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hot electrons in water: injection and ponderomotive acceleration by means of plasmonic nanoelectrodes

Light(Science & Applications) 2017年第1期6卷 744-751页

作者： Pierfrancesco Zilio Michele Dipalo Francesco Tantussi Gabriele C Messina Francesco de Angelis Istituto Italiano di Tecnologia 16163GenovaItaly

We present a theoretical and experimental study of a plasmonic nanoelectrode architecture that is able to inject bunches of hot electrons into an aqueous *** this approach,electrons are accelerated in water by ponderomotive forces up to energies capable of exciting or ionizing water *** ability is enabled by the nanoelectrode structure(extruding out of a metal baseplate),which allows for the production of an intense plasmonic hot spot at the apex of the structure while maintaining the electrical connection to a virtually unlimited charge *** electron injection is experimentally monitored by recording the current transmitted through the water medium,whereas the electron acceleration is confirmed by observation of the bubble generation for a laser power exceeding a proper *** understanding of the complex physics involved is obtained via a numerical approach that explicitly models the electromagnetic hot spot generation,electron-by-electron injection via multiphoton absorption,acceleration by ponderomotive forces and electron-water interaction through random elastic and inelastic *** model predicts a critical electron density for bubble nucleation that nicely matches the experimental findings and reveals that the efficiency of energy transfer from the plasmonic hot spot to the free electron cloud is much more efficient(17 times higher)in water than in a *** of their high kinetic energy and large reduction potential,these proposed wet hot electrons may provide new opportunities in photocatalysis,electrochemical processes and hot-electron driven chemistry.

关键词： hot electrons hydrated electrons lightwave electronics plasmonics ponderomotive acceleration strong-field photoemission water breakdown

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Direct observation and manipulation of hot electrons at room temperature

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National Science Review 2021年第9期8卷 32-40页

作者： Hailu Wang Fang Wang Hui Xia Peng Wang Tianxin Li Juzhu Li Zhen Wang Jiamin Sun Peisong Wu Jiafu Ye Qiandong Zhuang Zaixing Yang Lan Fu Weida Hu Xiaoshuang Chen Wei Lu State Key Laboratory of Infrared Physics Shanghai Institute of Technical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Henan Key Laboratory of Diamond Optoelectronic Materials and Devices School of Physics and Engineering Zhengzhou University School of Microelectronics Shandong University Department of Physics Lancaster University Department of Electronic Materials Engineering Research School of Physics and Engineering The Australian National University

In modern electronics and optoelectronics, hot electron behaviors are highly concerned, as they determine the performance limit of a device or system, like the associated thermal or power constraint of chips and the Shockley-Queisser limit for solar cell efficiency. To date, however, the manipulation of hot electrons has been mostly based on conceptual interpretations rather than a direct observation. The problem arises from a fundamental fact that energy-differential electrons are mixed up in real-space, making it hard to distinguish them from each other by standard measurements. Here we demonstrate a distinct approach to artificially(spatially) separate hot electrons from cold ones in semiconductor nanowire transistors, which thus offers a unique opportunity to observe and modulate electron occupied state, energy, mobility and even path. Such a process is accomplished through the scanning-photocurrent-microscopy measurements by activating the intervalley-scattering events and 1D charge-neutrality rule. Findings here may provide a new degree of freedom in manipulating non-equilibrium electrons for both electronic and optoelectronic applications.

关键词： hot electrons valley transfer photogating scanning photocurrent mapping

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Generation of hot electrons at Higher Temperatures from Solid Plasma with a Moderate—Intensity Femtosecond Laser

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Chinese Physics Letters 2002年第7期19卷 956-958页

作者：陶业争李业军等 ChinaInstituteofAtomicEnergy POBox275-7Beijing102413

We experimentally investigate the generation of hot electrons from the interaction of a moderate-intensity (1016W/cm2) pre-pulsed-free femtosecond laser (6mJ, 120fs, at 744nm) with a solid target. The temperature of the hot electrons is inferred from the hard x-ray (>30keV) continuum. The measured hard x-ray continuum is fitted by the Maxwellian distribution with two hot-electron temperatures of 45 and 85keV. electrons with the lower temperature were accelerated by ``vacuum heating''. However it is necessary to carry out an accurate numerical simulation to explain the generation of hot electrons at higher temperatures.

