Carrier Distribution Research Articles

Overcoming the Unfavorable Effects of "Boltzmann Tyranny:" Ultra-Low Subthreshold Swing in Organic Phototransistors via One-Transistor-One-Memristor Architecture.

Organic phototransistors (OPTs), as photosensitive organic field-effect transistors (OFETs), have gained significant attention due to their pivotal roles in imaging, optical communication, and night vision. However, their performance is fundamentally limited by the Boltzmann distribution of charge carriers, which constrains the average subthreshold swing (SSave ) to a minimum of 60mV/decade at room temperature. In this study, an innovative one-transistor-one-memristor (1T1R) architecture is proposed to overcome the Boltzmann limit in conventional OFETs. By replacing the source electrode in an OFET with a memristor, the 1T1R device exploits the memristor's sharp resistance state transitions to achieve an ultra-low SSave of 18mV/decade. Consequently, the 1T1R devices demonstrate remarkable sensitivity to photo illumination, with a high specific detectivity of 3.9 × 109 cm W-1 Hz1/2 , outperforming conventional OPTs (4.9 × 104 cm W-1 Hz1/2 ) by more than four orders of magnitude. The 1T1R architecture presents a potentially universal solution for overcoming the detrimental effects of "Boltzmann tyranny," setting the stage for the development of ultra-low SSave devices in various optoelectronic applications.

A novel dual-parameter proximity and touch sensor using SiO2 nanoparticles and NaCl with commercial acrylic-based encapsulation

This study shows the development and analysis of a novel capacity proximity sensor (CPS) based on a sensing layer made up of a mixture of silicon dioxide nanoparticles (SiO2) and sodium chloride (NaCl), and an encapsulation layer based on a commercial acrylic-based varnish. The encapsulated and non-encapsulated proximity sensors were characterised using impedance spectroscopy (IS), revealing that the resulting impedimetric and capacitance responses exhibit different sensitivities and working sensing ranges. The non-encapsulated sensor presents impedimetric and maximum capacitive sensitivities of 0.0775 cm−1 and -0.9831 cm−1, respectively, within a 2–14 cm sensing range. In contrast, the encapsulated CPS shows maximum impedimetric and capacitive sensitivities of 0.3447 cm−1 and −3.349 cm−1, respectively, and an operation sensing range of 0–3 cm. The results show a 75% decrease in the total sensing range that could be attributed to: (i) a reduction of the effective sensing area due to a reduction of the roughness as demonstrated by SEM analysis, (ii) insulation effects limiting the impact of the material under test (MUT) on the charge carriers distribution, and (iii) decreased charge carrier density involved in the sensing process. Despite the reduced operational range, the encapsulation layer maintains the dual-parameter sensing capabilities, preserves the integrity of the sensing layer, and enables its dual functionality as a proximity and touch sensor. The reported comparison between the encapsulated and non-encapsulated CPSs highlights the effects of the encapsulation layer. The encapsulated version introduces a simple, fast, and cost-effective novel approach for developing CPSs that outperforms some reported CPSs in terms of reliability due to its dual-parameter sensing capability and sensitivity.

Design of p–n heterojunction between CoWO4 and Zn-defective Zn0.3Cd0.7S for efficient photocatalytic H2 evolution

