Generation Of Free Electrons Research Articles

Simultaneous Structural and Electronic Engineering on Bi- and Rh-co-doped SrTiO3 for Promoting Photocatalytic Water Splitting.

Activating metal ion-doped oxides as visible-light-responsive photocatalysts requires intricate structural and electronic engineering, a task with inherent challenges. In this study, we employed a solid (template)-molten (dopants) reaction to synthesize Bi- and Rh-codoped SrTiO3 (SrTiO3 : Bi,Rh) particles. Our investigation reveals that SrTiO3 : Bi,Rh manifests as single-crystalline particles in a core (undoped)/shell (doped) structure. Furthermore, it exhibits a well-stabilized Rh3+ energy state for visible-light response without introducing undesirable trapping states. This precisely engineered structure and electronic configuration promoted the generation of high-concentration and long-lived free electrons, as well as facilitated their transfer to cocatalysts for H2 evolution. Impressively, SrTiO3 : Bi,Rh achieved an exceptional apparent quantum yield (AQY) of 18.9 % at 420 nm, setting a new benchmark among Rh-doped-based SrTiO3 materials. Furthermore, when integrated into an all-solid-state Z-Scheme system with Mo-doped BiVO4 and reduced graphene oxide, SrTiO3 : Bi,Rh enabled water splitting with an AQY of 7.1 % at 420 nm. This work underscores the significance of simultaneous structural and electronic engineering and introduces the solid-molten reaction as a viable approach for this purpose.

Highly Stable Solid Contact Calcium Ion-Selective Electrodes: Rapid Ion-Electron Transduction Triggered by Lipophilic Anions Participating in Redox Reactions of CunS Nanoflowers.

Solid contact (SC) calcium ion-selective electrodes (Ca2+-ISEs) have been widely applied in the analysis of water quality and body fluids by virtue of the unique advantages of easy operation and rapid response. However, the potential drift during the long-term stability test hinders their further practical applications. Designing novel redox SC layers with large capacitance and high hydrophobicity is a promising approach to stabilize the potential stability, meanwhile, exploring the transduction mechanism is also of great guiding significance for the precise design of SC layer materials. Herein, flower-like copper sulfide (CunS-50) composed of nanosheets is meticulously designed as the redox SC layer by modification with the surfactant (CTAB). The CunS-50-based Ca2+-ISE (CunS-50/Ca2+-ISE) demonstrates a near-Nernstian slope of 28.23 mV/dec for Ca2+ in a wide activity linear range of 10-7 to 10-1 M, with a low detection limit of 3.16 × 10-8 M. CunS-50/Ca2+-ISE possesses an extremely low potential drift of only 1.23 ± 0.13 μV/h in the long-term potential stability test. Notably, X-ray absorption fine-structure (XAFS) spectra and electrochemical experiments are adopted to elucidate the transduction mechanism that the lipophilic anion (TFPB-) participates in the redox reaction of CunS-50 at the solid-solid interface of ion-selective membrane (ISM) and redox inorganic SC layer (CunS-50), thereby promoting the generation of free electrons to accelerate ion-electron transduction. This work provides an in-depth comprehension of the transduction mechanism of the potentiometric response and an effective strategy for designing redox materials of ion-electron transduction triggered by lipophilic anions.

Interfacial carbon quantum dot thin film impacts on morphological and chemical structures of fluorine-doped tin oxide films

Morphology and chemical bonding states, including surface roughness, film density, F-doping, and oxygen vacancy (VO) concentration directly affect the electrical and optical properties of fluorine-doped tin oxide (FTO) films. In this study, morphology and chemical bonding states of FTO films are engineered simultaneously by introducing a carbon quantum dot (CQD) thin film as an interface layer during ultrasonic spray pyrolysis deposition. The abundant oxygen-containing surface functional groups and large surface free energy of the CQD thin film promoted (200) oriented crystal growth and accelerated nucleation of FTO, resulting in smooth and dense FTO film morphology. The abundant carboxyl surface functional groups on the CQDs generate active F− species that are effectively doped into SnO2. Formic acid, formed by dissociation of the carboxyl group, can serve as a strong reducing agent for extracting oxygen atoms from the SnO2 lattice, thereby increasing the VO concentration. The accelerated F-doping and VO concentration result in the generation of additional free electrons. The effects of the optimized CQD on the morphological and chemical structures of FTO films are demonstrated by their superior electrical (sheet resistance of ∼5.7 Ω/□) and optical properties (visible transmittance of ∼85.9 %) compared with bare FTO. Moreover, CQD/FTO used as transparent conducting electrodes in electrochromic (EC) application exhibited improved EC performances, including fast switching speeds (5.3 s and 2.3 s for bleaching and coloration, respectively) and high coloration efficiency (81.1 cm2/C) compared to that of bare FTO.

