arXiv subjects

S. Tongay

Publications and source records attributed to S. Tongay.

At least 19 recordsLinked to original sources

arXiv2023

Monolayer WS$_2$ electro- and photo-luminescence enhancement by TFSI treatment

Layered material heterostructures (LMHs) can be used to fabricate electroluminescent devices operating in the visible spectral region. A major advantage of LMH-light emitting diodes (LEDs) is that electroluminescence (EL) emission can be tuned across that of different exciton complexes (e.g. biexcitons, trions, quintons) by controlling the charge density. However, these devices have an EL quantum efficiency as low as$\sim$10$^{-4}$\%. Here, we show that the superacid bis-(triuoromethane)sulfonimide (TFSI) treatment of monolayer WS$_2$-LEDs boosts EL quantum efficiency by over one order of magnitude at room temperature. Non-treated devices emit light mainly from negatively charged excitons, while the emission in treated ones predominantly involves radiative recombination of neutral excitons. This paves the way to tunable and efficient LMH-LEDs

cond-mat.mtrl-sci↗

arXiv2021

Intrinsic circularly-polarized exciton emission in a twisted van-der-Waals heterostructure

The investigation of excitons in van-der-Waals heterostructures has led to profound insights into the interplay of crystal symmetries and fundamental effects of light-matter coupling. In particular, the polarization selection rules in undistorted, slightly twisted heterostructures of MoSe$_2$/WSe$_2$ were found to be connected with the Moiré superlattice. Here, we report the emergence of a significant degree of circular polarization of excitons in such a hetero-structure upon non-resonant driving with a linearly polarized laser. The effect is present at zero magnetic field, and sensibly reacts on perpendicularly applied magnetic field. The giant magnitude of polarization, which cannot be explained by conventional birefringence or optical activity of the twisted lattice, suggests a kinematic origin arising from an emergent pyromagnetic symmetry in our structure, which we exploit to gain insight into the microscopic processes of our device.

cond-mat.mes-hall↗

arXiv2021

Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder

Using time-resolved optical Kerr rotation, we measure the low temperature valley dynamics of resident electrons and holes in exfoliated WSe$_2$ monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically-gated WSe$_2$ monolayers having different dielectric environments. In a fully-encapsulated structure (hBN/WSe$_2$/hBN, where hBN is hexagonal boron nitride), valley relaxation is found to be monoexponential. The valley relaxation time $τ_v$ is quite long ($\sim$10~$μ$s) at low carrier densities, but decreases rapidly to less than 100~ns at high electron or hole densities $\gtrsim$2 $\times 10^{12}$~cm$^{-2}$. In contrast, in a partially-encapsulated WSe$_2$ monolayer placed directly on silicon dioxide (hBN/WSe$_2$/SiO$_2$), carrier valley relaxation is multi-exponential at low carrier densities. The difference is attributed to environmental disorder from the SiO$_2$ substrate. Unexpectedly, very small out-of-plane magnetic fields can increase $τ_v$, especially in the hBN/WSe$_2$/SiO$_2$ structure, suggesting that localized states induced by disorder can play an important role in depolarizing spins and mediating the valley relaxation of resident carriers in monolayer transition metal-dichalcogenide semiconductors.

cond-mat.mtrl-sci↗

arXiv2021

Purcell-enhanced single photon source based on a deterministically placed WSe$_{2}$ monolayer quantum dot in a circular Bragg grating cavity

We demonstrate a deterministic Purcell-enhanced single-photon source realized by integrating an atomically thin WSe$_{2}$ layer with a circular Bragg grating cavity. The cavity significantly enhances the photoluminescence from the atomically thin layer, and supports single-photon generation with $g^{(2)}(0)<0.25$. We observe a consistent increase of the spontaneous emission rate for WSe$_{2}$ emitters located in the center of the Bragg grating cavity. These WSe$_{2}$ emitters are self-aligned and deterministically coupled to such a broadband cavity, configuring a new generation of deterministic single-photon sources, characterized by their simple and low-cost production and intrinsic scalability.

quant-ph↗

arXiv2020

Synthesis, Engineering, and Theory of 2D van der Waals Magnets

Spontaneous magnetic order is a routine instance in three-dimensional (3D) materials but for a long time, it remained elusive in the 2D world. Recently, the first examples of (stand-alone) 2D van der Waals (vdW) crystals with magnetic order, either antiferromagnetic or ferromagnetic, have been reported. In this review, we describe the state of the art of the nascent field of magnetic 2D materials focusing on synthesis, engineering, and theory aspects. We also discuss challenges and some of the many different promising directions for future work.

cond-mat.mtrl-sci↗

arXiv2020

Demonstration of a polariton step potential by local variation of light-matter coupling in a van-der-Waals heterostructure

