Intensity Of Exciton Emission Research Articles

Excitonic properties of deep-blue emitting fragmented CsCl:Eu2+ nanocrystals

In this work, polycrystalline CsCl:Eu2+ nanocrystals were grown by the hot injection method. The CsCl:Eu2+ nanocrystals were fragmented into particles of a few nanometers by dispersion in organic solvents, and they exhibited strong deep-blue emission under ultraviolet light. Excitonic emission at room temperature was observed near 410 nm, with a full width at half-maximum of 37.8 nm and a photoluminescence quantum yield of 4.1%. Additionally, the average exciton lifetime was determined to be 6.45 ns. In the temperature range of 10 K to 300 K, the excitonic emission intensity gradually decreased while the energy of the peak position slightly increased, corresponding to an increase in the temperature. From the result, the exciton binding energy and average longitudinal phonon energy were calculated to be about 29 and 13 meV, respectively, comparable to the energy calculations of similar Cs-series perovskites. Thermal expansion and electron-phonon interaction also increased steadily with the temperature, and these two phenomena gave rise to a monotonic blue-shift.

Pressure-controlled free exciton and self-trapped exciton emission in quasi-one-dimensional hybrid lead bromides

Hybrid metal halides represent a novel type of semiconductor light emitters with intriguing excitonic emission properties, including free exciton emission and self-trapped exciton emission. Achieving precise control over these two excitonic emissions in hybrid metal halides is highly desired yet remains challenging. Here, the complete transformation from intrinsically broadband self-trapped exciton emission to distinctively sharp free exciton emission in a quasi-one-dimensional hybrid metal halide (C2H10N2)8[Pb4Br18]·6Br with a ribbon width of n = 4, is successfully achieved based on high-pressure method. During compression, pressure-induced phonon hardening continuously reduces exciton–phonon coupling, therefore suppressing excitonic localization and quenching the original self-trapped exciton emission. Notably, further compression triggers excitonic delocalization to induce intense free exciton emission, accompanied with reduced carrier effective masses and improved charge distribution. Controlled high-pressure investigations indicate that the ribbon width of n > 2 is necessary to realize excitonic delocalization and generate free exciton emissions in similar quasi-one-dimensional hybrid metal halides. This work presents an important photophysical process of excitonic transitions from self-trapped exciton emission to free exciton emission in quasi-one-dimensional hybrid metal halides without chemical regulation, promoting the rational synthesis of hybrid metal halides with desired excitonic emissions.

Two-Dimensional Exciton Oriented Diffusion via Periodic Potentials.

Excitonic devices operate based on excitons, which can be excited by photons as well as emitting photons and serve as a medium for photon-carrier conversion. Excitonic devices are expected to combine the advantages of both the high response rate of photonic devices and the high integration of electronic devices simultaneously. However, because of the neutral feature, exciton transport is generally achieved via diffusion rather than using electric fields, and the efficient control of exciton flux directionality has always been difficult. In this work, a precisely designed one-dimensional periodic nanostructure (1DPS) is used to introduce periodic strain field along with resonant mode to the WS2 monolayer, achieving exciton oriented diffusion with a 7.6-fold exciton diffusion coefficient enhancement relative to that of intrinsic, while enhancing the excitonic emission intensity by a factor of 10 and reducing exciton saturation threshold power by 2 orders of magnitude. Based on the analysis of the density functional theory (DFT) and the finite-element method (FEM), we attribute the anisotropy of exciton diffusion to exciton funneling induced by periodic potentials, which do not require excessive potential height difference for an efficient oriented diffusion. As a result of resonant emission, the exciton diffusion is dragged into the nonlinear regime owing to the high exciton density close to saturation, which improves the exciton diffusion coefficient and diffusion anisotropy more appreciably.

Enhancing Layer-Engineered Interlayer Exciton Emission and Valley Polarization in van der Waals Heterostructures via Strain.

Layer-engineered interlayer excitons from heterostructures of transition-metal dichalcogenides (TMDCs) exhibit a rich variety of emissive states and intriguing valley spin-selection rules, the effective modulation of which is crucial for excitonic physics and related device applications. Strain or high pressure provides the possibility to tune the energy of the interlayer excitons; however, the reported emission intensity is substantially quenched, which greatly limits their practical application in optoelectronic devices. Here, via applying uniaxial strain based on polyvinyl alcohol (PVA) encapsulation technique, we report enhanced layer-engineered interlayer exciton emission intensity with largely modulated emission energy in WSe2/WS2 heterobilayer and heterotrilayer. Both momentum-direct and momentum-indirect interlayer excitons were observed, and their emission energies show an opposite shift tendency upon applied strain, which agrees with our DFT calculations. We further demonstrate that intralayer and interlayer exciton states with low phonon interactions can be modulated through the mechanical strain applied to the PVA substrate at low temperatures. Due to strain-induced breaking of the 3-fold rotational symmetry, we observe the enhanced valley polarization of interlayer excitons. Our study contributes to the understanding and modulation of the optical properties of interlayer excitons, which could be exploited for optoelectronic device applications.

