Low dark current photocathode guns are highly desired for high-brightness continuous-wave operations.Direct-current superconducting radio-frequency(DC-SRF)gun,a hybrid photocathode gun combining a DC gap and an SRF ca...Low dark current photocathode guns are highly desired for high-brightness continuous-wave operations.Direct-current superconducting radio-frequency(DC-SRF)gun,a hybrid photocathode gun combining a DC gap and an SRF cavity,effectively isolates the photocathode from the SRF cavity and offers significant advantages in terms of minimizing dark current levels.This paper presents an in-depth analysis of the dark current of a newly developed high-brightness DC-SRF photocathode gun(DC-SRF-Ⅱ gun).Particularly,a systematic experimental investigation of the dark current was conducted,and a comprehensive understanding of its formation was achieved through compliant simulations and measurements.Additionally,measures for attaining sub-nanoampere dark currents in the DC-SRF-Ⅱ gun are presented,including design considerations,cavity processing,assembly,and conditioning.The findings of this study establish a strong foundation for achieving high-performance operation of the DC-SRF-Ⅱ gun and provide a valuable reference for other photocathode guns.展开更多
CuBi_(2)O_(4)is identified as a promising photocathode in photoelectrochemical(PEC)water splitting systems.However,the PEC performance of CuBi_(2)O_(4)is far from expected due to the limited separation and transport e...CuBi_(2)O_(4)is identified as a promising photocathode in photoelectrochemical(PEC)water splitting systems.However,the PEC performance of CuBi_(2)O_(4)is far from expected due to the limited separation and transport efficiency of photogenerated carriers.To address the above issues,a cost-effective ternary Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode was designed.Firstly,a thin Cu:NiO_(X)film was inserted between CuBi_(2)O_(4)and FTO conducting substrate as a hole-selective layer,which promotes the transmission of photogenerated holes to the FTO substrate effectively.Furthermore,the modification of CuO film on the CuBi_(2)O_(4)electrode not only increases the absorption of sunlight and generates more photogenerated carriers,but also constitutes a heterojunction with CuBi_(2)O_(4),creating a built-in electric field,which facilitates the separation of electrons and holes,and accelerates the electrons transfer to electrode–electrolyte interface.The fabricated Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode exhibits a surprisingly high photocurrent density of−1.51 mA·cm^(−2)at 0.4 V versus RHE,which is 2.6 times that of the pristine CuBi_(2)O_(4)photocathode.The improved PEC performance is attributed to the synergy effect of the Cu:NiO_(X)hole-selective layer and the CuBi_(2)O_(4)/CuO heterojunction.Moreover,the combination with the BiVO_(4)/CoS,an unbiased overall water splitting was achieved,which has a photocurrent of 0.193 mA·cm^(−2).展开更多
CuBi_(2)O_(4)(CBO)photocathodes hold significant promise for efficient photoelectrochemical(PEC)water splitting due to their favorable band gap and theoretical onset potential.However,their practical application is hi...CuBi_(2)O_(4)(CBO)photocathodes hold significant promise for efficient photoelectrochemical(PEC)water splitting due to their favorable band gap and theoretical onset potential.However,their practical application is hindered by poor charge separation efficiency.Herein,we introduce a characteristic in-situ solution Fe-doping strategy that markedly improves photoelectrochemical performance of CBO,doubling the photocurrent density and achieving an unprecedented 190 mV anodic shift in the onset potential.By integrating with an electrochemical oxidation post-treatment,a record incident photon-to-current efficiency(IPCE)exceeding 40% at 0.6 V vs.RHE under visible light illumination is achieved.The versatility of the doping strategy is demonstrated across CBO photocathodes synthesized by different methods with various morphologies,grain sizes,and crystallinities.Mechanistic studies reveal that the gradient distribution of Fe^(3+)ions generates an internal electric field that facilitates efficient charge separation and increases acceptor density.The strong Fe-O bonding also enhances structural stability against photoinduced corrosion.Notably,our investigation uncovers the non-temperature-dependent nature of CBO photocurrent,indicating that PEC performance enhancement primarily depends on reducing carrier recombination rather than improving bulk conductivity.This work lays the groundwork for future advancements in water splitting performance of CBO photocathodes,offering a complementary strategy to conventional methods for enhancing charge separation efficiency.展开更多
The temporal characteristics of GaAs NEA and alkali metal photocathodes are studied using Monte Carlo simulation method. The electron transit time and its distribution functions in the photocathodes are calculated. Ba...The temporal characteristics of GaAs NEA and alkali metal photocathodes are studied using Monte Carlo simulation method. The electron transit time and its distribution functions in the photocathodes are calculated. Based on the results, the time modulation transfer functions and temporal resolutions of the photocathodes are obtained. The results show that the response time and temporal resolution of alkali metal photocathode is in femitosecond order and those of GaAs NEA photocathode are in picosecond order.展开更多
