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Duncan K. Maude

Publications and source records attributed to Duncan K. Maude.

16 recordsLinked to original sources

Electrostatic gate-controlled quantum interference in a high-mobility two-dimensional electron gas at the (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)O$_3$/SrTiO$_3$ interface

We report quantum oscillations in magnetoresistance that are periodic in magnetic field ($B$), observed at the interface between (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)O$_3$ and SrTiO$_3$. Unlike Shubnikov-de Haas oscillations, which appear at magnetic fields $ > 7$ T and diminish quickly as the temperature rises, these $B$-periodic oscillations emerge at low fields and persist up to 10 K. Their amplitude decays exponentially with both temperature and field, specifying dephasing of quantum interference. Increasing the carrier density through electrostatic gating results in a systematic reduction in both the amplitude and frequency of the oscillations, with complete suppression beyond a certain gate voltage. We attribute these oscillations to the Altshuler-Aronov-Spivak effect, likely arising from naturally formed closed-loop paths due to the interconnected quasi-one-dimensional conduction channels along SrTiO$_3$ domain walls. The relatively long phase coherence length ($\sim$ 1.8 $μ$m at 0.1 K), estimated from the oscillation amplitude, highlights the potential of complex oxide interfaces as a promising platform for exploring quantum interference effects and advancing device concepts in quantum technologies, such as mesoscopic interferometers and quantum sensors.

cond-mat.mes-hall

Spin injection and emission helicity switching in a 2D perovskite/WSe2 heterostructure

The initialization and control of a long-lived spin population in lead halide perovskites are prerequisites for their use in spintronic applications. Here, we demonstrate circular polarization of the interlayer exciton emission in a (BA)2PbI4/WSe2 monolayer heterostructure. The helicity of this emission is controlled by tuning the energy of the excitation laser through the manifold of exciton resonances of the WSe2 monolayer, together with an emerging interlayer absorption feature of the heterostructure. Theoretical calculations show that this resonance arises from hybridized (BA)2PbI4/WSe2 states in the valence band. This hybrid character enables its observation in both linear absorption and ultrafast pump-probe spectroscopies, and plays a key role in controlling the sign of the helicity of the interlayer exciton emission. The tunable spin polarization demonstrated here, with the WSe2 monolayer effectively acting as a tunable spin filter, represents an important step toward the use of 2D perovskites in opto-spintronic applications.

cond-mat.mtrl-sci

Possible evidence for Harper broadening in the yellow exciton series of Cu2O at ultrahigh magnetic fields

Hydrogen-like systems in ultra-high magnetic fields are of significant interest in interdisciplinary research. Previous studies have focused on the exciton wavefunction shrinkage under magnetic fields down to artificial crystal lattices (e.g., quantum wells, superlattices), where the effective mass approximation remains valid. However, further compression toward the natural crystal lattice scale remains experimentally challenging. In this study, we report magneto-absorption measurements on the yellow-exciton series in Cu2O using pulsed magnetic fields of up to 500 T. The strong low energy absorption features are assigned to the spin Zeeman split 2p0 and 3p0 exciton states. The high field data provides a value for the reduced effective mass of the exciton u* = 0.415 \pm 0.01me. Intriguingly, the broadening of the 2p0 ground state transition exhibits a sudden increase for ultrahigh magnetic fields above 300 T, providing possible evidence for Harper broadening - an indication of the breakdown of the effective mass approximation when the magnetic length becomes comparable to the lattice constant of the crystal.

cond-mat.mtrl-sci

Quadrupolar Excitons in MoSe$_2$ Bilayers

The quest for platforms to generate and control exotic excitonic states has greatly benefited from the advent of transition metal dichalcogenide (TMD) monolayers and their heterostructures. Among the unconventional excitonic states, quadrupolar excitons - a superposition of two dipolar excitons with anti-aligned dipole moments - are of great interest for applications in quantum simulations and for the investigation of many-body physics. Here, we unambiguously demonstrate the emergence of quadrupolar excitons in natural MoSe$_2$ homobilayers, whose energy shifts quadratically in electric field. In contrast to trilayer systems, MoSe$_2$ homobilayers have many advantages, which include a larger coupling between dipolar excitons. Our experimental observations are complemented by many-particle theory calculations offering microscopic insights in the formation of quadrupolar excitons. Our results suggest TMD homobilayers as ideal platform for the engineering of excitonic states and their interaction with light and thus candidate for carrying out on-chip quantum simulations.

cond-mat.mes-hall

Approaching the Intrinsic Properties of Moiré Structures Using Atomic Force Microscopy Ironing

Stacking monolayers of transition metal dichalcogenides (TMDs) has led to the discovery of a plethora of new exotic phenomena, resulting from moiré pattern formation. Due to the atomic thickness and high surface-to-volume ratio of heterostructures, the interfaces play a crucial role. Fluctuations in the interlayer distance affect interlayer coupling and moiré effects. Therefore, to access the intrinsic properties of the TMD stack, it is essential to obtain a clean and uniform interface between the layers. Here, we show that this is achieved by ironing with the tip of an atomic force microscope. This post-stacking procedure dramatically improves the homogeneity of the interfaces, which is reflected in the optical response of the interlayer exciton. We demonstrate that ironing improves the layer coupling, enhancing moiré effects and reducing disorder. This is crucial for the investigation of TMD heterostructure physics, which currently suffers from low reproducibility.

