Opening Extra Transport Channels by Atomically Precise Doping in Gold Nanoclusters with Electronic Structure...

Area of Science:

• Materials Science
• Nanotechnology
• Computational Chemistry

Background:

• Electrode material and interface engineering are critical for charge transport in implantable devices.
• Silver electrodes offer high conductivity, while gold nanoclusters can modify interfaces.
• Atomically precise gold nanoclusters are emerging as promising interface modifiers.

Purpose of the Study:

• To investigate charge transport at nanocluster-electrode interfaces using model systems.
• To evaluate the impact of doping in gold nanoclusters on interfacial electronic structure and conductivity.
• To explore strategies for enhancing interfacial transport efficiency in electrode design.

Main Methods:

• Density functional theory-nonequilibrium Green's function (DFT-NEGF) calculations.
• Neuroevolution potential-based molecular dynamics (NEP-MD) simulations.
• Construction and analysis of Ag-X-Ag (X = Au25CH3, Au24CdCH3, Au24CuCH3) model systems.

Main Results:

• Relaxed gold nanocluster structures at the interface show enhanced charge transport.
• Dopant-induced geometric rearrangement and interfacial coupling improve conductivity.
• Cadmium doping resulted in the most significant enhancement: stronger resonant transmission, higher density of states near the Fermi level, increased current, and reduced impedance.
• Transport properties exhibited weak temperature dependence due to synergistic Ag electrode and nanocluster interaction.

Conclusions:

• Atomically precise doping in gold nanoclusters is an effective method to boost interfacial transport efficiency.
• Dopant position, particularly near the electrode, influences enhancement.
• This provides a generalizable strategy for designing high-performance next-generation transport devices.