Types Of Charge Carriers Research Articles

An ambipolar single-charge pump in silicon

The mechanism of single-charge pumping using a dynamic quantum dot needs to be precisely understood for high-accuracy and universal operation toward applications to quantum current standards and quantum information devices. The type of charge carrier (electron or hole) is an important factor for determining the pumping accuracy, but it has been so far compared just using different devices that could have different potential landscapes. Here, we report measurements of a silicon ambipolar single-charge pump. It allows a comparison between the single-electron and single-hole pumps that share the entrance tunnel barrier, which is a critical part of the pumping operation. By changing the frequency and temperature, we reveal that the entrance barrier has a better energy selectivity in the single-hole pumping, leading to a pumping error rate better than that in the single-electron pumping up to 400 MHz. This result implies that the heavy effective mass of holes is related to the superior characteristics in the single-hole pumping, which would be an important finding for stably realizing accurate single-charge pumping operation.

Gate induced metallicity and absence of superconductivity in BSTO/LCO heterostructure

We fabricated Ba0.8Sr0.2TiO3 (BSTO)/La2CuO4 (LCO) heterostructure on SrTiO3 (STO) substrate and investigated its structure and physical properties. X-ray diffraction and reciprocal space mapping confirm the epitaxial growth of BSTO/LCO/STO heterostructure. X-ray photoelectron spectroscopy and UV–Visible spectroscopy measurements reveal a straddling band alignment of the BSTO/LCO heterojunction. Such band alignment facilitates the accumulation of both electrons and holes at the interface. Their movement depends on the direction of the internal field of the BSTO film. Electrical transport measurements have revealed a signature of insulator-to-metal transition (IMT) in response to applied gate voltages ±Vg. Hall measurements confirm the presence of electron and hole type charge carriers under ＋Vg and −Vg, respectively. We have proposed a screening mechanism linked to the polarization state of the BSTO film to explain the observed IMT.

The effect of A-site cations on charge-carrier mobility in Fe-rich amphiboles

Abstract Elucidating the high-temperature behavior of rock-forming minerals such as amphiboles (AB2C5 T8O22W2) is critical for the understanding of large-scale geological processes in the lithosphere and, in particular, the development of high conductivity in the Earth’s interior. Recently, we have shown that at elevated temperatures, CFe-bearing amphiboles with a vacant A site develop two types of charge carriers: (1) small polarons and (2) delocalized H+ ions. To elucidate the effect of A-site cations on the formation and stability of charge carriers within the amphibole structure, here we analyzed synthetic potassic-ferro-richterite as a model Fe-rich amphibole with a fully occupied A site via in situ temperature-dependent Raman spectroscopy. We further compare the results from in situ time-dependent Raman-scattering experiments on pre-heated and rapidly quenched potassic-ferro-richterite and riebeckite as a model Fe-rich amphibole with a vacant A site. We show that the presence of A-site cations (1) reduces the activation temperature of mobile polarons and delocalized H+ cations; (2) decreases the magnitude of the polaron dipole moment; (3) slows down the process of re-localization of electrons on cooling; and (4) makes the electrons inert to rapid change in external conditions, supporting the persistence of a metastable state of pre-activated delocalized electrons even at room temperature. Our results have important geological implications demonstrating that the A-site cations may control the depth of development of high conductivity in subducted amphibole-bearing rocks. Moreover, from the viewpoint of mineral-inspired materials science, our results suggest that the amphibole-structure type has great potential for designing functional materials with tunable anisotropic-conductivity properties.

