Carrier-carrier Interaction Research Articles

Application of MEG in Increasing External Quantum Efficiency Over 100%

This review paper focuses on increasing the efficiency of Solar cell using Quantum Dot. The principle idea is using MEG (Multiple exciton Generation). MEG is more efficient in quantum confined nanostructures than in bulk semiconductors because the momentum preservation prerequisite is relaxed. Even the carrier-carrier interactions are huge due to strong confinement. The carrier multiplication decoupling from the effective band gap allows amplified photo-voltage for corresponding carrier multiplication. Along with this, it was also found that external quantum efficiency (EQE) would reach almost 100%, sometimes even exceeding it, for energy which is greater than twice the band gap energy. This is due to the fact that high energy photons have the ability to produce more than one photo carrier pair. MEG is definitely a promising route to increasing solar cell efficiency. If a threshold of twice the band gap energy could be realized for impact ionization in a colloid Quantum Dot cell, the theoretical maximum possible conversion efficiency would shift to above 60%. The goal is to capture maximum energy incident on a given plane and targeting highyield transportation of the resultant photo generated charge.

Voltage Matching, Étendue, and Ratchet Steps in Advanced-Concept Solar Cells

Many advanced solar cell concepts propose surpassing the Shockley Queisser (SQ) limit by introducing multiple quasi-Fermi level separations that are arranged in series and/or in parallel. Exceeding the SQ limit with any parallel arrangement involves intermediate states that deliver additional charge carriers at, ideally, the same electro-chemical potential as the other elements in the parallel network. This can be thought of as voltage matching individual parallel components and in intermediate band materials is intricately linked to solar concentration and \'etendue mismatch between absorption and emission. Generally, to achieve voltage matching under sub-optimal conditions, an additional degree of freedom in the absorption thresholds of the material through a carrier relaxation or ratchet step is required. We explain why the ideal ratchet step decreases with solar concentration and how it depends on radiative efficiency and emission \'etendue of the individual transitions. For solar cell concepts that use Auger type carrier-carrier interactions or molecular triplet states for energetic up- or down-conversion, ideal bandgap combinations and achievable efficiencies also depend on interaction rates. We show that Auger assisted solar cells suffer more strongly from finite interaction rates than carrier multiplication devices.

Ultrafast Charge Carrier Relaxation in Inorganic Halide Perovskite Single Crystals Probed by Two-Dimensional Electronic Spectroscopy.

Halide perovskites are promising optoelectronic materials. Despite impressive device performance, especially in photovoltaics, the femtosecond dynamics of elementary optical excitations and their interactions are still debated. Here we combine ultrafast two-dimensional electronic spectroscopy (2DES) and semiconductor Bloch equations (SBEs) to probe the room-temperature dynamics of nonequilibrium excitations in CsPbBr3 crystals. Experimentally, we distinguish between excitonic and free-carrier transitions, extracting a ∼30 meV exciton binding energy, in agreement with our SBE calculations and with recent experimental studies. The 2DES dynamics indicate remarkably short, <30 fs carrier relaxation at a ∼3 meV/fs rate, much faster than previously anticipated for this material, but similar to that in direct band gap semiconductors such as GaAs. Dynamic screening of excitons by free carriers also develops on a similarly fast <30 fs time scale, emphasizing the role of carrier-carrier interactions for this material's optical properties. Our results suggest that strong electron-phonon couplings lead to ultrafast relaxation of charge carriers, which, in turn may limit halide perovskites' carrier mobilities.

Phonon-Suppressed Auger Scattering of Charge Carriers in Defective Two-Dimensional Transition Metal Dichalcogenides.

Two-dimensional transition metal dichalcogenides (TMDs) draw strong interest in materials science, with applications in optoelectronics and many other fields. Good performance requires high carrier concentrations and long lifetimes. However, high concentrations accelerate energy exchange between charged particles by Auger-type processes, especially in TMDs where many-body interactions are strong, thus facilitating carrier trapping. We report time-resolved optical pump-THz probe measurements of carrier lifetimes as a function of carrier density. Surprisingly, the lifetime reduction with increased density is very weak. It decreases only by 20% when we increase the pump fluence 100 times. This unexpected feature of the Auger process is rationalized by our time-domain ab initio simulations. The simulations show that phonon-driven trapping competes successfully with the Auger process. On the one hand, trap states are relatively close to band edges, and phonons accommodate efficiently the electronic energy during the trapping. On the other hand, trap states localize around defects, and the overlap of trapped and free carriers is small, decreasing carrier-carrier interactions. At low carrier densities, phonons provide the main charge trapping mechanism, decreasing carrier lifetimes compared to defect-free samples. At high carrier densities, phonons suppress Auger processes and lower the dependence of the trapping rate on carrier density. Our results provide theoretical insights into the diverse roles played by phonons and Auger processes in TMDs and generate guidelines for defect engineering to improve device performance at high carrier densities.

Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures

The intriguing physics of carrier-carrier interactions, which likewise affect the operation of light emitting devices, stimulate the research on semiconductor structures at high densities of excited carriers, a limit reachable at large pumping rates or in systems with long-lived electron-hole pairs. By electrically injecting carriers into WSe2/MoS2 type-II heterostructures which are indirect in real and k-space, we establish a large population of typical optically silent interlayer excitons. Here, we reveal their emission spectra and show that the emission energy is tunable by an applied electric field. When the population is further increased by suppressing the radiative recombination rate with the introduction of an hBN spacer between WSe2 and MoS2, Auger-type and exciton-exciton annihilation processes become important. These processes are traced by the observation of an up-converted emission demonstrating that excitons gaining energy in non-radiative Auger processes can be recovered and recombine radiatively.

(Invited) Photoionization in Doped and Undoped Semiconductor Quantum Dots

Optoelectronic properties of semiconductor quantum dots strongly depend on the propensity of their band carriers to transition to states extrinsic to the nanocrystal. Photoionization events typically reduce the photoluminescence quantum yield and induce emission intermittency and therefore they are often suppressed in light-emitting applications by the use of passivating barriers in the form of protective ligands or core/shell heterostructuring. In other uses of quantum dots, e.g. as photocatalysts, photocathodes, photodetectors, or solar cells, fast and efficient extraction of carriers to extrinsic states is of key importance. Here, we investigate the photoemission of carriers induced by carrier-carrier or carrier-dopant interactions in intrinsic and intentionally doped nanocrystals. Our studies reveal the ultrafast time scale, spectral response, and interaction mechanism of hot-carrier photoemission in these systems. Application-relevant performance parameters such as quantum efficiency and temporal response will be discussed.

Markov model of quantum fluctuations at the transition to lasing of semiconductor nanolasers

A Markov model of semiconductor nanolaser is constructed in order to describe finely the effects of quantum fluctuations in the dynamics of the laser, in particular by considering the transition to lasing. Nanolasers are expected to contain only a small number of emitters, whose semiconductor bands are simulated using true carrier energy states. The model takes into account carrier-carrier interactions in the conduction and valence bands, but the result is a huge Markov chain that is often too demanding for direct Monte-Carlo simulation. We introduce here a technique to split the whole chain into two subchains, one referring to thermalization events within the bands and the other to laser photonic events of interest. The model is applied to the analysis of laser transition and enlightens the coexistence of a pulse regime triggered by the quantum nature of the photon with the birth of the known coherent cw regime. This conclusion is highlighted by calculated time traces. We show that on the ultrasmall scale of nanolasers, we are unable to define perfectly the threshold.

Soft pair excitations and double-log divergences due to carrier interactions in graphene

Interactions between charge carriers in graphene lead to logarithmic renormalization of observables mimicking the behavior known in (3+1)-dimensional quantum electrodynamics (QED). Here we analyze soft electron-hole (e-h) excitations generated as a result of fast charge dynamics, a direct analog of the signature QED effect - multiple soft photons produced by the QED vacuum shakeup. We show that such excitations are generated in photon absorption, when a photogenerated high-energy e-h pair cascades down in energy and gives rise to multiple soft e-h excitations. This fundamental process is manifested in a double-log divergence in the emission rate of soft pairs and a characteristic power-law divergence in their energy spectrum of the form $\frac{1}{\omega}\ln \left(\frac{\omega}{\Delta}\right) $. Strong carrier-carrier interactions make pair production a prominent pathway in the photoexcitation cascade.

