Deep Level Defect States Research Articles

Enhancing energy storage performance of polyethylene via passivation with oxygen atoms through C–H vacancy carbonylation

Low energy density of polymer film capacitors is regarded as one of the most serious drawbacks facing growing demands for equipment integration and miniaturization. Herein, ultraviolet light and ozone (UVO) surface modification is utilized to simultaneously improve dielectric constant and breakdown strength of polyethylene (PE) films. As a result, after 3 min of UVO treatment, an enhanced recoverable energy density of 4.79 J/cm3 with a charge-discharge efficiency of >95% is obtained under 650 MV/m at room temperature (RT). Significantly, stable energy storage performance under 200 MV/m is maintained throughout a broad temperature range from −90 °C to 90 °C and during 20,000 cycles of charge-discharge procedures. According to first-principles calculations and thermally stimulated depolarization current measurements, formation of carbonyl groups (C=O) after UVO treatment could effectively passivate initial deep-level defect states caused by H vacancies, which explains the improvement in capacitive energy storage. Moreover, the metalized UVO-modified PE exhibits valuable breakdown self-clearing ability, and the self-cleared specimen maintains stable energy storage performance over 20,000 cycles at 200 MV/m and RT. This work offers an effective and user-friendly method for enhancing comprehensive dielectric characteristics of PE-based materials and potential for applications in modern power systems and electronic devices.

Metastable defect curing by alkaline earth metal in chalcogenide thin-film solar cells

This study investigates the use of an alkaline earth metal precursor (MgF2) to enhance the performance of chalcogenide-based Cu(In,Ga)Se2 (CIGS) solar cells with a chemically bath deposited-Zn(O,S) (CBD-Zn(O,S)) buffer layer via post-deposited treatment (PDT). The optimal substrate temperature and layer thickness are 570 °C and 5 nm, and the light soaking (LS) treatment does not be required in this condition. The morphological properties and chemical reaction at the p-n junction of CIGS/CBD-Zn(O,S) are examined as a function of MgF2 PDT layer thickness. As the MgF2 PDT layer thickness increases, the CIGS surface becomes rough with vigorously agglomerated Cu clusters owing to the substantially high substrate temperature, which increases the incorporation of In-Se bonds and the oxygenation rate of MgF2. Density functional theory (DFT) clarifies the improved cell efficiency without the need for LS treatment (MgF2 PDT, 5 nm) by calculating the defect-related electronic behavior. The MgF2 phase effectively passivates metastable defect Cu-Se vacancy defects (VCu-Se), related to the LS effect without the additional formation of deep-level defect states into the CIGS bandgap. Moreover, VCu-Se states exert the most influence on the LS effect, and the control of defect states in the CIGS layer (not the buffer layer) is crucial for cell efficiency.

Physical passivation of deep-level defect states in polymer dielectrics for outstanding dielectric properties

The limited dielectric strength of polymer dielectrics hampers their reliable use in highly integrated electrical systems and high-energy storage film capacitors. This constraint is closely associated with the presence of deep-level defect states in polymer dielectrics. Here, we present an efficient and stable approach for the physical passivation of deep-level defect states aimed at enhancing the dielectric properties of polymer dielectrics. Employing inductively coupled plasma technology with argon as the carrier gas, the polymer undergoes substantial decreased deep-level defect states, as evidenced by nano-micro-region defect measurements. Consequently, the localized charge accumulation in the treated polymer dielectric is significantly reduced, resulting in a remarkable 62% increase in flashover voltage. The breakdown strength is also enhanced, and the treated material exhibits long-term stability. Moreover, materials featuring passivated deep-level defect states can boost discharge energy density without compromising efficiency. For instance, PTFE with passivated deep-level defect states maintains a discharge energy density of 1.18 J/cm3 and a charge-discharge efficiency of 95.06% at 200 °C and 300 MV/m. By focusing on deep-level defect states passivation, we introduce a strategy for receiving polymers with exceptional performance and stability.

Optically Reconfigurable Complementary Logic Gates Enabled by Bipolar Photoresponse in Gallium Selenide Memtransistor.