To enhance the efficiency of photocatalytic H2 evolution, numerous methods are employed by increasing the utilization of photogenerated charge carriers (PCCs), including catalyst design, defect regulation, and selection of suitable H+ resources. Using self-assembly method, CoWO4/ZnxCd1−xS with p–n heterojunction was synthesized. Although CoWO4 (CW) cannot produce H2 under visible light irradiation, it can provide photogenerated electrons (e−) to Zn0.3Cd0.7S (ZCS), and largely increase the photocatalytic activity of ZCS. The optimal CW/ZCS composite can reach 15.58 mmol·g−1·h−1, which is 45.8 and 24.3 times higher than the values of the pure CdS and ZCS, respectively. The largely enhanced photocatalytic H2 production is attributed to the Zn vacancies (VZn), p–n heterojunction, and p-chlorobenzyl alcohol (Cl–PhCH2OH) as the H+ source of H2 production. VZn on the ZCS surface as the capture center of photogenerated holes (h+), can regulate the carrier distribution, which results in more photogenerated e− and less generated h+. The combination of p–n heterojunction and VZn can enhance the separation and transfer efficiency of PCCs, and effectively inhibit the recombination of charge carriers. To further improve the utilization rate of PCCs, the photocatalytic H2 evolution is proceeded by Cl–PhCH2OH oxidation in N,N-dimethylformamide solution, with 4-chlorobenzaldehyde (Cl–PhCHO) generated. The separated photogenerated e− and h+ both participated in the redox reaction of H+ reduction and Cl–PhCH2OH oxidation, considering that the amount of H2 and Cl–PhCHO products are close to 1:1. This work not only facilitates the separation and transfer of PCCs, but also provides directions for the design of efficient photocatalysts and H2 evolution in the organic phase.

Hot Carrier Distribution Engineering by Alloying: Picking Elements for the Desired Purposes

Hot Carrier Distribution Engineering by Alloying: Picking Elements for the Desired Purposes

Radiative‐Recombination Thermodynamics in Boron‐Doped Diamond

AbstractBoron‐doped diamond is a wide‐bandgap semiconductor with excellent semiconductor properties, which is widely utilized in various applications. Till now, the thermodynamic rules governing the carrier transitions in this material have not been fully understood. In this research, the different luminescence behaviors of boron‐doped diamond under 193 nm pulse laser with high‐ and low‐ power density excitation are analyzed. Under high‐power density excitation (@≈63 kW cm−2), the emission intensity of excitons is nearly ten times higher than that of defect luminescence. Conversely, under low‐power density excitation (@≈1.4 kW cm−2, different emission peaks exhibit similar intensities, indicating a competitive relationship among them. Based on experimental and theoretical analyses, the difference is attributed to the thermodynamic distribution of carriers at varying excitation powers. Specifically, high excitation power brings an independent behavior of each emission peak, and the exciton emission is described by a phonon‐assisted radiation model; different from that, the competition among different emission centers under the condition of low excitation power cannot be neglected, and now the thermodynamic evolution of each emission peak is described by a carrier trapping‐dissociation model.

Evidence of hot carrier extraction in metal halide perovskite solar cells

AbstractThe presence of hot carriers is presented in the operational properties of an (FA,Cs)Pb(I, Br, Cl)3 solar cell at ambient temperatures and under practical solar concentration. Albeit, in a device architecture that is not suitably designed as a functional hot carrier solar cell. At 100 K, clear evidence of hot carriers is observed in both the high energy tail of the photoluminescence spectra and from the appearance of a nonequilibrium photocurrent at higher fluence in light J–V measurements. At room temperature, however, the presence of hot carriers in the emission at elevated laser fluence is shown to compete with a gradual red shift in the PL peak energy as photoinduced halide segregation begins to occur at higher lattice temperature. The effects of thermionic emission of hot carriers and the presence of a nonequilibrium carrier distribution are also shown to be distinct from simple lattice heating. This results in large unsaturated photocurrents at high powers as the Fermi distribution exceeds that of the heterointerface controlling carrier transport and rectification.

Growth Control of InP/ZnSe Heterostructured Nanocrystals.

The morphology of heterostructured semiconductor nanocrystals (h-NCs) dictates the spatial distribution of charge carriers and their recombination dynamics and/or transport, which are the main performance indicators of photonic applications utilizing h-NCs. The inability to control the morphology of heterovalent III-V/II-VI h-NCs composed of heavy-metal-free elements hinders their practical use. As a case study of III-V/II-VI h-NCs, the growth control of ZnSe epilayers on InP NCs is demonstrated here. The anisotropic morphology in InP/ZnSe h-NCs is attributed to the facet-dependent energy costs for the growth of ZnSe epilayers on different facets of InP NCs, and effective chemical means for controlling the growth rates of ZnSe on different surface planes are demonstrated. Ultimately, this article capitalizes on the controlled morphology of InP/ZnSe h-NCs to expand their photophysical characteristics from stable and pure emission to environment-sensitive one, which will facilitate their use in a variety of photonic applications.