The large oscillator strength of excitons in transition metal dichalcogenide layers facilitates the formation of exciton-polariton resonances for monolayers and van-der-Waals heterostructures embedded in optical microcavities. Here, we show, that locally changing the number of layers in a WSe2/hBN/WSe2 van-der-Waals heterostructure embedded in a monolithic, high-quality-factor cavity gives rise to a local variation of the coupling strength. This effect yields a polaritonic stair case potential, which we demonstrate at room temperature. Our result paves the way towards engineering local polaritonic potentials at length scales down to atomically sharp interfaces, based on purely modifying its real part contribution via the coherent light-matter coupling strength g.

cond-mat.mes-hall↗

arXiv2018

Pressure dependence of direct optical transitions in ReS2 and ReSe2

We present an experimental and theoretical study of the electronic band structure of ReS2 and ReSe2 at high hydrostatic pressures. The experiments are performed by photoreflectance spectroscopy and are analyzed in terms of ab initio calculations within the density functional theory. Experimental pressure coefficients for the two most dominant excitonic transitions are obtained and compared with those predicted by the calculations. We assign the transitions to the Z k-point of the Brillouin zone and other k-points located away from highsymmetry points. The origin of the pressure coefficients of the measured direct transitions is discussed in terms of orbital analysis of the electronic structure and van der Waals interlayer interaction. The anisotropic optical properties are studied at high pressure by means of polarization-resolved photoreflectance measurements.

cond-mat.mtrl-sci↗

arXiv2017

Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures

The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A-exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing to extrapolate an exciton binding energy of about 220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.

cond-mat.mtrl-sci↗

arXiv2017

Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics

The strong light matter interaction and the valley selective optical selection rules make monolayer (ML) MoS2 an exciting 2D material for fundamental physics and optoelectronics applications. But so far optical transition linewidths even at low temperature are typically as large as a few tens of meV and contain homogenous and inhomogeneous contributions. This prevented in-depth studies, in contrast to the better-characterized ML materials MoSe2 and WSe2. In this work we show that encapsulation of ML MoS2 in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as we measure in photoluminescence and reflectivity a FWHM down to 2 meV at T = 4K. This indicates that surface protection and substrate flatness are key ingredients for obtaining stable, high quality samples. Among the new possibilities offered by the well-defined optical transitions we measure the homogeneous broadening induced by the interaction with phonons in temperature dependent experiments. We uncover new information on spin and valley physics and present the rotation of valley coherence in applied magnetic fields perpendicular to the ML.

cond-mat.mtrl-sci↗

arXiv2016

Monolayer MoSe2: A candidate for room temperature polaritonics

Monolayered MoSe2 is a promising new material to investigate advanced light-matter coupling as it hosts stable and robust excitons with comparably narrow optical resonances. In this work, we investigate the evolution of the lowest lying excitonic transition, the so-called A-valley exciton, with temperature. We find a strong, phonon-induced temperature broadening of the resonance, and more importantly, a reduction of the oscillator strength for increased temperatures. Based on these experimentally extracted, temperature dependent parameters, we apply a coupled oscillator model to elucidate the possibility to observe the strong coupling regime between the A-exciton and a microcavity resonance in three prototypical photonic architectures with varying mode volumes. We find that the formation of exciton-polaritons up to ambient conditions in short, monolithic dielectric and Tamm-based structures seems feasible. In contrast, a temperature-induced transition into the weak coupling regime can be expected for structures with extended effective cavity length. Based on these findings, we calculate and draw the phase diagram of polariton Bosonic condensation in a MoSe2 cavity.

cond-mat.mes-hall↗

arXiv2016

Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers

We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $τ_{rad}=1.8\pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $\leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.

cond-mat.mtrl-sci↗

arXiv2015

Polarization and time-resolved photoluminescence spectroscopy of excitons in MoSe2 monolayers

We investigate valley exciton dynamics in MoSe2 monolayers in polarization- and time-resolved photoluminescence (PL) spectroscopy at 4K. Following circularly polarized laser excitation, we record a low circular polarization degree of the PL of typically $\leq5\%$. This is about 10 times lower than the polarization induced under comparable conditions in MoS2 and WSe2 monolayers. The evolution of the exciton polarization as a function of excitation laser energy and power is monitored in PL excitation (PLE) experiments. Fast PL emission times are recorded for both the neutral exciton of $\leq3$ ps and for the charged exciton (trion) of 12 ps.

cond-mat.mtrl-sci↗

arXiv2013

Anomalous Raman Spectra and Thickness Dependent Electronic properties of WSe2

Typical Raman spectra of transition metal dichalcogenides (TMDs) display two prominent peaks, E2g and A1g, that are well separated from each other. We find that these modes are degenerate in bulk WSe2 yielding one single Raman peak. As the dimensionality is lowered, the observed peak splits in two as a result of broken degeneracy. In contrast to our experimental findings, our phonon dispersion calculations reveal that these modes remain degenerate independent of the number of layers. Interestingly, for minuscule biaxial strain the degeneracy is preserved but once the crystal symmetry is broken by uniaxial strain, the degeneracy is lifted. Our calculated phonon dispersion for uniaxially strained WSe2 shows a perfect match to the measured Raman spectrum which suggests that uniaxial strain exists in WSe2 flakes possibly induced during the sample preparation and/or as a result of interaction between WSe2 and the substrate. Furthermore, we find that WSe2 undergoes an indirect to direct bandgap transition from bulk to monolayers which is ubiquitous for semiconducting TMDs. These results not only allow us to understand the vibrational properties of WSe2 but also provides detailed insight to their physical properties.

