The carrier type and density in Bi2Se3 single crystals are systematically tuned by introducing a calcium (Ca) dopant. A carrier density of ~1x1017 cm-3 which corresponds to ~25 meV in the Fermi energy is obtained in both n- and p-type materials. Electrical transport properties show that the insulating behavior is achieved in low carrier density crystals. In addition, both the band gap and reduced effective mass of carriers are determined.
Effect of doping-- and field--induced charge carrier density on the electron transport in nanocrystalline ZnO
研究了溶胶-凝胶法制备的掺杂浓度在0.8at%~ 10at%之间的未掺杂和Al掺杂氧化锌纳米粒子的薄膜的电荷输运性质。X射线衍射研究表明，在高掺杂样品的平均晶粒尺寸的减少。我们提供的电导率和由此产生的载流子密度相对于掺杂水平的估计。将由于非本征掺杂引起的载流子密度的增加与场效应晶体管结构中的载流子的积累进行比较。这允许评估由于非本征掺杂对电子迁移率的散射效应。随着掺杂密度的增加，后者从4.6*10^-3 cm ^2/Vs降低到4.5*10^-4 cm ^2/Vs。与此相反，积累导致迁移率增加到1.5*10^-2 cm ^2/Vs。与微晶之间的晶界相关的势垒高度来自温度相关的迁移率测量。非本征掺杂最初导致晶界势垒高度降低，随后由于掺杂引起的结构缺陷而增加。我们的结论是，溶胶-凝胶处理纳米ZnO：Al的导电性是由增强的载流子密度和掺杂诱导的载流子散射效应的相互作用，在我们的情况下，在0.8原子%达到最大值。
Ordinary doping by electrons (holes) generally means that the Fermi level shifts towards the conduction band (valence band) and that the conductivity of free carriers increases. Recently, however, some peculiar doping characteristics were sporadically recorded in different materials without noting the mechanism: electron doping was observed to cause a portion of the lowest unoccupied band to merge into the valance band, leading to a decrease in conductivity. This behavior we dub as 'anti-doping' was seen in rare-earth nickel oxides SmNiO3, cobalt oxides SrCoO2.5, Li-ion battery materials and e…
Undesired unintentional doping and doping limits in semiconductors are typically caused by compensating defects with low formation energies. Since the formation energy of a charged defect depends linearly on the Fermi level, doping limits can be especially pronounced in wide bandgap semiconductors where the Fermi level can vary substantially. Introduction of non-equilibrium carrier concentrations during growth or processing alters the chemical potentials of band carriers and thus provides the possibility of modifying populations of charged defects in ways impossible at thermal equilibrium. Her…
The control of spin without magnetic field is one of challenges in developing spintronic devices. In an attempt to solve this problem, we proposed a novel hypothetic LaMn0.5Zn0.5AsO alloy from two experimentally synthesized rare earth element transition metal arsenide oxides, i.e. LaMnAsO and LaZnAsO. On the basis of the first-principles calculations with strong-correlated correction, we found that the LaMn0.5Zn0.5AsO alloy is an antiferromagnetic semiconductor at ground state, while bipolar magnetic semiconductor at ferromagnetic state. Both electron and hole doping in the LaMn0.5Zn0.5AsO all…
High contact resistance is one of the primary concerns for electronic device applications of two-dimensional (2D) layered semiconductors. Here, we explore the enhanced carrier transport through metal-semiconductor interfaces in WS2 field effect transistors (FETs) by introducing a typical transition metal, Cu, with two different doping strategies: (i) a "generalized" Cu doping by using randomly distributed Cu atoms along the channel and (ii) a "localized" Cu doping by adapting an ultrathin Cu layer at the metal-semiconductor interface. Compared to the pristine WS2 FETs, both the generalized Cu …
We show that doped cubic iron pyrite, which is a diamagnetic semiconductor, becomes ferromagnetic when $p$-type doped. We furthermore find that this material can exhibit high spin polarization both for tunneling and transport devices. These results are based on first principles electronic structure and transport calculations. This illustrates the use of $p$-type doping without magnetic impurities as a strategy for obtaining ferromagnetic semiconducting behavior, with implications for spintronic applications that require both magnetic ordering and good mobility. This is a combination that has b…
We investigated the role of oxygen vacancy in n-type interface of LaAlO3 (LAO) overlayer on SrTiO3 (STO) (001) by carrying out density-functional-theory calculations. Comparing the total energies of the configurations with one vacancy in varying locations we found that oxygen vacancies favor to appear first in LAO surface. These oxygen vacancies in the surface generate a two-dimensional distribution of carriers at the interface, resulting in band bending at the interface in STO side. Dependent on the concentration of oxygen vacancies in LAO surface, the induced carrier charge at the interface …
We report the electronic properties of single crystals of candidate nodal-line semimetal CaAgP. The transport properties of CaAgP are understood within the framework of a hole-doped nodal-line semimetal. In contrast, Pd-doped CaAgP shows a drastic increase of magnetoresistance at low magnetic fields and a strong decrease of electrical resistivity at low temperatures probably due to weak antilocalization. Hall conductivity data indicated that the Pd-doped CaAgP has not only hole carriers induced by the Pd doping, but also high-mobility electron carriers in proximity of the Dirac point. Electric…