Coherent Terahertz Detection via Ultrafast Dynamics of Hot Dirac Fermions in Graphene.

Graphene has recently been shown to exhibit ultrafast conductivity modulation due to periodic carrier heating by either terahertz (THz) waves, leading to self-induced harmonic generation, or the intensity beat note of two-color optical radiation. We exploit the latter to realize an optoelectronic photomixer for coherent, continuous-wave THz detection, based on a photoconductive antenna with multilayer CVD-grown graphene in the gap. While for biased THz emitters the dark current would pose a serious detriment for performance, we show that this is not the case for bias-free THz detection and demonstrate detection up to frequencies of at least 700 GHz at room temperature, even without optimized tuning of the doping. We account for the photocurrent and photomixing response using detailed simulations of the time-dependent carrier distribution, which also indicate significant potential for enhancement of the sensitivity, to become competitive with well-established semiconductor photomixers.

Plasmon induced hot carrier distribution in Ag20 -CO composite.

The interaction between plasmons and the molecules leads to the transfer of plasmon-induced hot carriers, presenting innovative opportunities for controlling chemical reactions on sub-femtosecond timescales. Through real-time time-dependent density functional theory simulations, we have investigated the enhancement of the electric field due to plasmon excitation and the subsequent generation and transfer of plasmon-induced hot carriers in a linear atomic chain of Ag20 and an Ag20 -CO composite system. By applying a Gaussian laser pulse tuned to align with the plasmon frequency, we observe a plasmon-induced transfer of hot electrons from the occupied states of Ag to the unoccupied molecular orbitals of CO. Remarkably, there is a pronounced accumulation of hot electrons and hot holes on the C and O atoms. This phenomenon arises from the electron migration from the inter-nuclear regions of the C-O bond towards the individual C and O atoms. The insights garnered from our study hold the potential to drive advancements in the development of more efficient systems for catalytic processes empowered by plasmonic interactions.

Multiple-carrier-lifetime model for carrier dynamics in InGaN/GaN LEDs with a non-uniform carrier distribution

We introduce a multiple-carrier-lifetime model (MCLM) for light-emitting diodes (LEDs) with non-uniform carrier distribution, such as in multiple-quantum-well (MQW) structures. By employing the MCLM, we successfully explain the modulation response of V-pit engineered MQW LEDs, which exhibit an S21 roll-off slower than −20 dB/decade. Using the proposed model and employing a gradient descent method, we extract effective recombination and escape lifetimes by averaging the carrier behavior across the quantum wells. Our results reveal slower effective carrier recombination and escape in MQW LEDs compared with LEDs emitting from a single QW, indicating the advantages of lower carrier density achieved through V-pit engineering. Notably, the effective carrier recombination time is more than one order of magnitude lower than the effective escape lifetime, suggesting that most carriers in the quantum wells recombine, while the escape process remains weak. To ensure the reliability and robustness of the MCLM, we subject it to a comprehensive threefold validation process. This work confirms the positive impact of spreading carriers into several quantum wells through V-pit engineering. In addition, the MCLM is applicable to other LEDs with a non-uniform carrier distribution, such as micro-LEDs with significant surface recombination and non-uniform lateral carrier profiles.

Carrier modulation of one-dimensional MAPbxSr1-x(IyCl1-y)3 core-shell perovskite nanowires.

