Excitons In Monolayer Research Articles

Strong coupling between excitons in transition metal dichalcogenides and optical bound states in the continuum

Being motivated by recent achievements in the rapidly developing fields of optical bound states in the continuum (BICs) and excitons in monolayers of transition metal dichalcogenides, we analyze strong coupling between BICs in $\rm Ta_2O_5$ periodic photonic structures and excitons in $\rm WSe_2$ monolayers. We demonstrate that giant radiative lifetime of BICs allow to engineer the exciton-polariton lifetime enhancing it three orders of magnitude compared to a bare exciton. We show that maximal lifetime of hybrid light-matter state can be achieved at any point of $\mathbf{k}$-space by shaping the geometry of the photonic structure. Our findings open new route for the realization of the moving exciton-polariton condensates with non-resonant pump and without the Bragg mirrors which is of paramount importance for polaritonic devices.

Optical properties of excitons in buckled two-dimensional materials in an external electric field

We study the binding energies and optical properties of direct and indirect excitons in monolayers and double layer heterostructures of Xenes: silicene, germanene, and stanene. It is demonstrated that an external electric field can be used to tune the eigenenergies and optical properties of excitons by changing the effective mass of charge carriers. The Schr\"{o}dinger equation with field-dependent exciton reduced mass is solved by using the Rytova-Keldysh (RK) potential for direct excitons, while both the RK and Coulomb potentials are used for indirect excitons. It is shown that for indirect excitons, the choice of interaction potential can cause huge differences in the eigenenergies at large electric fields and significant differences even at small electric fields. Furthermore, our calculations show that the choice of material parameters has a significant effect on the binding energies and optical properties of direct and indirect excitons. These calculations contribute to the rapidly growing body of research regarding the excitonic and optical properties of this new class of two dimensional semiconductors.

Light-matter interaction between photonic bound states in the continuum and bright excitons in transition metal dichalcogenides

Being motivated by recent achievements in the rapidly developing fields of optical bound states in the continuum (BICs) and excitons in monolayers of transition metal dichalcogenides, we analyze strong coupling between BICs in Ta2O5 periodic photonic structures and excitons in WSe2 monolayers. We demonstrate that giant radiative lifetime of BICs allow to engineer the exciton-polariton lifetime enhancing it three orders of magnitude compared to a bare exciton.

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

Bosonic condensation belongs to the most intriguing phenomena in physics, and was mostly reserved for experiments with ultra-cold quantum gases. More recently, it became accessible in exciton-based solid-state systems at elevated temperatures. Here, we demonstrate bosonic condensation 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 between a Tamm-plasmon resonance, GaAs quantum well excitons, and two-dimensional excitons confined in the monolayer crystal. Polariton condensation in a monolayer crystal manifests by a superlinear increase of emission intensity from the hybrid polariton mode, its density-dependent blueshift, and a dramatic collapse of the emission linewidth, a hallmark of temporal coherence. Importantly, we observe a significant spin-polarization in the injected polariton condensate, a fingerprint for spin-valley locking in monolayer excitons. Our results pave the way towards highly nonlinear, coherent valleytronic devices and light sources.

Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers

We investigate the optical properties of spin-triplet interlayer excitons in heterobilayer transition metal dichalcogenides in comparison with the spin-singlet ones. Surprisingly, the optical transition dipole of the spin-triplet exciton is found to be in the same order of magnitude to that of the spin-singlet exciton, in sharp contrast to the monolayer excitons where the spin-triplet species is considered as dark compared to the singlet. Unlike the monolayer excitons whose spin-conserved (spin-flip) transition dipole can only couple to light of in-plane (out-of-plane) polarisation, such restriction is removed for the interlayer excitons due to the breaking of the out-of-plane mirror symmetry. We find that as the interlayer atomic registry changes, the optical transition dipole of interlayer exciton crosses between in-plane ones of opposite circular polarizations and the out-of-plane one for both the spin-triplet and spin-singlet species. As a result, excitons of both species have non-negligible coupling into photon modes of both in-plane and out-of-plane propagations, another sharp difference from the monolayers where the exciton couples predominantly into the out-of-plane propagation channel. At given atomic registry, the spin-triplet and spin-singlet excitons have distinct valley polarisation selection rules, allowing the selective optical addressing of both the valley configuration and the spin-singlet/triplet configuration of interlayer excitons.