Negative bias stress stable PtOx/InGaZnOx Schottky barrier diodes optimized by oxygen annealing

In this work, bottom-Schottky-structure InGaZnOx (IGZO) Schottky barrier diodes (SBDs) with sputtered PtOx anodes were fabricated and annealed in oxygen at different temperatures. Critical parameters and negative bias stress (NBS) stability of SBDs with different annealing temperatures are investigated. With the annealing temperature increases, the barrier height and rectification ratio of the SBDs exhibited a rising-then-declining trend, while the ideality factor slightly increased until 200 °C. The SBDs show up overall reliability except for a leakage current rising trend under light, which can be attributed to free electron generation from the ionized oxygen vacancy. Among all the SBDs, the 175 °C annealed ones exhibited the best overall performance, including a high barrier height of 0.89 eV, an ideality factor of 1.14, and a large rectification ratio of over 108. Compared to the initial SBDs, the annealed ones showed up great improvement in NBS stability except for the 200 °C annealed ones, which was permanently degraded and not able to recover to original states. According to experimental result analysis and IGZO material characteristics, a stability model based on the subgap trap transition from VO2+ to VO and new VO2+ creation was proposed, which applies to both the short-term and long-term NBS tests. The results above demonstrate that oxygen annealing at appropriate temperature is an effective method to improve both device performance and NBS stability for PtOx–IGZO SBDs.

Study on Cs2AgIn(Cl1−xBrx)6 perovskite based on the balance of stability and optical absorption properties

The Cs2AgIn(Cl1−xBrx)6 (x = 0, 1/6, 1/3, 1/2, 2/3, 5/6, 1) lead-free perovskites show great advantages as a stable and non-toxic alternative to lead halide perovskite. In this study, Cs2AgIn(Cl1−xBrx)6 are treated by replacing Cl with Br in a stepwise manner to balance its stability and optical properties. Density functional theory is used to investigate the structural, electronic, and optical properties of Cs2AgIn(Cl1−xBrx)6. The results show that the doping of Br make the average bond length of metal-halides longer, resulting in an increase in volume. The value of the bandgap decreases from 3.168 eV to 2.095 eV. The decomposition energy (−92.3365 to −70.4435 meV/atom) of the material gradually increases, the stability decreases gently (−92.3365 to −90.934 meV/atom, Δ0–1/2 = 0.4675) when the amount of Br doping is less than 1/2, and it decreases significantly (−90.934 to −70.4435 meV/atom, Δ1/2–1 = 6.83) when it exceeds 1/2. The partial density of states reveal that the electronic contribution is mainly related to the [AgX6]5- (X = Cl, Br) octahedral. The analysis of charge density indicates that partially or completely replacing Cl with Br is beneficial for the generation of free electrons, which may improve its photoelectric performance. The analysis of the complex dielectric function and the optical absorption coefficient shows a more significant increase in the absorption coefficient when half of the Br is incorporated compared to full substitution. According to our results, adjusting x in Cs2AgIn(Cl1−xBrx)6 can expand the material's range of spectroscopic applications. Based on the trade-off between stability and light absorbance, Cs2AgInCl3Br3 exhibits the best overall performance.

Effect of zinc on structural, dielectric, ferroelectric, and optical properties of Ba(Fe1/2V1/2)O3 complex perovskite ceramic

The synthesis and characterization (structure, dielectric, electrical, and optical properties) of Ba1-xZnx(Fe1/2V1/2)O3(x = 0,0.05,0.10,0.15) have been reported in this paper. The development of a single-phase orthorhombic structure has been confirmed by analyzing room temperature X-rays diffraction (XRD) patterns/data. The crystallite size decreases with an increase in the concentration of Zn2+. Different vibration modes are confirmed from Raman Spectroscopy. Analysis of FESEM microstructure confirms the reduction in average grain size with increased Zn2+ concentration. Some electrical parameters (dielectric constant, conductivity, and impedance) have provided valuable data on the conduction mechanism, structure-properties relationship, etc. The non-Debye relaxation is confirmed from the Nyquist plot. It also ensures the grain boundary and the bulk effect of the materials. The coercive field and efficiency are maximum (7.419 kV/cm, 60.83%) for the higher concentration of Zn2+(x = 0.15). The direct band gap varies from 3.28 to 3.10 eV with increasing Zn2+ concentration. It confirms the generation of more free electrons in the conduction band and high conductivity.