Super-Resolution Exciton Imaging of Nanobubbles in 2D Semiconductors with Near-Field Nanophotoluminescence Microscopy.

Two-dimensional (2D) semiconductors, such as transition metal dichalcogenides, have emerged as important candidate materials for next-generation chip-scale optoelectronic devices with the development of large-scale production techniques, such as chemical vapor deposition (CVD). However, 2D materials need to be transferred to other target substrates after growth, during which various micro- and nanoscale defects, such as nanobubbles, are inevitably generated. These nanodefects not only influence the uniformity of 2D semiconductors but also may significantly alter the local optoelectronic properties of the composed devices. Hence, super-resolution discrimination and characterization of nanodefects are highly demanded. Here, we report a near-field nanophotoluminescence (nano-PL) microscope that can quickly screen nanobubbles and investigate their impact on local excitonic properties of 2D semiconductors by directly visualize the PL emission distribution with a very high spatial resolution of ∼10 nm, far below the optical diffraction limit, and a high speed of 10 ms/point under ambient conditions. By using nano-PL microscopy to map the exciton and trion emission intensity distributions in transferred CVD-grown monolayer tungsten disulfide (1L-WS2) flakes, it is found that the PL intensity decreases by 13.4% as the height of the nanobubble increases by every nanometer, which is mainly caused by the suppression of trion emission due to the strong doping effect from the substrate. In addition to the nanobubbles, other types of nanodefects, such as cracks, stacks, and grain boundaries, can also be characterized. The nano-PL method is proven to be a powerful tool for the nondestructive quality inspection of nanodefects as well as the super-resolution exploration of local optoelectronic properties of 2D materials.

Local piezoelectric doping of monolayer WSe2

We report non-contact local doping of a monolayer WSe2 transferred onto a piezoelectric substrate having surface potential wells (SPWs) induced by structural inhomogeneities. We used epitaxial GaN and InP/GaInP2 structures, in which there are SPWs ∼0.2 V deep and 0.1–2 μm in size. Using surface topography and potential scanning probe microscopy, as well as optical reflectance, photoluminescence, and Raman spectroscopy measurements, we observed strong enhancement of charged exciton emission and Raman intensity in the SPW regions of the monolayer WSe2, which indicate on piezoelectric doping at a level n ≥ 1012 cm−2 on a length scale ∼0.2–1 μm. Our results can be used to create electron/hole quantum puddles with anyon states in transition metal dichalcogenides, promising for the development of room temperature and magnetic-field-free fault-tolerant topological quantum computing.

Growth of non-polar m-plane GaN pseudo-substrates by Molecular beam epitaxy

Non-polar m-plane GaN films were grown by Plasma Assisted Molecular Beam Epitaxy on γ-LiAlO2 (100) substrates by a controlled coalescence of GaN nanocolumns obtained by a two-step process including a top-down nanopillars etching from a GaN buffer and a subsequent bottom-up overgrowth. Transmission electron microscopy data show a significant reduction of extended defects density in the coalesced film as compared to the initial GaN buffer, most likely due to a filter effect by the regrowth process on the nanopillars inclined walls. Low temperature photoluminescence spectra back this reduction by a strong intensity decrease of the stacking faults fingerprint emission peaks, while a very intense donor-bound excitonic emission at 3.472 eV, 2.8 meV wide, becomes dominant.

Optical properties of heterostructure CdTe/CdMgTe doped in various ways

The reflection and luminescence spectra of a CdTe/CdMgTe heterostructures doped with iodine are studied. Iodine was introduced either into a barrier layer or into a wide CdTe quantum well. It is shown how the doping method and level affect the spectra and the temperature dependence of the quantum well exciton emission intensity. Keywords: heterostructure CdTe/CdMgTe, doping, exciton, luminescence.

Оптические свойства гетероструктуры CdTe/CdMgTe, легированной различными способами

The reflection and luminescence spectra of a CdTe/CdMgTe heterostructures doped with iodine are studied. Iodine was introduced either into a barrier layer or into a wide CdTe quantum well. It is shown how the doping method and level affect the spectra and the temperature dependence of the quantum well exciton emission intensity.

