Direct Exciton Research Articles

Control resonant excitation of surface plasmon polariton in quantum-dot molecule system via tunneling induced transparency and Autler–Townes splitting

Electromagnetic induced transparency (EIT) and Autler–Townes splitting (ATS) both produce a transparency window in an absorption profile, yet EIT is distinct in that it can create a transparency window for a weak control field. To elucidate the distinct physical mechanisms underlying EIT and ATS effects, we explore the controlled resonant excitation of surface plasmon polaritons (SPPs) within these regimes. Our setup is composed of three layers: a top vacuum or air layer, a central metal film, and a bottom layer of dielectric medium based on the quantum-dot molecules (QDMs) system. Unlike typical systems, that employ prism or grating coupling scheme, our setup takes advantage of the unique features of the QDMs medium to investigate the direct resonance excitation of SPPs. A weak probe and a strong control field are carried through air or vacuum to the top layer. Our results demonstrate that the permittivity of the bottom medium displays tunneling induced transparency (TIT) if the tunneling strength (Te) and the decay rate of the direct exciton (Γ1) follow the condition Te/Γ1⩽0.5; otherwise, it represents the ATS effect. In both instances, the permittivity of the QDMs medium satisfy the low-loss (high transmission) criteria, i.e., Re [ɛd]<1 and Im [ɛd]≪1, providing a framework for exploring the control resonant excitation of SPPs. We simulate the reflection and transmission spectra using the Fresnel’s formula and noticed sharp dips in reflection and peaks in the transmission spectra, which are the signature of coupler free resonance excitation of SPPs. We noticed that the narrow peak in TIT allows for strong light transmission and thus a high peak in SPP resonance excitation, resulting in higher sensitivity in plasmonic sensors. Conversely, the large spacing between the two peaks in the ATS effect broadens the range of effective excitation frequencies for SPPs, increasing the system’s adaptability and efficiency in applications requiring broad spectrum responses.

Abnormal Response of Indirect Excitons to Non‐Uniform Elastic Strain in MoS2 Flakes

AbstractRegulating the electronic structures and carrier dynamics in 2D materials via elastic strain is a fascinating avenue for tailoring their optoelectronic properties at atomic scale. Here, the abnormal response of indirect excitons to non‐uniform elastic strain in MoS2 flakes is reported. The non‐uniform elastic strain in the MoS2 flakes is introduced by transferring them to pre‐prepared convex cross structures on a SiO2/Si substrate, where the topography and strain distribution are determined by atomic force microscopy and Raman spectroscopy, respectively. It is observed that the emission energy of the indirect excitons shows an unexpected blue‐shift followed by a red‐shift with increasing the local tensile strain, which is in sharp contrast to the linear red‐shift of the direct excitons. Density functional theory calculations reveal that the abnormal energy shift of the indirect excitons in the MoS2 flakes arises from the strain‐induced competition between two indirect bandgap transitions and the spatial exciton funnel effect in the non‐uniform strain field. This work provides new insights into the elastic strain effect on the indirect excitons in 2D semiconductors, which possesses potential applications in flexible optoelectronic devices.

Excitonic Bose Polarons in Electron-Hole Bilayers.

Bose polarons are mobile particles of one kind dressed by excitations of the surrounding degenerate Bose gas of particles of another kind. These many-body objects have been realized in ultracold atomic gases and become a subject of intensive studies. In this work, we show that excitons in electron-hole bilayers offer new opportunities for exploring polarons in strongly interacting, highly tunable bosonic systems. We found that Bose polarons are formed by spatially direct excitons immersed in degenerate Bose gases of spatially indirect excitons (IXs). We detected both attractive and repulsive Bose polarons by measuring photoluminescence excitation spectra. We controlled the density of IX Bose gas by optical excitation and observed an enhancement of the energy splitting between attractive and repulsive Bose polarons with increasing IX density, in agreement with our theoretical calculations.

Direct, Indirect, and Self-Trapped Excitons in Cs2AgBiBr6.

