Optical properties of orthorhombic germanium sulfide: unveiling the anisotropic nature of Wannier excitons.

To fully explore exciton-based applications and improve their performance, it is essential to understand the exciton behavior in anisotropic materials. Here, we investigate the optical properties of anisotropic excitons in GeS encapsulated by h-BN using different approaches that combine polarization- and temperature-dependent photoluminescence (PL) measurements, ab initio calculations, and effective mass approximation (EMA). Using the Bethe-Salpeter Equation (BSE) method, we found that the optical absorption spectra in GeS are significantly affected by the Coulomb interaction included in the BSE method, which shows the importance of excitonic effects besides it exhibits a significant dependence on the direction of polarization, revealing the anisotropic nature of bulk GeS. By combining ab initio calculations and EMA methods, we investigated the quasi-hydrogenic exciton states and oscillator strength (OS) of GeS along the zigzag and armchair axes. We found that the anisotropy induces lifting of the degeneracy and mixing of the excitonic states in GeS, which results in highly non-hydrogenic features. A very good agreement with the experiment is observed.

Nickel Chalcogenide Nanoparticles-Assisted Photothermal Solar Driven Membrane Distillation (PSDMD).

Developing photothermal solar driven membrane distillation (PSDMD) is of great importance in providing fresh water for remote off-grid regions. The production of freshwater through the PSDMD is driven by the temperature difference between feed and distillate sides created via the addition of efficient photothermal nanostructures. Here we proposed nickel sulfides and nickel tellurium nanoparticles (NPs) to be loaded into the polymeric membrane to enhance its performance. Ag and CuSe NPs are also considered for comparison as they are previously used for membrane distillation (MD). Our theoretical approach showed that all of the considered NPs increased the temperature of the PVDF membrane by around a few degrees. NiS and NiTe2 NPs are the most efficient solar light-to-heat converters compared to NiTe and NiS2 NPs due to their efficient absorption over the visible range. PVDF membrane loaded with 25% of NiCs NPs and a porosity of 32% produced a transmembrane vapor flux between 22 and 27 L/m2h under a 10-times-amplified sun intensity. Under the same conditions, the PVDF membrane loaded with CuSe and Ag NPs produced 15 and 18 L/m2h of vapor flux, respectively. The implantation of NPs through the membrane not only increased its surface temperature but also possessed a high porosity which provided a higher distillation and energy efficiency that reached 58% with NiS NPs. Finally, great agreement between our theoretical model and experimental measurement is obtained.

THz mobility and polarizability: impact of transformation and dephasing on the spectral response of excitons in a 2D semiconductor.

We introduce a response theory based transformation for excitonic polarizability into mobility, which allows an in-depth analysis of optical pump-THz probe conductivity experiments, and compare the results with those of a conventional oscillator model. THz spectroscopy is of high interest e.g. for investigations in high bandwidth and low noise nanoelectronics or solar energy harvesting nanomaterials. In contrast to simple ω scaling of estimated static polarizability, suggested in the literature, an appropriate transformation of the spectral response into mobility can be achieved in principle forward and backward due to the presence of dephasing, as we show for the exemplary system of CdSe nanoplatelets. Common analysis approaches capture the excitonic properties only under specific conditions, and do not apply in many cases. We demonstrate that a thermal distribution of excitons and transitions between higher states in general have to be considered and that dephasing has to be taken into account for a proper transformation at all temperatures. The presented in-depth understanding of the exciton mobility in nanoparticles can help improve e.g. solar hydrogen generation, charge extraction efficiencies of solar cells, or light emission performance of LEDs.

Tuning optoelectronic response of lateral core-alloyed crown nanoplatelets: type-II CdSe-CdSe1-xTex.

