More Like this

1. Local structure elucidation of tungsten-substituted vanadium dioxide (V$$_{1-x}$$W$$_x$$O$$_2$$)

   https://doi.org/10.1038/s41598-022-18575-0  

   Wilson, Catrina E. ; Gibson, Amanda E. ; Cuillier, Paul M. ; Li, Cheng-Han ; Crosby, Patrice H. N. ; Trigg, Edward B. ; Najmr, Stan ; Murray, Christopher B. ; Jinschek, Joerg R. ; Doan-Nguyen, Vicky ( August 2022 , Scientific Reports)

   Initially, vanadium dioxide seems to be an ideal first-order phase transition case study due to its deceptively simple structure and composition, but upon closer inspection there are nuances to the driving mechanism of the metal-insulator transition (MIT) that are still unexplained. In this study, a local structure analysis across a bulk powder tungsten-substitution series is utilized to tease out the nuances of this first-order phase transition. A comparison of the average structure to the local structure using synchrotron x-ray diffraction and total scattering pair-distribution function methods, respectively, is discussed as well as comparison to bright field transmission electron microscopy imaging through a similar temperature-series as the local structure characterization. Extended x-ray absorption fine structure fitting of thin film data across the substitution-series is also presented and compared to bulk. Machine learning technique, non-negative matrix factorization, is applied to analyze the total scattering data. The bulk MIT is probed through magnetic susceptibility as well as differential scanning calorimetry. The findings indicate the local transition temperature ($$T_c$$$T_c$) is less than the average$$T_c$$$T_c$supporting the Peierls-Mott MIT mechanism, and demonstrate that in bulk powder and thin-films, increasing tungsten-substitution instigates local V-oxidation through the phase pathway VO$$_2\, \rightarrow$$${}_2\to$V$$_6$$${}_6$O$$_{13} \, \rightarrow$$${}_{13}\to$V$$_2$$${}_2$O$$_5$$${}_5$.

    

   more » « less
2. Emergent charge order near the doping-induced Mott-insulating quantum phase transition in Sr3Ru2O7

   https://doi.org/10.1038/s42005-019-0138-4  

   Leshen, Justin ; Kavai, Mariam ; Giannakis, Ioannis ; Kaneko, Yoshio ; Tokura, Yoshi ; Mukherjee, Shantanu ; Lee, Wei-Cheng ; Aynajian, Pegor ( March 2019 , Communications Physics)

   Search for novel electronically ordered states of matter emerging near quantum phase transitions is an intriguing frontier of condensed matter physics. In ruthenates, the interplay between Coulomb correlations among the 4delectronic states and their spin-orbit interactions, lead to complex forms of electronic phenomena. Here we investigate the double layered Sr₃(Ru_1−xMn_x)₂O₇and its doping-induced quantum phase transition from a metal to an antiferromagnetic Mott insulator. Using spectroscopic imaging with the scanning tunneling microscope, we visualize the evolution of the electronic states in real- and momentum-space. We find a partial-gap at the Fermi energy that develops with doping to form a weak Mott insulating state. Near the quantum phase transition, we discover a spatial electronic reorganization into a commensurate checkerboard charge order. These findings bear a resemblance to the universal charge order in the pseudogap phase of cuprates and demonstrate the ubiquity of charge order that emanates from doped Mott insulators.

    

   more » « less
3. Electrical Transition in Isostructural VO2 Thin-Film Heterostructures

   https://doi.org/10.1038/s41598-019-39529-z  

   Moatti, Adele ; Sachan, Ritesh ; Cooper, Valentino R. ; Narayan, Jagdish ( February 2019 , Scientific Reports)

