arXiv subjects

Sefaattin Tongay

Publications and source records attributed to Sefaattin Tongay.

At least 73 records · Page 4Linked to original sources

arXiv2019

Optical detection of Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices

Moiré superlattices are emerging as a new route for engineering strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states in magic-angle twisted bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices. Transition metal dichalcogenide (TMDC) moiré heterostructures provide another exciting model system to explore correlated quantum phenomena, with the addition of strong light-matter interactions and large spin-orbital coupling. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moiré superlattices. Our sensitive optical detection technique reveals a Mott insulator state at one hole per superlattice site (ν = 1), and surprising insulating phases at fractional filling factors ν = 1/3 and 2/3, which we assign to generalized Wigner crystallization on an underlying lattice. Furthermore, the unique spin-valley optical selection rules of TMDC heterostructures allow us to optically create and investigate low-energy spin excited states in the Mott insulator. We reveal an especially slow spin relaxation lifetime of many microseconds in the Mott insulating state, orders-of-magnitude longer than that of charge excitations. Our studies highlight novel correlated physics that can emerge in moiré superlattices beyond graphene.

cond-mat.mes-hall↗

arXiv2019

Tunable Electronic Structure in Gallium Chalcogenide van der Waals Compounds

Transition metal monochalcogenides comprise a class of two-dimensional materials with electronic band gaps that are highly sensitive to material thickness and chemical composition. Here, we explore the tunability of the electronic excitation spectrum in GaSe using angle-resolved photoemission spectroscopy. The electronic structure of the material is modified by $\textit{in-situ}$ potassium deposition as well as by forming GaS$_{x}$Se$_{1-x}$ alloy compounds. We find that potassium decouples the top-most tetra-layer of the GaSe unit cell, leading to a substantial change of the dispersion around the valence band maximum (VBM). The observed band dispersion of a single tetralayer is consistent with a transition from the direct gap character of the bulk to the indirect gap character expected for monolayer GaSe. Upon alloying with sulfur, we observe a phase transition from AB to $\text{AA}^{\prime}$ stacking. Alloying also results in a rigid energy shift of the VBM towards higher binding energies which correlates with a blue shift in the luminescence. The increase of the band gap upon sulfur alloying does not appear to change the dispersion or character of the VBM appreciably, implying that it is possible to engineer the gap of these materials while maintaining their salient electronic properties.

cond-mat.mes-hall↗

arXiv2019

Near-unity light absorption in a monolayer WS2 van der Waals heterostructure cavity

Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultra-low excitation powers. Our results are in full agreement with a quantum theoretical framework introduced to describe the light-exciton-cavity interaction. We find that the subtle interplay between the radiative, non-radiative and dephasing decay rates plays a crucial role, and unveil a universal absorption law for excitons in 2D systems. This enhanced light-exciton interaction provides a platform for studying excitonic phase-transitions and quantum nonlinearities and enables new possibilities for 2D semiconductor-based optoelectronic devices.

physics.optics↗

arXiv2019

Direct Observation of Gate Tunable Dark Trions in Monolayer WSe2

Spin-forbidden intravalley dark exciton in tungsten-based transition metal dichalcogenides (TMDCs), owing to its unique spin texture and long lifetime, has attracted intense research interest. Here, we show that we can control the dark exciton electrostatically by dressing it with one free electron or free hole, forming the dark trions. The existence of the dark trions is suggested by the unique magneto-photoluminescence spectroscopy pattern of the boron nitride (BN) encapsulated monolayer WSe2 device at low temperature. The unambiguous evidence of the dark trions is further obtained by directly resolving the radiation pattern of the dark trions through back focal plane imaging. The dark trions possess binding energy of ~ 15 meV, and it inherits the long lifetime and large g-factor from the dark exciton. Interestingly, under the out-of-plane magnetic field, dressing the dark exciton with one free electron or hole results in distinctively different valley polarization of the emitted phonon, a result of the different intervalley scattering mechanism for the electron and hole. Finally, the lifetime of the positive dark trion can be further tuned from ~ 50 to ~ 215 ps by controlling the gate voltage. The gate tunable dark trions ushers in new opportunities for excitonic optoelectronics and valleytronics.