Low dimensional hybrid organic-inorganic perovskites (HOIPs) have become one of the most promising materials in solar cells, photodetectors, and lasers due to their low exciton binding energy, high bipolar carrier mobility, and long carrier lifetime. The effective separation and collection of photo-generated electrons and holes have always been crucial for a perovskite as a working medium for optoelectronic devices. However, the surface state of pristine perovskite nanowires causes recombination of electrons and holes at the edge of the energy band, leading to deactivation of charge carriers. In this work, we constructed MAPbxSr1-xI3 core-shell nanowires, which adjust the band gap and control the spatial distribution of charge carriers by changing the Pb composition ratio, achieving spontaneous separation of electron-hole pairs to avoid surface recombination. In addition, MAPbxSr1-x(IyCl1-y)3 core-shell nanowires with different component ratios (x, y) can be constructed by further doping the Cl element, and the spatial distribution of charge carriers in the nanowires can be flexibly manipulated to achieve exchange between type-I and type-II band alignment orders. This study provides a feasible method for enhancing the carrier separation of organic-inorganic hybrid perovskites and improving the performance of optoelectronic devices.

Pattern-illumination time-resolved phase microscopy and its applications for photocatalytic and photovoltaic materials.

Pattern-illumination time-resolved phase microscopy (PI-PM) is a technique used to study the microscopic charge carrier dynamics in photocatalytic and photovoltaic materials. The method involves illuminating a sample with a pump light pattern, which generates charge carriers and they decay subsequently due to trapping, recombination, and transfer processes. The distribution of photo-excited charge carriers is observed through refractive index changes using phase-contrast imaging. In the PI-PM method, the sensitivity of the refractive index change is enhanced by adjusting the focus position, the method takes advantage of photo-excited charge carriers to observe non-radiative processes, such as charge diffusion, trapping in defect/surface states, and interfacial charge transfer of photocatalytic and photovoltaic reactions. The quality of the image sequence is recovered using various informatics calculations. Categorizing and mapping different types of charge carriers based on their response profiles using clustering analysis provides spatial information on charge carrier types and the identification of local sites for efficient and inefficient photo-induced reactions, providing valuable information for the design and optimization of photocatalytic materials such as the cocatalyst effect.

Temperature dependence of MXenes plasmons induced hot carrier generation and transport

Unlike conventional optoelectronic devices, plasmon-driven optoelectronic devices can efficiently realize energy conversion and regulate the energy distribution of hot carriers through high-energy, non-equilibrium “hot” electron-hole pairs (hot carriers) generated by surface plasmon non-radiative decay, thereby presenting new opportunities for realizing hot carrier optoelectronic devices. As the basis for the practical application of plasmon optoelectronic devices, searching for plasmon metal materials with exceptional performance has always been an important topic in the field of hot carrier optoelectronic devices. Currently, MXenes can be synthesized on a large scale and has excellent photoelectric properties, so it can be used to build a variety of hot carrier photodetectors with unique structures and functions. Unlike the fixed surface ends of two-dimensional materials such as graphene, MoS<sub>2</sub> and borophene, MXenes has an abundance of surface functional groups. However, the increase of ambient temperature will accelerate the oxidation modification of surface functional groups, thus affecting the life and performance stability of optoelectronic devices. In view of the inherent limitations of experimental research on dynamic characteristics of hot carriers at continuous temperatures, we study the temperature effects on the electronic state distributions and scattering effects by using the theory of multi-body perturbation and quantum mechanics. Particularly, we introduce temperature effect into interband electron transition and phonon-assisted electron transition process to obtain temperature dependent dielectric function. From the perspective of non-radiative decay of surface plasmon, we quantify the hot carrier generation efficiency, energy distribution and transport characteristics by first principles calculations, in order to systematically study the ambient temperature dependence of plasmon-induced hot carriers in MXenes. The results show that the interband transition and the phonon-assisted electron transition in MXenes together efficiently produce high-energy hot hole-dominated carriers with a long lifetime and transport distance, which is comparable to borophene. The increase of ambient temperature significantly improves the hot carrier generation efficiency in the infrared range. Meanwhile, the physical mechanism of hot carrier generation in visible light is almost unaffected by the increase of ambient temperature, and the generated hot holes show excellent ambient temperature stability. In addition, the lifetime and transport distance of hot carriers decrease with ambient temperature increasing, which is mainly due to the enhanced scattering of electrons and optical phonons. The research results will provide theoretical and data support for quantitatively evaluating the ambient temperature stability of MXenes plasmon optoelectronic devices in practical environment.