   Control over the concurrent occurrence of structural (monoclinic to tetragonal) and electrical (insulator to the conductor) transitions presents a formidable challenge for VO₂-based thin film devices. Speed, lifetime, and reliability of these devices can be significantly improved by utilizing solely electrical transition while eliminating structural transition. We design a novel strain-stabilized isostructural VO₂epitaxial thin-film system where the electrical transition occurs without any observable structural transition. The thin-film heterostructures with a completely relaxed NiO buffer layer have been synthesized allowing complete control over strains in VO₂films. The strain trapping in VO₂thin films occurs below a critical thickness by arresting the formation of misfit dislocations. We discover the structural pinning of the monoclinic phase in (10 ± 1 nm) epitaxial VO₂films due to bandgap changes throughout the whole temperature regime as the insulator-to-metal transition occurs. Using density functional theory, we calculate that the strain in monoclinic structure reduces the difference between long and short V-V bond-lengths (Δ_V−V) in monoclinic structures which leads to a systematic decrease in the electronic bandgap of VO₂. This decrease in bandgap is additionally attributed to ferromagnetic ordering in the monoclinic phase to facilitate a Mott insulator without going through the structural transition.

    

   more » « less
4. Room-temperature valence transition in a strain-tuned perovskite oxide

   https://doi.org/10.1038/s41467-022-35024-8  

   Chaturvedi, Vipul ; Ghosh, Supriya ; Gautreau, Dominique ; Postiglione, William M. ; Dewey, John E. ; Quarterman, Patrick ; Balakrishnan, Purnima P. ; Kirby, Brian J. ; Zhou, Hua ; Cheng, Huikai ; et al ( December 2022 , Nature Communications)

   Cobalt oxides have long been understood to display intriguing phenomena known as spin-state crossovers, where the cobalt ion spin changes vs. temperature, pressure, etc. A very different situation was recently uncovered in praseodymium-containing cobalt oxides, where a first-order coupled spin-state/structural/metal-insulator transition occurs, driven by a remarkable praseodymium valence transition. Such valence transitions, particularly when triggering spin-state and metal-insulator transitions, offer highly appealing functionality, but have thus far been confined to cryogenic temperatures in bulk materials (e.g., 90 K in Pr_1-xCa_xCoO₃). Here, we show that in thin films of the complex perovskite (Pr_1-yY_y)_1-xCa_xCoO_3-δ, heteroepitaxial strain tuning enables stabilization of valence-driven spin-state/structural/metal-insulator transitions to at least 291 K, i.e., around room temperature. The technological implications of this result are accompanied by fundamental prospects, as complete strain control of the electronic ground state is demonstrated, from ferromagnetic metal under tension to nonmagnetic insulator under compression, thereby exposing a potential novel quantum critical point.

    

   more » « less
5. In‐Operando Spatiotemporal Imaging of Coupled Film‐Substrate Elastodynamics During an Insulator‐to‐Metal Transition

   https://doi.org/10.1002/adma.202312673  

   Stone, Greg ; Shi, Yin ; Jerry, Matthew ; Stoica, Vladimir ; Paik, Hanjong ; Cai, Zhonghou ; Schlom, Darrell G. ; Engel‐Herbert, Roman ; Datta, Suman ; Wen, Haidan ; et al ( March 2024 , Advanced Materials)

   The drive toward non‐von Neumann device architectures has led to an intense focus on insulator‐to‐metal (IMT) and the converse metal‐to‐insulator (MIT) transitions. Studies of electric field‐driven IMT in the prototypical VO₂thin‐film channel devices are largely focused on the electrical and elastic responses of the films, but the response of the corresponding TiO₂substrate is often overlooked, since it is nominally expected to be electrically passive and elastically rigid. Here, in‐operando spatiotemporal imaging of the coupled elastodynamics using X‐ray diffraction microscopy of a VO₂film channel device on TiO₂substrate reveals two new surprises. First, the film channel bulges during the IMT, the opposite of the expected shrinking in the film undergoing IMT. Second, a microns thick proximal layer in the substrate also coherently bulges accompanying the IMT in the film, which is completely unexpected. Phase‐field simulations of coupled IMT, oxygen vacancy electronic dynamics, and electronic carrier diffusion incorporating thermal and strain effects suggest that the observed elastodynamics can be explained by the known naturally occurring oxygen vacancies that rapidly ionize (and deionize) in concert with the IMT (MIT). Fast electrical‐triggering of the IMT via ionizing defects and an active “IMT‐like” substrate layer are critical aspects to consider in device applications.

    

   more » « less