关键词： hot electrons

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Fraction and Temperature of hot electrons Generated by Laser—Plasma Interaction at the shenguang—Ⅱ Laser Facility

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Chinese Physics Letters 2002年第2期19卷 224-226页

作者：张家泰祁兰英等 InstituteofAppliedPhysicsandComputationalMathematics P.O.Box8009Beijing100088 CentreofLaserFusion ChinaAcademyofEngineeringPhysicsP.O.Box919Mianyang621900

We have developed a three-dimensional electron-photon Monte Carlo transmission (MCT) code. The conversion-transmissivity coefficient of hot electron x-ray, ηct, is analysed theoretically and simulated numerically using the MCT code. Experiments of disc and cylindrical targets have been performed at the Shenguang-II laser facility. A multi-channel filter-fluorescence spectrometer was used to obtain the hard x-ray spectrum. The temperature and energy of hot electrons are induced from the hard x-ray spectrum and the ηct value. The average energy fraction of hot electrons is 14% of incident laser energy for the 1ωNd laser and the spherical target with an average temperature of hot electrons of 36keV, while it is 15% for the 1ωNd laser and the cavity target with an average temperature of 54keV. We have also obtained the results of 5.6% and 13.3 keV for the 3ωNd laser and the disc target, 4.9% and 17.9keV for the 3ωNd laser and the half cavity target with a thin wall, and 2.1% and 22.4keV for those with a thick wall. The experimental results agree with theory and simulation.

关键词： hot electrons

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Double Jet Emission of hot electrons from a Micro-droplet Spray

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Chinese Physics Letters 2004年第4期21卷 693-696页

作者：彭晓昱张杰梁天骄盛政明金展李玉同王兆华于全芝郑志远刘运全武慧春郝作强远晓辉魏志义 LaboratoryofOpticalPhysics InstituteofPhysicsChineseAcademyofSciencesBeijing100080 ResearchInstituteofChemicalDefenses Beijing102205

Spatial distribution of hot electrons with energies above 50keV are investigated by an ethanol micro-droplet spray irradiated by linearly and elliptically polarized 150fs laser pulses at an intensity of 1016W/cm2. Two symmetric hot electron jets with respect to the laser propagation direction are observed in the polarization plane for a linearly polarized laser field and in the plane of the long electric vector for an elliptically polarized laser field, respectively. Particle-in-cell simulations suggest that the resonance absorption on the spherical surface of the droplets is mainly responsible for the generation of the double-jet emission of hot electrons.

关键词： hot electrons

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Collective Oscillation of Relativistic electrons in hot Plasma

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Chinese Physics Letters 2003年第8期20卷 1306-1308页

作者：马瑾怡邱锡钧朱志远 DepartmentofPhysics ShanghaiUniversityShanghai200436 ShanghaiInstitutionofNuclearResearch ChineseAcademyofSciencesShanghai201800

The interactions between relativistic electrons in a hot plasma are analysed theoretically. By splitting the electron density fluctuations into the individual part and the collective part, we are concerned with the collective oscillation of the relativistic electrons resulting from the Coulomb interactions. Consequently, we derive the frequency of the hot plasma and the ``Debye length'' with relativistic modification.

关键词： hot electrons

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Rapidly and mildly transferring anatase phase of graphene-activated TiO2 to rutile with elevated Schottky barrier:Facilitating interfacial hot electron injection for Vis-NIR driven photocatalysis

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Nano Research 2022年第12期15卷 10142-10147页

作者： Weiyao Hu Qiyuan Li Dong Xu Guangyao Zhai Shinan Zhang Dong Li Xiaoxiao He Jinping Jia Jiesheng Chen Xinhao Li School of Chemistry and Chemical Engineering Environmental Science and Engineeringand Frontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai200240China State Key Laboratory of Precision Spectroscopy East China Normal UniversityShanghai200241China

Visible and even infrared(IR)light-initiated hot electrons of graphene(Gr)catalysts are a promising driven power for green,safe,and sustainable H2O2 synthesis and organic synthesis without the limitation of bandgap-dominated narrow light absorption to visible light confronted by conventional ***,the life time of photogenerated hot electrons is too short to be efficiently used for various photocatalytic ***,we proposed a straightforward method to prolong the lifetime of photogenerated hot electrons from graphene by tuning the Schottky barrier at Gr/rutile interface to facilitate the hot electron *** rational design of Gr-coated TiO2 heterojunctions with interface synergy-induced decrease in the formation energy of the rutile phase makes the phase transfer of TiO2 support proceed smoothly and rapidly via ball *** optimized Gr/rutile dyad could provide a H2O2 yield of 1.05 mM·g-1·h-1 under visible light irradiation(λ≥400 nm),which is 30 times of the state-of-the-art noble-metal-free titanium oxide-based photocatalyst,and even achieves a H2O2 yield of 0.39 mM·g-1·h-1 on photoexcitation by near-infrared-region light(~800 nm).

关键词： hot electrons phase transition Schottky barrier heterojunction catalyst visible-near infrared ray(Vis-NIR)driven photocatalysis

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Near-field and photocatalytic properties of mono-and bimetallic nanostructures monitored by nanocavity surface-enhanced Raman scattering

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Nano Research 2023年第1期16卷 1545-1551页

作者： Rui Wang Zhe He Dmitry Kurouski State Key Laboratory of Bioelectronics School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Department of Biochemistry and Biophysics Texas A&M UniversityCollege StationTX 77843USA Department of Biomedical Engineering California Institute of TechnologyPasadenaCA 91125USA The Institute for Quantum Science and Engineering Texas A&M UniversityCollege StationTX 77843USA

