arXiv subjects

Sefaattin Tongay

Publications and source records attributed to Sefaattin Tongay.

At least 37 records · Page 2Linked to original sources

arXiv2023

Measurements of Correlated Insulator Gaps in a Transition Metal Dichalcogenide Moiré Superlattice

Moiré superlattices of transitional metal dichalcogenides exhibit strong electron-electron interaction that has led to experimental observations of Mott insulators and generalized Wigner crystals. In this letter, we report direct measurements of the thermodynamic gaps of these correlated insulating states in a dual-gate WS2/WSe2 moiré bilayer. We employ the microwave impedance microscopy to probe the electronic features in both the graphene top gate and the moiré bilayer, from which we extract the doping dependence of the chemical potential of the moiré bilayer and the energy gaps for various correlated insulating states utilizing the Landau quantization of graphene. These gaps are relatively insensitive to the application of an external electric field to the WS2/WSe2 moiré bilayer.

cond-mat.str-el↗

arXiv2023

Quadrupolar Excitons and Hybridized Interlayer Mott Insulator in a Trilayer Moiré Superlattice

Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe2-WS2-WSe2 trilayer moiré superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe2 valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe2 layers share one hole laterally confined in one moiré unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions.

cond-mat.mes-hall↗

arXiv2023

Thermodynamic behavior of correlated electron-hole fluids in van der Waals heterostructures

Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton superfluids. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe2/hBN/WSe2 heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~$0.8\times {10}^{12} \mathrm{cm}^{-2}$ and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems.

cond-mat.str-el↗

arXiv2023

Imaging Moiré Excited States with Photocurrent Tunneling Microscopy

Moiré superlattices provide a highly tunable and versatile platform to explore novel quantum phases and exotic excited states ranging from correlated insulators1-17 to moiré excitons7-10,18. Scanning tunneling microscopy has played a key role in probing microscopic behaviors of the moiré correlated ground states at the atomic scale1,11-15,19. Atomic-resolution imaging of quantum excited state in moiré heterostructures, however, has been an outstanding experimental challenge. Here we develop a novel photocurrent tunneling microscopy by combining laser excitation and scanning tunneling spectroscopy (laser-STM) to directly visualize the electron and hole distribution within the photoexcited moiré exciton in a twisted bilayer WS2 (t-WS2). We observe that the tunneling photocurrent alternates between positive and negative polarities at different locations within a single moiré unit cell. This alternating photocurrent originates from the exotic in-plane charge-transfer (ICT) moiré exciton in the t-WS2 that emerges from the competition between the electron-hole Coulomb interaction and the moiré potential landscape. Our photocurrent maps are in excellent agreement with our GW-BSE calculations for excitonic states in t-WS2. The photocurrent tunneling microscopy creates new opportunities for exploring photoexcited non-equilibrium moiré phenomena at the atomic scale.

cond-mat.mes-hall↗

arXiv2023

Strain Anisotropy Driven Spontaneous Formation of Nanoscrolls from Two-Dimensional Janus Layers

Two-dimensional Janus transition metal dichalcogenides (TMDs) have attracted attention due to their emergent properties arising from broken mirror symmetry and self-driven polarisation fields. While it has been proposed that their vdW superlattices hold the key to achieving superior properties in piezoelectricity and photovoltiacs, available synthesis has ultimately limited their realisation. Here, we report the first packed vdW nanoscrolls made from Janus TMDs through a simple one-drop solution technique. Our results, including ab-initio simulations, show that the Bohr radius difference between the top sulphur and the bottom selenium atoms within Janus M_Se^S (M=Mo, W) results in a permanent compressive surface strain that acts as a nanoscroll formation catalyst after small liquid interaction. Unlike classical 2D layers, the surface strain in Janus TMDs can be engineered from compressive to tensile by placing larger Bohr radius atoms on top (M_S^Se) to yield inverted C scrolls. Detailed microscopy studies offer the first insights into their morphology and readily formed Moiré lattices. In contrast, spectroscopy and FETs studies establish their excitonic and device properties and highlight significant differences compared to 2D flat Janus TMDs. These results introduce the first polar Janus TMD nanoscrolls and introduce inherent strain-driven scrolling dynamics as a catalyst to create superlattices.

cond-mat.mtrl-sci↗

arXiv2023

Confined-state physics and signs of fermionization of moiré excitons in WSe$_2$/MoSe$_2$ heterobilayers

