Carrier Diffusion Research Articles

Quantitative photothermal investigation of nonradiative recombination parameters in GaAs/InAs(QD)/GaAs quantum dot structures using a three-layer laser beam deflection model

In this paper, we developed a theoretical model for the photothermal deflection technique in order to investigate the electronic parameters of three-layer semiconductor structures. This model is based on the resolution of thermal and photogenerated carrier diffusion-wave equations in different media. Theoretical results show that the amplitude and phase of the photothermal deflection signal is very sensitive to the nonradiative recombination parameters. The theoretical model is applied to one layer of InAs quantum dots (QDs) inserted in GaAs matrix InAs/GaAs QDs in order to investigate the QD density effects on nonradiative recombination parameters in InAs through fitting the theoretical photothermal beam deflection signal to the experimental data. It was found that the minority carrier lifetime and the electronic diffusivity decrease as functions of increasing InAs QD density. This result is also related to the decrease in the mobility from 21.58 to 4.17 (±12.9%) cm2/V s and the minority carrier diffusion length from 0.62 (±5.8%) to 0.14 (±10%) μm, respectively. Furthermore, both interface recombination velocities S2/3 of GaAs/InAs (QDs) and S1/2 of InAs (QDs)/GaAs increase from 477.7 (±6.2%) to 806.5 (±4%) cm/s and from 75 (±7.8%) to 148.1 (±5.5%) cm/s, respectively.

As‐Doped Polycrystalline CdSeTe: Localized Defects, Carrier Mobility and Lifetimes, and Impact on High‐Efficiency Solar Cells

AbstractThe efficiency potential for single‐junction photovoltaics (PV) is described by the detailed balance model, which requires the elimination of nonradiative recombination and perfect minority carrier collection. Improvements in GaAs, Si, and perovskite PV follow this model. It might be more complex for CdTe, a leading thin‐film PV technology. While lifetime, passivation, and doping goals for 25% efficient CdTe solar cells are largely reached, voltage is ≈20% below the detailed balance limit. Why is that? In Se‐alloyed CdSexTe1‐x (Se is required for >20% efficiency) additional losses can occur due to electrostatic and bandgap fluctuations and due to electronic trap states. To understand mechanisms limiting CdSeTe solar cell performance and to suggest improvements, carrier dynamics, and transport in CdSexTe1‐x with variation in Se composition and as doping is analyzed. It is shown that trapping, likely due to anion‐site defects and their complexes, is correlated with low charge carrier mobility of 0.1–0.6 cm2 (Vs)−1. Even with 1000 ns charge carrier lifetimes, carrier diffusion length is less than the absorber thickness, reducing efficiency to ≈23%. Device simulations are used to analyze the performance of CdSexTe1‐x solar cells; thermodynamic models are not sufficient for absorbers with electronic disorder and trapping.

Strong Grain Boundary Passivation Effect of Coevaporated Dopants Enhances the Photoemission of Lead Halide Perovskites.

Herein, we demonstrate that coevaporated dopants provide a means to passivate buried interfacial defects occurring at perovskite grain boundaries in evaporated perovskite thin films, thus giving rise to an enhanced photoluminescence. By means of an extensive photophysical characterization, we provide experimental evidence that indicate that the codopant acts mainly at the grain boundaries. They passivate interfacial traps and prevent the formation of photoinduced deep traps. On the other hand, the presence of an excessive amount of organic dopant can lead to a barrier for carrier diffusion. Hence, the passivation process demands a proper balance between the two effects. Our analysis on the role of the dopant, performed under different excitation regimes, permits evaluation of the performance of the material under conditions more adapted to photovoltaic or light emitting applications. In this context, the approach taken herein provides a screening method to evaluate the suitability of a passivating strategy prior to its incorporation into a device.

