Anomalous Emission Behavior Research Articles

Observation of anomalous excitonic emission in V-doped WS2 QDs synthesized by hydrothermal method and subsequent mechanical exfoliation

This study focuses on synthesizing vanadium (V) doped 2H phase WS2 via a facile hydrothermal method and subsequent liquid phase mechanical exfoliation of the material into QD-like nanostructures. An increment in dopant percentage from 1 % to 7 % red shifted the band gap of WS2 from 4.15 eV to 3.78 eV. The nanostructures show electronic transition due to B, A, and defect-bound excitons and demonstrate modulation of excitonic behavior with V doping. Low V doping provides the WS2 material with a reduced B/A excitonic peak intensity ratio because of the nonradiative pathways favoring the relaxation of high energy B excitons to A excitons. High V doping results in anomalous emission behavior marked by an increased B/A ratio, attributed to positive trion formation as a result of excess free hole concentration due to the p-type vanadium. The study suggests that V-doped WS2 nanostructures hold potential for technological applications, particularly in spintronics and photonics, emphasizing the importance of engineering exciton dynamics in two-dimensional materials using p-type substitutional dopants.

Anomalous emission behavior of excitons at low temperature in monolayer WS2

We report on the anomalous emission behavior of excitons (X) in monolayer WS2 using temperature dependent photoluminescence spectroscopy. In general, PL emission from excitons enhances with decreasing temperature due to suppression of phonon mediated non-radiative transitions. Here, we observe that excitonic PL is temperature independent, although with decreasing temperature, the emission intensity for trion (X −) and biexciton or defect-bound excitons (XX/L 1) increases up to 123 K and then decreases. Analysis of experimental data with a model derived from the Boltzmann distribution and Saha equation reveal conversion of excitons into trions, biexcitons or defect-bound excitons and an increase of spin forbidden dark state with reduction in temperature. These findings could provide better strategies for designing future quantum devices.

Photoluminescence study and observation of unusual optical transitions in Cu2ZnSnSe4/CdS/ZnO solar cells

In this paper, we examine photoluminescence spectra (PL) of Cu2ZnSnSe4/CdS/ZnO solar cells, based on an absorber layer fabricated by selenization of sputtered Cu, Zn, Sn multilayers, via temperature-dependent and illumination power-dependent measurements. We observe anomalous emission behavior: the PL peak initially decreases with increasing temperature (red shift) in the temperature range 10–60K, followed by a blue shift at higher temperature in the range 60–180K. A recombination model is proposed that is able to explain both temperature dependent PL as well as power-dependent PL. The important aspect of the proposed model is taking into account the presence of strong potential fluctuations in the absorber layer, which can also contribute to the low Voc values generally observed in Cu2ZnSnSe4, based solar cells.

Correlation between optical properties surface morphology of porous silicon electrodeposited by Fe3+ ion

In this paper, we analyze the photoluminescence spectra (PL) of porous silicon (PS) layer which is elaborated by electrochemical etching and passivated by Fe3+ ions (PSF) via current density, electro-deposition and temperature measurements. We observe unusual surface morphology of PSF surface and anomalous emission behavior. The PSF surface shows regular distribution of cracks, leaving isolated regions or “platelets” of nearly uniform thickness. These cracks become more pronounced for high current densities. The temperature dependence of the PL peak energy (EPL) presents anomalous behaviors, i.e., the PL peak energy shows a successive red/blue/redshift (S-shaped behavior) with increasing temperature that we attribute to the existence of strong potential fluctuations induced by the electrochemical etching of PS layers. A competition process between localized and delocalized excitons is used to discuss these PL properties. In this case, the potential confinement plays a key role on the enhancement of PL intensity in PSF. To explain the temperature dependence of the PL intensity, we have proposed a recombination model based on the tunneling and dissociation of excitons.

Preparation, optical properties and solar cell applications of CdS quantum dots synthesized by chemical bath deposition

We reported on temperature-dependent photoluminescence (PL) studies of CdS quantum dots (QDs, ~5 nm in diameter) grown onto TiO2 nanorod arrays by chemical bath deposition. By constructing a liquid-junction solar cell, a power conversion efficiency of 0.88 % was demonstrated. In addition, we observed anomalous emission behavior, specifically a ‘Λ’-shaped (blueshift–redshift) temperature dependence of the peak energy for CdS related PL with increasing temperature. From a study of the integrated PL intensity as a function of temperature, it was revealed that thermionic dissociation of excitons (carriers) out of local potential minima into higher energy states was the dominant mechanism leading to the quenching behavior of the QDs related PL. At 110 K, the localized excitons were totally dissociated and converted to the free excitons. Our results shed light on the exciton-dissociation process in CdS QDs and can be used for the proposed solar cell application.

