Bulk single crystal Molybdenum diselenide has been studied for its electronic and thermal transport properties. We perform resistivity measurements with current in-plane (CIP) and current perpendicular to plane (CPP) as a function of temperature. The CIP measurements exhibit metal to semiconductor transition at $\simeq 31$ K. In the semiconducting phase ($T > 31$ K), the transport is best explained by variable range hopping (VRH) model. Large magnitude of resistivity in CPP mode indicates strong structural anisotropy. Seebeck coefficient as a function of temperature measured in the range $90 - 300$ K, also agrees well with the VRH model. The room temperature Seebeck coefficient is found to be $139$ $μ$V/K. VRH fittings of the resistivity and Seebeck coefficient data indicate high degree of localization.
Molecular beam epitaxy technique has been used to deposit a single layer and a bilayer of MoSe 2 on sapphire. Extensive characterizations including in-situ and ex-situ measurements show that the layered MoSe 2 grows in a scalable manner on the substrate and reveals characteristics of a stoichiometric 2H-phase. The layered MoSe 2 exhibits polycrystalline features with domains separated by defects and boundaries. Temperature and magnetic field dependent resistivity measurements unveil a carrier hopping character described within two-dimensional variable range hopping mechanism. Moreover, a negat…
Interlayer excitons are observed coexisting with intralayer excitons in bi-layer, few-layer, and bulk MoSe2 single crystals by confocal reflection contrast spectroscopy. Quantitative analysis using the Dirac-Bloch-Equations provides unambiguous state assignment of all the measured resonances. The interlayer excitons in bilayer MoSe2 have a large binding energy of 153 meV, narrow linewidth of 20 meV, and their spectral weight is comparable to the commonly studied higher-order intralayer excitons. At the same time, the interlayer excitons are characterized by distinct transition energies and per…
Understanding thermal transport in layered transition metal dichalcogenide (TMD) crystals is crucial for a myriad of applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood. Here, we present a combined experimental-theoretical study of the intrinsic lattice thermal conductivity of the representative TMD MoSe$_2$, focusing on the effect of material thickness and the material's environment. We use Raman thermometry measurements on suspended crystals, where we identify and eliminate crucial artefact…
Transition metal dichalcogenides (TMDCs), together with other two-dimensional (2D) materials have attracted great interest due to the unique optical and electrical properties of atomically thin layers. In order to fulfill their potential, developing large-area growth and understanding the properties of TMDCs have become crucial. Here, we used molecular beam epitaxy (MBE) to grow atomically thin MoSe$_2$ on GaAs(111)B. No intermediate compounds were detected at the interface of as-grown films. Careful optimization of the growth temperature can result in the growth of highly aligned films with o…
Expressions for dependences of the pre-exponential factor σ_3 and the thermal activation energy ε_3 of hopping electric conductivity of holes via boron atoms on the boron atom concentration N and the compensation ratio K are obtained in the quasiclassical approximation. It is assumed that the acceptors (boron atoms) in charge states (0) and (-1) and the donors that compensate them in the charge state (+1) form a nonstoichiometric simple cubic lattice with translational period R_h = [(1 + K)N]^{-1/3} within the crystalline matrix. A hopping event occurs only over the distance R_h at a thermally…
We have performed terahertz time-domain spectroscopy of carrier-doped nanoporous crystal 12CaO7Al2O3 showing the Mott variable range hopping at room temperature. The real part of the dielectric constant clearly demonstrates the nature of localized carriers. The frequency dependence of both the real and imaginary parts of the dielectric constant can be simply explained by assuming two contributions: a dielectric response by the parent compound with no carriers and an AC hopping conduction with the Jonscher law generally reported up to GHz range. The possible obedience to the Jonscher law in the…
A structure prediction method is presented based on the Minima Hopping method. Optimized moves on the configurational enthalpy surface are performed to escape local minima using variable cell shape molecular dynamics by aligning the initial atomic and cell velocities to low curvature directions of the current minimum. The method is applied to both silicon crystals and binary Lennard-Jones mixtures and the results are compared to previous investigations. It is shown that a high success rate is achieved and a reliable prediction of unknown ground state structures is possible.