Magneto-photoconductivity of three dimensional topological insulator bismuth telluride

Magnetic field dependence of the photocurrent in a 3D topological insulator is studied. Among the 3D topological insulators bismuth telluride has unique hexagonal warping and spin texture which has been studied by photoemission, scanning tunnelling microscopy and transport. Here, we report on low temperature magneto-photoconductivity, up to 7 T, of two metallic bismuth telluride topological insulator samples with 68 and 110 nm thicknesses excited by 2.33 eV photon energy along the magnetic field perpendicular to the sample plane. At 4 K, both samples exhibit negative magneto-photoconductance below 4 T, which is as a result of weak-antilocalization of Dirac fermions similar to the previous observations in electrical transport. However the thinner sample shows positive magneto-photoconductance above 4 T. This can be attributed to the coupling of surface states. On the other hand, the thicker sample shows no positive magneto-photoconductance up to 7 T since there is only one surface state at play. By fitting the magneto-photoconductivity data of the thicker sample to the localization formula, we obtain weak antilocalization behaviour at 4, 10, and 20 K, as expected; however, weak localization behaviour at 30 K, which is a sign of surface states masked by bulk states. Also, from the temperature dependence of phase coherence length bulk carrier-carrier interaction is identified separately from the surface states. Therefore, it is possible to distinguish surface states by magneto-photoconductivity at low temperature, even in metallic samples.

Controllable population dynamics in Landau-quantized graphene

In this paper, we carry out a theoretical investigation on the population dynamics of graphene system under continuous-wave (cw) laser and chirped pulse excitation. Results of our numerical simulations reveal that complete population transfer from an initially occupied ground state to the initially unoccupied excited states can be achieved by choosing appropriate values of the chirp rate, the laser field intensity and frequency, as well as other system parameters. Also, we observe coherent Rabi-like population oscillations between the initial ground state and the excited final state. It is induced by the combined effect of cw and chirped-pulse laser fields. These results will contribute to the understanding of carrier-carrier and carrier-phonon interactions in graphene system, and may find applications in graphene-based high-speed electronic and optoelectronic devices.

PEG-coumarin nanoaggregates as π–π stacking derived small molecule lipophile containing self-assemblies for anti-tumour drug delivery

Polymeric self-assemblies formed by non-covalent interactions such as hydrophobic interactions, hydrogen bonding, π–π stacking, host-guest and electrostatic interactions have been utilised widely and exhibit controlled release of encapsulated drug. Beside carrier-carrier interactions, small molecule amphiphiles exhibiting carrier-drug interactions have recently been an area of interest for cancer drug delivery, as most of the hydrophobic anti-tumour drugs are aromatic and exhibit π–π conjugated structure. In the present study PEG-coumarin (PC) conjugates forming self-assembled nanoaggregates were synthesised with PEG (polyethylene glycol) as hydrophilic block and coumarin as small molecule lipophilic segment. Curcumin (CUR) as model conjugated aromatic drug was loaded in to the nanoaggregates via dual hydrophobic and π–π stacking interactions. The interactions between the conjugates and CUR, drug release profile and in vitro anti-tumour efficacy were investigated in detail. CUR-loaded nanoaggregate self-assembly was driven by π–π interactions and a maximum loading level of about 18 wt.% (~60 % encapsulation efficiency) was achieved. The average hydrodynamic diameter (Dav) was in the range of 120–160 nm and a spherical morphology was observed by transmission electron microscopy (TEM). A sustained release of CUR was observed for 90 h. Cytotoxicity evaluation of CUR-loaded nanoaggregates on pancreatic cancer cell lines indicated higher efficacy, IC50 ~11 and ~15 μM as compared to free CUR, IC50 ~14 and ~20 μM on human pancreatic carcinoma (MIA PaCa-2) and human pancreatic duct epithelioid carcinoma (PANC-1) cell lines respectively. PC conjugates provided a new strategy of fabricating nanoparticles for drug delivery and may form the basis for the development of advanced biomaterials in near future.

