RESUMO
Traditionally, the Coulomb repulsion or Peierls instability causes the metal-insulator phase transitions in strongly correlated quantum materials. In comparison, magnetic stress is predicted to drive the metal-insulator transition in materials exhibiting strong spin-lattice coupling. However, this mechanism lacks experimental validation and an in-depth understanding. Here we demonstrate the existence of the magnetic stress-driven metal-insulator transition in an archetypal material, chromium nitride. Structural, magnetic, electronic transport characterization, and first-principles modeling analysis show that the phase transition temperature in CrN is directly proportional to the strain-controlled anisotropic magnetic stress. The compressive strain increases the magnetic stress, leading to the much-coveted room-temperature transition. In contrast, tensile strain and the inclusion of nonmagnetic cations weaken the magnetic stress and reduce the transition temperature. This discovery of a new physical origin of metal-insulator phase transition that unifies spin, charge, and lattice degrees of freedom in correlated materials marks a new paradigm and could lead to novel device functionalities.
RESUMO
Harnessing solar energy by employing concentrated solar power (CSP) systems requires materials with high electrical conductivity and optical reflectivity. Silver, with its excellent optical reflectance, is traditionally used as a reflective layer in solar mirrors for CSP technologies. However, silver is soft and expensive, quickly tarnishes, and requires a protective layer of glass for practical applications. Moreover, supply-side constraints and high-temperature instability of silver have led to the search for alternative materials that exhibit high solar and infrared reflectance. Transition metal nitrides, such as titanium nitride, have emerged as alternative plasmonic materials to gold starting from a spectral range of â¼500 nm. However, to achieve high solar reflection (â¼320-2500 nm), materials with epsilon-near-zero starting from the near-ultraviolet (UV) spectral region are required. Here, we show the development of refractory epitaxial hafnium nitride (HfN) and zirconium nitride (ZrN) thin films as excellent mirrors with a solar reflectivity of â¼90.3% and an infrared reflectivity of â¼95%. Low-loss and high-quality epsilon-near-zero resonance at near-UV (â¼340-380 nm) spectral regions are achieved in HfN and ZrN by carefully controlling the stoichiometry, leading to a sharp increase in the reflection edge that is on par with silver. Temperature-dependent reflectivity and dielectric constants are further measured to demonstrate their high-temperature suitability. The development of refractory epitaxial HfN and ZrN thin films with high solar and infrared reflectance makes them excellent alternative plasmonic materials to silver and would pave their applications in CSP, daytime radiative cooling, and others.
RESUMO
The interaction of light with collective charge oscillations, called plasmon-polariton, and with polar lattice vibrations, called phonon-polariton, are essential for confining light at deep subwavelength dimensions and achieving strong resonances. Traditionally, doped-semiconductors and conducting metal oxides (CMO) are used to achieve plasmon-polaritons in the near-to-mid infrared (IR), while polar dielectrics are utilized for realizing phonon-polaritons in the long-wavelength IR (LWIR) spectral regions. However, demonstrating low-loss plasmon- and phonon-polaritons in one host material will make it attractive for practical applications. Here, we demonstrate high-quality tunable short-wavelength IR (SWIR) plasmon-polariton and LWIR phonon-polariton in complementary metal-oxide-semiconductor compatible group III-V polar semiconducting scandium nitride (ScN) thin films. We achieve both resonances by utilizing n-type (oxygen) and p-type (magnesium) doping in ScN that allows modulation of carrier concentration from 5 × 1018 to 1.6 × 1021 cm-3. Our work enables infrared nanophotonics with an epitaxial group III semiconducting nitride, opening the possibility for practical applications.
RESUMO
Plastic deformation in ceramic materials is normally only observed in nanometre-sized samples. However, we have observed high levels of plasticity (>50% plastic strain) and excellent elasticity (6% elastic strain) in perovskite oxide Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3, under compression along <100>pc pillars up to 2.1 µm in diameter. The extent of this deformation is much higher than has previously been reported for ceramic materials, and the sample size at which plasticity is observed is almost an order of magnitude larger. Bending tests also revealed over 8% flexural strain. Plastic deformation occurred by slip along {110} <1[Formula: see text]0 > . Calculations indicate that the resulting strain gradients will give rise to giant flexoelectric polarization. First principles models predict that a high concentration of oxygen vacancies weaken the covalent/ionic bonds, giving rise to the unexpected plasticity. Mechanical testing on oxygen vacancies-rich Mn-doped Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 confirmed this prediction. These findings will facilitate the design of plastic ceramic materials and the development of flexoelectric-based nano-electromechanical systems.
RESUMO
Perovskite oxides are regarded as promising electrocatalysts for water splitting due to their cost-effectiveness, high efficiency and durability in the oxygen evolution reaction (OER). Despite these advantages, a fundamental understanding of how critical structural parameters of perovskite electrocatalysts influence their activity and stability is lacking. Here, we investigate the impact of structural defects on OER performance for representative LaNiO3 perovskite electrocatalysts. Hydrogen reduction of 700 °C calcined LaNiO3 induces a high density of surface oxygen vacancies, and confers significantly enhanced OER activity and stability compared to unreduced LaNiO3 ; the former exhibit a low onset overpotential of 380â mV at 10â mA cm-2 and a small Tafel slope of 70.8â mV dec-1 . Oxygen vacancy formation is accompanied by mixed Ni2+ /Ni3+ valence states, which quantum-chemical DFT calculations reveal modify the perovskite electronic structure. Further, it reveals that the formation of oxygen vacancies is thermodynamically more favourable on the surface than in the bulk; it increases the electronic conductivity of reduced LaNiO3 in accordance with the enhanced OER activity that is observed.
RESUMO
Device failure from diffusion short circuits in microelectronic components occurs via thermally induced migration of atoms along high-diffusivity paths: dislocations, grain boundaries, and free surfaces. Even well-annealed single-grain metallic films contain dislocation densities of about 1014 m-2; hence dislocation-pipe diffusion (DPD) becomes a major contribution at working temperatures. While its theoretical concept was established already in the 1950s and its contribution is commonly measured using indirect tracer, spectroscopy, or electrical methods, no direct observation of DPD at the atomic level has been reported. We present atomically-resolved electron microscopy images of the onset and progression of diffusion along threading dislocations in sequentially annealed nitride metal/semiconductor superlattices, and show that this type of diffusion can be independent of concentration gradients in the system but governed by the reduction of strain fields in the lattice.