Hot Electron Transport Research Articles

Plasmonic Ag-nanoparticles decorated phosphorus and boron co-doped g-C3N4 for enhanced photocatalytic H2 production

Solar water splitting by semiconductor photocatalysts has emerged as a favorable approach for green hydrogen production. Graphitic carbon nitride (g-C3N4) has gained substantial recognition amongst numerous semiconductor photocatalysts as a metal-free semiconductor with suitable band gap, appropriate band edge positions, and satisfactory photocatalytic activity for hydrogen production. However, its practical application is severely affected by high charge carrier recombination rate and inefficient visible light absorption. Introducing non-metal dopants into the g-C3N4 structure could suppress charge carrier recombination and tune the electronic property. Also, metal nanoparticles exhibit surface plasmon resonance (SPR) upon light interaction increasing the visible light absorption by the transport of hot electrons into the g-C3N4 framework. In this work, we report hybrid photocatalytic materials containing Ag-plasmonic metal and non-metal (B/P) dual heteroatom-doped g-C3N4 prepared via in-situ thermal polycondensation and succeeded by the photodeposition of Ag NPs. The structure of the prepared materials was studied through PXRD and FTIR spectroscopy; XPS was used for chemical analysis; SEM was used to study the morphology; and optical characteristics were studied through UV–Vis and PL spectroscopic techniques. The synergistic effects of SPR and heteroatom co-doping exhibit superior photocatalytic hydrogen production compared to pristine, B or P individual-doped, and B/P co-doped g-C3N4 samples. The optimized 1Ag/PBCN photocatalyst has demonstrated the highest photocatalytic hydrogen production rate of 1825 μmolh-1g−1, 18.3 times greater than g-C3N4. The modified hybrid material shows better activity due to the efficient charge carriers separation and extended visible light absorption. This work indicates that elemental co-doping and loading plasmonic nanoparticles on g-C3N4 to form hybrid nanocomposites may be a potential strategy to achieve better photocatalytic hydrogen evolution. The proposed methodology and outcomes will be helpful in the design and development of plasmon-enhanced hybrid photocatalysts for solar-driven green hydrogen production from water splitting.

Spin-polarized hot electron transport versus spin pumping mediated by local heating

A ‘toy model’—aimed at capturing the essential physics—is presented that jointly describes spin-polarized hot electron transport and spin pumping driven by local heating. These two processes both contribute to spin-current generation in laser-excited magnetic heterostructures. The model is used to compare the two contributions directly. The spin-polarized hot electron current is modeled as one generation of hot electrons with a spin-dependent excitation and relaxation scheme. Upon decay, the excess energy of the hot electrons is transferred to a thermalized electron bath. The elevated electron temperature leads to an increased rate of electron-magnon scattering processes and yields a local accumulation of spin. This process is dubbed as spin pumping by local heating. The built-up spin accumulation is effectively driven out of the ferromagnetic system by (interfacial) electron transport. Within our model, the injected spin current is dominated by the contribution resulting from spin pumping, while the hot electron spin current remains relatively small. We derive that this observation is related to the ratio between the Fermi temperature and Curie temperature, and we show what other fundamental parameters play a role.

Comprehensively analysis of hot electron transport in as-grown and thermally annealed n-type modulation-doped Al0.15Ga0.85As/GaAs0.96Bi0.4 quantum well structure

We report experimental and analytical results on hot electron transport in as-grown and thermally annealed n-type modulation-doped Al0.15Ga0.85As/GaAs0.96Bi0.4 quantum well (QW) structures at room temperature. The drift mobility of as-grown and thermally annealed samples is 2265 and 1414 cm2/Vs at a low electric field region, respectively. The lower electric field electron mobility for the thermally annealed sample is due to the increased 2D electron density following the annealing process. The drift velocity (vdrift) of the as-grown sample tends to saturate at 6.1 × 106 cm/s, contrary to the thermally annealed sample, for which no saturation is observed. The vdrift of the annealed sample is also lower due to the higher 2D electron density caused by annealing. Analyzing the experimental results concerning the theoretical model reveals that i) hot electron transport occurs in parallel mode due to the presence of electrons in both Al0.15Ga0.85As (barrier) and QW layers, ii) hot electrons transferred from QW to the barrier layer via so-called real space transfer (RST) mechanism is suppressed at higher electric fields even though the lower energy barrier between the barrier and QW layers, and iii) transfer of electrons from QW (Γ-valley) to the nearest L-valley, inter-valley transfer (IVT), dominates on the hot electron transfer at higher electric fields even with a higher energy barrier.