(Invited) Effects of Composition and Doping on the Optoelectronic Properties of Lead Halide Perovskite Nanocrystals

Colloidally synthesized lead halide perovskite nanocrystals have been recently demonstrated as active materials with great promise for a range of applications, from high-efficiency photovoltaics to color-converting phosphors and light-emitting diodes. Tailoring their optical and electronic properties through various synthetic routes in order to meet application-specific design parameters requires a good understanding of structure-property relationships. Here, by using a variety of steady-state and time-resolved spectroscopies, we explore carrier-carrier and carrier-dopant interactions in cesium lead halide nanocrystals as their halide component (Cl, Br, I, and their mixture) and doping level (Mn2+) is continuously tuned through a wide parameter space. We quantify such fundamental optical properties as exciton radiative lifetimes, absorption cross-sections, and derive the degeneracies of the band-edge electron and hole states. We also characterize the rates of intraband cooling and nonradiative Auger recombination and evaluate the strength of exciton–exciton coupling.1 Through impurity doping with Mn2+ ions, we also introduce new optical functionalities such as dual-color emission and establish the mechanism of carrier-dopant coupling in these materials.2

Study on ultrafast dynamics of low-temperature grown GaAs by optical pump and terahertz probe spectroscopy

Low-temperature-grown GaAs (LT-GaAs) possesses high carrier mobility, fast charge trapping, high dark resistance, and large threshold breakdown voltage, which make LT-GaAs a fundamental material for fabricating the ultrafast photoconductive switch, high efficient terahertz emitter, and high sensitive terahertz detector. Although lots of researches have been done on the optical and optoelectrical properties of LT-GaAs, the ultrafast dynamics of the photoexcitation and the relaxation mechanism are still unclear at present, especially when the photocarrier density is close to or higher than the defect density in the LT-GaAs, the dispersion of photocarriers shows a complicated pump fluence dependence. With the development of THz science and technology, the terahertz spectroscopy has become a powerful spectroscopic method, and the advantages of this method are contact-free, highly sensitive to free carriers, and sub-picosecond time resolved. In this article, by employing optical pump and terahertz probe spectroscopy, we investigate the ultrafast carrier dynamics of photogenerated carriers in LT-GaAs. The results reveal that the LT-GaAs has an ultrafast carrier capture process in contrast with that in GaAs wafer. The photoconductivity in LT-GaAs increases linearly with pump fluence at low power, and the saturation can be reached when the pump fluence is higher than 54 J/cm2. It is also found that the fast process shows a typical relaxation time of a few ps contributed by the capture of defects in the LT-GaAs, which is strongly dependent on pump fluence: higher pump fluence shows longer relaxation time and larger carrier mobility. By employing Cole-Cole Drude model, we can reproduce the photoconductivity well. Our results reveal that photocarrier relaxation time is dominated by the carrier-carrier Coulomb interaction: under low carrier density, the carrier-carrier Coulomb interaction is too small to screen the impurity-carrier scattering, and impurity-carrier scattering plays an important role in the photocarrier relaxation process. On the other hand, under high pump fluence excitation, the carrier-carrier Coulomb interaction screens partially the impurity-carrier scattering, which leads to the reduction of impurity-carrier scattering rate. As a result, the photocarrier lifetime and mobility increase with increasing pump fluence. The experimental findings provide fundamental information for developing and designing an efficient THz emitter and detector.

Probing indirect exciton complexes in a quantum dot molecule via capacitance-voltage spectroscopy

Capacitance-voltage spectroscopy has proved to be a very powerful experimental technique towards the investigation of carrier-carrier interactions both qualitatively and quantitatively in complex coupled nanostructures. Here, we exploit this method to observe indirect exciton complexes in a quantum dot molecule and to quantify the electron-hole interactions between two dots in a quantum dot molecule, formed by vertical stacking of self-assembled quantum dot layers. While frequency-dependent measurements distinguish between the $s$- and $p$-charging behavior, under perpendicular magnetic fields, reordering of the quantized states charging sequence is observed along with the formation of a Landau fan in the wetting layer that is used to reconstruct the Fermi energy level.

Rapid thermal annealing and modulation-doping effects on InAs/GaAs quantum dots photoluminescence dependence on excitation power

The optical properties of p-doped and annealed InAs/GaAs quantum dots (QDs) was investigated by photoluminescence (PL) as a function of temperature and excitation power density (Pexc). At low-T, PL spectra of rapid thermal annealing (RTA) and p-modulation doped QDs show an energy blueshift and redshift, respectively. A superlinear dependence of integrated PL intensity on Pexc at high-T was found only for undoped QD. The superlinearity was suppressed by modulation-doping and RTA effects. A linear dependence of IPL at all temperatures and a decrease of the carrier-carrier Coulomb interaction at high-T was found after RTA.

Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy

Attosecond science has paved the way for direct probing of electron dynamics in gases and solids. This review provides an overview of recent attosecond measurements, focusing on the wealth of knowledge obtained by the application of isolated attosecond pulses in studying dynamics in gases and solid-state systems. Attosecond photoelectron and photoion measurements in atoms reveal strong-field tunneling ionization and a delay in the photoemission from different electronic states. These measurements applied to molecules have shed light on ultrafast intramolecular charge migration. Similar approaches are used to understand photoemission processes from core and delocalized electronic states in metal surfaces. Attosecond transient absorption spectroscopy is used to follow the real-time motion of valence electrons and to measure the lifetimes of autoionizing channels in atoms. In solids, it provides the first measurements of bulk electron dynamics, revealing important phenomena such as the timescales governing the switching from an insulator to a metallic state and carrier-carrier interactions.

Large-signal characterization of millimeter-wave IMPATTs: effect of reduced impact ionization rate of charge carriers due to carrier-carrier interactions

In this paper, we study the effect of energy loss of charge carriers due to carrier-carrier interactions prior to impact ionization on the static and large-signal characteristics of double-drift region impact avalanche transit time (IMPATT) diodes based on Si designed to operate at millimeter-wave (mm-wave) atmospheric window frequencies such as 94, 140, and 220 GHz. The above mentioned effect has been incorporated in the simulation by taking into account a recently reported generalized analytical model of impact ionization rate of charge carriers based on multistage scattering phenomena in the base semiconductor. Results are compared with static and large-signal signal simulation results of the same diodes that we have reported earlier by taking into account the empirical relation of ionization rates fitted from the experimental data (experiment was carried out on IMPATT structures suitable for operating near 100 GHz). It is observed that both the large-signal RF power output and DC to RF conversion efficiency of the diodes are deteriorated significantly due to reduced ionization rates as a consequence of carrier-carrier collision events prior to the impact ionization. This effect is found to be more pronounced in 140 and 220 GHz diodes due to the enhanced carrier-carrier collisions within those diodes having greater background doping densities as compared to 94 GHz diode. The simulation results presented in this paper found to be in closer agreement with the experimental results as compared to the results that we have reported earlier.

Impact of doping on the carrier dynamics in graphene.

We present a microscopic study on the impact of doping on the carrier dynamics in graphene, in particular focusing on its influence on the technologically relevant carrier multiplication in realistic, doped graphene samples. Treating the time- and momentum-resolved carrier-light, carrier-carrier, and carrier-phonon interactions on the same microscopic footing, the appearance of Auger-induced carrier multiplication up to a Fermi level of 300 meV is revealed. Furthermore, we show that doping favors the so-called hot carrier multiplication occurring within one band. Our results are directly compared to recent time-resolved ARPES measurements and exhibit an excellent agreement on the temporal evolution of the hot carrier multiplication for n- and p-doped graphene. The gained insights shed light on the ultrafast carrier dynamics in realistic, doped graphene samples.

Carrier-carrier and carrier-phonon interactions in the dynamics of photoexcited electrons in graphene

In this work we use the Monte Carlo method to simulate the photoexcited carrier relaxation dynamics in suspended monolayer graphene to unveil the role of the different scattering mechanisms involved. The results show a strong activity of carrier-carrier and carrier-optical phonon interactions in the very early stages of the relaxation process driving the thermalization and cooling dynamics. The consideration of the coupling between the electron and phonon population reveals an intense damping in the cooling rates that is dependent on the pumped carrier concentration.

Stacking dependence of carrier interactions in multilayer graphene systems

We identify qualitative trends in the stacking sequence dependence of carrier-carrier interaction phenomena in multilayer graphene. Our theory is based on a new approach which explicitly exhibits the important role in interaction phenomena of the momentum-direction dependent intersite phases determined by the stacking sequence. Using this method, we calculate and compare the self-energies, density--density response functions, collective modes, and ground-state energies of several different few layer graphene systems. The influence of electron--electron interactions on important electronic properties can be understood in terms of competition between intraband exchange, interband exchange and correlation contributions that vary systematically with stacking arrangement.