Search

Two-dimensional molybdenum disulfide (MoS2) has been proved to be a good candidate in photodetectors, and MoS2/graphene (MoS2/G) heterostructure has been widely used to expand the optical response wavelength of MoS2. To clarify the carrier transfer dynamics in the MoS2/G heterostructure, time-resolved transient absorption and two-color pump–probe measurements are performed. By comparing the carrier dynamics in MoS2 and MoS2/G under different pump wavelengths, we find that interfacial excitons are formed in the heterostructure, and fast hot carriers transfer (<200 fs) from graphene to MoS2 are observed. The results indicate that the formed heterostructure with graphene can not only expand the optical response wavelength of MoS2 but also improve the response time of the device in the near-infrared region. [ABSTRACT FROM AUTHOR]

Understanding and modulating the spin-pair correlation of conjugated polymer materials in π-conjugated polymer light-emitting devices (PLEDs) plays a crucial role in the development of their applications. We investigated the relationships between the internal hyperfine interactions (HFIs), triplet–triplet annihilation (TTA), and triplet–charge annihilation (TCA) spin evolution processes in π-conjugated PLED. Research has shown that in a unipolar π-conjugated PLED, the "M" shaped ultra-small magnetic field effect is due to the HFI between hole polarons and the spin-mixing process of charge carriers. Under high magnetic fields (15 mT<|B|<350 mT), the TCA process dominates the negative magneto-conductance (MC), and its intensity and sign are not controlled by temperature. In polar π-conjugated PLED, excess carriers can provide conditions for the generation of TCA. Moreover, π-conjugated polymers (emission layers) have relatively strong electron–phonon coupling, which can capture triplet excitons into adjacent organic layers to obtain higher triplet exciton concentrations, resulting in the TTA process. Under low-temperature conditions, excess carriers induce the magneto-electroluminescence (MEL) effect to undergo TTA and form P-type delayed fluorescence. This study can provide a new mechanism explanation for the HFI in PLED devices and a new approach for the effective utilization of triplets. [ABSTRACT FROM AUTHOR]

The luminescence efficiency of AlxGa1−xN quantum dots (QDs) and quantum wells (QWs), buried in AlN cladding layers and emitting in the ultraviolet range between 234 and 310 nm, has been investigated. The growth and optical properties have been done using similar aluminum composition (varying from 0.4 to 0.75) for both QDs and QWs. In order to compare as much as possible the optical properties, the QWs were fabricated with a growth time tuned such that the QW width is similar to the average height of the QDs. The photoluminescence (PL) showed emission ranging from 4 to 5.4 eV, putting into evidence differences in terms of full width at half maximum, PL intensity, and asymmetry of the line shape between QDs and QWs. The results show shorter wavelengths and a slightly narrower PL linewidth for QWs. To determine the light emission dependence with the electric field direction in the crystal, the evolutions of the emission diagrams for all samples were recorded along two orthogonal directions, namely, the "in-plane" (growth) and the "on-side" directions, from which the light emission was collected. For the whole QDs and QWs samples' series, the shapes of the emission diagram indicate emission in both in-plane and on-side directions, as evidenced by intra-valence band mixings caused by strain effects combined with the anisotropic Coulomb interactions that are particularly contributing to the polarization at wavelengths below 260 nm. Furthermore, the degree of polarization, determined for each sample, showed good agreement with results from the literature. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) perovskites have gained much attention lately owing to their excellent optoelectronic properties, chemical tunability, and environmental stability. Multiple methods have been devised to synthesize high quality 2D perovskite single crystals, and recent progress in fabricating its heterostructures is notable as well. In particular, with growing interest in 2D van der Waals heterostructures, 2D perovskites have become a strong candidate as a new building block for heterostructures to reveal unique physical properties across different interfaces. Until now, various heterostructure devices of 2D perovskite single crystals with other types of 2D materials such as transition metal dichalcogenides (TMDs) and graphene have been studied, which have shown intriguing results including interlayer excitons and enhanced electronic properties. Here, we introduce various synthetic approaches to realize 2D perovskite single crystals and unique characteristics of their single crystal heterostructures fabricated with precision, possessing sharp interfaces. Moreover, recent studies of semiconductor devices based on 2D perovskite single crystal heterostructures are discussed in-depth. New perspectives to further the horizon in the field of 2D perovskite heterostructures are suggested in this work including the consideration of metal–2D material van der Waals contact, application of dry transfer techniques, electric bias driven ion diffusion studies, and nanocrystal array fabrication. 2D perovskite heterostructure single crystal devices factoring in these novel perspectives will further uncover the true potential of these materials for highly efficient and stable semiconductor devices. [ABSTRACT FROM AUTHOR]

Interlayer excitons in two-dimensional semiconductor heterostructures show suppressed electron–hole overlap resulting in longer radiative lifetimes as compared to intralayer excitons. Such tightly bound interlayer excitons are relevant for important optoelectronic applications, including light storage and quantum communication. Their optical accessibility is, however, limited due to their out-of-plane transition dipole moment. In this work, we design a complementary metal–oxide–semiconductor-compatible photonic integrated chip platform for enhanced near-field coupling of these interlayer excitons with the whispering gallery modes of a microresonator, exploiting the high confinement of light in a small modal volume and high-quality factor of the system. Our platform allows for highly selective emission routing via engineering an asymmetric light transmission that facilitates efficient readout and channeling of the excitonic valley state from such systems. [ABSTRACT FROM AUTHOR]

The behavior of excitons excited in anatase crystalline materials affects the photocatalytic performance of the materials. Thus, investigating the properties of such excitons is essential for understanding the origin of their influence on photocatalytic performance. Here, angle-resolved electron energy-loss spectroscopy was applied to evaluate the size of the spatial spread of excitons in anatase TiO2. Three kinds of excitons (I–III), which were reported by polarized light absorption experiments, were experimentally identified in the electron energy-loss spectroscopy (EELS) spectra. Exciton size was evaluated from absorption intensity, which was derived by the Kramers–Kronig analysis of the EELS spectra, depending on the momentum transfer (q). The sizes of excitons I, II, and III were evaluated to be 8, 5, and 6 nm, respectively. The larger size of exciton I than that of III was with the same tendency as in the theoretical results. Exciton II, which was evaluated as a delocalized one, was evaluated to have a finite size in this experiment. The largest size of exciton I, approximately 8 nm, is the same order of the exciton diffusion lengths of the material. Therefore, exciton I should significantly influence the photocatalytic activity of anatase. [ABSTRACT FROM AUTHOR]