cond-mat.mes-hall↗

arXiv2019

Strain-tunable Single Photon Sources in WSe2 Monolayers

The appearance of single photon sources in atomically thin semiconductors holds great promises for the development of a flexible and ultra-compact quantum technology, in which elastic strain engineering can be used to tailor their emission properties. Here, we show a compact and hybrid 2D-semiconductor-piezoelectric device that allows for controlling the energy of single photons emitted by quantum emitters localized in wrinkled WSe2 monolayers. We demonstrate that strain fields exerted by the piezoelectric device can be used to tune the energy of localized excitons in WSe2 up to 18 meV in a reversible manner, while leaving the single photon purity unaffected over a wide range. Interestingly, we find that the magnitude and in particular the sign of the energy shift as a function of stress is emitter dependent. With the help of finite element simulations we suggest a simple model that explains our experimental observations and, furthermore, discloses that the type of strain (tensile or compressive) experienced by the quantum emitters strongly depends on their localization across the wrinkles. Our findings are of strong relevance for the practical implementation of single photon devices based on two-dimensional materials as well as for understanding the effects of strain on their emission properties.

cond-mat.mes-hall↗

arXiv2019

Emerging Photoluminescence from the Dark-Exciton Phonon Replica in Monolayer WSe2

Tungsten-based monolayer transition metal dichalcogenides host a long-lived dark exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E" phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin.

cond-mat.mes-hall↗

arXiv2019

Optical valley Hall effect for highly valley-coherent exciton-polaritons in an atomically thin semiconductor

Spin-orbit coupling is a fundamental mechanism that connects the spin of a charge carrier with its momentum. Likewise, in the optical domain, a synthetic spin-orbit coupling is accessible, for instance, by engineering optical anisotropies in photonic materials. Both, akin, yield the possibility to create devices directly harnessing spin- and polarization as information carriers. Atomically thin layers of transition metal dichalcogenides provide a new material platform which promises intrinsic spin-valley Hall features both for free carriers, two-particle excitations (excitons), as well as for photons. In such materials, the spin of an exciton is closely linked to the high-symmetry point in reciprocal space it emerges from. Here, we demonstrate, that spin, and hence valley selective propagation is accessible in an atomically thin layer of MoSe2, which is strongly coupled to a microcavity photon mode. We engineer a wire-like device, where we can clearly trace the flow, and the helicity of exciton-polaritons expanding along a channel. By exciting a coherent superposition of K and K- tagged polaritons, we observe valley selective expansion of the polariton cloud without neither any applied external magnetic fields nor coherent Rayleigh scattering. Unlike the valley Hall effect for TMDC excitons, the observed optical valley Hall effect (OVHE) strikingly occurs on a macroscopic scale, and clearly reveals the potential for applications in spin-valley locked photonic devices.

cond-mat.mes-hall↗

arXiv2019

Resolving spin, valley, and moiré quasi-angular momentum of interlayer excitons in WSe2/WS2 heterostructures

Moiré superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moiré effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moiré superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moiré quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at different moiré sites. Here we report the observation of multiple interlayer exciton states coexisting in a WSe2/WS2 moiré superlattice and unambiguously determine their spin, valley, and moiré QAM through novel resonant optical pump-probe spectroscopy and photoluminescence excitation spectroscopy. We demonstrate that interlayer excitons localized at different moiré sites can exhibit opposite optical selection rules due to the spatially-varying moiré QAM. Our observation reveals new opportunities to engineer interlayer exciton states and valley physics with moiré superlattices for optoelectronic and valleytronic applications.

cond-mat.mes-hall↗

arXiv2018

Valley-dependent Exciton Fine Structure and Autler-Townes Doublets from Berry Phases in Monolayer Molybdenum Diselenide

The Berry phase of Bloch states can have profound effects on electron dynamics lead to novel transport phenomena, such as the anomalous Hall effect and the valley Hall effect. Recently, it was predicted that the Berry phase effect can also modify the exciton states in transition metal dichalcogenide monolayers, and lift the energy degeneracy of exciton states with opposite angular momentum through an effective valley-orbital coupling. Here, we report the first observation and control of the Berry-phase induced splitting of the 2p-exciton states in monolayer molybdenum diselenide using the intraexciton optical Stark spectroscopy. We observe the time-reversal-symmetric analog of the orbital Zeeman effect resulting from the valley-dependent Berry phase, which leads to energy difference of +14 (-14) meV between the $2p^+$ and $2p^-$ exciton states in +K (-K) valley, consistent with the ordering from our ab initio GW-BSE results. In addition, we show that the light-matter coupling between intraexciton states are remarkably strong, leading to prominent valley-dependent Autler-Townes doublet under resonant driving. Our study opens up new pathways to coherently manipulate the quantum states and excitonic excitation with infrared radiation in two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2018