By calculating the energy distribution of electrons reaching the photocathode surface and solving the Schrodinger equation that describes the behavior of an electron tunneling through the surface potential barrier,we ...By calculating the energy distribution of electrons reaching the photocathode surface and solving the Schrodinger equation that describes the behavior of an electron tunneling through the surface potential barrier,we obtain an equation to calculate the emitted electron energy distribution of transmission-mode NEA GaAs photocathodes. Accord- ing to the equation,we study the effect of cathode surface potential barrier on the electron energy distribution and find a significant effect of the barrier-Ⅰ thickness or end height,especially the thickness,on the quantum efficiency of the cath- ode. Barrier Ⅱ has an effect on the electron energy spread, and an increase in the vacuum level will lead to a narrower electron energy spread while sacrificing a certain amount of cathode quantum efficiency. The equation is also used to fit the measured electron energy distribution curve of the transmission-mode cathode and the parameters of the surface barri- er are obtained from the fitting. The theoretical curve is in good agreement with the experimental curve.展开更多
The effect of changing Be doping concentration in GaAs layer on the integrated photosensitivity for nega- tive-electron-affinity GaAs photocathodes is investigated. Two GaAs samples with the monolayer structure and th...The effect of changing Be doping concentration in GaAs layer on the integrated photosensitivity for nega- tive-electron-affinity GaAs photocathodes is investigated. Two GaAs samples with the monolayer structure and the muhilayer structure are grown by molecular beam epitaxy. The former has a constant Be concentration of 1 × 10^19 cm^-3, while the latter includes four layers with Be doping concentrations of 1 × 10^19, 7 × 10^18, 4 × 10^18, and 1 × 10^18 cm^-3 from the bottom to the surface. Negative-electron-affinity GaAs photocathodes are fabricated by exciting the sample surfaces with alternating input of Cs and O in the high vacuum system. The spectral response results measured by the on-line spectral response measurement system show that the integrated photosensitivity of the photocathode with the muhilayer structure enhanced by at least 50% as compared to that of the monolayer structure. This attributes to the improvement in the crystal quality and the increase in the surface escape probability. Different stress situations are observed on GaAs samples with monolayer structure and muhilayer structure, respectively.展开更多
The stability of a reflection-mode GaAs photocathode has been investigated by monitoring the photocurrent and the spectral response at room temperature. We observe the photocurrent of the cathode decaying with time in...The stability of a reflection-mode GaAs photocathode has been investigated by monitoring the photocurrent and the spectral response at room temperature. We observe the photocurrent of the cathode decaying with time in the vacuum system under the action of Cs current, and find that the Cs atoms residing in the vacuum system are helpful in prolonging the life of the cathode. We examine the evolution and analyse the influence of the barrier on the spectral response of the cathode. Our results support the double dipolar mode] for the explanation of the negative electron affinity effect.展开更多
The gradient-doping structure is first applied to prepare the transmission-mode GaAs photocathode and the integral sensitivity of the sealed image tube achieves 1420μA/lm. This paper studies the inner carrier concent...The gradient-doping structure is first applied to prepare the transmission-mode GaAs photocathode and the integral sensitivity of the sealed image tube achieves 1420μA/lm. This paper studies the inner carrier concentration distribution of the gradient-doping transmission-mode GaAs photocathode after molecular beam epitaxy （MBE） growth using the electrochemical capacitance-voltage profiling. The results show that an ideal gradient-doping structure can be obtained by using MBE growth. The total band-bending energy in the gradient-doping GaAs active-layer with doping concentration ranging from 1×10^19 cm-3 to 1×1018 cm-3 is calculated to be 46.3 meV, which helps to improve the photoexcited electrons movement toward surface for the thin epilayer. In addition,by analysis of the band offsets, it is found that the worse carrier concentration discrepancy between GaAs and GaA1As causes a lower back interface electron potential barrier which decreases the amount of high-energy photoelectrons and affects the short-wave response.展开更多
Delafossite CuFeO_(2) is a promising photocathode material for cost-efficiently photoelectrochemical(PEC)water splitting,but the unfavorable conductivity and fast recombination dynamics of photogenerated carriers limi...Delafossite CuFeO_(2) is a promising photocathode material for cost-efficiently photoelectrochemical(PEC)water splitting,but the unfavorable conductivity and fast recombination dynamics of photogenerated carriers limit its PEC activity for water reduction.Here,we developed a heterostructure photocathode consisting of the Cu-doped NiO(Cu:NiO)hole selective layer(HSL)and Ni-doped CuFeO_(2)(Ni:CuFeO_(2))active layer by simply annealing a homogeneous Cu-Fe oxalate layer grown on the Ni film deposited on the fluorine doped tin oxide(FTO)substrate.The obtained heterostructure of Cu:NiO/Ni:CuFeO_(2) with enhanced charge carrier transportability and high-quality interface greatly promotes the separation of photogenerated carriers.Accordingly,the Cu:NiO/Ni:CuFeO_(2) photocathode exhibits a high photocurrent density of~0.9 mA·cm^(-2 )at 0.2 V(vs.reversible hydrogen electrode,RHE),outperforming most of the reported bare CuFeO_(2) photocathodes in the literature.And the photocurrent density can be further improved to 1.2 mA·cm^(-2) after decorating NiSx cocatalyst.展开更多