Cs2AgBiBr6 exhibits promising photovoltaic and light-emitting properties, making it a candidate for next-generation solar cells and LED technologies. Additionally, it serves as a model system within the family of halide double perovskites, offering insights into a broader class of materials. Here, we study various possible excited states of this material to understand its absorption and emission properties. We use time-dependent density functional theory (TD-DFT) coupled with nonempirical hybrid functionals, specifically PBE0(α) and dielectric-dependent hybrids (DDH) to explore direct, indirect, and self-trapped excitons in this material. Based on comparison with experiment, we show that these methods can give excellent predictions of the absorption spectrum and that the fundamental band gap has been underestimated in previous computational studies. We connect the experimental photoluminescence signals at 1.9-2.0 eV to the emission from self-trapped excitons and electron polarons. Finally, we reveal a complex landscape with energetically competing direct, indirect, and self-trapped excitons in the material.

Twist-angle-dependent optical behaviors of excitons in twisted bilayer MoS2 at low temperature

Twisted bilayers of two-dimensional materials provide a powerful and attractive platform to control band structure and tailor optical properties since the twist angle θ between the bilayer has been shown to be a critical parameter in engineering the moiré potential. Here, we demonstrate the θ-driven effects on excitons in twisted bilayer MoS2 (tBLMs) by measuring photoluminescence (PL) spectra. The localized state exciton between 1.70 eV and 1.80 eV is observed at 7 K with properties periodically modulated by θ. The θ is also a crucial factor affecting direct excitons. Furthermore, the phonon around 410 cm−1 has a θ dependence similar to excitons by measuring Raman spectra. The localized stacking patterns, the recombination of excitons, and the phonon-exciton interactions are confirmed in tBLMs. Our work provides the help to investigate the new quantum phenomena of tBLMs by optical methods and provides possibilities to manipulate the emission of excitons in tBLMs.

Electrically induced direct to indirect exciton transition in CdTe/CdMnTe concentric double quantum ring rooted in SiO2 matrix

Effect of electric field and ring dimension on the localization of direct and indirect exciton formed inside a CdTe/CdMnTe Concentric Double Quantum Ring (CDQR) has been studied using variational technique. The whole double ring structure is embedded inside a SiO2 matrix to enhance exciton localization. Electric field applied along the axial (z) axis tilts the band structure which promotes the carrier localization more in the edges than in the center of the ring. Thus, the stronger electric field gives a triangular confinement to the carrier in the edges which enhances the carrier stability. Along with the effect of electric field the ring dimension which determines the stability of the exciton retains has been estimated through the mean square distance. The effect of the location of the constituent carriers on the excitonic stability and the efficient carrier transfer from inner ring to outer ring has been calculated for both symmetric and asymmetric ring dimensions. Height of the ring has been varied to understand its effect on the localization of both direct and indirect exciton.

Composition and Surface Optical Properties of GaSe:Eu Crystals before and after Heat Treatment.

This work studies the technological preparation conditions, morphology, structural characteristics and elemental composition, and optical and photoluminescent properties of GaSe single crystals and Eu-doped β-Ga2O3 nanoformations on ε-GaSe:Eu single crystal substrate, obtained by heat treatment at 750-900 °C, with a duration from 30 min to 12 h, in water vapor-enriched atmosphere, of GaSe plates doped with 0.02-3.00 at. % Eu. The defects on the (0001) surface of GaSe:Eu plates serve as nucleation centers of β-Ga2O3:Eu crystallites. For 0.02 at. % Eu doping, the fundamental absorption edge of GaSe:Eu crystals at room temperature is formed by n = 1 direct excitons, while at 3.00 at. % doping, Eu completely shields the electron-hole bonds. The band gap of nanostructured β-Ga2O3:Eu layer, determined from diffuse reflectance spectra, depends on the dopant concentration and ranges from 4.64 eV to 4.87 eV, for 3.00 and 0.05 at. % doping, respectively. At 0.02 at. % doping level, the PL spectrum of ε-GaSe:Eu single crystals consists of the n = 1 exciton band, together with the impurity band with a maximum intensity at 800 nm. Fabry-Perrot cavities with a width of 9.3 μm are formed in these single crystals, which determine the interference structure of the impurity PL band. At 1.00-3.00 at. % Eu concentrations, the PL spectra of GaSe:Eu single crystals and β-Ga2O3:Eu nanowire/nanolamellae layers are determined by electronic transitions of Eu2+ and Eu3+ ions.