Monte Carlo Simulation of Electron Beam Induced Current in Au/Si Schottky Diodes: effects of metal layer thickness and minority carrier diffusion length

The Electron Beam Induced Current (EBIC) technique, when combined with scanning electron microscopy (SEM), offers valuable insights into the electronic properties of semiconductor materials at the nanoscale. This study leverages EBIC and Monte Carlo simulations to investigate the behavior of Schottky diodes, particularly focusing on the influence of gold layer thickness on current gain and backscatter electron (BSE) yield. The simulation results reveal the significant effects of depletion depth and minority carrier diffusion length on the diode’s performance. A key finding is that the EBIC current decreases with increased gold layer thickness, due to a higher BSE fraction. Additionally, at low beam energies, the current is negligible when the interaction volume is confined within the metal layer, while at higher energies, some penetration into the semiconductor occurs, generating a measurable EBIC current. These findings provide a better understanding of the interplay between metal layer thickness and semiconductor performance, which is crucial for optimizing semiconductor devices.

DFT and AIMD Evaluation of Boron‐Doped Biphenylene as an Anode Material in Lithium‐ and Sodium‐Ion Batteries

AbstractDesign and proposal of high‐efficiency anode materials are crucial for the development of batteries with enhanced power and energy density, a key factor in their commercialization. This study presents a comparative theoretical study to evaluate the potential of boron‐doped biphenylene (B‐BP) as an anode electrode in lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). Current research investigates the impact of boron doping on the structural, electronic, and stability properties of pristine biphenylene. Computational calculations reveal strong interactions between charge carriers (Li and Na atoms) and the proposed anode with a charge transfer from Li/Na atom to the surface. According to kinetic studies, a low energy barrier for charge carrier diffusion has been obtained which makes it a promising candidate for fast‐charge battery applications. Theoretical capacity calculations show that B‐BP outperforms graphite as the commercial case of anode material, with calculated values of 560.67 mAh g−1 for Li and 934.45 mAh g−1 for Na storage.

Boosting the Quantum Efficiency of Ionic Carbon Nitrides in Photocatalytic H2O2 Evolution via Controllable n → π* Electronic Transition Activation.

Hydrogen peroxide (H2O2) is a crucial chemical used in numerous industrial applications, yet its manufacturing relies on the energy-demanding anthraquinone process. Solar-driven synthesis of H2O2 is gaining traction as a promising research area, providing a sustainable method for its production. Herein, a controllable activation of n → π* electronic transition is presented to boost the photocatalytic H2O2 evolution in ionic carbon nitrides. This enhancement is achieved through the simultaneous introduction of structural distortions and defect sites (─C ≡ N groups and N vacancies) into the KPHI framework. The optimal catalyst (2%Ox-KPHI) reached an apparent quantum yield of 41% at 410nm without the need for any cocatalysts, outperforming most previously reported carbon nitride-based photocatalysts. Extensive experimental characterizations and theoretical calculations confirm that a corrugated configuration and the presence of defects significantly broaden the light absorption profile, improve carrier separation and migration, promote O2 adsorption, and lower the energy barriers for H2O2 desorption. Transient absorption spectroscopy indicates that the enhanced photocatalytic performance of 2%Ox-KPHI is largely attributed to the preferential migration of electrons at defect sites over extended timescales, following the diffusion of geminate carriers across the PHI sheets.

Disentangling the Optoelectronic Behavior of Lead Iodide Governed by Two-Dimensional Electron Confinement.

We present a joint experimental and theoretical study for complete spectroscopic characterization and optoelectronic properties of lead iodide. Experimentally, we combine X-ray diffraction experiments to elucidate the structure with photoelectron spectroscopy to explore its electronic structure. Computationally, simulations are performed in the frame of density functional theory. We show that PbI2 presents a two-dimensional layered structure and exhibits a large transient photocurrent effect under visible light illumination, which are compatible with the surface photovoltage scenario. The transient photocurrent has an extremely long lifetime: when the sample is lightened with visible light, it shows very long relaxation times and, consequently, huge charge carrier diffusion lengths. We explain this anomalous behavior with the slow carrier mobility of holes and electrons caused by the 2D electron confinement in the layered material. Our results can be used as a simple model for understanding the optoelectronic properties of more complex 2D hybrid perovskites.

