Modeling of laser-pulse induced water decomposition on two-dimensional materials by simulations based on time-dependent density functional theory

Physical Review B 96, 115451 (2017)

Modeling of laser-pulse induced water decomposition on two-dimensional materials by simulations based on time-dependent density functional theory

Yoshiyuki Miyamoto,Hong Zhang,Xinlu Cheng, Angel Rubio

We use time-dependent density functional theory to study laser-pulse induced decomposition vofH2Omolecules above the two-dimensional (2D) materials graphene, hexagonal boron nitride, and graphitic carbon nitride. We examine femtosecond-laser pulses with a full width at half maximum of 10 or 20 fs for laser-field intensity and wavelengths of 800 or 400 nm by varying the intensity of the laser field from 5 to 9 V/A° , with the corresponding range of fluence per pulse up to 10.7 J/cm2. For a H2O molecule above the graphitic sheets, the threshold for laser-field H2O decomposition is reduced by more than 20% compared with that of an isolated H2O molecule.We also show that hole doping enhances the water adsorption energy above graphene. The present results indicate that the graphitic materials should support laser-induced chemistry and that other 2D materials that can enhance laser-induced H2O decomposition should be investigated.

Additional Information

Doi
http://dx.doi.org/10.1103/PhysRevB.96.115451
Notes
Calculations were performed with the Parallel Computing System, AIST; the High-Performance Computing System of the Cybermedia Center, Osaka University; and the Cyberscience Center, Tohoku University. Y.M. thanks M. Kakehata for discussions about the experimental accessibility of current femtosecond lasers and acknowledges funding from JSPS KAKENHI Grants No. JP16H00925, No. JP16H04103, and No. JP16K05049. Y.M. also acknowledges support from the Research Organization of Information Science and Technology (RIST), Tokyo. H.Z. and X.C. acknowledge financial support from the National Key R&D Program of China 2017YFA0303603 and the National Natural Science Foundation of China (Grants No. 11474207 and No. 11374217). A.R. acknowledges financial support from the JSPS Fellowship program and from the European Research Council (QSpec- NewMat ERC-2015-AdG-694097) and Grupos Consolidados (IT578-13).

Related Projects

Related Research Areas