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New strings for my fretless single coil?

TI Jazz Rounds. They’re absolutely amazing on fretless.
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I use Chromes a lot and also TIs. I have one bass with labella DTFs too. I do usually prefer the TIs on a fretless, but I am going for a more modern or round sound. As for traditional flats I am very happy with the chromes and I am not sure you will find a cure with a string change, except maybe the TI flats.
Have you played with the pickup height?
 
If you want strings that are not stiff and you want "bright and articulate" why are you even looking at flats? Since it's fretless you can use round wounds without concern about fret clank.

TI Jazz Flats are far less stiff and more articulate than most roundwounds. In fact, the main complaint about these strings is that they aren't stiff enough.
 
Another plus with the TI Jazz Flats is that unlike most other flats they don't really need a break-in period (maybe a day or two to get rid of the TINY bit of metallic brightness you get with a fresh set).
 
In that case I think the TI Jazz Flats could be a perfect match, as long as you can handle the supple feel and low tension. This is a matter of personal taste. Some people love them, others make references to wet noodles...

I think that I would probably like these better on a fretted instrument though.

When I heard that the Ernie Ball Group III was a bit more flexible than the Chromes, and hearing them sound like the tone in my head, I had to go with those for now.

The main problem with the Chromes is that they lose their tone as they age.
 
I wouldn't put too much stock into youtube sound samples. It has been my experience that a certain brand/gauge of string may sound just "meh" on one instrument, but sound great on another. You just have to bite the bullet and try them all for yourself on your own gear. (Plus we all have our own preference for "good" tone.)
 
It's been a while since I went down the flatwound hole, but I spend a good bit of time with most of the strings being discussed. Since the OP has already bought some Ernie Balls (good choice), I'll be briefish.

First on a fretted jazz. I LOVED the tone of Fender flats and so did the people I was playing with at the time. But, the stuffness got to me aver time and I had some issues with the neck that may or may not have been related... let's go with "not".

A experimented with a bunch of alternatives and landed on EB. I tried a few of the groups/gauges. Don't remember where I landed,. The EB's were most of what I loved about the Fenders, but felt less stiff and more manageable.

I spend a couple of years with a fretless P-Bass and the EB's we're great on it too, but I wasn't through fooling around so I spent most of a year with TIs followed by LaBellas.

I liked everything. I didn't find TIs "weird" or "noodley" or any of the other things that people here warned me about. I was using that bass for pretty low volume jazz, I might have noticed more if I was trying to rock out on them though.

From what I remember, the LaBellas didn't stand out to me. Nothing I didn't like a out them. They were good strings similar to Ernie Balls.

I think you made a good choice.