Theses Doctoral

Spectroscopic Study of Localized States in Twisted Semiconducting Heterostructures and Charge Transfer Driven Phenomena in a-RuCl₃ Heterointerfaces

Shabani, Sara

This thesis investigates the unique properties of 2D devices such as twisted semiconducting bilayers and a-RuCl₃ heterostructures employing scanning tunneling microscopy (STM) and spectroscopy (STS) probes. The research presented here sheds light on the vast opportunities that 2D materials provide in condensed matter systems as well as future device applications. Among 2D materials, transition metal dichalcogenide (TMD) heterobilayers provide a promising platform to study many quantum phenomena such as excitonic states due to their tunability of band gap. In addition, TMDs are excellent candidates to achieve localized states and carrier confinement, crucial for single photon emitters used in quantum computation and information. We begin this thesis with a brief overview of STM/STS and utilizing these techniques on 2D materials in the first and second chapters.The third chapter of this work investigates the twisted bilayer of WSe₂ and MoSe₂ in the H-stacking configuration using STM/STS which was previously challenging to measure. The spectroscopic results obtained from the heterobilayer indicate that a combination of structural rippling and electronic coupling generates unexpectedly large \moire potentials, in the range of several hundred meV. Our analysis reveals that the \moire structure and internal strain, rather than interlayer coupling, are the main factors of the moire potential. Large moire potentials lead to deeply trapped carriers such as electron-hole pairs, so-called excitons. Our findings open new routes toward investigating excitonic states in twisted TMDs.

In the next chapter, we investigate the ultralocalized states of twisted WSe₂/MoSe₂ nanobubbles. Mechanical and electrical nanostructurings are expected to modify the band properties of transition metal dichalcogenides at the nanoscale. To visualize this effect, we use STM and near-field photoluminescence to examine the electronic and optical properties of nanobubbles in the semiconducting heterostructures. Our findings reveal a significant change in the local bandgap at the nanobubble, with a continuous evolution towards the edge of the bubble. Moreover, at the edge of the nanobubble, we show the formation of in gap bound states. A continuous redshift of the interlayer exciton on entering the bubble is also detected by the nano-PL. Using self-consistent Schrodinger-Poisson simulations, we further show that strong doping in the bubble region leading to band bending is responsible for achieving ultralocalized states. Overall, this work demonstrates the potential of 2D TMDs for developing well-controlled optical emitters for quantum technologies and photonics.

We next turn to the effect of the electric field in band gap tuning of WSe₂/WS₂ heterobilayer. The tunability of band gap is a crucial element in device engineering to achieve quantum emitters. The electrostatic gate generates doping and an electric field giving access to continuous tunability, higher doping level, and integration capability to nanoelectronic devices. We employ scanning tunneling microscopy (STM) and spectroscopy (STS) to probe the band properties of twisted heterobilayer with high energy and spatial resolution. We observe continuous band gap tuning up to several hundreds of meV change by sweeping the back gate. We introduced a capacitance model to take into account the finite tip size leading to an enhanced electric field. The result of our calculation captures well the band gap change observed by STS measurements. Our study offers a new route toward creating highly tunable semiconductors for carrier confinement in quantum technology.

In the next chapters, we focus on a-RuCl₃ heterointerfaces. We first explore the nanobubble of graphene/a-RuCl3 to create sharp p-n junctions. The ability to create sharp lateral p-n junctions is a critical requirement for the observation of numerous quantum phenomena. To accomplish this, we used a charge-transfer based heterostructure consisting of graphene and a-RuCl₃ to create nanoscale lateral p-n junctions in the vicinity of nanobubbles. Our approach relied on a combination of scanning tunneling microscopy (STM) and spectroscopy (STS), as well as scattering-type scanning near-field optical microscopy (s-SNOM), which allowed us to examine both the electronic and optical responses of these nanobubble p-n junctions. Our results showed a massive doping variation across the nanobubble with a band offset of 0.6 eV. Further, we observe the formation of an abrupt junction along nanobubble boundaries with an exceptionally sharp lateral width (<3 nm). This is one order of magnitude smaller length scale than previous lithographic methods. Our work paves the way toward device engineering via interfacial charge transfer in graphene and other low-density 2D materials.
In chapter 7, we describe the use of low-temperature scanning tunneling microscopy (STM) measurements to observe the \moire pattern in graphene/a-RuCl3 heterostructure to validate the InterMatch method. This method is effective in predicting the charge transfer, strain, and stability of an interface. The InterMatch method was applied to moire patterns of graphene/a-RuCl3 to predict the stable interface structure. STM topographs show three regions with distinct moire wavelengths due to atomic reconstructions. Using the InterMatch method, we perform a comprehensive mapping of the space of superlattice configurations and we identify the energetically favorable superlattices that occur in a small range of twist angles. This range is consistent with the STM results. Moreover, the spectra on these regions exhibit strong resonances with the spacing between resonances following the expectation from Landau levels on a Dirac spectrum due to strain and doping. The results of our scanning tunneling microscopy (STM) measurements confirm that the InterMatch method is effective in predicting the charge transfer and stability of interfaces between materials.

We next investigate WSe₂/a-RuCl₃ heterostructure through a multi-faceted approach. Our exploration encompassed diverse techniques such as STM, and optical measurements. We detect a significant charge transfer between the two layers by STM measurements, leading to a shift in the Fermi level towards the valence band of WSe₂. Our findings are supported by optical measurements and DFT calculations, which confirm the p-doped WSe₂ observed through STM. The results of this work highlight a-RuCl₃ potential for contact engineering of TMDs and unlocking their functionalities for the next generation optoelectronic devices.

In the last chapter of this thesis, I provide a brief conclusion as well as a few future directions and insights for investigating 2D materials.


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More About This Work

Academic Units
Thesis Advisors
Pasupathy, Abhay Narayan
Ph.D., Columbia University
Published Here
May 24, 2023