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Nicolò D'Anna

Publications and source records attributed to Nicolò D'Anna.

7 recordsLinked to original sources

Dynamic nanoscale spatial heterogeneity in a perovskite to brownmillerite topotactic phase transformation

Phase transitions are omnipresent in modern condensed matter physics and its applications. In solids, first-order phase transformations typically occur by nucleation and growth under non-equilibrium conditions. Under constant external conditions, $\textit{e.g.}$, constant annealing temperature and pressure, the nucleation and growth dynamics are often thought of as spatially and temporally independent. Here, $\textit{in-situ}$ Bragg X-ray photon correlation spectroscopy (XPCS) reveals nanoscale spatial and dynamical heterogeneity in the perovskite-to-brownmillerite topotactic phase transformation in La$_{0.7}$Sr$_{0.3}$CoO$_3$ thin films annealed under constant reducing conditions over a time span of multiple hours. Specifically, a timescale associated with domain growth remains stable, with a corresponding domain wall speed of $v_d = 6 \pm 0.5 \times10^{-4}$~nm/s ($2 \pm 0.2$~nm/h), while a slower timescale, associated with temperature-driven de-pinning of domains, leads to accelerating dynamics with timescales following an aging power law with exponent -2.2$\pm$0.5. This experiment demonstrates that Bragg XPCS is a powerful tool to study nanoscale dynamics in structural phase transformations, with the ability to extract quantitative average values related to nano-domain motion $\textit{in-situ}$. The results are relevant for phase engineering of phase-change devices, as they show that nanoscale dynamics, linked to domain and domain-wall motion, can continuously evolve and speed up with time, even hours after the initiation of the phase transformation, with potential repercussions on electrical performance.

cond-mat.mtrl-sci↗

Jamming-controlled stochasticity in metal-insulator switching

Understanding and controlling phase transitions is a fundamental part of physics and has been central to many technological revolutions, from steam engines to field-effect transistors. At present, there is strong interest in materials with strongly coupled structural and electronic phase transitions, which hold promise for energy-efficient technologies. Utilizing a structural phase transition and controlling its plasticity naturally leads to built-in memory, a key feature for emulating neurons and synapses in neuromorphic technologies. Here, $\textit{operando}$ Bragg X-ray photon correlation spectroscopy is used to study the evolution of the nano-domain distribution at the micron-scale in neuromorphic devices made from the archetypal Mott insulator vanadium dioxide. It is found that after electrical switching, slow nano-domain reconfiguration occurs on timescales of thousands of seconds and that the domains undergo a jamming transition, offering control over switching stochasticity at the micron scale. More precisely, repetitive above-threshold currents plastically drive the system into a jammed/glassy state where switching becomes deterministic, while sub-threshold currents erase the short-term memory contained in the nano-domain distribution, recovering stochastic switching, thus offering a path for in-device learning. The results illustrate the importance of studying the nanoscale physics associated with phase transitions in strongly correlated materials, even for macroscopic devices, and offer guidance for future device operation schemes.

cond-mat.mes-hall↗

Strong electron-electron interactions in a dilute weakly-localized metal near a metal-to-insulator transition

Because it is easily switched from insulator to metal either via chemical doping or electrical gating, silicon is at the core of modern information technology and remains a candidate platform for quantum computing. The metal-to-insulator transition in this material has therefore been one of the most studied phenomena in condensed matter physics, and has been revisited with considerable profit each time a new fabrication technology has been introduced. Here we take advantage of recent advances in creating ultra-thin layers of Bohr-atom-like dopants to realize the two-dimensional disordered Hubbard model at half-filling and its metal-to-insulator transition (MIT) as a function of mean distance between atoms. We use gas-phase dosing of dopant precursor molecules on silicon to create arsenic and phosphorus $δ$-layers as thin as 0.4~nm and as dilute as 10$^{13}$~cm$^{-2}$. On approaching the insulating state, the conventional weak localization effects, prevalent at high dopant densities and due to orbital motion of the electrons in the plane, become dominated by electron-electron interaction contributions which obey a paramagnetic Zeeman scaling law. The latter make a negative contribution to the conductance, and thus cannot be interpreted in terms of an emergent Kondo regime near the MIT.

quant-ph↗

Self-strain suppression of the metal-to-insulator transition in phase-change oxide devices