We present a theoretical study showing that the exciton emission in the CdSe-CdSe1-xTexcore-alloyed crown heterostructure results from the tunable quasi-type II to pure type II behavior by adjusting the Te to Se ratio. We suggest that the direct crown exciton or interface indirect exciton or a dual emission can be tuned due to the altered conduction band offset. We also found that these different emissions are red-shifted with increasing the nanoplatelets (NPLs) monolayer (ML) thickness due to the quantum confinement effect. The double exciton emission develops caused by the band bowing effect occurring in the alloyed crown. The band bowing is originated from the difference between the bonding nature of the Se and Te orbitals with the Cd orbitals in the conduction band edge states. We also found that the band bowing is sensitive on the alloyed-crown ML thickness and the in-plane strain due to hybridization magnitude between the cation (Cd) and anion (Se, Te). Our results are in accord with the available experimental data. We propose the CdSe-CdSe1-xTexcore-alloyed crown NPLs as a promising contender for the near-infrared-emitting heterostructures preparation used for light-harvesting applications.

Correction: Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties.

Correction for 'Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties' by Sabrine Ayari et al., Nanoscale, 2020, 12, 14448-14458, DOI: .

Optical properties of excitons in two-dimensional transition metal dichalcogenide nanobubbles.

Strain in two-dimensional transition metal dichalcogenide has led to localized states with exciting optical properties, in particular, in view of designing one photon sources. The naturally formed nanobubbles when the MoS2 monolayer is deposited on an hBN substrate lead to a local reduction in the band gap due to strain developing in the nanobubble. The photogenerated particles are thus confined in the strain-induced potential. Using numerical diagonalization, we simulate the spectra of the confined exciton states, their oscillator strengths, and their radiative lifetimes. We show that a single state of the confined exciton is optically active, which suggests that the MoS2/hBN nanobubbles are a good candidate for the realization of single-photon sources. Furthermore, our calculations show that the localized exciton gains in activation energy and radiative lifetime inside the nanobubble, the latter decreasing toward the one of free excitons when the nanobubble size increases.

Tuning exciton diffusion, mobility and emission line width in CdSe nanoplatelets via lateral size.

We investigate the lateral size tunability of the exciton diffusion coefficient and mobility in colloidal quantum wells by means of line width analysis and theoretical modeling. We show that the exciton diffusion coefficient and mobility in laterally finite 2D systems like CdSe nanoplatelets can be tuned via the lateral size and aspect ratio. The coupling to acoustic and optical phonons can be altered via the lateral size and aspect ratio of the platelets. Subsequently the exciton diffusion and mobility become tunable since these phonon scattering processes determine and limit the mobility. At 4 K the exciton mobility increases from ∼ 4 × 103 cm2 V-1 s-1 to more than 1.4 × 104 cm2 V-1 s-1 for large platelets, while there are weaker changes with size and the mobility is around 8 × 101 cm2 V-1 s-1 for large platelets at room temperature. In turn at 4 K the exciton diffusion coefficient increases with the lateral size from ∼ 1.3 cm2 s-1 to ∼ 5 cm2 s-1, while it is around half the value for large platelets at room temperature. Our experimental results are in good agreement with theoretical modeling, showing a lateral size and aspect ratio dependence. The findings open up the possibility for materials with tunable exciton mobility, diffusion or emission line width, but quasi constant transition energy. High exciton mobility is desirable e.g. for solar cells and allows efficient excitation harvesting and extraction.

Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties.

We present a theoretical study combined with experimental validations demonstrating that CdSe nanoplatelets are a model system to investigate the tunability of trions and excitons in laterally finite 2D semiconductors. Our results show that the trion binding energy can be tuned from 36 meV to 18 meV with the lateral size and decreasing aspect ratio, while the oscillator strength ratio of trions to excitons decreases. In contrast to conventional quantum dots, the trion oscillator strength in a nanoplatelet at low temperature is smaller than that of the exciton. The trion and exciton Bohr radii become lateral size tunable, e.g. from ∼3.5 to 4.8 nm for the trion. We show that dielectric screening has strong impact on these properties. By theoretical modeling of transition energies, binding energies and oscillator strength of trions and excitons and comparison with experimental findings, we demonstrate that these properties are lateral size and aspect ratio tunable and can be engineered by dielectric confinement, allowing to suppress e.g. detrimental trion emission in devices. Our results strongly impact further in-depth studies, as the demonstrated lateral size tunable trion and exciton manifold is expected to influence properties like gain mechanisms, lasing, quantum efficiency and transport even at room temperature due to the high and tunable trion binding energies.

Dependence of the magnetic interactions in MoS2 monolayer on Mn-doping configurations.