Phase Distribution Dictates Charge Transfer and Transport Dynamics in Layered Quasi-2D Perovskite.

Strategic manipulation of spatiotemporal evolution of charge carriers is critical for optimizing performance of quasi-two-dimensional (2D) perovskite-based optoelectronic devices. Nonetheless, the inhomogeneous phase distribution and band alignment engender intricate energy landscapes, complicating internal charge and energy funneling processes. Herein, we integrate high spatiotemporal resolution transient absorption microscopy with multiple time-resolved spectroscopy and find that asynchronous electron and hole transfers rather than direct energy transfer govern the funneling mechanisms. Notably, the charge funneling pathways and transport behaviors can be modifiable by phase manipulation. The accumulation of small-n phases suppresses the electron funneling toward large-n phases and doubles the carrier diffusion rate from 0.085 to 0.20 cm2/s, yielding a 1.5-fold enhancement in diffusion length. Phase order engineering is further corroborated for facilitating charge separation. Our investigation underscores the prospects of manipulating the phase distribution to control internal charge funneling and transport, thereby substantiating the theoretical foundations for optimizing optoelectronic devices.

Defect Passivation of Mn2+-Doped CsPbX3(X=Cl,Br) Perovskite Nanocrystals as Electriccatalyst for Overall Water Splitting.

Mn:CsPbX3(X= Cl, Br) nanosheets with excellent electrocatalytic properties are reported in this paper. Compared to conventional catalyst arrays, the band gap of Mn:CsPbBr3nanocrystalline is easily tuned, the carrier diffusion distance is remote, the band edge position of the band structure is favorable for a wide range of electrocatalytic redoxreactions, and the catalytic active site is maximally exposed.The Mn:CsPbBr3exhibited preferable electrocatalytic hydrogen evolution(HER)performance in 1 mol/L KOH. The excess potential of the oxygen evolution reaction(OER) required to drive current densities of 10 and 100 mAcm-2is only 114.4and 505.4mV, with a Tafel slope of 43 mVdec-1. At a current density of 10 mAcm-2, the excess potential required for the HERis 158.6mV and it exhibitedexcellent electrochemical stability. The Mn:CsPbBr3nanocrystalline consists of two electrodes for the overallwater splitting, requiring a voltage of only 1.45V. Which in turn provides implications for the optimization of electrocatalysts in alkaline electrolytes with the aim of developing the next generation of 2D electrocatalysts for overallwater splitting.

Solution-Processed Micro-Nanostructured Electron Transport Layer via Bubble-Assisted Assembly for Efficient Perovskite Photovoltaics.

Organic-inorganic halide perovskite solar cells (PSCs) have attracted significant attention in photovoltaic research, owing to their superior optoelectronic properties and cost-effective manufacturing techniques. However, the unbalanced charge carrier diffusion length in perovskite materials leads to the recombination of photogenerated electrons and holes. The inefficient charge carrier collecting process severely affects the power conversion efficiency (PCE) of the PSCs. Herein, a solution-processed SnO2 array electron transport layer with precisely tunable micro-nanostructures is fabricated via a bubble-template-assisted approach, serving as both electron transport layers and scaffolds for the perovskite layer. Due to the optimized electron transporting pathway and enlarged perovskite grain size, the PSCs achieve a PCE of 25.35% (25.07% certificated PCE).

Gradient-doped BiVO4 Dual Photoanodes for Highly Efficient Photoelectrochemical Water splitting.

Bismuth vanadate (BiVO4) is regarded as a promising photoanode candidate for photoelectrochemical (PEC) water splitting, but is limited by low efficiency of charge carrier transport and short carrier diffusion length. In this work, we report a strategy comprised of the gradient doping of W and back-to-back stacking of transparent photoelectrodes, where the 3-2 wt.% W gradient doping enhances charge carrier transport by optimizing the band bending degree and back-to-back stack configuration shortens carrier diffusion length without much sacrifice of photons. As a result, the photocurrent density of 3-2% W:BiVO4 photoanode reaches 2.20 mA cm-2 at 1.23 V vs. hydrogen electrode (RHE) with a charge transport efficiency of 76.1% under AM 1.5G illumination, and the back-to-back stacked 3-2% W:BiVO4 photoanodes achieves a photocurrent of 4.63 mA cm-2 after loading Co-Pi catalyst and anti-reflective coating under AM 1.5G illumination, with long-term stability of 10 hours.

