Self-organized transient facilitated atomic transport in Pt/Al(111)

TL;DR

This study reveals a novel spontaneous atomic transport mechanism in Pt/Al(111) at ultra-low temperatures, driven by local thermalization and self-organization, enabling intermixing without external bias or tunneling.

Contribution

It introduces a new transient atomic exchange process driven by self-organization and local thermalization, not previously reported at ultra-low temperatures.

Findings

Transient inter-layer atomic transport occurs without tunneling.

Self-organized local thermalization reaches ~1000 K.

Atomic injection is independent of impurity-host interaction strength.

Abstract

During the course of atomic transport in a host material, impurity atoms need to surmount an energy barrier driven by thermodynamic bias or at ultra-low temperatures by quantum tunneling. In the present article we demonstrate using atomistic simulations that at ultra-low temperature transient inter-layer atomic transport is also possible without tunneling when the Pt/Al(111) impurity/host system self-organizes itself spontaneously into an intermixed configuration. No such extremely fast athermal concerted process has been reported before at ultra low temperatures. The outlined novel transient atomic exchange mechanism could be of general validity. We find that the source of ultra-low temperature heavy particle barrier crossing is intrinsic and no external bias is necessary for atomic intermixing and surface alloying in Pt/Al although the dynamic barrier height is few eV. The mechanism is driven by the local thermalization of the Al(111) surface in a self-organized manner arranged spontaneously by the system without any external stimulus. The core of the short lived thermalized region reaches the local temperature of $\sim 1000$ K (including few tens of Al atoms) while the average temperature of the simulation cell is $\sim 3$ K. The transient facilitated intermixing process also takes place with repulsive impurity-host interaction potential leading to negative atomic mobility hence the atomic injection is largely independent of the strength of the impurity-surface interaction. We predict that similar exotic behaviour is possible in other materials as well.