This paper describes a solution-phase synthesis of high-quality vanadium dioxide thermochromic thin films. The films obtained showed excellent visible transparency and a large change in transmittance at near-infrared (NIR) wavelengths before and after the metal-insulator phase transition (MIPT). For a 59 nm thick single-layer VO(2) thin film, the integral values of visible transmittance (T(int)) for metallic (M) and semiconductive (S) states were 54.1% and 49.1%, respectively, while the NIR switching efficiencies (DeltaT) were as high as 50% at 2000 nm. Thinner films can provide much higher transmittance of visible light, but they suffer from an attenuation of the switching efficiency in the near-infrared region. By varying the film thickness, ultrahigh T(int) values of 75.2% and 75.7% for the M and S states, respectively, were obtained, while the DeltaT at 2000 nm remained high. These results represent the best data for VO(2) to date. Thicker films in an optimized range can give enhanced NIR switching efficiencies and excellent NIR blocking abilities; in a particularly impressive experiment, one film provided near-zero NIR transmittance in the switched state. The thickness-dependent performance suggests that VO(2) will be of great use in the objective-specific applications. The reflectance and emissivity at the wavelength range of 2.5-25 microm before and after the MIPT were dependent on the film thickness; large contrasts were observed for relatively thick films. This work also showed that the MIPT temperature can be reduced simply by selecting the annealing temperature that induces local nonstoichiometry; a MIPT temperature as low as 42.7 degrees C was obtained by annealing the film at 440 degrees C. These properties (the high visible transmittance, the large change in infrared transmittance, and the near room-temperature MIPT) suggest that the current method is a landmark in the development of this interesting material toward applications in energy-saving smart windows.
This paper reports the successful preparation of Mg-doped VO2 nanoparticles via hydrothermal synthesis. The metal-insulator transition temperature (T(c)) decreased by approximately 2 K per at% Mg. The Tc decreased to 54 °C with 7.0 at% dopant. The composite foils made from Mg-doped VO2 particles displayed excellent visible transmittance (up to 54.2%) and solar modulation ability (up to 10.6%). In addition, the absorption edge blue-shifted from 490 nm to 440 nm at a Mg content of 3.8 at%, representing a widened optical band gap from 2.0 eV for pure VO2 to 2.4 eV at 3.8 at% doping. As a result, the colour of the Mg-doped films was modified to increase their brightness and lighten the yellow colour over that of the undoped-VO2 film. A first principle calculation was conducted to understand how dopants affect the optical, Mott phase transition and structural properties of VO2.
Quasi-spherical VO 2 nanoparticles with uniform size and high crystallinity are ideal functional materials for applications in field-effect transistors, smart window coatings and switches. However, the synthesis of these VO 2 nanoparticles has long been a challenge. This article presents a novel doping strategy for the simultaneous control of the size, morphology and polymorphology of VO 2 nanoparticles. Doping can induce the change in crystal structure and exhibits a significant promoting effect on the formation of doped monoclinic VO 2 (VO 2 (M)). Specifically, by antimony (Sb 3+ ) doping, hexagonal-shaped, well crystalline monoclinic VO 2 nanoparticles with tunable sizes (8-30 nm) and controllable polymorphs were synthesized via a one-pot, hydrothermal method. Sb 3+ dopants, which are larger in radius and lower in valence than V 4+ ions, can introduce extra oxygen vacancies during the nucleation and growth of VO 2 nanoparticles. These positively charged nuclei may suppress the adsorption of VO 2+ aqua ions, and therefore inhibit the growth of the VO 2 (M) nanoparticles. Comparably, Sb 5+ dopants that possess higher valence counts than V 4+ ions can induce the growth of VO 2 (M) particles to 200-300 nm width and above 500 nm length. The Sb 3+ -doped VO 2 (M) nanoparticles exhibit excellent properties in metal-semiconductor transformation at transition temperatures ranging from 55-68 C. Films obtained by casting these nanoparticles show excellent optical properties (both visible transmittance and infrared regulation), compared with those prepared from gas phases, such as sputtering. This synthetic strategy that involves the doping of an element with a different valence count than the matrix cation may be useful for controlling the solution growth of some technologically significant nanomaterials. In addition, the formation mechanism of solid and crystalline transformation was also studied by designing a specific reaction autoclave.
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