Minimal-gain-printed silicon nanolaser.

While there have been notable advancements in Si-based optical integration, achieving compact and efficient continuous-wave (CW) III-V semiconductor nanolasers on Si at room temperature remains a substantial challenge. This study presents an innovative approach: the on-demand minimal-gain-printed Si nanolaser. By using a carefully designed minimal III-V optical gain structure and a precise on-demand gain-printing technique, we achieve lasing operation with superior spectral stability under pulsed conditions and observe a strong signature of CW operation at room temperature. These achievements are attributed to addressing both fundamental and technological issues, including carrier diffusion, absorption loss, and inefficient thermal dissipation, through minimal-gain printing in the nanolaser. Moreover, our demonstration of the laser-on-waveguide structure emphasizes the integration benefits of this on-demand gain-printed Si nanolaser, highlighting its potential significance in the fields of Si photonics and photonic integrated circuits.

Using TiO2 to capture hot electrons for self-powered position-sensitive photodetection.

As environmental issues arise, the demand for self-powered position-sensitive detectors (PSDs) is increasing because of their advantages in miniaturization and low power consumption. Finding higher efficiency schemes for energy conversion is paramount for realizing high-performance self-powered PSDs. Here, a surface plasmon-based approach was used to improve the energy conversion efficiency, and a plasmon-enhanced lateral photovoltaic effect (LPE) was observed in PSD with TiO2/Au nanorods (NRs)/Si structure. The Au NRs convert absorbed light energy into electricity by generating hot electrons, which are efficiently captured by the TiO2 layer, and the PSD is capable of generating position sensitivity as high as 251.75 mV/mm when illuminated by a 780 nm laser without any external power supply, i.e. about five times higher than similar sensors in previous studies. In addition, the position sensitivity can be tailored by the thickness of TiO2 films. The enhancement mechanism is investigated by a localized surface plasmon (LSP)-driven carrier diffusion model. These findings reveal an important strategy for high sensitivity and low energy cost PSDs while opening up new avenues for energy harvesting self-powered position sensors.

Assessment of photovoltaic efficacy in antimony-based cesium halide perovskite utilizing transition metal chalcogenide

Antimony-based perovskites have been recognized for their distinctive optoelectronic attributes, standard fabrication methodologies, reduced toxicity, and enhanced stability. The objective of this study is to systematically investigate and enhance the performance of all-inorganic solar cell architectures by integrating Cs3Sb2I9, a perovskite-analogous material, with WS2—a promising transition metal dichalcogenide—used as the electron transport layer (ETL), and Cu2O serving as the hole transport layer (HTL). This comprehensive assessment extends beyond the mere characterization of material attributes such as layer thickness, doping levels, and defect densities, to include a thorough investigation of interfacial defect effects within the structure. Optimal efficiency was observed when the Cs3Sb2I9 absorber layer thickness was maintained within the 600-700 nm range. The defect tolerance for the absorber layer was identified at 1×1015/cm3, with the ETL and HTL layers exhibiting significant defect tolerance at 1×1016/cm3 and 1×1017/cm3, respectively. Furthermore, this study calculated the minority carrier lifetime and diffusion length, establishing a strong correlation with defect density; a minority carrier lifetime of approximately 1 µs was noted for a defect density of1×1014/cm3 in the absorber layer. A noteworthy finding pertains to the balance between the high work function of the back contact and the incorporation of p-type back surface field layers, revealing that interposing a highly doped p+ layer between the Cu2O and the metal back contact can elevate the efficiency to 21.60%. This approach also provides the freedom to select metals with lower work functions, offering a cost-effective advantage for commercial-scale applications.

A stochastic Schrödinger equation and matrix product state approach to carrier transport in organic semiconductors with nonlocal electron-phonon interaction.