cond-mat.mes-hall

Unveiling the double-peak structure of quantum oscillations in the specific heat

Quantum oscillation phenomenon is an essential tool to understand the electronic structure of quantum matter. Here we report a systematic study of quantum oscillations in the electronic specific heat $C_{el}$ in natural graphite. We show that the crossing of a single spin Landau level and the Fermi energy give rise to a double-peak structure, in striking contrast to the single peak expected from Lifshitz-Kosevich theory. Intriguingly, the double-peak structure is predicted by the kernel term for $C_{el}/T$ in the free electron theory. The $C_{el}/T$ represents a spectroscopic tuning fork of width 4.8 $k_B T$ which can be tuned at will to resonance. Using a coincidence method, the double-peak structure can be used to accurately determine the Lande $g$-factor of quantum materials. More generally, the tuning fork can be used to reveal any peak in fermionic density of states tuned by magnetic field, such as Lifshitz transition in heavy-fermion compounds.

physics.app-ph

Symmetry breakdown in franckeite: spontaneous strain, rippling and interlayer moiré

Franckeite is a naturally occurring layered mineral with a structure composed of alternating stacks of SnS2-like and PbS-like layers. Although this superlattice is composed of a sequence of isotropic two-dimensional layers, it exhibits a spontaneous rippling that makes the material structurally anisotropic. We demonstrate that this rippling comes hand in hand with an inhomogeneous in-plane strain profile and anisotropic electrical, vibrational and optical properties. We argue that this symmetry breakdown results from a spatial modulation of the van der Waals interaction between layers due to the SnS2-like and PbS-like lattices incommensurability.

cond-mat.mes-hall

Giant Fine Structure Splitting of the Bright Exciton in a Bulk MAPbBr$_3$ Single Crystal

Exciton fine structure splitting in semiconductors reflects the underlying symmetry of the crystal and quantum confinement. Since the latter factor strongly enhances the exchange interaction, most work has focused on nanostructures. Here, we report on the first observation of the bright exciton fine structure splitting in a bulk semiconductor crystal, where the impact of quantum confinement can be specifically excluded, giving access to the intrinsic properties of the material. Detailed investigation of the exciton photoluminescence and reflection spectra of a bulk methylammonium lead tribromide single crystal reveals a zero magnetic field splitting as large as $\sim 200μ$eV. This result provides an important starting point for the discussion of the origin of the large bright exciton fine structure observed in perovskite nanocrystals.

cond-mat.mes-hall

Phase Transition Induced Carrier Mass Enhancement in 2D Ruddlesden-Popper Perovskites

There is a variety of possible ways to tune the optical properties of 2D perovskites, though the mutual dependence between different tuning parameters hinders our fundamental understanding of their properties. In this work we attempt to address this issue for (C$_n$H$_{2n+1}$NH$_3$)$_2$PbI$_4$ (with n=4,6,8,10,12) using optical spectroscopy in high magnetic fields up to 67T. Our experimental results, supported by DFT calculations, clearly demonstrate that the exciton reduced mass increases by around 30% in the low temperature phase. This is reflected by a 2-3 fold decrease of the diamagnetic coefficient. Our studies show that the effective mass, which is an essential parameter for optoelectronic device operation, can be tuned by the variation of organic spacers and/or moderate cooling achievable using Peltier coolers. Moreover, we show that the complex absorption features visible in absorption/transmission spectra track each other in magnetic field providing strong evidence for the phonon related nature of the observed side bands.

cond-mat.mes-hall

Moiré Intralayer Excitons in a MoSe$_2$/MoS$_2$ Heterostructure

Spatially periodic structures with a long range period, referred to as moiré pattern, can be obtained in van der Waals bilayers in the presence of a small stacking angle or of lattice mismatch between the monolayers. Theoretical predictions suggest that the resulting spatially periodic variation of the band structure modifies the optical properties of both intra and interlayer excitons of transition metal dichalcogenides heterostructures. Here, we report on the impact of the moiré pattern formed in a MoSe$_2$/MoS$_2$ heterobilayer encapsulated in hexagonal boron nitride. The periodic in-plane potential results in a splitting of the MoSe$_2$ exciton and trion in both emission and absorption spectra. The observed energy difference between the split peaks is fully consistent with theoretical predictions.

cond-mat.mes-hall

Intervalley Scattering of Interlayer Excitons in a MoS$_2$/MoSe$_2$/MoS$_2$ Heterostructure in High Magnetic Field

Degenerate extrema in the energy dispersion of charge carriers in solids, also referred to as valleys, can be regarded as a binary quantum degree of freedom, which can potentially be used to implement valleytronic concepts in van der Waals heterostructures based on transition metal dichalcogenides. Using magneto-photoluminescence spectroscopy, we achieve a deeper insight into the valley polarization and depolarization mechanisms of interlayer excitons formed across a MoS$_2$/MoSe$_2$/MoS$_2$ heterostructure. We account for the non-trivial behavior of the valley polarization as a function of the magnetic field by considering the interplay between exchange interaction and phonon mediated intervalley scattering in a system consisting of Zeeman-split energy levels. Our results represent a crucial step towards the understanding of the properties of interlayer excitons, with strong implications for the implementation of atomically thin valleytronic devices.

