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Register a new userSubstrate-induced microstructure effects on the dynamics of the photo-induced Metal-insulator transition in VO$_2$ thin films
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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.
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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.
We have carried out a systematic experimental investigation to address the question why thin films of Fe$_3$O$_4$ (magnetite) generally have a very broad Verwey transition with lower transition temperatures as compared to the bulk. We observed using x-ray photoelectron spectroscopy, x-ray diffraction and resistivity measurements that the Verwey transition in thin films is drastically influenced not only by the oxygen stoichiometry but especially also by the substrate-induced microstructure. In particular, we found (1) that the transition temperature, the resistivity jump, and the conductivity gap of fully stoichiometric films greatly depends on the domain size, which increases gradually with increasing film thickness, (2) that the broadness of the transition scales with the width of the domain size distribution, and (3) that the hysteresis width is affected strongly by the presence of antiphase boundaries. Films grown on MgO (001) substrates showed the highest and sharpest transitions, with a 200 nm film having a T$_V$ of 122K, which is close to the bulk value. Films grown on substrates with large lattice constant mismatch revealed very broad transitions, and yet, all films show a transition with a hysteresis behavior, indicating that the transition is still first order rather than higher order.
We utilize near-infrared pump and mid-infrared probe spectroscopy to investigate the ultrafast electronic response of pressurized VO$_2$. Distinct pump-probe signals and a pumping threshold behavior are observed even in the pressure-induced metallic state showing a noticeable amount of localized electronic states. Our results are consistent with a scenario of a bandwidth-controlled Mott-Hubbard transition.
VO2 is a strongly correlated material, which undergoes a reversible metal insulator transition (MIT) coupled to a structural phase transition upon heating (T= 67{deg} C). Since its discovery the nature of the insulating state has long been debated and different solid-state mechanisms have been proposed to explain its nature: Mott-Hubbard correlation, Peierls distortion or a combination of both. Moreover, still now there is a lack of consensus on the interplay between the different degrees of freedom: charge, lattice, orbital and how they contribute to the MIT. In this manuscript we will investigate across the MIT the orbital evolution induced by a tensile strain applied to thin VO2 films. The strained films allowed to study the interplay between orbital and lattice degrees of freedom and to clarify MIT properties.
We have investigated the evolution of the electronic properties of La1-xSrxCrO3 (for the full range of x) epitaxial films deposited by molecular beam epitaxy (MBE) using x-ray diffraction, x-ray photoemission spectroscopy, Rutherford backscattering spectrometry, x-ray absorption spectroscopy, electrical transport, and ab initio modeling. LaCrO3 is an antiferromagnetic insulator whereas SrCrO3 is a metal. Substituting Sr2+ for La3+ in LaCrO3 effectively dopes holes into the top of valence band, leading to Cr4+ (3d2) local electron configurations. Core-level and valence-band features monotonically shift to lower binding energy with increasing x, indicating downward movement of the Fermi level toward the valence band maximum. The material becomes a p-type semiconductor at lower doping levels and an insulator-to-metal transition is observed at x greater than or equal to 0.65, but only when the films are deposited with in-plane compression via lattice-mismatched heteroepitaxy. Valence band x-ray photoemission spectroscopy reveals diminution of electronic state density at the Cr 3d t2g-derived top of the valence band while O K-edge x-ray absorption spectroscopy shows the development of a new unoccupied state above the Fermi level as holes are doped into LaCrO3. The evolution of these bands with Sr concentration is accurately captured using density functional theory with a Hubbard U correction of 3.0 eV (DFT + U). Resistivity data in the semiconducting regime (x less than or equal to 0.50) do not fit perfectly well to either a polaron hopping or band conduction model, but are best interpreted in terms of a hybrid model. The activation energies extracted from these fits are well reproduced by DFT + U.
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