you realized this yet, but your Ryzen Master picture actually shows CL16. You would only be able to go to CL14 with GDM enabled. It is notoriously hard to turn GDM off successfully since it is a setting that adds stability to the Memory during specific Memory operations by using 2 clock cycles instead of 1, hence the need to have an even CL as well as a couple other timings that I'm not 100% sure of.
Overclocking 5000 Series Ryzen
As far as manual overclocking goes, it's not really much different from past Ryzen CPUs and is highly dependent on what your BIOS allows you to change. Your setup is still just limited by heat. Most of the "OC" guides you will find for 5000 series, and even 3000 series are how to set PBO and Curve Optimizer settings, and/or how great the out-of-the-box algorithm is and to just leave everything on auto. I'm pretty sure PBO settings are just limits for amps and watts that the automatic algorithm uses to determine your power/heat limits anyways, and yours appear to just be set to the motherboard limits.
Here are the current methods I see people using to OC that you can find general instructions for pretty easily:
Manual OC
Manually find and set the highest stable (no crashing or errors during stress testing) clock speed at the voltages you can adequately cool to prevent throttling. Basically what you're already doing. You can potentially get even more performance out of this option if you clock your CCD's individually. Ex. One of my CCD's cores will all do 4850mhz under load just fine, but the other CCD has 2 cores that only boost to 4700mhz without crashing. So if I set an all-core overclock it is capped at 4700mhz on the current BIOS. Unfortunately I can't set per-core clock and voltages or I'd have at least 3 cores set to 4975mhz

.
CTR 2.1
Use the program VPII recommended (CTR 2.1) to automatically find optimized settings for the on-board algorithm to use. This software will even change settings on-the-fly based on load, you would probably want to disable this auto profile switching feature and just run whatever profile it gives you for the best all-core workload though. You can do all of this manually with PBO settings and Curve Optimizer, but there's really no need to waste your time, just use the program if you choose this route.
Note. CTR 2.1 might be better than Manual OC for tasks that don't require all of your cores since the cores that can boost higher will boost higher, but from all my testing the actual average speed of all cores will be lower than a manual OC... If it's worth your time I would try both and see which one works better with your program.
Curve Optimizer?
Pretty much the manual version of using CTR 2.1 from above.
Here's a simple overview because I don't know every aspect of tweaking AMD's algorithm, but it works ok as an "Auto" OC with a few wiggle-room settings for personalization.
-Leave CPU clock/Vcore on auto and adjust Curve Optimizer (CO) settings and max boost offset. These settings adjust a table(?) in the boost algorithm that says "Use ____ volts when going ____ghz". If you set a negative offset for the Curve Optimizer it will result in less heat which results in a higher frequency because it's pretty much a feedback loop and boosts higher if cooler, to a point. The cores themselves will still only boost to a safe clock, for that specific core, for the workload. At a certain point the core just won't boost any higher. You can also set this too much into the negative and lose stability because the voltage ends up being too low to sustain the boosted frequency. This setting also only goes to a value of 30, so some cores might be able to handle lower voltages, but the algorithm only allows you to offset it by so much. I'm also not sure what the actual value of this setting stands for, is -30 = -.03v? IDK.
PBO settings adjust your power limits. Not sure if they can be used to add more of an undervolt in conjunction with the Curve Optimizer or what else the PBO settings would even be good for OC'ing-wise.
Note: Curve Optimizer will do nothing if you're running a set clock and voltage because you've manually overwritten clock and voltage settings at that point.
I'm 99.99% sure that not everything written here is 100% correct, so it's best to do your own research. But I tried, and hopefully something in here helps. It was fun to write it up either way.