Observation of Moiré Excitons in WSe2/WS2 Heterostructure Superlattices

Moiré superlattices provide a powerful tool to engineer novel quantum phenomena in two-dimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moiré superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices. In addition to their dramatic effects on the single particle states, moiré superlattices were recently predicted to host novel excited states, such as moiré exciton bands. Here we report the first observation of moiré superlattice exciton states in nearly aligned WSe2/WS2 heterostructures. These moiré exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe2 monolayers and in large-twist-angle WSe2/WS2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moiré potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.

cond-mat.mes-hall↗

arXiv2018

Excitonic Complexes and Emerging Interlayer Electron-Phonon Coupling in BN Encapsulated Monolayer Semiconductor Alloy: WS0.6Se1.4

Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. While WS2 and WSe2 are known for their excellent valley polarization due to the strong spin-orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS2xSe2(1-x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN encapsulated monolayer WS0.6Se1.4 inherits the superior optical properties of tungsten-based TMDs, including a trion splitting of ~ 6 meV and valley polarization as high as ~60%. In particular, we demonstrate for the first time the emerging and gate-tunable interlayer electron-phonon coupling in the BN/WS0.6Se1.4/BN van der Waals heterostructure, which renders the otherwise optically silent Raman modes visible. In addition, the emerging Raman signals can be drastically enhanced by the resonant coupling to the 2s state of the monolayer WS0.6Se1.4 A exciton. The BN/WS2xSe2(1-x)/BN van der Waals heterostructure with a tunable bandgap thus provides an exciting platform for exploring the valley degree of freedom and emerging excitonic physics in two-dimension.

cond-mat.mes-hall↗

arXiv2018

Integration of atomically thin layers of transition metal dichalcogenides into high-Q, monolithic Bragg-cavities - an experimental platform for the enhancement of optical interaction in 2D-materials

We demonstrate a new approach to integrate single layer MoSeR2R and WSeR2R flakes into monolithic all-dielectric planar high-quality micro-cavities. These distributed-Bragg-reflector (DBR) cavities may e.g. be tuned to match the exciton resonance of the 2D-materials. They are highly robust and compatible with cryogenic and room-temperature operation. The integration is achieved by a customized ion-assisted physical vapor deposition technique, which does not degrade the optical properties of the 2D-materials. The monolithic 2D resonator is shown to have a high Q-factor in excess of 4500. We use photoluminescence (PL) experiments to demonstrate that the coating procedure with an SiO2 coating on a prepared surface does not significantly alter the electrooptical properties of the 2D-materials. Moreover, we observe a resonance induced modification of the PL-spectrum for the DBR embedded flake. Our system thus represents a versatile platform to resonantly enhance and tailor light-matter-interaction in 2D-materials. The gentle processing conditions would also allow the integration of other sensitive materials into these highly resonant structures.

physics.optics↗

arXiv2018

Dynamics of liquid crystal on hexagonal lattice

Nematic liquid crystal (LC) molecules adsorbed on two dimensional materials are aligned along the crystal directions of the hexagonal lattice. It was demonstrated that short electric pulses can reorient the aligned LC molecules in the preferred armchair direction of hexagonal boron nitride (h-BN). Several states with a variety of colors were obtained by changing the direction and strength of the electric pulses. The ab initio calculations based on density functional theory was carried out to determine the favorable adsorption configurations of the LC molecules on the h-BN surface. A non-volatile display, in which pixel resolution can be determined by grains of hexagonal surface, is proposed, which can offer a pathway towards dynamic high-quality pixels with low power consumption, and could define a new paradigm for all non-volatile display applications.

cond-mat.soft↗

arXiv2018

Charge-tuneable biexciton complexes in monolayer WSe$_{2}$

Multi-exciton states such as biexcitons, albeit theoretically predicted, have remained challenging to identify in atomically thin transition metal dichalcogenides so far. Here, we use excitation-power, electric-field and magnetic-field dependence of photoluminescence to report direct experimental evidence of two biexciton complexes in monolayer tungsten diselenide: the neutral and the negatively charged biexciton. We demonstrate bias-controlled switching between these two states, we determine their internal structure and we resolve a fine-structure splitting of 2.5 meV for the neutral biexciton. Our results unveil multi-particle exciton complexes in transition metal dichalcogenides and offer direct routes to their deterministic control in many-body quantum phenomena.