Moiré lattices formed in twisted and lattice-mismatched van der Waals heterostructures have emerged as a platform to engineer the novel electronic and excitonic states at the nanoscale. This Perspective reviews the materials science of moiré heterostructures with a focus on the structural properties of the interface and its structural–property relationships. We first review the studies of the atomic relaxation and domain structures in moiré superlattices and how these structural studies provide critical insights into understanding the behaviors of quantum-confined electrons and excitons. We discuss the general frameworks to manipulate moiré structures and how such control can be harnessed for engineering new phases of matter and simulating various quantum phenomena. Finally, we discuss routes toward large-scale moiré heterostructures and give an outlook on their applications in quantum electronics and optoelectronics. Special emphasis will be placed on the challenges and opportunities of the reliable fabrication and dynamical manipulation of moiré heterostructures. [ABSTRACT FROM AUTHOR]

We studied the excitation-dependent photoluminescence (PL) quantum yield (QY) of monolayer MoS2 (1L-MoS2) with various flake areas grown on SiO2/Si substrates. The PL measurements were carried out by 532, 488, and 325 nm excitations which fulfill the conditions of quasi-resonant excitation of A-exciton, above bandgap, and far above the bandgap excitations, respectively. The PL QY was found to be reduced by decreasing the excitation wavelength, and it is attributed to variation in the thermal energy dissipated to the lattice. PL emission from 1L-MoS2 was observed with 325 nm excitation in large-area flakes (≥532 μm2) because of efficient heat dissipation. In the literature, PL emission of 1L-MoS2 is hardly reported with 325 nm laser excitations. Under 325 nm laser irradiation, 50% of excitation energy is converted to heat, which substantially increases the local temperature. From the temperature-dependent Raman analysis, the rise in the local temperature is approximated to be ∼382 K in the case of a small-area flake, whereas such an effect is alleviated in large-area flakes. Moreover, inter-valley exciton scattering dominates as the excitation wavelength decreases because of a substantial rise in the phonon population for small-area flakes. As a consequence of inter-valley exciton scattering, dark excitons (K-Σ) dominate over the bright excitons (K-K) under the 325 nm excitation. Hence, total suppression of PL emission was observed for small-area flakes because of dark exciton recombination. The noticeable PL emission of large-area flakes is attributed to the improved bright exciton recombination. [ABSTRACT FROM AUTHOR]

Recent studies of transition metal dichalcogenides (TMDs) have revealed exciting optical properties, such as stable excitons and chiral light–matter interactions. Chemical vapor deposition techniques provide a platform for the fabrication of nanostructures with diverse geometries, ranging from horizontal flakes to flower-like structures. Raman spectroscopy is commonly used to characterize TMDs and their properties. Here, we use polarization-resolved Raman spectroscopy to probe the nanogeometry and orientation of WS 2 nanoflower petals. Exciting the nanoflowers with linearly polarized light, we observe an enhanced Raman response from flower petals oriented along the excitation polarization direction. Furthermore, the helicity-resolved Raman response of vertically oriented wall-like flower petals exhibits clear differences with horizontally oriented flakes. Although the photoluminescence from the nanoflowers is strongly reduced, the Raman response upon excitation in resonance with the WS 2 excitonic transition does reveal the presence of the exciton, which results in a distinct temperature dependence of the Raman response. [ABSTRACT FROM AUTHOR]

Semiconductor nanostructures of various material systems are heavily researched for information processing applications as single-photon sources for communication and as a spin memory for storage. Here, exciton, electron, and hole properties in single InAs/InP asymmetric quantum dots (quantum dashes) emitting in a broad spectral range from 0.8 to above 1 eV are studied experimentally and theoretically. Experiments using magneto-microphotoluminescence allowed us to determine g-factor tensor components and diamagnetic coefficients. The growth-axis exciton g-factor is in a 0.0–2.9 range with a constant hole g-factor of 4.5 and variation governed by electron contribution. The in-plane g-factor is more stable with the size of the nanostructure exhibiting values of around −0.7 and −1.6 for holes and electrons, respectively. The diamagnetic coefficients are 13 and 5 μ eV T 2 in the growth and in-plane directions, respectively. Simulations based on the eight-band k⋅p model qualitatively reproduce the key experimental features, including the vanishing of the inverse fine-structure splitting of bright exciton at around 3 T, making these structures prospective for the generation of entangled photons. [ABSTRACT FROM AUTHOR]

Controlling the polarization of the emitted light at room temperature is critical for the transition metal dichalcogenides monolayer based photonic devices. One way is to integrate the complicated man-made photonic structures with the monolayer where the photoluminescence (PL) couples with linearly polarized radiation. However, the PL polarization of the monolayer is fixed and cannot be tuned in these structures. In this work, through transferring the WS 2 monolayer onto a simple organic β -perylene (Pe) layer, we show the PL of the WS 2 monolayer can be linearly polarized by virtue of the coupling with the anisotropic modes, which are created due to the reflection of photons between the surface of the Pe substrate. More importantly, we demonstrate tunable linearly polarized excitonic emission from the WS 2 monolayer by varying the thickness of the β -Pe substrate. Our work paves the way to engineer the exciton polarization of 2D materials without complicated fabrication structures at room temperature. [ABSTRACT FROM AUTHOR]

Muon spin rotation has long been recognized as one of the few methods for experimentally accessing the electronic state of dilute hydrogen (H) in semiconductors and dielectrics, where muon behaves as a pseudo-H (designated by the elemental symbol Mu). Meanwhile, predictions on the electronic state of H in these materials by density functional theory (DFT) do not always agree with the observed states of Mu. Most notably, Mu frequently occurs in wide-gap oxides simultaneously in a neutral ( Mu 0) and a diamagnetic state ( Mu + or Mu −), which DFT calculations do not explain; they predict that H is stable only in a diamagnetic state with the polarity determined by the equilibrium charge-transition level (E + / − ) vs the Fermi level. To address this issue, we developed a semi-quantitative model that allows a systematic understanding of the electronic states reported for Mu in the majority of oxides. Our model assumes that muons interact with self-induced excitons to produce relaxed-excited states corresponding to donor-like ( Mu D) and/or acceptor-like ( Mu A) states and that these states correspond to the non-equilibrium electronic level (E + / 0 or E 0 / − ) predicted by DFT calculations for H. The known experimental results are then explained by the relative position of E + / 0 and E 0 / − in the host's energy band structure. In addition, the model sheds new light on the polaron-like nature of the electronic states associated with shallow donor Mu complexes. [ABSTRACT FROM AUTHOR]

