Charge Carrier Mobility Research Articles

Oxygen enriched PAni-based counter electrode network toward efficient dye-sensitized solar cells (DSSCs)

Dye-sensitized solar cells (DSSCs) have great potential as a renewable energy technology assisting combat climate change due to its low cost, adaptability, and sustainability. Oxygen plasma ion doping is a promising strategy to improve the capacity of a low-cost, platinum-free counter-electrodes (CEs) to absorb photons and drive high-performance DSSCs via generating an abundance of active absorption sites. In this instance, novel PAni–ZnO (PZ) composite layers were designed as a CE material and received various in-situ oxygen plasma dosages, including 0, 2, 4, 6, 8, and 10 min, to improve their physiochemical and microstructural feature for the first time, to the best of our knowledge. Physical evaluations of the microstructure, porosity, morphology, contact angle, roughness, electrical, and optical, electrochemical impedance spectroscopy (EIS) features of CEs were conducted in along with an evaluation of J–V variables. Compared to pristine CE substance, the surface nature of the modified hybrids was gradually enhanced as the plasma level rose, reaching an optimum after 8 min (i.e. 0.2 µm for average pore size and average roughness Ra = 7.21 µm). Expanded plasma treatment doses also improved PV cell performance even further: after 4 min at a plasma level, η = 5.41% was obtained, and after 6 min in a oxygen plasma environment, η = 5.81% was obtained. Mixing high energetic plasma ions increased the mobility of charge carriers in PAni composites along with lowered charge carrier recombination through generating an environment that was conducive to charge dissociation. Therefore, longer lifespans and more effective charge transfer inside the photovoltaic cell as a consequence of the increased mobility less resistive losses. In this respect, following 8 min of plasma surface modification of the PZ CE, the optimized efficiency of 6.31% and Jsc of 15.6 mA/cm2 were obtained. The improvement in efficiency equated to a proportion growth of 77% versus a pristine one. This gain was explained by the reality that suffusing a quantity of oxygen plasma free radicals into the PAni system developed continuous channels that enabled the mixture to move electrons more rapidly, hence raising the photovoltaic efficiency. Overall, this study highlights the advantages of regulating heteroatom species and their co-doping, offering a new perspective for the application of heteroatom-doped CE in DSSCs.

CsSnBr3 and Cs3Bi2Br9: Structural, Optical Characteristics, and Application in a Schottky Barrier Diode

The search for alternatives to Pb‐based perovskites, due to concerns about stability and toxicity, has led to the exploration of Pb‐free options. Tin (Sn) and bismuth (Bi) are promising candidates, given their similar ionic radii to Pb and the isoelectronic nature of Pb2+ and Bi3+, which suggest comparable chemical properties. Among these, CsSnBr3 and Cs3Bi2Br9 are relatively underexplored but offer lower toxicity and enhanced stability while demonstrating optoelectronic properties suitable for various applications. In this study, CsSnBr3 and Cs3Bi2Br9 nanocrystals are synthesized using a colloidal method and integrated into Schottky diodes. X‐ray photoelectron spectroscopy analysis of the surface chemistry confirms improved thermal and phase stability compared to Pb‐based perovskites. Schottky diode parameters, including ideality factor, barrier height, and series resistance are assessed using conventional thermionic emission, modified Cheung's, and Norde's models. The Cs3Bi2Br9‐based Schottky diode exhibits superior electrical performance with the lowest series resistance and optimal barrier height. Electrical impedance spectroscopy results indicated that CsSnBr3 has higher resistances and lower capacitances than Cs3Bi2Br9, reflecting lower charge carrier mobility and more defects, although the R1C1 regions in both materials demonstrated faster charge dynamics, making them ideal for high‐speed applications.

Ultrafast Charge and Exciton Diffusion in Monolayer Films of 9-Armchair Graphene Nanoribbons.