Long needle-shaped single crystals of Zn1-xCoxO were grown at low temperatures using a molten salt solvent technique, up to x=0.10. The conduction process at low temperatures is determined to be by Mott variable range hopping. Both pristine and cobalt doped crystals clearly exhibit a crossover from negative to positive magnetoresistance as the temperature is decreased. The positive magnetoresistance of the Zn1-xCoxO single crystals increases with increased Co concentration and reaches up to 20% at low temperatures (2.5 K) and high fields (>1 T). SQUID magnetometry confirms that the Zn1-xCoxO c…
Transition metal dichalcogenides (TMDs) are van der Waals layered materials with sizable and tunable bandgaps, offering promising platforms for two-dimensional electronics and optoelectronics. To this end, the bottleneck is how to acquire high-quality single crystals in a facile and efficient manner. As one of the most widely employed method of single-crystal growth, conventional chemical vapor transport (CVT) generally encountered problems including the excess nucleation that leads to small crystal clusters and slow growth rate. To address these issues, a seed crystal is introduced to suppres…
Charge carriers that execute multi-phonon hopping generally interact strongly enough with phonons to form polarons. A polarons sluggish motion is linked to slowly shifting atomic displacements that severely reduce the intrinsic width of its transport band. Here a means to estimate hopping polarons bandwidths from Seebeck-coefficient measurements is described. The magnitudes of semiconductors Seebeck coefficients are usually quite large (greater than 86 microvolts/K) near room temperature. However, in accord with the third law of thermodynamics, Seebeck coefficients must vanish at absolute zero…
Ionic transport in conventional ionic solids is generally considered to proceed via independent diffusion events or "hops''. This assumption leads to well-known Arrhenius expressions for transport coefficients, and is equivalent to assuming diffusion is a Poisson process. Using molecular dynamics simulations of the low-temperature B1, B3, and B4 AgI polymorphs, we have compared rates of ion-hopping with corresponding Poisson distributions to test the assumption of independent hopping in these common structure-types. In all cases diffusion is a non-Poisson process, and hopping is strongly corre…
Investigation of Hopping Conduction and Its Impact on the Subthreshold and Transition Region Transport in Oxide Semiconductor Transistors by Magneto-Transport Measurements
National Key Laboratory of Advanced Micro and Nano Manufacture Technology and School of Information Science and Electronic Engineering, Shanghai Jiao Tong University（上海交通大学信息科学与电子工程学院）；School of Integrated Circuits, Huazhong University of Science and Technology（华中科技大学集成电路学院）
Predicting charge transport in organic molecular crystals is notoriously challenging. Carrier mobility calculations in organic semiconductors are dominated by quantum chemistry methods based on charge hopping, which are laborious and only moderately accurate. We compute from first principles the electron-phonon scattering and the phonon-limited hole mobility of naphthalene crystal in the framework of ab initio band theory. Our calculations combine GW electronic bandstructures, ab initio electron-phonon scattering, and the Boltzmann transport equation. The calculated hole mobility is in very go…
Predicting the electrical properties of organic molecular crystals (OMCs) is challenging due to their complex crystal structures and electron-phonon (e-ph) interactions. Charge transport in OMCs is conventionally categorized into two limiting regimes $-$ band transport, characterized by weak e-ph interactions, and charge hopping due to localized polarons formed by strong e-ph interactions. However, between these two limiting cases there is a less well understood intermediate regime where polarons are present but transport does not occur via hopping. Here we show a many-body first-principles ap…
Hall effect is detected in organic field-effect transistors, using appropriately shaped rubrene (C42H28) single crystals. It turned out that inverse Hall coefficient, having a positive sign, is close to the amount of electric-field induced charge upon the hole accumulation. The presence of the normal Hall effect means that the electromagnetic character of the surface charge is not of hopping carriers but resembles that of a two-dimensional hole-gas system.