Localized surface plasmon resonances(LSPR)generated in a particle-film nanocavity enhance electric fields within a nanoscale *** can also decay into hot carriers,highly energetic species that catalyze photocatalytic reactions in molecular analytes located in close proximity to metal *** this study,we examined the intensity of the electric field(near-field)and photocatalytic properties of plasmonic nanocavities formed by single nanoparticles(SNP)on single nanoplates(SNL).Using 4-nitrobenzenethiol(4-NBT)as a molecular reporter,we determined the near-field responses,as well as measured rates of 4-NBT dimerization into 4,4-dimercaptoazobenzene(DMAB)in the gold(Au)SNP on AuSNL nanocavity(Au-Au),as well as in AuSNP on AgSNL(Au-Ag),AgSNP on AuSNL(Ag-Au),and AgSNP on AgSNL(Ag-Ag)nanocavities using 532,660,and 785 nm *** observed the strongest near-field signals of 4-NBT at 660 nm in all examined plasmonic systems that is found to be substantially red-shifted relative to the LSPR of the corresponding *** also found that rates of DMAB formation were significantly greater in heterometal nanocavities(Au-Ag and Ag-Au)compared to their monometallic counterparts(Au-Au and Ag-Ag).These results point to drastic differences in plasmonic and photocatalytic properties of mono and bimetallic nanostructures.

关键词： bimetal photocatalysis surface-enhanced Raman spectroscopy(SERS) plasmonic nanocavity hot electrons plasmoninduced photocatalysis

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Nanostructured materials with localized surface plasmon resonance for photocatalysis

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Chinese Chemical Letters 2022年第3期33卷 1154-1168页

作者： Juan Li Zaizhu Lou Baojun Li Institute of Nanophotonics Jinan UniversityGuangzhou 511443China State Key Laboratory for Crystal Materials Shandong UniversityJi'nan 250100China

Localized surface plasmon resonance (LSPR) enhanced photocatalysis has fascinated much interest and considerable efforts have been devoted toward the development of plasmonic photocatalysts. In the past decades, noble metal nanoparticles (Au and Ag) with LSPR feature have found wide applications in solar energy conversion. Numerous metal-based photocatalysts have been proposed including metal/semiconductor heterostructures and plasmonic bimetallic or multimetallic nanostructures. However, high cost and scarce reserve of noble metals largely limit their further practical use, which drives the focus gradually shift to low-cost and abundant nonmetallic nanostructures. Recently, various heavily doped semiconductors (such as WO_(3-x), MoO_(3-x), Cu_(2-x)S, TiN) have emerged as potential alternatives to costly noble metals for efficient photocatalysis due to their strong LSPR property in visible-near infrared region. This review starts with a brief introduction to LSPR property and LSPR-enhanced photocatalysis, the following highlights recent advances of plasmonic photocatalysts from noble metal to semiconductor-based plasmonic nanostructures. Their synthesis methods and promising applicability in plasmon-driven photocatalytic reactions such as water splitting, CO_(2) reduction and pollution decomposition are also summarized in details. This review is expected to give guidelines for exploring more efficient plasmonic systems and provide a perspective on development of plasmonic photocatalysis.

关键词： Localized surface plasmon resonance Plasmonic photocatalysis Plasmonic semiconductor hot electrons Solar energy harvesting

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Synchronous activation of Ag nanoparticles and BiOBr for boosting solar-driven CO_(2)reduction

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Chinese Chemical Letters 2023年第6期34卷 252-255页

作者： Gaopeng Liu Lin Wang Bin Wang Xingwang Zhu Jinman Yang Pengjun Liu Wenshuai Zhu Ziran Chen Jiexiang Xia Key Laboratory of Medicinal and Edible Plants Resources of Hainan Province Hainan vocational university of Science and TechnologyHaikou 571126China School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013China Department of Architecture and Environment Engineering Sichuan Vocational and Technical CollegeSuining 629000China

Artificial photosynthesis of valuable chemicals from CO_(2)is a potential way to achieve sustainable carbon *** CO_(2)conversion activity is still inhibited by the sluggish charge kinetics and poor CO_(2)***,Ag nanoparticles coupled Bi OBr have been constructed by in-situ photoreduction *** crafting of interface between Ag nanoparticles and Bi OBr nanosheets,achieving an ultra-fast charge *** Bi OBr semiconductor excited electrons and plasmonic Ag nanoparticles generated high-energy hot electrons synchronous accelerates the C=O double bond ***,the optimized Ag/BiOBr-2 heterostructure shows excellent CO_(2)photoreduction activity with CO production of 133.75 and 6.83μmol/g under 5 h of 300 W Xe lamp and visible light(λ>400 nm)irradiation,which is 1.51 and 2.81 folds versus the pristine Bi OBr,*** mechanism of CO_(2)photoreduction was in-depth understood through in-situ FT-IR spectrum and density functional theory *** study provides some new perspectives into efficient photocatalytic CO_(2)reduction.

关键词： Ag nanoparticles BiOBr hot electrons Charge transfer CO_(2)photoreduction

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