We investigated the influence of oxygen on the performance of P3HT:PCBM (poly(3-hexylthiophene):[6,6]-phenyl C61 butyric acid methyl ester) solar cells by current--voltage, thermally stimulated current (TSC) and charge extraction by linearly increasing voltage (CELIV) measurement techniques. The exposure to oxygen leads to an enhanced charge carrier concentration and a decreased charge carrier mobility. Further, an enhanced formation of deeper traps was observed, although the overall density of traps was found to be unaffected upon oxygen exposure. With the aid of macroscopic simulations, base…
To obtain high-performance spintronic devices with high integration density, two-dimensional (2D) half-metallic materials are eagerly pursued all along. Here, we propose a stable 2D material with a honeycomb-kagome lattice, i.e., the Mg3C2 monolayer, based on first-principles calculations. This monolayer is an anti-ferromagnetic (AFM) semiconductor at its ground state. We further demonstrate that a transition from AFM semiconductor to ferromagnetic half-metal in this 2D material can be induced by carrier (electron or hole) doping. This magnetic transition can be understood by the Stoner criter…
From electrodeless time-resolved microwave conductivity measurements, the efficiency of charge carrier generation, their mobility, and decay kinetics on photo-excitation were studied in arrays of Si nanowires grown by the vapor-liquid-solid mechanism. A large enhancement in the magnitude of the photoconductance and charge carrier lifetime are found depending on the incorporation of impurities during the growth. They are explained by the internal electric field that builds up, due to a higher doped sidewalls, as revealed by detailed analysis of the nanowire morphology and chemical composition.
Strontium titanate (SrTiO3) is widely used as a promising photocatalyst due to its unique band edge alignment with respect to the oxidation and reduction potential corresponding to oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). However, further enhancement of the photocatalytic activity in this material could be envisaged through the effective control of oxygen vacancy states. This could substantially tune the photoexcited charge carrier trapping under the influence of elemental functionalization in SrTiO3, corresponding to the defect formation energy. The charge trappi…
A modulation-doping approach to control the carrier density of the high-density electron gas at a prototype polar/non-polar oxide interface is presented. It is shown that the carrier density of the electron gas at a GdTiO3/SrTiO3 interface can be reduced by up to 20% from its maximum value (~ 3x10^14 cm^-2) by alloying the GdTiO3 layer with Sr. The Seebeck coefficient of the two-dimensional electron gas increases concurrently with the decrease in its carrier density. The experimental results provide insight into the origin of charge carriers at oxide interfaces exhibiting a polar discontinuity…
Structural, resistivity, thermoelectric power and magneto-transport properties of Cu doped Bi2Te3 topological insulators have been investigated. The occurrence of the tuning of charge carriers from n type to p type by Cu doping at Te sites of Bi2Te3 is observed both from Hall effect and thermoelectric power measurements. Carrier mobility decreases with the doping of Cu which provides evidence of the movement of Fermi level from bulk conduction band to the bulk valence band. Thermoelectric power also increaseswith doping of Cu.Moreover linear magnetoresistance (LMR) has been observed at high ma…
The doping of semiconductor materials is a fundamental part of modern technology, but the classical approaches have in many cases reached their limits both in regard to achievable charge carrier density, as well as mobility. Modulation doping, a mechanism that exploits the energy band alignment at an interface between two materials to induce free charge carriers in one of them, has been shown to circumvent the mobility restriction. Due to an alignment of doping limits by intrinsic defects, however, the carrier density limit cannot be lifted using this approach. Here we present a novel doping s…
We fabricate LaxSr2-x-yBayIrO4-delta thin films by pulsed laser deposition, in an effort to realize the effective carrier doping and metallization in the Sr2IrO4 system. We design ideal in-plane Ir-O-Ir frame structure by utilizing tensile substrate strain and Ba substitution, as well as control La doping and oxygen deficiency. This enables us to elucidate relation between the charge transport and the carrier density through systematic changes from original p-type spin-orbit Mott insulator to highly doped n-type metal.
