Direct synthesis of layer-tunable and transfer-free graphene on technologically important substrates is highly valued for various electronics and device applications.State of the art in the field is currently a two-st...Direct synthesis of layer-tunable and transfer-free graphene on technologically important substrates is highly valued for various electronics and device applications.State of the art in the field is currently a two-step process:a high-quality graphene layer synthesis on metal substrate through chemical vapor deposition(CVD)followed by delicate layer transfer onto device-relevant substrates.Here,we report a novel synthesis approach combining ion implantation for a precise graphene layer control and dual-metal smart Janus substrate for a diffusion-limiting graphene formation to directly synthesize large area,high quality,and layer-tunable graphene films on arbitrary substrates without the post-synthesis layer transfer process.Carbon(C)ion implantation was performed on Cu-Ni film deposited on a variety of device-relevant substrates.A well-controlled number of layers of graphene,primarily monolayer and bilayer,is precisely controlled by the equivalent fluence of the implanted C-atoms(1 monolayer~4×10^(15)C-atoms/cm^(2)).Upon thermal annealing to promote Cu-Ni alloying,the pre-implanted C-atoms in the Ni layer are pushed toward the Ni/substrate interface by the top Cu layer due to the poor C-solubility in Cu.As a result,the expelled C-atoms precipitate into a graphene structure at the interface facilitated by the Cu-like alloy catalysis.After removing the alloyed Cu-like surface layer,the layer-tunable graphene on the desired substrate is directly realized.The layer-selectivity,high quality,and uniformity of the graphene films are not only confirmed with detailed characterizations using a suite of surface analysis techniques but more importantly are successfully demonstrated by the excellent properties and performance of several devices directly fabricated from these graphene films.Molecular dynamics(MD)simulations using the reactive force field(ReaxFF)were performed to elucidate the graphene formation mechanisms in this novel synthesis approach.With the wide use of ion implantation technology in the microelectronics industry,this novel graphene synthesis approach with precise layer-tunability and transfer-free processing has the promise to advance efficient graphene-device manufacturing and expedite their versatile applications in many fields.展开更多
Nitrogen-doped three-dimensional graphene(N-doped 3D-graphene)is a graphene derivative with excellent adsorption capacity,large specific surface area,high porosity,and optoelectronic properties.Herein,N-doped 3D-graph...Nitrogen-doped three-dimensional graphene(N-doped 3D-graphene)is a graphene derivative with excellent adsorption capacity,large specific surface area,high porosity,and optoelectronic properties.Herein,N-doped 3D-graphene/Si heterojunctions were grown in situ directly on silicon(Si)substrates via plasma-assisted chemical vapor deposition(PACVD),which is promising for surface-enhanced Raman scattering(SERS)substrates candidates.Combined analyses of theoretical simulation,incorporating N atoms in 3D-graphene are beneficial to increase the electronic state density of the system and enhance the charge transfer between the substrate and the target molecules.The enhancement of the optical and electric fields benefits from the stronger light-matter interaction improved by the natural nano-resonator structure of N-doped 3D-graphene.The as-prepared SERS substrates based on N-doped 3D-graphene/Si heterojunctions achieve ultra-low detection for various molecules:10^(-8)M for methylene blue(MB)and 10^(-9)M for crystal violet(CRV)with rhodamine(R6G)of 10^(10)M.In practical detected,10^(-8)M thiram was precisely detected in apple peel extract.The results indicate that N-doped 3D-graphene/Si heterojunctions based-SERS substrates have promising applications in low-concentration molecular detection and food safety.展开更多
Highly sensitive and uniform three-dimensional(3D)hybrid heterogeneous structures for use in surface-enhanced Raman scattering(SERS)experiments were fabricated by sequentially decorating high-quality,ultra-clean,graph...Highly sensitive and uniform three-dimensional(3D)hybrid heterogeneous structures for use in surface-enhanced Raman scattering(SERS)experiments were fabricated by sequentially decorating high-quality,ultra-clean,graphene quantum dots(GQDs)and Ag nanoparticles(Ag-NPs)onto 3D-graphene.Finite-difference time-domain calculations and scanning Kelvin probe microscopy were used to verify that the Ag-NPs/GQDs/3D-graphene system facilitates substantial electromagnetic enhancement(due to the occurrence of two kinds of"gaps"between the Ag-NPs that