If we were talking about AM I would assume you mean the audio signal isn't bandlimited and so high-frequency audio components get upconverted by the carrier frequency, but I don't know what the spectrum of an FM signal looks like. Are we talking about a broad comb that results in an analogous way from sudden changes in the frequency? Do they go away if you vary the frequency of a 50%-duty-cycle square wave smoothly, like maybe with second- or third-order continuity, instead of suddenly?
see https://en.wikipedia.org/wiki/Phase_noise
It's surprisingly difficult to generate a clean carrier which doesn't have a broad band of spectral components, but this is essential for the design of effective Receivers and Transmitters.
These sidebands are generated by noise in the oscillator, spurs caused by mixing products, jitter in the synthesiser, and non-linearities in the modulation process.
The bottom line is to look at the output with a high-quality spectrum analyser and compare the result with the spectral mask which is published by the FCC.
He doesn't seem to be using a mixer, so I don't think you'll get any spurs caused by mixing products in this case.
I'm no expert obviously but I'd think the phase noise of a PLL driven from a quartz crystal would be negligible.
That makes it do some weired things - and I suspect one of those is that when adjusting the clock frequency (by changing the divisors), sometimes it stops oscillating for many microseconds.
Not sure what impact that has in the frequency domain, but I can't imagine it's good...
But that is before we get to the modulation. That again will be digital (rather than analog) so by definition will be chock full of jitter, especially if the FM is generated by stepping the clock frequency in finite steps. Not only will this generate large amounts of jitter, but it will generate spurs of the PWM clock over a wide range of frequencies.
While it's relatively easy to remove harmonics, it is pretty much impossible to remove the broad comb of spurious signals either side of the carrier.
Which why transmitters are not designed this way in the real world.