Strongly correlated materials show unique solid-state phase transitions with rich nanoscale phenomenology that can be controlled by external stimuli. Particularly interesting is the case of light–matter interaction in the proximity of the metal–insulator transition of heteroepitaxial nickelates. In this work, we use near-infrared laser light in the high-intensity excitation regime to manipulate the nanoscale phase separation in NdNiO3. By tuning the laser intensity, we can reproducibly set the coverage of insulating nanodomains, which we image by photoemission electron microscopy, thus semipermanently configuring the material state. With the aid of transport measurements and finite element simulations, we identify two different timescales of thermal dynamics in the light–matter interaction: a steady-state and a fast transient local heating. These results open interesting perspectives for locally manipulating and reconfiguring electronic order at the nanoscale by optical means.@en

Hydrogen-related technologies are rapidly developing, driven by the necessity of efficient and high-density energy storage. This poses new challenges to the detection of dangerous gases, in particular the realization of cheap, sensitive, and fast hydrogen sensors. Several materials are being studied for this application, but most present critical bottlenecks, such as high operational temperature, low sensitivity, slow response time, and/or complex fabrication procedures. Here, we demonstrate that WO3 in the form of single-crystal, ultrathin films with a Pt catalyst allows high-performance sensing of H2 gas at room temperature. Thanks to the high electrical resistance in the pristine state, this material is able to detect hydrogen concentrations down to 1 ppm near room temperature. Moreover, the high surface-to-volume ratio of WO3 ultrathin films determines fast sensor response and recovery, with characteristic times as low as 1 s when the concentration exceeds 100 ppm. By modeling the hydrogen (de)intercalation dynamics with a kinetic model, we extract the energy barriers of the relevant processes and relate the doping mechanism to the formation of oxygen vacancies. Our results reveal the potential of single-crystal WO3 ultrath@en

Strain engineering is one of the most effective approaches to manipulate the physical state of materials, control their electronic properties, and enable crucial functionalities. Because of their rich phase diagrams arising from competing ground states, quantum materials are an ideal playground for on-demand material control and can be used to develop emergent technologies, such as adaptive electronics or neuromorphic computing. It was recently suggested that complex oxides could bring unprecedented functionalities to the field of nanomechanics, but the possibility of precisely controlling the stress state of materials is so far lacking. Here, we demonstrate the wide and reversible manipulation of the stress state of single-crystal WO3 by strain engineering controlled by catalytic hydrogenation. Progressive incorporation of hydrogen in freestanding ultrathin structures determines large variations of their mechanical resonance frequencies, inducing static deformation. Our results demonstrate hydrogen doping as a new paradigm to reversibly manipulate the mechanical properties of nanodevices based on materials control.@en

This thesis is an experimental investigation of the physical properties of different transition metal oxide ultra-thin films. A common feature of these various materials and structures is that they exhibit a solid-state phase transition from a metallic to an insulating state, which is triggered upon changing sample composition, or by varying an external stimulus such as temperature, illumination or gas pressure. The experiments performed cover a broad spectrum of condensed matter, from material growth, structural characterisation and nanodevice fabrication to low-temperature magnetotransport, synchrotron microscopy and gas sensing.@en

Interfaces between complex oxides constitute a unique playground for two-dimensional electron systems (2DESs), where superconductivity and magnetism can arise from combinations of bulk insulators. The 2DES at the LaAlO3/SrTiO3 interface is one of the most studied in this regard, and its origin is determined by the polar field in LaAlO3 as well as by the presence of point defects, like oxygen vacancies and intermixed cations. These defects usually reside in the conduction channel and are responsible for a decrease of the electronic mobility. In this work, we use an amorphous WO3 overlayer to obtain a high-mobility 2DES in WO3/LaAlO3/SrTiO3 heterostructures. The studied system shows a sharp insulator-to-metal transition as a function of both LaAlO3 and WO3 layer thickness. Low-temperature magnetotransport reveals a strong magnetoresistance reaching 900% at 10 T and 1.5 K, the presence of multiple conduction channels with carrier mobility up to 80 000 cm2 V-1 s-1, and quantum oscillations of conductance.@en