Photoelectrochemical(PEC) cells involved with semiconductor electrodes can simultaneously absorb solar energy and perform chemical reactions, which are considered as an attractive strategy to produce renewable and cle...Photoelectrochemical(PEC) cells involved with semiconductor electrodes can simultaneously absorb solar energy and perform chemical reactions, which are considered as an attractive strategy to produce renewable and clean hydrogen energy. Sb_(2)Se_(3) has been widely investigated in constructing PEC photocathodes benefitting of its low toxicity, suitable band gap, superior optoelectronic properties, and outstanding photocorrosion stability. We first present a brief overview of basic concepts and principles of PEC water splitting as well as a comparison between Sb_(2)Se_(3) and other numerous candidates. Then the material characteristics and preparation methods of Sb_(2)Se_(3) are introduced. The development of Sb_(2)Se_(3)-based photocathodes in PEC water splitting with various architectures and engineering efforts(i.e., absorber engineering, interfaces engineering, co-catalyst engineering and tandem engineering) to improve solar-to-hydrogen(STH) efficiency are highlighted. Finally, we debate the possible future directions to further explore the researching fields of Sb_(2)Se_(3)-based photocathodes with a strongly positive outlook in PEC processed solar hydrogen production.展开更多
Two types of transmission-mode GaAs photocathodes grown by molecular beam epitaxy are compared in terms of activation process and spectral response, one has a gradient-doping structure and the other has a uniform-dopi...Two types of transmission-mode GaAs photocathodes grown by molecular beam epitaxy are compared in terms of activation process and spectral response, one has a gradient-doping structure and the other has a uniform-doping structure. The experimental results show that the gradient-doping photocathode can obtain a higher photoemission capability than the uniform-doping one. As a result of the downward graded band-bending structure, the cathode performance parameters, such as the electron average diffusion length and the surface electron escape probability obtained by fitting quantum yield curves, are greater for the gradient-doping photocathode. The electron diffusion length is within a range of from 2.0 to 5.4μm for doping concentration varying from 10^19 to 10^18 cm^-3 and the electron average diffusion length of the gradient-doping photocathode achieves 3.2 μm.展开更多
The next generation of advanced light sources requires photons with large average flux and high brightness,which needs advanced electron gun matched with excellent photocathode materials. K_(2)CsSb photocathode has th...The next generation of advanced light sources requires photons with large average flux and high brightness,which needs advanced electron gun matched with excellent photocathode materials. K_(2)CsSb photocathode has the advantages of high quantum efficiency, long lifetime and instantaneous response. This study introduces the design of a set of K_(2)CsSb photocathode preparation systems and detailed preparation process of K_(2)CsSb photocathodes, including sequential deposition process and co-deposition process, and finally develops a K_(2)CsSb photocathode. The influence of laser power on the quantum efficiency is also investigated.展开更多
CdS sensitized NiO electrode was used as the photoactive cathode in a photoelectrochemical cell for water splitting,avoiding the use of a sacrificial electron donor.Photocurrent increment under visible light irradiati...CdS sensitized NiO electrode was used as the photoactive cathode in a photoelectrochemical cell for water splitting,avoiding the use of a sacrificial electron donor.Photocurrent increment under visible light irradiation was observed after integration of[Co（dmgH）_2（4-Me-py）Cl]（1） to the photocathode,suggesting 1 could accept electrons from photoexcited CdS for water reduction and NiO could move the holes in the valence band of CdS to anode for water oxidation.展开更多
CuO,as a promising photocathode material,suffers from severe photocorrosion in photoelectrochemical water splitting applications.Herein,a Cu_(3)N protection shell was used to protect the CuO photocathode for the first...CuO,as a promising photocathode material,suffers from severe photocorrosion in photoelectrochemical water splitting applications.Herein,a Cu_(3)N protection shell was used to protect the CuO photocathode for the first time to effectively suppress the photocorrosion of CuO.Consequently,the Cu_(3)N‐protected CuO photocathode shows improved stability,retaining 80% of its initial current density in a 20‐min test,while only 10%of the initial current density can be retained for the bare photocathode.This work may provide an important strategy for using Cu_(3)N shells to stabilize unstable photocathodes.展开更多
The resolution characteristic can be obtained by the modulation transfer function （MTF） of a GaAs/GaA1As photocathode. After establishing the theoretical model of GaAs（100）-oriented atomic configuration and the fo...The resolution characteristic can be obtained by the modulation transfer function （MTF） of a GaAs/GaA1As photocathode. After establishing the theoretical model of GaAs（100）-oriented atomic configuration and the formula for the ionized impurity scattering of the non-equilibrium carriers, this paper calculates the trajectories of photoelectrons in a photocathode. Thus the distribution of photoelectron spots on the emit-face is obtained, which is namely the point spread function. The MTF is obtained by Fourier transfer of the line spread function obtained from the point spread function. The MTF obtained from these calculations is shown to depend heavily on the electron diffusion length, and enhanced considerably by decreasing the electron diffusion length and increasing the doping concentration. Furthermore, the resolution is enhanced considerably by increasing the active-layer thickness, especially at high spatial frequencies. The best spatial resolution is 860 lp/mm, for the GaAs photocathode of doping concentration 1 ×10^19 cm 3 electron diffusion length 3.6 μm and the active-layer thickness 2 μm, under the 633-nm light irradiated. This research will contribute to the future improvement of the cathode＇s resolution for preparing a high performance GaAs photocathode, and improve the resolution of a low light level image intensifier.展开更多
