KD - It's extremely cool on MANY levels that the computing power of, say, the diminutive LF2XT is probably greater than the UNIVAC! In the grand scheme of things, that happened very quickly, and has produced wondrous things, which makes it easy sometimes to hope that computational speed could over-ride physical law. But alas, as always, there are the natural properties of materials. "Nature, to be commanded, must be obeyed" as the famous quote goes (damned if I remember who said it!).
So goes the presently designed LED.
In order to do what you're looking for (which actually sounds like a pretty cool idea BTW), we have to turn to different emitter materials and designs. Combining PWM with voltage regulation is exactly what a PWM driver already does. It allows a timed pulse of a pre-determined current to happen.
That certainly doesn't provide an easy answer, but hopefully it'll give the peace of mind of not wanting to force something against it's nature, and help with a perspective of looking toward different technologies to achieve your desired goal... one which some researcher may have already thought of, and is working towards!