All electronic, optoelectronic or photovoltaic applications of silicon depend on controlling majority charge carriers via doping with impurity atoms. Nanoscale silicon is omnipresent in fundamental research (quantum dots, nanowires) but also approached in future technology nodes of the microelectronics industry. In general, silicon nanovolumes, irrespective of their intended purpose, suffer from effects that impede conventional doping due to fundamental physical principles such as out-diffusion, statistics of small numbers, quantum- or dielectric confinement. In analogy to the concept of modul…
We have investigated the transport and magnetic properties of group-IV ferromagnetic semiconductor Ge1-xFex films (x = 1.0 and 2.3 %) with and without boron doping grown by molecular beam epitaxy (MBE). In order to accurately measure the transport properties of 100-nm-thick Ge1-xFex films, (001)-oriented silicon-on-insulator (SOI) wafers with an ultra-thin Si body layer (~5 nm) were used as substrates. Owing to the low Fe content, the hole concentration and mobility in the Ge1-xFex films were exactly estimated by Hall measurements because the anomalous Hall effect in these films was found to b…
Doping inhomogeneities in solids are not uncommon, but their microscopic observation and understanding are limited due to the lack of bulk-sensitive experimental techniques with high-enough spatial and spectral resolution. Here, we demonstrate nanoscale imaging of both dopants and free charge carriers in La-doped BaSnO3 (BLSO) using high-resolution electron energy-loss spectroscopy (EELS). By analyzing both high- and low-energy excitations in EELS, we reveal chemical and electronic inhomogeneities within a single BLSO nanocrystal. The inhomogeneous doping leads to distinctive localized infrare…
We demonstrate the tunability of the photoluminescence (PL) properties of monolayer (1L)-MoS2 via chemical doping. The PL intensity of 1L-MoS2 was drastically enhanced by the adsorption of p-type dopants with high electron affinity, but reduced by the adsorption of n-type dopants. This PL modulation results from switching between exciton PL and trion PL depending on carrier density in 1L-MoS2. Achievement of the extraction and injection of carriers in 1L-MoS2 by this solution-based chemical doping method enables convenient control of optical and electrical properties of atomically thin MoS2.
In this work, we introduce models for deriving lower limits for the key parameters doping efficiency, charge carrier concentration, and charge carrier mobility from conductivity data of doped organic semiconductors. The models are applied to data of thin layers of Fullerene C60 n-doped by four different n-dopants. Combining these findings with thermoelectric Seebeck data, the energetic position of the transport level can be narrowed down and trends for the absolute values are derived.