Influence of non-linear diffusion controlled phenomena on the sorption capability of PEO-Salt-SiO2 composite electrolyte: A study on property optimization

The present research, reports the hygrothermal behavior of poly [ethylene oxide] (PEO) based composite film (500 and1000 μm) containing NH4I and KBr (5–20 wt%) as the mobile phase and non-reactive silica (15 wt%) as the filler. These are termed as PK/NSiO2-series for solvent sorbed and (PK/NSiO2)NS for non-swelled film. The novelty of the research lies in the analyses of non-Fickian solvent diffusion trait of films using python programming. The presence of ions and its variable polarizable nature is found to influence the number density of bonded and free solvent content along with the extend of cross linkage. Introduction of silica is found to enhance the ionic conductivity (about one order higher) of the film irrespective of the type of charge carrier owing to the improved dispersion within the matrix. Non-Fickian diffusion is found to influence the ionic conductivity of P2K20SiO2 (10−5Scm−1 to 10−2 Scm−1) minimizing the degradation to 0.2 %ΔC/1000 h (>1 %ΔC/1000 h, tested for 2000 h) compared to P2N20NSiO2. In contrast, ion migration in P2NSiO2 is guided by Rice and Roth model and being more polarizable ions, the mobility is significant which maximizes the conductivity to ∼10−1 Scm−1. Microstructural study shows heterogenous nucleation to be more pronounced upon addition of silica filler wherein the homogeneity, inter fibrillar interaction and grain growth of spherulites is higher. This tends to extend amorphous regions thereby propagating the ion migration path. The influence of sorption process is studied in terms of electrochemical impedance, dielectric analyses and long term cyclability (20,000 h) in terms of loss tangent.

(Invited) Electronic Doping in Two-Dimensional Semiconductors

Quantum-confined semiconductors provide highly tunable optical and electrical properties for a wide variety of emerging applications. Two-dimensional semiconductors possess tunable bandgaps, high charge carrier mobilities, and strong light-matter interactions that can enable applications in photovoltaics, quantum information processing, and spintronics. Electronic doping, the intentional introduction of controlled charge carrier density and type (electrons or holes) is a fundamental enabler for many emerging applications of two-dimensional semiconductors. While electrostatic doping in transistor geometries is useful for certain applications, it is important to develop additional methods based on e.g. molecular redox doping and substitutional atomic doping that can provide tunable Fermi level control in the absence of an applied bias. In this presentation, I will discuss our efforts to develop such doping strategies for a variety of two-dimensional semiconductors. I will discuss how electronic doping modulates opto-electronic properties, including ground-state absorbance, charge transport, and excited-state dynamics in these 2D semiconductors. These studies provide fundamental insights into the degree to which molecular and substitutional doping strategies can modulate Fermi level, charge transport, and excitonic optical transitions in 2D semiconductors.

Nanostructuring of AlSiCrMnFeNiCu High‐Entropy Alloy via Cryomilling: Exploring Structural, Magnetic, and Thermoelectric Properties

Efforts are made to understand the influence of milling intensity on structure, morphology, magnetic and thermoelectric properties of nonequiatomic nanostructured AlSiCrMnFeNiCu high‐entropy alloy (HEA) powders prepared by cryomilling. These powders are cryomilled with different ball‐to‐powder ratios (BPR) and present a dual‐phase structure containing a major B2‐type and a minor Cr5Si3‐type phase. An increase in BPR enhances the refinement of crystallite size, grain size, and particle size accompanied by a decrease in the phase fraction of the minor Cr5Si3‐type phase. Magnetic measurements revealed that at room temperature, sufficient increase in BPR leads to a transition from multi‐domain behavior to single‐domain behavior which leads to enhancement in soft magnetic properties. Thermal measurements show the presence of different magnetic phase transitions which vary with an increase in BPR. A change of charge carrier type from p to n‐type was observed as the grain size is reduced. The figure of merit decreases with the decrease in grain size from 2 × 10–5 for as‐cast powders and is lowest for the smallest grain‐sized sample due to a decrease in electrical conductivity. This study shows the possibility of exploring nonequiatomic low‐density HEAs whose functional properties can be tailored, offering flexibility in material design for specific applications.

Identification of the conductivity type of single-walled carbon nanotubes via dual-modulation dielectric force microscopy.