3D Monte-Carlo model to study the transport of hot electrons in the context of inertial confinement fusion. Part I

We describe the development of a 3D Monte-Carlo model to study hot-electron transport in ionized or partially ionized targets, considering regimes typical of inertial confinement fusion. Electron collisions are modeled using a mixed simulation algorithm that considers both soft and hard scattering phenomena. Soft collisions are modeled according to multiple-scattering theories, i.e., considering the global effects of the scattering centers on the primary particle. Hard collisions are simulated by considering a two-body interaction between an electron and a plasma particle. Appropriate differential cross sections are adopted to correctly model scattering in ionized or partially ionized targets. In particular, an analytical form of the differential cross section that describes a collision between an electron and the nucleus of a partially ionized atom in a plasma is proposed. The loss of energy is treated according to the continuous slowing down approximation in a plasma stopping power theory. Validation against Geant4 is presented. The code will be implemented as a module in 3D hydrodynamic codes, providing a basis for the development of robust shock ignition schemes and allowing more precise interpretations of current experiments in planar or spherical geometries.

3D Monte-Carlo model to study the transport of hot electrons in the context of inertial confinement fusion. Part II

We describe two numerical investigations performed using a 3D plasma Monte-Carlo code, developed to study hot-electron transport in the context of inertial confinement fusion. The code simulates the propagation of hot electrons in ionized targets, using appropriate scattering differential cross sections with free plasma electrons and ionized or partially ionized atoms. In this paper, we show that a target in the plasma state stops and diffuses electrons more effectively than a cold target (i.e., a target under standard conditions in which ionization is absent). This is related to the fact that in a plasma, the nuclear potential of plasma nuclei has a greater range than in the cold case, where the screening distance is determined by the electronic structure of atoms. However, in the ablation zone created by laser interaction, electrons undergo less severe scattering, counterbalancing the enhanced diffusion that occurs in the bulk. We also show that hard collisions, i.e., collisions with large polar scattering angle, play a primary role in electron beam diffusion and should not be neglected. An application of the plasma Monte-Carlo model to typical shock ignition implosions suggests that hot electrons will not give rise to any preheating concerns if their Maxwellian temperature is lower than 25–30 keV, although the presence of populations at higher temperatures must be suppressed. This result does not depend strongly on the initial angular divergence of the electron beam set in the simulations.

Controllable hot electron transfer in the Ag/MoO3 layer by layer system: Thickness-dependent MoO3 layer

The Ag and MoO3 layer-by-layer sputtering method was employed to fabricate Ag/MoO3 coated on a polystyrene (PS) array (Ag/MoO3@PS), which exhibited excellent surface-enhanced Raman scattering (SERS) activity. The thickness of the MoO3 layer was controlled by changing the sputtering power. The SERS intensity of 4-aminothiophenol (PATP) on Ag/MoO3@PS with a 2 nm thickness of the MoO3 layer was comparable to that on pure Ag coated on the PS array (Ag@PS). This is possible because hot electrons were injected from Ag into the MoO3 layer to enhance the photocatalyst reaction; thus, the SERS spectra of coupled PATP were obtained. The transport of hot electrons rapidly decayed and was blocked with increasing thickness of the MoO3 layer from 2 nm to 9 nm. Thus, the SERS intensity decreased, and interestingly, the b2 mode of PATP decreased and nearly disappeared. This study provides new insight into the control of hot electron reduction for catalytic reduction process monitoring.

Influence of band structure on ballistic transport revealed by molecular nanoprobe

In this study we characterize the tautomerization of HPc on Cu(111) as a charge-carrier-induced reversible one-electron process. An analysis of the bias-dependent tautomerization rate finds an energy threshold that corresponds to the energy of the N-H stretching mode. By using the tautomerization of the molecule as a detector for charge carrier transport in the so-called molecular nanoprobe (MONA) technique, we provide evidence for an inhomogeneous coupling between the fourfold-symmetric molecule and sixfold-symmetric surface. We conclude the study by comparing the energy dependence of charge carrier transport on the Cu(111) to the Ag(111) surface. While the MONA technique is limited to the detection of hot-electron transport for Ag(111), our data reveal that the lower onset energy of the Cu surface state also allows for the detection of hot-hole transport. The influence of surface and bulk transport on the MONA technique is discussed.