To avoid the complexity of the circuit for in-memory computing, simultaneous execution of multiple logic gates (OR, AND, NOR, and NAND) and memory behavior are demonstrated in a single device of oxygen plasma-treated gallium selenide (GaSe) memtransistor. Resistive switching behavior with RON /ROFF ratio in the range of 104 to 106 is obtained depending on the channel length (150 to 1600nm). Oxygen plasma treatment on GaSe film created shallow and deep-level defect states, which exhibit carriers trapping/de-trapping, that lead to negative and positive photoconductanceat positive and negative gate voltages, respectively. This distinguishing feature of gate-dependent transition of negative to positive photoconductance encourages the execution of four logic gates in the single memory device, which is elusive in conventional memtransistor. Additionally, it is feasible to reversibly switch between two logic gates by just adjusting the gate voltages, e.g., NAND/NOR and AND/NAND. All logic gates presented high stability. Additionally, memtransistor array (1×8) is fabricated and programmed into binary bits representing ASCII (American Standard Code for Information Interchange) code for the uppercase letter "N". This facile device configuration can provide the functionality of both logic and memory devices for emerging neuromorphic computing.

Contaction of atoms for outstanding dielectric characteristics in KX-passivated polymer dielectrics

High-power, high-integration, and high-energy storage density electrical devices and film capacitors require polymer dielectrics with high dielectric characteristics. However, polymer dielectrics accumulate significant charge during operation, causing local electric field distortion, flashover and breakdown. The deep-level defect state (electron/hole accumulation center) fundamentally affects the dielectric strength. Unfortunately, research on passivating deep-level defects in polymer dielectrics is limited. In this study, KX (X = F, Cl, Br, I) effectively passivated deep-level defect states in polymer dielectrics. The cation dipole effect on polymers was found to be the deep-level defect passivation principle. The principle of anion passivation of deep-level defects by suspending anions and cations is the key to producing more stable C covalent bonds. Such bonds transfer the local charge from C with the lone electron pair that originally contains the hanging bond. Therefore, some transfer occurs, and the anion implements effective passivation. We also investigated the passivation mechanism of KX anion-passivated polymer dielectrics. We found that anions can transform bonding-state defects into antibonding-state defects at deep-level defects in the gap. Therefore, the energy of the defect state rises and disappears in the deep band gap. This study addressed the design of high-performance polymer dielectrics, providing a reference for experimental and theoretical analyses.

Surface morphological and optical evolution of RF sputtered AZO films for optoelectronic devices

Herein, aluminium-doped zinc oxide (AZO) films were fabricated onto borosilicate glass and fluorine-doped tin oxide (FTO) substrates by RF sputtering. Surface morphology and scaling studies of these films revealed the formation of large grain in AZO films fabricated onto the glass substrates. Several fractal parameters of all samples have been evaluated to understand the deeper morphological insights of observed surfaces. Optical investigations revealed a higher transmittance of ∼93% in the visible region for FTO/AZO films. Estimated values of Urbach energy are found to be 0.20 eV and 0.17 eV for glass/AZO and FTO/AZO films, respectively. Important optical constants such as refractive indices, extinction coefficients, etc have been investigated to explore the optical mechanism of these films. Furthermore, photoluminescence studies suggest the reduction in the deep-level emission defect states for AZO films fabricated onto FTO substrate. These results propose that AZO films may be suitable for use in optoelectronics.

Insights Into to the KX (X = Cl, Br, I) Adsorption-Assisted Stabilization of CsPbI2 Br Surface.

Despite the excellent optoelectronic properties, organic-inorganic hybrid perovskite solar cells (PSCs) still present significant challenges in terms of ambient stability. CsPbI2 Br, a member of all-inorganic perovskites, may respond to this challenge because of its inherent high stability against light, moisture, and heat, and therefore has gained tremendous attraction recently. However, the practical application of CsPbI2 Br is still impeded by the notorious phenomenon of photoinduced halide segregation. Herein, by applying first-principles calculations, the stability, electronic structure, defect properties, and ion-diffusion properties of the stoichiometric CsPbI2 Br (110) surface and that with the adsorption of KX (X = Cl, Br, I) are systematically investigated. It is found that the adsorbed KX can serve as an external substitute of the halogen vacancies on the surface, therefore inhibiting halogen segregation and improving the stability of the CsPbI2 Br surface. The KX can also eliminate deep-level defect states caused by antisites, thereby contributing to the promoted optoelectronic properties of CsPbI2 Br. The mechanistic understanding of surface passivation in this work can lay the foundation for the future design of CsPbI2 Br PSCs with optimized optoelectronic performance.

