https://gcc.gnu.org/bugzilla/show_bug.cgi?id=112919

--- Comment #4 from Xi Ruoyao <xry111 at gcc dot gnu.org> ---
On LA664:

19970.709626     -falign-labels=4 -falign-functions=16 -falign-loops=64
-falign-jumps=16
19970.709626     -falign-labels=4 -falign-functions=32 -falign-loops=32
-falign-jumps=16
19976.028765     -falign-labels=4 -falign-functions=64 -falign-loops=32
-falign-jumps=16
19978.689398     -falign-labels=4 -falign-functions=8 -falign-loops=16
-falign-jumps=16
19997.333689     -falign-labels=4 -falign-functions=4 -falign-loops=32
-falign-jumps=32
20009.337691     -falign-labels=4 -falign-functions=32 -falign-loops=8
-falign-jumps=32
20009.337691     -falign-labels=4 -falign-functions=4 -falign-loops=32
-falign-jumps=16
20010.672359     -falign-labels=4 -falign-functions=64 -falign-loops=8
-falign-jumps=32
20050.795348     -falign-labels=4 -falign-functions=32 -falign-loops=8
-falign-jumps=64
20065.547455     -falign-labels=4 -falign-functions=64 -falign-loops=8
-falign-jumps=64

So it seems -falign-labels > 4 is just harming.  And interestingly a high
-falign-functions / -falign-jumps helps Coremark...

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