Determining the electronic transport properties of graphene nanoribbons is crucial for assessing their suitability for applications. So far, this has been highly challenging both through experimental and theoretical approaches. This is particularly the case for graphene nanoribbons that are prepared by chemical vapor deposition, which is a scalable and industry-compatible bottom-up growth method that results in closely packed arrays of ribbons with relatively short lengths of a few tens of nanometers. In this study, the experimental technique of spatiotemporal microscopy is applied to study monolayer films of 9-armchair graphene nanoribbons prepared using this growth method, and combined with linear-scaling quantum transport calculations of arrays of thousands of nanoribbons. Both approaches directly resolve electronic spreading in space and time through diffusion and give an initial diffusivity approaching 200 cm2 s-1 during the first picosecond after photoexcitation. This corresponds to a mobility up to 550 cm2 V-1 s-1. The quasi-free carriers then form excitons, which spread with a diffusivity of tens of cm2 s-1. The results indicate that this relatively large charge carrier mobility is the result of electronic transport not being hindered by defects nor inter-ribbon hopping. This confirms their suitability for applications that require efficient electronictransport.

Bulk Heterojunction Perovskite Solar Cells Incorporated with Conjugated Polyfluorenes

Ambipolar transport characteristics of metal halide perovskites (MHPs) enable both hole and electron to be transported simultaneously in perovskite solar cells (PSCs); however, unbalanced charge transport is a fundamental limitation in boosting power conversion efficiency (PCE) of PSCs. Compared to the PSCs with either n–i–p or p–i–n device structures, bulk heterojunction (BHJ) PSCs, inspired by organic photovoltaics, are recognized as superior for balancing charge transport and maximizing interface interactions. This study reports high‐performance BHJ PSCs, where the BHJ composites are composted with the n‐type MHPs mixed with the p‐type conjugated polyfluorenes. In the systematic studies, it is indicated that a small amount of conjugated polyfluorenes component can boost the crystallinity and grain size of the MHP thin film. Moreover, BHJ composite thin films possess boosted charge carrier mobility and a tendency of balanced charge transport and suppress both radiative and non‐radiative charge carrier recombinations. Most importantly, an efficient photoinduced charge transport within the BHJ composite thin film boosts photocurrent. As a result, the PSCs based on the n‐type MHPs:p‐type conjugated polyfluorenes BHJ composite thin film exhibit 23.46% of PCE and boost stability. The results demonstrate a facial method to approach high‐performance PSCs.

Soft hydrogel semiconductors with augmented biointeractive functions.

Hydrogels, known for their mechanical and chemical similarity to biological tissues, are widely used in biotechnologies, whereas semiconductors provide advanced electronic and optoelectronic functionalities such as signal amplification, sensing, and photomodulation. Combining semiconducting properties with hydrogel designs can enhance biointeractive functions and intimacy at biointerfaces, but this is challenging owing to the low hydrophilicity of polymer semiconductors. We developed a solvent affinity-induced assembly method that incorporates water-insoluble polymer semiconductors into double-network hydrogels. These semiconductors exhibited tissue-level moduli as soft as 81 kilopascals, stretchability of 150% strain, and charge-carrier mobility up to 1.4 square centimeters per volt per second. When they are interfaced with biological tissues, their tissue-level modulus enables alleviated immune reactions. The hydrogel's high porosity enhances molecular interactions at semiconductor-biofluid interfaces, resulting in photomodulation with higher response and volumetric biosensing with higher sensitivity.

As‐Doped Polycrystalline CdSeTe: Localized Defects, Carrier Mobility and Lifetimes, and Impact on High‐Efficiency Solar Cells

AbstractThe efficiency potential for single‐junction photovoltaics (PV) is described by the detailed balance model, which requires the elimination of nonradiative recombination and perfect minority carrier collection. Improvements in GaAs, Si, and perovskite PV follow this model. It might be more complex for CdTe, a leading thin‐film PV technology. While lifetime, passivation, and doping goals for 25% efficient CdTe solar cells are largely reached, voltage is ≈20% below the detailed balance limit. Why is that? In Se‐alloyed CdSexTe1‐x (Se is required for >20% efficiency) additional losses can occur due to electrostatic and bandgap fluctuations and due to electronic trap states. To understand mechanisms limiting CdSeTe solar cell performance and to suggest improvements, carrier dynamics, and transport in CdSexTe1‐x with variation in Se composition and as doping is analyzed. It is shown that trapping, likely due to anion‐site defects and their complexes, is correlated with low charge carrier mobility of 0.1–0.6 cm2 (Vs)−1. Even with 1000 ns charge carrier lifetimes, carrier diffusion length is less than the absorber thickness, reducing efficiency to ≈23%. Device simulations are used to analyze the performance of CdSexTe1‐x solar cells; thermodynamic models are not sufficient for absorbers with electronic disorder and trapping.