In order to develop the photodetector for effective blue-green response, the 18-mm-diameter vacuum image tube combined with the transmission-mode Alo.7Gao.3Aso.9Po.1/GaAso.9Po.1 photocathode grown by molecular beam ep...In order to develop the photodetector for effective blue-green response, the 18-mm-diameter vacuum image tube combined with the transmission-mode Alo.7Gao.3Aso.9Po.1/GaAso.9Po.1 photocathode grown by molecular beam epitaxy is tentatively fabricated. A comparison of photoelectric property, spectral characteristic and performance parameter be- tween the transmission-mode GaAsP-based and blue-extended GaAs-based photocathodes shows that the GaAsP-based photocathode possesses better absorption and higher quantum efficiency in the blue-green waveband, combined with a larger surface electron escape probability. Especially, the quantum efficiency at 532 nm for the GaAsP-based photocathode achieves as high as 59%, nearly twice that for the blue-extended GaAs-based one, which would be more conducive to the underwater range-gated imaging based on laser illumination. Moreover, the simulation results show that the favorable blue-green response can be achieved by optimizing the emission-layer thickness in a range of 0.4 μm-0.6 μm.展开更多
The synthesis of renewable chemical fuels from CO_(2) and H_(2)O via photoelectrochemical(PEC)route reprensents a promising room-temperature approach for transforming greenhouse gas into value-added chemicals(e.g.,syn...The synthesis of renewable chemical fuels from CO_(2) and H_(2)O via photoelectrochemical(PEC)route reprensents a promising room-temperature approach for transforming greenhouse gas into value-added chemicals(e.g.,syngas),but to date it has been hampered by the lack of efficient photocathode for CO_(2) reduction.Herein,we report efficient PEC CO_(2) reduction into syngas by photocathode engineering.The photocathode is consisting of a planar p-n Si junction for strong light harvesting,GaN nanowires for efficient electron extraction and transfer,and Au/TiO_(2)for rapid electrocatalytic syngas production.The photocathode yields a record-high solar energy conversion efficiency of 2.3%.Furthermore,desirable syngas compositions with CO/H_(2)ratios such as 1:2 and 1:1 can be produced by simply varying the size of Au nanoparticle.Theoretical calculations reveal that the active sites for CO and H_(2)generation are the facet and undercoordinated sites of Au particles,respectively.展开更多
Silicon, as a promising semiconductor for fabricating photocathode toward photoelectrochemical hydrogen evolution reaction(PEC-HER), should be improved in light harvesting ability and catalytic kinetics to obtain high...Silicon, as a promising semiconductor for fabricating photocathode toward photoelectrochemical hydrogen evolution reaction(PEC-HER), should be improved in light harvesting ability and catalytic kinetics to obtain high PEC performance. Herein, a novel amorphous Nickel Oxysulfide(NiS_xO_y) film is effectively integrated with a Ti protected n^+p-Si micropyramid photocathode by the electrodeposition method. The fabricated n^+p-Si/Ti/Ni SxOyphotocathode exhibits excellent PEC-HER performance with an onset potential of 0.5 V(at J =-0.1 mA/cm^2), a photocurrent density of-26 mA/cm^2 at 0 V vs. RHE, and long term stability of six hours in alkaline solution(pH ≈ 14). The synergy of unique n^+p-Si micropyramid architectures(omnidirectional broadband light harvesting ability), novel amorphous NiS_xO_y catalyst(high HER electrocatalytic activity and good optical transparency) results in the high performance of n^+pSi/Ti/Ni S_xO_y. This work offers a novel strategy for effectively integrating electrocatalysts with semiconductor to design efficient photoelectrode toward PEC water splitting.展开更多
The built-in electric fields within a varied doping GaAs photocathode may promote the transport of electrons from the bulk to the surface, thus the quantum efficiency of the cathode can be enhanced remarkably. But thi...The built-in electric fields within a varied doping GaAs photocathode may promote the transport of electrons from the bulk to the surface, thus the quantum efficiency of the cathode can be enhanced remarkably. But this enhancement, which might be due to the increase in either the number or the energy of electrons reaching the surface, is not clear at present. In this paper, the energy distributions of electrons in a varied doping photocathode and uniform doping photocathode before and after escaping from the cathode surface are analysed, and the number of electrons escaping from the surface in different cases is calculated for the two kinds of photocathodes. The results indicate that the varied doping structure can not only increase the number of electrons reaching the surface but also cause an offset of the electron energy distribution to high energy. That is the root reason for the enhancement of the quantum efficiency of a varied doping GaAs photocathode.展开更多
A transmission-mode GaAs photocathode includes four layers of glass, Si3N4, Gal-xAlxAs and GaAs. A gradientdoping photocathode sample was obtained by molecular beam epitaxy and its transmittance was measured by spectr...A transmission-mode GaAs photocathode includes four layers of glass, Si3N4, Gal-xAlxAs and GaAs. A gradientdoping photocathode sample was obtained by molecular beam epitaxy and its transmittance was measured by spectrophotometer from 600 nm to 1100 nm. The theoretical transmittance is derived and simulated based on the matrix formula for thin film optics. The simulation results indicate the influence of the transition layers and the three thin-film layers except glass on the transmittance spectra. In addition, a fitting coefficient needed for error modification enters into the fitted formula. The fitting results show that the relative error in the full spectrum reduces from 19.51% to 4.35% after the formula is modified. The coefficient and the thicknesses are gained corresponding to the minimum relative error, meanwhile each layer and total thin-film thickness deviation in the module can be controlled within 73. The presence of glass layer roughness, layer interface effects and surface oxides is interpreted on the modification.展开更多
基金partially supported by the National Key Research and Development Program of China(Nos.2016YFA0401904 and 2017YFA0701001)the State Key Laboratory of Nuclear Physics and Technology,Peking University(Nos.NPT2022ZZ01).