We revisit and extend the standard bosonic interpretation of interlayer excitons in the moiré potential of twisted heterostructures of transition-metal dichalcogenides. In our experiments, we probe a high quality MoSe$_2$/WSe$_2$ van der Waals bilayer heterostructure via density-dependent photoluminescence spectroscopy and reveal strongly developed, unconventional spectral shifts of the emergent moiré exciton resonances. The observation of saturating blueshifts of successive exciton resonances allow us to explain their physics in terms of a model utilizing fermionic saturable absorbers. This approach is strongly inspired by established quantum-dot models, which underlines the close analogy of interlayer excitons trapped in pockets of the moiré potential, and quantum emitters with discrete eigenstates.

cond-mat.mes-hall↗

arXiv2023

Correlated insulator of excitons in WSe2/WS2 moiré superlattices

A panoply of unconventional electronic states has been observed in moiré superlattices. Engineering similar bosonic phases remains, however, largely unexplored. We report the observation of a bosonic correlated insulator in WSe2/WS2 moiré superlattices composed of excitons, i.e., tightly bound electron-hole pairs. We develop a pump probe spectroscopy method that we use to observe an exciton incompressible state at exciton filling ν_ex = 1 and charge neutrality, indicating a correlated insulator of excitons. With varying charge density, the bosonic correlated insulator continuously transitions into an electron correlated insulator at charge filling ν_e = 1, suggesting a mixed correlated insulating state between the two limits. Our studies establish semiconducting moiré superlattices as an intriguing platform for engineering bosonic phases.

cond-mat.str-el↗

arXiv2023

Interplay of trapped species and absence of electron capture in Moiré heterobilayers

Moiré heterobilayers host interlayer excitons in a natural, periodic array of trapping potentials. Recent work has elucidated the structure of the trapped interlayer excitons and the nature of photoluminescence (PL) from trapped and itinerant charged complexes such as interlayer trions in these structures. In this paper, our results serve to add to the understanding of the nature of PL emission and explain its characteristic blueshift with increasing carrier density, along with demonstrating a significant difference between the interlayer exciton-trion conversion efficiency as compared to both localized and itinerant intra-layer species in conventional monolayers. Our results show the absence of optical generation of trions in these materials, which we suggest arises from the highly localized, near sub-nm confinement of trapped species in these Moiré potentials.

cond-mat.mtrl-sci↗

arXiv2023

Ultra-bright single photon source based on an atomically thin material

Solid-state single photon sources are central building blocks in quantum communication networks and on-chip quantum information processing. Atomically thin crystals were established as possible candidates to emit non-classical states of light, however, the performance of monolayer-based single photon sources has so far been lacking behind state-of-the-art devices based on volume crystals. Here, we implement a single photon source based on an atomically thin sheet of WSe2 coupled to a spectrally tunable optical cavity. It is characterized by a high single photon purity with a $g^{(2)}(0)$ value as low as $4.7 \pm 0.7 \%$ and a record-high first lens brightness of linearly polarized photons as large as $65 \pm 4 \%$. Interestingly, the high performance of our devices allows us to observe genuine quantum interference phenomena in a Hong-Ou-Mandel experiment. Our results demonstrate that open cavities and two-dimensional materials constitute an excellent platform for ultra-bright quantum light sources: the unique properties of such two-dimensional materials and the versatility of open cavities open an inspiring avenue for novel quantum optoelectronic devices.

quant-ph↗

arXiv2022

Charge transfer dynamics in MoSe$_{2}$/hBN/WSe$_{2}$ heterostructures

Ultrafast charge transfer processes provide a facile way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated heterostructures composed of TMD/hBN/TMD enable new ways to control interlayer exciton properties and achieve novel exciton phenomena, such as exciton insulators and condensates, where longer lifetimes are desired. In this work, we experimentally study the charge transfer dynamics in a heterostructure composed of a 1 nm thick hBN spacer between MoSe$_{2}$ and WSe$_{2}$ monolayers. We observe the hole transfer from MoSe$_{2}$ to WSe$_{2}$ through the hBN barrier with a time constant of 500 ps, which is over 3 orders of magnitude slower than that between TMD layers without a spacer. Furthermore, we observe strong competition between the interlayer charge transfer and intralayer exciton-exciton annihilation processes at high excitation densities. Our work opens possibilities to understand charge transfer pathways in TMD/hBN/TMD heterostructures for the efficient generation and control of interlayer excitons.