Ultrafast transport and energy relaxation of hot electrons in Au/Fe/MgO(001) heterostructures analyzed by linear time-resolved photoelectron spectroscopy

In condensed matter, scattering processes determine the transport of charge carriers. In case of heterostructures, interfaces determine many dynamic properties like charge transfer and transport and spin current dynamics. Here we discuss optically excited electron dynamics and their propagation across a lattice-matched, metal-metal interface of single crystal quality. Using femtosecond time-resolved linear photoelectron spectroscopy upon optically pumping different constituents of the heterostructure we establish a technique which probes the electron propagation and its energy relaxation simultaneously. In our approach a near-infrared pump pulse excites electrons directly either in the Au layer or in the Fe layer of epitaxial Au/Fe/MgO(001) heterostructures while the transient photoemission spectrum is measured by an ultraviolet probe pulse on the Au surface. Upon femtosecond laser excitation, we analyze the relative changes in the electron distribution close to the Fermi energy and assign characteristic features of the time-dependent electron distribution to transport of hot and non-thermalized electrons from the Fe layer to the Au surface and vice versa. From the measured transient electron distribution we determine the excess energy which we compare with a calculation based on the two-temperature model and takes diffusive electron transport into account. On this basis we identify a transition from a super-diffusive to a diffusive transport regime to occur for a Au layer thickness of 20-30~nm.

Anti-oil-fouling Au/BiOCl coating for visible light-driven photocatalytic inactivation of bacteria

In this work, gold/bismuth oxychloride (Au/BiOCl) nanocomposites with different morphologies were successfully prepared by simple solvothermal method and sodium borohydride reduction method, which exhibited significantly efficient visible-light-driven photocatalytic disinfection for Staphylococcus aureus (S.aureus). Particularly, the flower-like Au/BiOCl nanocomposite showed the highest photocatalytic bactericidal performance among the prepared Au/BiOCl samples. The radical trapping experiments revealed that the hole was the main reactive species responsible for the inactivation of S.aureus over Au/BiOCl composite. The enhanced photocatalytic bactericidal effect could be attributed to the enhanced adsorption intensity of visible light that originated from the surface plasmon resonance (SPR) effect of Au, rapid transfer and space transport of hot electrons caused by the hierarchical structure of BiOCl layered compound. Furthermore, the Au/BiOCl coating prepared on stainless steel wire mesh via in-situ synthesis method exhibited excellent superhydrophilic/underwater superoleophobic performance, which endowed the coating with anti-oil-fouling in water. More importantly, compared with Au/BiOCl powder catalyst, the prepared Au/BiOCl coating with anti-oil-fouling also possessed high photocatalytic bactericidal activity and stable recycling performance.

The Impact of Secondary Building Units in Metal–Organic Frameworks on Plasmonic Gold‐Sensitized Photocatalysis

AbstractEmbedding plasmonic metals in metal–organic frameworks (MOFs) can build an advanced visible‐light photocatalyst architecture utilizing the localized surface plasmon resonance (LSPR) effect, while the practical performances have been restricted by the sluggish charge transfer at metal–MOF interface and through the secondary building units (SBUs) of the adopted carboxylate MOFs currently. Herein, a pyrazolate Ni‐MOF (PFC‐9) featured with an 1D SBU chain is selected to be the host catalyst to immobilize Au nanoparticles as a novel and optimized construction for LSPR photocatalysis. Compared with the common 3D‐connected SBUs of carboxyl‐ZrOx and pyrazole‐NiOx configurations in the reference MOFs, the 1D (−Ni−NPz−NPz−)∞ chain in PFC‐9 creates abundant Au/MOF contacts, a short and low‐resistant pathway for Au‐to‐Ni2+ transport of hot electrons, and enables fluent electron utilization at the continuous active Ni sites. Consequently, the Au/PFC‐9 photocatalyst achieves the optimum activity for visible‐light‐driven H2 production. This work shows an example to promote the LSPR‐sensitized photocatalysis taking the advantage of MOFs’ structural tunability, providing significant guidance for the rational design of highly efficient photocatalysts.

