A comprehensive survey is given of the thermoballistic approach to charge carrier transport in semiconductors. This semiclassical approach bridges the gap between the drift-diffusion and ballistic ("thermionic") models of carrier transport, whose validity is limited to the range of very small and very large values, respectively, of the carrier mean free path. The physical concept underlying the thermoballistic approach, while incorporating basic features of the drift-diffusion and ballistic descriptions, constitutes a novel, unifying scheme. It is based on the introduction of "ballistic configurations" defined by a random partitioning of the length of a semiconducting sample into ballistic transport intervals, which are linked by points of local thermodynamic equilibrium at which carriers are emitted or absorbed. By averaging the carrier currents in the ballistic intervals over all ballistic configurations, a position-dependent thermoballistic current is derived for arbitrary magnitude of the carrier mean free path. This current is the key element of the thermoballistic concept and forms the point of departure of the calculation of various transport quantities. The present article starts out with an account of the standard drift-diffusion and ballistic transport models, and of a prototype model which paves the way for the fully developed form of that concept. In the main body of the article, a coherent exposition of the thermoballistic approach is given within a general formulation that takes into account arbitrarily shaped, spin-split potential energy profiles and spin relaxation during the carrier motion across ballistic intervals. The calculational procedures devised for implementing the thermoballistic concept are described. Specific examples relevant to present-day semiconductor and spintronics research are considered.
Reverse-biased graphene (Gr)/semiconductor Schottky diodes exhibit much enhanced sensitivity for gas sensing. However, carrier transport across the junctions is not fully understood yet. Here, Gr/SiC, Gr/GaAs and Gr/Si Schottky junctions under reverse-bias are investigated by temperature-dependent current-voltage measurements. A reduction in barrier height with increasing reverse-bias is observed for all junctions, suggesting electric-field enhanced thermionic emission. Further analysis of the field dependence of the reverse current reveals that while carrier transport in Gr/SiC Schottky junct…
We have experimentally tested the hypothesis of free charge carrier mediated spin-transport in the small molecule organic semiconductor Alq3 at room temperature. A spin current was pumped into this material by pulsed ferromagnetic resonance of an adjacent NiFe layer, while a charge current resulting from this spin current via the inverse spin-Hall effect (ISHE) was detected in a Pt layer adjacent on the other side of the Alq3 layer, confirming a pure spin current through the Alq3 layer. Charge carrier spin states in Alq3, were then randomized by simultaneous application of electron paramagneti…
The theoretical effects of phase separation on encounter-limited charge carrier recombination in organic semiconductor blends are investigated using kinetic Monte Carlo (KMC) simulations of pump-probe experiments. Using model bulk heterojunction morphologies, the dependence of the recombination rate on domain size and charge carrier mobility are quantified. Unifying competing models and simulation results, we show that the mobility dependence of the recombination rate can be described using the power mean of the electron and hole mobilities with a domain size dependent exponent. Additionally, …
Using time-resolved optical Kerr rotation, we measure the low temperature valley dynamics of resident electrons and holes in exfoliated WSe$_2$ monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically-gated WSe$_2$ monolayers having different dielectric environments. In a fully-encapsulated structure (hBN/WSe$_2$/hBN, where hBN is hexagonal boron nitride), valley relaxation is found to…
One of the fundamental properties of semiconductors is their ability to support highly tunable electric currents in the presence of electric fields or carrier concentration gradients. These properties are described by transport coefficients such as electron and hole mobilities. Recently, advances in electronic structure methods for real materials have made it possible to study these properties with predictive accuracy and without resorting to empirical parameters. Here, we review the most recent developments in the area of ab initio calculations of carrier mobilities of semiconductors. In the …
We show that the carrier recombination rate of noncentrosymmetric materials can be strongly modified by spin-orbit coupling. Our proposed mechanism involves the separation of conduction and valence bands into their respective spin components, which changes the transition dipole moments between them. The change in the carrier recombination can be either positive or negative in sign, or vary depending on the location of carriers in the Brillouin zone. We have performed a large scale DFT screening study to identify candidate materials that display this effect. We have selected three materials, Pb…
Auger recombination in semiconductors is a many-body phenomenon in which recombination of electrons and holes is accompanied by excitation of other charge carriers. Being nonradiative, it is detrimental to light emission. The excess energy of the excited carriers is normally rapidly converted to heat, making Auger processes difficult to probe directly. Here, we employ a technique in which the Auger-excited carriers are detected by their ability to tunnel out of the semiconductor through a thin barrier, generating a current. We employ vertical van der Waals (vdW) heterostructures with monolayer…