cond-mat.mes-hall↗

arXiv2022

Identification of exciton complexes in a charge-tuneable Janus WSeS monolayer

Janus transition-metal dichalcogenide monolayers are fully artificial materials, where one plane of chalcogen atoms is replaced by chalcogen atoms of a different type. Theory predicts an in-built out-of-plane electric field, giving rise to long-lived, dipolar excitons, while preserving direct-bandgap optical transitions in a uniform potential landscape. Previous Janus studies had broad photoluminescence (>15 meV) spectra obfuscating their excitonic origin. Here, we identify the neutral, and negatively charged inter- and intravalley exciton transitions in Janus WSeS monolayer with $\sim 6$ meV optical linewidth. We combine a recently developed synthesis technique, with the integration of Janus monolayers into vertical heterostructures, allowing doping control. Further, magneto-optic measurements indicate that monolayer WSeS has a direct bandgap at the K points. This work provides the foundation for applications such as nanoscale sensing, which relies on resolving excitonic energy shifts, and photo-voltaic energy harvesting, which requires efficient creation of long-lived excitons and integration into vertical heterostructures.

cond-mat.mes-hall↗

arXiv2022

Mapping Charge Excitations in Generalized Wigner Crystals

Transition metal dichalcogenide-based moire superlattices exhibit very strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. Here we describe a new scanning single-electron charging (SSEC) spectroscopy technique with nanometer spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS2 moire heterostructures. High-resolution SSEC spectroscopy was achieved by combining scanning tunneling microscopy (STM) with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of order 50meV exist for the 1/3 and 2/3 generalized Wigner crystal states.

cond-mat.mes-hall↗

arXiv2022

Revealing the order parameter dynamics of 1T-TiSe$_2$ following optical excitation

The formation of a charge density wave state is characterized by an order parameter. The way it is established provides unique information on both the role that correlation plays in driving the charge density wave formation and the mechanism behind its formation. Here we use time and angle resolved photoelectron spectroscopy to optically perturb the charge-density phase in 1T-TiSe$_2$ and follow the recovery of its order parameter as a function of energy, momentum and excitation density. Our results reveal that two distinct orders contribute to the gap formation, a CDW order and pseudogap-like order, manifested by an overall robustness to optical excitation. A detailed analysis of the magnitude of the the gap as a function of excitation density and delay time reveals the excitonic long-range nature of the CDW gap and the short-range Jahn-Teller character of the pseudogap order. In contrast to the gap, the intensity of the folded Se$_{4p}$* band can only give access to the excitonic order. These results provide new information into the the long standing debate on the origin of the gap in TiSe$_2$ and place it in the same context of other quantum materials where a pseudogap phase appears to be a precursor of long-range order.

cond-mat.str-el↗

arXiv2022

Hysteresis-Free High Mobility Graphene Encapsulated in Tungsten Disulfide

High mobility is a crucial requirement for a large variety of electronic device applications. The state-of-the-art for high quality graphene devices is based on heterostructures made with graphene encapsulated in $>80\,$nm-thick flakes of hexagonal boron nitride (hBN). Unfortunately, scaling up multilayer hBN while precisely controlling the number of layers remains an elusive challenge, resulting in a rough material unable to enhance the mobility of graphene. This leads to the pursuit of alternative, scalable materials, which can be simultaneously used as substrate and encapsulant for graphene. Tungsten disulfide (WS$_2$) is a transition metal dichalcogenide, which was successfully grown in large ($\sim$mm-size) multi-layers by chemical vapour deposition. However, the resistance \textit{vs} gate voltage characteristics when gating graphene through WS$_2$ exhibit largely hysteretic shifts of the charge neutrality point (CNP) in the order of $Δn\sim$2.6$\cdot$10$^{11}$ cm$^{-2}$, hindering the use of WS$_2$ as a reliable encapsulant. The hysteresis originates due to the charge traps from sulfur vacancies present in WS$_2$. In this work, we report for the first time the use of WS$_2$ as a substrate and the overcoming of hysteresis issues by chemically treating WS$_2$ with a super-acid, which passivates these vacancies and strips the surface from contaminants. The hysteresis is significantly reduced below the noise level by at least a factor five (to $Δn<$5$\cdot$10$^{10}$ cm$^{-2}$) and, simultaneously, the room-temperature mobility of WS$_2$-encapsulated graphene is as high as $\sim$6.2$\cdot$10$^{4}$ cm$^{-2}$V$^{-1}$s$^{-1}$ at a carrier density $n$ $\sim$1$\cdot$ 10$^{12}$ cm$^{-2}$. Our results promote WS$_2$ to a valid alternative to hBN as encapsulant for high-performance graphene devices.

cond-mat.mes-hall↗

arXiv2022

Skyrmion formation in Ni-based Janus dihalide monolayers: Interplay between magnetic frustration and Dzyaloshinskii-Moriya interaction