Unusual Cross-Conjugation in Cyclic Dipeptide-Based Building Blocks for Donor-Acceptor Semiconducting Conjugated Polymers.

Cross conjugation, though prevalent in many organic compounds, is typically considered less effective for electron delocalization compared to linear conjugation. Consequently, it is rarely used as the backbone structure for semiconducting conjugated polymers. In this study, we designed and synthesized a novel building block, TIDP, which features a central cyclic dipeptide with cross conjugation characteristics. Strong intramolecular hydrogen bonding interactions confer TIDP with a highly rigid and coplanar conformation. Importantly, theoretical calculations reveal that π electrons are well delocalized across the entire structure, despite its low aromaticity. Conjugated polymers incorporating TIDP exhibit high charge carrier mobilities, demonstrating the effective π electrons delocalization of this innovative building block. Our findings show that with rational design, cross conjugation can achieve effective π electrons delocalization, providing a valuable approach for developing high-performance conjugated polymers for organic electronic materials.

Modelling of Cut-off Frequency of Armchair Graphene Nanoribbon Tunnel Field Effect Transistor Using Transfer Matrix Method

Graphene is considered as a promising two-dimensional material for electronic device applications due to its high charge carrier mobility and it is extremely thin in size. As a material, graphene has great potential for the development of high-speed nano electric devices. Graphene can be used as a channel material in Tunnel Field Effect Transistor (TFET). In this study, the cut-off frequency of the armchair graphene nanoribbon tunnel field effect transistor (AGNR-TFET) device was modelled quantum mechanically. The solution of the Dirac-like Hamiltonian and Poisson equations self-consistently is used to determine the potential profile of device and the transmittance is calculated using the transfer matrix method (TMM). The Landauer formulation with the help of Gauss Legendre Quadrature Method (GLQM) is used to calculate the tunnelling current and the cut-off frequency of AGNR-TFET. The calculation results showed that the cut-off frequency increased as the drain voltage increased, while the increase in channel length and the N-index graphene made the cut-off frequency decreased. Moreover, the thicker the oxide layer could increase the cut-off frequency and the higher the temperature on the device would reduce the cut-off frequency.

Unusual Cross‐Conjugation in Cyclic Dipeptide‐Based Building Blocks for Donor–Acceptor Semiconducting Conjugated Polymers

AbstractCross conjugation, though prevalent in many organic compounds, is typically considered less effective for electron delocalization compared to linear conjugation. Consequently, it is rarely used as the backbone structure for semiconducting conjugated polymers. In this study, we designed and synthesized a novel building block, TIDP, which features a central cyclic dipeptide with cross conjugation characteristics. Strong intramolecular hydrogen bonding interactions confer TIDP with a highly rigid and coplanar conformation. Importantly, theoretical calculations reveal that π electrons are well delocalized across the entire structure, despite its low aromaticity. Conjugated polymers incorporating TIDP exhibit high charge carrier mobilities, demonstrating the effective π electrons delocalization of this innovative building block. Our findings show that with rational design, cross conjugation can achieve effective π electrons delocalization, providing a valuable approach for developing high‐performance conjugated polymers for organic electronic materials.

CsPbBr3 and Cs2AgBiBr6 Composite Thick Films with Potential Photodetector Applications

This paper investigates the optoelectronic properties of CsPbBr3, a lead-based perovskite, and Cs2AgBiBr6, a lead-free double perovskite, in composite thick films synthesized using mechanochemical and hot press methods, with poly(butyl methacrylate) as the matrix. Comprehensive characterization was conducted, including X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), UV–visible spectroscopy (UV–Vis), and photoluminescence (PL). Results indicate that the polymer matrix does not significantly impact the crystalline structure of the perovskites but has a direct impact on the grain size and surface area, enhancing the interfacial charge transfer of the composites. Optical characterization indicates minimal changes in bandgap energies across all different phases, with CsPbBr3 exhibiting higher photocurrent than Cs2AgBiBr6. This is attributed to the CsPbBr3 superior charge carrier mobility. Both composites showed photoconductive behavior, with Cs2AgBiBr6 also demonstrating higher-energy (X-ray) photon detection. These findings highlight the potential of both materials for advanced photodetector applications, with Cs2AgBiBr6 offering an environmentally Pb-free alternative.

