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Correlated electron materials (CEMs) host a rich variety of condensed matter phases. Vanadium dioxide (VO2) is a prototypical CEM with a temperature-dependent metal-to-insulator (MIT) transition with a concomitant crystal symmetry change. External control of MIT in VO2 - especially without inducing structural changes - has been a long-standing challenge. In this work, we design and synthesize modulation-doped VO2-based thin film heterostructures that closely emulate a textbook example of filling control in a correlated electron insulator. Using a combination of charge transport, hard x-ray photoelectron spectroscopy, and structural characterization, we show that the insulating state can be doped to achieve carrier densities greater than 5x10^21 cm^(-3) without inducing any measurable structural changes. We find that the MIT temperature (T_MIT) continuously decreases with increasing carrier concentration. Remarkably, the insulating state is robust even at doping concentrations as high as ~0.2 e-/vanadium. Finally, our work reveals modulation-doping as a viable method for electronic control of phase transitions in correlated electron oxides with the potential for use in future devices based on electric-field controlled phase transitions., Comment: Main paper 21 pages, 5 Figures. Supporting Information, 18 Pages,15 SI Figures and 1 SI Section

All solid state Li-ion batteries employing metallic lithium as an anode offer higher energy densities while also being safer than conventional liquid electrolyte based Li-ion batteries. However, the growth of tiny filaments of lithium (dendrites) across the solid state electrolyte layer leads to premature shorting of cells and limits their practical viability. The microscopic mechanisms that lead to lithium dendrite growth in solid state cells are still unclear. Using garnet based lithium ion conductor as a model solid state electrolyte, we show that interfacial void growth during lithium dissolution precedes dendrite nucleation and growth. Using a simple electrostatic model, we show that current density at the edges of the voids could be amplified by as much as four orders of magnitude making the cells highly susceptible to dendrite growth after void formation. We propose the use of metallic interlayers with low solubility and high nucleation overpotential for lithium to delay void growth. These interlayers increase dendrite growth tolerance in solid state electrolytes without the undue necessity for high stack pressures., Comment: 21 pages and 6 figures in the main manuscript. Supplementary Information of 36 pages contains sections S1.1 to S1.9, Figures S1-S25 and Tables S1 and S2

Atomically-abrupt interfaces in transition metal oxide (TMO) heterostructures could host a variety of exotic condensed matter phases that may not be found in the bulk materials at equilibrium. A critical step in the development of such atomically-sharp interfaces is the deposition of atomically-smooth TMO thin films. Optimized deposition conditions exist for the growth of perovskite oxides. However, the deposition of rutile oxides, such as VO$_2$, with atomic-layer precision has been challenging. In this work, we used pulsed laser deposition (PLD) to grow atomically-smooth VO$_2$ thin films on rutile TiO$_2$ (101) substrates. We show that optimal substrate preparation procedure followed by the deposition of VO$_2$ films at a temperature conducive for step-flow growth mode is essential for achieving atomically-smooth VO$_2$ films. The films deposited at optimal substrate temperatures show a step and terrace structure of the underlying TiO$_2$ substrate. At lower deposition temperatures, there is a transition to a mixed growth mode comprising of island growth and layer-by-layer growth modes. VO$_2$ films deposited at optimal substrate temperatures undergo a metal to insulator transition at a transition temperature of $\sim$325 K with $\sim$10$^3$ times increase in resistance, akin to MIT in bulk VO$_2$., Comment: 5 pages, 4 figures, Supplementary Information with 2 pages and 1 Figure