arXiv subjects

Riccardo Pisoni

Publications and source records attributed to Riccardo Pisoni.

18 recordsLinked to original sources

arXiv2023

Resonant band hybridization in alloyed transition metal dichalcogenide heterobilayers

Bandstructure engineering using alloying is widely utilised for achieving optimised performance in modern semiconductor devices. While alloying has been studied in monolayer transition metal dichalcogenides, its application in van der Waals heterostructures built from atomically thin layers is largely unexplored. Here, we fabricate heterobilayers made from monolayers of WSe$_2$ (or MoSe$_2$) and Mo$_x$W$_{1-x}$Se$_2$ alloy and observe nontrivial tuning of the resultant bandstructure as a function of concentration $x$. We monitor this evolution by measuring the energy of photoluminescence (PL) of the interlayer exciton (IX) composed of an electron and hole residing in different monolayers. In Mo$_x$W$_{1-x}$Se$_2$/WSe$_2$, we observe a strong IX energy shift of $\approx$100 meV for $x$ varied from 1 to 0.6. However, for $x<0.6$ this shift saturates and the IX PL energy asymptotically approaches that of the indirect bandgap in bilayer WSe$_2$. We theoretically interpret this observation as the strong variation of the conduction band K valley for $x>0.6$, with IX PL arising from the K-K transition, while for $x<0.6$, the bandstructure hybridization becomes prevalent leading to the dominating momentum-indirect K-Q transition. This bandstructure hybridization is accompanied with strong modification of IX PL dynamics and nonlinear exciton properties. Our work provides foundation for bandstructure engineering in van der Waals heterostructures highlighting the importance of hybridization effects and opening a way to devices with accurately tailored electronic properties.

cond-mat.mtrl-sci↗

arXiv2019

Gap Opening in Twisted Double Bilayer Graphene by Crystal fields

Crystal fields occur due to a potential difference between chemically different atomic species. In Van-der-Waals heterostructures such fields are naturally present perpendicular to the planes. It has been realized recently that twisted graphene multilayers provide powerful playgrounds to engineer electronic properties by the number of layers, the twist angle, applied electric biases, electronic interactions and elastic relaxations, but crystal fields have not received the attention they deserve. Here we show that the bandstructure of large-angle twisted double bilayer graphene is strongly modified by crystal fields. In particular, we experimentally demonstrate that twisted double bilayer graphene, encapsulated between hBN layers, exhibits an intrinsic bandgap. By the application of an external field, the gaps in the individual bilayers can be closed, allowing to determine the crystal fields. We find that crystal fields point from the outer to the inner layers with strengths in the bottom (top) bilayer of -0.13 V/nm (0.12 V/nm). We show both by means of first principles calculations and low energy models that crystal fields open a band gap in the groundstate. Our results put forward a physical scenario in which a crystal field effect in carbon substantially impacts the low energy properties of twisted double bilayer graphene, suggesting that such contributions must be taken into account in other regimes to faithfully predict the electronic properties of twisted graphene multilayers.

cond-mat.mes-hall↗

arXiv2019

Fully automated identification of 2D material samples

Thin nanomaterials are key constituents of modern quantum technologies and materials research. Identifying specimens of these materials with properties required for the development of state of the art quantum devices is usually a complex and lengthy human task. In this work we provide a neural-network driven solution that allows for accurate and efficient scanning, data-processing and sample identification of experimentally relevant two-dimensional materials. We show how to approach classification of imperfect imbalanced data sets using an iterative application of multiple noisy neural networks. We embed the trained classifier into a comprehensive solution for end-to-end automatized data processing and sample identification.

cond-mat.mes-hall↗

arXiv2019

Predicting retrosynthetic pathways using a combined linguistic model and hyper-graph exploration strategy

We present an extension of our Molecular Transformer architecture combined with a hyper-graph exploration strategy for automatic retrosynthesis route planning without human intervention. The single-step retrosynthetic model sets a new state of the art for predicting reactants as well as reagents, solvents and catalysts for each retrosynthetic step. We introduce new metrics (coverage, class diversity, round-trip accuracy and Jensen-Shannon divergence) to evaluate the single-step retrosynthetic models, using the forward prediction and a reaction classification model always based on the transformer architecture. The hypergraph is constructed on the fly, and the nodes are filtered and further expanded based on a Bayesian-like probability. We critically assessed the end-to-end framework with several retrosynthesis examples from literature and academic exams. Overall, the frameworks has a very good performance with few weaknesses due to the bias induced during the training process. The use of the newly introduced metrics opens up the possibility to optimize entire retrosynthetic frameworks through focusing on the performance of the single-step model only.