Hot carrier creation in a nanoparticle dimer-molecule composite.

Light-matter interactions have garnered considerable interest owing to their burgeoning applications in quantum optics and plasmonics. Utilizing first principles calculations, this work explores the hot carrier (HC) generation and distribution within a composite system made up of a plasmonic nanoparticle dimer and linear polycyclic aromatic hydrocarbon (PAH) molecules. We examine the spatial and energetic distributions of HCs by initiating photoexcitation and allowing localized surface plasmon dephasing. By positioning PAH molecules within the plasmonic nanodimer's gap region, our investigation uncovers HC tuning. Notably, depending on the size of the PAH molecules, there are significant alterations in the HC distribution. Hot electrons (HEs) are distributed across both the nanodimer and the PAH molecule, while hot holes (HHs) become entirely localized on the PAH as the PAH grows larger. These findings improve our understanding of plasmon-molecule coupled states and provide guidance on how to customize HC distributions through the creation of hybrid plasmonic materials.

Size onset of metallic behavior in neutral aluminum clusters.

The excited state lifetimes of neutral (Al)n clusters up to ∼1 nm in diameter in size, where n ≤ 43, are systematically measured with femtosecond time-resolved mass spectrometry. The onset of metallic behavior is identified as a distinct change in the relaxation behavior initiated with single ultraviolet (400 nm) photon excitation. The experimentally measured excited state lifetimes gradually decrease with size for small molecular scale clusters (n < 10) before becoming indistinguishable for larger clusters (n > 9), where the measurements are comparable to electron-lattice relaxation time of bulk Al (∼300 fs). Particularly intense, or magic, Aln clusters do not exhibit any significant excited state lifetime behavior. Time-dependent density functional theory quantify the excited state properties and are presented to show that dynamics are strongly tied to the excited state charge carrier distributions and overlap, rather than detailed changes related to changes in the cluster's electronic and geometric structure. The consistency in excited state lifetimes for clusters larger than n = 9 is attributed to the hybridization of the s- and p-orbitals as well as increasing delocalization. Al3 exhibits unique temporal delay in its transient behavior that is attributed to a transition from triangular ground state to linear structure upon excitation.

Radiation effects of high-fluence reactor neutron on Ni/ β -Ga2O3 Schottky barrier diodes

This study investigates the broad-energy-spectrum reactor-neutron irradiation effects on the electrical characteristics of Ni/β-Ga2O3 Schottky barrier diodes (SBDs), where the irradiated neutron fluence was up to 1 × 1016 cm−2. On the one hand, the high neutron fluence of 1016 cm−2 resulted in a reduction in forward current density by two orders of magnitude and an extremely high on-resistance property due to the radiation-generated considerable series resistance in the SBD. On the other hand, the irradiation brought little influence on the Ni/β-Ga2O3 Schottky contact, since the extracted ideality factor and barrier height from temperature-dependent current–voltage (I–V–T) characteristics showed no significant changes after the radiation. Moreover, the capacitance–voltage (C–V) characterization revealed that the net carrier density in the β-Ga2O3 material was only reduced by 25% at the neutron fluence of 1015 cm−2 but a significant reduction by 2–3 orders at 1016 cm−2. Within the neutron fluence range of 2 × 1014 cm−2 up to 1016 cm−2, the carrier removal rates trended to be saturated with the increased fluences, following an exponential regular. In addition, the C–V measurement on the 1016 cm−2 irradiated sample exhibited an obvious frequency dispersion, and the extracted carrier distribution was not uniform.

Plasmon-induced hot carrier distribution in a composite nanosystem: role of the adsorption site.