文摘Low dark current photocathode guns are highly desired for high-brightness continuous-wave operations.Direct-current superconducting radio-frequency(DC-SRF)gun,a hybrid photocathode gun combining a DC gap and an SRF cavity,effectively isolates the photocathode from the SRF cavity and offers significant advantages in terms of minimizing dark current levels.This paper presents an in-depth analysis of the dark current of a newly developed high-brightness DC-SRF photocathode gun(DC-SRF-Ⅱ gun).Particularly,a systematic experimental investigation of the dark current was conducted,and a comprehensive understanding of its formation was achieved through compliant simulations and measurements.Additionally,measures for attaining sub-nanoampere dark currents in the DC-SRF-Ⅱ gun are presented,including design considerations,cavity processing,assembly,and conditioning.The findings of this study establish a strong foundation for achieving high-performance operation of the DC-SRF-Ⅱ gun and provide a valuable reference for other photocathode guns.
基金supported by the National Natural Science Foundation of China(No.61804039)the University Natural Sciences Research Project of Anhui Province(No.2022AH010096)+1 种基金the Talent Research Fund of Hefei University(No.20RC35)the Natural Science Foundation of Anhui Higher Education Institution of China(No.2023AH040160).
文摘CuBi_(2)O_(4)is identified as a promising photocathode in photoelectrochemical(PEC)water splitting systems.However,the PEC performance of CuBi_(2)O_(4)is far from expected due to the limited separation and transport efficiency of photogenerated carriers.To address the above issues,a cost-effective ternary Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode was designed.Firstly,a thin Cu:NiO_(X)film was inserted between CuBi_(2)O_(4)and FTO conducting substrate as a hole-selective layer,which promotes the transmission of photogenerated holes to the FTO substrate effectively.Furthermore,the modification of CuO film on the CuBi_(2)O_(4)electrode not only increases the absorption of sunlight and generates more photogenerated carriers,but also constitutes a heterojunction with CuBi_(2)O_(4),creating a built-in electric field,which facilitates the separation of electrons and holes,and accelerates the electrons transfer to electrode–electrolyte interface.The fabricated Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode exhibits a surprisingly high photocurrent density of−1.51 mA·cm^(−2)at 0.4 V versus RHE,which is 2.6 times that of the pristine CuBi_(2)O_(4)photocathode.The improved PEC performance is attributed to the synergy effect of the Cu:NiO_(X)hole-selective layer and the CuBi_(2)O_(4)/CuO heterojunction.Moreover,the combination with the BiVO_(4)/CoS,an unbiased overall water splitting was achieved,which has a photocurrent of 0.193 mA·cm^(−2).
基金financial support by the National Natural Science Foundation of China(NSFC,Grant No.22379153 and 22109128)the Ningbo Key Research and Development Project(2023Z147)the Ningbo 3315 Program。
文摘CuBi_(2)O_(4)(CBO)photocathodes hold significant promise for efficient photoelectrochemical(PEC)water splitting due to their favorable band gap and theoretical onset potential.However,their practical application is hindered by poor charge separation efficiency.Herein,we introduce a characteristic in-situ solution Fe-doping strategy that markedly improves photoelectrochemical performance of CBO,doubling the photocurrent density and achieving an unprecedented 190 mV anodic shift in the onset potential.By integrating with an electrochemical oxidation post-treatment,a record incident photon-to-current efficiency(IPCE)exceeding 40% at 0.6 V vs.RHE under visible light illumination is achieved.The versatility of the doping strategy is demonstrated across CBO photocathodes synthesized by different methods with various morphologies,grain sizes,and crystallinities.Mechanistic studies reveal that the gradient distribution of Fe^(3+)ions generates an internal electric field that facilitates efficient charge separation and increases acceptor density.The strong Fe-O bonding also enhances structural stability against photoinduced corrosion.Notably,our investigation uncovers the non-temperature-dependent nature of CBO photocurrent,indicating that PEC performance enhancement primarily depends on reducing carrier recombination rather than improving bulk conductivity.This work lays the groundwork for future advancements in water splitting performance of CBO photocathodes,offering a complementary strategy to conventional methods for enhancing charge separation efficiency.
文摘The temporal characteristics of GaAs NEA and alkali metal photocathodes are studied using Monte Carlo simulation method. The electron transit time and its distribution functions in the photocathodes are calculated. Based on the results, the time modulation transfer functions and temporal resolutions of the photocathodes are obtained. The results show that the response time and temporal resolution of alkali metal photocathode is in femitosecond order and those of GaAs NEA photocathode are in picosecond order.
文摘By calculating the energy distribution of electrons reaching the photocathode surface and solving the Schrodinger equation that describes the behavior of an electron tunneling through the surface potential barrier,we obtain an equation to calculate the emitted electron energy distribution of transmission-mode NEA GaAs photocathodes. Accord- ing to the equation,we study the effect of cathode surface potential barrier on the electron energy distribution and find a significant effect of the barrier-Ⅰ thickness or end height,especially the thickness,on the quantum efficiency of the cath- ode. Barrier Ⅱ has an effect on the electron energy spread, and an increase in the vacuum level will lead to a narrower electron energy spread while sacrificing a certain amount of cathode quantum efficiency. The equation is also used to fit the measured electron energy distribution curve of the transmission-mode cathode and the parameters of the surface barri- er are obtained from the fitting. The theoretical curve is in good agreement with the experimental curve.
