Ultraviolet surface plasmon-mediated low temperature hydrazine decomposition

Conventional methods require elevated temperatures in order to dissociate high-energy nitrogen bonds in precursor molecules such as ammonia or hydrazine used for nitride film growth. We report enhanced photodissociation of surface-absorbed hydrazine (N2H4) molecules at low temperature by using ultraviolet surface plasmons to concentrate the exciting radiation. Plasmonic nanostructured aluminum substrates were designed to provide resonant near field concentration at lambda = 248 nm (5 eV), corresponding to the maximum optical cross section for hydrogen abstraction from N2H4. We employed nanoimprint lithography to fabricate 1mm X 1mm arrays of the resonant plasmonic structures, and ultraviolet reflectance spectroscopy confirmed resonant extinction at 248 nm. Hydrazine was cryogenically adsorbed to the plasmonic substrate in a low-pressure ambient, and 5 eV surface plasmons were resonantly excited using a pulsed KrF laser. Mass spectrometry was used to characterize the photodissociation products and indicated a 6.2X overall enhancement in photodissociation yield for hydrazine adsorbed on plasmonic substrates compared with control substrates. The ultraviolet surface plasmon enhanced photodissociation demonstrated here may provide a valuable method to generate reactive precursors for deposition of nitride thin film materials at low temperatures. (C) 2015 AIP Publishing LLC.