Quantum materials exhibiting phase transitions which can be controlled through external stimuli, such as electric fields, are promising for future computing technologies beyond conventional semiconductor transistors. Devices that take advantage of structural phase transitions have inherent built-in memory, reminiscent of synapses and neurons, and are thus natural candidates for neuromorphic computing. Of particular interest are phase-change oxides, which allow for control over the metal-to-insulator transition. Here, we report X-ray nano-diffraction structural imaging of micro-devices fabricated with the archetypal phase-change material vanadium sesquioxide (V$_2$O$_3$). The devices contain a Ga ion-irradiated region where the metal-to-insulator transition critical temperature is lowered, a useful feature for controlling neuron-like spiking behavior. Results show that strain, induced by crystal lattice mismatch between the pristine and irradiated material, leads to a suppression of the metal-to-insulator-transition. Suppression occurs within the irradiated region or along its edges, depending on the defect-distribution and the size of the region. The observed self-straining effect could extend to other phase-change oxides and dominate as device dimensions are reduced and become too small to dissipate strain within the irradiated region. The findings are important for phase engineering in phase-change devices and highlight the necessity to study phase transitions at the nanoscale.

cond-mat.mes-hall↗

Element-specific, non-destructive profiling of layered heterostructures

Fabrication of semiconductor heterostructures is now so precise that metrology has become a key challenge for progress in science and applications. It is now relatively straightforward to characterize classic III-V and group IV heterostructures consisting of slabs of different semiconductor alloys with thicknesses of $\sim$5 nm and greater using sophisticated tools such as X-ray diffraction, high energy X-ray photoemission spectroscopy, and secondary ion mass spectrometry. However, profiling thin layers with nm or sub-nm thickness, e.g. atomically thin dopant layers ($δ$-layers), of impurities required for modulation doping and spin-based quantum and classical information technologies is more challenging. Here, we present theory and experiment showing how resonant-contrast X-ray reflectometry meets this challenge. The technique takes advantage of the change in the scattering factor of atoms as their core level resonances are scanned by varying the X-ray energy. We demonstrate the capability of the resulting element-selective, non-destructive profilometry for single arsenic $δ$-layers within silicon, and show that the sub-nm electronic thickness of the $δ$-layers corresponds to sub-nm chemical thickness. In combination with X-ray fluorescence imaging, this enables non-destructive three-dimensional characterization of nano-structured quantum devices. Due to the strong resonances at soft X-ray wavelengths, the technique is also ideally suited to characterize layered quantum materials, such as cuprates or the topical infinite-layer nickelates.

quant-ph↗

Momentum-space imaging of ultra-thin electron liquids in delta-doped silicon

Two-dimensional dopant layers ($δ$-layers) in semiconductors provide the high-mobility electron liquids (2DELs) needed for nanoscale quantum-electronic devices. Key parameters such as carrier densities, effective masses, and confinement thicknesses for 2DELs have traditionally been extracted from quantum magnetotransport. In principle, the parameters are immediately readable from the one-electron spectral function that can be measured by angle-resolved photoemission spectroscopy (ARPES). Here, buried 2DEL $δ$-layers in silicon are measured with soft X-ray (SX) ARPES to obtain detailed information about their filled conduction bands and extract device-relevant properties. This study takes advantage of the larger probing depth and photon energy range of SX-ARPES relative to vacuum ultraviolet (VUV) ARPES to accurately measure the $δ$-layer electronic confinement. The measurements are made on ambient-exposed samples and yield extremely thin ($\approx 1$ $nm$) and dense ($\approx$ $10^{14}$ $cm^2$) 2DELs. Critically, this method is used to show that $δ$-layers of arsenic exhibit better electronic confinement than $δ$-layers of phosphorus fabricated under identical conditions.

cond-mat.mtrl-sci↗

Non-destructive X-ray imaging of patterned delta-layer devices in silicon

The progress of miniaturisation in integrated electronics has led to atomic and nanometre-sized dopant devices in silicon. Such structures can be fabricated routinely by hydrogen resist lithography, using various dopants such as phosphorous and arsenic. However, the ability to non-destructively obtain atomic-species-specific images of the final structure, which would be an indispensable tool for building more complex nano-scale devices, such as quantum co-processors, remains an unresolved challenge. Here we exploit X-ray fluorescence to create an element-specific image of As dopants in silicon, with dopant densities in absolute units and a resolution limited by the beam focal size (here $\sim1~μ$m), without affecting the device's low temperature electronic properties. The As densities provided by the X-ray data are compared to those derived from Hall effect measurements as well as the standard non-repeatable, scanning tunnelling microscopy and secondary ion mass spectroscopy, techniques. Before and after the X-ray experiments, we also measured the magneto-conductance, dominated by weak localisation, a quantum interference effect extremely sensitive to sample dimensions and disorder. Notwithstanding the $1.5\times10^{10}$ Sv ($1.5\times10^{16}$ Rad/cm$^{-2}$) exposure of the device to X-rays, all transport data were unchanged to within experimental errors, corresponding to upper bounds of 0.2 Angstroms for the radiation-induced motion of the typical As atom and 3$\%$ for the loss of activated, carrier-contributing dopants. With next generation synchrotron radiation sources and more advanced optics, we foresee that it will be possible to obtain X-ray images of single dopant atoms within resolved radii of 5 nm.

quant-ph↗