Encapsulated Silicon Nitride Nanobeam Cavity for Hybrid Nanophotonics

Most existing implementations of silicon nitride photonic crystal cavities rely on suspended membranes due to the low refractive index of silicon nitride. Such floating membranes are not mechanically robust, making them suboptimal for developing a hybrid optoelectronic platform where new materials, such as layered 2D materials, are transferred on a pre-existing optical cavity. To address this issue, we propose a silicon nitride nanobeam resonator design where the silicon nitride membrane is encapsulated by material with a refractive index of ~1.5, such as silicon dioxide or PMMA. The theoretically calculated quality factor of the cavities can be as large as 100,000 , with a mode-volume of 2.5 times the cubic wavelength. We fabricated the cavity, and measured the transmission spectrum with highest quality factor of 7000. We also successfully transferred monolayer tungsten diselenide on the encapsulated silicon nitride nanobeam, and demonstrated coupling of the cavity with the monolayer exciton and the defect emissions.

Optical nonlinearities of excitons in monolayer MoS2

We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of mono- layer MoS2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second harmonic generation in monolayer MoS2, and find that the third- harmonic process is efficient only for linearly polarized input light while the third-order two photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton state. The absence of linear absorption due to the band gap and the unusually strong two-photon third-order nonlinearity make the monolayer MoS2 excitonic structure a promising resource for coherent nonlinear photonics.

Microsecond dark-exciton valley polarization memory in two-dimensional heterostructures

Transition metal dichalcogenides have valley degree of freedom, which features optical selection rule and spin-valley locking, making them promising for valleytronics devices and quantum computation. For either application, a long valley polarization lifetime is crucial. Previous results showed that it is around picosecond in monolayer excitons, nanosecond for local excitons and tens of nanosecond for interlayer excitons. Here we show that the dark excitons in two-dimensional heterostructures provide a microsecond valley polarization memory thanks to the magnetic field induced suppression of valley mixing. The lifetime of the dark excitons shows magnetic field and temperature dependence. The long lifetime and valley polarization lifetime of the dark exciton in two-dimensional heterostructures make them promising for long-distance exciton transport and macroscopic quantum state generations.

Temperature dependent excitonic transition energies and linewidths of monolayer MoS2 probed by magnetic circular dichroism spectroscopy

Layered transition metal dichalcogenides (TMDs), as a new class of two-dimensional material, have received wide attention of scientific community due to their peculiar electronic and optical properties. Monolayer TMDs such as MoS2, MoSe2, WS2 and WSe2 are semiconductors with band gap energies in the visible and near-infrared region, which promises the applications in logic nano-devices, ultra-high speed photoelectric detectors and nano-lasers. Temperature has strong influences on the electronic and optical properties of semiconductors, and their applications in photonic and optoelectronic devices. Thus, the research on the temperature dependence of the energy band of monolayer TMDs is important and meaningful. Monolayer MoS2, as a prototype of TMDs, displays a weak absorption line with a strong background in original reflection or absorption spectra. The strong background has a tremendous influence on the determination of excitonic transition energy and linewidth. In this work, we adopt the reflection magnetic circular dichroism (MCD) spectroscopy in which reflection spectra and MCD spectra can be simultaneously obtained. We demonstrate that the background disturbance is eliminated in the MCD spectra, in contrast to the reflectivity spectra. And we discuss the optimization of our home-built experimental setup in detail. Through the elaborate analysis of the MCD theory, we demonstrate that the excitonic transition energy and linewidth can be directly and accurately extracted from the MCD spectrum. We perform the reflection MCD measurements on monolayer MoS2 in a temperature range of 65–300 K. The transition energies and linewidths of A and B excitons of monolayer MoS2 are extracted, respectively. Those functional parameters that describe the temperature dependence of the energy and linewidth of both excitonic transitions are evaluated and analyzed. We find that the broadening of the linewidth is related to the LO phonon scattering, and the linewidth of A exciton is clearly narrower than that of B exciton. The linewidth difference between A and B excitons might result from the stronger inter-valley coupling of B exciton. Our results indicate that MCD spectroscopy, as a modulated spectroscopy by magnetic fields, provides an easy tool to determine the features of monolayer excitons.

Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides

We present low-temperature magneto-photoluminescence experiments which demonstrate the brightening of dark excitons by an in-plane magnetic field B applied to monolayers of different semiconducting transition metal dichalcogenides. For WSe2 and WS2 monolayers, the dark exciton emission is observed at ∼50 meV below the bright exciton peak and displays a characteristic doublet structure whose intensity grows with B2, while no magnetic field induced emission peaks appear for MoSe2 monolayer. Our experiments also show that the MoS2 monolayer has a dark exciton ground state with a dark-bright exciton splitting energy of ∼100 meV.

Inverse Funnel Effect of Excitons in Strained Black Phosphorus

We study the effects of strain on the properties and dynamics of Wannier excitons in monolayer (phosphorene) and few-layer black phosphorus (BP), a promising two-dimensional material for optoelectronic applications due to its high mobility, mechanical strength and strain-tuneable direct band gap. We compare the results to the case of molybdenum disulphide (MoS$_2$) monolayers. We find that the so-called funnel effect, i.e. the possibility of controlling exciton motion by means of inhomogeneous strains, is much stronger in few-layer BP than in MoS$_2$ monolayers and, crucially, is of opposite sign. Instead of excitons accumulating isotropically around regions of high tensile strain like in MoS$_2$, excitons in BP are pushed away from said regions. This \emph{inverse} funnel effect is moreover highly anisotropic, with much larger funnel distances along the armchair crystallographic direction, leading to a directional focusing of exciton flow. A strong inverse funnel effect could enable simpler designs of funnel solar cells, and offer new possibilities for the manipulation and harvesting of light.

Stark shift and electric-field-induced dissociation of excitons in monolayerMoS2andhBN/MoS2heterostructures

Efficient conversion of photons into electrical current in two-dimensional semiconductors requires, as a first step, the dissociation of the strongly bound excitons into free electrons and holes. Here we calculate the dissociation rates and energy shift of excitons in monolayer ${\mathrm{MoS}}_{2}$ as a function of an applied in-plane electric field. The dissociation rates are obtained as the inverse lifetime of the resonant states of a two-dimensional hydrogenic Hamiltonian which describes the exciton within the Mott-Wannier model. The resonances are computed using complex scaling, and the effective masses and screened electron-hole interaction defining the hydrogenic Hamiltonian are computed from first principles. For field strengths above 0.1 V/nm the dissociation lifetime is shorter than 1 ps, which is below the lifetime associated with competing decay mechanisms. Interestingly, encapsulation of the ${\mathrm{MoS}}_{2}$ layer in just two layers of hexagonal boron nitride ($h\mathrm{BN}$), enhances the dissociation rate by around one order of magnitude due to the increased screening. This shows that dielectric engineering is an effective way to control exciton lifetimes in two-dimensional materials.

Coherent Coupling of WS2 Monolayers with Metallic Photonic Nanostructures at Room Temperature.

Room temperature strong coupling of WS2 monolayer exciton transitions to metallic Fabry-Pérot and plasmonic optical cavities is demonstrated. A Rabi splitting of 101 meV is observed for the Fabry-Pérot cavity. The enhanced magnitude and visibility of WS2 monolayer strong coupling is attributed to the larger absorption coefficient, the narrower line width of the A exciton transition, and greater spin-orbit coupling. For WS2 coupled to plasmonic arrays, the Rabi splitting still reaches 60 meV despite the less favorable coupling conditions, and displays interesting photoluminescence features. The unambiguous signature of WS2 monolayer strong coupling in easily fabricated metallic resonators at room temperature suggests many possibilities for combining light-matter hybridization with spin and valleytronics.

Radiative and nonradiative exciton energy transfer in monolayers of two-dimensional group-VI transition metal dichalcogenides

We present results on the rates of interlayer energy transfer between excitons in monolayers of two-dimensional group-VI transition metal dichalcogenides (TMDs). We consider both radiative (mediated by real photons) and nonradiative (mediated by virtual photons) mechanisms of energy transfer using a unified Green's function approach that takes into account modification of the exciton energy dispersions as a result of interactions. The large optical oscillator strengths associated with excitons in TMDs result in very fast energy transfer rates. The energy transfer times depend on the exciton momentum, exciton linewidth, and the interlayer separation and can range from values less than 100 femtoseconds to more than tens of picoseconds. Whereas inside the light cone the energy transfer rates of longitudinal and transverse excitons are comparable, outside the light cone the energy transfer rates of longitudinal excitons far exceed those of transverse excitons. Average energy transfer times for a thermal ensemble of longitudinal and transverse excitons is temperature dependent and can be smaller than a picosecond at room temperature for interlayer separations smaller than 10 nm. Energy transfer times of localized excitons range from values less than a picosecond to several tens of picoseconds. When the exciton scattering and dephasing rates are small, energy transfer dynamics exhibit coherent oscillations. Our results show that electromagnetic interlayer energy transfer can be an efficient mechanism for energy exchange between TMD monolayers.