The conductivity type is one of the most fundamental transport properties of semiconductors, which is usually identified by fabricating the field-effect transistor, the Hall-effect device, etc. However, it is challenging to obtain an Ohmic contact if the sample is down to nanometer-scale because of the small size and intrinsic heterogeneity. Noncontact dielectric force microscopy (DFM) can identify the conductivity type of the sample by applying a DC gate voltage to the tip, which is effective in tuning the accumulation or depletion of charge carriers. Here, we further developed a dual-modulation DFM, which simplified the conductivity type identification from multiple scan times under different DC gate voltages to a single scan under an AC gate voltage. Taking single-walled carbon nanotubes as testing samples, the semiconducting-type sample exhibits a more significant charge carrier accumulation/depletion under each half-period of the AC gate voltage than the metallic-type sample due to the stronger rectification effect. The charge carrier accumulation or depletion of the p-type sample is opposite to that of the n-type sample at the same half-period of the AC gate voltage because of the reversed charge carrier type.

Dual Exciton Polarization in Bipolar CeO2-x Nanocrystals Controlled by Defect-Based Redox Processes.

Discovering alternative means to control electronic states in semiconductor nanostructures is the key to the development of new quantum technologies. Controlling the cyclotron motion of free charge carriers in semiconductor nanocrystals using an external magnetic field generates a tunable angular momentum, as a collective electronic degree of freedom, which can be imparted to the electronic band states to achieve complete exciton polarization. The sign of this polarization is determined by the type of majority charge carriers in a given lattice. Using magnetic circular dichroism spectroscopy, we demonstrate a simultaneous polarization of excitonic states in substoichiometric oxygen-deficient CeO2-x nanocrystals associated with electrons and holes, which can be controlled by the thermal treatment of colloidal nanocrystals in oxidizing or reducing conditions. The presence of both occupied and unoccupied midgap states, due to Ce3+ 4f and Ce4+ 4f orbitals, respectively, allows for selective probing of the effect of holes in the valence band (VB → Ce4+ 4f) and electrons in the conduction band (Ce3+ 4f → CB). The two transitions show the opposite sign at 300 K due to the opposite angular momenta associated with cyclotron electrons and holes. The ability to manipulate Ce 4f-derived midgap states by defect formation during the synthesis or postsynthesis treatment allows for a range of new technological applications of CeO2-x nanocrystals in optoelectronics.

Effect of niobium doping on excitonic dynamics in MoSe2

Transition metal dichalcogenides (TMDs) have emerged as attractive two-dimensional semiconductors for future electronic and optoelectronic applications. Their charge transport properties, such as conductivity and the type of charge carriers, can be effectively controlled by substitutional doping of the transition metal atoms. However, the effects of doping on the excitonic properties, particularly their dynamical properties, have been less studied. Using Nb-doped MoSe2 as a case study, we experimentally investigate the effect of doping on excitonic dynamics in TMDs. Transient absorption measurements are used to directly compare the dynamical properties of excitons in Nb-doped MoSe2 across monolayer, bilayer, and bulk flakes with their undoped counterparts. The exciton lifetimes in Nb-doped flakes are significantly shorter than those in their undoped counterparts. This effect is attributed to the trapping of excitons in defect states introduced by Nb impurities. These results reveal an important consequence of Nb doping on excitonic dynamics in TMDs.

Correlation between morphology and transport properties of Au/Co/Au/Si wedge ultra-thin film