Metasurfaces enable flat optical elements by leveraging optical resonances in metallic or dielectric nanoparticles to obtain accurate control over the amplitude and phase of the scattered light. While highly efficient, these resonances are static and difficult to tune actively. Exciton resonances in atomically thin 2D semiconductors provide a novel and uniquely strong resonant light–matter interaction, which presents a new opportunity for optical metasurfaces. Their resonant properties are intrinsic to the band structure of the material, do not rely on nanoscale patterns, and are highly tunable using external stimuli. In this tutorial, we present the role that exciton resonances can play for atomically thin optics. We describe the essentials of metasurface physics and provide background on exciton physics and a comprehensive overview of excitonic materials. Excitons demonstrate to provide new degrees of freedom and enhanced light–matter interactions in hybrid metasurfaces through coupling with metallic and dielectric metasurfaces. Using the high sensitivity of excitons to the medium's electron density, the first demonstrations of electrically tunable nanophotonic devices and atomically thin optical elements are also discussed. The future of excitons in metasurfaces looks promising, while the main challenge lies in large-area growth and precise integration of high-quality materials. [ABSTRACT FROM AUTHOR]

As an effective means to endow lead halide perovskite nanocrystals (NCs) with new properties, ion doping has been widely applied. Transition metal Mn-doped CsPbCl3 is of particular interest, as the Mn doping introduces new emission bands, improves photoluminescence quantum yield (PLQY), and even enhances stability. However, it is still insufficient to catch insight of the energy transfer process and luminescence characteristics of these high defect tolerance NCs doped with Mn ion. Here, we systematically studied the energy transfer from exciton to Mn2+ ions in Mn-doped CsPbCl3 NCs by variable temperature steady-state fluorescence spectra and time-resolved spectra. The abnormal attenuation behavior of the exciton and Mn2+ with the change of temperature was observed, from which we predict the existence of shallow traps near the conduction band and these shallow traps will affect the luminescence properties by influencing the energy transfer process. We show a simple physical model invoking only shallow trap states that uniquely describe the temperature-dependent energy transfer between the exciton and the Mn2+ ion. The thermometric performance (30–290 K) was studied in terms of relative thermal sensitivity, in which the calculated relative sensitivity range is ∼0.12%–1% K−1. [ABSTRACT FROM AUTHOR]

From the canonical and rotating-wave transformations, we obtained the effective lower-polariton Hamiltonian depending on the applied magnetic field from the coupling of one of the quantum-well excitons and photons in a semiconductor microcavity. When the pump field is circularly polarized, the nonlinear interaction can induce a strong polariton blockade near the resonant peaks, which can be suppressed by a large pump in weak magnetic field situations. Thus, the platform behavior in the variation of the polariton occupation proves the polariton quantum blockade. On the other hand, when the pump field is linearly polarized, we achieve a single-photon emitter whose polariton polarization can be adjusted by an applied magnetic field. Polaritons with opposite spins, on the other hand, are anti-bunching in the lower excitation regime and become bunching only in weak magnetic field situations and a high excitation regime. Our findings constitute a potential step toward the realization of strongly coupled polaritonic systems. [ABSTRACT FROM AUTHOR]

We develop a theoretical study to evaluate the dynamic of the time-resolved photoemission spectrum arising from the dissociation of exciton steady-states 1s, 2s in a monolayer transition metal dichlacogenides. We discuss the dielectric environment effect on the exciton binding energies. Quantum beat signatures in photoemission intensity demonstrate coherent coupling between 1s and 2s excitons. The beating contribution due to excitonic coherence is also discussed. The periodic oscillations arising from coherent superposition states and quantum beats enable exploration of novel coherent phenomena. [ABSTRACT FROM AUTHOR]

The emission lines of strongly confined (211)B InAs/GaAs quantum dots (QDs), embedded in short-period GaAs/AlAs superlattices, are thoroughly characterized by a range of single-dot spectroscopy techniques, including cross correlation photon-counting measurements. Contrary to what is expected for a piezoelectric QD system, the single-dot biexciton line is found redshifted with respect to the exciton one by as many as 6 meV. This comes in striking contrast to previous reports on the same QD system, without additional confinement, where the biexciton lines always showed up at higher energies than the exciton, by 4–13 meV. In addition, two charged exciton lines are identified for the first time in a piezoelectric InAs-based QD. A positively charged (Χ+) and a negatively charged (Χ−) trion line are observed 1.5 and 7.5 meV below the neutral exciton line, respectively. Our results pave the way to an enhanced understanding of the excitonic transitions in (211)B QDs and highlight the possible role of strong confinement and accompanying correlation effects as a means to tailor the transition energies of multi-particle states in semiconductor QDs. [ABSTRACT FROM AUTHOR]

Atomically thin semiconducting 2D transition metal dichalcogenides have garnered remarkable attention from the scientific community due to their prodigious contributions in the field of next-generation electronic and optoelectronic devices. In this continuation, we report a facile synthesis protocol of monolayer WSe2 films via the atmospheric-pressure chemical vapor deposition (APCVD) technique using hydrothermally synthesized hexagonal-phase tungsten oxide (h-WO3) nanorods. The as synthesized WSe2 crystal is a monolayer of ∼0.9 nm thickness as confirmed by atomic force microscopy. The confocal Raman and photoluminescence (PL) mapping suggests that the grown monolayer WSe2 triangles have lattice defects at edge sites, with a slight red-shift of ∼2 nm in PL, a blue-shift of ∼2 cm−1 in Raman peak and reduction in both the intensities. Confocal time-resolved PL mapping at edges reveals a fast-decay component of ∼582 ps and a slow-decay component of ∼2.18 ns that also signifies the presence of lattice defects, which serves as localized-states for photon-generated charge excitons. Furthermore, we have also investigated its electrical property by devising field-effect transistors (FETs). The fabricated WSe2 based FET shows intrinsic n-type behavior. WSe2 FET offers an electron mobility (μ) of ∼13.2 cm2 V−1 s−1, current ON/OFF ratio of ∼107 with a subthreshold slope (SS) of ∼397 mV/decade, which is relatable to the other reported works on WSe2 based FETs. In addition, the device exhibits very high on-current of order of ∼150 μA/μm. These results indicate that h-WO3 nanorod assisted APCVD synthesized WSe2 has prospective of being a competitor for next-generation optoelectronic, and valley-tronic devices. [ABSTRACT FROM AUTHOR]

