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Gabriel Aeppli

Publications and source records attributed to Gabriel Aeppli.

At least 19 recordsLinked to original sources

Kinetics of electron-phonon scattering in silicon resolved by Rydberg transitions of donors

Rydberg states of atoms in vacuum are now well recognized as a resource for quantum technologies. Donors in semiconductors also display analogous states, which have been proposed for similar applications. While they benefit from permanent locations in their host crystals, electron-lattice coupling leads to much shorter excited-state lifetimes than for neutral atoms in vacuum. Here we provide a quantitative description of donor-phonon kinetics, creating a basis for engineering donor systems in realistic material stacks for quantum devices. Our theory incorporates both form factors for the Rydberg states, which given their large extents in real space provide strong selectivity in momentum space, and tabulated deformation potentials for all six phonon branches throughout the Brillouin zone. By confronting this framework with carefully controlled time-resolved free electron laser measurements, we show that the widely quoted position of the silicon conduction band minimum, $k_0$, is inconsistent with observed donor relaxation rates and that quantitative agreement is obtained for a value further from the X-point than commonly assumed. This stringent experiment-theory comparison establishes donor relaxation as a precision metrology for conduction band parameters and scattering processes in silicon, with consequences spanning from quantum devices to classical electronics.

quant-ph

Analog-Digital Quantum Computing with Quantum Annealing Processors

Quantum annealing processors typically control qubits in unison, attenuating quantum fluctuations uniformly until the applied system Hamiltonian is diagonal in the computational basis. This simplifies control requirements, allowing annealing QPUs to scale to much larger sizes than gate-based systems, but constraining the class of available operations. Here we expand the class by performing analog-digital quantum computing in a highly-multiplexed, superconducting quantum annealing processor. This involves evolution under a fixed many-body Hamiltonian that, in the weak-coupling regime, is well-described by an effective XY model, together with arbitrary-basis initialization and measurement via auxiliary qubits. Operationally, this is equivalent to implementing single-qubit gates at the beginning and end of an analog quantum evolution. We demonstrate this capability with several foundational applications: single-qubit and two-qubit coherent oscillations with varying initialization and measurement bases, a multi-qubit quantum walk with fermionic dispersion in line with theory, and Anderson localization in a disordered chain. These experiments open the door to a wide range of new possibilities in quantum computation and simulation, greatly expanding the applications of commercially available quantum annealing processors.

quant-ph

Rapid high-temperature initialisation and readout of spins in silicon with 10 THz photons

Each cycle of a quantum computation requires a quantum state initialisation. For semiconductor-based quantum platforms, initialisation is typically performed via slow microwave processes and usually requires cooling to temperatures where only the lowest quantum level is occupied. In silicon, boron atoms are the most common impurities. They bind holes in orbitals including an effective spin-3/2 ground state as well as excited states analogous to the Rydberg series for hydrogen. Here we show that initialisation temperature demands may be relaxed and speeds increased over a thousand-fold by importing, from atomic physics, the procedure of optical pumping via excited orbital states to preferentially occupy a target ground state spin. Spin relaxation within the orbital ground state of unstrained silicon is too fast to measure for conventional pulsed microwave technology, except at temperatures below 2 K, implying a need not only for fast state preparation but also fast state readout. Circularly polarised ~10 THz photon pulses from a free electron laser meet both needs at temperatures above 3 K: a 9 ps pulse enhances the population of one spin eigenstate for the "1s"-like ground state orbital, and the second interrogates this imbalance in spin population. Using parameters given by our data, we calculate that it should be possible to initialise 99% of spins for boron in strained silicon within 250 ps at 3 K. The speedup of both state preparation and measurement gained for THz rather than microwave photons should be explored for the many other solid state quantum systems hosting THz excitations potentially useful as intermediate states.

quant-ph

Quantum Printing

We introduce the concept of quantum printing -- the imprinting of quantum states from photons and phonons onto quantum matter. The discussion is focusing on charged fluids (metals, superconductors, Hall fluids) and neutral systems (magnets, excitons). We demonstrate how structured light can generate topological excitations, including vortices in superconductors and skyrmions in magnets. We also discuss how quantum printing induces magnetization in quantum paraelectrics and strain-mediated magnetization in Dirac materials. Finally, we propose future applications, such as printing entangled photon states, creating entangled topological excitations, and discuss applications of quantum printing to light induced quantum turbulence in a charged fluid. This review represents the expanded version of the shorter review submitted to Nature Physics.