cond-mat.mes-hall↗

arXiv2018

Observation of bosonic condensation in a hybrid monolayer MoSe2-GaAs microcavity

Condensation of bosons into a macroscopic quantum state belongs to the most intriguing phenomena in nature. It was first realized in quantum gases of ultra-cold atoms, but more recently became accessible in open-dissipative, exciton-based solid-state systems at elevated temperatures. Semiconducting monolayer crystals have emerged as a new platform for studies of strongly bound excitons in ultimately thin materials. Here, we demonstrate the formation of a bosonic condensate driven by excitons hosted in an atomically thin layer of MoSe2, strongly coupled to light in a solid-state resonator. The structure is operated in the regime of collective strong coupling, giving rise to hybrid exciton-polariton modes composed of a Tamm-plasmon resonance, GaAs quantum well excitons and two-dimensional excitons confined in a monolayer of MoSe2. Polariton condensation in a monolayer crystal manifests by a superlinear increase of emission intensity from the hybrid polariton mode at injection powers as low as 4.8 pJ/pulse, as well as its density-dependent blueshift and a dramatic collapse of the emission linewidth as a hallmark of temporal coherence. Importantly, we observe a significant spin-polarization in the injected polariton condensate, a fingerprint of the core property of monolayer excitons subject to spin-valley locking. The observed effects clearly underpin the perspective of building novel highly non-linear valleytronic devices based on light-matter fluids, coherent bosonic light sources based on atomically thin materials, and paves the way towards studying materials with unconventional topological properties in the framework of bosonic condensation.

cond-mat.quant-gas↗

arXiv2017

Optically discriminating carrier-induced quasiparticle band gap and exciton energy renormalization in monolayer MoS2

Optoelectronic excitations in monolayer MoS2 manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena - critical to both many-body physics exploration and device applications - presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energies. The results explicitly disentangle the competing effects and highlight longstanding theoretical predictions of large carrier-induced band gap and exciton renormalization in 2D semiconductors.

cond-mat.mtrl-sci↗

arXiv2017

Synthesis of Highly Anisotropic Semiconducting GaTe Nanomaterials and Emerging Properties Enabled by Epitaxy

Pseudo-one dimensional (pseudo-1D) materials are a new-class of materials where atoms are arranged in chain like structures in two-dimensions (2D). Examples include recently discovered black phosphorus, ReS2 and ReSe2 from transition metal dichalcogenides, TiS3 and ZrS3 from transition metal trichalcogenides and most recently GaTe. The presence of structural anisotropy impacts their physical properties and leads to direction dependent light-matter interactions, dichroic optical responses, high mobility channels, and anisotropic thermal conduction. Despite the numerous reports on the vapor phase growth of isotropic TMDCs and post transition metal chalcogenides such as MoS2 and GaSe, the synthesis of pseudo-1D materials is particularly difficult due to the anisotropy in interfacial energy, which stabilizes dendritic growth rather than single crystalline growth with well-defined orientation. The growth of monoclinic GaTe has been demonstrated on flexible mica substrates with superior photodetecting performance. In this work, we demonstrate that pseudo-1D monoclinic GaTe layers can be synthesized on a variety of other substrates including GaAs (111), Si (111) and c-cut sapphire by physical vapor transport techniques. High resolution transmission electron microscopy (HRTEM) measurements, together with angle resolved micro-PL and micro-Raman techniques, provide for the very first time atomic scale resolution experiments on pseudo-1D structures in monoclinic GaTe and anisotropic properties. Interestingly, GaTe nanomaterials grown on sapphire exhibit highly efficient and narrow localized emission peaks below the band gap energy, which are found to be related to select types of line and point defects as evidenced by PL and Raman mapping scans. It makes the samples grown on sapphire more prominent than those grown on GaAs and Si, which demonstrate more regular properties.

cond-mat.mtrl-sci↗

arXiv2016

Observation of Ultralong Valley Lifetime in WSe2/MoS2 Heterostructures

The valley degree of freedom in two-dimensional (2D) crystals recently emerged as a novel information carrier in addition to spin and charge. The intrinsic valley lifetime in 2D transition metal dichalcoginides (TMD) is expected to be remarkably long due to the unique spin-valley locking behavior, where the inter-valley scattering of electron requires simultaneously a large momentum transfer to the opposite valley and a flip of the electron spin. The experimentally observed valley lifetime in 2D TMDs, however, has been limited to tens of nanoseconds so far. Here we report efficient generation of microsecond-long lived valley polarization in WSe2/MoS2 heterostructures by exploiting the ultrafast charge transfer processes in the heterostructure that efficiently creates resident holes in the WSe2 layer. These valley-polarized holes exhibit near unity valley polarization and ultralong valley lifetime: we observe a valley-polarized hole population lifetime of over 1 us, and a valley depolarization lifetime (i.e. inter-valley scattering lifetime) over 40 us at 10 Kelvin. The near-perfect generation of valley-polarized holes in TMD heterostructures with ultralong valley lifetime, orders of magnitude longer than previous results, opens up new opportunities for novel valleytronics and spintronics applications.

cond-mat.mtrl-sci↗