Publications by authors named "Duncan Maude"

The mixed-valence compound YbB displays paradoxical quantum oscillations in electrical resistivity and magnetic torque in a regime with a well-developed insulating charge gap and in the absence of an electronic Fermi surface. However, signatures of such unusual fermionic quasiparticles in other bulk thermodynamic observables have been missing. Here we report the observation of a series of sharp double-peak features in the specific heat as a function of the magnetic field.

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In metal halide perovskites, the complex dielectric screening together with low energy of phonon modes leads to non-negligible Fröhlich coupling. While this feature of perovskites has already been used to explain some of the puzzling aspects of carrier transport in these materials, the possible impact of polaronic effects on the optical response, especially excitonic properties, is much less explored. Here, with the use of magneto-optical spectroscopy, we revealed the non-hydrogenic character of the excitons in metal halide perovskites, resulting from the pronounced Fröhlich coupling.

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Article Synopsis
  • The optical behavior of 2D perovskites relies heavily on excitons, which can be manipulated by altering the thickness of the perovskite layers.
  • Researchers studied the exciton fine structure in a specific 2D perovskite by varying the number of inorganic layers from 1 to 4.
  • Their findings reveal splitting of excitonic states across different confinement levels and show how the optical properties transition from 2D to 3D as the layer thickness increases.
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  • The optical response of 2D layered perovskites features closely spaced spectral signatures, interpreted as phonon replicas, with an energy separation ranging from 12 to 40 meV, depending on the material.
  • These materials also show a strong scattering response in resonant Raman spectroscopy above roughly 200 cm (or 25 meV), which is linked to the presence of polarons, exhibiting a distinctive spectral pattern deviating from the Rayleigh line.
  • A significant Huang-Rhys factor (S > 6) suggests strong coupling between charge carriers and the lattice, with polaron binding energies between 20-35 meV, influencing the optical properties critical for future opto-electronic applications.
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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 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.

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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.

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The optimized exploitation of perovskite nanocrystals and nanoplatelets as highly efficient light sources requires a detailed understanding of the energy spacing within the exciton manifold. Dark exciton states are particularly relevant because they represent a channel that reduces radiative efficiency. Here, we apply large in-plane magnetic fields to brighten optically inactive states of CsPbBr-based nanoplatelets for the first time.

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Applications of two-dimensional (2D) perovskites have significantly outpaced the understanding of many fundamental aspects of their photophysics. The optical response of 2D lead halide perovskites is dominated by strongly bound excitonic states. However, a comprehensive experimental verification of the exciton fine structure splitting and associated transition symmetries remains elusive.

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Article Synopsis
  • Optically inactive dark exciton states are crucial in semiconductor light emission as they provide a nonradiative recombination pathway.
  • Research on the exciton fine structure of two-dimensional perovskites (PEA)SnI, (PEA)PbI, and (PEA)PbBr shows that applying an in-plane magnetic field can mix these dark states with bright states, enhancing their visibility.
  • The observed hot photoluminescence suggests a non-Boltzmann distribution of exciton populations due to weak coupling between excitons and acoustic phonons, leading to strong emission despite significant bright-dark exciton splitting.
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van der Waals heterostructures are currently the focus of intense investigation; this is essentially due to the unprecedented flexibility offered by the total relaxation of lattice matching requirements and their new and exotic properties compared to the individual layers. Here, we investigate the hybrid transition-metal dichalcogenide/2D perovskite heterostructure WS/(PEA)PbI (where PEA stands for phenylethylammonium). We present the first density functional theory (DFT) calculations of a heterostructure ensemble, which reveal a novel band alignment, where direct electron transfer is blocked by the organic spacer of the 2D perovskite.

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Article Synopsis
  • The excitonic properties and band structure of atomically thin 2D perovskite crystals change significantly with thickness, allowing for new explorations in exciton physics.
  • Researchers examined the fundamental excitonic characteristics, such as reduced mass and binding energy, in 2D perovskites using high magnetic field optical spectroscopy.
  • Their findings challenge traditional ideas about quantum confinement, showing that the effective mass of carriers actually increases with the number of inorganic layers, indicating unique design potential for electronic properties in 2D perovskites.
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Lanthanide-doped nanoparticles enable conversion of near-infrared photons to visible ones. This property is envisioned as a basis of a broad range of applications: from optoelectronics, via energy conversion, to bio-sensing and phototherapy. The spectrum of applications can be extended if magnetooptical properties of lanthanide dopants are well understood.