Electroabsorption (EA) measurements can be used to identify the type of excitons contributing to the absorption spectra of semiconductors. However, the shape of the EA spectrum may vary depending on the mode of measurement due to the optical interference effects. Analysis without considering these effects may lead to erroneous conclusions. In this work, we present EA measurements and analysis for reflection mode measurements considering optical interference effects. We compared the inferences with transmission mode measurements and discuss the limitations. We identified the nature of excitons associated with each transition in the absorption spectrum of poly[(2,5-bis(2-hexyldecyloxy)-phenylene)-alt-(5,6-difluoro-4,7-di(thiophen-2-yl)benzo[c]-[1,2,5]-thiadiazole)] thin film from EA measurements. The bands at 1.89, 2.05, and 2.27 eV had a mixed nature consisting of charge transfer and Frenkel characteristics. Of these, the band at 2.05 eV showed the strongest charge transfer characteristic. From thickness dependent measurements, we showed that the interference effects increase with the thickness of the semiconductor layer. The nature of excitons, however, could still be deduced qualitatively from reflection mode EA measurements. [ABSTRACT FROM AUTHOR]

We theoretically propose a hybrid nanomechanical resonator (NR) system, where a doubly clamped suspended NR with an embedded quantum dot driven by two-tone fields is coupled to another NR via the Coulomb interaction, and we investigate the absorption spectra of the probe field under different exciton-pump field detuning. In the condition of pump on-resonance, the absorption spectrum gives a method to determine the coupling strength of the two NRs. In the pump off resonance, the absorption spectra exhibit double-Fano resonance, which is determined by the interaction of the two NRs, the frequencies of the two NRs, as well as the pump detuning. Furthermore, the double-Fano resonances are accompanied by the rapid normal phase dispersion, which indicates the slow- and fast-light effect. The results show that the group velocity index is tunable by the interaction of the two NRs, the detuning, and the different resonator frequencies, which can achieve the conversion from fast light to slow light. [ABSTRACT FROM AUTHOR]

Due to the exceptional photophysical properties and great potential applications in solid state lighting, zero-dimensional halide perovskites with broadband emitting have recently attracted much attention. In this work, to reveal the origin of the broadband absorption and emission spectra of 0D (C 4 N 2 H 14 Br) 4 SnBr x I 6 − x (x = 3), the ground state and exciton dynamics properties have been studied by hybrid PBE0 functional and the GW+BSE method. Different self-trapped excitons (STEs) are obtained, and their emission energies by PBE0 are consistent well with experimental data. By considering the vibrational broadening of emission, our calculated full width at half maximum of emission accords well with the experiment. The absorption of free exciton and STEs is also calculated by considering the quasiparticle and excitonic effect. Our results show that these light-induced trapped states can be observed by experiments, as confirmed in other similar systems by the femtosecond transient absorption spectra. [ABSTRACT FROM AUTHOR]

The parameters related to the localized states in green-emitting indium gallium nitride (InGaN) have been evaluated by considering the energy diagrams derived by five different methods: (1) the exponential tail of the low-energy side of photoluminescence (PL) spectra, (2) the photon energy dependence of PL decay time, (3) excitation energy dependence of the PL peak energy, (4) the PL excitation spectrum, and (5) the temperature dependence of PL peak energy. The results indicate that the energy diagram of InGaN is divided into four regions: deep localized states, migration region, transition region, and extended states. It is suggested that wider localized states and a narrower transition region are preferable in order to achieve higher PL efficiency. In addition, the dependence of carrier density on PL properties supports the fact of photo-generated carriers forming localized excitons in green-emitting InGaN, although the carriers do not form localized excitons in orange-emitting InGaN and instead exist as localized electrons and holes. [ABSTRACT FROM AUTHOR]

The optical response of a hybrid structure consisting of a metal nanoparticle in the vicinity of a quantum dot under an external field is studied. The effect of the nanoparticle shape as it evolves from a sphere to a rod is investigated for various structural parameters. Significant changes are observed in the phase diagram of the optical response at the borders between Fano, exciton-induced transparency, suppression, and bistable regions. In the appropriate limits, the configuration exhibits a response where notable variations are particularly observed in suppression and bistable regions. In the presence of the nanorod, the suppression region is found as the beginning of bistability. Our calculations show that the nanorod can generate significant nonlinearities at the site of quantum dot in the bistable region, making the hybrid structure suitable for devices involving optical switching or information transfer. By considering the effect of other structural parameters, for example the configuration state, background dielectric constant, and interparticle distance, one can obtain additional control of the optical response of the system, engineering it to achieve particular objectives. [ABSTRACT FROM AUTHOR]

We study the potential for controlled transfer of population to the biexciton state of a semiconductor quantum dot coupled with a metal nanoparticle, under the influence of an electromagnetic pulse with hyperbolic secant shape, and derive analytical solutions of the density matrix equations for both zero and nonzero biexciton energy shifts. These solutions lead to efficient transfer to the biexciton state for various interparticle distances including relatively small values. In certain cases, when the distance between the two particles is small, the transfer of population is strongly modified because of the influence of surface plasmons to the excitons, and the effect is more pronounced for shorter pulses. The hybrid nanostructure that we study has been proposed for generating efficient polarization-entangled photons, and thus, the successful biexciton state preparation considered here is expected to contribute in this line of research. [ABSTRACT FROM AUTHOR]