Active Light Control of the MoS2 Monolayer Exciton Binding Energy.

Plasmonic excitation of Au nanoparticles deposited on a MoS2 monolayer changes the absorption and photoluminescence characteristics of the material. Hot electrons generated from the Au nanoparticles are transferred into the MoS2 monolayers, resulting in n-doping. The doping effect of plasmonic hot electrons modulates the dielectric permittivity of materials, resulting in a red shift of both the absorption and the photoluminescence spectrum. This spectroscopic tuning was further investigated experimentally by using different Au nanoparticle concentrations, excitation laser wavelengths, and intensities. An analytical model for the photoinduced modulation of the MoS2 dielectric function and its exciton binding energy change is developed and used to estimate the doping density of plasmonic hot electrons. Our approach is important for the development of photonic devices for active control of light by light.

Spatiotemporal dynamics of excitons in monolayer and bulk WS2.

Spatiotemporal dynamics of excitons in monolayer and bulk WS2 at room temperature is studied by transient absorption microscopy in the reflection geometry. Excitons are formed from photocarriers injected by a tightly focused 390 nm pump pulse, and monitored by detecting different reflection of a time-delayed and spatially scanned 620 nm probe pulse. We obtain exciton lifetimes of 22 ± 1 and 110 ± 10 ps in monolayer and bulk WS2, respectively. Both lifetimes are independent of the exciton density, showing the absence of multi-exciton recombination processes. Exciton diffusion coefficients of 60 ± 20 and 3.5 ± 0.5 cm(2) s(-1) are obtained in monolayer and bulk samples, respectively. These results provide a foundation for understanding excitons in this new material and its optoelectronic applications.

Excitons in a mirror: Formation of “optical bilayers” using MoS2 monolayers on gold substrates

We report coupling of excitons in monolayers of molybdenum disulphide to their mirror image in an underlying gold substrate. Excitons at the direct band gap are little affected by the substrate whereas strongly bound C-excitons associated with a van-Hove singularity change drastically. On quartz substrates only one C-exciton is visible (in the blue) but on gold substrates a strong red-shifted extra resonance in the green is seen. Exciton coupling to its image leads to formation of a “mirror biexciton” with enhanced binding energy. Estimates of this energy shift in an emitter-gold system match experiments well. The absorption spectrum of MoS2 on gold thus resembles a bilayer of MoS2 which has been created by optical coupling. Additional top-mirrors produce an “optical bulk.”

Transient Absorption Microscopy of Monolayer and Bulk WSe2

We present an experimental investigation on the exciton dynamics of monolayer and bulk WSe2 samples, both of which are studied by femtosecond transient absorption microscopy. Under the excitation of a 405 nm pump pulse, the differential reflection signal of a probe pulse (tuned to the A-exciton resonance) reaches a peak rapidly that indicates an ultrafast formation process of excitons. By resolving the differential reflection signal in both time and space, we directly determine the exciton lifetimes of 18±1 and 160±10 ps and the exciton diffusion coefficients of 15±5 and 9±3 cm2/s in the monolayer and bulk samples, respectively. From these values, we deduce other parameters characterizing the exciton dynamics such as the diffusion length, the mobility, the mean free path, and the mean free length. These fundamental parameters are useful for understanding the excitons in monolayer and bulk WSe2 and are important for applications in optoelectronics, photonics, and electronics.

Theory of neutral and charged excitons in monolayer transition metal dichalcogenides

We present a microscopic theory of neutral excitons and charged excitons (trions) in monolayers of transition metal dichalcogenides, including molybdenum disulfide. Our theory is based on an effective mass model of excitons and trions, parametrized by ab initio calculations and incorporating a proper treatment of screening in two dimensions. The calculated exciton binding energies are in good agreement with high-level many-body computations based on the Bethe-Salpeter equation. Furthermore, our calculations for the more complex trion species compare very favorably with recent experimental measurements, and provide atomistic insight into the microscopic features which determine the trion binding energy.