We report the thermoelectric power (TEP) and electrical resistivity characterization supported by structural and surface morphological properties on a wedge shaped ultra-thin sample of Au/Co/Au/Si (100) with Co have varying thickness from 0.5 nm to 4 nm across the sample. The sample was prepared by Ion Beam Sputtering method, with an ultrathin layer of Co sandwiched between two layers of Au (3 nm thicknesses each). The observed TEP results showed that the system is semiconductor in nature and the concentration of the charge carrier is inversely proportional to the Seebeck coefficient (S) and also concentration of charge carrier modifies with the film thickness leading to a change in thermo power, which is found to be higher at lower thicknesses of Co sandwiched layer. The type of charge carrier was also determined to be electrons in this system. The observed results are in good agreement with the resistivity measurement carried out as a function of film thickness indicating a decrease in resistivity as a function of film thickness due to enhancement in charge carrier mobility. The thermal activation energy was seen to increase from ∼29.5 meV to ∼280.3 meV as the film thickness increased from the minimum to the highest. Corresponding Atomic Force Microscopy (AFM) measurement revealed island type grain growth with the introduction of a significant amount of roughness, while Magnetic Force Microscopy (MFM) experiments exhibit randomly oriented magnetic domain structures. The overall results suggest that lowest thickness film shows semiconducting nature, while variable range hopping phenomena due to some localized energy levels near the valence and conduction band is observed in the highest thickness film. This result is also well supported by XRD measurement, which revealed crystalline nature of the films. Such low cost, easy to fabricate materials may find applications in Peltier cooling or energy harvesting applications without the harmful carbon dioxide emission. For this, advance experiments will be done in future.

Transport properties and electronic phase transitions in two-dimensional tellurium at high pressure

Utilizing in situ Raman spectroscopy, resistivity, and Hall-effect measurements, we conducted an extensive investigation on the continuous electronic phase transitions and transport properties of two-dimensional (2D) tellurium (Te) under high pressure at room and low temperature (80–300 K). The distinguishable decrease in the A1 Raman mode's full width at half maximum in the trigonal phase (Te-I) indicated an electronic phase transition at 2.2 GPa. The following Hall-effect experiments located the Lifshitz transition and the semiconductor-semimetal transition at 0.9 and 1.9 GPa, respectively, and the semiconductor-semimetal transition was also confirmed by resistivity variation through temperature. The charge carrier types of the Te changed from hole to electron during the phase transition from Te-I to Te-II (triclinic phase) at low temperature, while the transport parameters remained almost unchanged during the phase transition from Te-II to Te-III (monoclinic phase). The results offered complete and thorough electronic phase transitions and transport characteristics of 2D Te, hence great advancing the potential application of Te in electronic devices.

Modulating the majority charge carrier type and performance of organic heterojunction ammonia sensors by increasing peripheral fluorination of the silicon phthalocyanine sublayer

Silicon phthalocyanines (R2-SiPcs) are an emerging class of high-performance organic semiconductors which have recently found application in highly sensitive and selective bilayer organic heterojunction devices for ammonia (NH3) sensing. We report bilayer heterojunction devices based on axially-substituted bis(pentafluorophenoxy)silicon phthalocyanines of increasing peripheral fluorination ((F5PhO)2-FXSiPc) as a bottom layer and lutetium bis-phthalocyanine (LuPc2) and demonstrate how increased peripheral fluorination changes device operation from p-type to n-type in response to NH3. Sensors fabricated with (F5PhO)2-F16SiPc exhibits the smallest apparent energy barrier for interfacial charge transport by impedance spectroscopy due to better alignment of the semiconductor molecular orbitals with the semi-occupied molecular orbital of LuPc2. Bilayer heterojunction devices all demonstrated a limit of detection (LOD) below 1 ppm with (F5PhO)2-SiPc/LuPc2 yielding an LOD of 307 ppb and a sensitivity of −0.72%·ppm−1. Postdeposition thermal annealing of the (F5PhO)2-SiPc/LuPc2 device is shown to further enhance sensor performance with a 1.5-fold increase in sensitivity to −1.15%·ppm−1 and a LOD of 198 ppb.

Controllable Modulation of the Electronic Properties of a Two-Dimensional Ambipolar Semiconductor by Interface Ferroelectric Polarization.