Growing green and amber emitting InGaN/GaN quantum wells in the zincblende, rather than the wurtzite, crystal phase has the potential to improve efficiency. However, optimization of the emission efficiency of these heterostructures is still required to compete with more conventional alternatives. Photoluminescence time decays were used to assess how the quantum well width and number of quantum wells affect the recombination rates, and temperature dependent photoluminescence was used to determine the factors affecting recombination efficiency. The radiative recombination lifetime was found to be approximately 600 ps and to increase weakly with well width, consistent with a change in the exciton binding energy. The relative efficiency at room temperature was found to increase by a factor of five when the number of wells was increased from one to five. Furthermore, the efficiency increased by factor 2.2 when the width was increased from 2.5 to 7.5 nm. These results indicate that thermionic emission is the most important process reducing efficiency at temperatures in excess of 100 K. Moreover, the weak dependence of the rate of radiative recombination on well width means that increasing well thickness is an effective way of suppressing thermionic emission and thereby increasing efficiency in zincblende InGaN/GaN quantum wells, in contrast to those grown in the wurtzite phase. [ABSTRACT FROM AUTHOR]

We study the efficient preparation of the exciton state in a hybrid nanostructure composed by a semiconductor quantum dot and a metallic nanoparticle, when starting from the ground state, using pulses derived with the method of shortcuts to adiabaticity. We show with numerical simulations that high levels of exciton population can be obtained for a wide range of interparticle distances and for short pulse durations. This behavior appears also to be robust against small positioning errors of the system. The fidelity of the population inversion degrades for smaller distances and longer pulses, as the nonlinear terms in the equations, expressing the quantum dot–metal nanoparticle interaction, become stronger and affect the evolution for longer times. The present work is expected to help schemes toward the generation of single photons on demand or ultrafast nanoswitches, where the controlled population inversion in semiconductor quantum dots coupled to metal nanoparticles is an important task. [ABSTRACT FROM AUTHOR]

Photoluminescence (PL) spectroscopy is a powerful tool in studying semiconductor properties and identifying point defects. Gallium nitride (GaN) is a remarkable semiconductor material for its use in a new generation of bright white LEDs, blue lasers, and high-power electronics. In this Tutorial, we present details of PL experiments and discuss possible sources of mistakes. A brief analysis of near-band-edge emission includes basic characterization of GaN, essential findings about excitons in this material, and the explanation of less known details. We review modern approaches of quantitative analysis of PL from point defects in GaN. The updated classification of defects in undoped GaN and their latest identifications are presented. Typical mistakes in the interpretation of PL spectra from GaN are discussed, and myths about PL are refuted. [ABSTRACT FROM AUTHOR]

Photoluminescence (PL) spectra of atomically thin 2D lead iodide perovskite films are shown to depend on excited-state density, especially at cryogenic temperatures. At high excited-state densities and low temperatures, free exciton (FE) emission is so suppressed by exciton–exciton annihilation (EEA) that other—normally much weaker—emissions dominate the PL spectrum, such as emission from bound excitons (BEs) or PbI 2 inclusions. In the Ruddlesden–Popper perovskite with phenethylammonium (PEA) ligands (PEA 2 PbI 4 , PEPI), FE emission dominates at all temperatures at the excited-state densities reached with continuous wave excitation. At higher excited state densities reached with femtosecond pulsed excitation, the PL at temperatures under 100 K is dominated by BE emission redshifted from that of FE by 40.3 meV. Weak emission from PbI 2 inclusions 170 meV higher in energy than FE PL is also observable under these conditions. Equilibrium between BE and FE states explains why FE emission first increases with decreasing temperature from 290 until 140 K and then decreases with decreasing temperature as the BEs become stable. A Dion–Jacobson (DJ) material based on 1,4-phenyl-enedimethanammonium (PDMA) supports the reduction of FE emission by EEA at cryogenic temperatures. However, in the PDMA-based DJ material, BE emission is never as pronounced. At low temperatures and high-excited state densities caused by pulsed excitation, a broad emission redshifted by 390 meV from the FE dominates. Based on comparison with temperature-dependent measurements of PbI 2 films, this emission is suggested to arise from PbI 2 inclusions in the material. Possible avenues for improving PL at room temperature are discussed concerning these findings. [ABSTRACT FROM AUTHOR]

We present the numerical tool DECaNT (Diffusion of Excitons in Carbon NanoTubes) that simulates exciton transport in thin films of carbon nanotubes. Through a mesh of nanotubes generated using the Bullet Physics C++ library, excitons move according to an ensemble Monte Carlo algorithm, with the scattering rates that account for tube chirality, orientation, and distance. We calculate the diffusion tensor from the position–position correlation functions and analyze its anisotropy and dependence on the film composition, morphology, and defect density. [ABSTRACT FROM AUTHOR]

Photon upconversion assisted by sensitized triplet–triplet annihilation (sTTA-UC) is a wavelength-shifting technique where high-energy photons are emitted from the radiative recombination of high-energy singlets populated through the annihilation of the metastable triplets of two annihilator/emitter molecules. The emitter triplets are previously populated via energy transfer from a light-harvester/sensitizer moiety that absorbs the incident low-energy photons. In solutions, this process is efficient even at low excitation powers, whereas the limited molecular mobility and short exciton lifetimes typically observed in solid matrices hinder the bi-molecular interactions making the sTTA-UC process rather ineffective. We show here that controlling the confinement of the upconverting dye pairs in nanostructured or nanosized materials results in an increased effective local density of the excitation energy. This also activates a specific sTTA-UC kinetics independent of the triplet excitons' mobility that improves the material performance at low powers. We provide a complete modeling of the sTTA-UC process in confined systems. The results obtained afford useful guidelines for the future development of upconverting photonic devices operating at subsolar irradiances suitable for technological implementation. [ABSTRACT FROM AUTHOR]

The carrier density dependence of photoluminescence (PL) spectra, PL efficiency, and time-resolved PL (TRPL) in InGaN/GaN nanocolumns with orange emission has been measured over a wide range of carrier densities to investigate the carrier recombination dynamics at low and room temperatures. The TRPL decay curves were analyzed by stretched exponential functions to obtain a distribution of the decay times. The results indicate that the emission origin in InGaN with orange emission under low excitation intensity is the recombination of localized electrons and holes, not from localized excitons. Our analysis shows that the total density of localized states is an important factor to increase PL efficiency, which implies that red-emitting InGaN with a high density of localized states due to large indium fluctuation has the potential to achieve high PL efficiency. In addition, we have shown that the stretched exponential function is an effective approach to analyze several carrier relaxation processes with different decay times. [ABSTRACT FROM AUTHOR]