Progress in ultrafast spintronics research

Ultrafast spintronics is one of the most promising fields for information processing technology innovation. When compared with traditional electronic devices, new spin-based devices have advantages such as low power consumption, high speed, and nonvolatility. Exploring novel physical phenomena and mechanisms relating to electronic spins significantly promotes the development of next-generation spintronic devices. In this review, we outline a sequence of advances in the fields of ultrafast magnetics and spintronics. First, a quick overview of spintronics and the discovery of ultrafast demagnetization induced by a femtosecond laser is provided. The proposed physical mechanisms and theories of ultrafast spin dynamics are then summarized, including the phenomenological three-temperature model, computations based on the time-dependent density functional theory, the Elliott-Yafet spin-flip mechanism, and the nonlocal superdiffusive spin transport model. Following that, the most recent experimental and theoretical studies on all-optical switching of ferrimagnetic and ferromagnetic metals are thoroughly reviewed. Furthermore, the discovery of hot-electron spin transport induced by ultrashort lasers as well as its influence on ultrafast magnetization dynamics, ultrafast spin transfer torque, spin injection into semiconductors, and spin accumulation and dissipation in hot-electron transport are described. The advancements in the optimization and manipulation of spintronics-based terahertz emitters are reviewed and analyzed. Finally, we discuss the current challenges in ultrafast spintronics research as well as possible future studies.

Dynamics of hot refluxing electrons in ultra-short relativistic laser foil interactions

We investigate the dynamics of hot refluxing electrons in the interaction of an ultra-short relativistic laser pulse with a thin foil target via particle-in-cell (PIC) simulations, which is governed by the multidimensional spatiotemporal evolution of a self-generated sheath field. The comparison of time-integrated energy spectra of refluxing and escaping electrons indicates the refluxing efficiency is higher than 95% in average for each bounce. The characteristics of wide transverse spatial distribution and energy-resolved angular distribution caused by the refluxing electrons show a direct correlation with the angular-dependent photon yield of bremsstrahlung emission, as verified by the hybrid simulations of coupling the PIC results with Monte Carlo particle transport code. We further clarify the energy dissipation mechanisms of refluxing electrons through the recirculation in the thin target under the electron-refluxing dominated regime and conclude that the self-generated sheath field plays a dominant role over the competing processes, such as the radiation loss, collisional stopping, and anomalous inhibition via the resistive field. The lifetime of recirculation is calculated to be a few hundred femtoseconds, that is, one order of magnitude shorter than the timescale of collisional dissipation, while it is one order of magnitude longer than the laser pulse duration. The results could provide useful insights to understand the hot electron transport and stopping, secondary radiation generation, and ion acceleration in the high energy density plasmas.

Schottky-Contacted WSe2 Hot-Electron Photodetectors with Fast Response and High Sensitivity

Utilizing the short lifetime of hot electrons, ultrasensitive hot-electron photodetectors with fast response speed can be developed that have the potential to carve a niche among the photoconductive devices. Herein, high-performance WSe2 photodetectors are fabricated based on hot-electron transportation, in which an ultrathin Al2O3 layer enables screening of high-energy hot electrons and promises ultrasensitive response to incident light, and the built-in electric field in Schottky junctions separates the photoinduced carriers for fast transient recovery. The hot-electron photodetectors demonstrated a high rectification ratio of 107 and an extremely low dark current of 1 pA/μm with a high Ilight/Idark ratio of 1.8 × 106. Moreover, a high responsivity of 3.69 A/W and detectivity of 2.39 × 1013 Jones at an incident light power of 5.0 μW/cm2 are simultaneously achieved. The present strategy offers an alternative route for ultrasensitive photodetectors with fast response.

Manipulation of laser-accelerated proton beam spatial distribution by laser machined microstructure targets

Experimental study of laser proton acceleration was carried out using laser machined line targets and cross targets with tens of micrometers scale. We have found that both the shape and material of the microstructure targets have significant influences on the distribution of the proton beam. For the aluminum line target, the proton beam spot expands in a direction perpendicular to the boundary of the target; while for the plastic line target, it expands parallel to the boundary of the target. Detailed PIC simulations of the aluminum target have been carried out, which show that due to the lateral transport of hot electrons and the sheath fields accumulated at the edge of the microstructure target, the divergence angle of the accelerated proton beam is changed accordingly, thereby modulating the spatial distribution: the elliptical beam spot can be obtained from the line target, and the quasi-square beam spot can be obtained from the cross target. Simulations of the plastic target indicate that the difference in the electron transport properties for the two types of targets may be the reason for the completely different beam spot shapes. This work shows that the microstructure targets can be a potential method to manipulate the spatial distribution and uniformity of the proton beam.