Static and transient optical properties of thin film indium tin oxide during laser excitation

The mechanisms of ultrafast laser-induced free electron generation and the effect of the free electrons on the transient optical properties in indium tin oxide is investigated by means of numerically solving rate equations and ultrafast transient experiments. A dynamical model for the transient optical properties of indium tin oxide thin films during excitation with an ultrashort laser pulse with fluences between 0.4 J cm−2 to 2.3 J cm−2 is developed and compared to pump probe microscopy during and after excitation with laser pulses. In the non-excited case, thin film interferences dominate the shape of the reflection spectrum. During laser excitation, (quasi-)free electron dynamics drastically alter the optical properties. The temporal evolution of the (quasi-)free electron density is numerically computed using rate equations for irradiation with laser pulses with various peak fluences for a pulse duration of 700 fs and a central wavelength of 1056 nm. We found that a thermal ionization term that takes electronic states within the band gap into account has to be considered to reproduce the reflectivities obtained by pump probe measurements. Additionally, we found that cascade ionization dominates the multiphoton ionization for indium tin oxide.

Marine Colloids Promote the Adaptation of Diatoms to Nitrate Contamination by Directional Electron Transfer.

Nitrate contamination from human activities (e.g., domestic pollution, livestock breeding, and fertilizer application) threatens marine ecosystems and net primary productivity. As the main component of primary productivity, diatoms can adapt to high nitrate environments, but the mechanism is unclear. We found that electron transfer from marine colloids to diatoms enhances nitrogen uptake and assimilation under visible-light irradiation, providing a new pathway for nitrogen adaptation. Under irradiation, marine colloids exhibit semiconductor properties (e.g., the separation of electron-hole pairs) and can trigger the generation of free electrons and singlet oxygen. They also exhibit electron acceptor and donor properties, with the former being stronger than the latter, reacting with polysaccharides in extracellular polymeric substances (EPSs) under high nitrogen stress, enhancing the elasticity and permeability of cells, and promoting nitrogen assimilation and electron transfer to marine diatom EPSs. Electron transfer promotes extracellular-to-intracellular nitrate transport by upregulating membrane nitrate transporters and nitrate reductase. The upregulation of anion transport genes and unsaturated fatty acids contributes to nitrogen assimilation. We estimate that colloids may increase the nitrate uptake efficiency of marine diatoms by 10.5-82.2%. These findings reveal a mechanism by which diatoms adapt to nitrate contamination and indicate a low-cost strategy to control marine pollution.

Multi-Pass Free Electron Laser Assisted Spectral and Imaging Applications in the Terahertz/Far-IR Range Using the Future Superconducting Electron Source BriXSinO

Free-Electron Lasers are a rapidly growing field for advanced science and applications, and worldwide facilities for intense field generation, characterization and usage are becoming increasingly popular due to their peculiarities, including extremely bright, coherent, wide band tunable ultra-short pulses which are not achievable with other techniques up to now. In this review we give a thorough survey of the latest advances in the Free-Electron Laser-based field generation and detection methodologies and then present the main characteristics of a future THz/IR source, named TerRa@BriXSinO, based on a superconducting linear accelerator. The foreseen source is strongly monochromatic, with a bandwidth of 1% or smaller, highly coherent both transversally and longitudinally, with extreme versatility and high frequency tunability. After introducing the most recent and novel FEL-assisted scientific investigations, including fundamental explorations into complex systems and time-dependent interactions and material dynamics, we present our vision on the potential use of the TerRa facility and analyze some possible applications, ranging from non-linear physics under extreme conditions to polarization sensitive imaging and metamaterial-based sensing.

Smart Surfaces: Photocatalytic Degradation of Priority Pollutants on TiO2-Based Coatings in Indoor and Outdoor Environments-Principles and Mechanisms.