cs.LG↗

arXiv2019

The Electronic Thickness of Graphene

The van-der-Waals stacking technique enables the fabrication of heterostructures, where two conducting layers are atomically close. In this case, the finite layer thickness matters for the interlayer electrostatic coupling. Here we investigate the electrostatic coupling of two graphene layers, twisted by 22 degrees such that the layers are decoupled by the huge momentum mismatch between the K and K' points of the two layers. We observe a splitting of the zero-density lines of the two layers with increasing interlayer energy difference. This splitting is given by the ratio of single-layer quantum capacitance over interlayer capacitance C and is therefore suited to extract C. We explain the large observed value of C by considering the finite dielectric thickness d of each graphene layer and determine d=2.6 Angstrom. In a second experiment we map out the entire density range with a Fabry-Pérot resonator. We can precisely measure the Fermi-wavelength in each layer, showing that the layers are decoupled. We find that the Fermi wavelength exceeds 600nm at the lowest densities and can differ by an order of magnitude between the upper and lower layer. These findings are reproduced using tight-binding calculations.

cond-mat.mes-hall↗

arXiv2019

Absence of inter-layer tunnel coupling of $K$-valley electrons in bilayer MoS$_{2}$

In Bernal stacked bilayer graphene interlayer coupling significantly affects the electronic bandstructure compared to monolayer graphene. Here we present magnetotransport experiments on high-quality $n$-doped bilayer MoS$_{2}$. By measuring the evolution of the Landau levels as a function of electron density and applied magnetic field we are able to investigate the occupation of conduction band states, the interlayer coupling in pristine bilayer MoS$_{2}$, and how these effects are governed by electron-electron interactions. We find that the two layers of the bilayer MoS$_{2}$ behave as two independent electronic systems where a two-fold Landau level's degeneracy is observed for each MoS$_{2}$ layer. At the onset of the population of the bottom MoS$_{2}$ layer we observe a large negative compressibility caused by the exchange interaction. These observations, enabled by the high electronic quality of our samples, demonstrate weak interlayer tunnel coupling but strong interlayer electrostatic coupling in pristine bilayer MoS$_{2}$. The conclusions from the experiments may be relevant also to other transition metal dichalcogenide materials.

cond-mat.mes-hall↗

arXiv2018

Interactions and magnetotransport through spin-valley coupled Landau levels in monolayer MoS$_{2}$

The strong spin-orbit coupling and the broken inversion symmetry in monolayer transition metal dichalcogenides (TMDs) results in spin-valley coupled band structures. Such a band structure leads to novel applications in the fields of electronics and optoelectronics. Density functional theory calculations as well as optical experiments have focused on spin-valley coupling in the valence band. Here we present magnetotransport experiments on high-quality n-type monolayer molybdenum disulphide (MoS$_{2}$) samples, displaying highly resolved Shubnikov-de Haas oscillations at magnetic fields as low as $2~T$. We find the effective mass $0.7~m_{e}$, about twice as large as theoretically predicted and almost independent of magnetic field and carrier density. We further detect the occupation of the second spin-orbit split band at an energy of about $15~meV$, i.e. about a factor $5$ larger than predicted. In addition, we demonstrate an intricate Landau level spectrum arising from a complex interplay between a density-dependent Zeeman splitting and spin and valley-split Landau levels. These observations, enabled by the high electronic quality of our samples, testify to the importance of interaction effects in the conduction band of monolayer MoS$_{2}$.

cond-mat.mes-hall↗

arXiv2018

Transport through a network of topological states in twisted bilayer graphene

We explore a network of electronic quantum valley Hall (QVH) states in the moiré crystal of minimally twisted bilayer graphene. In our transport measurements we observe Fabry-Pérot and Aharanov-Bohm oscillations which are robust in magnetic fields ranging from 0 to 8T, in strong contrast to more conventional 2D systems where trajectories in the bulk are bent by the Lorentz force. This persistence in magnetic field and the linear spacing in density indicate that charge carriers in the bulk flow in topologically protected, one dimensional channels. With this work we demonstrate coherent electronic transport in a lattice of topologically protected states.

