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Electron dynamics in layered materials

Abstract : Currently,layered materials attract great interest due to their electrical and optical properties. Such crystals display an electronic band structure that strongly depends on the sample thickness.The large tunability of the electronic screening and gap size can be very attracting for the creation of heterostructures whose properties can be designed on demand. We can say that the research field of low dimensional materials has been boosted by the discovery of graphene and quickly has been enlarged to other materials as transition metal dichalcogenides,black phosphorous and Indium selenide.Our work will focus on the excited state dynamics in these compounds,as well as on the evolution of the band structure upon surface doping.The manuscript is organized as follow:Chapter1 provides a general introduction of layered materials.In particular,we discuss the structural and electronic properties of some relevant compounds.Chapter2 describes the principles of ultrafast spectroscopic methods and shows many applications to the case of the layered materials.We mainly focus our attention on the electron dynamics in semiconducting crystals and charge density waves systems. The electron dynamics of layered materials have been investigated by means of time-and angle-resolved photoelectron spectroscopy (TrARPES),which is a powerful tool to directly map the electronic band structure and to follow the dynamics of the electrons photoinjected via an ultrafast laser source.Chapter3 discusses the experimental technique of choice and the setup where we have been performed in the reported measurements.we begin the discussion of our original data in Chapter4.The TrARPES measurements of layered black phosphorus(BP) monitor the electronic distribution in the conduction and valence band as a function of delay time from photoexcitation.The data show that,after thermalization,the photo-injected electrons do not lead to sizable band gap renormalization,neither do they generate an appreciable amount of carrier multiplication.On the other hand,a Stark broadening of the valence band is ascribed to the inhomogeneous screening of a local potential around charge defects.Chapter5 shows time resolved ARPES data on a BP surface that is doped in-situ by means of alkali metals evaporation. We monitor the collapse of the band-gap in the accumulation layer with unmatched accuracy and we observe that the buried states detected by the low energy photons of our probing pulse acquire a surprisingly high band velocity at large dopants concentration.Chapter6 deals with the modification of hot carrier dynamics upon increasing the surface doping of BP.In this case the reported analysis is still preliminary and needs to be backed by ab-initio calculations.Chapter7 contains our work on layered ɛ-InSe.As in the case of BP,we generate an accumulation layer of varying electronic density on the surface of such semiconductor.By spanning the doping level from the semiconducting to the metallic limit,we observe that quantum screening of Longitudinal Optical phonons is not as efficient as it would be in a strictly bidimensional system,indicating a remote coupling of confined states to polar phonons of the bulk.Furthermore,we show that a 3D Fröhlich interaction with Thomas-Fermi screening can be used to mimic the effects of such a remote coupling at the ɛ-InSe surface.In Chapter8,we study the layered 1T-TaS2.This material belongs to the Charge density waves (CDW) systems and has been extensively investigated by several research groups.In 1T-TaS2,the combination of structural distortion with high electronic correlations leads to a complex and fascinating phase diagram.We could reproduce controversial data that have been recently published in the literature and that identify a new instability in proximity of the metal to-insulator transition.Finally,chapter9 summarizes the conclusions of our work and briefly discusses the perspectives of some future directions of research.
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Jingwei Dong. Electron dynamics in layered materials. Physics [physics]. Institut Polytechnique de Paris, 2021. English. ⟨NNT : 2021IPPAX019⟩. ⟨tel-03221132⟩

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