cond-mat.mes-hall

Probing Landau levels of strongly interacting massive Dirac electrons in layer-polarized MoS$_2$

Monolayer transition metal dichalcogenides are recently emerged 2D electronic systems with various novel properties, such as spin-valley locking, circular dichroism, valley Hall effects, Ising superconductivity. The reduced dimensionality and large effective masses further produce unconventional many-body interaction effects. Although recent hole transport measurements in WSe$_2$ indicate strong interactions in the valence bands, many-body interaction effects, particularly in the conduction bands, remain elusive to date. Here, for the first time, we perform transport measurements up to a magnetic field of $29$T to study the massive Dirac electron Landau levels (LL) in layer-polarized MoS$_2$ samples with mobilities of $22000$cm$^2$/(V$\cdot$s) at $1.5$K and densities of $\sim10^{12}$cm$^{-2}$. With decreasing the density, we observe LL crossing induced valley ferrimagnet-to-ferromagnet transitions, as a result of the interaction enhancement of the g-factor from $5.64$ to $21.82$. Near integer ratios of Zeeman-to-cyclotron energies, we discover LL anticrossings due to the formation of quantum Hall Ising ferromagnets, the valley polarizations of which appear to be reversible by tuning the density or an in-plane magnetic field. Our results provide compelling evidence for many-body interaction effects in the conduction bands of monolayer MoS$_2$ and establish a fertile ground for exploring strongly correlated phenomena of massive Dirac electrons.

cond-mat.mes-hall

Defect healing and charge transfer mediated valley polarization in MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructures

Monolayer transition metal dichalcogenides (TMDC) grown by chemical vapor deposition (CVD) are plagued by a significantly lower optical quality compared to exfoliated TMDC. In this work we show that the optical quality of CVD-grown MoSe$_2$ is completely recovered if the material is sandwiched in MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructures. We show by means of density-functional theory that this remarkable and unexpected result is due to defect healing: S atoms of the more reactive MoS$_2$ layers are donated to heal Se vacancy defects in the middle MoSe$_2$ layer. In addition, the trilayer structure exhibits a considerable charge-transfer mediated valley polarization of MoSe$_2$ without the need for resonant excitation. Our fabrication approach, relying solely on simple flake transfer technique, paves the way for the scalable production of large-area TMDC materials with excellent optical quality.

cond-mat.mes-hall

Unraveling the exciton binding energy and the dielectric constant in single crystal methylammonium lead tri-iodide perovskite

We have accurately determined the exciton binding energy and reduced mass of single crystals of methylammonium lead tri-iodide using magneto-reflectivity at very high magnetic fields. The single crystal has excellent optical properties with a narrow line width of $\sim 3$meV for the excitonic transitions and a 2s transition which is clearly visible even at zero magnetic field. The exciton binding energy of $16 \pm 2$meV in the low temperature orthorhombic phase is almost identical to the value found in polycrystalline samples, crucially ruling out any possibility that the exciton binding energy depends on the grain size. In the room temperature tetragonal phase, an upper limit for the exciton binding energy of $12 \pm 4$ meV is estimated from the evolution of 1s-2s splitting at high magnetic field.

cond-mat.mtrl-sci

How Graphene-like is Epitaxial Graphene? \\Quantum Oscillations and Quantum Hall Effect

We investigate the transport properties of high-quality single-layer graphene, epitaxially grown on a 6H-SiC(0001) substrate. We have measured transport properties, in particular charge carrier density, mobility, conductivity and magnetoconductance of large samples as well as submicrometer-sized Hall bars which are entirely lying on atomically flat substrate terraces. The results display high mobilities, independent of sample size and a Shubnikov-de Haas effect with a Landau level spectrum of single-layer graphene. When gated close to the Dirac point, the mobility increases substantially, and the graphene-like quantum Hall effect occurs. This proves that epitaxial graphene is ruled by the same pseudo-relativistic physics observed previously in exfoliated graphene.

cond-mat.mes-hall

Approaching the Dirac point in high mobility multi-layer epitaxial graphene

Multi-layer epitaxial graphene (MEG) is investigated using far infrared (FIR) transmission experiments in the different limits of low magnetic fields and high temperatures. The cyclotron-resonance like absorption is observed at low temperature in magnetic fields below 50 mT, allowing thus to probe the nearest vicinity of the Dirac point and to estimate the conductivity in nearly undoped graphene. The carrier mobility is found to exceed 250,000 cm$^2$/(V.s). In the limit of high temperatures, the well-defined Landau level (LL) quantization is observed up to room temperature at magnetic fields below 1 T, a phenomenon unique in solid state systems. A negligible increase in the width of the cyclotron resonance lines with increasing temperature indicates that no important scattering mechanism is thermally activated, supporting recent expectations of high room-temperature mobilities in graphene.

cond-mat.other