We perform general-relativistic hydrodynamical simulations of dynamical capture binary neutron star mergers, emphasizing the role played by the neutron star spin. Dynamical capture mergers may take place in globular clusters, as well as other dense stellar systems, where most neutron stars have large spins. We find significant variability in the merger outcome as a function of initial neutron star spin. For cases where the spin is aligned with the orbital angular momentum, the additional

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... ugal support in the remnant hypermassive neutron star can prevent the prompt collapse to a black hole, while for antialigned cases the decreased total angular momentum can facilitate the collapse to a black hole. We show that even moderate spins can significantly increase the amount of ejected material, including the amount unbound with velocities greater than half the speed of light, leading to brighter electromagnetic signatures associated with kilonovae and interaction of the ejecta with the interstellar medium. Furthermore, we find that the initial neutron star spin can strongly affect the already rich phenomenology in the postmerger gravitational wave signatures that arise from the oscillation modes of the hypermassive neutron star. In several of our simulations, the resulting hypermassive neutron star develops the one-arm (m=1) spiral instability, the most pronounced cases being those with small but non-negligible neutron star spins. For long-lived hypermassive neutron stars, the presence of this instability leads to improved prospects for detecting these events through gravitational waves, and thus may give information about the neutron star equation of state.