We studied the optical properties of a composition graded WS 2 (1 − x) Se 2 x alloy monolayer. A symmetric gradual composition gradient from a Se-rich center to the relatively less Se-rich edges of an equilateral triangle shaped flake is confirmed by Raman mapping. Photoluminescence (PL) mapping shows a large 100 meV variation in the exciton energy, resulting from the composition dependent bandgap variation and carrier localization. The alloying leads to symmetry breaking and large nonlinear optical susceptibility. Second harmonic generation (SHG) mapping was carried out to study the non-linear properties and additionally to determine the lattice strain of the alloy flake. In contrast to PL and Raman mappings, SHG intensity is found to be spatially uniform. However, polarization dependent SHG reveals a unidirectional strain parallel to the (zigzag) edge of the flake, in addition to the sixfold symmetry expected from the transition metal dichalcogenide (TMD) lattice. Our results suggest potential applications of composition graded TMD alloys as ultra-compact color-tunable light sources and miniaturized spectrometers. [ABSTRACT FROM AUTHOR]

The correlation between the recombination dynamics of excitons and the internal quantum efficiency (IQE) of AlGaN-based UV-A multiple quantum wells (MQWs) was studied via photoluminescence (PL) and time-resolved PL (TRPL) spectroscopy. The probability ratio of the capture of excitons by nonradiative recombination centers (NRCs) and the radiative recombination of excitons was evaluated individually via two different experimental analyses. The IQE was evaluated via temperature- and excitation power density-dependent PL measurements and its dependence on excitation density was analyzed using a rate equation model based on the radiative and nonradiative recombination of excitons. Moreover, the radiative and nonradiative recombination lifetimes were evaluated via temperature-dependent TRPL measurements; furthermore, they were analyzed as functions of temperature and excitation energy density. The probability ratios obtained from the two individual analyses were in agreement. This quantitative agreement indicated that the analysis based on the radiative and nonradiative recombination processes of excitons, which included the process of filling NRCs, was valid for AlGaN-based UV-A MQWs. [ABSTRACT FROM AUTHOR]

The substrate effect is an important issue in the properties of two-dimensional transition metal dichalcogenides (2D TMDs). Quantitatively determining the dependence of the photoluminescence (PL) emission properties and the excitonic behavior of single-layer 2D materials in a specific dielectric environment would provide helpful guidance for the rational design of substrates for high performance 2D TMD PL emission devices. Here, using a WSe2 monolayer on different substrates as a model system, it is demonstrated that the PL emission intensities can drastically change depending on the substrate effect. From the analysis of the excitonic behavior, the results reveal that the spectral weight between the neutral and charged excitons in the PL spectra is significantly modified by the substrate types, and the weight factor is dependent on the laser excitation density. The charged exciton binding energy is obviously negatively related to the substrate dielectric constant. Furthermore, the change trends of the binding energy of the monolayer WSe2 on different substrates are basically the same for the increase of the excitation density. These results suggest that the choice of the substrate plays a significant role in the modulation of the PL properties and exciton states of atomically thin WSe2; hence, substrate engineering should be carefully considered in the design of future 2D devices. [ABSTRACT FROM AUTHOR]

We use time-resolved optical reflectivity with femtosecond resolution to study the ultrafast dynamics of photoexcited carriers in bulk GaAs. We observe an emergence of short-lived excitons at room temperature right after photoexcitation, in terms of a sharp dip and sub-ps lifetime in the transient reflectivity changes, as long as the pump fluence increases above a critical value F c. Our findings help understand ultrafast physics in this material. [ABSTRACT FROM AUTHOR]

We fabricated organic–inorganic perovskite nanocrystals in nanoporous glasses (OIPiG) where (C6H5C2H4NH3)2PbBr4 (Phe) was incorporated into about 4 nm diameter pores and evaluated their photoluminescence and scintillation properties, compared with the Phe single crystal. Both the samples showed emissions due to the recombination of free excitons in the inorganic layer under 280 nm excitation light. In scintillation, a weak and broad scintillation peak possibly due to the free excitons and bound excitons was observed in the OIPiG, while the Phe single crystal showed efficient scintillation due to free exciton emissions with a peak approximately at 435 nm. The scintillation decay time constant (4.4 ns) due to the free excitons for the OIPiG was found to be faster than that (6.6 ns) for the Phe single crystal. In addition, the afterglow levels were confirmed to be 340 ppm for the OIPiG and 20 ppm for the Phe single crystal. The afterglow level of the OIPiG was higher than that of the Phe single crystal but was almost equivalent to that for the commonly used inorganic scintillator CsI:Tl. [ABSTRACT FROM AUTHOR]

InAs quantum dots (QDs) have been grown on a GaAs (001) substrate in the subcritical region of InAs coverage for transition from a 2-dimensional (2D) to a 3-dimensional growth mode. Evolution of QDs and the corresponding wetting layer (WL) with InAs coverage has been investigated. Under specific growth conditions, quantum dot formation was observed only in samples where InAs coverage is more than 1.48 ML. The QD density increases sharply with InAs deposition initially but slows down with increased coverage. Photoluminescence (PL) shows the existence of a third peak, other than QD and WL peaks, at the low energy side of the WL peak, which is named the precursor peak. Evidence is presented supporting the theory that this peak is due to 2D InAs islands on a monolayer of InAs, which are small enough to localize excitons. Meanwhile, the WL peak is due to larger InAs islands under high compressive strain. During QD formation, the WL peak energy increases with the increase in InAs deposition. This is due to the sudden transfer of material from the bigger size of InAs islands to the QD. Our results show that the QD, WL, and precursor peaks coexist near the onset of QD formation. The power dependence of the three PL peaks is evident, which supports to our conclusion. [ABSTRACT FROM AUTHOR]