Analysis of Nitrogen-Doping Effect on Sub-Gap Density of States in a-IGZO TFTs by TCAD Simulation.

In this work, the impact of nitrogen doping (N-doping) on the distribution of sub-gap states in amorphous InGaZnO (a-IGZO) thin-film transistors (TFTs) is qualitatively analyzed by technology computer-aided design (TCAD) simulation. According to the experimental characteristics, the numerical simulation results reveal that the interface trap states, bulk tail states, and deep-level sub-gap defect states originating from oxygen-vacancy- (Vo) related defects can be suppressed by an appropriate amount of N dopant. Correspondingly, the electrical properties and reliability of the a-IGZO TFTs are dramatically enhanced. In contrast, it is observed that the interfacial and deep-level sub-gap defects are increased when the a-IGZO TFT is doped with excess nitrogen, which results in the degeneration of the device’s performance and reliability. Moreover, it is found that tail-distributed acceptor-like N-related defects have been induced by excess N-doping, which is supported by the additional subthreshold slope degradation in the a-IGZO TFT.

Deep level defect states in β-, α-, and ɛ-Ga2O3 crystals and films: Impact on device performance

A review is given of reported trap states in the bandgaps of different polymorphs of the emerging ultrawide bandgap semiconductor Ga2O3. The commonly observed defect levels span the entire bandgap range in the three stable (β) or meta-stable polymorphs (α and ɛ) and are assigned either to impurities such as Fe or to native defects and their complexes. In the latter case, the defects can occur during crystal growth or by exposure to radiation. Such crystalline defects can adversely affect material properties critical to device operation of transistors and photodetectors, including gain, optical output, threshold voltage by reducing carrier mobility, and effective carrier concentration. The trapping effects lead to degraded device operating speed and are characterized by long recovery transients. There is still significant work to be done to correlate experimental results based on deep level transient spectroscopy and related optical spectroscopy techniques to density functional theory and the dominant impurities present in the various synthesis methods to understand the microscopic nature of defects in Ga2O3.

Effect of Cation Occupancy Ordering in Double Perovskites To Overcome Hurdles in Carrier Transport: Cs2AgBiBr6 as a Case Study

In spite of environmental stability and toxic-free merits, the performance of double perovskite solar cells (Cs2AgBiBr6 to be specific) has not excelled due to their large indirect band gap, low absorption of solar spectrum, and more importantly hurdles in carrier transport processes. A large number of intrinsic defects and self-trapped excitons (STE) appear in the double perovskite due to a disordered arrangement of Ag/Bi octahedra in the perovskite lattice. In this work, we investigate the role of cation ordering in Cs2AgBiBr6 through the use of phenethylammonium bromide (PEABr) in the precursor toward suppression of STEs and deep-level defect states, such as antisite defects of Ag+/Bi3+, for an improved carrier conduction process. While cation ordering has been verified from X-ray diffraction studies and Raman spectroscopy, a reduction in the defect density and inhibition of STE formation have been witnessed from optical spectroscopy results. The transport gap, obtained from scanning tunneling spectroscopy and density of states spectra thereof, has been found to increase, suggesting the defect states to become suppressed. The effect of cation ordering toward an efficient carrier transport in the ordered lattice of Cs2AgBiBr6 has been demonstrated by Kelvin probe force microscopy and conductive atomic force microscopy. Finally, a fair improvement in photovoltaic parameters was observed in devices based on the ordered double perovskite.

Recent Progress on Perovskite Surfaces and Interfaces in Optoelectronic Devices.

