Phase segregation in Mg$_{x}$Zn$_{1-x}$O probed by optical absorption and photoluminescence at high pressure

TL;DR

This study uses high-pressure optical techniques to detect phase segregation in Mg$_x$Zn$_{1-x}$O thin films, revealing hidden nanocrystalline phases and extending pressure-dependent band gap data up to x≈0.3.

Contribution

It introduces a high-pressure approach to identify phase segregation in MgZnO thin films, surpassing limitations of crystallographic methods and extending the pressure coefficient analysis.

Findings

Phase segregation occurs for x>0.3, with a segregated Mg-rich wurtzite phase at x≈0.1.

High-pressure optical measurements reveal phase separation not detectable by crystallography.

Pressure coefficient of the band gap extends up to x≈0.3, showing different values for segregated and non-segregated phases.

Abstract

The appearance of segregated wurtzite Mg$_x$Zn$_{1-x}$O with low Mg content in thin films with $x>0.3$ affected by phase separation, cannot be reliably probed with crystallographic techniques owing to its embedded nanocrystalline configuration. Here we show a high-pressure approach which exploits the distinctive behaviors under pressure of wurtzite Mg$_x$Zn$_{1-x}$O thin films with different Mg contents to unveil phase segregation for $x>0.3$. By using ambient conditions photoluminescence (PL), and with optical absorption and PL under high pressure for $x=0.3$ we show that the appearance of a segregated wurtzite phase with a magnesium content of x $\sim$ 0.1 is inherent to the wurtzite and rock-salt phase separation. We also show that the presence of segregated wurtzite phase in oversaturated thin films phase is responsible for the low-energy absorption tail observed above $x=0.3$ in our Mg$_x$Zn$_{1-x}$O thin films. Our study has also allowed us to extend the concentration dependence of the pressure coefficient of the band gap from the previous limit of $x$ = 0.13 to $x \approx 0.3$ obtaining d$E_g$/d$P$ = 29 meV/GPa for wurtzite with $x \approx 0.3$ and 25 meV/GPa for the segregated $x\approx 0.09$ wurtzite phase.