Direct Observation of an Ordered Phase in (1120) Plane InGaN Alloy

A polar-dependent phase with spontaneous atomic ordering is found in a nonpolar (1120) plane In0.08Ga0.92N film grown by metalorganic vapor-phase epitaxy. An atomic arrangement is a periodic sequence of group-III sublattices, such as In0.04Ga0.96N/In0.12Ga0.88N, that is only observed in a nitrogen polar region through systematic transmission electron microscopy investigation. Cathodoluminescence (CL) in the nitrogen polar region, i.e., spontaneously ordered atomic structure of InGaN, reveals anomalous emission behavior, specifically an S-shape-like (increase–decrease) temperature dependence of CL peak energy. It is suggested that the spontaneous ordered atomic structure of InGaN plays the role of a localized center owing to band gap shrinkage, which has been reported in other III–V alloy systems.

Dynamics of Anomalous Temperature-Induced Emission Shift in MOCVD-grown (Al, In)GaN Thin Films

We present a comprehensive study of the optical characteristics of (Al, In)GaN epilayers measured by photoluminescence (PL), integrated PL intensity, and time-resolved PL spectroscopy. For not only InGaN, but also AlGaN epilayers with large Al content, we observed an anomalous PL temperature dependence: (i) an “S-shaped” PL peak energy shift (decrease-increase-decrease) and (ii) an “inverted S-shaped” full width at half maximum (FWHM) change (increase-decrease-increase) with increasing temperature. Based on time-resolved PL, the S shape (inverted S shape) of the PL peak position (FWHM) as a function of temperature, and the much smaller PL intensity decrease in the temperature range showing the anomalous emission behavior, we conclude that strong localization of carriers occurs in InGaN and even in AlGaN with rather high Al content. We observed that the following increase with increasing Al content in AlGaN epilayers: (i) a Stokes shift between the PL peak energy and the absorption edge, (ii) a redshift of the emission with decay time, (iii) the deviations of the PL peak energy, FWHM, and PL intensity from their typical temperature dependence, and (iv) the corresponding temperature range of the anomalous emission behavior. This indicates that the band-gap fluctuation responsible for these characteristics is due to energy tail states caused by non-random inhomogeneous alloy potential variations enhanced with increasing Al content.

Dynamics of Anomalous Temperature-Induced Emission Shift in MOCVD-grown (Al, In)GaN Thin Films

AbstractWe present a comprehensive study of the optical characteristics of (Al, In)GaN epilayers measured by photoluminescence (PL), integrated PL intensity, and time-resolved PL spectroscopy. For not only InGaN, but also AlGaN epilayers with large Al content, we observed an anomalous PL temperature dependence: (i) an “S-shaped” PL peak energy shift (decrease-increase-decrease) and (ii) an “inverted S-shaped” full width at half maximum (FWHM) change (increase-decrease-increase) with increasing temperature. Based on time-resolved PL, the S shape (inverted S shape) of the PL peak position (FWHM) as a function of temperature, and the much smaller PL intensity decrease in the temperature range showing the anomalous emission behavior, we conclude that strong localization of carriers occurs in InGaN and even in AlGaN with rather high Al content. We observed that the following increase with increasing Al content in AlGaN epilayers: (i) a Stokes shift between the PL peak energy and the absorption edge, (ii) a redshift of the emission with decay time, (iii) the deviations of the PL peak energy, FWHM, and PL intensity from their typical temperature dependence, and (iv) the corresponding temperature range of the anomalous emission behavior. This indicates that the band-gap fluctuation responsible for these characteristics is due to energy tail states caused by non-random inhomogeneous alloy potential variations enhanced with increasing Al content.

“S-shaped” temperature-dependent emission shift and carrier dynamics in InGaN/GaN multiple quantum wells

We report temperature-dependent time-integrated and time-resolved photoluminescence (PL) studies of InGaN/GaN multiple quantum wells (MQWs) grown by metalorganic chemical vapor deposition. We observed anomalous emission behavior, specifically an S-shaped (decrease–increase–decrease) temperature dependence of the peak energy (Ep) for InGaN-related PL with increasing temperature: Ep redshifts in the temperature range of 10–70 K, blueshifts for 70–150 K, and redshifts again for 150–300 K with increasing temperature. In addition, when Ep redshifts, the spectral width is observed to narrow, while when Ep blueshifts, it broadens. From a study of the integrated PL intensity as a function of temperature, it is found that thermionic emission of photocarriers out of local potential minima into higher energy states within the wells is the dominant mechanism leading to the thermal quenching of the InGaN-related PL. We demonstrate that the temperature-induced S-shaped PL shift is caused by a change in the carrier dynamics with increasing temperature due to inhomogeneity and carrier localization in the InGaN/GaN MQWs.

Structure in the lowest absorption feature of CdSe quantum dots

We use transient differential absorption experiments to investigate the ‘‘single dot’’ absorption line shape of CdSe quantum dots. We observe both a narrow (full width half maximum ∼5 meV) and a broad (∼50 meV) bleach component within the inhomogeneously broadened first absorption line of our samples. We deduce the single dot absorption line shape which is most consistent with the experimental results. This line shape, which contains structure in the lowest quantum dot absorption feature, explains the large ‘‘Stokes’’ shift seen in the full band edge luminescence of CdSe quantum dots. We discuss the structure within the context of several competing models. The data appear inconsistent with models which use surface states to explain the anomalous emission behavior of II–VI quantum dots. Instead they imply that exciton fine structure is observed in our samples.