Enhanced Spontaneous Emission of CsPbI3 Perovskite Nanocrystals Using a Hyperbolic Metamaterial Modified by Dielectric Nanoantenna.

In this work, we demonstrate, theoretically and experimentally, a hybrid dielectric-plasmonic multifunctional structure able to provide full control of the emission properties of CsPbI3 perovskite nanocrystals (PNCs). The device consists of a hyperbolic metamaterial (HMM) composed of alternating thin metal (Ag) and dielectric (LiF) layers, covered by TiO2 spherical MIE nanoresonators (i.e., the nanoantenna). An optimum HMM leads to a certain Purcell effect, i.e., an increase in the exciton radiative rate, but the emission intensity is reduced due to the presence of metal in the HMM. The incorporation of TiO2 nanoresonators deposited on the top of the HMM is able to counteract such an undesirable intensity reduction by the coupling between the exciton and the MIE modes of the dielectric nanoantenna. More importantly, MIE nanoresonators result in a preferential light emission towards the normal direction to the HMM plane, increasing the collected signal by more than one order of magnitude together with a further increase in the Purcell factor. These results will be useful in quantum information applications involving single emitters based on PNCs together with a high exciton emission rate and intensity.

The influence of Si on the properties of MOVPE grown GaN thin films: Optical and EPR study

Metal Organic Vapour Phase epitaxy (MOVPE) grown GaN layers doped with Si were studied by means of radio-, photo- and thermally stimulated luminescence, scintillation decay kinetics, as well as electron paramagnetic resonance. Two luminescence bands were observed: the narrow and fast peaking at about 3.45 eV (ascribed to excitons) and the broad and slow one having maximum at about 2.2 eV (produced by the defect – a carbon occupying nitrogen site). The decay time and the intensity of exciton and defect-related emission exhibit dependence on the doping level of Si. Both bands are getting faster upon the increased Si content. Moreover, the presence of Si influences drastically the charge trapping processes as well – the changes in the intensity of the glow peaks within the 100–300 K temperature range were observed. Besides, the new glow peaks appear and are getting stronger in the 300–450 K region upon Si doping. Interestingly, the effect of Si on the conductivity properties of the GaN samples was observed by means of electron paramagnetic resonance.

Cd2V2O7–ZnO mixed oxide for extended wavelength absorption with suppressed charge carrier recombination: A photocatalytic material

A type-II mixed oxide Cd2V2O7–ZnO was prepared by hydrothermal method and its morphological and optical properties were analysed with various scientific techniques. FESEM and AFM images showed the aggregated porous morphology by the individual spherical particles. The X-ray diffraction studies confirmed its formation, crystallinity and size of the particles as 47 nm. The UV–visible DRS spectrum showed its visible light-responsive nature and the optical band gap of bare ZnO and Cd2V2O7–ZnO mixed oxide to be 3.3 and 3.0 eV respectively. The mixed oxide also revealed the extended lifetime of the charge carriers by means of decreased excitonic emission intensity from the conduction band to valence band. The prepared mixed oxide was employed as photocatalyst in the degradation of methylene blue dye under solar radiation, the results indicated that the mixed oxide degraded the dye to an extent of 90% in just 30 min of light reaction in comparison to bare ZnO which degraded the dye to an extent of 69% in the same period. The degradation reaction followed pseudo-first-order reaction kinetics with the rate constant of 4.097 × 10−2 min−1 for ZnO and 6.665 × 10−2 min−1 for Cd2V2O7–ZnO mixed oxide composite.

Orientation-Mediated Luminescence Enhancement and Spin-Orbit Coupling in ZnO Single Crystals.

Temperature-, excitation wavelength-, and excitation power-dependent photoluminescence (PL) spectroscopy have been utilized to investigate the orientation-modulated near band edge emission (NBE) and deep level emission (DLE) of ZnO single crystals (SCs). The near-band-edge emission of ZnO SC with <0001> orientation exhibits strong and sharp emission intensity with suppressed deep level defects (mostly caused by oxygen vacancies Vo). Furthermore, Raman analysis reveals that <0001> orientation has dominant E2 (high) and E2 (low) modes, indicating that this direction has better crystallinity. At low temperature, the neutral donor-to-bound exciton (DoX) transition dominates, regardless of the orientation, according to the temperature-dependent PL spectra. Moreover, free-exciton (FX) transition emerges at higher temperatures in all orientations. The PL intensity dependence on the excitation power has been described in terms of power-law (I~Lα). Our results demonstrate that the α for <0001>, <1120>, and <1010> is (1.148), (1.180), and (1.184) respectively. In short, the comprehensive PL analysis suggests that DoX transitions are dominant in the NBE region, whereas oxygen vacancies (Vo) are the dominant deep levels in ZnO. In addition, the <0001> orientation contains fewer Vo-related defects with intense excitonic emission in the near band edge region than other counterparts, even at high temperature (~543 K). These results indicate that <0001> growth direction is favorable for fabricating ZnO-based highly efficient optoelectronic devices.