Evaluation of the charge transport property of organic semiconductors requires exact quantum dynamics simulation of large systems. We present a numerically nearly exact approach to investigate carrier transport dynamics in organic semiconductors by extending the non-Markovian stochastic Schrödinger equation with complex frequency modes to a forward-backward scheme and by solving it using the matrix product state (MPS) approach. By utilizing the forward-backward formalism for noise generation, the bath correlation function can be effectively treated as a temperature-independent imaginary part, enabling a more accurate decomposition with fewer complex frequency modes. Using this approach, we study the carrier transport and mobility in the one-dimensional Peierls model, where the nonlocal electron-phonon interaction is taken into account. The reliability of this approach was validated by comparing carrier diffusion motion with those obtained from the hierarchical equations of motion method across various parameter regimes of the phonon bath. The efficiency was demonstrated by the modest virtual bond dimensions of MPS and the low scaling of the computational time with the system size.

In situ tracking anisotropic photocarrier dynamics in two-dimensional ternary Ta2NiSe5 via digital micromirror device-based pump-probe microscopy

In two-dimensional (2D) material studies, tracking the anisotropic ultrafast carrier dynamics is essential for the development of optoelectronic nano-devices. Conventionally, the anisotropic optical and electronic properties are investigated via either polarization-dependent Raman spectroscopy or field-effect transistors measurements. However, study of the anisotropic transient carrier behaviors is still challenging, due largely to the lack of picosecond-resolved acquisition or programmable scanning capabilities in the current characterization systems. In this work, we select Ta2NiSe5 as a model system to investigate the ultrafast anisotropic transportation properties of photo-excited carriers and transient polarized responses via a digital micromirror device (DMD)-based pump-probe microscope, where the probe beam scans along the armchair and zigzag directions of a crystal structure via binary holography to obtain distinct carrier diffusion coefficients, respectively. The results reveal the nonlinear diffusion behaviors of Ta2NiSe5 in tens of picoseconds, which are attributed to the interplay between excited electrons and phonons. The trend of the measured local polarization-dependent transient reflectivity is consistent with the polarized Raman spectra results. These results show that the DMD-based pump-probe microscope is an effective and versatile tool to study the optoelectronic properties of 2D materials.

Magneto-photo-thermoelastic influences on a semiconductor hollow cylinder via a series-one-relaxation model

This article discusses the deformation of semiconductor cylinders in the context of photothermoelastic theory. The proposed model is used to describe thermal waves, plasma waves, and elastic waves and analyze the theoretical analysis of thermal deformation effects on semiconductor hollow cylinders. The interior of the hollow cylinder is clamped and unaffected by thermal loads and carrier concentrations, while the exterior is subject to sinusoidal heating and limited carrier density. In addition, the surface of the cylinder is surrounded by magnets in the direction of its axis. Initially, the governing equations are explained in Laplace domain and the Laplace inversion is used numerically. The results from thermal physics are presented graphically to investigate the impact of thermal relaxation and temperature on temperature of plasma thermoelastic waves. The effects of carrier diffusion coefficient and surface recombination rate on carrier concentration distribution are also discussed in detail.

Perovskite versus Standard Photodetectors.

Perovskites have been largely implemented into optoelectronics as they provide several advantages such as long carrier diffusion length, high absorption coefficient, high carrier mobility, shallow defect levels and finally, high crystal quality. The brisk technological development of perovskite devices is connected to their relative simplicity, high-efficiency processing and low production cost. Significant improvement has been made in the detection performance and the photodetectors' design, especially operating in the visible (VIS) and near-infrared (NIR) regions. This paper attempts to determine the importance of those devices in the broad group of standard VIS and NIR detectors. The paper evaluates the most important parameters of perovskite detectors, including current responsivity (R), detectivity (D*) and response time (τ), compared to the standard photodiodes (PDs) available on the commercial market. The conclusions presented in this work are based on an analysis of the reported data in the vast pieces of literature. A large discrepancy is observed in the demonstrated R and D*, which may be due to two reasons: immature device technology and erroneous D* estimates. The published performance at room temperature is even higher than that reported for typical detectors. The utmost D* for perovskite detectors is three to four orders of magnitude higher than commercially available VIS PDs. Some papers report a D* close to the physical limit defined by signal fluctuations and background radiation. However, it is likely that this performance is overestimated. Finally, the paper concludes with an attempt to determine the progress of perovskite optoelectronic devices in the future.