Precise control of charge carrier type and density of two-dimensional (2D) ambipolar semiconductors is the prerequisite for their applications in next-generation integrated circuits and electronic devices. Here, by fabricating a heterointerface between a 2D ambipolar semiconductor (hydrogenated germanene, GeH) and a ferroelectric substrate (PbMg1/3Nb2/3O3-PbTiO3, PMN-PT), fine-tuning of charge carrier type and density of GeH is achieved. Due to ambipolar properties, proper band gap, and high carrier mobility of GeH, by applying the opposite local bias (±8 V), a lateral polarization in GeH is constructed with a change of work function by 0.6 eV. Besides, the built-in polarization in GeH nanoflake could promote the separation of photoexcited electron-hole pairs, which lead to 4 times enhancement of the photoconductivity after poling by 200 V. In addition, a gradient regulation of the work function of GeH from 4.94 to 5.21 eV by adjusting the local substrate polarization is demonstrated, which could be used for data storage at the micrometer size by forming p-n homojunctions. This work of constructing such heterointerfaces provides a pathway for applying 2D ambipolar semiconductors in nonvolatile memory devices, photoelectronic devices, and next-generation integrated circuit.

Pattern-illumination time-resolved phase microscopy and its applications for photocatalytic and photovoltaic materials.

Pattern-illumination time-resolved phase microscopy (PI-PM) is a technique used to study the microscopic charge carrier dynamics in photocatalytic and photovoltaic materials. The method involves illuminating a sample with a pump light pattern, which generates charge carriers and they decay subsequently due to trapping, recombination, and transfer processes. The distribution of photo-excited charge carriers is observed through refractive index changes using phase-contrast imaging. In the PI-PM method, the sensitivity of the refractive index change is enhanced by adjusting the focus position, the method takes advantage of photo-excited charge carriers to observe non-radiative processes, such as charge diffusion, trapping in defect/surface states, and interfacial charge transfer of photocatalytic and photovoltaic reactions. The quality of the image sequence is recovered using various informatics calculations. Categorizing and mapping different types of charge carriers based on their response profiles using clustering analysis provides spatial information on charge carrier types and the identification of local sites for efficient and inefficient photo-induced reactions, providing valuable information for the design and optimization of photocatalytic materials such as the cocatalyst effect.

CuO:V2O5 driven alterations in dielectric, ferroelectric and structural properties of Barium Zirconate Titanate ceramics

This study focuses on the properties of Vanadium and Copper co-doped Barium Zirconate Titanate (BZT) for potential technological applications. Various doping ratios of CuO:V2O5 were used to synthesize the materials, and X-ray diffraction (XRD) confirmed a tetragonal phase in all samples. The grain density and dimensions decreased with higher concentrations of V2O5 and CuO. FTIR spectra confirmed the compositional structure and bonding of the samples. The impedance analysis indicated that higher doping concentrations facilitated charge conduction at grain boundaries. Dielectric relaxation was studied using the Havriliak–Negami model and electrical modulus behavior was analyzed. Activation energy values from Arrhenius fitting matched those from impedance data, suggesting the same type of charge carriers. The study revealed that elevated levels of V concentration induced charge carriers to exhibit hopping behavior, thereby enhancing conductivity. Conversely, higher Cu concentration impeded hopping, leading to a swift rise in activation energy.

Pressure-Induced Superconductivity and Topological Quantum Phase Transitions in the Topological Semimetal ZrTe2.

Topological transition metal dichalcogenides (TMDCs) have attracted much attention due to their potential applications in spintronics and quantum computations. In this work, the structural and electronic properties of topological TMDCs candidate ZrTe2 are systematically investigated under high pressure. A pressure-induced Lifshitz transition is evidenced by the change of charge carrier type as well as the Fermi surface. Superconductivity is observed at around 8.3GPa without structural phase transition. A typical dome-shape phase diagram is obtained with the maximum Tc of 5.6K for ZrTe2 . Furthermore, the theoretical calculations suggest the presence of multiple pressure-induced topological quantum phase transitions, which coexists with emergence of superconductivity. The results demonstrate that ZrTe2 with nontrivial topology of electronic states displays new ground states upon compression.

Coexistent, Competing Tunnelling, and Hopping Charge Transport in Compressed Metal Nanocluster Crystals.