The generation of hot carriers (HCs) through the excitation of localized surface plasmon resonance (LSPR) in metal nanostructures is a fascinating phenomenon that fuels both fundamental and applied research. However, gaining insights into HCs at a microscopic level has posed a complex challenge, limiting our ability to create efficient nanoantennas that utilize these energized carriers. In this investigation, we employ real-time time-dependent density functional theory (rt-TDDFT) calculations to examine the creation and distribution of HCs within a model composite system consisting of a silver (Ag) nanodisk and a carbon monoxide (CO) molecule. We find that the creation and distribution of HCs are notably affected by the CO adsorption site. Particularly, when the CO molecule adsorbs onto the hollow site of the Ag nanodisk, it exhibits the highest potential among various composite systems in terms of structural stability, enhanced orbital hybridization, and HC generation and transfer. Utilizing a Gaussian laser pulse adjusted to match the LSPR frequency, we observe a marked buildup of hot electrons and hot holes on the C and O atoms. Conversely, the region encompassing the C-O bond exhibits a depletion of hot electrons and hot holes. We believe that these findings could have significant implications in the field of HC photocatalysis.

Analysis of the Operation Mechanism of Superjunction in RC-IGBT and a Novel Snapback-Free Partial Schottky Collector Superjunction RC-IGBT.

This paper explores the operation mechanism of the superjunction structure in RC-IGBTs based on carrier distribution and analyzes the advantages and challenges associated with its application in RC-IGBTs for the first time. A Partial Schottky Collector Superjunction Reverse Conduction IGBT (PSC-SJ-RC-IGBT) is proposed to address these issues. The new structure eliminates the snapback phenomenon. Furthermore, by leveraging the unipolar conduction of the Schottky diode and its fast turn-off characteristics, the proposed device significantly reduces the turn-off power consumption and reverse recovery charge. With medium pillar doping concentration, the turn-off loss of the PSC-SJ-RC-IGBT decreases by 54.1% compared to conventional superjunction RC-IGBT, while the reverse recovery charge is reduced by 52.6%.

Leveraging plasmonic hot electrons to quench defect emission in metal-semiconductor nanostructured hybrids.

Modeling light-matter interactions in hybrid plasmonic materials is vital to their widening relevance from optoelectronics to photocatalysis. Here, we explore photoluminescence (PL) from ZnO nanorods (ZNRs) embedded with gold nanoparticles (Au NPs). A progressive increase in Au NP concentration introduces significant structural disorder and defects in ZNRs, which paradoxically quenches defect related visible PL while intensifying the near band edge (NBE) emission. Under UV excitation, the simulated semi-classical model realizes PL from ZnO with sub-bandgap defect states, eliciting visible emissions that are absorbed by Au NPs to generate a non-equilibrium hot carrier distribution. The photo-stimulated hot carriers, transferred to ZnO, substantially modify its steady-state luminescence, reducing NBE emission lifetime and altering the abundance of ionized defect states, finally reducing visible emission. The simulations show that the change in the interfacial band bending at the Au-ZnO interface under optical illumination facilitates charge transfer between the components. This work provides a general foundation to observe and model the hot carrier dynamics and strong light-matter interactions in hybrid plasmonic systems.

Dark Current Mechanisms and Suppression Strategies for Infrared Photodetectors Based on Two‐Dimensional Materials

AbstractNarrow‐bandgap 2D materials and semimetals, for example, graphene, black phosphorus (BP), tellurium (Te), and some novel transition metal dichalcogenides (TMDs), have been demonstrated to be promising building blocks for constructing next‐generation state‐of‐the‐art infrared (IR) photodetectors. However, these devices suffer from a significant dark current, primarily attributed to the intrinsic thermal excitation‐induced high carrier concentration. Suppressing the dark current is an essential issue in pursuing higher specific detectivity of IR photodetectors. Here, the authors demonstrate recent advances in suppressing dark current for 2D IR photodetectors. First, a brief insight into the dark current composition and mechanisms of 2D IR photodetectors is illustrated. Then, the varied band alignment for blocking dark current by the interfacial barrier is discussed. Next, localized electric field modulation by applying a gate voltage and ferroelectric materials is discussed. This method can effectively tune the concentration and distribution of carriers in the device conductive channel. Following that, interfacial engineering is summarized, by which interfacial defects can be passivated and interlayer defect‐induced dark current can be suppressed. Finally, the challenges and an outlook are delivered for developing state‐of‐the‐art IR photodetectors.