Charge Carrier Dynamics of SnO2 Electron‐Transporting Layers in Perovskite Solar Cells

Perovskite solar cells (PSCs) have demonstrated remarkable increase in their photovoltaic efficiencies over the past several years. Charge carrier properties including charge selectivity, extraction, and transport play key roles in device performances. Therefore, a comprehensive insight into the charge carrier dynamics and mobility within the bulk materials and at the interface is of great importance for the future development of this cutting‐edge technology. This review discusses the recent advances that have been made in SnO2 electron‐transporting layers and their limitations, followed by outlining the key development of novel strategies in improving SnO2 films through surface defect engineering, interface modification, and doping approaches. In addition, the recent developments are highlighted for identifying the origin of defect and trap center, and promoting SnO2 electron extraction and transporting capacity in PSCs. Importantly, the novel approaches are also discussed for studying photogenerated charge carrier dynamics of the devices. In conclusion, the own prospectives and outlooks are presented for the development of SnO2‐based PSCs, with a particular focus on addressing current difficulties in SnO2 and providing in‐depth understanding on the relationships between materials and devices.

The mercurial rise in research of halide perovskites: what´s next

AbstractPerovskites are of high potential in the ongoing academic research, due to their distinctive electrical properties and crystalline structures. Halide perovskites show high light emissive properties and panchromatic light absorption across the visible spectrum. The exceptional electrical characteristics, such as their long carrier lifespan, high diffusion length, and charge carrier mobility, allow the electric charges to be transported and collected effectively. Furthermore, by tuning the cations and anions composition, perovskite’s opto-electrical properties can be altered. Moreover, dimension reduction affects their band gap and intrinsic features to induce higher structural stability but at the cost of the quantum confinement effect. Owing to their exceptional properties, halide perovskites are being researched in energy-related and semiconducting applications, hold high promise and the future looks bright. But challenges remain, and the larger question is what needs to be done to make them more stable.

(Ag–NiO)/g-C3N4 with enhanced photocatalytic activity for hydrogen evolution under simulated sunlight

g-C3N4 is a promising metal-free photocatalyst for hydrogen production, whose application is difficult due to the low mobility of charge carriers and rapid electron-hole recombination. Here we propose a new route to improve its response to simulated sunlight and prevent electron-hole recombination by grafting mixed Ag–NiO (1:1 nominal Ag/NiO weight ratio) materials, as an alternative to platinum group metal co-catalysts. g-C3N4 was prepared by urea pyrolysis, whereas Ag–NiO was prepared by a co-precipitation method, and then the composites were prepared by physical mixing using sonication-grinding. The presence of Ag–NiO on the surface plays a key role in accepting excited electrons and enhancing their lifetime for a subsequent reduction of protons to hydrogen. Hydrogen production was carried out from the photoreforming of ethanol under simulated sunlight. The results revealed that 2% (Ag–NiO)/g-C3N4 is effective among others with 5.2 times higher H2 production than unmodified g-C3N4. The percentage of ethanol in the ethanol/water ratio is very important as we have found that with increasing its quantity, the evolution of hydrogen becomes significant.

