Self-starting nonlinear mode-locking in random lasers

In ultra-fast multi-mode lasers, mode-locking is implemented by means of ad hoc devices, like saturable absorbers or modulators, allowing for very short pulses. This comes about because of nonlinear interactions induced among modes at different, well equispaced, frequencies. Theory predicts that the same locking of modes would occur in random lasers but, in absence of any device, its detection is unfeasible so far. Because of the general interest in the phenomenology and understanding of random lasers and, moreover, because it is a first example of self-starting mode-locking we devise and test a way to measure such peculiar non-linear coupling. Through a detailed analysis of multi-mode correlations we provide clear evidence for the occurrence of nonlinear mode-coupling in the cavity-less random laser made of a powder of GaAs crystals and its self-starting mode-locking nature. The behavior of multi-point correlations among intensity peaks is tested against the nonlinear frequency matching condition equivalent to the one underlying phase-locking in ordered ultrafast lasers. Non-trivially large multi-point correlations are clearly observed for spatially overlapping resonances and turn out to sensitively depend on the frequency matching being satisfied, eventually demonstrating the occurrence of non-linear mode-locked mode-coupling.