Electronic, excitonic and magnetic properties of two-dimensional heterostructures

Alberto Ciarrocchi
EPFL, 2020
Thèse EPFL

Résumé

Two-dimensional (2D) crystals such as graphene or transition metal dichalcogenides (TMDCs) are a fascinating class of quantum materials. These compounds are obtained isolating the single atomic sheets that normally form bulk layered crystals, and the reduced dimensionality endows them with unique physical properties. These peculiar characteristics have made them a very interesting research topic, with potential for fundamental discoveries but also technological applications. This thesis focuses on the behaviour of semiconducting two-dimensional materials of the TMDC family, which possess unusual spin- and valley-dependent optical and transport characteristics. The aim is to engineer their properties and build 2D heterostructures to investigate multiple quantum degrees of freedom (charge, spin and valley) for applications in energy-efficient information technologies.

To this end, the first part of the dissertation explores the layered material PtSe2 for its potential as a channel material for nano electronic devices. By studying charge transport as a function of material thickness, temperature and carrier concentration, one finds that PtSe2 allows for multiple kinds of band-structure engineering. First, a metal-semiconductor transition driven by interlayer interaction is observed. Further magneto-transport studies show the presence of layer-dependent, defect-induced magnetism. These results show the potential of nanoscale engineering to obtain designed physical properties in 2D materials.

The second part of the thesis instead deals with indirect excitons in 2D heterostructures as a promising platform to realize new computing devices. First, a room temperature excitonic switch is demonstrated, taking advantage of the large exciton binding energies found in TMDCs. The work then focuses on the control of valley-polarized excitons, demonstrating the possibility to electrically control the polarization, energy and brightness of interlayer excitons. Building on top of these two results, an excitonic switch for currents of valley-polarized excitons, i.e. a valleytronic transistor, is realized. These results highlight how excitonic devices could be a capable platform for computing schemes based on the pseudo-spin degree of freedom.

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https://infoscience.epfl.ch/record/279549?ln=fr

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Alberto Ciarrocchi
EPFL, 2020
Thèse EPFL

Résumé

Official source

https://infoscience.epfl.ch/record/279549?ln=fr

À propos de ce résultat

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Spin-valley optoelectronics based on two-dimensional materials

Dmitrii Unuchek

Two-dimensional (2D) materials, in particular graphene and transition metal dichalcogenides (TMDC), have attracted great scientific interest over the last decade, revealing exceptional mechanical, electrical and optical properties. Owing to their layered nature, subnanometer-thick single-layer forms of these crystals can be chemically grown or mechanically isolated, representing an ultimately scaled-down platform for further miniaturization of electronic devices. Indeed, the large family of 2D materials contains hundreds of members, including metals, semiconductors, insulators, and others, covering the whole spectrum of potential applications. Availability of all necessary building blocks for the construction of all-2D solid-state devices makes this platform ideal for fabrication of ultrathin, transparent and flexible devices. Extensively investigated graphene has demonstrated excellent electrical properties. However, the absence of a bandgap is an obstacle for its interaction with light and therefore limits applications in optics. In this aspect, atomically thin TMDC semiconductors appear to be an alternative, more promising platform, as they possess a direct band gap in the visible range in the monolayer form. Despite being only three atoms thick, these semiconductors demonstrate exceptionally large light absorption, efficient light emission, and strong light-matter interaction, attracting justified interest from the optics community. We will focus on their potential applications for optoelectronics in Chapter 4. Even more, broken inversion symmetry and strong spin-orbit coupling in single-layer TMDC crystals reveal a new quantum number, the so-called valley index. Indeed, this unique degree of freedom of charge carriers is known for some materials since the 1970s. However, in the case of 2D semiconductors, spin-valley locking mechanism and valley contrasting optical selection rules open new ways for addressing, manipulation and sensing of this pseudospin, opening the whole new field of valleytronics. Due to the large splitting of the valence band, spin and valley degree of freedom become locked in these atomically thin materials. We employ this unique feature in Chapter 5 for indirect injection of spins into graphene by pumping valley polarized carriers in an adjacent TMDC monolayer. Being gapless, graphene does not allow direct optical injection of spins. Another striking feature of 2D materials is their unique ability to be stacked in vertical heterostructures with strong electrical coupling between layers. The weak van der Waals force, which keeps components together, provides freedom in the assembly process, so that a lattice mismatch or a twist angle becomes unimportant in the first approximation. This provides a novel platform for harvesting complementary properties of the constituent materials, allowing the engineering of new artificial meta-materials as we demonstrate in Chapter 6. Furthermore, synergistic effects in van der Waals heterostructures enable completely new properties and phenomena, which do not exist in the single materials, with twist angle being an important knob for tuning these effects. We observe and exploit such novel phenomena arising in heterostructures of 2D semiconductors in the last chapter of this thesis. On the way to the realization of practical optoelectronic and valleytronic applications, this thesis studies fundamental aspects of rich spin-valley physics of atomically thin semiconductors