Heterogeneous photocatalysis using semiconductor oxides such as TiO2, provides an up-and-coming solution for the degradation of environmental pollutants compared with other technologies. TiO2-containing construction materials and paints activated by UV/solar light destroy the ozone precursors NO and NO2 up to 80% and 30%, respectively. The majority of TiO2 materials developed so far are primarily for outdoor use. In recent years, substantial efforts have been made to investigate further the photocatalytic activity of materials containing TiO2 toward priority air pollutants such as NO, NO2, and volatile organic compounds (VOCs) frequently accumulated at high concentration levels, particularly in indoor spaces. The intention of the investigations was to modify the titanium dioxide (TiO2), so that it may be activated by visible light and subsequently used as additive in building envelop materials and indoor paints. This has been achieved, to a high extent, through doping of TiO2 with transition metals such as V, Cr, Fe, Mn, Ni, Co, Cu, and Zn, which reduce the energy gap of TiO2, facilitating the generation of free electrons and holes, thus, extending the absorption spectral range of modified TiO2 to the area of visible light (bathochromic shift-redshift). A substantial problem using TiO2-containing paints and other building materials in indoor environments is the formation of byproducts, e.g., formaldehyde, through the heterogeneous photocatalytic reaction of TiO2 with organic matrices. This affects the air quality in confined spaces and, thus, becomes a possible risk for human health and wellbeing. This work describes the principles and mechanisms of the photocatalytic reactions at the air/catalyst interface of priority pollutants such as NO, benzene, and toluene as individual compounds or mixtures. Emphasis is placed on the reaction and recombination processes of the charge carriers, valence band positive holes (h+) and free electrons (e−), on the surface of TiO2, and on key factors affecting the photocatalytic processes, such as humidity. A hypothesis on the role of aromatic compounds in suppressing the recombination process (h+ and e−) is formulated and discussed. Furthermore, the results of the photocatalytic degradation of NO under visible light conditions using different admixtures of TiO2 and manganese doped (Mn–TiO2) are presented and discussed.

Critical study of partial discharge inception in voids: statistical behavior to stochastic nature

Although many studies have been done and advanced progress has been made in understanding partial discharge (PD) behavior in the void, this is not the case firinception of PD, especially its stochastic nature. The statistical behaviors of PD inception voltage (PDIV) and inception time delay (PDTD) inside the void were investigated in this study through repeated tests to observe the stochastic nature of PD inception. The results show that the PDIV and PDTD of the void are highly dispersed and obey Weibull and exponential distributions, respectively. The significant dispersion of PDIV can be attributed to the statistical time delay of PD inception. The lengthy inception delay is attributable to a lack of free electrons. The exponential distribution of PDTD indicates that free-electron generation is completely random; further, the stochastic nature of void PD inception is determined by the supply of free electrons. The test method (voltage rise rate, test time, and test time interval), void parameters (size, material, and surface condition), and background radiation determine PD inception by affecting the volume ionization or surface-emission process providing free electrons. Enhanced background ionization or significant increase in test voltage and test time allow for the effective detection of void defects during PD tests. This work contributes to an empirical understanding of the physical process of PD inception in voids and improving existing PD testing technologies.

The influence of Mn doping on the leakage current mechanisms and resistance degradation behavior in lead zirconate titanate films

The electrical reliability of lead zirconate titanate (PZT) films was improved by incorporating Mn; the time dependent dielectric breakdown lifetimes and the associated activation energy both remarkably increased with Mn concentration. The correlation between the defect chemistry and the resistance degradation was studied to understand the physical mechanism(s) responsible for enhanced electrical reliability. At lower electric fields, Poole-Frenkel emission was responsible for the leakage current. Beyond a threshold electric field, Schottky emission controlled the leakage. After electrical degradation of a 2 mol.% Mn doped PZT film, no significant change in potential barrier height for injecting electrons from the cathode into the anode was observed. This suggests that the degradation is mostly controlled by Poole-Frenkel conduction via some combination of hole migration between lead vacancies, small polaron hopping between Mn sites, and hole hopping between Pb2+ and Pb3+. No variation in the valence state of Ti near the cathode was observed in degraded Mn doped PZT films, implying that multivalent Mn provides trap sites for electrons and holes; free electron generation due to compensation of oxygen vacancies at the cathode and free hole formation at the anode region might be suppressed by the valence changes from Mn3+ to Mn2+ and Mn2+ to Mn3+ respectively.