Emergence of half-semiconductor behavior and tunable magnetism via carrier doping in Janus VXSe (X=Cl, Br, I) monolayers
Southwest University（西南大学）；Hanhong College, Southwest University（汉弘学院，西南大学）；AECC Hunan Aviation Powerplant Research Institute（中国航发湖南航空发动机研究所）；Chengdu University of Technology（成都理工大学）；Leshan Normal University（乐山师范学院）；Shanghai Jiao Tong University（上海交通大学）
In spite of great appeal of two-dimensional (2D) semiconductors for electronics and optoelectronics, to achieve required charge carrier concentrations by means of chemical doping remains a challenge, due to large defect ionization energies (IEs). Here by decomposing the defect IEs into the neutral single-electron defect level, the structural relaxation energy gain, and the electronic relaxation energy cost, we propose a conceptual picture that the large defect IEs are caused by two effects of reduced dimensionality. While the quantum confinement effect (QCE) makes the neutral single-electron p…
Metallic anti-ThCr$_2$Si$_2$-type $RE_2$O$_2$Bi ($RE$ = rare earth) with Bi square nets show superconductivity while insulating La$_2$O$_2$Bi shows high hole mobility, by expanding the c-axis length through oxygen intercalation. In this study, alkaline earth metal oxides (CaO, SrO, and BaO) were co-sintered with La$_2$O$_2$Bi. CaO and BaO served as oxygen intercalants without incorporation of Ca and Ba in La$_2$O$_2$Bi. On the other hand, SrO served as not only oxygen intercalant but also hole dopant via Sr substitution with La in La$_2$O$_2$Bi. The oxygen intercalation and hole doping resulte…
Density functional calculations are used to explain the charge transfer doping mechanism by which species physisorptively bonded to graphene can increase its free hole or electron density, without giving rise to defects, and thus maintain a high carrier mobility. Typical dopants studied are FeCl3, AuCl3, SbF5, HNO3, MoO3, Cs2O and O2. These systems do not break the π bonding of the basal plane are particularly important as these do not degrade the carrier mobility. In contrast, more reactive radicals like -OH cause a puckering of the basal plane and thereby act as defects.
Co-doping of Ce-doped LaBr$_3$ with Ba, Ca, or Sr improves the energy resolution that can be achieved by radiation detectors based on these materials. Here, we present a mechanism that rationalizes of this enhancement that on the basis of first principles electronic structure calculations and point defect thermodynamics. It is shown that incorporation of Sr creates neutral $V_\text{Br}$-Sr$_\text{La}$ complexes that can temporarily trap electrons. As a result, Auger quenching of free carriers is reduced, allowing for a more linear, albeit slower, scintillation light yield response. Experimenta…
A new kind of intrinsic magnetic topological insulators (MTI) MnBi2Te4 family have shed light on the observation of novel topological quantum effect such as quantum anomalous Hall effect (QAHE). However, the strong anti-ferromagnetic (AFM) coupling and high carrier concentration in the bulk hinder the practical applications. In closely related materials MnBi4Te7 and MnBi6Te10, the interlayer magnetic coupling is greatly suppressed by Bi2Te3 layer intercalation. However, AFM is still the ground state in these compounds. Here by magnetic and transport measurements, we demonstrate that Sb substit…
It was recently shown that the energy resolution of Ce-doped LaBr$_3$ scintillator radiation detectors can be crucially improved by co-doping with Sr, Ca, or Ba. Here we outline a mechanism for this enhancement on the basis of electronic structure calculations. We show that (i) Br vacancies are the primary electron traps during the initial stage of thermalization of hot carriers, prior to hole capture by Ce dopants; (ii) isolated Br vacancies are associated with deep levels; (iii) Sr doping increases the Br vacancy concentration by several orders of magnitude; (iv) $\text{Sr}_\text{La}$ binds …
We investigated the dependence of N$\acute{\textrm{e}}$el temperature as a critical temperature on the electric field and hole-electron doping in the antiferromagnetically ordered zigzag graphene nanoribbon. The temperature was calculated by averaging the magnon energy in the Brillouin zone within the mean-field approximation. We employed the generalized Bloch theorem instead of the supercell approach to reduce the computational cost significantly to obtain the magnon spectrum. We showed that the N$\acute{\textrm{e}}$el temperature reduces when increasing both the electric field and the hole-e…
The optical properties of graphene are strongly affected by electron-electron (e-e) and electron-hole (e-h) interactions. Here we tune these many-body interactions through varying the density of free charge carriers. Measurements from the infrared to the ultraviolet reveal significant changes in the optical conductivity of graphene for both electron and hole doping. The shift, broadening, and modification in shape of the saddle-point exciton resonance reflect strong screening of the many-body interactions by the carriers, as well as changes in quasi-particle lifetimes. Ab initio calculations b…
