Surfactant mediated growth of ferromagnetic Mn {\delta}-doped Si

TL;DR

This study explores how a Pb surfactant influences the structural and magnetic properties of Mn δ-doped silicon layers, revealing conditions for ferromagnetism and nanocrystal formation with potential for dilute magnetic semiconductors.

Contribution

It demonstrates that Pb surfactant significantly alters Mn incorporation and magnetic behavior in Si, identifying growth conditions for ferromagnetic phases and elucidating underlying mechanisms.

Findings

Pb surfactant enhances ferromagnetism in Mn-doped Si.

Distinct magnetic phases correlate with specific nanocrystal structures.

Pb modifies Mn incorporation pathways, promoting substitutional sites.

Abstract

We present an investigation of Mn {\delta}-doped layers in Si(001) grown by molecular beam epitaxy. We discovered that a Pb surfactant has significant effect on the structural and magnetic properties of the submonolayer of Mn, which depends on the Si capping layer growth temperature, T_Si, and the Mn coverage, {\theta}_Mn. The results presented in this paper identify three regions in the growth-phase-diagram characterized by distinct magnetic behaviors and crystal structures. In one region, X-ray absorption fine structure (XAFS) and transmission electron microscopy (TEM) experiments indicate that MnSi nanocrystallites form with B2-like crystal type structures. At the optimal growth conditions, T_Si = 200 C and {\theta}_Mn = 0.26 monolayer, a ferromagnetic phase develops with a Curie temperature T_C > 400 K and a saturation moment m_sat = 1.56 {\mu}_B/Mn, whereas T_C drops to zero for a control sample prepared without Pb. For T_Si > 200 C, MnSi-B20 type precipitates form with a T_C ~ 170 K. Rutherford backscattering spectroscopy shows that the increase in the remanent magnetization in these two phases is possibly correlated with an increase in the Mn substitutional fraction, which suggests that a Si_{1-x}Mn_x dilute magnetic semiconductor may be forming in the matrix between the precipitates. Density functional calculations show that Pb changes the pathway by which the Mn atoms access the Si substitutional sites, Mn_Si. While the Pb increases the formation energy of Mn_Si at the Si surface, it enables substitutional incorporation by lowering the formation energy of Si vacancies by 0.92 eV.