文摘The effect of changing Be doping concentration in GaAs layer on the integrated photosensitivity for nega- tive-electron-affinity GaAs photocathodes is investigated. Two GaAs samples with the monolayer structure and the muhilayer structure are grown by molecular beam epitaxy. The former has a constant Be concentration of 1 × 10^19 cm^-3, while the latter includes four layers with Be doping concentrations of 1 × 10^19, 7 × 10^18, 4 × 10^18, and 1 × 10^18 cm^-3 from the bottom to the surface. Negative-electron-affinity GaAs photocathodes are fabricated by exciting the sample surfaces with alternating input of Cs and O in the high vacuum system. The spectral response results measured by the on-line spectral response measurement system show that the integrated photosensitivity of the photocathode with the muhilayer structure enhanced by at least 50% as compared to that of the monolayer structure. This attributes to the improvement in the crystal quality and the increase in the surface escape probability. Different stress situations are observed on GaAs samples with monolayer structure and muhilayer structure, respectively.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 60678043,60871012,and 60801036)the Research Funding of Nanjing University of Science and Technology (Grant No. 2010ZYTS032)
文摘The stability of a reflection-mode GaAs photocathode has been investigated by monitoring the photocurrent and the spectral response at room temperature. We observe the photocurrent of the cathode decaying with time in the vacuum system under the action of Cs current, and find that the Cs atoms residing in the vacuum system are helpful in prolonging the life of the cathode. We examine the evolution and analyse the influence of the barrier on the spectral response of the cathode. Our results support the double dipolar mode] for the explanation of the negative electron affinity effect.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 60678043 and 60801036)
文摘The gradient-doping structure is first applied to prepare the transmission-mode GaAs photocathode and the integral sensitivity of the sealed image tube achieves 1420μA/lm. This paper studies the inner carrier concentration distribution of the gradient-doping transmission-mode GaAs photocathode after molecular beam epitaxy （MBE） growth using the electrochemical capacitance-voltage profiling. The results show that an ideal gradient-doping structure can be obtained by using MBE growth. The total band-bending energy in the gradient-doping GaAs active-layer with doping concentration ranging from 1×10^19 cm-3 to 1×1018 cm-3 is calculated to be 46.3 meV, which helps to improve the photoexcited electrons movement toward surface for the thin epilayer. In addition,by analysis of the band offsets, it is found that the worse carrier concentration discrepancy between GaAs and GaA1As causes a lower back interface electron potential barrier which decreases the amount of high-energy photoelectrons and affects the short-wave response.
基金financially supported by the National Key Research and Development Program of China(No.2021YFA1500800)the National Natural Science Foundation of China(Nos.51825204,52072377,521888101 and 51402199)+6 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2020192)the International Partnership Program of Chinese Academy of Sciences(No.174321KYSB20200005)China Postdoctoral Science Foundation(No.2017M621137)Liaoning Revitalization Talents Program(No.XLYC2007193)the Natural Science Foundation of Liaoning Province(Nos.2021-MS-014 and 2021NLTS1210)the University Innovation Talent Foundation of Liaoning Province(No.LR2018074)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(No.KF1708)。
文摘Delafossite CuFeO_(2) is a promising photocathode material for cost-efficiently photoelectrochemical(PEC)water splitting,but the unfavorable conductivity and fast recombination dynamics of photogenerated carriers limit its PEC activity for water reduction.Here,we developed a heterostructure photocathode consisting of the Cu-doped NiO(Cu:NiO)hole selective layer(HSL)and Ni-doped CuFeO_(2)(Ni:CuFeO_(2))active layer by simply annealing a homogeneous Cu-Fe oxalate layer grown on the Ni film deposited on the fluorine doped tin oxide(FTO)substrate.The obtained heterostructure of Cu:NiO/Ni:CuFeO_(2) with enhanced charge carrier transportability and high-quality interface greatly promotes the separation of photogenerated carriers.Accordingly,the Cu:NiO/Ni:CuFeO_(2) photocathode exhibits a high photocurrent density of~0.9 mA·cm^(-2 )at 0.2 V(vs.reversible hydrogen electrode,RHE),outperforming most of the reported bare CuFeO_(2) photocathodes in the literature.And the photocurrent density can be further improved to 1.2 mA·cm^(-2) after decorating NiSx cocatalyst.
基金supported by the National Natural Science Foundation of China(No.62074102)Natural Science Foundation of Guangdong Province(2020A1515010805)China+1 种基金the Key Project of Department of Education of Guangdong Province(No.2018KZDXM059)Chinathe Science and Technology plan project of Shenzhen(20200812000347001,JCYJ20190808153409238)China。
文摘Photoelectrochemical(PEC) cells involved with semiconductor electrodes can simultaneously absorb solar energy and perform chemical reactions, which are considered as an attractive strategy to produce renewable and clean hydrogen energy. Sb_(2)Se_(3) has been widely investigated in constructing PEC photocathodes benefitting of its low toxicity, suitable band gap, superior optoelectronic properties, and outstanding photocorrosion stability. We first present a brief overview of basic concepts and principles of PEC water splitting as well as a comparison between Sb_(2)Se_(3) and other numerous candidates. Then the material characteristics and preparation methods of Sb_(2)Se_(3) are introduced. The development of Sb_(2)Se_(3)-based photocathodes in PEC water splitting with various architectures and engineering efforts(i.e., absorber engineering, interfaces engineering, co-catalyst engineering and tandem engineering) to improve solar-to-hydrogen(STH) efficiency are highlighted. Finally, we debate the possible future directions to further explore the researching fields of Sb_(2)Se_(3)-based photocathodes with a strongly positive outlook in PEC processed solar hydrogen production.