Cathodoluminescence spectroscopy of monolayer hexagonal boron nitride

Cathodoluminescence (CL) spectroscopy is a suitable technique for studying the luminescent properties of optoelectronic materials because CL has no limitation on the excitable bandgap energy and eliminates ambiguous signals due to simple light scattering and resonant Raman scattering potentially involved in the photoluminescence spectra. However, direct CL measurements of atomically thin two-dimensional materials have been difficult due to the small excitation volume that interacts with high-energy electron beams. Herein, distinct CL signals from a monolayer hexagonal BN (hBN), namely mBN, epitaxial film grown on a graphite substrate are shown by using a CL system capable of large-area and surface-sensitive excitation. Spatially resolved CL spectra at 13 K exhibited a predominant 5.5-eV emission band, which has been ascribed to originate from multilayered aggregates of hBN, markedly at thicker areas formed on the step edges of the substrate. Conversely, a faint peak at 6.04 ± 0.01 eV was routinely observed from atomically flat areas, which is assigned as being due to the recombination of phonon-assisted direct excitons of mBN. The CL results support the transition from indirect bandgap in bulk hBN to direct bandgap in mBN. The results also encourage one to elucidate emission properties of other low-dimensional materials by using the present CL configuration.

Anthracene derivatives with strong spin-orbit coupling and efficient high-lying reverse intersystem crossing beyond the El-Sayed rule.

The attention to materials with hot exciton channel and triplet-triplet fusion (TTF) mediated high-lying reverse intersystem crossing (hRISC) has been raised for their ability to convert non-emissive 'dark' triplets into radiative singlet excitons. This spin conversion process results in high exciton utilization efficiency (EUE) that exceeds the theoretical limits. Notably, it is known that such spin conversion processes from the high-lying excited triplet to the singlet state are facilitated by the orthogonal orbital transition effect governed by the El-Sayed's rule. In this study, an anthracene derivative with indenoquinoline substituent 7,7-dimethyl-9-(10-(4-(naphthalen-1-yl)phenyl)anthracen-9-yl)-7H-indeno[1,2-f]quinoline (2MIQ-NPA) was synthesized and analyzed to investigate whether the hRISC process occurs in these molecules, even when the El-Sayed's rule is not followed. The hRISC channels of the emitter were fully unraveled through DFT calculations and experiments, which were quantitatively subdivided using transient electroluminescence measurements. The results showed that 2MIQ-NPA, which does not follow the El-Sayed's rule and has a relatively strong spin-orbit coupling matrix element of 0.116 cm-1 between the high-lying triplet state of T4 and the lowest singlet state of S1, effectively converted triplet excitons into singlet excitons with an EUE of 64.3%, contributed by a direct hot exciton channel of 19.2% and a TTF-mediated hot exciton channel of 15.1%. Despite the low outcoupling efficiency, the non-doped device with 2MIQ-NPA achieved an excellent device performance with an external quantum efficiency of 7.0%.

Promising TMDC-like optical and excitonic properties of the TiBr2 2H monolayer.

The presented simulation protocol provides a solid foundation for exploring two-dimensional materials. Taking the TiBr2 2H monolayer as an example, this material displays promising TMDC-like optical and excitonic properties, making it an excellent candidate for optoelectronic and valleytronic applications. The direct band gap semiconductor (1.19 eV) is both structurally and thermodynamically stable, with spin-orbit coupling effects revealing a broken mirror symmetry in the K and K' valleys of the band structure, as confirmed by opposite values of the Berry curvature. A direct and bright exciton ground state was found, with an exciton binding energy of 0.56 eV. The study also revealed an optical helicity selection rule, suggesting selectivity in the valley excitation by specific circular light polarizations.

Exciton properties for MoS2 grown with the horizontal and vertical orientation

The exciton properties play a crucial role in controlling the optical properties of molybdenum disulfide (MoS2). In this work, horizontally oriented MoS2 (H-MoS2), horizontally and vertically oriented MoS2 (HV-MoS2), and vertically oriented MoS2 (V-MoS2) on the same SiO2/Si substrate have been synthesized and investigated using temperature-dependent photoluminescence spectroscopy from 7 to 300 K. Except for direct excitons called as A and B peaks, indirect exciton named as I peak is discovered with the splitting of three peaks. Compared with direct excitons, indirect excitons appear to be more susceptible to the orientation of MoS2. The exciton activation energies are larger, and the exciton–phonon coupling is stronger in V-MoS2 than in H-MoS2. The exciton properties of HV-MoS2 are more similar to those of V-MoS2, but there are some unusual phenomena. Our work provides a reference for optoelectronic applications based on transition-metal dichalcogenides represented by MoS2 grown with horizontal and vertical orientations.

