RESUMO
First-order phase transitions in solids are notoriously challenging to study. The combination of change in unit cell shape, long range of elastic distortion and flow of latent heat leads to large energy barriers resulting in domain structure, hysteresis and cracking. The situation is worse near a triple point, where more than two phases are involved. The well-known metal-insulator transition in vanadium dioxide, a popular candidate for ultrafast optical and electrical switching applications, is a case in point. Even though VO2 is one of the simplest strongly correlated materials, experimental difficulties posed by the first-order nature of the metal-insulator transition as well as the involvement of at least two competing insulating phases have led to persistent controversy about its nature. Here we show that studying single-crystal VO2 nanobeams in a purpose-built nanomechanical strain apparatus allows investigation of this prototypical phase transition with unprecedented control and precision. Our results include the striking finding that the triple point of the metallic phase and two insulating phases is at the transition temperature, Ttr = Tc, which we determine to be 65.0 ± 0.1 °C. The findings have profound implications for the mechanism of the metal-insulator transition in VO2, but they also demonstrate the importance of this approach for mastering phase transitions in many other strongly correlated materials, such as manganites and iron-based superconductors.
RESUMO
Hydrogen intercalation in solids is common, complicated, and very difficult to monitor. In a new approach to the problem, we have studied the profile of hydrogen diffusion in single-crystal nanobeams and plates of VO2, exploiting the fact that hydrogen doping in this material leads to visible darkening near room temperature connected with the metal-insulator transition at 65 °C. We observe hydrogen diffusion along the rutile c-axis but not perpendicular to it, making this a highly one-dimensional diffusion system. We obtain an activated diffusion coefficient, [Formula: see text] applicable in metallic phase. In addition, we observe dramatic supercooling of the hydrogen-induced metallic phase and spontaneous segregation of the hydrogen into stripes implying that the diffusion process is highly nonlinear, even in the absence of defects. Similar complications may occur in hydrogen motion in other materials but are not revealed by conventional measurement techniques.
RESUMO
The generation of a current by light is a key process in optoelectronic and photovoltaic devices. In band semiconductors, depletion fields associated with interfaces separate long-lived photo-induced carriers. However, in systems with strong electron-electron and electron-phonon correlations it is unclear what physics will dominate the photoresponse. Here, we investigate photocurrent in VO(2), an exemplary strongly correlated material known for its dramatic metal-insulator transition at T(c) ≈ 68 °C, which could be useful for optoelectronic detection and switching up to ultraviolet wavelengths. Using scanning photocurrent microscopy on individual suspended VO(2) nanobeams we observe a photoresponse peaked at the metal-insulator boundary but extending throughout both insulating and metallic phases. We determine that the response is photothermal, implying efficient carrier relaxation to a local equilibrium in a manner consistent with strong correlations. Temperature-dependent measurements reveal subtle phase changes within the insulating state. We further demonstrate switching of the photocurrent by optical control of the metal-insulator boundary arrangement. Our work shows the value of applying scanning photocurrent microscopy to nanoscale crystals in the investigation of strongly correlated materials, and the results are relevant for designing and controlling optoelectronic devices employing such materials.