Basic ideas to try
I have a few comments, but I do not keep Tiger Barbs so this is sort of general.
First, invest in more plants and decor. As you noticed the chasing is likely to end when the aggressor looses sight of the one he's after.
Then, go on and get several more tiger barbs, like 4 or 6, to add to this tank at the same time. I ordinarily prefer to suggest keeping new fish in Quarantine, but this may be the exception. You need at least six, more is better. And you may yet have some losses.
Add all of these fish at once, and rearrange the tank at the same time. The dominant fish will be terribbly stressed by this, he may get ill. Here he had everything all under control, maybe even a female for his own control, now the tank is full of fish, running and hiding everywhere, the tiny despot is toppled. When you add one or two at a time, he can destroy them, but adding 6 or 7 will totally overwhelm him. He will spend all his time trying to get everyone back in line, but they all look alike and keep running away, he can't concentrate on any one fish long enough to kill him.
Now, I don't know how many you can fit in that tank. Tiger barbs are sort of bulky.
You may need to get rid of some of the other fish to fit in the size group you need for the barbs. Persoanlly, I'd keep the barbs and nothing else, but I like that sort of tank, it allows for more natural behavior IMO. Maybe one or two other fish that fit into a different niche, like a bottom dweller or top dweller, but no other midlevel fish.
Now there may be some preferences on males to females, my serpae tetras have 4 males and 2 females (just chance in the picking) With 4 males 3 of them spend their time strutting and sparring with each other, the other keeps the females hiding in the bushes. I'd just try to get some of each, don't pick just males.