Phonon-limited mobility for electrons and holes in highly-strained silicon

Strain engineering is a widely used technique for enhancing the mobility of charge carriers in semiconductors, but its effect is not fully understood. In this work, we perform first-principles calculations to explore the variations of the mobility of electrons and holes in silicon upon deformation by uniaxial strain up to 2% in the [100] crystal direction. We compute the π11 and π12 electron piezoresistances based on the low-strain change of resistivity with temperature in the range 200 K to 400 K, in excellent agreement with experiment. We also predict them for holes which were only measured at room temperature. Remarkably, for electrons in the transverse direction, we predict a minimum room-temperature mobility about 1200 cm2 V−1 s−1 at 0.3% uniaxial tensile strain while we observe a monotonous increase of the longitudinal transport, reaching a value of 2200 cm2 V−1 s−1 at high strain. We confirm these findings experimentally using four-point bending measurements, establishing the reliability of our first-principles calculations. For holes, we find that the transport is almost unaffected by strain up to 0.3% uniaxial tensile strain and then rises significantly, more than doubling at 2% strain. Our findings open new perspectives to boost the mobility by applying a stress in the [100] direction. This is particularly interesting for holes for which shear strain was thought for a long time to be the only way to enhance the mobility.

Experimental Detection of Topological Electronic State and Large Linear Magnetoresistance in SrSn4 Superconductor

AbstractWhile recent experiments confirm the existence of hundreds of topological electronic materials, only a few exhibit the coexistence of superconductivity (SC) and a topological electronic state. These compounds attract significant attention in forefront research because of the potential for the existence of topological SC, paving the way for future technological advancements. SrSn4 is known for exhibiting unusual SC below the transition temperature (TC) of 4.8 K. Recent theory predicts a topological electronic state in this compound, which is yet to be confirmed by experiments. Systematic and detailed studies of the magnetotransport properties of SrSn4 and its Fermi surface characterizations are also absent. For the first time, a quantum oscillation study reveals a nontrivial 𝝅‐Berry phase, very light effective mass, and high quantum mobility of charge carriers in SrSn4. Magnetotransport experiment unveils large linear transverse magnetoresistance (TMR) of more than 1200% at 5 K and 14 T. Angle‐dependent transport experiments detect anisotropic and fourfold symmetric TMR, with the maximum value (≈2000%) occurring when the angle between the magnetic field and the crystallographic b‐axis is 45°. The results suggest that SrSn4 is the first topological material with SC above the boiling point of helium that displays such high magnetoresistance.

Designing Contact Independent High-Performance Low-Cost Flexible Electronics.

Organic semiconductors enable low-cost solution processing of optoelectronic devices on flexible substrates. Their use in contemporary applications, however, is sparse due to persistent challenges in achieving the requisite performance levels in a reliable and reproducible manner. A critical bottleneck is the inefficiency associated with charge injection. Here, large-scale simulations are employed to identify operational windows where key device parameters that are difficult to control experimentally, such as the contact resistance, become less consequential to overall device functionality. This design methodology overcomes injection barrier limitations in organic field-effect transistors (OFETs), leading to high charge carrier mobility and significantly expanding the range of suitable electrode materials. Leveraging this new understanding, all-organic, solution-deposited OFETs are successfully fabricated on flexible substrates. These devices incorporate printed contacts and showcase mobilities exceeding 5cm2Vs-1. These results provide a route for accessing the fundamental limits of material properties even in the absence of ideal contacts - a critical step in establishing reliable structure/property relationships and optimal material design paradigms. While reducing the injection barrier and contact resistance remains critical for achieving high OFET performance, this work demonstrates a path toward consistently achieving high charge carrier mobility through device geometry design, ultimately reducing processing complexity and cost.

Synthesis and characterization of zinc-doped hematite nanoparticles for photocatalytic applications and their electronic structure studies by density functional theory

Hematite nanoparticles doped with 1, 3 and 5 % Zn (all % are in molar) were prepared using mechanical alloying. Morphological and phase structure studies using scanning electron microscopy and X-ray diffraction showed nanoparticles possessing a semi-spherical shape and particle size of <50 nm crystallized in rhombohedral structure. The lattice parameters of hematite increased upon Zn doping. The energy-dispersive X-ray and Fourier-transform infrared results demonstrated that Zn was successfully incorporated. The optical behavior of nanoparticles was examined by UV–Vis diffuse reflectance spectroscopy and revealed that Zn doping increased the absorption intensity in the visible light region and decreased the band gap from 1.95 (hematite) to 1.83 eV (3 % Zn). Methylene blue dye degradation by the 3 % Zn sample proved doubling of the photocatalytic activity due to electronic structure modification upon Zn doping. First principles studies using density functional theory performed to investigate the effect of Zn on the electronic band structure of hematite showed that Zn doping caused band gap reduction, causing formation of new energy states, mainly above the valence band. Eventually, the enhancement of Urbach energy and reduction of effective mass, respectively accountable for increasing the relaxation time and mobility of charge carriers, were considered the two main mechanisms regarding the increased photocatalytic behavior of hematite by Zn doping.