Direct Patterning of Optoelectronic Nanostructures Using Encapsulated Layered Transition Metal Dichalcogenides.

Direct top-down nanopatterning of semiconductors is a powerful tool for engineering properties of optoelectronic devices. Translating this approach to two-dimensional semiconductors such as monolayer transition metal dichalcogenides (TMDs) is challenging because of both the small scales required for confinement and the degradation of electronic and optical properties caused by high-energy and high-dose electron radiation used for high-resolution top-down direct electron beam patterning. We show that encapsulating a TMD monolayer with hexagonal boron nitride preserves the narrow exciton linewidths and emission intensity typical in such heterostructures after electron beam lithography, allowing direct patterning of functional optical monolayer nanostructures on scales of a few tens of nanometers. We leverage this fabrication method to study size-dependent effects on nanodot arrays of MoS2 and MoSe2 as well as laterally confined electrical transport devices, demonstrating the potential of top-down lithography for nanoscale TMD optoelectronics.

Si−doped In0.145Ga0.855As0.123Sb0.877: A novel p−type quaternary alloy with high crystalline quality

Antimonide−based p−n junctions are particularly attractive for a wide variety of optoelectronic applications in the near and mid-infrared wavelength range. In this work, novel p−type Si−doped In0.145Ga0.855As0.123Sb0.877 epitaxial layers were grown on GaSb(100) substrates by Liquid Phase Epitaxy (LPE) technique. The XPS spectra measured on Si−doped In0.145Ga0.855As0.123Sb0.877 layers indicate that Si atoms behave as acceptors. The analysis of the surface depletion region and its relationship with phonon−plasmon L_ coupling were investigated using Raman spectroscopy, giving an acceptor concentration of NA ∼ 5.8 × 1017 cm−3 for a depletion region thickness of d ∼ 9.4 nm. Low temperature photoluminiscence (PL) spectrum for the Si−doped In0.145Ga0.855As0.123Sb0.877 layers showed a bound excitonic emission peak associated to neutral Sb acceptors, with an activation energy of ∼10meV and a donor−acceptor transition. It was observed that the Si doping reduces the excitonic emission intensity and increases the donor−acceptor pair recombination intensity.

Plasmon-mediated exciton-phonon coupling in CdS microbelts

Investigating underlying coupling mechanism between surface plasmons (SPs) and excitons is playing a very important role to achieve higher efficient and more stable excitonic optoelectronic devices. Here, cadmium sulfide (CdS) microbelts sputtered with Au nanoparticles (NPs) have been prepared for exploring the SP-mediated energy coupling effect. The enhancement of excitonic emission intensity and a red-shift of the peaks have been surveyed in the Fabry-Perot (F-P) resonant lasing spectra. The investigation on temperature-dependent photoluminescence (TDPL) spectra from these samples demonstrate that the optical phenomenon can be attributed to the exciton–phonon coupling. The research results will provide a paramount importance of theoretical support for building effective and bright photoelectric devices based on the complex SP materials system.

Structural, Optical, and Photocatalytic Properties of ZnSe Nanoparticles Influenced by the Milling Time

ZnSe nanoparticles (NPs) were prepared by combining both hydrothermal and mechanical milling methods. Transmission electron microscopy images show that fabricated ZnSe NPs with a sphere-like shape have an average size (d) in the range of 20–100 nm, affected by changing the milling time from 10 to 60 min. All the samples crystalize in zincblende-type structure without impurities, as confirmed by analyzing X-ray diffraction patterns, Raman spectra, and energy-dispersive X-ray spectroscopy. Carefully checking Raman spectra, we have observed the broadening and redshift of vibration modes as decreasing NP size, which are ascribed to extra appearance of disorder and defects. The photoluminescence study has found a blue emission at 462 nm attributed to the excitonic near-band edge and a broad defect-related emission around 520–555 nm. Increasing milling time leads to the decrease in the exciton-emission intensity, while the defect-related emissions increase gradually. Interestingly, as decreasing d, we have observed an improved photodegradation of Rhodamine B under UV irradiation, proving application potentials of ZnSe NPs in photocatalytic activity.