cond-mat.mes-hall↗

arXiv2018

Tunneling spectroscopy of graphene nanodevices coupled to large-gap superconductors

We performed tunneling spectroscopy measurements of graphene coupled to niobium/niobium-nitride superconducting electrodes. Due to the proximity effect, the graphene density of states depends on the phase difference between the superconductors and exhibits a hard induced gap at zero phase, consistent with a continuum of Andreev bound states. At energies larger than the superconducting gap, we observed phase-dependent energy levels displaying the Coulomb blockade effect, which are interpreted as arising from spurious quantum dots, presumably embedded in the heterostructures and coupled to the proximitized graphene.

cond-mat.mes-hall↗

arXiv2018

Spin and Valley States in Gate-defined Bilayer Graphene Quantum Dots

In bilayer graphene, electrostatic confinement can be realized by a suitable design of top and back gate electrodes. We measure electronic transport through a bilayer graphene quantum dot, which is laterally confined by gapped regions and connected to the leads via p-n junctions. Single electron and hole occupancy is realized and charge carriers $n = 1, 2,\dots 50$ can be filled successively into the quantum system with charging energies exceeding $10 \ \mathrm{meV}$. For the lowest quantum states, we can clearly observe valley and Zeeman splittings with a spin g-factor of $g_{s}\approx 2$. In the low field-limit, the valley splitting depends linearly on the perpendicular magnetic field and is in qualitative agreement with calculations.

cond-mat.mes-hall↗

arXiv2018

Coupled quantum dots in bilayer graphene

Electrostatic confinement of charge carriers in bilayer graphene provides a unique platform for carbon-based spin, charge or exchange qubits. By exploiting the possibility to induce a band gap with electrostatic gating, we form a versatile and widely tunable multi-quantum dot system. We demonstrate the formation of single, double and triple quantum dots that are free of any sign of disorder. In bilayer graphene we have the possibility to form tunnel barriers using different mechanisms. We can exploit the ambipolar nature of bilayer graphene where pn-junctions form natural tunnel barriers. Alternatively, we can use gates to form tunnel barriers, where we can vary the tunnel coupling by more than two orders of magnitude tuning between a deeply Coulomb blockaded system and a Fabry-Pérot-like cavity. Demonstrating such tunability is an important step towards graphene-based quantum computation.

cond-mat.mes-hall↗

arXiv2018

Magnetotransport and lateral confinement in an InSe van der Waals Heterostructure

In the last six years, Indium selenide (InSe) has appeared as a new van der Waals heterostructure platform which has been extensively studied due to its unique electronic and optical properties. Such as transition metal dichalcogenides (TMDCs), the considerable bandgap and high electron mobility can provide a potential optoelectronic application. Here we present low-temperature transport measurements on a few-layer InSe van der Waals heterostructure with graphene-gated contacts. For high magnetic fields, we observe magnetoresistance minima at even filling factors related to two-fold spin degeneracy. By electrostatic gating with negatively biased split gates, a one-dimensional channel is realized. Close to pinch-off, transport through the constriction is dominated by localized states with charging energies ranging from 2 to 5 meV. This work opens new possibility to explore the low-dimensional physics including quantum point contact and quantum dot.

cond-mat.mes-hall↗

arXiv2018

Gate-Tunable Quantum Dot in a High Quality Single Layer MoS$_{\mathrm{2}}$ Van der Waals Heterostructure

We have fabricated an encapsulated monolayer MoS$_{\mathrm{2}}$ device with metallic ohmic contacts through a pre-patterned hBN layer. In the bulk, we observe an electron mobility as high as 3000 cm$^{\mathrm{2}}$/Vs at a density of 7 $\times$ 10$^{\mathrm{12}}$ cm$^{\mathrm{-2}}$ at a temperature of 1.7 K. Shubnikov-de Haas oscillations start at magnetic fields as low as 3.3 T. By realizing a single quantum dot gate structure on top of the hBN we are able to confine electrons in MoS$_{\mathrm{2}}$ and observe the Coulomb blockade effect. By tuning the middle gate voltage we reach a double dot regime where we observe the standard honeycomb pattern in the charge stability diagram.