The influence of screening function on exciton mott transition in an asymmetric double quantum well

The semiconductor-to-metal transition (SMT) due to excitons exciton mott transition (EMT) in GaAs/Al[Formula: see text]Ga[Formula: see text]As asymmetric double quantum well (ADQW) has been studied theoretically by tuning direct (DX) and indirect (IDX) exciton densities using variation technique combined with the Monte Carlo approximation. The interaction of the optically pumped exciton densities is accounted for through the Thomas–Fermi (TF) dielectric screening and compared with Hartree–Fock (HF) screening. The screening effects of IDX at the barrier regime have been accounted for through size-dependent screening. The important characteristics of EMT, such as (i). binding energy and (ii), diamagnetic susceptibility have been studied in both coupled ([Formula: see text]Å) and isolated ([Formula: see text]Å) regimes of ADQW. The effect of asymmetry on the EMT of DX (IDX) is significant only for [Formula: see text] in the case of the coupled regime of ADQW, which may be due to the dynamic tunneling mechanism. The impact of the screening among the exciton densities to bring out the avalanche breakdown of excitons at the critical concentration has been studied for different kinds of excitons.

Optical bistability and multistability with coupled quantum wells in the presence of second- and third-order nonlinearities

In this work, we explore the intriguing phenomena of bistability and multistability in a cavity comprising two coupled quantum wells via electron tunneling. The cavity is driven by squeezed light produced by an optical parametric oscillator. Our results show that the frequency detunings relative to direct and indirect excitons are crucial for the occurrence of bistability, which is governed by the Kerr effects. Furthermore, we reveal that multistable behavior in the excitonic and photonic intensities can be attributed to the interaction between second- and third-order nonlinearities. We also investigate the controllability of the transition between bistability and multistability. The switch between bistability and multistability is controlled by adjusting the squeezed light’s amplitude or the cavity’s frequency detuning between the external coherent drive and the cavity. The tunneling has a contrasting double impact for the emergence or destruction of bistability and multistability, depending on the consideration of direct and indirect exciton nonlinearities. As a consequence, the switch between bistability and multistability can be ensured also by adjusting the tunneling rate between the wells, which in turn depends on the distance separating them.

Anomalous luminescence temperature dependence of (In,Ga)(As,Sb)/GaAs/GaP quantum dots overgrown by a thin GaSb capping layer for nanomemory applications

We study (In,Ga)(As,Sb)/GaAs quantum dots (QDs) embedded in a GaP (100) matrix, which are overgrown by a thin GaSb capping layer with variable thickness. QD samples are studied by temperature-dependent photoluminescence, and we observe that the QD emission shows anomalous temperature dependence, i.e. increase of energy with temperature increase from 10 K to ∼70 K, followed by energy decrease for larger temperatures. With the help of fitting of luminescence spectra by Gaussian bands with energies extracted from eight band theory with multiparticle corrections calculated using the configuration interaction method, we explain the anomalous temperature dependence as mixing of momentum direct and indirect exciton states. We also find that the k-indirect electron–hole transition in type-I regime at temperatures K is optically more intense than k-direct. Furthermore, we identify a band alignment change from type-I to type-II for QDs overgrown by more than one monolayer of GaSb. Finally, we predict the retention time of (In,Ga)(As,Sb)/GaAs/AlP/GaP QDs capped with GaSb layers with varying thickness, for usage as storage units in the QD-Flash nanomemory concept and observe that by using only a 2 ML-thick GaSb capping layer, the projected storage time surpasses the non-volatility limit of ten years.

Phosphorescent Dye Sensitized Quantum-Dot Light-Emitting Diodes with 37% External Quantum Efficiency.