Artificial tuning of dielectric parameters can result from interface conductivity in polycrystalline materials. In ferroelectric single crystals, it was already shown that ferroelectric domain walls can be the source of such artificial coupling. We show here that low temperature dielectric losses can be tuned by a dc magnetic field. Since such losses were previously ascribed to polaron relaxation we suggest this results from the interaction of hopping polarons with the magnetic field. The fact that this losses alteration has no counterpart on the real part of the dielectric permittivity confir…
The dynamic disorder model for charge carrier transport in organic semiconductors has been extensively studied in recent years. Although it is successful on determining the value of bandlike mobility in the organic crystalline materials, the incoherent hopping, the typical transport characteristic in organic semiconductors, cannot be described. In this work, the decoherence process is taken into account via a phenomenological parameter, say decoherence time, and the projective and Monte Carlo method is applied for this model to determine the waiting time and thus the diffusion coefficient. We …
Thermal transport in solids changes its nature from phonon propagation that suffers from perturbative scattering to thermally activated hops between localized vibrational modes as the level of disorder increases. Models have been proposed to understand these two distinct extremes that predict opposite temperature dependence of the thermal conductivity, but not for the transition or the intermediate regime. Here we explore thermal transport in two-dimensional crystalline and amorphous silica with varying levels of disorder, α, by performing atomistic simulations as well as analysis based on the…
Two-dimensional crystals, single sheets of layered materials, often show distinct properties desired for optoelectronic applications, such as larger and direct band gaps, valley- and spinorbit effects. Being atomically thin, the low amount of material is a bottleneck in photophysical and photochemical applications. Here, we propose the formation of stacks of two-dimensional crystals intercalated with small surfactant molecules. We show, using first principles calculations, that already the very short surfactant methyl amine electronically decouples the layers. We demonstrate the indirect-direc…
A Wigner crystal, a regular electron lattice arising from strong correlation effects, is one of the earliest predicted collective electronic states. This many-body state exhibits quantum and classical phase transitions and has been proposed as a basis for quantum information processing applications. In semiconductor platforms, two-dimensional Wigner crystals have been observed under magnetic field or moiré-based lattice potential where the electron kinetic energy is strongly suppressed. Here, we report bilayer Wigner crystal formation without a magnetic or confinement field in atomically thin …
We investigated the dielectric properties of Pb(Fe1/2Nb1/2)1-xTixO3 single crystals below room temperature. Two dielectric anomalies were detected in sample A while only one was detected in sample B in the temperature range 90~300 K. A Debye-like relaxation with strong frequency dispersion was detected in both samples. The pre-edge XAFS suggests that this dielectric anomaly is induced by the hopping conductivity between Fe2+ and Fe3+. The EXAFS results give us a clear picture of the local structure of iron ions. The weak frequency dependent dielectric anomaly only observed in sample A is suppo…
3D topological solitons are marvels of mathematical physics that arise in theoretical models in elementary particle and nuclear physics, condensed matter, and cosmology. A particularly interesting type of them is described by the mathematical Hopf map from a hypersphere to an ordinary sphere, which in the physical 3D space exhibits inter-linked circle-like or knotted localized regions of constant order parameter values. Despite their prevalence in models, such solitons remained experimentally elusive until recently, when hopfions were discovered in colloids and chiral liquid crystals, whereas …
We report measurements of in-plane $ρ_{ab}$ and out-of-plane $ρ_{c}$ resistivities on a single crystal of the half-doped bilayer manganite LaSr$_{2}$Mn$_{2}$O$_{7}$. In the temperature $T$ range 220 to 300 K, the resistive anisotropy $ρ_{c}/ρ_{ab}=A+B/T$ ($A$ and $B$ constants), which provides evidence for the variable-range-hopping conduction in the presence of a Coulomb gap. This hopping mechanism also accounts for the quadratic magnetic field $H$ and $\sin^{2}ϕ$ dependences of the negative magnetoresistivity $\ln [ρ_{i}(T,H,ϕ)/ρ_{i}(T,H=0)]$ ($i=ab,c$), where $ϕ$ is the in-plane angle betwe…
Moiré superlattices in twistronic heterostructures are a powerful tool for materials engineering. In marginally twisted (small misalignment angle, $θ$) bilayers of nearly lattice-matched two-dimensional (2D) crystals moiré patterns take the form of domains of commensurate stacking, separated by a network of domain walls (NoDW) with strain hot spots at the NoDW nodes. Here, we show that, for type-II transition metal dichalcogenide bilayers MoX$_2$/WX$_2$ (X=S, Se), the hydrostatic strain component in these hot spots creates quantum dots for electrons and holes. We investigate the electron/hole …