Understanding charge transport among metal particles with sizes of approximately 1 nm poses a great challenge due to the ultrasmall nanosize, yet it holds great significance in the development of innovative materials as substitutes for traditional semiconductors, which are insulative and unstable in less than ∼10 nm thickness. Herein, atomically precise gold nanoclusters with well-defined compositions and structures were investigated to establish a mathematical relation between conductivity and interparticle distance. This was accomplished using high-pressure in situ resistance characterizations, synchrotron X-ray diffraction (XRD), and the Murnaghan equation of state. Based on this precise correlation, it was predicted that the conductivity of Au25(SNap)18 (SNap: 1-naphthalenethiolate) solid is comparable to that of bulk silver when the interparticle distance is reduced to approximately 3.6 Å. Furthermore, the study revealed the coexisting, competing tunneling, and incoherent hopping charge transport mechanisms, which differed from those previously reported. The introduction of conjugation-structured ligands, tuning of the structures of metal nanoclusters, and use of high-pressure techniques contributed to enhanced conductivity, and thus, the charge carrier types were determined using Hall measurements. Overall, this study provides valuable insight into the charge transport in gold nanocluster solids and represents an important advancement in metal nanocluster semiconductor research.

Ambipolar Superconductivity with Strong Pairing Interaction in Monolayer 1T'-MoTe2.

Gate tunable two-dimensional (2D) superconductors offer significant advantages in studying superconducting phase transitions. Here, we address superconductivity in exfoliated 1T'-MoTe2 monolayers with an intrinsic band gap of ∼7.3 meV using field effect doping. Despite large differences in the dispersion of the conduction and valence bands, superconductivity can be achieved easily for both electrons and holes. The onset of superconductivity occurs near 7-8 K for both charge carrier types. This temperature is much higher than that in bulk samples. Also the in-plane upper critical field is strongly enhanced and exceeds the BCS Pauli limit in both cases. Gap information is extracted using point-contact spectroscopy. The gap ratio exceeds multiple times the value expected for BCS weak-coupling. All of these observations suggest a strong enhancement of the pairing interaction.

Role of defects on carrier dynamics and transport mechanism in Bi2Te3 single crystals

Defects play an important role in determining the type of carriers as well as in tunning the physical properties of layered materials. In this study, we have demonstrated that by varying the growth kinetics one can control the defects and can achieve electrons or holes dominated Bi2Te3 single crystals using the modified Bridgman method. The correlation between structural defects and the type of dominant charge carriers in crystals is discussed using X-ray diffraction and Hall resistivity. Electrons are found to be originating from Te vacancy type defects, while holes are manifested from predominant structural defects viz. BiTe antisite defects or interstitial Te atoms. We observe that the alteration of charge carriers from electrons to holes has enhanced magnetoresistance from 103% to 224%. The enhancement in magnetoresistance emerges from the 2D multichannel quantum coherent conduction mechanism.

Anisotropic transport properties and high-mobility of charge carriers of antiferromagnetic GdAgSb2

We report detailed magnetic and magnetotransport properties of single-crystalline GdAgSb2 antiferromagnet. The electronic transport properties show metallic behavior along with large, anisotropic, and non-saturating magnetoresistance (MR) in transverse experimental configuration. At 2 K and 9 T, the value of MR reaches as high as ∼1.8×103%. The anisotropic MR along with additional features for applied magnetic field along some specific crystallographic directions reveal the quasi-two-dimensional nature of the Fermi surface of GdAgSb2. Hall resistivity confirms the presence of two types of charge carriers. The high carrier mobilities (∼1.2×104 cm2 V−1 s−1) and nearly-compensated electron and hole-density (∼1019 cm−3) could be responsible for the large transverse MR in GdAgSb2. We have also observed the de Haas–van Alphen oscillations in the magnetization measurements below 7 K. Furthermore, the robust planar Hall effect, which persists up to high temperatures, could indicate the nontrivial nature of the electronic band structure for GdAgSb2.