Ultrafast Charge Transfer and Delayed Recombination in Graphitic-CN/WTe₂ van der Waals Heterostructure: A Time Domain...

In search of an efficient solar energy harvester, we herein performed a time domain density functional study coupled with nonadiabatic molecular dynamics (NAMD) simulation to gain atomistic insight into the charge carrier dynamics of a graphitic carbon nitride (g-CN)-tungsten telluride (WTe₂) van der Waals heterostructure. Our NAMD study predicted ultrafast electron (589 fs) and hole-transfer (807 fs) dynamics in g-CN/WTe₂ heterostructure and a delayed electron-hole recombination process (2.404 ns) as compared to that of the individual g-CN (3 ps) and WTe₂ (0.55 ps) monolayer. The ultrafast charge transfer is due to strong electron-phonon coupling during the charge-transfer process while comparatively weak electron-phonon coupling, sufficient band gap, comparatively lower nonadiabatic coupling (NAC), and fast decoherence time slow down the electron-hole recombination process. The NAMD results of exciton relaxation dynamics are valuable for insightful understanding of charge carrier dynamics and in designing photovoltaic devices based on organic-inorganic 2D van der Waals heterostructures.