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Register a new userEffect of inhomogeneities and substrate on the dynamics of the metal-insulator transition in VO$_2$ thin films
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Martin Rodriguez-Vega
Publication date
2015
fields
Physics
and research's language is
English
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We study the thermal relaxation dynamics of VO$_2$ films after the ultrafast photo-induced metal-insulator transition for two VO$_2$ film samples grown on Al$_2$O$_3$ and TiO$_2$ substrates. We find two orders of magnitude difference in the recovery time (a few ns for the VO$_2$/Al$_2$O$_3$ sample vs. hundreds of ns for the VO$_2$/TiO$_2$ sample). We present a theoretical model that accurately describes the MIT thermal properties and interpret the experimental measurements. We obtain quantitative results that show how the microstructure of the VO$_2$ film and the thermal conductivity of the interface between the VO$_2$ film and the substrate affect long time-scale recovery dynamics. We also obtain a simple analytic relationship between the recovery time-scale and some of the film parameters.
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In this paper we used Raman spectroscopy to investigate the optical properties of vanadium dioxide (VO2) thin films during the thermally induced insulating to metallic phase transition. We observed a significant difference in transition temperature in similar VO2 films grown on quartz and sapphire substrates: the film grown on quartz displayed the phase transition at a lower temperature (Tc=50C) compared a film grown on sapphire (Tc=68C). We also investigated differences in the detected Raman signal for different wavelengths and polarizations of the excitation laser. We found that for either substrate, a longer wavelength (in our case 785 nm) yielded the clearest VO2 Raman spectra, with no polarization dependence.
We investigate the differences in the dynamics of the ultrafast photo-induced metal-insulator transition (MIT) of two VO$_2$ thin films deposited on different substrates, TiO$_2$ and Al$_2$O$_3$, and in particular the temperature dependence of the threshold laser fluence values required to induce various MIT stages in a wide range of sample temperatures (150 K - 320 K). We identified that, although the general pattern of MIT evolution was similar for the two samples, there were several differences. Most notably, the threshold values of laser fluence required to reach the transition to a fully metallic phase in the VO$_2$ film on the TiO$_2$ substrate were nearly constant in the range of temperatures considered, whereas the VO$_2$/Al$_2$O$_3$ sample showed clear temperature dependence. Our analysis qualitatively connects such behavior to the structural differences in the two VO$_2$ films.
The insulator-to-metal transition (IMT) of the simple binary compound of vanadium dioxide VO$_2$ at $sim 340$ K has been puzzling since its discovery more than five decades ago. A wide variety of photon and electron probes have been applied in search of a satisfactory microscopic mechanistic explanation. However, many of the conclusions drawn have implicitly assumed a {em homogeneous} material response. Here, we reveal inherently {em inhomogeneous} behavior in the study of the dynamics of individual VO$_2$ micro-crystals using a combination of femtosecond pump-probe microscopy with nano-IR imaging. The time scales of the photoinduced bandgap reorganization in the ultrafast IMT vary from $simeq 40 pm 8$ fs, i.e., shorter than a suggested phonon bottleneck, to $sim 200pm20$ fs, with an average value of $80 pm 25$ fs, similar to results from previous studies on polycrystalline thin films. The variation is uncorrelated with crystal size, orientation, transition temperature, and initial insulating phase. This together with details of the nano-domain behavior during the thermally-induced IMT suggests a significant sensitivity to local variations in, e.g., doping, defects, and strain of the microcrystals. The combination of results points to an electronic mechanism dominating the photoinduced IMT in VO$_2$, but also highlights the difficulty of deducing mechanistic information where the intrinsic response in correlated matter may not yet have been reached.
The vanadates VO$_2$ and V$_2$O$_3$ are prototypical examples of strongly correlated materials that exhibit a metal-insulator transition. While the phase transitions in these materials have been studied extensively, there is a limited understanding of how the properties of these materials are affected by the presence of defects and doping. In this study we investigate the impact of native point defects in the form of Frenkel defects on the structural, magnetic and electronic properties of VO$_2$ and V$_2$O$_3$, using first-principles calculations. In VO$_2$ the vanadium Frenkel pairs lead to a non-trivial insulating state. The unpaired vanadium interstitial bonds to a single dimer, which leads to a trimer that has one singlet state and one localized single-electron $S=1/2$ state. The unpaired broken dimer created by the vanadium vacancy also has a localized $S=1/2$ state. Thus, the insulating state is created by the singlet dimers, the trimer and the two localized $S=1/2$ states. Oxygen Frenkel pairs, on the other hand, lead to a metallic state in VO$_2$, but are expected to be present in much lower concentrations. In contrast, the Frenkel defects in V$_2$O$_3$ do not directly suppress the insulating character of the material. However, the disorder created by defects in V$_2$O$_3$ alters the local magnetic moments and in turn reduces the energy cost of a transition between the insulating and conducting phases of the material. We also find self-trapped small polarons in V$_2$O$_3$, which has implications for transport properties in the insulating phase.
BiFeO3 thin films have been deposited on Pt/sapphire and Pt/Ti/SiO2/Si substrates with pulsed laser deposition using the same growth conditions, respectively. Au was sputtered as the top electrode. The microscopic structure of the thin film varies by changing the underlying substrate. Thin films on Pt/sapphire are not resistively switchable due to the formation of Schottky contacts at both the top and the bottom interface. However, thin films on Pt/Ti/SiO2/Si exhibit an obvious resistive switching behavior under forward bias. The conduction mechanisms in BiFeO3 thin films on Pt/sapphire and Pt/Ti/SiO2/Si substrates are discussed to understand the different resistive switching behaviors.
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