Exciton harvesting is of paramount importance for quantum-dot light-emitting diodes (QLEDs). Direct exciton harvesting by quantum dots (QDs) emitting layer suffers from poor hole injection due to the low conduction bands and valence bands of QDs, leading to unbalanced electron-hole injection and recombination. To address this issue, here we report an exciton sensitizing approach, where excitons form on a phosphorescent dye doped layer which then transfer their energies to adjacent QDs layer for photon emission. Due to the very efficient exciton formation and energy transfer processes, higher device performance could be achieved. To demonstrate the above strategy, red QLEDs with a phosphorescent dye Iridium (III) bis (2 - methyldibenzo - [f, h] quinoxaline) (acetylacetonate), Ir(MDQ)2 (acac) doped hole transporting layer were fabricated and studied. At a doping concentration of 10wt.%, the best device achieves record high current efficiency, power efficiency and external quantum efficiency of 37.3cd A-1 , 41.0lm W-1 and 37.0%, respectively. Simultaneously, the efficiency roll-off characteristic was greatly improved that 35.0% EQE can be well remained at high luminance level of 450 000cd m-2 . Moreover, the devices also exhibit good stability and reproducibility. This article is protected by copyright. All rights reserved.

Coherent driving of direct and indirect excitons in a quantum dot molecule

Quantum dot molecules (QDMs) are one of the few quantum light sources that promise deterministic generation of one- and two-dimensional photonic graph states. The proposed protocols rely on coherent excitation of the tunnel-coupled and spatially indirect exciton states. Here, we demonstrate power-dependent Rabi oscillations of direct excitons, spatially indirect excitons, and excitons with a hybridized electron wave function. An off-resonant detection technique based on phonon-mediated state transfer allows for spectrally filtered detection under resonant excitation. Applying a gate voltage to the QDM-device enables a continuous transition between direct and indirect excitons and, thereby, control of the overlap of the electron and hole wave function. This does not only vary the Rabi frequency of the investigated transition by a factor of $\approx3$, but also allows to optimize graph state generation in terms of optical pulse power and reduction of radiative lifetimes.

Effect of WS2 nanoparticles on the current-voltage characteristics of a polymer solar cell

The paper presents the results of studies of the effect of tungsten disulfide nanoparticles on the optical and electrotransport characteristics of PEDOT: PSS thin films in polymer solar cells. Tungsten disulfide (WS2) nanoparticles were obtained by laser ablation in isopropyl alcohol. The average size of nanoparticles were determined by dynamic light scattering and is ~38 nm. The concentration of WS2 nanoparticles in the solution was calculated based on the density of the WS2 substance. The absorption spectrum of nanoparticles in isopropyl alcohol has been measured. Two bands are observed in 500-900 nm regions, which are associated with direct exciton transitions A1 and B1 in two-dimensional transition metal dichalcogenides with 2H phase. WS2 nanoparticles were added in PEDOT: PSS solution and thin films were deposited from the preparedsolution by spin-coating. PEDOT: PSS thin films doped with WS2 were studied by atomic force microscopy (AFM). The arithmetic mean deviation of the surface roughness (Ra) was estimated. Doping with WS2 nanoparticles leads to the increase in Ra of PEDOT: PSS thin films. The optical absorption spectra of doped films have been measured. Also, doping PEDOT: PSS with WS2 nanoparticles results in a long-wavelength shift of the PEDOT absorption maximum. The optimal concentration of WS2 nanoparticles for the preparation of doped PEDOT: PSS thin films is determined, at which the film resistance decreases by almost 2 times, the recombination resistance of charge carriers increases by 4.7 times, and the efficiency of the polymer solar cell increases to 1.94 %.

Free exciton and bound excitons on Pb and I vacancies and O and I substituting defects in PbI2: Photoluminescence and DFT calculations

A complete study of structure, chemical composition, morphology and photoluminescence (PL) is performed for multilayer PbI2 flakes. The reduction of thickness results in uneven spatial mapping of PL and Raman intensities, while the positions and shapes of the spectra do not undergo notable changes. The most intense peaks in the PL spectra are the direct free exciton (FX) peak at 2.44 eV (508 nm) and the bound exciton (BX) at 2.41 eV (516 nm). The variation of above/below-bandgap excitation has allowed to find three more defect-related peaks at 2.35, 2.19 and 2.04 eV. So far, these three BXs have not been studied. Our DFT calculations combined with the experimental results allow to clarify the origins of BX peaks as the recombination from the optical conduction band edge to the defect levels located above the valence band: 2.41 eV to O substituting I (OI), 2.35 eV to Pb vacancy (VPb), and 2.19/2.04 eV to IPb with split level. We have defined that the known absorption at 1.55 eV (800 nm) is related to VI nonradiative recombination center. The temperature behaviors allow to determine the thermal dissociation energy of FX of 0.22 eV. The dependences also show a co-interaction between defect levels.