In a ZnO microcavity, the exciton-polariton effect with ultralarge Rabi splitting (can be as large as several hundreds of millielectron volts) may dominate the optical properties at the energies near the band edge. Due to the light-matter coupling, the renormalized energy states, i.e., the exciton-polariton states are expected to show very different dynamical behavior compared to the free exciton state. In this work, we used a femtosecond laser to pump a high-quality ZnO whispering gallery microcavity at room temperature. In the time-resolved photoluminescence measurements, we observed that both the fast and slow decay rates of the exciton-polaritons are faster than that of the free exciton due to the strong coupling between excitons and photons in a microcavity. The decay time constants are found to depend on the exciton-photon energy detuning (δ = E p h o t o n − E e x c i t o n ). [ABSTRACT FROM AUTHOR]

Control of unwanted low-energy emission originating due to trap states is crucial for improving the emission efficiency and for maintaining the color purity in blue light-emitting diodes. Here, a truxene-based emitter (T-pyrene) that is a good candidate for the blue emitter is investigated using photophysical studies. Steady-state absorption of the emitter reveals the presence of a charge-transfer state, and the photoluminescence spectrum suggests an occurrence of a strong interchain/exciplex state. Time-resolved photoluminescence (TRPL) and fluence-dependent measurements of the material in the dilute solution show the presence of multiple excitonic processes contributing to the delayed fluorescence. Similar studies on the pristine film suggest that the delayed fluorescence is dominated by the presence of the traps. By blending the oligomer with a higher bandgap polymer matrix, poly(9-vinyl carbazole) (PVK), a type I heterojunction at the T-pyrene:PVK interface is obtained that confines the generated excitons in T-pyrene. With this architecture, device efficiencies with T-pyrene (20 wt. %):PVK show significantly enhanced efficiency than those of the pristine device. We elucidate the relevance of the matrix:T-pyrene system using TRPL and fluence-dependent studies on T-pyrene (20 wt. %):PVK. Time-resolved emission spectra on the T-pyrene (20 wt. %):PVK films do not show red-shifted emission with time delays, which suggests the passivation of the quenching sites due to the dispersion of T-pyrene in PVK to prevent the intermolecular interactions. [ABSTRACT FROM AUTHOR]

The phonon-assisted cyclotron-resonance (PACR) effect due to the one-photon (1P) and two-photon (2P) absorption processes in a quantum well (QW) with the Pöschl-Teller (PT) potential is studied. The magneto-optical absorption coefficient as functions of photon energy for different QW-parameters, magnetic fields, and temperatures is presented. The calculations are done for four different possible cases: both 1P- and 2P-processes as well as both phonon emission and absorption processes. The numerical results for a GaAs, InAs, InSb, and GaSb PT-QW show that the PACR peaks are blueshifted with κ and magnetic field, redshifted with QW-length, but remained unchanged with temperature. Peak intensities are found to increase with κ and magnetic field and decrease with QW-length but have a complex dependency on the temperature. The full-width at half-maximum is found to increase with κ , magnetic field, and temperature but found to decrease with QW-length. The phonon emission process is always dominant in comparison with absorption. The 2P-process is comparable with the 1P-process and should be taken into account when studying the PACR in QWs. [ABSTRACT FROM AUTHOR]

The investigation of the fluctuations and their influence on the exciton in the perovskite structure is topical. These fluctuations can be due to the prolongation of the annealing or the increasing of the temperature in the perovskite monolayers. This fact generates structural imperfections, which may arise from vacancies and lattice structural defects. In this work, we propose a theoretical approach in order to study the optical properties characterized by excitons in (RNH 3) 2 (CH 3 NH 3) p − 1 Pb p I 3 p + 1 perovskite structures. For high quality samples, we investigate the free exciton taking into account the quantum and the dielectric confinements. For low quality samples, we model the surface disorder of perovskite monolayers through a randomized potential in the layer plane. Finally, we investigate the dependence of the perovskite layer thickness (p -value) on the shift between the relaxed exciton compared to the free exciton, and we show that our model allows us to simulate the experimental spectra of the exciton states. [ABSTRACT FROM AUTHOR]

A methodology is described to extract the absorption coefficient spectrum and exciton oscillator strength of GaN layers and GaN/AlGaN quantum wells by analyzing microtransmittance experiments in high-quality, free-standing membranes with thicknesses in the 160–230 nm range. The absorbance of a subwavelength GaN membrane is found to be an oscillating function of its thickness, in keeping with the standing wave effect. We analyze our results using two alternative models including interference effects and extract identical absorption coefficient values. The room-temperature absorption coefficient of bulk GaN membranes at the main exciton peak is found to be 9 × 104 cm−1. In the case of GaN/AlGaN quantum wells, the enhancement and blue shift of the excitonic absorption are observed, as a result of quantum confinement. [ABSTRACT FROM AUTHOR]

Disintegration and formation of excitons in graphene nanodots are investigated within the framework of mean-field approximation to the Hubbard model. Optically active excitons are found to be disintegrated in the non-magnetic nanodots and are shown to form only when the system enters into the antiferromagnetic state. As the Hubbard parameter U / t exceeds a critical value, the nanodot is found to undergo a phase transition from the non-magnetic to an antiferromagnetic phase. Before the phase transition, both optical and quasiparticle gaps are found to be nearly independent of the interaction strength. After the phase transition, however, the quasiparticle gap is revealed to increase more rapidly than the optical gap, which eventually leads to a positive binding energy of the bright exciton in the antiferromagnetic nanodot. The understanding of this extraordinary disintegration and formation of excitons in different magnetic phases of graphene nanodots is believed to be of paramount importance for their potential optoelectronic applications. [ABSTRACT FROM AUTHOR]

We report on a systematic study of the determination of the internal quantum efficiency (IQE) in AlGaN-based multiple-quantum-well (MQW) structures using different optical evaluation methodologies and experimental conditions, in order to derive a standard set of measurement conditions for reliable IQE determination. Several potential sources of error that may distort the IQE obtained by optical measurements are discussed, such as carrier transport effects, excitation conditions failing to fulfill ideal resonance conditions, and morphology issues. A series of nominally identical AlGaN-based MQW structures is grown on an AlGaN layer separated by an AlN interlayer of varying thickness. The MQW structures are studied both by resonant and quasiresonant photoluminescence spectroscopy, and IQEs are determined via different commonly employed methods. The obtained values are shown to be significantly affected by the employed excitation conditions, as well as the evaluation techniques. In addition, growth morphology issues and carrier transport effects need to be considered in the interpretation of the measured data, with the latter being investigated in greater detail. The results emphasize the need for an appropriate choice of both experimental conditions and evaluation methodology in order to extract reliable and comparable IQE values. [ABSTRACT FROM AUTHOR]