EPFL2019

Chargement

Submonolayer epitaxial growth is obtained by the deposition of less than a complete layer of atoms on a single crystal surface. It is of fundamental interest for industrial applications (e.g. in the semiconductor industry) as well as from the point of view of basic research. For example, it is known that nanometer-sized atomic structures (nanostructures) exhibit remarkable physical and chemical properties which can differ greatly from those of bulk matter. In order to investigate these properties, it is often necessary to create large quantities of well defined and possibly spatially ordered nanostructures. One way to achieve this result is self-organized growth where one deposits atoms on a clean crystalline surface and lets the growth process evolve freely. Here, nanostructures result from the atomic diffusion and aggregation processes taking place at the surface. Understanding the exact nature of these processes is of ongoing interest in the field of nanostructure growth. In this thesis we report about submonolayer growth experiments of the ferromagnetic transition metal cobalt. Cobalt was chosen because it exhibits remarkable magnetic properties. These experiments were performed in an ultra-high vacuum chamber and molecular beam epitaxy was used to grow the nanostructures. Observations of the surface were made using a variable-temperature scanning tunneling microscope (STM). In order to get a better understanding of the atomic processes happening at the surface, we developed two adapted computational simulation methods. Kinetic Monte-Carlo (KMC) simulations were used to get an atomistic picture of the surface while mean field rate equations were integrated numerically to yield cluster densities. We study the growth of cobalt on three different surfaces. By depositing Co on a clean Pt(111) crystal surface, we observe that the platinum surface reconstructs by forming star-shaped partial dislocations for sample temperatures above 180 K (-93°C). We also observe that island densities deviate from predictions of all known models towards higher values for these same temperatures. By simulation we are able to show that insertion of Co into the topmost platinum layer creates a repulsive network of dislocations. We show that these dislocations act as diffusion inhibiting barriers and thus influence the island density by constraining the free movement of atoms at the surface. We also show that the Co dimer and trimer diffuse on Pt(111) before dissociating and are able to extract corresponding activation barriers. We also study the deposition of Co on a Ru(0001) surface which shows a more conventional temperature dependence. By comparing simulation and experiment we extract all relevant diffusion activation barriers and show that at high temperatures the Co dimer and trimer dissociate. Finally, we investigate the growth of Co on the hexagonal boron nitride superlattice which forms on a Rh(111) surface. On this surface Co clusters form three-dimensional hemispherical dots. We show how the substrate corrugation influences diffusion of Co atoms and that clusters up to the size of the pentamer can diffuse. By simulation, we also extract the relevant migrations and desorption barriers.

EPFL2008

Chargement

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We present magnetization and Se-77 Nuclear Magnetic Resonance (NMR) measurements in single crystals of the magnetoelectric compound Cu2OSeO3. The temperature and field dependence of the magnetization suggest a ferrimagnetic ordering at T-c similar or equal to 60 K in a 3up-1down configuration. The easy axis of the magnetization is along the [100] crystallographic direction. The Se-77 NMR line shape data collected at 14.09 T are consistent with the symmetries imposed by the cubic P2(1)3 space group in the temperature range 20-290 K and confirm that the magnetic transition is not accompanied by any lowering of the crystal symmetry as has recently been proposed by Bos et al. [Phys. Rev. B 78 094416 (2008)].

Iop Publishing Ltd, Dirac House, Temple Back, Bristol Bs1 6Be, England2011

Chargement

Spin-valley optoelectronics based on two-dimensional materials

Dmitrii Unuchek

EPFL2019

EPFL2008