We report magneto-absorption spectroscopy of gated WSe$_2$ monolayers in high magnetic fields up to 60~T. When doped with a 2D Fermi sea of mobile holes, well-resolved sequences of optical transitions are observed in both $σ^\pm$ circular polarizations, which unambiguously and separately indicate the number of filled Landau levels (LLs) in both $K$ and $K'$ valleys. This reveals the interaction-enhanced valley Zeeman energy, which is found to be highly tunable with hole density $p$. We exploit this tunability to align the LLs in $K$ and $K'$, and find that the 2D hole gas becomes unstable agai…
Understanding how the complex intermolecular- and nano-structure present in organic semiconductor donor-acceptor blends impacts charge carrier motion, interactions, and recombination behavior is a critical fundamental issue with a particularly major impact on organic photovoltaic applications. In this study, kinetic Monte Carlo (KMC) simulations are used to numerically quantify the complex bimolecular charge carrier recombination behavior in idealized phase-separated blends. Recent KMC simulations have identified how the encounter-limited bimolecular recombination rate in these blends deviates…
In reduced-dimensional semiconductors, doping-induced carrier plasmons can strongly couple with quasiparticle excitations, leading to a significant band gap renormalization. We develop a new plasmon-pole theory that efficiently and accurately capture this coupling. Using monolayer molybdenum disulfide (MoS2) as a prototype two-dimensional (2D) semiconductor, we reveal an enhanced band gap renormalization around 400 meV and an unusual nonlinear evolution of its band gap with doping. This 2D prediction significantly differs from the linear behaviors that are common to one-dimensional structures.…
The large scale various shapes and orientation defects influence into carrier scattering was theoretically analyzed using Monte Carlo method and compared to the experimental measurements. It was shown how the large scale defects screen themselves from the interaction with free charge carriers. The comparison of quantum and classical transport regimes was performed.
We have applied the photoexcited muon spin spectroscopy technique (photo-$μ$SR) to intrinsic germanium with the goal of developing a new method for characterizing excess carrier kinetics in a wide range of semiconductors. Muon spin relaxation rates can be a unique measure of excess carrier density and utilized to investigate carrier dynamics. The obtained carrier lifetime spectrum can be modeled with a simple diffusion equation to determine bulk recombination lifetime and carrier mobility. Temperature dependent studies of these parameters can reveal the recombination and diffusion mechanism.
While being extensively studied as an important physical process to alter exciton population in nanostructures at fs time scale, carrier multiplication has not been considered seriously as a major mechanism for phase transition. Real-time time-dependent density functional theory study of Ge2Sb2Te5 reveals that carrier multiplication can induce ultrafast phase transition in solid state despite that the lattice remains cold. The results also unify the experimental findings in other semiconductors for which the explanation remains to be the 30-year old phenomenological plasma annealing model.
In this work, the consequence of the high band-edge density of states on the carrier statistics and quantum capacitance in transition metal dichalcogenide two-dimensional semiconductor devices is explored. The study questions the validity of commonly used expressions for extracting carrier densities and field-effect mobilities from the transfer characteristics of transistors with such channel materials. By comparison to experimental data, a new method for the accurate extraction of carrier densities and mobilities is outlined. The work thus highlights a fundamental difference between these mat…
When exploring new materials for their potential in (opto)electronic device applications, it is important to understand the role of various carrier interaction and scattering processes. Research on transition metal dichalcogenide (TMD) semiconductors has recently progressed towards the realisation of working devices, which involve light-emitting diodes, nanocavity lasers, and single-photon emitters. In these two-dimensional atomically thin semiconductors, the Coulomb interaction is known to be much stronger than in quantum wells of conventional semiconductors like GaAs, as witnessed by the 50 …
Quantized spin-wave known as magnon, a bosonic quasiparticle, can drag electrons or holes via sd exchange interaction and boost the thermopower over the conventional diffusive thermopower. P-type magnon-drag thermopower has been observed in both ferromagnetic and antiferromagnetic metallic and degenerate semiconductors. However, it has been less reported for intrinsic or n-type magnetic semiconductors; therefore, the impact of magnon-bipolar carrier drag on thermopower has remained unexplored. Here, a theoretical model for magnon-bipolar carrier drag thermopower is derived based on the magnon-…
We probe the accuracy limit of {\it ab initio} calculations of carrier mobilities in semiconductors, within the framework of the Boltzmann transport equation. By focusing on the paradigmatic case of silicon, we show that fully predictive calculations of electron and hole mobilities require many-body quasiparticle corrections to band structures and electron-phonon matrix elements, the inclusion of spin-orbit coupling, and an extremely fine sampling of inelastic scattering processes in momentum space. By considering all these factors we obtain excellent agreement with experiment, and we identify…
Two-dimensional (2D) semiconductors have demonstrated great potential for next-generation electronics and optoelectronics. However, the current 2D semiconductors suffer from intrinsically low carrier mobility at room temperature, which significantly limits its applications. Here we discover a variety of new 2D semiconductors with mobility one order of magnitude higher than the current ones. The discovery is made by developing effective descriptors for high-throughput computationally screening of the 2D materials database, followed by using state-of-the-art first principles method to accurately…