Surfaces and heterojunction interfaces, where defects and energy levels dictate charge-carrier dynamics in optoelectronic devices, are critical for unlocking the full potential of perovskite semiconductors. In this progress report, chemical structures of perovskite surfaces are discussed and basic physical rules for the band alignment are summarized at various perovskite interfaces. Common perovskite surfaces are typically decorated by various compositional and structural defects such as residual surface reactants, discrete nanoclusters, reactions by products, vacancies, interstitials, antisites, etc. Some of these surface species induce deep-level defect states in the forbidden band forming very harmful charge-carrier traps and affect negatively the interface band alignments for achieving optimal device performance. Herein, an overview of research progresses on surface and interface engineering is provided to minimize deep-level defect states. The reviewed subjects include selection of interface and substrate buffer layers for growing better crystals, materials and processing methods for surface passivation, the surface catalyst for microstructure transformations, organic semiconductors for charge extraction or injection, heterojunctions with wide bandgap perovskites or nanocrystals for mitigating defects, and electrode interlayer for preventing interdiffusion and reactions. These surface and interface engineering strategies are shown to be critical in boosting device performance for both solar cells and light-emitting diodes.

Light-matter interactions in high quality manganese-doped two-dimensional molybdenum diselenide

Introducing magnetic dopants into two-dimensional transition metal dichalcogenides has recently attracted considerable attention due to its promising applications in spintronics and valleytronics. Herein we realized manganese-doped molybdenum diselenide (MoSe2) single crystal via chemical vapor transport (CVT) reaction, containing up to 2.9% (atomic concentration) Mn dopants, and investigated the light-matter interaction in these samples. We observed a suppressed trion intensity, a longer photoluminescence lifetime, and prominent blue- and red-shift of E 2g 2 (in-plane) and A1g (out-of-plane) Raman modes, respectively. Moreover, the Mn dopants increase the valley Zeeman splitting of the MoSe2 monolayer by ∼50%, while preserving the linear dependence on magnetic field. First-principles calculations indicate that the spin-polarized deep level defect states are formed due to the Mn substitutional dopants in the MoSe2 lattice. The resulting defect potential favors the funnelling of excitons towards the defects. The Mn dopants reduce the magnitude of the interatomic force constants, explaining the red-shift of the A1g mode. The Mn atoms and their immediate Mo and Se neighbors carry significant magnetic moments, which enhance the observed exciton g-factors due to the exchange interactions affecting defect-bound excitons.

Interaction of ZnO nanorods with plasmonic metal nanoparticles and semiconductor quantum dots

We model the enhancement of near band edge emission from ZnO nanorods using plasmonic metal nanoparticles and compare it with emission enhancement from ZnO with semiconducting quantum dots. Selected CdSe quantum dots with absorption energies close to those of Ag and Au nanoparticles are chosen to construct model systems with ZnO to comprehend the role of ZnO's intrinsic defects and plasmonic excitation in realizing the spectrally selective luminescence enhancement. Excitation wavelength dependent photoluminescence spectra along with theoretical models quantifying the related transitions and plasmonic absorption reveal that a complex mechanism of charge transfer between the ZnO nanorods and metal nanoparticles or quantum dots is essential along with an optimal energy band alignment for realizing emission enhancement. The theoretical model presented also provides a direct method of quantifying the relative transition rate constants associated with various electronic transitions in ZnO and their change upon the incorporation of plasmonic nanoparticles. The results indicate that, while the presence of deep level defect states may facilitate the essential charge transfer process between ZnO and the plasmonic nanoparticles, their presence alone does not guarantee UV emission enhancement and strong plasmonic coupling between the two systems. The results offer clues to designing novel multicomponent systems with coupled plasmonic and charge transfer effects for applications in charge localization, energy harvesting, and luminescence enhancement, especially in electrically triggered nanophotonic applications.

Effective growth and characterization of piperazinium orthophthalate single crystal yielding high second harmonic generation efficiency

Good quality organic non-linear optical single crystal of piperazinium orthophthalate (PPA) was grown successfully by solution growth at room temperature by achieving the supersaturation state in slow evaporation method. The powder XRD analysis confirms the crystalline nature and structural parameters of the grown PPA crystal. The FTIR and Raman spectra confirm the existence of acid-base functional groups along with their vibrational mode exhibited, present in the grown PPA crystal. UV–Vis spectrum exhibits better transparency in the visible region with cut-off wavelength of 330 nm and the energy band gap (Eg) is analyzed to be 3.8 eV. Photoluminescence spectra shows good optical property with the excitation of 342 nm and two emission peaks in near edge UV band with blue emission at 364 and the energy transition in deep level defect states in crystals by exhibiting the green emission at 533 nm respectively. The thermal stability and the thermal absorption of the PPA crystal were identified by the TG - DTA analysis and obtained thermal stability was up to 88 °C. Vickers micro hardness test illustrates the mechanical stability of the grown PPA crystal and it belong to soft category (n = 4.6). Etching studies illustrates the growth pattern of the grown crystal using water as etchant. FE-SEM analysis shows the perfect smooth morphology of the grown PPA crystal. Second harmonic generation study illustrates the grown PPA crystal (λ = 532 nm) exhibit good nonlinear optical response.