Asymmetries in ionization of atomic superposition states by ultrashort laser pulses

Progress in ultrafast science allows for probing quantum superposition states with ultrashort laser pulses in the new regime where several linear and nonlinear ionization pathways compete. Interferences of pathways can be observed in the photoelectron angular distribution and in the past they have been analyzed for atoms and molecules in a single quantum state via anisotropy and asymmetry parameters. Those conventional parameters, however, do not provide comprehensive tools for probing superposition states in the emerging research area of bright and ultrashort light sources, such as free-electron lasers and high-order harmonic generation. We propose a new set of generalized asymmetry parameters which are sensitive to interference effects in the photoionization and the interplay of competing pathways as the laser pulse duration is shortened and the laser intensity is increased. The relevance of the parameters is demonstrated using results of state-of-the-art numerical solutions of the time-dependent Schrödinger equation for ionization of helium atom and neon atom.

Looking at Electron Dynamics to Better Understand Photo-Active Materials

The generation of free and energetic electrons is the key to the next generation of photo-voltaic and photo-catalysts. In order to produce such electrons, the sunlight is so far the most promising sustainable source of energy. However, the conversion efficiency from light to the liberation of a functional electron depends on numerous factors and processes that are difficult to account for. One of the reasons is the difficulty of monitoring the early electron dynamics such as the charge separation event and the subsequent electronic relaxation and migration. Here, I propose the use of ultrafast transient absorption spectroscopy to watch these electronic events “live” in the femto- to nano-seconds (10-15-10-9 sec.) time scales. In this presentation, I will demonstrate this technique on iron and copper oxides thin films. In this study, we produce ultrashort laser pulses to mimic sunlight and trigger charge separations that ultimately lead to the generation of the reactive oxygen species that confer the films their antibacterial properties. With this technique, we are able to harvest information such as the charge separation efficiency, electron dynamics, excited state’s bandgap energy, and even material deformation upon photo-excitation, all of which are key to understand, control and enhance the conversion process.

Femtosecond Plasmonic Laser Nanosurgery (fs-PLN) mediated by molecularly targeted gold nanospheres at ultra-low pulse fluences

Plasmonic Laser Nanosurgery (PLN) is a novel photomodification technique that exploits the near-field enhancement of femtosecond (fs) laser pulses in the vicinity of gold nanoparticles. While prior studies have shown the advantages of fs-PLN to modify cells, further reduction in the pulse fluence needed to initiate photomodification is crucial to facilitate deep–tissue treatments. This work presents an in-depth study of fs-PLN at ultra-low pulse fluences using 47 nm gold nanoparticles, conjugated to antibodies that target the epithelial growth factor receptor and excited off-resonance using 760 nm, 270 fs laser pulses at 80 MHz repetition rate. We find that fs-PLN can optoporate cellular membranes with pulse fluences as low as 1.3 mJ/cm2, up to two orders of magnitude lower than those used at lower repetition rates. Our results, corroborated by simulations of free-electron generation by particle photoemission and photoionization of the surrounding water, shed light on the off-resonance fs-PLN mechanism. We suggest that photo-chemical pathways likely drive cellular optoporation and cell damage at these off-resonance, low fluence, and high repetition rate fs-laser pulses, with clusters acting as local concentrators of ROS generation. We believe that the low fluence and highly localized ROS-mediated fs-PLN approach will enable targeted therapeutics and cancer treatment.

Sensing the Generation of Intracellular Free Electrons Using the Inactive Catalytic Subunit of Cytochrome P450s as a Sink.