Signatures of Electric Field and Layer Separation Effects on the Spin-Valley Physics of MoSe2/WSe2 Heterobilayers: From Energy Bands to Dipolar Excitons.

Multilayered van der Waals heterostructures based on transition metal dichalcogenides are suitable platforms on which to study interlayer (dipolar) excitons, in which electrons and holes are localized in different layers. Interestingly, these excitonic complexes exhibit pronounced valley Zeeman signatures, but how their spin-valley physics can be further altered due to external parameters-such as electric field and interlayer separation-remains largely unexplored. Here, we perform a systematic analysis of the spin-valley physics in MoSe2/WSe2 heterobilayers under the influence of an external electric field and changes of the interlayer separation. In particular, we analyze the spin (Sz) and orbital (Lz) degrees of freedom, and the symmetry properties of the relevant band edges (at K, Q, and Γ points) of high-symmetry stackings at 0° (R-type) and 60° (H-type) angles-the important building blocks present in moiré or atomically reconstructed structures. We reveal distinct hybridization signatures on the spin and the orbital degrees of freedom of low-energy bands, due to the wave function mixing between the layers, which are stacking-dependent, and can be further modified by electric field and interlayer distance variation. We find that H-type stackings favor large changes in the g-factors as a function of the electric field, e.g., from -5 to 3 in the valence bands of the Hhh stacking, because of the opposite orientation of Sz and Lz of the individual monolayers. For the low-energy dipolar excitons (direct and indirect in k-space), we quantify the electric dipole moments and polarizabilities, reflecting the layer delocalization of the constituent bands. Furthermore, our results show that direct dipolar excitons carry a robust valley Zeeman effect nearly independent of the electric field, but tunable by the interlayer distance, which can be rendered experimentally accessible via applied external pressure. For the momentum-indirect dipolar excitons, our symmetry analysis indicates that phonon-mediated optical processes can easily take place. In particular, for the indirect excitons with conduction bands at the Q point for H-type stackings, we find marked variations of the valley Zeeman (∼4) as a function of the electric field, which notably stands out from the other dipolar exciton species. Our analysis suggests that stronger signatures of the coupled spin-valley physics are favored in H-type stackings, which can be experimentally investigated in samples with twist angle close to 60°. In summary, our study provides fundamental microscopic insights into the spin-valley physics of van der Waals heterostructures, which are relevant to understanding the valley Zeeman splitting of dipolar excitonic complexes, and also intralayer excitons.

Indirect Exciton–Phonon Dynamics in MoS2 Revealed by Ultrafast Electron Diffraction

AbstractTransition metal dichalcogenides layered nano‐crystals are emerging as promising candidates for next‐generation optoelectronic and quantum devices. In such systems, the interaction between excitonic states and atomic vibrations is crucial for many fundamental properties, such as carrier mobilities, quantum coherence loss, and heat dissipation. In particular, to fully exploit their valley‐selective excitations, one has to understand the many‐body exciton physics of zone‐edge states. So far, theoretical and experimental studies have mainly focused on the exciton–phonon dynamics in high‐energy direct excitons involving zone‐center phonons. Here, ultrafast electron diffraction and ab initio calculations are used to investigate the many‐body structural dynamics following nearly‐ resonant excitation of low‐energy indirect excitons in MoS2. By exploiting the large momentum carried by scattered electrons, the excitation of in‐plane K‐ and Q‐ phonon modes are identified with 𝑬′ symmetry as key for the stabilization of indirect excitons generated via near‐infrared light at 1.55 eV, and light is shed on the role of phonon anharmonicity and the ensuing structural evolution of the MoS2 crystal lattice. The results highlight the strong selectivity of phononic excitations directly associated with the specific indirect‐ exciton nature of the wavelength‐dependent electronic transitions triggered in the system.