Temperature-driven confinements of surface electrons and adatoms in a weakly interacting 2D organic porous network

TL;DR

This study demonstrates a temperature-controlled reversible phase transition in a weakly interacting 2D organic porous network on Cu(111), enabling quantum confinement of surface electrons and adatoms, and potential spin control.

Contribution

It introduces a novel weakly interacting 2D organic porous network that can reversibly switch structures and control surface electron and spin states through temperature-driven phase transitions.

Findings

Low-temperature porous network confines surface electrons and adatoms.

Significant electronic band renormalization occurs due to confinement.

Confined Co atoms form ordered quantum dots with spin transfer capabilities.

Abstract

Two-dimensional organic porous networks (2DOPNs) have opened new vistas for tailoring the physicochemical characteristics of metallic surfaces. These typically chemically bound nanoporous structures act as periodical quantum wells leading to the 2D confinements of surface electron gases, adatoms and molecular guests. Here we propose a new type of porous network with weakly interacting 2,4,6-triphenyl-1,3,5-triazine (TPT) molecules on a Cu(111) surface, in which a temperature-driven (T-driven) phase transition can reversibly alter the supramolecular structures from a close-packed (CP-TPT) phase to a porous-network (PN-TPT) phase. Crucially, only the low-temperature PN-TPT exhibits subnano-scale cavities that can confine the surface state electrons and metal adatoms. The confined surface electrons undergo a significant electronic band renormalization. To activate the spin degree of freedom, the T-driven PN-TPT structure can additionally trap Co atoms within the cavities, forming highly ordered quantum dots. Our theoretical simulation reveals a complex spin carrier transfer from the confined Co cluster to the neighbouring TPT molecules via the underlying substrate. Our results demonstrate that weakly interacting 2DOPN offers a unique quantum switch capable of steering and controlling electrons and spin at surfaces via tailored quantum confinements.