We present a comprehensive theory of the magnetic phases in monolayer nickel-based Janus dihalides (NiIBr, NiICl, NiBrCl) through a combination of first-principles calculations and atomistic simulations. Phonon band structure calculations and finite temperature molecular dynamics simulations show that Ni-dihalide Janus monolayers are stable. The parameters of the interacting spin Hamiltonian extracted from ab initio calculations show that nickel-dihalide Janus monolayers exhibit varying degrees of magnetic frustration together with a large Dzyaloshinskii-Moriya interaction due to their inherent inversion symmetry breaking. The atomistic simulations reveal a delicate interplay between these two competing magnetic interactions in giving rise to skyrmion formation.

cond-mat.str-el↗

arXiv2022

Strong Effects of Interlayer Interaction on Valence-Band Splitting in Transition Metal Dichalcogenides

Understanding the origin of valence band maxima (VBM) splitting in transition metal dichalcogenides (TMDs) is important because it governs the unique spin and valley physics in monolayer and multilayer TMDs. In this work, we present our systematic study of VBM splitting ($Δ$) in atomically thin MoS$_2$ and WS$_2$ by employing photocurrent spectroscopy as we change the temperature and the layer numbers. We found that VBM splitting in monolayer MoS$_2$ and WS$_2$ depends strongly on temperature, which contradicts the theory that spin-orbit coupling solely determines the VBM splitting in monolayer TMDs. We also found that the rate of change of VBM splitting with respect to temperature ($m=\frac{\partialΔ}{\partial T}$) is the highest for monolayer (-0.14 meV/K for MoS$_2$) and the rate decreases as the layer number increases ($m ~ 0$ meV/K for 5 layers MoS$_2$). We performed density functional theory (DFT) and the GW with Bethe-Salpeter Equation (GW-BSE) calculations to determine the electronic band structure and optical absorption for a bilayer MoS$_2$ with different interlayer separations. Our simulations agree with the experimental observations and demonstrate that the temperature dependence of VBM splitting in atomically thin monolayer and multilayer TMDs originates from the changes in the interlayer coupling strength between the neighboring layers. By studying two different types of TMDs and many different layer thicknesses, we also demonstrate that VBM splitting also depends on the layer numbers and type of transition metals. Our study will help understand the role spin-orbit coupling and interlayer interaction play in determining the VBM splitting in quantum materials and develop next-generation devices based on spin-orbit interactions.

cond-mat.mes-hall↗

arXiv2022

Mapping the dispersion of the occupied and unoccupied band structure in photoexcited 1T-TiSe$_2$

Charge density waves (CDW) are states of broken symmetry with a periodic modulation of charge and lattice typically leading to the opening of a gap in the band structure. In the model CDW system 1T-TiSe$_2$ such a gap opens up between its Se$_{4p}$ valence and Ti$_{3d}$ conduction band, accompanied by a change of dispersion. These changes are crucial in understanding the CDW phase, as they provide a measure of the Se$_{4p}$-Ti$_{3d}$ hybridization strength and characteristic mechanistic features. Using time- and angle-resolved photoelectron spectroscopy (trARPES), the unoccupied band structure is populated with near-infrared (NIR) pump pulses which allows to to directly visualize the parabolically-shaped Ti$_{3d}$ conduction band. Furthermore, we observe a transient change of effective mass in the Se$_{4p}$ valence band following photoexcitation. This occurs alongside an overall reduction due to weakening of the CDW phase and is accompanied by an oscillating component with the frequency of the characteristic A$_{1g}$ phonon. These observations, enabled by trAPRES, highlight the importance of the lattice contributions in establishing the CDW order in 1T-TiSe$_2$.

cond-mat.str-el↗

arXiv2022

Brightening of a dark monolayer semiconductor via strong light-matter coupling in a cavity

Engineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe2 with spin-forbidden, optically dark ground state. In our experiments, we harness the strong light-matter coupling between cavity photon and the high energy, spin-allowed bright exciton, and thus creating two bright polaritonic modes in the optical bandgap with the lower polariton mode pushed below the WSe2 dark state. We demonstrate that in this regime the commonly observed luminescence quenching stemming from the fast relaxation to the dark ground state is prevented, which results in the brightening of this intrinsically dark material. We probe this effective brightening by temperature-dependent photoluminescence, and we find an excellent agreement with a theoretical model accounting for the inversion of the band ordering and phonon-assisted polariton relaxation.

cond-mat.mes-hall↗