基金supported by the National Natural Science Foundation of China(Grant Nos.60801036 and 61067001)the Key Science and Technology Project of Henan Province of China(Grant No.112102210202)the Research and Innovation Plan for Graduate Students of Jiangsu Higher Education Institutions of China(Grant No.CX09B_096Z)
文摘Two types of transmission-mode GaAs photocathodes grown by molecular beam epitaxy are compared in terms of activation process and spectral response, one has a gradient-doping structure and the other has a uniform-doping structure. The experimental results show that the gradient-doping photocathode can obtain a higher photoemission capability than the uniform-doping one. As a result of the downward graded band-bending structure, the cathode performance parameters, such as the electron average diffusion length and the surface electron escape probability obtained by fitting quantum yield curves, are greater for the gradient-doping photocathode. The electron diffusion length is within a range of from 2.0 to 5.4μm for doping concentration varying from 10^19 to 10^18 cm^-3 and the electron average diffusion length of the gradient-doping photocathode achieves 3.2 μm.
文摘The next generation of advanced light sources requires photons with large average flux and high brightness,which needs advanced electron gun matched with excellent photocathode materials. K_(2)CsSb photocathode has the advantages of high quantum efficiency, long lifetime and instantaneous response. This study introduces the design of a set of K_(2)CsSb photocathode preparation systems and detailed preparation process of K_(2)CsSb photocathodes, including sequential deposition process and co-deposition process, and finally develops a K_(2)CsSb photocathode. The influence of laser power on the quantum efficiency is also investigated.
基金supported by the Fundamental Research Funds for the Central Universities(No.HIT.IBRSEM.A.201409)the Program for Innovation Research of Science in Harbin Institute of Technology(PIRS of HIT No.A201418,A201416)+1 种基金the National Natural Science Foundation of China(Nos.21171044 and21371040)the National key Basic Research Program of China(973 Program,No.2013CB632900)
文摘CdS sensitized NiO electrode was used as the photoactive cathode in a photoelectrochemical cell for water splitting,avoiding the use of a sacrificial electron donor.Photocurrent increment under visible light irradiation was observed after integration of[Co（dmgH）_2（4-Me-py）Cl]（1） to the photocathode,suggesting 1 could accept electrons from photoexcited CdS for water reduction and NiO could move the holes in the valence band of CdS to anode for water oxidation.
文摘CuO,as a promising photocathode material,suffers from severe photocorrosion in photoelectrochemical water splitting applications.Herein,a Cu_(3)N protection shell was used to protect the CuO photocathode for the first time to effectively suppress the photocorrosion of CuO.Consequently,the Cu_(3)N‐protected CuO photocathode shows improved stability,retaining 80% of its initial current density in a 20‐min test,while only 10%of the initial current density can be retained for the bare photocathode.This work may provide an important strategy for using Cu_(3)N shells to stabilize unstable photocathodes.
基金Project supported by the National Natural Science Foundation of China (Grant No. 60678043)the Research and Innovation Plan for Graduate Students of Jiangsu Higher Education Institutions,China (Grant No. CX09B 096Z)
文摘The resolution characteristic can be obtained by the modulation transfer function （MTF） of a GaAs/GaA1As photocathode. After establishing the theoretical model of GaAs（100）-oriented atomic configuration and the formula for the ionized impurity scattering of the non-equilibrium carriers, this paper calculates the trajectories of photoelectrons in a photocathode. Thus the distribution of photoelectron spots on the emit-face is obtained, which is namely the point spread function. The MTF is obtained by Fourier transfer of the line spread function obtained from the point spread function. The MTF obtained from these calculations is shown to depend heavily on the electron diffusion length, and enhanced considerably by decreasing the electron diffusion length and increasing the doping concentration. Furthermore, the resolution is enhanced considerably by increasing the active-layer thickness, especially at high spatial frequencies. The best spatial resolution is 860 lp/mm, for the GaAs photocathode of doping concentration 1 ×10^19 cm 3 electron diffusion length 3.6 μm and the active-layer thickness 2 μm, under the 633-nm light irradiated. This research will contribute to the future improvement of the cathode＇s resolution for preparing a high performance GaAs photocathode, and improve the resolution of a low light level image intensifier.
基金supported by the National Natural Science Foundation of China(Grant No.61301023)the Science and Technology on Low-Light-Level Nigh Vision Laboratory Foundation,China(Grant No.BJ2014001)
文摘In order to develop the photodetector for effective blue-green response, the 18-mm-diameter vacuum image tube combined with the transmission-mode Alo.7Gao.3Aso.9Po.1/GaAso.9Po.1 photocathode grown by molecular beam epitaxy is tentatively fabricated. A comparison of photoelectric property, spectral characteristic and performance parameter be- tween the transmission-mode GaAsP-based and blue-extended GaAs-based photocathodes shows that the GaAsP-based photocathode possesses better absorption and higher quantum efficiency in the blue-green waveband, combined with a larger surface electron escape probability. Especially, the quantum efficiency at 532 nm for the GaAsP-based photocathode achieves as high as 59%, nearly twice that for the blue-extended GaAs-based one, which would be more conducive to the underwater range-gated imaging based on laser illumination. Moreover, the simulation results show that the favorable blue-green response can be achieved by optimizing the emission-layer thickness in a range of 0.4 μm-0.6 μm.