(Invited) Exciton Dissociation in Mixed-Dimensionality SWCNT-Based Heterojunctions

Quantum-confined semiconductors provide highly tunable optical and electrical properties for a wide variety of emerging applications. Semiconducting single-walled carbon nanotubes (s-SWCNTs) have shown tremendous potential in applications ranging from digital logic, biological imaging, quantum information processing, photovoltaics, and thermoelectric energy harvesting. Energy harvesting applications rely critically upon the creation of tailored interfaces that enable the movement of energetic species (excitons, electrons, holes) in specified directions. In this talk, I will discuss the use of a variety of rationally designed “mixed-dimensionality” heterojunctions between s-SWCNTs and transition metal dichalcogenide (TMDC) monolayers to harvest visible/near-infrared photons and convert these excitations into long-lived charge-separated states. Type-II heterojunctions between s-SWCNTs and TMDCs enable rapid exciton dissociation and microsecond charge-separated state lifetimes. We have developed new TMDC/SWCNT/TMDC trilayer architectures that enable charge transfer cascades for improving charge separation yield and lifetime. These trilayer architectures allow us to probe out-of-plane carrier diffusion in the nanotube layer and the degree to which bound interfacial excitons impact the photophysics in these mixed-dimensionality heterostructures. I will also discuss the methodology by which we attempt to quantify the photoinduced exciton dissociation quantum yields in these nanoscale heterostructures. Using several heterostructure results, we are attempting to narrow in on appropriate ways to quantify the local dielectric constant and exciton size in both the SWCNT and TMDC components, each of which impact the estimated charge carrier yields. Taken together, these studies provide fundamental insights into the links between ground-state thermodynamics and excited-state dynamics for model nanoscale heterojunctions used to harvest solar energy and produce long-lived charge-separated states.

Electrospun Nano-Porous Cellulose Acetate Membrane Casted with Chitosan for Solid-State Sodium-Ion Batteries

Emerging as a safe and economically viable alternative to lithium-ion batteries, the solid-state sodium ion battery (ss-SIB) has captured increasing attention as a transformative technology for realizing a decarbonized economy and ensuring a sustainable energy supply. Here we report a nanoarchitecture strategy of biodegradable, biocompatible, and naturally abundant cellulose derivative (cellulose acetate, CA) and chitosan (CH) biopolymer-based nano-porous electrospun composite electrolyte (ECE) for flexible and wearable ss-SIBs. A simple combination of electrospinning and solution casting was utilized to fabricate mechanically robust (13.76 MPa), thin-film (0.067 mm), highly flexible, and high room temperature Na-ion conductive (1.04 x 10-4 S.cm-2) ECE. Lower activation energy (Ea = 0.13 eV) indicates easy charge carrier diffusion ability of as prepared ECE. The electrochemical stability window (ESW = 3.45 V) of ECE is studied by the linear sweep voltammetry (LSV) with respect to stainless steel and sodium metal electrodes. Uniform galvanostatic Na plating and stripping at room temperature is observed over 900 hrs at 0.5 mA•cm-2 current density in symmetric (Na|ECE|Na) cell performance, this underscores impressive electrochemical stability and compatibility with sodium metal. Using Na3V2(PO4)3 (NVP) as cathode, ECE, and Na metal as anode in the full cell, specific discharge capacity of 83 mA×h×g-1 at room temperature was attained at 0.1 C rate, highlighting the practical applicability of the nanostructured electrospun composite electrolyte for flexible and wearable ss-SIBs. Keywords Cellulose acetate, chitosan, electrospun, solid-state sodium-ion battery, specific discharge capacity.