Ultrafast real-time tracing of surface electric field generated via hot electron transport in polar semiconductors

We trace an ultrafast real-space motion of photo-excited free carriers just near the surface of polar semiconductors GaAs and InAs by using the optical second-harmonic generation (SHG) technique. With a flat distribution of photo-carriers as an initial condition, ultrafast diffusion and drift motion followed by a rapid surface recombination develop a surface electric field which is efficiently probed by the electric-field-induced SHG. From the simulation based on the drift–diffusion equation combined with the ensemble Monte-Carlo approach, we could explain the experimental observation of the temporal evolution of the surface electric field, and extract time constants related to the hot electron cooling. Whereas the hot carrier cooling time is determined to be about 8 ps at room temperature for GaAs, it can be further extended to about 35 ps at 100 K due to the increase of the longitudinal optic phonon life time enhancing the hot phonon effect. Our work can be an important guide in designing optoelectronic nano-devices by providing a clear understanding of the ultrafast electron-hole separation near the surface of polar semiconductors in connection with the hot carrier cooling process.

Improved spatial soliton theory on the example of photorefractive gallium arsenide

This article presents a critical look at the standard theory of bright and dark photorefractive screening solitons. We pay attention to the commonly overlooked fact of the inconsistency of the theory in the context of the accordance of soliton solution with the microscopic band transport models. Taking into account the material equations for the semi-insulating semiconductor (SI-GaAs) and including the nonlinear transport of hot electrons, a simple differential equation has been developed to determine the distribution of refractive index changes in the material for a localized optical beam. An amendment to the standard solution of (1 + 1)D solitons has been proposed, which particularly should be used for dark solitons to obtain the plausible self-consistent solutions

Estimate of pre-thermal quench non-thermal electron density profile during Ar pellet shutdowns of low-density target plasmas in DIII-D

The radial density profile of pre-thermal quench (pre-TQ) early-time non-thermal (hot) electrons is estimated by combining electron cyclotron emission and soft x-ray data during the rapid shutdown of low-density (ne≲1019 m−3) DIII-D target plasmas with cryogenic argon pellet injection. This technique is mostly limited in these experiments to the pre-TQ phase and quickly loses validity during the TQ. Two different cases are studied: a high (10 keV) temperature target and a low (4 keV) temperature target. The results indicate that early-time, low-energy (∼10 keV) hot electrons form ahead of the argon pellet as it enters the plasma, affecting the pellet ablation rate; it is hypothesized that this may be caused by rapid cross field transport of argon ions ahead of the pellet or by rapid cross field transport of hot electrons. Fokker–Planck modeling of the two shots suggests that the hot electron current is quite significant during the pre-TQ phase (up to 50% of the total current). Comparison between modeled pre-TQ hot electron current and post-TQ hot electron current inferred from avalanche theory suggests that hot electron current increases during the high-temperature target TQ but decreases during the low-temperature target TQ. The uncertainties in this estimate are large; however, if true, this suggests that TQ radial loss of hot electron current could be larger than previously estimated in DIII-D.

Simulation of Space-Charge-Limited Current for Hot Electrons With Initial Velocity in a Vacuum Diode

In this article, a sheet model is utilized to model and simulate hot electron transport properties in vacuum gap. Based on this model, emitted electrons with constant initial velocities and Maxwell–Boltzmann distribution are considered. Numerical analyses of the potential, electric field, current density, velocity, and phase-space distribution are also performed. The accuracy of this model is verified by comparing with analytical results. Furthermore, we studied the velocity distribution of the emitted electrons at any position in the interelectrode gap and observed a significant change in the distribution.

Unraveling the Ultrafast Hot Electron Dynamics in Semiconductor Nanowires.

Hot electron relaxation and transport in nanostructures involve a multitude of ultrafast processes whose interplay and relative importance are still not fully understood, but which are relevant for future applications in areas such as photocatalysis and optoelectronics. To unravel these processes, their dynamics in both time and space must be studied with high spatiotemporal resolution in structurally well-defined nanoscale objects. We employ time-resolved photoemission electron microscopy to image the relaxation of photogenerated hot electrons within InAs nanowires on a femtosecond time scale. We observe transport of hot electrons to the nanowire surface within 100 fs caused by surface band bending. We find that electron–hole scattering substantially influences hot electron cooling during the first few picoseconds, while phonon scattering is prominent at longer time scales. The time scale of cooling is found to differ between the well-defined wurtzite and zincblende crystal segments of the nanowires depending on excitation light polarization. The scattering and transport mechanisms identified will play a role in the rational design of nanostructures for hot-electron-based applications.

Hot Electron Transport Characteristics in a Conical-Entry-Multilayer Target Driven by Intense Laser

Hot Electron Transport Characteristics in a Conical-Entry-Multilayer Target Driven by Intense Laser