Influence of neutron irradiation on deep levels in Ge-doped (010) β-Ga2O3 layers grown by plasma-assisted molecular beam epitaxy

The impact of high energy neutron irradiation on the creation of specific radiation-induced deep level defect states and the ensuing influence of these defects on the electronic properties of (010) β-Ga2O3, doped with Ge and grown by plasma-assisted molecular beam epitaxy, were explored. A significant amount of carrier removal was observed in the irradiated samples exposed to 1 MeV equivalent neutron fluences of 8.5 × 1014 cm−2 and 1.7 × 1015 cm−2, which suggests the formation of compensating defects by neutron irradiation. Using a combination of deep level transient/optical spectroscopy (DLTS/DLOS) techniques to probe the entire ∼4.8 eV bandgap with high energy resolution, three specific trap states were introduced by neutron irradiation at EC-1.22 eV, EC-2.00 eV, and EC-0.78 eV. Of these, the former two states, observed by DLOS, were also present prior to irradiation, whereas the trap at EC-0.78 eV, observed by DLTS, was not evident prior to neutron irradiation. The radiation dependence suggests that intrinsic point defects are the likely physical sources for these states. Subsequent lighted capacitance-voltage measurements further revealed that these three states are the source for the observed strong carrier compensation, with the trap at EC-2.00 eV appearing as the strongest compensating defect for the neutron-irradiated β-Ga2O3.

Tunable and anisotropic photoresponse of layered Re0.2Sn0.8Se2 ternary alloy

In order to produce high-performance optoelectronic devices, alloy engineering has been exploited in ternary transition metal dichalcogenides. In the present study, we demonstrated the effect of rhenium incorporation on the structural and electrical response in SnSe2 layered crystals grown by direct vapour transport technique. Elemental conformation was characterized by EDAX. The powder X-ray diffraction shows the hexagonal phase and high crystallinity of grown compounds, which is also confirmed by the TEM SAED pattern. Perfectly hexagonal shaped microcrystals are shown in SEM surface micrograph. Raman spectra indicate the redshift in the vibrational mode peaks of SnSe2 with the rhenium doping. Current-time characteristic was measured to study to the effect of alloy engineering on the photoresponse ability of the grown compound. Among all, Re0.2Sn0.8Se2 ternary alloy shows the enhanced photoresponse under polychromatic illumination, showing the suppression of deep-level defect states after incorporation of Re in SnSe2 lattice structure. These materials have a layered structure and exhibit the anisotropic conductivity. Hence the anisotropic photodetection characteristics of Re0.2Sn0.8Se2 ternary alloy based photodetectors are further studied in detail. Photocurrent and photo responsivity are higher along the symmetric contacts, whereas along the asymmetric contacts both the quantities are lower in magnitude because the photogenerated carriers have to cross the perpendicular resistance of is layers stacked together by the weak Vander Waal's forces. Increasing the bias voltage enhances the photoresponsivity from 5.141 mAW−1 to 67.231 mAW−1 and photodetectivity 0.971 to 3.452 × 109 Jones. Anisotropic photoresponse was also studied under the monochromatic light. Results provide the significant understanding of tunable and layered structure dependent anisotropic photoresponse ability of TMDC materials.

