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Register a new userHighly repeatable nanoscale phase coexistence in vanadium dioxide films
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The metal-insulator transition (MIT) in vanadium dioxide (VO2) has the potential to lead to a number of disruptive technologies, including ultra-fast data storage, optical switches, and transistors which move beyond the limitations of silicon. For applications, VO2 films are deposited on crystalline substrates to prevent cracking observed in bulk VO2 crystals across the thermally driven MIT. Near the MIT, VO2 films exhibit nanoscale coexistence between metallic and insulating phases, which opens up further potential applications such as memristors, tunable capacitors, and optically engineered devices such as perfect absorbers. It is generally believed that the formation of phase domains must be affected to some extent by random processes which lead to unreliable performance in nanoscale MIT based devices. Here we show that nanoscale randomness is suppressed in the thermally driven MIT in sputtered VO2 films; the observed domain patterns of metallic and insulating phases in the vicinity of the MIT in these films behave in a strikingly reproducible way. This result opens the door for realizing reliable nanoscale VO2 devices.
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We investigate the electronic and structural changes at the nanoscale in vanadium dioxide (VO2) in the vicinity of its thermally driven phase transition. Both electronic and structural changes exhibit phase coexistence leading to percolation. In addition, we observe a dichotomy between the local electronic and structural transitions. Nanoscale x-ray diffraction reveals local, non-monotonic switching of the lattice structure, a phenomenon that is not seen in the electronic insulator-to-metal transition mapped by near-field infrared microscopy.
Phase competition in correlated oxides offers tantalizing opportunities as many intriguing physical phenomena occur near the phase transitions. Owing to a sharp metal-insulator transition (MIT) near room temperature, correlated vanadium dioxide (VO2) exhibits a strong competition between insulating and metallic phases that is important for practical applications. However, the phase boundary undergoes strong modification when strain is involved, yielding complex phase transitions. Here, we report the emergence of the nanoscale M2 phase domains in VO2 epitaxial films under anisotropic strain relaxation. The phase states of the films are imaged by multi-length-scale probes, detecting the structural and electrical properties in individual local domains. Competing evolution of the M1 and M2 phases indicates a critical role of lattice-strain on both the stability of the M2 Mott phase and the energetics of the MIT in VO2 films. This study demonstrates how strain engineering can be utilized to design phase states, which allow deliberate control of MIT behavior at the nanoscale in epitaxial VO2 films.
We use apertureless scattering near-field optical microscopy (SNOM) to investigate the nanoscale optical response of vanadium dioxide (VO2) thin films through a temperature-induced insulator-to-metal transition (IMT). We compare images of the transition at both mid-infrared (MIR) and terahertz (THz) frequencies, using a custom-built broadband THz-SNOM compatible with both cryogenic and elevated temperatures. We observe that the character of spatial inhomogeneities in the VO2 film strongly depends on the probing frequency. In addition, we find that individual insulating (or metallic) domains have a temperature-dependent optical response, in contrast to the assumptions of a classical first-order phase transition. We discuss these results in light of dynamical mean-field theory calculations of the dimer Hubbard model recently applied to VO2.
Amorphous vanadium dioxide (VO$_{2}$) films deposited by atomic layer deposition (ALD) were crystallized with an ex situ anneal at 660-670 ${deg}$C for 1-2 hours under a low oxygen pressure (10$^{-4}$ to 10$^{-5}$ Torr). Under these conditions the crystalline VO$_{2}$ phase was maintained, while formation of the V$_{2}$O$_{5}$ phase was suppressed. Electrical transition from the insulator to the metallic phase was observed in the 37-60 ${deg}$C range, with a R$_{ON}$/R$_{OFF}$ ratio of up to about 750 and critical transition temperature of 7-10 ${deg}$C. Electric field applied across two-terminal device structures induced a reversible phase change, with a room temperature transition field of about 25 kV/cm in the VO$_{2}$ sample processed with the 2 hr long anneal. Both the width and slope of the field induced MIT hysteresis were dependent upon the VO$_{2}$ crystalline quality.
Nucleation processes of mixed-phase states are an intrinsic characteristic of first-order phase transitions, typically related to local symmetry breaking. Direct observation of emerging mixed-phase regions in materials showing a first-order metal-insulator transition (MIT) offers unique opportunities to uncover their driving mechanism. Using photoemission electron microscopy, we image the nanoscale formation and growth of insulating domains across the temperature-driven MIT in NdNiO3 epitaxial thin films. Heteroepitaxy is found to strongly determine the nanoscale nature of the phase transition, inducing preferential formation of striped domains along the terraces of atomically flat stepped surfaces. We show that the distribution of transition temperatures is an intrinsic local property, set by surface morphology and stable across multiple temperature cycles. Our data provides new insights into the MIT of heteroepitaxial nickelates and points to a rich, nanoscale phenomenology in this strongly correlated material.
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