quant-ph

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 $\delta$-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

Tunable, phase-locked hard X-ray pulse sequences generated by a free-electron laser

The ability to arbitrarily dial in amplitudes and phases enables the fundamental quantum state operations pioneered for microwaves and then infrared and visible wavelengths during the second half of the last century. Self-seeded X-ray free-electron lasers (FELs) routinely generate coherent, high-brightness, and ultrafast pulses for a wide range of experiments, but have so far not achieved a comparable level of amplitude and phase control. Here we report the first tunable phase-locked, ultra-fast hard X-ray (PHLUX) pulses by implementing a recently proposed method: A fresh-bunch self-seeded FEL, driven by an electron beam that was shaped with a slotted foil and a corrugated wakefield structure, generates coherent radiation that is intensity-modulated on the femtosecond time scale. We measure phase-locked (to within a shot-to-shot phase jitter corresponding to 0.1 attoseconds) pulse triplets with a photon energy of 9.7 keV, a pulse energy of several tens of microjoules, a freely tunable relative phase, and a pulse delay tunability between 4.5 and 11.9 fs. Such pulse sequences are suitable for a wide range of applications, including coherent spectroscopy, and have amplitudes sufficient to enable hard X-ray quantum optics experiments. More generally, these results represent an important step towards a hard X-ray arbitrary waveform generator.

physics.acc-ph

Effect of Interlayer Stacking on the Electronic Properties of 1$T$-TaS$_2$

Controlled stacking of van der Waals materials is a powerful tool for exploring the physics of quantum condensed matter. Given the small binding between layers, exploitation for engineering will require a breakthrough in stacking methodology, or an ability to take advantage of thicker defective stacks. Here we describe computational groundwork for the latter, using -- on account of its promise for cold memory applications -- 1$T$-TaS$_2$ as a model system. Comparing recursive Hendricks-Teller calculations and Monte Carlo simulations to published X-ray diffraction data, we obtain the key parameters describing the random stacking in mesoscopic flakes. These then regulate the electronic structures via specification of the random stacks in dynamical mean-field theory simulations. Hubbard repulsion induces strongly correlated metallic, band and Mott insulating layers, providing compelling evidence that electronic properties follow from the coexistence of more than the metallic and insulating planes associated by ordinary band theory.

cond-mat.str-el

Roadmap on Atomic-scale Semiconductor Devices

Spin states in semiconductors provide exceptionally stable and noise-resistant environments for qubits, positioning them as optimal candidates for reliable quantum computing technologies. The proposal to use nuclear and electronic spins of donor atoms in silicon, introduced by Kane in 1998, sparked a new research field focused on the precise positioning of individual impurity atoms for quantum devices, utilising scanning tunnelling microscopy and ion implantation. This roadmap article reviews the advancements in the 25 years since Kane's proposal, the current challenges, and the future directions in atomic-scale semiconductor device fabrication and measurement. It covers the quest to create a silicon-based quantum computer and expands to include diverse material systems and fabrication techniques, highlighting the potential for a broad range of semiconductor quantum technological applications. Key developments include phosphorus in silicon devices such as single-atom transistors, arrayed few-donor devices, one- and two-qubit gates, three-dimensional architectures, and the development of a toolbox for future quantum integrated circuits. The roadmap also explores new impurity species like arsenic and antimony for enhanced scalability and higher-dimensional spin systems, new chemistry for dopant precursors and lithographic resists, and the potential for germanium-based devices. Emerging methods, such as photon-based lithography and electron beam manipulation, are discussed for their disruptive potential. This roadmap charts the path toward scalable quantum computing and advanced semiconductor quantum technologies, emphasising the critical intersections of experiment, technological development, and theory.

quant-ph

Imaging of electrically controlled van der Waals layer stacking in 1T-TaS2

Van der Waals (vdW) materials exhibit a variety of states that can be switched with low power at low temperatures, offering a viable cryogenic "flash memory" required for the classical control electronics for solid-state quantum information processing. In 1T-TaS2, a non-volatile metallic 'hidden' state can be induced from an insulating equilibrium charge-density wave ground state using either optical or electrical pulses. Given that conventional memristors form localized, filamentary channels which support the current, a key question for design concerns the geometry of the conduction region in highly energy-efficient 1T-TaS2 devices. Here, we report in operando micro-beam X-ray diffraction, fluorescence, and concurrent transport measurements, allowing us to spatially image the non-thermal hidden state induced by electrical switching of 1T-TaS2. Our results reveal a long-range ordered, non-filamentary switched state that extends well below the electrodes, implying that the self-organized, collective growth of the hidden phase is driven by a combination of charge flow and lattice strain. Our unique combination of techniques showcases the potential of non-destructive, three-dimensional X-ray imaging to study bulk switching properties in microscopic detail, namely electrical control of the vdW layer stacking.

