Molecular doping of monolayer MoS2 provides a great opportunity to modulate its electronic properties for the potential applications in high performance devices. Density functional theory computations are performed to investigate the charge transfer and electrostatic potential modulation upon the adsorption of pentacene molecule on the surface of MoS2 monolayer (ML). Theoretical calculations indicate that interfacial charge transfer is negligible between pentacene and 2H‐MoS2 ML while significant in the pentacene/1T‐MoS2 ML complex, which is attributed to the match of energy levels near the Fermi level in the latter case. Moreover, molecular doping of pentacene induces substantial structure changes of the substrate resulting in large adsorption energy, which helps stabilize the 1T‐MoS2 ML. Depending on different substrate phases and doping configurations, the interfacial dipole barrier and related work function of MoS2 ML may be modulated in a wide range of the order of about 1 eV. The findings therefore shed light on the possibility of developing the desired organic/inorganic complex for electrical and optoelectronic devices by molecular doping via charge transfer modulation and interface engineering.

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Recently a coherence controlled (CC) approach to nonadiabatic dynamics was proposed by one of the authors based on the mapping between the decomposed classical state space and different types of nuclear dynamics. Here we elaborate the state-space decomposition scheme and the corresponding state-space-to-dynamics mapping of the CC approach in a general high-dimensional framework. In the CC formalism, dynamical properties such as the full electronic matrix can be evaluated by means of the ensemble of trajectories in the active state space, which consists of single-state domains and coherence domains. The feasibility of the state space decomposition and related mappings and the performance of the CC approach are demonstrated by the implementation to benchmark problems of nonadiabatic molecular dynamics in condensed phase including the spin-boson model and the excitation energy transfer problem in photosynthesis. The results obtained from the CC approach are in reasonably good agreement with exact or benchmark calculations, and it is also shown that the CC approach satisfies the detailed balance approximately and is capable of efficiently describing condensed phase nonadiabatic molecular dynamics at reasonable accuracy.

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Prussian blue analogues (PBAs) as a promising high-voltage cathode material for aqueous zinc-ion batteries (ZIBs) are usually subjected to an ephemeral lifespan and low Coulombic efficiency due to the irreversible phase change and high Zn2+ insertion potential. Besides, Zn dendrites, H2 evolution reaction, and corrosion derived from a Zn anode interface remain huge challenges. Given this, a highly stable zinc hexacyanoferrate (KZnHCF) cathode together with a mixed concentrated electrolyte is prepared to realize a high-voltage and long-life aqueous ZIB, in which the mixed concentrated electrolyte consisting of 30 m KFSI + 1 m Zn­(CF3SO3)2 possesses a unique Zn2+ solvation sheath (Zn­(CF3SO3)0.3(FSI)3.1(H2O)2.6) that can not only stabilize the cathode interface and improve the Coulombic efficiency but also fundamentally solve the Zn anode interface issues. As a result, the aqueous KZnHCF/Zn battery achieves an ultralong life over 3000 cycles without any capacity decay even under a high discharge voltage of 1.78 V (vs Zn2+/Zn). Such extraordinary performance represents significant progress in aqueous PBA-based ZIBs. This work shares guidance to improve the performance of aqueous ZIBs through optimizing the electrolyte in tuning the stable operation of the cathode and the zinc anode.