The control over material properties attainable through molecular doping is essential to many technological applications of organic semiconductors, such as OLED or thermoelectrics. These excitonic semiconductors typically reach the degenerate limit only at impurity concentrations of 5-10\%, a phenomenon that has been put in relation to the strong Coulomb binding between charge carriers and ionized dopants, and whose comprehension remained elusive so far. This study proposes a general mechanism for the release of carriers at finite doping in terms of collective screening phenomena. A multiscale…
The hole diffusion length in n-InGaAs is extracted for two samples of different doping concentrations using a set of long and thin diffused junction diodes separated by various distances on the order of the diffusion length. The methodology is described, including the ensuing analysis which yields diffusion lengths between 70 - 85 um at room temperature for doping concentrations in the range of 5 - 9 x 10^15 cm-3. The analysis also provides insight into the minority carrier mobility which is a parameter not commonly reported in the literature. Hole mobilities on the order of 500 - 750 cm2/Vs a…
Terahertz properties of mercury telluride (HgTe) films with critical thickness are presented and discussed. The density of the charge carriers is controlled using contact-free optical doping by visible light. In the magneto-optical response of HgTe the contribution of two types of carriers (electrons and holes) can be identified. The density of the electrons can be modified by light illumination by more than one order of magnitude. As the hole density is roughly illuminationindependent, the terahertz response of the illuminated samples becomes purely electronic. In some cases, light illuminati…
The high carrier mobility in graphene promises its utility in electronics applications. Azobenzene is a widely studied organic molecule for switchable optoelectronic devices that can be synthesized with a wide variety of ligands and deposited on graphene. Using first-principles calculations, we investigate graphene doping by physisorbed azobenzene molecules with various electron-donating and -accepting ligands. We confirm previous experimental results that demonstrate greater p-doping of graphene for the trans compared to cis configuration when using a SO$_3$ electron-accepting ligand, however…
Electrically tuning long-range magnetic orders has been realized in two-dimensional (2D) semiconductors via electrostatic doping. On the other hand, the observations are highly diverse: the transition can be realized by either electrons or holes or both depending on specific materials. Moreover, doped carriers seem to always favor the ferromagnetic (FM) ground state. The mechanism behind those diverse observations remains uncovered. Combining first-principles simulations, we analyze the spin superexchange paths of the correlated d/f orbitals around band edges and assign 2D magnetic semiconduct…
We have demonstrated that the island nucleation in the initial stage of epitaxial thin film growth can be tuned by substrate surface charge doping. This charge effect was investigated using spin density functional theory calculation in Fe-deposition on graphene substrate as an example. It was found that hole-doping can apparently increase both Fe-adatom diffusion barrier and Fe inter-adatom repulsion energy occurring at intermediate separation, whereas electron-doping can decrease Fe-adatom diffusion barrier but only slightly modify inter-adatom repulsion energy. Further kinetic Monte Carlo si…
Doping ferroelectrics with carriers is often detrimental to polarization. This makes the design and discovery of metals that undergo a ferroelectric-like transition challenging. In this letter, we show from first principles that the oxygen octahedral rotations in perovskites are often enhanced by electron doping, and this can be used as a means to strengthen the structural polarization in certain hybrid-improper ferroelectrics -- compounds in which the polarization is not stabilized by the long range Coulomb interactions but is instead induced by a trilinear coupling to octahedral rotations. W…
We describe a new regime for low-field magnetoresistance in organic semiconductors, in which the spin-relaxing effects of localized nuclear spins and electronic spins interfere. The regime is studied by the controlled addition of localized electronic spins to a material that exhibits substantial room-temperature magnetoresistance ($\sim 20$\%). Although initially the magnetoresistance is suppressed by the doping, at intermediate doping there is a regime where the magnetoresistance is insensitive to the doping level. For much greater doping concentrations the magnetoresistance is fully suppress…
Tin monosulfide (SnS) is a naturally p-type semiconductor with a layered crystal structure, but no reliable n-type SnS has been obtained by conventional aliovalent ion substitution. In this work, carrier polarity conversion to n-type was achieved by isovalent ion substitution for polycrystalline SnS thin films on glass substrates. Substituting Pb2+ for Sn2+ converted the majority carrier from hole to electron, and the free electron density ranged from 1012 to 1015 cm-3 with the largest electron mobility of 7.0 cm2/(Vs). The n-type conduction was confirmed further by the position of the Fermi l…