cond-mat.mes-hall↗

arXiv2018

Edge channel confinement in a bilayer graphene $n$-$p$-$n$ quantum dot

We combine electrostatic and magnetic confinement to define a quantum dot in bilayer graphene. The employed geometry couples $n$-doped reservoirs to a $p$-doped dot. At magnetic field values around $B = 2~$T, Coulomb blockade is observed. This demonstrates that the coupling of the co-propagating modes at the $p$-$n$ interface is weak enough to form a tunnel barrier, facilitating transport of single charge carriers onto the dot. This result may be of use for quantum Hall interferometry experiments.

cond-mat.mes-hall↗

arXiv2018

Electrostatically induced quantum point contact in bilayer graphene

We report the fabrication of electrostatically defined nanostructures in encapsulated bilayer graphene, with leakage resistances below depletion gates as high as $R \sim 10~$G$Ω$. This exceeds previously reported values of $R =~$10 - 100 k$Ω$.\cite{Zou2010,Yan2010,Zhu2016a} We attribute this improvement to the use of a graphite back gate. We realize two split gate devices which define an electronic channel on the scale of the Fermi-wavelength. A channel gate covering the gap between the split gates varies the charge carrier density in the channel. We observe device-dependent conductance quantization of $ΔG = 2~e^2/h$ and $ΔG = 4~e^2/h$. In quantizing magnetic fields normal to the sample plane, we recover the four- fold Landau level degeneracy of bilayer graphene. Unexpected mode crossings appear at the crossover between zero magnetic field and the quantum Hall regime.

cond-mat.mes-hall↗

arXiv2017

Gate-Defined One-Dimensional Channel and Broken Symmetry States in MoS$_2$ van der Waals Heterostructures

We have realized encapsulated trilayer MoS$_2$ devices with gated graphene contacts. In the bulk, we observe an electron mobility as high as 7000~cm$^{2}$/(V s) at a density of 3 $\times$ 10$^{12}$~cm$^{-2}$ at a temperature of 1.9~K. Shubnikov--de Haas oscillations start at magnetic fields as low as 0.9~T. The observed 3-fold Landau level degeneracy can be understood based on the valley Zeeman effect. Negatively biased split gate electrodes allow us to form a channel that can be completely pinched off for sufficiently large gate voltages. The measured conductance displays plateau-like features.

cond-mat.mes-hall↗

arXiv2017

Tunnelling Spectroscopy of Andreev States in Graphene

A normal conductor placed in good contact with a superconductor can inherit its remarkable electronic properties. This proximity effect microscopically originates from the formation in the conductor of entangled electron-hole states, called Andreev states. Spectroscopic studies of Andreev states have been performed in just a handful of systems. The unique geometry, electronic structure and high mobility of graphene make it a novel platform for studying Andreev physics in two dimensions. Here we use a full van der Waals heterostructure to perform tunnelling spectroscopy measurements of the proximity effect in superconductor-graphene-superconductor junctions. The measured energy spectra, which depend on the phase difference between the superconductors, reveal the presence of a continuum of Andreev bound states. Moreover, our device heterostructure geometry and materials enable us to measure the Andreev spectrum as a function of the graphene Fermi energy, showing a transition between different mesoscopic regimes. Furthermore, by experimentally introducing a novel concept, the supercurrent spectral density, we determine the supercurrent-phase relation in a tunnelling experiment, thus establishing the connection between Andreev physics at finite energy and the Josephson effect. This work opens up new avenues for probing exotic topological phases of matter in hybrid superconducting Dirac materials.

cond-mat.mes-hall↗

arXiv2015

Tuning of the Thermoelectric Figure of Merit of CH$_3$NH$_3$MI$_3$ (M=Pb,Sn) Photovoltaic Perovskites

The hybrid halide perovskites, the very performant compounds in photovoltaic applications, possess large Seebeck coefficient and low thermal conductivity making them potentially interesting high figure of merit ($ZT$) materials. For this purpose one needs to tune the electrical conductivity of these semiconductors to higher values. We have studied the CH$_3$NH$_3$MI$_3$ (M=Pb,Sn) samples in pristine form showing very low $ZT$ values for both materials; however, photoinduced doping (in M=Pb) and chemical doping (in M=Sn) indicate that, by further doping optimization, $ZT$ can be enhanced toward unity and reach the performance level of the presently most efficient thermoelectric materials.

cond-mat.mtrl-sci↗