Diabatic Hamiltonian construction in van der Waals heterostructure complexes

Abstract

A diabatization method is developed for the approximated description of the photoinduced charge separation/transfer processes in the van der Waals (vdW) heterostructure complex, which is based on the wavefunction projection approach using a plane wave basis set in the framework of the single-particle picture. We build the diabatic Hamiltonian for the description of the interlayer photoinduced hole-trans fer process of the two-dimensional vdW MoS2/WS2 heterostructure complexes. The diabatic Hamiltonian gives the energies of the localized valence band states (located at MoS2 and valence band states (located at WS2), as well as the couplings between them.The wavefunction projection method provides a practical and reasonable approach to construct the diabatic model in the description of photoinduced charge transfer processes in the vdW heterostructure complexes.

The direct Z-scheme character and roles of S vacancy in BiOCl/Bi2S3-(001) heterostructures for superior photocatalytic activity: a hybrid density functional investigation

“…[7][8][9] Among these methods, constructing a heterostructure with other semiconductors is considered the most promising and popular method for enhancing its photocatalytic efficiency. [10][11][12][13] For example, another significant Bi-based semiconductor photocatalyst Bi 2 S 3 (space group Pbnm (#62)) was adopted to build BiOCl/Bi 2 S 3 heterostructures by many experimental working groups, [2][3][4][5][6][14][15][16][17][18] in order to enhance the photocatalytic activities of both BiOCl and Bi 2 S 3 . One important reason is that Bi 2 S 3 has a narrow band gap of 1.33-1.70 eV that can strongly absorb visible light, 5,14 also has a layered structure, and complements the larger band gap of BiOCl when BiOCl and Bi 2 S 3 are coupled to form a heterostructure.…”

Improved nitrogen reduction activity of NbSe2 tuned by edge chirality

“…8,[17][18][19] Due to the versatile physical and chemical properties of transition metal dichalcogenides, this family of materials attracted tremendous interest in the catalysis community. 18,[20][21][22][23] For instance, Nb-based compounds have been considered as efficient NRR catalysts, where the partially occupied d-orbitals of Nb 4+ cations provide empty states for strong N 2 adsorption and activate the N 2 triple bond with the back donation mechanism. 24 Skúlason et al predicted that the limiting potential of the (110) facet of NbO 2 (À0.57 V) would be much lower than that of the Ru(0001) step surfaces (À1.08 V), 25,26 where the latter has been widely adopted as a reference system for NRR.…”

Resonant Charge Transport Assisted by the Molecular Vibration in Single-Molecule Junction from Time-Domain ab initio Nonadiabatic Molecular Dynamics Simulations

“…In recent decades, the nonadiabatic molecular dynamics (NAMD) simulation approach, which combines the time-dependent Kohn-Sham (TDKS) equation with the surface hopping scheme and ab initio molecular dynamics, has been rapidly developed. [36][37][38][39][40][41][42][43][44][45][46][47] It accounts for electronvibration coupling in the real-time domain and has been applied to many different materials to understand the photoexcited carrier dynamics. [48][49][50][51][52] In this Letter, we use the time-domain NAMD approach to simulate the real-time electron transport dynamics in a single-molecule device.…”