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  • The family of 2D Ruddlesden-Popper perovskites is gaining significant attention for their potential in energy harvesting and light emission technologies.
  • Despite being known for decades, recent studies highlight that their optical properties are influenced by exciton-phonon coupling, largely affected by the organic spacers in the material.
  • This research reveals that the complex absorption spectra of a specific 2D perovskite (PEA)(CHNH)PbI are linked to a vibronic progression in excitonic transitions and a notable coupling to a high-energy phonon mode, likely stemming from the organic spacer's torsional motion.
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Franckeite is a naturally occurring layered mineral with a structure composed of alternating stacks of SnS-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.

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Article Synopsis
  • The study observes exciton fine structure splitting in a bulk semiconductor crystal, highlighting its intrinsic properties by excluding quantum confinement effects.
  • The research focuses on methylammonium lead tribromide single crystals, revealing a significant zero magnetic field splitting of about 200 μeV.
  • These findings serve as a foundation for understanding the large bright exciton fine structure splitting seen in perovskite nanocrystals.
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Two-dimensional transition metal dichalcogenides (TMDCs) are recently emerged electronic systems with various novel properties, such as spin-valley locking, circular dichroism, valley Hall effect, and superconductivity. The reduced dimensionality and large effective masses further produce unconventional many-body interaction effects. Here we reveal strong interaction effects in the conduction band of MoS by transport experiment.

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The encapsulation of two-dimensional layered materials such as black phosphorus is of paramount importance for their stability in air. However, the encapsulation poses several questions, namely, how it affects, via the weak van der Waals forces, the properties of the black phosphorus and whether these properties can be tuned on demand. Prompted by these questions, we have investigated the impact of hexagonal boron nitride encapsulation on the structural and vibrational properties of few layer black phosphorus, using a first-principles method in the framework of density functional theory.

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Spatially periodic structures with a long-range period, referred to as a 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 dichalcogenide heterostructures. Here, we report on the impact of the moiré pattern formed in a MoSe/MoS heterobilayer encapsulated in hexagonal boron nitride.

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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/MoSe/MoS heterostructure. We account for the nontrivial 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.

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Monolayer transition metal dichalcogenides (TMDCs) grown by chemical vapor deposition (CVD) are plagued by a significantly lower optical quality compared to exfoliated TMDCs. In this work, we show that the optical quality of CVD-grown MoSe is completely recovered if the material is sandwiched in MoS/MoSe/MoS 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 layers are donated to heal Se vacancy defects in the middle MoSe layer.

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We have accurately determined the exciton binding energy and reduced mass of single crystals of methylammonium lead triiodide using magneto-reflectivity at very high magnetic fields. The single crystal has excellent optical properties with a narrow line width of ∼3 meV for the excitonic transitions and a 2s transition that is clearly visible even at zero magnetic field. The exciton binding energy of 16 ± 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.

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The extent to which the soft structural properties of metal halide perovskites affect their optoelectronic properties is unclear. X-ray diffraction and micro-photoluminescence measurements are used to show that there is a coexistence of both tetragonal and orthorhombic phases through the low-temperature phase transition, and that cycling through this transition can lead to structural changes and enhanced optoelectronic properties.

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Article Synopsis
  • Heterostructures featuring high-mobility two-dimensional electron gas were formed into freestanding helical Hall bars for testing.
  • Magnetotransport measurements showed significant results, such as minima in the longitudinal magnetoresistance linked to both integer and fractional filling factors under high magnetic fields.
  • An observed asymmetry in magnetoresistance depending on magnetic field direction led to an analysis using an edge state model and Landauer-Büttiker calculations.
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In this paper we show the electronic transport and the quantum phase transitions that characterize the quantum Hall regime in graphene placed on SiO(2) substrates at magnetic fields up to 28 T and temperatures down to 4 K. The analysis of the temperature dependence of the Hall and longitudinal resistivity reveals intriguing non-universalities of the critical exponents of the plateau-insulator transition. These exponents depend on the type of disorder that governs the electrical transport and its characterization is important for the design and fabrication of novel graphene nano-devices.

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We have investigated the polarization-resolved photoluminescence (PL) in an asymmetric n-type GaAs/AlAs/GaAlAs resonant tunneling diode under magnetic field parallel to the tunnel current. The quantum well (QW) PL presents strong circular polarization (values up to -70% at 19 T). The optical emission from GaAs contact layers shows evidence of highly spin-polarized two-dimensional electron and hole gases which affects the spin polarization of carriers in the QW.

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