New data are reported from the operation of the PICO-60 dark matter detector, a bubble chamber filled with 36.8 kg of CF$_3$I and located in the SNOLAB underground laboratory. PICO-60 is the largest bubble chamber to search for dark matter to date. With an analyzed exposure of 92.8 livedays, PICO-60 exhibits the same excellent background rejection observed in smaller bubble chambers. Alpha decays in PICO-60 exhibit frequency-dependent acoustic calorimetry, similar but not identical to that reported recently in a C$_3$F$_8$ bubble chamber. PICO-60 also observes a large population of unknown background events, exhibiting acoustic, spatial, and timing behaviors inconsistent with those expected from a dark matter signal. These behaviors allow for analysis cuts to remove all background events while retaining $48.2%$ of the exposure. Stringent limits on weakly interacting massive particles interacting via spin-dependent proton and spin-independent processes are set, and most interpretations of the DAMA/LIBRA modulation signal as dark matter interacting with iodine nuclei are ruled out.
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