Patterning of transition metal dichalcogenides catalyzed by surface plasmons with atomic precision

Summary Plasmon-induced charge transfer has drawn considerable interests and spurred rapid developments of photovoltaics and photocatalysis. Various plasmonic metal/transition metal dichalcogenide (TMD) heterostructures have been developed to promote charge separation. For plasmon-induced catalysis, the transformation of TMDs is rare, and the erosion of TMDs has not yet been reported. Here, we report the etching of two-dimensional TMDs by planar surface plasmon polaritons (SPPs). We found that SPPs can etch various TMDs into desired layers and lateral size through controlling the light power and incident direction. In aqueous media, the strong plasmonic coupling at Au/MoS2 interface generates holes in the valence band of MoS2 that can weaken its interlayer interaction. As a synergistic effect, the plasmonic hot electrons produce oxidizing H2O2 to dissolve MoS2 from the top layers. Our results provide a new perspective for understanding the plasmonic coupling at metal-TMD interfaces and a reliable route toward fabricating well-defined TMDs.

Synthesis, characterization, and temperature-dependent electronic properties of ZnO nanorods using CBD techniques

High-quality and partially oriented ZnO nanorod films were synthesized by chemical bath deposition on top of a ZnO sol–gel spin-coating seed layer deposited on glass substrates. Two different ratios (0.625 and 6.25) of hexamethylenetetramine to zinc acetate were considered for the synthesis of the ZnO nanorod films and their optical, structural and electronic properties were studied. The ZnO nanorod films showed the wurtzite structure with a crystallite size about 50–55 nm, a dislocation density in the range of 1015 lines-m−2 and a strain in the range of 10–3. Energy dispersive spectroscopy and photoluminescence measurements indicated the existence of oxygen vacancies in the films. The ZnO nanorod films showed a bandgap energy about 3.24 eV. From photoluminescence results, an intense ultraviolet excitonic emission band was observed in the films. The films resulted with a carrier concentration in the range of 1015 and 1016 cm−3. From impedance spectroscopy measurements, a noticeable temperature-dependent electronic conductivity was observed, related probably to the nanostructured morphology of the films. In both films it was observed that the electronic conductivity decreased in the intermediate temperature region with the increment of temperature, probably due to chemisorption or desorption phenomena. But the electronic conductivity in the low and the high-temperature regions obeyed the grain boundary carrier-trapping model with the increment of the temperature, showing in both regions an activation energy close to 0.6 eV, attributed to the appearance of trap states due to the chemisorption of oxygen at the grain boundaries of the ZnO nanorods.

Sm3+ driven enhancement in photocatalytic degradation of hazardous dyes and photoluminescence properties of hexagonal-ZnO nanocolumns

Samarium doped ZnO (Sm-ZnO) nanocolumns were grown by wet chemical method and the doping effect of Sm3+ on visible light photocatalytic (PC) and photoluminescence (PL) properties of ZnO was investigated. Methylene blue (MB) and methyl orange (MO) were considered for the degradation study as a step initiated towards the remediation of industrial wastewater. Subsequent characterization studies by x-ray diffraction (XRD) and field emission scanning electron microscopy (FESEM) enumerate that the hexagonal-wurtzite structured Sm-ZnO is highly crystalline in nature and possesses hexagonal column like nano-architectures. Although, a charge imbalance exists between the ions, the substitutional effects of Sm3+ at Zn2+ sites have been observed from the XRD spectra and discussed by suitable mechanisms. FTIR measurement gives the information on the evolution of peaks related to metal-oxygen bond in Sm-ZnO which may be linked with Sm ions. PC measurement shows that the degradation efficiency of 95% can be achieved by Sm-ZnO photocatalysts in degrading MB and 91% for MO. Sm doping induces high charge separation efficiency and generation of OH ions in ZnO leading to such improvisation in degradation efficiency. The prepared Sm-ZnO nanocatalysts possess high degree of photostability and reusability even after fourth cycle of photodegradation. PL spectra show the suppression of the sharp and intense excitonic emission band of ZnO in Sm-ZnO due to low rated direct recombination of carriers. Incorporation of Sm3+ ends up with intrinsic defect mediated enhancement in the visible emissions especially in the blue, yellow and red region of light spectrum.