Gravitational-wave searches for subsolar-mass compact binaries have left a gap between the planetary-mass regime accessible to long-duration searches and the higher masses probed by conventional compact-binary analyses. We close this gap by searching for the inspiral of ultra-compact binaries with chirp masses – in LIGO O4ab data. Using the statistically robust BinaryGFH-v2 method, a time-frequency technique to search for rapidly evolving inspirals lasting minutes to hours, we cover this previously challenging parameter space with a computational cost of only CPU-hours, and find no significant candidates. We thus set 90% confidence upper limits on the binary merger-rate density, providing the first gravitational-wave constraints across this chirp-mass range. Assuming that primordial-black-hole binaries formed in the early Universe with no binary suppression (), these results provide the first gravitational-wave constraints on the primordial-black-hole \dmh fraction in this mass range, yielding upper limits with for equal-mass binaries with component masses – and asymmetric binaries with secondary masses – for a primary mass .

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