Impact of Irreversible Adsorption on Molecular Ordering and Charge Transport in Poly(3-hexylthiophene) Thin Films on Solid Substrates.

We investigate the irreversible adsorption of poly(3-hexylthiophene) (P3HT) polymer thin films on silicon dioxide/silicon (SiO2/Si) substrates during thermal annealing at a temperature below the melting temperature (Tm) but far above the glass transition temperature (Tg), i.e., Tg ≪ T = 170 °C < Tm, and its effect on their crystalline ordering and charge transport properties. It was found that short-time annealing enhances the molecular ordering of P3HT films, while prolonged thermal annealing gradually disrupts the crystalline structures and reduces the overall crystallinity of the film. Concurrently, thermal annealing at this temperature facilitates the slow irreversible adsorption of P3HT chains at the polymer-solid interface, resulting in the formation of a 1.7 Rg-thick (∼18 nm thick) adsorbed layer on SiO2/Si substrates that is fully amorphous and contains a large fraction of loosely adsorbed chains. We postulate that such irreversible adsorption is responsible for the reduced crystalline packing of P3HT at the polymer-solid interface at Tg ≪ T < Tm, which further disrupts the molecular ordering of the entire 46 nm thick P3HT film by a long-range perturbation effect. Electrical measurements using an organic field-effect transistor (OFET) device reveal that the enhanced charge carrier mobility of P3HT films correlates with an optimized annealing time at Tg ≪ T < Tm, which achieves a balance between maximizing molecular ordering and minimizing the impact of irreversible chain adsorption. These findings provide new insights into the underlying mechanism of thermal annealing in tailoring the structure and property of conjugated polymer thin films prepared on solid substrates.

Exploring the photocatalytic production of hydrogen by Co, Cu or Pd species as co-catalysts supported on a ZnxTiyOz perovskite/TiO2 structure

A key factor for improving the performance of the hydrogen photocatalytic reaction is the logical, functional, and effective design of the photogenerated charge transfer through the solid-solid interface in a heterojunction. This point is particularly crucial in cases such as the one of TiO2, where a relatively rapid recombination occurs. In this work, a ZnxTiyOz/TiO2 heterojunction using the sol-gel nucleation is presented. This method gives rise to a strong and efficient interaction between ZnxTiyOz and TiO2, increasing the photocatalytic activity. Moreover, the addition of Co, Cu or Pd species to the heterojunction surface increases the hydrogen production, due to the strong interaction between them as shown by HRTEM and XPS analyses. Furthermore, the (photo)electrochemical characterization shows that the resistance to charge transfer decreases with co-catalysts, observing the following trend: Pd < Cu < Co. This outcome is related to the mobility and separation of charge carriers and the role played by co-catalysts in hydrogen production.

Research on the Fabrication and X‐Ray Detection Performance of MAPbBr3‐Based 3D/2D Heterojunctions

Perovskite materials, renowned for their high mean atomic number, charge carrier mobility–lifetime product, and X‐ray absorption coefficient, have emerged as exceptional candidates for the fabrication of high‐sensitivity X‐ray detectors. Herein, a BA2PbBr4/MAPbBr3 heterojunction is epitaxially grown, with ion migration effectively suppressed through the passivation of surface defects of the 3D heterojunction. Additionally, the presence of an internal electric field within the heterojunction facilitated the extraction and accumulation of photoinduced charge carriers, further enhancing device sensitivity (5964.05 μC Gy−1 cm−2). The fabricated 2D/3D perovskite heterojunction devices show outstanding self‐driven X‐ray detection performance at 0 V mm−1 bias (1195.5 μC Gy−1 cm−2), surpassing that of α‐Se detectors (20 μC Gy−1 cm−2). The proposed method for the fabrication of self‐driven detectors is relatively simple and is therefore expected to contribute to the commercialization of perovskite‐based X‐ray detectors.