Mn valence state mediated room temperature ferromagnetism in nonpolar Mn doped GaN

In this work, we demonstrate room temperature ferromagnetism in nonpolar, m-plane manganese doped gallium nitride (m-GaN:Mn) epitaxial thin films synthesized using plasma-assisted molecular beam epitaxy on nonpolar, m-plane sapphire (Al2O3) substrates. We observed that Mn doping concentration plays a key role in stabilizing the valence state of Mn ions thereby influencing the magnetic and transport properties. Chemical characterization by X-ray photoelectron spectroscopy, X-ray absorption near edge spectra, and energy dispersive X-ray spectroscopy affirm homogeneous valence state Mn+3 in lightly doped samples, while higher doping levels cause a heterogeneous Mn+0 and Mn+2 mixed valence states. Magnetic measurements indicate that films with low doping levels show the signature of room temperature ferromagnetism, while films with higher doping show antiferromagnetic/spin glass behavior besides the indication of MnGa alloys. Temperature dependent resistivity measurements show that both the samples are semiconducting with deep level defect states. Our findings suggest the possibility of incorporating spin functionality in non-polar optoelectronic devices.

Enhancement of transport properties in single ZnSe nanowire field-effect transistors

Wide-gap semiconductors are excellent candidates for next-generation optoelectronic devices, including tunable emitters and detectors. ZnSe nanowire-based devices show great promise in blue emission applications, since they can be easily and reproducibly fabricated. However, their utility is limited by deep level defect states that inhibit optoelectronic device performance. The primary objective of this work is to show how the performance of ZnSe nanowire devices improves when nanowires are subjected to a post-growth anneal treatment in a zinc-rich atmosphere. We use low temperature photoluminescence spectroscopy to determine the primary recombination mechanisms and associated defect states. We then characterize the electronic properties of ZnSe nanowire field effect transistors fabricated from both as-grown and Zn-annealed nanowires, and measure an order-of-magnitude improvement to the electrical conductivity and mobility after the annealing treatment. We show that annealing reduces the concentration of zinc vacancies, which are responsible for strong compensation and high amounts of scattering in the as-grown nanowires.

Annealing of deep level defects in GaAs nanostructures by ion beam irradiation

Present study reports the fabrication of Gallium Arsenide (GaAs) nanostructures on silicon (Si) substrates with the help of GaAs ions produced by hot and dense argon plasma in a modified dense plasma focus device. The fabricated nanostructures are further irradiated by Ar2+ ion beam having energy of 100 keV and fluences of 1 × 1013 ions/cm2, 5 × 1014 ions/cm2 and 5 × 1015 ions/cm2 in a ion beam accelerator. The morphological, stoichiometric and optical properties of as-fabricated and ion beam irradiated nanostructures have been compared to study the presence of defect states. As-deposited GaAs nanodots were found to be modified as nanostructured films upon ion irradiation. Excess arsenic present in as-deposited nanodots as deep level defect, is removed from ion irradiated nanostructured films. Thus, we found that the deep level defect states i.e., arsenic antisite (EL2) were annealed out in ion irradiated samples as is evident from Raman and photoluminescence spectra. It is found that ion irradiation reduces the EL2 defects in nanostructured films which have immense potential applications in enhancing efficiency of optoelectronic and electronic devices.

Molecular beam epitaxial growth, transmittance and photoluminescence spectra of zinc-blende CdTe thin films with high-quality on perovskite SrTiO3 (1 1 1) substrates

High-crystalline quality CdTe thin films are grown on the largely lattice-mismatched SrTiO3 (STO) (1 1 1) substrates by molecular beam epitaxy. A transformation from a three dimensional regime to a two dimensional one is observed by the reflection high energy electron diffraction (RHEED) and atomic force microscopy (AFM). The formation of an elastic deformation CdTe layer on STO (1 1 1), namely a pseudomorphic growth mode with a critical thickness of ∼40 nm, is supported by the RHEED, AFM and X-ray diffraction. Crystal structures and epitaxial relationships of CdTe epitaxial films on STO (1 1 1) are characterized by 2θ-ω scans and reciprocal space mapping. Two strong absorption peaks at the energies of ∼1.621 eV and ∼1.597 eV at 5 K are clearly observed for a ∼120 nm thick CdTe epitaxial film, which are proposed to be ascribed to the strained and unstrained epitaxial CdTe layers, respectively. Moreover, the presence of the exciton band while the absence of deep level defect states for the ∼120 nm thick CdTe film characterized by the temperature dependent photoluminescence spectra further supports the high-crystalline quality.