We present a study of germanium as n-type dopant in wurtzite GaN films grown by plasma-assisted molecular beam epitaxy, reaching carrier concentrations of up to 6.7E20 cm-3 at 300K, well beyond the Mott density. The Ge concentration and free carrier density were found to scale linearly with the Ge flux in the studied range. All the GaN:Ge layers present smooth surface morphology with atomic terraces, without trace of pits or cracks, and the mosaicity of the samples has no noticeable dependence on the Ge concentration. The variation of the GaN:Ge band gap with the carrier concentration is consi…
Doping is a fundamental property of semiconductors and constitutes the basis of modern microelectronic and optoelectronic devices. Their miniaturization requires contactless characterization of doping with nanometer scale resolution. Here, we use low- and room-temperature cathodoluminescence (CL) measurements to analyze p-type and n-type GaAs thin films over a wide range of carrier densities ($2\times 10^{17}$ to $1\times 10^{19}$ cm$^{-3}$). The spectral shift and broadening of CL spectra induced by shallow dopant states and band filling are the signature doping. We fit the whole spectral lin…
Bottom-up production of semiconductor nanomaterials is often accompanied by inhomogeneity resulting in a spread in electronic properties which may be influenced by the nanoparticle geometry, crystal quality, stoichiometry or doping. Using photoluminescence spectroscopy of a population of more than 20,000 individual Zn-doped GaAs nanowires, we reveal inhomogeneity in, and correlation between doping and nanowire diameter by use of a Bayesian statistical approach. Recombination of hot-carriers is shown to be responsible for the photoluminescence lineshape; by exploiting lifetime variation across …
The generalized Bloch theorem was applied to calculate the spin stiffness and to consider its tendencies when introducing the doping in zigzag graphene nanoribbons. To reach the intentions, two different flat spin spiral formations were constructed by fixing the ferromagnetic and antiferromagnetic spin arrangements at the two different edges by applying a constraint scheme method. A spin stiffness was then calculated by means of a quadratic order function, which maps the total energy difference in the self-consistent calculations onto the Heisenberg Hamiltonian. We found a very high spin stiff…
High thermoelectric energy conversion efficiency requires a large figure-of-merit, zT, over a broad temperature range. To achieve this, we optimize the carrier concentrations of n-type PbTe from room up to hot-end temperatures by co-doping Bi and Ag. Bi is an efficient n-type dopant in PbTe, often leading to excessive carrier concentration at room temperature. As revealed by density functional theory calculations, the formation of Bi and Ag defect complexes is exploited to optimize the room temperature carrier concentration. At elevated temperatures, we demonstrate the dynamic dissolution of A…
Heterostructures and superlattices consisting of a prototype Mott insulator, GdTiO3, and the band insulator SrTiO3 are grown by molecular beam epitaxy and show intrinsic electronic reconstruction, approximately 1/2 electron per surface unit cell at each GdTiO3/SrTiO3 interface. The sheet carrier densities in all structures containing more than one unit cell of SrTiO3 are independent of layer thicknesses and growth sequences, indicating that the mobile carriers are in a high concentration, two-dimensional electron gas bound to the interface. These carrier densities closely meet the electrostati…
Unlocking extreme doping and strain in epitaxial monocrystalline silicon
Centre de Nanosciences et de Nanotechnologies, Université Paris-Saclay, CNRS（纳米科学和纳米技术研究中心，巴黎萨克雷大学，法国国家科学研究中心）；Probion Analysis（普罗比昂分析公司）；CNR-IMM（意大利国家研究委员会微电子与微系统研究所）
We report on large exciton tuning in WSe$_2$ monolayers via substrate induced non-degenerate doping. We observe a redshift of $\sim$62 meV for the $A$ exciton together with a 1-2 orders of magnitude photoluminescence (PL) quenching when the monolayer WSe$_2$ is brought in contact with highly oriented pyrolytic graphite (HOPG) compared to the dielectric substrates such as hBN and SiO$_2$. As the evidence of doping from HOPG to WSe$_2$, a drastic increase of the trion emission intensity was observed. Using a systematic PL and Kelvin probe force microscopy (KPFM) investigation on WSe$_2$/HOPG, WS…
Cobalt and silver co-doping has been undertaken in ZnO thin films grown by pulsed laser deposition in order to investigate the ferromagnetic properties in ZnO-based diluted magnetic materials and to understand the eventual relation between ferromagnetism and charge carriers. Hall transport measurements reveal that Ag doping up to 5% leads to a progressive compensation of the native n-type carriers. The magnetization curves show ferromagnetic contributions for all samples at both 5 K and room temperature, decreasing with increasing the Ag concentration. First principles modeling of the possible…