Understanding the magnetic properties of the various Mn doping configurations that can be encountered in 2H-MoS2 monolayer could be beneficial for its use in spintronics. Using density functional theory plus Hubbard term (DFT + U) approach, we study how a single isolated, double- and triple-substitution configurations of Mn atoms within a MoS2 monolayer could contribute to its total magnetization. We find that the doping-configuration plays a critical role in stabilizing a ferromagnetic state in a Mn-doped MoS2 monolayer. Indeed, the Mn-Mn magnetic interaction is found to be ferromagnetic and strong for Mn in equidistant substitution positions where the separation average range of 6-11 [Formula: see text]. The strongest ferromagnetic interaction is found when substitutions are in second nearest neighbor Mo-sites of the armchair chain. Clustering is energetically favorable but it strongly reduces the ferromagnetic exchange energies. Furthermore, in term of electronic properties, we show that the Mn-doped MoS2 monolayer can change its electronic behavior from semiconductor to half-metallic depending on the doping configuration. Our results suggest that ordering the Mn dopants on MoS2 monolayer is needed to increase its potential ferromagnetism.

Indium selenide monolayer: strain-enhanced optoelectronic response and dielectric environment-tunable 2D exciton features.

Electronic and optical performances of the ß-InSe monolayer (ML) are considerably boosted by tuning the corresponding band energies through lattice in-plane compressive strain engineering. First principles calculations show an indirect-direct gap transition with a large bandgap size. The crossover is due to different responses of the near-gap state energies with respect to strain. This is explained by the variation of In-Se bond length, the bond nature of near-band-edge electronic orbital and of the momentum angular contribution versus in-plane compressive strain. The effective masses of charge carriers are also found to be highly modulated and significantly light at the indirect-direct-gap transition. The tuned optical response of the resulting direct-gap ML ß-InSe is evaluated versus applied energy to infer the allowed optical transitions, dielectric constants, semiconductor-metal behavior and refractive index. The environmental dielectric engineering of exciton behavior of the resulting direct-gap ML ß-InSe is handled within the effective mass Wannier-Mott model and is expected to be important. Our results highlight the increase of binding energy and red-shifted exciton energy with decreasing screening substrates, resulting in a stable exciton at room temperature. The intensity and energy of the ground-state exciton emission are expected to be strongly influenced under substrate screening effect. According to our findings, the direct-gap ML ß-InSe assures tremendous 2D optoelectronic and nanoelectronic merits that could overcome several limitations of unstrained ML ß-InSe.

Polariton condensation threshold investigation through the numerical resolution of the generalized Gross-Pitaevskii equation.

We present a numerical approach for the solution of the dissipative Gross-Pitaevskii equation coupled to the reservoir equation governing the exciton-polaritons Bose-Einstein condensation. It is based on the finite difference method applied to space variables and on the fourth order Range-Kutta algorithm applied to the time variable. Numerical tests illustrate the stability and accuracy of the proposed scheme. Then results on the behavior of the condensate under large Gaussian pumping and around the threshold are presented. We determine the threshold through the particular behavior of the self-energy and characterize it by tracking the establishment time of the steady state.

Strain- and surface-induced modification of photoluminescence from self-assembled GaN/Al0.5Ga0.5N quantum dots: strong effect of capping layer and atmospheric condition.

We report on the influence of a capping layer on the photoluminescence properties of self-assembled GaN quantum dots grown on an Al(0.5)Ga(0.5)N template. Self-assembled GaN quantum dots show a large quantum confined Stark shift and long carrier recombination time due to strong built-in spontaneous and piezoelectric polarization fields. Nevertheless, owing to strong carrier localization and suppressed nonradiative processes, these quantum dots have a high-quantum efficiency even at room temperature. Here, we show that the capping thickness has an important role on the optical properties of the GaN quantum dots. The radiative and nonradiative recombination processes of quantum dots are strongly affected by adjusting the capping thickness, and the GaN quantum dots with 12 monolayers-thick Al(0.5)Ga(0.5)N capping layer show a remarkably high internal quantum efficiency of more than 80% at room temperature. We also studied photoluminescence quenching and enhancement for surface (uncapped) quantum dots caused by photoadsorption and photodesorption of oxygen.