基金supported by the National Natural Science Foundation of China(22005048,51822604,51906040)the Natural Science Foundation of Jiangsu Province(Grants No BK20200399)+2 种基金Emissions Reduction Alberta(ERA)McGill Engineering Doctoral AwardNational Sciences and Engineering Research Council(NSERC)Discovery grant(grant#RGPIN2017-05187)support from“Zhishan Young Scholar”Program of Southeast University。
文摘The synthesis of renewable chemical fuels from CO_(2) and H_(2)O via photoelectrochemical(PEC)route reprensents a promising room-temperature approach for transforming greenhouse gas into value-added chemicals(e.g.,syngas),but to date it has been hampered by the lack of efficient photocathode for CO_(2) reduction.Herein,we report efficient PEC CO_(2) reduction into syngas by photocathode engineering.The photocathode is consisting of a planar p-n Si junction for strong light harvesting,GaN nanowires for efficient electron extraction and transfer,and Au/TiO_(2)for rapid electrocatalytic syngas production.The photocathode yields a record-high solar energy conversion efficiency of 2.3%.Furthermore,desirable syngas compositions with CO/H_(2)ratios such as 1:2 and 1:1 can be produced by simply varying the size of Au nanoparticle.Theoretical calculations reveal that the active sites for CO and H_(2)generation are the facet and undercoordinated sites of Au particles,respectively.
基金supported by Zhejiang Provincial Natural Science Foundation of China [Grant no.LR17B060003]Major Science and Technology Project of Water Pollution Control and Management[No.2017ZX07101003]financially supported by the Natural Science Foundation of China [Project nos.21436007,21522606,21476201,21676246,U1462201,and 21776248]
文摘Silicon, as a promising semiconductor for fabricating photocathode toward photoelectrochemical hydrogen evolution reaction(PEC-HER), should be improved in light harvesting ability and catalytic kinetics to obtain high PEC performance. Herein, a novel amorphous Nickel Oxysulfide(NiS_xO_y) film is effectively integrated with a Ti protected n^+p-Si micropyramid photocathode by the electrodeposition method. The fabricated n^+p-Si/Ti/Ni SxOyphotocathode exhibits excellent PEC-HER performance with an onset potential of 0.5 V(at J =-0.1 mA/cm^2), a photocurrent density of-26 mA/cm^2 at 0 V vs. RHE, and long term stability of six hours in alkaline solution(pH ≈ 14). The synergy of unique n^+p-Si micropyramid architectures(omnidirectional broadband light harvesting ability), novel amorphous NiS_xO_y catalyst(high HER electrocatalytic activity and good optical transparency) results in the high performance of n^+pSi/Ti/Ni S_xO_y. This work offers a novel strategy for effectively integrating electrocatalysts with semiconductor to design efficient photoelectrode toward PEC water splitting.
基金supported by the National Natural Science Foundation of China (Grant No.60678043) the Research and Innovation Plan for Graduate Students of Jiangsu Higher Education Institutions of China (Grant No. CX09B-096Z)
文摘The built-in electric fields within a varied doping GaAs photocathode may promote the transport of electrons from the bulk to the surface, thus the quantum efficiency of the cathode can be enhanced remarkably. But this enhancement, which might be due to the increase in either the number or the energy of electrons reaching the surface, is not clear at present. In this paper, the energy distributions of electrons in a varied doping photocathode and uniform doping photocathode before and after escaping from the cathode surface are analysed, and the number of electrons escaping from the surface in different cases is calculated for the two kinds of photocathodes. The results indicate that the varied doping structure can not only increase the number of electrons reaching the surface but also cause an offset of the electron energy distribution to high energy. That is the root reason for the enhancement of the quantum efficiency of a varied doping GaAs photocathode.
基金supported by the National Natural Science Foundation of China (Grant No. 60678043)the Research and Innovation Plan for Graduate Students of Jiangsu Higher Education Institutions of China (Grant No. CX09B-096Z)
文摘A transmission-mode GaAs photocathode includes four layers of glass, Si3N4, Gal-xAlxAs and GaAs. A gradientdoping photocathode sample was obtained by molecular beam epitaxy and its transmittance was measured by spectrophotometer from 600 nm to 1100 nm. The theoretical transmittance is derived and simulated based on the matrix formula for thin film optics. The simulation results indicate the influence of the transition layers and the three thin-film layers except glass on the transmittance spectra. In addition, a fitting coefficient needed for error modification enters into the fitted formula. The fitting results show that the relative error in the full spectrum reduces from 19.51% to 4.35% after the formula is modified. The coefficient and the thicknesses are gained corresponding to the minimum relative error, meanwhile each layer and total thin-film thickness deviation in the module can be controlled within 73. The presence of glass layer roughness, layer interface effects and surface oxides is interpreted on the modification.