Relaxation oscillators consist of periodic variations of a physical quantity triggered by a static excitation. They are a typical consequence of nonlinear dynamics and can be observed in a variety of systems. VO2 is a correlated oxide with a solid-state phase transition above room temperature, where both electrical resistance and lattice parameters undergo a drastic change in a narrow temperature range. This strong nonlinear response allows to realize spontaneous electrical oscillations in the megahertz range under a DC voltage bias. These electrical oscillations are employed to set into mechanical resonance a microstructure without the need of any active electronics, with small power consumption and with the possibility to selectively excite specific flexural modes by tuning the value of the DC electrical bias in a range of few hundreds of millivolts. This actuation method is robust and flexible and can be implemented in a variety of autonomous DC-powered devices.@en

Relaxation oscillators consist of periodic variations of a physical quantity triggered by a static excitation. They are a typical consequence of nonlinear dynamics and can be observed in a variety of systems. VO2 is a correlated oxide with a solid-state phase transition above room temperature, where both electrical resistance and lattice parameters undergo a drastic change in a narrow temperature range. This strong nonlinear response allows to realize spontaneous electrical oscillations in the megahertz range under a DC voltage bias. These electrical oscillations are employed to set into mechanical resonance a microstructure without the need of any active electronics, with small power consumption and with the possibility to selectively excite specific flexural modes by tuning the value of the DC electrical bias in a range of few hundreds of millivolts. This actuation method is robust and flexible and can be implemented in a variety of autonomous DC-powered devices.@en

Nucleation processes of mixed-phase states are an intrinsic characteristic of first-order phase transitions, typically related to local symmetry breaking. Direct observation of emerging mixed-phase regions in materials showing a first-order metal-insulator transition (MIT) offers unique opportunities to uncover their driving mechanism. Using photoemission electron microscopy, we image the nanoscale formation and growth of insulating domains across the temperature-driven MIT in NdNiO3 epitaxial thin films. Heteroepitaxy is found to strongly determine the nanoscale nature of the phase transition, inducing preferential formation of striped domains along the terraces of atomically flat stepped surfaces. We show that the distribution of transition temperatures is a local property, set by surface morphology and stable across multiple temperature cycles. Our data provide new insights into the MIT of heteroepitaxial nickelates and point to a rich, nanoscale phenomenology in this strongly correlated material.@en

Obtaining high-quality thin films of 5d transition metal oxides is essential to explore the exotic semimetallic and topological phases predicted to arise from the combination of strong electron correlations and spin-orbit coupling. Here, we show that the transport properties of SrIrO3 thin films, grown by pulsed laser deposition, can be optimized by considering the effect of laser-induced modification of the SrIrO3 target surface. We further demonstrate that bare SrIrO3 thin films are subject to degradation in air and are highly sensitive to lithographic processing. A crystalline SrTiO3 cap layer deposited in-situ is effective in preserving the film quality, allowing us to measure metallic transport behavior in films with thicknesses down to 4 unit cells. In addition, the SrTiO3 encapsulation enables the fabrication of devices such as Hall bars without altering the film properties, allowing precise (magneto)transport measurements on micro- and nanoscale devices.@en

We investigate the thickness-dependent electronic properties of ultrathin SrIrO3 and discover a transition from a semimetallic to a correlated insulating state below 4 unit cells. Low-temperature magnetoconductance measurements show that spin fluctuations in the semimetallic state are significantly enhanced while approaching the transition point. The electronic properties are further studied by scanning tunneling spectroscopy, showing that 4 unit cell SrIrO3 is on the verge of a gap opening. Our density functional theory calculations reproduce the critical thickness of the transition and show that the opening of a gap in ultrathin SrIrO3 requires antiferromagnetic order.@en

Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We measure the dynamics of the lattice and that of the charge disproportionation in NdNiO3, when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO3 substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the NdNiO3 film, followed by a sonic lattice wave. When combined with measurements of magnetic disordering and of the metal-insulator transition, these results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces.@en

Relating the band structure of correlated semimetals to their transport properties is a complex and often open issue. The partial occupation of numerous electron and hole bands can result in properties that are seemingly in contrast with one another, complicating the extraction of the transport coefficients of different bands. The 5d oxide SrIrO3 hosts parabolic bands of heavy holes and light electrons in gapped Dirac cones due to the interplay between electron-electron interactions and spin-orbit coupling. We present a multifold approach relying on different experimental techniques and theoretical calculations to disentangle its complex electronic properties. By combining magnetotransport and thermoelectric measurements in a field-effect geometry with first-principles calculations, we quantitatively determine the transport coefficients of different conduction channels. Despite their different dispersion relationships, electrons and holes are found to have strikingly similar transport coefficients, yielding a holelike response under field-effect and thermoelectric measurements and a linear electronlike Hall effect up to 33 T.@en