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Tongay, Sefaattin

Publications and source records attributed to Tongay, Sefaattin.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Electronic and catalytic engineering in two-dimensional vdW metal–organic frameworks through alloying

Bimetallic metal-organic framework (MOF s ) alloys, in which heterogeneous metal clusters are incorporated into their backbone, are capable of highly selective separations and catalysis. Due to limitations in our fundamental understanding of their alloying, however, established methods result in phase-separated or amorphous two-dimensional (2D) MOF s or lack precise control over alloy ratios. Here, our results demonstrate 2D MOF alloys where metal cation ratios (M 1 and M 2 ) in M 1 xM 2 1-x BDC (M 1 or M 2 = Zn, Cu, Ni, Co, Fe, Mn) can be engineered on demand by controlling the metal salt dissociation constants. Resulting MOF alloys exhibit a highly 2D nature with excellent crystallinity and minute control over metal cation ratios. Overall, our experimental and theoretical results show that their electronic bandgaps and photoexcited carrier lifetimes can be engineered by metal cation alloying. Interestingly, 2D alloyed MOF s enable high-efficiency photo-catalytic water reduction performance in Co/Ni MOF alloys owing to the spatially separated metal clusters in 2D MOF alloys.

2D materials↗
DOE OSTI2021

Imaging local discharge cascades for correlated electrons in WS 2 /WSe 2 moiré superlattices

Transition metal dichalcogenide moiré heterostructures provide an ideal platform to explore the extended Hubbard model, where long-range Coulomb interactions play a critical role in determining strongly correlated electron states. This has led to experimental observations of Mott insulator states at half filling as well as a variety of extended Wigner crystal states at different fractional fillings. However, a microscopic understanding of these emerging quantum phases is still lacking. Here we describe a scanning tunnelling microscopy (STM) technique for the local sensing and manipulation of correlated electrons in a gated WS 2 /WSe 2 moiré superlattice, which enables the experimental extraction of fundamental extended Hubbard model parameters. We demonstrate that the charge state of the local moiré sites can be imaged by their influence on the STM tunnelling current. In addition to imaging, we are also able to manipulate the charge state of correlated electrons. When we ramp the bias on the STM tip, there is a local discharge cascade of correlated electrons in the moiré superlattice, which allows us to estimate the nearest-neighbour Coulomb interaction. Two-dimensional mapping of the moiré electron charge states also enables us to determine the on-site energy fluctuations at different moiré sites. Furthermore, our technique should be broadly applicable to many semiconductor moiré systems, offering a powerful tool for the microscopic characterization and control of strongly correlated states in moiré superlattices.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moiré superlattice

Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied. When the system is in one of such states, the PL of interlayer excitons is relatively amplified at increased optical excitation power due to reduced mobility, and the valley polarization of interlayer excitons is enhanced. The moiré superlattice of the TMDC heterobilayer presents an exciting platform to engineer interlayer excitons through the periodic correlated electron states.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Advances in Rare-Earth Tritelluride Quantum Materials: Structure, Properties, and Synthesis

A distinct class of 2D layered quantum materials with the chemical formula of RTe 3 (R = lanthanide) has gained significant attention owing to the occurrence of collective quantum states, superconductivity, charge density waves (CDW), spin density waves, and other advanced quantum properties. To study the Fermi surface nesting driven CDW formation, the layered RTe 3 family stages an excellent low dimensional genre system. In addition to the primary energy gap feature observed at higher energy, optical spectroscopy study on some RTe 3 evidence a second CDW energy gap structure indicating the occurrence of multiple CDW ordering even with light and intermediate RTe 3 compounds. Here, a comprehensive review of the fundamentals of RTe 3 layered tritelluride materials is presented with a special focus on the recent advances made in electronic structure, CDW transition, superconductivity, magnetic properties of these unique quantum materials. A detailed description of successful synthesis routes including the flux method, self-flux method, and CVT along with potential applications is summarized.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Imaging moiré flat bands in three-dimensional reconstructed WSe 2 /WS 2 superlattices

Moiré superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moiré flat bands and strong, long-range Coulomb interactions. However, microscopic knowledge of the atomically reconstructed moiré superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moiré phenomena. Here we quantitatively study the moiré flat bands in three-dimensional (3D) reconstructed WSe 2 /WS 2 moiré superlattices by comparing scanning tunnelling spectroscopy (STS) of high-quality exfoliated TMD heterostructure devices with ab initio simulations of TMD moiré superlattices. A strong 3D buckling reconstruction accompanied by large in-plane strain redistribution is identified in our WSe 2 /WS 2 moiré heterostructures. STS imaging demonstrates that this results in a remarkably narrow and highly localized K-point moiré flat band at the valence band edge of the heterostructure. A series of moiré flat bands are observed at different energies that exhibit varying degrees of localization. Our observations contradict previous simplified theoretical models but agree quantitatively with ab initio simulations that fully capture the 3D structural reconstruction. Furthermore, our results reveal that the strain redistribution and 3D buckling in TMD heterostructures dominate the effective moiré potential and the corresponding moiré flat bands at the Brillouin zone K points.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Excitons in Bilayer MoS 2 Displaying a Colossal Electric Field Splitting and Tunable Magnetic Response

van der Waals heterostructures composed of transition metal dichalcogenide monolayers (TMDCs) are characterized by their truly rich excitonic properties which are determined by their structural, geometric, and electronic properties: In contrast to pure monolayers, electrons and holes can be hosted in different materials, resulting in highly tunable dipolar many-particle complexes. However, for genuine spatially indirect excitons, the dipolar nature is usually accompanied by a notable quenching of the exciton oscillator strength. Via electric and magnetic field dependent measurements, we demonstrate that a slightly biased pristine bilayer MoS 2 hosts strongly dipolar excitons, which preserve a strong oscillator strength. We scrutinize their giant dipole moment, and shed further light on their orbital and valley physics via bias-dependent magnetic field measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Nanoscale Conductivity Imaging of Correlated Electronic States in WSe 2 /WS 2 Moiré Superlattices