cond-mat.str-el

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$5 nm and greater using sophisticated tools such as X-ray diffraction, high energy X-ray photoemission spectroscopy, and secondary ion mass spectrometry. However, profiling thin layers with nm or sub-nm thickness, e.g. atomically thin dopant layers ($\delta$-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 $\delta$-layers within silicon, and show that the sub-nm electronic thickness of the $\delta$-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

Large inverse Faraday effect for Rydberg states of free atoms and isolated donors in semiconductors

We report on the induction of magnetization in Rydberg systems by means of the inverse Faraday effect, and propose the appearance of the effect in two such systems, Rydberg atoms proper and shallow dopants in semiconductors. Rydberg atoms are characterized by a large orbital radius. This large radius gives such excited states a large angular moment, which when driven with circularly polarized light, translates to a large effective magnetic field ${B}_{\text{eff}}$. We calculate this effect to generate effective magnetic fields of $O(1\,\mu\text{T})\times\left( \frac{\omega}{1\,\text{THz}} \right)^{-1} \left( \frac{I}{10\,\text{W cm}^{-2}} \right) n^4$ in the Rydberg states of atoms such as Rb and Cs for off-resonant photon beams with frequency omega and intensity ${I}$ expressed in units of the denominators and $n$ the principal quantum number. Additionally, terahertz spectroscopy of phosphorus doped silicon reveals a large cross-section for excitation of shallow dopants to Rydberg-like states, which even for small $n$ have the potential to be driven similarly with circularly polarized light to produce an even larger magnetization. Our theoretical calculations estimate ${B}_{\text{eff}}$ as $O(10^2\,\text{T})$ for Si:P with a beam intensity of $10^8\,\text{W cm}^{-2}$.

physics.atom-ph

Resistless EUV lithography: photon-induced oxide patterning on silicon

In this work, we show the feasibility of extreme ultraviolet (EUV) patterning on an HF-treated Si(100) surface in the absence of a photoresist. EUV lithography is the leading lithography technique in semiconductor manufacturing due to its high resolution and throughput, but future progress in resolution can be hampered because of the inherent limitations of the resists. We show that EUV photons can induce surface reactions on a partially H-terminated Si surface and assist the growth of an oxide layer, which serves as an etch mask. This mechanism is different from the H-desorption in scanning tunneling microscopy-based lithography. We achieve SiO2/Si gratings with 75 nm half-pitch and 31 nm height, demonstrating the efficacy of the method and the feasibility of patterning with EUV lithography without the use of a photoresist. Further development of the resistless EUV lithography method can be a viable approach to nm-scale lithography by overcoming the inherent resolution and roughness limitations of photoresist materials.

physics.app-ph

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

Two-dimensional dopant layers ($\delta$-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 $\delta$-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 $\delta$-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 $\delta$-layers of arsenic exhibit better electronic confinement than $\delta$-layers of phosphorus fabricated under identical conditions.

cond-mat.mtrl-sci

Impact of static disorder on quasiparticle spectra: Debye-Waller, mean free path and potential fluctuation effects

ARPES is a widely used characterization technique in condensed matter physics, providing direct access to the single-electron spectral function of crystals, including their electronic band structure and Fermi surface. Measuring the band structure of novel quantum materials has been fundamentally important for determining, for example, non-trivial band topology or for identifying new classes of materials. A key challenge with these emerging quantum materials is that their initial crystalline quality is rarely optimized, which directly affects the spectra measured by ARPES. Here, we present a theoretical framework and experimental evidence addressing two common consequences of static disorder in photoemission experiments: the loss of coherent spectral weight and the broadening of spectral features. ARPES spectra can be understood as a sum of coherent and incoherent intensities, with their relative contributions controlled by atomic disorder. Under thermal disorder, the coherent intensity is exponentially suppressed as temperature increases, a phenomenon analogous to the Debye-Waller factor in diffraction, where Bragg peaks diminish in favor of diffuse scattering as disorder increases. In this work, we report a soft X-ray study of the deliberately disordered (via Ar ion sputtering) InAs(110) surface, characterized both by STM and LEED. We introduce a new framework that enables quantification of coherent photoemission intensity loss with increasing disorder, allowing both thermal and static disorder to be treated within a unified approach. Additionally, we identify a second major effect of disorder beyond lifetime broadening: inhomogeneous spectral broadening arising from local potential fluctuations. We show that such fluctuations increase the linewidths of the spectra of localized and delocalized states, and contribute to the suppression of ARPES intensity from states near the Fermi level.