Engineering thermal transport in two dimensional materials, alloys and heterostructures is critical for the design of next-generation flexible optoelectronic and energy harvesting devices. Direct experimental characterization of lattice thermal conductivity in these ultra-thin systems is challenging and the impact of dopant atoms and hetero-phase interfaces, introduced unintentionally during synthesis or as part of deliberate material design, on thermal transport properties is not understood. Here, we use non-equilibrium molecular dynamics simulations to calculate lattice thermal conductivity …
To perform a local orbital analysis of electronic and magnetic interactions, we construct the Wannier functions (WFs) of the Fe $3d$ orbitals in the parent compound of the recently discovered iron pnictide superconductors, LaFeAsO, and a comparison material LaFePO. Comparing the WFs for the stripe antiferromagnetic order with those for no magnetic order, the difference is a significant spreading (``{\it de}localization'') of specifically the $d_{xy}$ and $d_{xz}$ (but not $d_{yz}$) WFs, where parallel Fe spins lie along the $x$ direction. The WF basis gives a tight-binding representation of th…
Presently, cerium-doped LaMnO$_3$ is vividly discussed as an electron-doped counterpart prototype to the well-established hole-doped mixed-valence manganites. Here, La$_{0.7}$Ce$_{0.3}$MnO$_3$ thin films of different thicknesses, degrees of CeO$_2$ phase segregation, and oxygen deficiency, grown on SrTiO$_3$ single crystal substrates, are compared with respect to their resistance-vs.-temperature (R vs. T) behavior from 300~K down to 90~K. While the variation of the film thickness (and thus the degree of epitaxial strain) in the range between 10~nm and 100~nm has only a weak impact on the elect…
We report anisotropic resistivity measurements on a La$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ single crystal over a temperature $T$ range from 2 to 400 K and in magnetic fields $H$ up to 14 T. For $T\geq 218$ K, the temperature dependence of the zero-field in-plane $ρ_{ab}(T)$ resistivity obeys the adiabatic small polaron hopping mechanism, while the out-of-plane $ρ_{c}(T)$ resistivity can be ascribed by an Arrhenius law with the same activation energy. Considering the magnetic character of the polarons and the close correlation between the resistivity and magnetization, we developed a model which a…
Topological band insulators and (semi-) metals can arise out of atomic insulators when the hopping strength between electrons increases. Such topological phases are separated from the atomic insulator by a bulk gap closing. In this work, we show that in many (magnetic) space groups, the crystals with certain Wyckoff positions and orbitals being occupied must be semimetal or metals in the atomic limit, e.g. the hopping strength between electrons is infinite weak but not vanishing, which then are termed atomic (semi-)metals (ASMs). We derive a sufficient condition for realizing ASMs in spinless …
This article presents studies on low-field electrical conduction in the range 4-to-300 K for a ultrafast material: InGaAs:ErAs grown by molecular beam epitaxy. The unique properties include nano-scale ErAs crystallines in host semiconductor, a deep Fermi level, and picosecond ultrafast photocarrier recombination. As the temperature drops, the conduction mechanisms are in the sequence of thermal activation, nearest-neighbor hopping, variable-range hopping, and Anderson localization. In the low-temperature limit, finite-conductivity metallic behavior, not insulating, was observed. This unusual c…
The anisotropic electron transport in the (001) plane of sublimation-grown Cl$_{2}$-NDI (naphthalene diimide) single crystals is analysed over a temperature range between 175 K and 300 K. Upon cooling from room temperature to 175 K the electron mobility along the direction of preferred transport monotonously increases from 1.5 cm$^{2}$/Vs to 2.8 cm$^{2}$/Vs according to a distinct temperature relation of $~T^{-1.3}$. At first glance, these characteristics allude to a coherent, i.e. band-like charge carrier transport predominantly governed by inelastic scattering with accoustic phonons. However…
The resistivity of a dense crystalline array of semiconductor nanocrystals (NCs) depends in a sensitive way on the level of doping as well as on the NC size and spacing. The choice of these parameters determines whether electron conduction through the array will be characterized by activated nearest-neighbor hopping or variable-range hopping (VRH). Thus far, no general theory exists to explain how these different behaviors arise at different doping levels and for different types of NCs. In this paper we examine a simple theoretical model of an array of doped semiconductor NCs that can explain …