cond-mat.mtrl-sci↗

arXiv2012

Rectification at Graphene-Semiconductor Interfaces: Zero-Gap Semiconductor Based Diodes

Using current-voltage (I-V) and capacitance-voltage (C-V) measurements, we report on the unusual physics and promising technical applications associated with the formation of Schottky barriers at the interface of a one-atom-thick zero-gap semiconductor (graphene) and conventional semiconductors. When chemical vapor deposited graphene is transferred onto n-type Si, GaAs, 4H-SiC and GaN semiconductor substrates, there is a strong van der Waals attraction that is accompanied by charge transfer across the interface and the formation of a rectifying (Schottky) barrier. Thermionic emission theory in conjunction with the Schottky-Mott model within the context of bond-polarization theory provides a surprisingly good description of the electrical properties. Applications, such as to sensors where in forward bias there is exponential sensitivity to changes in the Schottky barrier height due to the presence of absorbates on the graphene or to analogue devices for which Schottky barriers are integral components are promising because of graphene's mechanical stability, its resistance to diffusion, its robustness at high temperatures and its demonstrated capability to embrace multiple functionalities.

cond-mat.mtrl-sci↗

arXiv2011

Ultrapure Multilayer Graphene in Bromine Intercalated Graphite

We investigate the optical properties of bromine intercalated highly orientated pyrolytic graphite (Br-HOPG) and provide a novel interpretation of the data. We observe new absorption features below 620 meV which are absent in the absorption spectrum of graphite. Comparing our results with those of theoretical studies on graphite, single and bilayer graphene as well as recent optical studies of multilayer graphene, we conclude that Br-HOPG contains the signatures of ultrapure bilayer, single layer graphene, and graphite. The observed supermetallic conductivity of Br-HOPG is identified with the presence of very high mobility (~ 121,000 cm2V-1s-1 at room temperature and at very high carrier density) multilayer graphene components in our sample. This could provide a new avenue for single and multilayer graphene research.

cond-mat.mtrl-sci↗

arXiv2010

Finite size effects with variable range exchange coupling in thin-film Pd/Fe/Pd trilayers

The magnetic properties of thin-film Pd/Fe/Pd trilayers in which an embedded ~1.5 A-thick ultrathin layer of Fe induces ferromagnetism in the surrounding Pd have been investigated. The thickness of the ferromagnetic trilayer is controlled by varying the thickness of the top Pd layer over a range from 8 A to 56 A. As the thickness of the top Pd layer decreases, or equivalently as the embedded Fe layer moves closer to the top surface, the saturated magnetization normalized to area and the Curie temperature decrease whereas the coercivity increases. These thickness-dependent observations for proximity-polarized thin-film Pd are qualitatively consistent with finite size effects that are well known for regular thin-film ferromagnets. The critical exponent $β$ of the order parameter (magnetization) is found to approach the mean field value of 0.5 as the thickness of the top Pd layer increases. The functional forms for the thickness dependences, which are strongly modified by the nonuniform exchange interaction in the polarized Pd, provide important new insights to understanding nanomagnetism in two-dimensions.

cond-mat.mes-hall↗

arXiv2009

Graphite based Schottky diodes formed on Si, GaAs and 4H-SiC substrates

We demonstrate the formation of semimetal graphite/semiconductor Schottky barriers where the semiconductor is either silicon (Si), gallium arsenide (GaAs) or 4H-silicon carbide (4H-SiC). Near room temperature, the forward-bias diode characteristics are well described by thermionic emission, and the extracted barrier heights, which are confirmed by capacitance voltage measurements, roughly follow the Schottky-Mott relation. Since the outermost layer of the graphite electrode is a single graphene sheet, we expect that graphene/semiconductor barriers will manifest similar behavior.

cond-mat.mtrl-sci↗

arXiv2009

Supermetallic conductivity in bromine-intercalated graphite

Exposure of highly oriented pyrolytic graphite to bromine vapor gives rise to in-plane charge conductivities which increase monotonically with intercalation time toward values (for ~6 at% Br) that are significantly higher than Cu at temperatures down to 5 K. Magnetotransport, optical reflectivity and magnetic susceptibility measurements confirm that the Br dopes the graphene sheets with holes while simultaneously increasing the interplanar separation. The increase of mobility (~ 5E4 cm^2/Vs at T=300 K) and resistance anisotropy together with the reduced diamagnetic susceptibility of the intercalated samples suggests that the observed supermetallic conductivity derives from a parallel combination of weakly-coupled hole-doped graphene sheets.

cond-mat.mtrl-sci↗