We report the nanoscale conductivity imaging of correlated electronic states in angle-aligned WSe 2 /WS 2 heterostructures using microwave impedance microscopy. Here, the noncontact microwave probe allows us to observe the Mott insulating state with one hole per moiré unit cell that persists for temperatures up to 150 K, consistent with other characterization techniques. In addition, we identify for the first time a Mott insulating state at one electron per moiré unit cell. Appreciable inhomogeneity of the correlated states is directly visualized in the hetero-bilayer region, indicative of local disorders in the moiré superlattice potential or electrostatic doping. Our work provides important insights on 2D moiré systems down to the microscopic level.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Chemical trends of deep levels in van der Waals semiconductors

Abstract Properties of semiconductors are largely defined by crystal imperfections including native defects. Van der Waals (vdW) semiconductors, a newly emerged class of materials, are no exception: defects exist even in the purest materials and strongly affect their electrical, optical, magnetic, catalytic and sensing properties. However, unlike conventional semiconductors where energy levels of defects are well documented, they are experimentally unknown in even the best studied vdW semiconductors, impeding the understanding and utilization of these materials. Here, we directly evaluate deep levels and their chemical trends in the bandgap of MoS 2 , WS 2 and their alloys by transient spectroscopic study. One of the deep levels is found to follow the conduction band minimum of each host, attributed to the native sulfur vacancy. A switchable, DX center - like deep level has also been identified, whose energy lines up instead on a fixed level across different hosts, explaining a persistent photoconductivity above 400 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Author Correction: Chemical trends of deep levels in van der Waals semiconductors

The original version of this Article omitted the following from the Acknowledgements: This research was partially conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. This has now been corrected in both the PDF and HTML versions of the Article.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Anisotropic band structure of TiS 3 nanoribbon revealed by polarized photocurrent spectroscopy

A re-discovered member of the layered material family, Titanium Trisulfide (TiS 3 ), has attracted intense research interest recently for the possibility of realizing an exciton insulator in the monolayer limit. However, due to their quasi-one-dimensional nature, thin TiS 3 flakes are typically in the form of nanoribbons that are challenging to characterize by optical absorption spectra, due to their small cross section. Here, we employ a sensitive photocurrent spectroscopy technique to probe the absorption of a thin TiS 3 nanoribbon in a field-effect transistor configuration. We have found a significant modification of the band structure of the thin TiS 3 nanoribbon, compared to its bulk counterpart. In addition, the polarization-dependent photocurrent spectra of thin TiS 3 nanoribbons exhibit greatly enhanced anisotropy compared to that of a thick TiS 3 device. The atomically thin TiS 3 flake, thus, not only provides an exciting platform for investigating many-body physics but also enables anisotropic quantum optoelectronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Anomalous Behavior of 2D Janus Excitonic Layers under Extreme Pressures

Newly discovered 2D Janus transition metal dichalcogenides layers have gained much attention from a theory perspective owing to their unique atomic structure and exotic materials properties, but little to no experimental data are available on these materials. Here, experimental and theoretical studies establish the vibrational and optical behavior of 2D Janus S–W–Se and S–Mo–Se monolayers under high pressures for the first time. Chemical vapor deposition (CVD)-grown classical transition metal dichalcogenides (TMD) monolayers are first transferred onto van der Waals (vdW) mica substrates and converted to 2D Janus sheets by surface plasma technique, and then integrated into a 500 µm size diamond anvil cell for high-pressure studies. Overall, the results show that 2D Janus layers do not undergo phase transition up to 15 GPa, and in this pressure regime, their vibrational modes exhibit a nonmonotonic response to the applied pressures (dω/dP). Interestingly, these 2D Janus monolayers exhibit unique blueshift in photoluminescence (PL) upon compression, which is in contrast to many other traditional semiconductor materials. Overall theoretical simulations offer in-depth insights and reveal that the overall optical response is a result of competition between the ab-plane (blueshift) and c-axis (redshift) compression. The overall findings shed the very first light on how 2D Janus monolayers respond under extreme pressures and expand the fundamental understanding of these materials.

2D Janus monolayers↗
DOE OSTI2020

Harnessing biological applications of quantum materials: opportunities and precautions

Since the discovery of graphene, research on two-dimensional (2D) quantum materials has generated a plethora of novel materials with the potential to significantly change our lives. Owing to their unique quantum, electronic, and excitonic properties, biosensing and bio-imaging are two specific areas where these quantum materials have started to make a large impact. This article provides a holistic overview into the properties, synthesis methods, biological applications, and toxicology studies of commonly studied quantum materials. Recent research into the biological applications of graphene and transition metal dichalcogenides is highlighted and their unique electronic properties are explored. Though tremendous research is generated in discovering new 2D materials, toxicology studies in the area are lacking. Historically, toxicology studies have lagged significantly behind new material discovery often with dire consequences. The product development cycle of polymeric materials is a testament to the negative consequences of having a reactionary approach to toxicology. With 2D materials set to become a widespread part of everyday life in the near future, we comment on the need for a proactive approach to examining and understanding their toxicology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