Siligraphene belonging to the family of two-dimensional (2D) materials has great potential in optoelectronics due to its considerable excitonic effects. In this study, the strain effects on the electronic structure and the real-space exciton wave functions of g - SiC 7 are investigated using the first-principles calculations based on the ab initio many-body perturbation theory. Alongside the increase (decrease) of the bandgap with compressive (tensile) strain, our results show that the exciton in the siligraphene monolayer under in-plane biaxial compressive strains is much more localized than that in the case of tensile one, leading to the higher and lower exciton binding energies, respectively. Moreover, the π ↦ π and π ↦ σ exciton state transition emerges when applying the compressive and tensile strains, respectively. Overall, our study reveals that a desirable way to dissociate the electron-hole coupling and to reduce the electron-hole recombination process is applying "in-plane biaxial tensile strain," making g - SiC 7 an excellent potential functional 2D semiconductor in optoelectronics. [ABSTRACT FROM AUTHOR]

Exciton decay dynamics can be optically controlled by changing the excitation conditions, particularly, the excitation intensity. In this study, we report how the exciton dynamics in cyanine thin films depend on the excitation intensity and sequence. The excitons in these films have two decay components, and the ratio of the population of the fast decay component to the total population depends on the excitation intensity. Conversely, sequential excitation by a second optical pulse does not alter this ratio. Although the total excitation power is comparable, the change in the dynamics by the second pulse is different from the simple increase in the excitation power. Therefore, the sequential excitation by the second pulse can be a key point for realizing low-power optical switches. [ABSTRACT FROM AUTHOR]

In this work, we present a detailed investigation of the low temperature emission properties of ZnSeO alloys by means of photoluminescence, micro-photoluminescence, and time-resolved photoluminescence. We show that the low temperature broad photoluminescence spectrum of ZnSeO attributed to the recombination of localized excitons is composed of sharp lines related to individual trapping states. Based on studies of photoluminescence thermal quenching from individual trapping states and photoluminescence dynamics, the mechanism of nonradiative recombination in ZnSeO alloys is discussed. Moreover, an unexpected decrease of the low temperature Stokes shift with increasing oxygen content is observed in contrast to what has been reported for GaAs based highly mismatched alloys. The possible origin of this effect is proposed. [ABSTRACT FROM AUTHOR]

The 1S-exciton density N X (1) in GaN, AlN, and ZnO is calculated for thermal-nonequilibrium states where the temperatures of an electron–hole system and phonons are different in the range of 10–400 K. The ratio of N X (1) in AlN to that in ZnO reaches 21 despite the similar exciton-binding energies of AlN and ZnO, which is due to the higher rate of excitation by LO-phonon absorption in ZnO. This result reveals that thermal-nonequilibrium states significantly affect the validity of evaluation methods for physical parameters such as internal quantum efficiency of radiation. The ratio of N X (1) in AlN to that in ZnO is enhanced from 2.2 to 18 by the occupation of states of the principal quantum number n from 2 to 5. This result demonstrates the importance of the discussion on the n ≥ 3 states which have not been taken into account in other analyses. The main reason for the decrease in N X (1) is found to be the increase in the temperature of LO phonons rather than LA phonons, which indicates the importance of LO-phonon control in light-emitting devices. The results for general thermal-nonequilibrium states are nontrivial because the mechanisms of the population balance are complicated owing to the several-n occupation and the transition rates determined by various factors. Our analyses and discussions quantitatively unveil the LO- and LA-phonon effects on the thermal-nonequilibrium excitation and deexcitation dynamics of excitons and provide the basis for design of highly efficient light-emitting devices particularly in the ultraviolet region. [ABSTRACT FROM AUTHOR]

We use a master equation model for numerical simulations of triplet loss mechanisms in phosphorescent organic light-emitting diodes (OLEDs). In addition to the IV characteristics, which were successfully simulated in our previous work, the measurements of luminous efficacy (LE) for the OLEDs with various doping profiles of the emitter fac-tris(2-phenylpyridine)iridium (III) (Ir(ppy) 3) can be reproduced based on a single set of excitonic parameters, which is a strong indication of the validity of the model. In order to minimize the strong Dexter diffusion of triplets out of the emission layer (EML) and the nonradiative decays, an additional exciton blocking layer and stronger exciton confinement on guest molecules are investigated in the simulations to improve the device efficiency. With the modifications, the LE of the lowest-doped OLED with 4% Ir(ppy) 3 can be more than twofold increased at a luminance up to 20 000 cd / m 2 . However, due to the enhanced triplet-triplet annihilation, the roll-off in electrophosphorescence efficiencies under high current injections of the upgraded devices becomes stronger, which can nevertheless be suppressed by a higher emitter concentration in the EML. [ABSTRACT FROM AUTHOR]

The exciton bound to a pair of nitrogen atoms situated at nearby lattice sites in dilute GaAs:N provides an energetically uniform electronic system, spectrally distinct from pairs with larger or smaller separations, and can even be grown with a uniform pair orientation in the crystal. We use photoluminescence excitation spectroscopy on an ensemble of N pairs to study the narrow continuous energy distribution within two of the individual exchange- and symmetry-split exciton states. Inhomogeneous linewidths of 50–60 μeV vary across the crystal on a mesoscopic scale and can be 30 μeV at microscopic locations indicating that the homogeneous linewidth inferred from previous time-domain measurements is still considerably broadened. While excitation and emission linewidths are similar, results show a small energy shift between them indicative of exciton transfer via phonon-assisted tunneling between spatially separated N pairs. We numerically simulate the tunneling in a spatial network of randomly distributed pairs having a normal distribution of bound exciton energies. Comparing the ensemble excitation-emission energy shift with the measured results shows that the transfer probability is higher than expected from the dilute pair concentration and what is known of the exciton wavefunction spatial extent. Both the broadening and the exciton transfer have implications for the goal of pair-bound excitons as a single- or multi-qubit system. [ABSTRACT FROM AUTHOR]