Contribution of photogenerated charge carriers to photothermal effect in optically opaque semiconductor samples
Faculty of Philosophy, University of East Sarajevo（东萨拉热窝大学哲学系）；Faculty of Physics, University of Belgrade（贝尔格莱德大学物理系）；Vinca Institute of Nuclear Sciences—National Institute of the Republic of Serbia, University of Belgrade（塞尔维亚共和国国家研究所文查核科学研究所，贝尔格莱德大学）
A large number of non-adiabatic dynamical studies have been applied to reveal the nature of carrier transport in organic semiconductors with different approximations. We present here a "nearly exact" graphical process unit (GPU) based finite temperature TD-DMRG method to evaluate the carrier mobility in organic semiconductors as described by electron-phonon model, in particular to rubrene crystal, one of the prototypical organic semiconductors, with parameters derived from first-principles. We find that (i) TD-DMRG is a general and robust method that can bridge the gap between hopping and band…
To investigate the initial process of Joule heating in semiconductors microscopically and quantitatively, we developed a theoretical framework for the ab initio evaluation of the carrier energy relaxation in semiconductors under a high electric field using a combination of the two-temperature model and the Boltzmann equation. We employed the method for bulk silicon as a typical example. Consequently, we found a remarkable difference in the energy relaxation processes of the electron and hole carriers. The longitudinal acoustic and optical phonons at the zone boundary contribute to the energy r…
Quantum interference between optical absorption processes can excite carriers with a polarized distribution in the Brillouin zone depending on properties of the incident optical fields. The polarized distribution of carriers introduces a current that can be controlled by the phases and polarizations of the incident optical fields. Here we study the quantum interference of 2- and 3-photon absorption processes in AlGaAs. We present theoretical predictions for carrier and current injection rates considering different frequencies, phases, and polarizations of the incident fields. We also discuss t…
Hall effect measurements are important for elucidating the fundamental charge transport mechanisms and intrinsic mobility in organic semiconductors. However, Hall effect studies frequently reveal an unconventional behavior that cannot be readily explained with the simple band-semiconductor Hall effect model. Here, we develop an analytical model of Hall effect in organic field-effect transistors in a regime of coexisting band and hopping carriers. The model, which is supported by the experiments, is based on a partial Hall voltage compensation effect, occurring because hopping carriers respond …
In many semiconductors, compensating defects set doping limits, decrease carrier mobility, and reduce minority carrier lifetime thus limiting their utility in devices. Native defects are responsible in many cases, but extrinsic dopants may also act as their own compensation when occupying an alternate lattice site. Suppressing the concentrations of compensating defects during processing close to thermal equilibrium is difficult because formation enthalpies are lowered as the Fermi level moves towards the majority band edge. Excess carriers, introduced for example by photogeneration, modify the…
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…
Two-dimensional (2D) mobile carriers are a wellspring of quantum phenomena. Among various 2D-carrier systems, such as field effect transistors and heterostructures, polar materials hold a unique potential; the spontaneous electric polarization in the bulk could generate positive and negative 2D carriers at the surface. Although several experiments have shown ambipolar carriers at the surface of a polar semiconductor BiTeI, their origin is yet to be specified. Here we provide compelling experimental evidences that the ambipolar 2D carriers at the surface of BiTeI are induced by the spontaneous …
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 dynamics of charge carriers in amorphous semiconductors fundamentally differ from those in crystalline semiconductors due to the lack of long-range order and the high defect density. Despite intensive technology-driven research interests and the existence of well-established experimental techniques, such as photoconductivity time-of-flight and ultrafast optical measurements, many aspects of the dynamics of photo-excited charge carriers in amorphous semiconductors remain poorly understood. Here we demonstrate direct imaging of carrier dynamics in space and time after photo-excitation in hyd…
The perturbation of a semiconductor from the thermodynamic equilibrium often leads to the display of nonlinear dynamics and formation of spatiotemporal patterns due to the spontaneous generation of competing processes. Here, we describe the ultrafast imaging of nonlinear carrier transport in silicon, excited by an intense femtosecond laser pulse. We use scanning ultrafast electron microscopy (SUEM) to show that, at a sufficiently high excitation fluence, the transport of photoexcited carriers slows down by turning into an oscillatory process. We attribute this nonlinear response to the electri…
We demonstrated the control of ferromagnetism in a surface quantum well containing a 5-nm-thick n-type ferromagnetic semiconductor (In,Fe)As layer sandwiched between two InAs layers, by manipulating the carrier wavefunction. The Curie temperature (Tc) of the (In,Fe)As layer was effectively changed by up to 12 K (ΔTc/Tc = 55%). Our calculation using the mean-field Zener theory reveals an unexpectedly large s-d exchange interaction in (In,Fe)As. Our results establish an effective way to control the ferromagnetism in quantum heterostructures of n-type FMSs, as well as require reconsideration on t…