cond-mat.mtrl-sci

Spin waves and orbital contribution to ferromagnetism in a topological metal

Special arrangements of atoms with more than one atom per unit cell, including honeycomb or kagome (woven bamboo mat) lattices, can host propagating excitations with non-trivial topology as defined by their evolution along closed paths in momentum space. Excitations on such lattices can also be momentum-independent, meaning that they are localized notwithstanding strong hopping of the underlying disturbances between neighbouring sites. The associated flat bands are interesting because the interactions between the heavy quasiparticles inhabiting them will become much more important than for strong dispersion, resulting in novel quantum solid and liquid states. Different stackings of two-dimensional lattices, for example twisted graphene bilayers, provide routes to further engineer topology and many-body effects. Here, we report the discovery, using circularly polarized x-rays for the unambiguous isolation of magnetic signals, of a nearly flat spin wave band and large (compared to elemental iron) orbital moment for the metallic ferromagnet Fe3Sn2, built from compact AB-stacked kagome bilayers and which has a topologically non-trivial electronic band structure controllable by modest external magnetic fields. As a function of out-of-plane momentum, the nearly flat optical mode and the global rotation symmetry-restoring acoustic mode are out of phase, consistent with a bilayer exchange coupling that is larger than the already large in-plane couplings. The defining units of this topological metal are therefore a triangular lattice of octahedral iron clusters rather than weakly coupled kagome planes. The spin waves are strongly damped when compared to elemental iron, opening the topic of interactions of topological bosons (spin waves) and fermions (electrons) with the very specific target of explaining boson lifetimes.

cond-mat.str-el

Transfer Learning Application of Self-supervised Learning in ARPES

Recent development in angle-resolved photoemission spectroscopy (ARPES) technique involves spatially resolving samples while maintaining the high-resolution feature of momentum space. This development easily expands the data size and its complexity for data analysis, where one of it is to label similar dispersion cuts and map them spatially. In this work, we demonstrate that the recent development in representational learning (self-supervised learning) model combined with k-means clustering can help automate that part of data analysis and save precious time, albeit with low performance. Finally, we introduce a few-shot learning (k-nearest neighbour or kNN) in representational space where we selectively choose one (k=1) image reference for each known label and subsequently label the rest of the data with respect to the nearest reference image. This last approach demonstrates the strength of the self-supervised learning to automate the image analysis in ARPES in particular and can be generalized into any science data analysis that heavily involves image data.

physics.ins-det

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 $\sim1~\mu$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

Kapitza stabilization of quantum critical order

Dynamical perturbations modify the states of classical systems in surprising ways and give rise to important applications in science and technology. For example, Floquet engineering exploits the possibility of band formation in the frequency domain when a strong, periodic variation is imposed on parameters such as spring constants. We describe here Kapitza engineering, where a drive field oscillating at a frequency much higher than the characteristic frequencies for the linear response of a system changes the potential energy surface so much that maxima found at equilibrium become local minima, in precise analogy to the celebrated Kapitza pendulum where the unstable inverted configuration, with the mass above rather than below the fulcrum, actually becomes stable. Our starting point is a quantum field theory of the Ginzburg-Devonshire type, suitable for many condensed matter systems, including particularly ferroelectrics and quantum paralectrics. We show that an off-resonance oscillatory electric field generated by a laser-driven THz source can induce ferroelectric order in the quantum-critical limit. Heating effects are estimated to be manageable using pulsed radiation; ``hidden" radiation-induced order can persist to low temperatures without further pumping due to stabilization by strain. We estimate the Ginzburg-Devonshire free-energy coefficients in SrTiO${}_{3}$ using density-functional theory (DFT) and the stochastic self-consistent harmonic approximation accelerated by a machine-learned force field. Although we find that SrTiO${}_{3}$ is not an optimal choice for Kapitza stabilization, we show that scanning for further candidate materials can be performed at the computationally convenient density-functional theory level. We suggest second-harmonic-generation, soft-mode-spectroscopy, and X-ray-diffraction experiments to characterize the induced order.

cond-mat.str-el