Effect of extreme pump pulse reshaping on intense terahertz emission in lithium niobate at multimilliJoule pump energies.

We report on terahertz (THz) generation via optical rectification in a room-temperature lithium niobate crystal under variable pump pulse durations, ranging from 100 to 300 fs, at 800 nm center wavelength. The efficiency for the process is predicted to have an order of magnitude increase when longer duration Fourier-limited pump pulses are used. Our results confirm this increase in efficiency, and we report a record 800 nm pump energy conversion efficiency of 0.35% with a saturation at >240  fs pulse duration. While promising, our findings show a series of key problems that must be overcome before the theoretical limit can be achieved, including the influence of the pump bandwidth broadening due to the cascaded nonlinearity taking place within the crystal.