Cytochrome P450 reductase (CPR) abstracts electrons from Nicotinamide adenine dinucleotide phosphate H (NADPH), transferring them to an active Cytochrome P450 (CYP) site to provide a functional CYP. In the present study, a yeast strain was genetically engineered to delete the endogenous CPR gene. A human CYP expressed in a CPR-null (yRD−) strain was inactive. It was queried if Bax—which induces apoptosis in yeast and human cells by generating reactive oxygen species (ROS)—substituted for the absence of CPR. Since Bax-generated ROS stems from an initial release of electrons, is it possible for these released electrons to be captured by an inactive CYP to make it active once again? In this study, yeast cells that did not contain any CPR activity (i.e., because the yeasts’ CPR gene was completely deleted) were used to show that (a) human CYPs produced within CPR-null (yRD-) yeast cells were inactive and (b) low levels of the pro-apoptotic human Bax protein could activate inactive human CYPs within this yeast cells. Surprisingly, Bax activated three inactive CYP proteins, confirming that it could compensate for CPR’s absence within yeast cells. These findings could be useful in research, development of bioassays, bioreactors, biosensors, and disease diagnosis, among others.

Mechanism insight of dual synergistic effects of plasmonic Pd-SrTiO3 for enhanced solar energy photocatalysis

This study presents the integration of UV-active semiconductor with plasmonic noble metal nanoparticles for enhanced solar energy photocatalysis. Nanocubes strontium titanate (SrTiO3) is synthesized via a simple hydrothermal process. Then palladium (Pd) nanoparticles will be deposited onto the surface of SrTiO3 by simple photochemical deposition route. The deposition of plasmonic Pd nanoparticles significantly increased the light absorption, especially in visible and near-infrared region and enhanced charge separation efficiency. The photocatalytic performance of Pd-deposited SrTiO3 is assessed by photodegradation of bisphenol A (BPA) and 4-chlorophenol (4CP) under solar light. The results confirm that the existence of Pd nanoparticles in SrTiO3 has improved the photocatalysis efficiency compared to pure SrTiO3. The higher weight percentage of Pd loading achieved better photocatalytic performance compared to lower weight percentage of Pd loading. This improvement can be deduced from the dual localized surface plasmon resonance effects that led to higher photoresponse and generation of free electrons. Moreover, the existence of Pd nanoparticles further retards the recombination rate of electron and hole pairs. This leads to the excess presence of electrons that contributed to the formation of active radicals that enhanced the oxidation of BPA and 4CP. Thus, this study will provide a new mechanism insight and approach to modify visible and near-infrared light-driven photocatalysts in degrading various organic pollutants.

Controllable photon energy deposition efficiency in laser processing of fused silica by temporally shaped femtosecond pulse: Experimental and theoretical study

Photon energy deposition plays a crucial role in femtosecond laser irradiation followed by chemical etching processing, which is an emerging technique for the better control of micro/nano structures on fused silica. In this study, we have experimentally and theoretically studied the controllable photon energy deposition in laser irradiation of fused silica by temporally shaped femtosecond laser pulse trains. The experimental result shows that the photon energy deposition efficiency could be either reduced or enhanced by adjusting the total fluence of shaped pulse trains. Furthermore, the sub-pulse interval and intensity ratio of temporally shaped pulse trains were revealed to play a critical role in photon energy deposition. The corresponding experimental observations are qualitatively explained by a plasma model that considers the free electron generation processes and corresponding feedback on the photon energy deposition.

Unified model of field assisted sintering and related phenomena

Critical elements of the model are temperature-assisted generation of free electrons, field-assisted transport and trapping of free electrons to generate defects, segregation of defects to dislocations and grain boundaries through elastic and electrostatic interactions, and creation of percolation paths along grain boundaries. There is a critical electric field required to establish these percolation paths, where free electrons-defects-free electrons bootstrapping avalanche occurs, leading to selective Joule heating and localized melting to achieve near theoretical density. The critical field for percolation is a function of microstructure, temperature and time (incubation period), and it is much higher for single crystals than polycrystalline materials.

Charge Transfer Processes in a Sodium-Doped Carbon Composite Based on Fullerenes and Thermally Exfoliated Graphite

The results of doping of a carbon composite material, in which fullerenes are located in a conductive matrix based on thermally exfoliated graphite, with a sodium dopant are presented. Charge transfer processes taking place in samples with different initial ratios of components are studied. It turns out that the electrical resistivity of the samples increases with the introduction of sodium and an increase in its content, since the mobility of the main charge carriers, which are holes as in the undoped material, decreases. The concentration of charge carriers in different types of samples varies in both directions and can increase by more than an order of magnitude. It is concluded that Na plays an ambiguous role. It can contribute not only to the generation of free electrons, but also to an additional increase in the concentration of various defects that can generate free holes and can affect, being effective traps and scattering centers, all types of charge carriers.