I've had trouble determining whether one timestamp falls between two others across tens of thousands of rows (with the polars team suggesting I use a massive cross product and filter -- which worked but excludes the memory requirement), whereas in pandas I was able to sort the timestamps and thereby only need to compare against the preceding / following few based on the index of the last match.
The other issue I've had with resampling is with polars automatically dropping time periods with zero events, giving me a null instead of zero for the count of events in certain time periods (which then gets dropped from aggregations). This has caught me a few times.
But other than that I've had good luck.