form 3D"hot spots")and additional chemical enhancement(in detecting someπ-conjugated molecules).The SERS mechanism was explored in further detail via experimental analysis and confirmed by performing theoretical calculations.The large surface area of the 3D substrate(due to the large specific surface areas of the GQDs and 3D-graphene)results in a better enrichment effect which helps produce lower detection limits.In particular,the detection limits obtained using the Ag-NPs/GQDs/3D-graphene platform can reach 10^(-11)M for rhodamine 6G,10^(-10)M for methylene blue and dopamine,and 10^(-7)M for tetramethylthiuram disulfide and methyl parathion in apple juice(these are superior to most of the results reported using graphene-based SERS substrates).In summary,the 3D-platform Ag-NPs/GQDs/3D-graphene/Si shows outstanding SERS performance.It therefore has excellent application prospects in biochemical molecular detection and food safety monitoring.展开更多
基金supported by the National Key R&D Program of China(No.2022YFA1203400)the National Natural Science Foundation of China under Grant(Nos.62174093 and 12075307)+7 种基金the Ningbo Youth Science and Technology Innovation Leading Talent Project under Grant(No.2023QL006)the Open Research Fund of China National Key Laboratory of Materials for Integrated Circuits(No.NKLJC-K2023-01)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110628)the support by LDRD Seedling ER project at Los Alamos National Laboratory,NM,USA(No.20210867ER)partially supported by Guangdong Provincial Key Laboratory of Computational Science and Material Design(No.2019B030301001)supported by Center for Computational Science and Engineering at Southern University of Science and TechnologyShanghai Rising-Star Program(No.21QA1410900)the support from the Youth Innovation Promotion Association CAS
文摘Direct synthesis of layer-tunable and transfer-free graphene on technologically important substrates is highly valued for various electronics and device applications.State of the art in the field is currently a two-step process:a high-quality graphene layer synthesis on metal substrate through chemical vapor deposition(CVD)followed by delicate layer transfer onto device-relevant substrates.Here,we report a novel synthesis approach combining ion implantation for a precise graphene layer control and dual-metal smart Janus substrate for a diffusion-limiting graphene formation to directly synthesize large area,high quality,and layer-tunable graphene films on arbitrary substrates without the post-synthesis layer transfer process.Carbon(C)ion implantation was performed on Cu-Ni film deposited on a variety of device-relevant substrates.A well-controlled number of layers of graphene,primarily monolayer and bilayer,is precisely controlled by the equivalent fluence of the implanted C-atoms(1 monolayer~4×10^(15)C-atoms/cm^(2)).Upon thermal annealing to promote Cu-Ni alloying,the pre-implanted C-atoms in the Ni layer are pushed toward the Ni/substrate interface by the top Cu layer due to the poor C-solubility in Cu.As a result,the expelled C-atoms precipitate into a graphene structure at the interface facilitated by the Cu-like alloy catalysis.After removing the alloyed Cu-like surface layer,the layer-tunable graphene on the desired substrate is directly realized.The layer-selectivity,high quality,and uniformity of the graphene films are not only confirmed with detailed characterizations using a suite of surface analysis techniques but more importantly are successfully demonstrated by the excellent properties and performance of several devices directly fabricated from these graphene films.Molecular dynamics(MD)simulations using the reactive force field(ReaxFF)were performed to elucidate the graphene formation mechanisms in this novel synthesis approach.With the wide use of ion implantation technology in the microelectronics industry,this novel graphene synthesis approach with precise layer-tunability and transfer-free processing has the promise to advance efficient graphene-device manufacturing and expedite their versatile applications in many fields.
基金supported by the National Natural Science Foundation of China under Grant(No.62174093)the Natural Science Foundation of Ningbo under Grant(No.202003N4097)+5 种基金the support from the Beijing Institute of Technology Research Fund Program for Young Scholarsthe support from Guangdong Provincial Medical Science and Technology Research(A2019434)the support from Guangdong Provincial Key Laboratory of Computational Science and Material Design(2019B030301001)Fundamental Research Program of Shenzhen(JCYJ20190809174203802)National Natural Science Foundation of Guangdong Province(2022A1515110628)supported by Center for Computational Science and Engineering at Southern University of Science and Technology
文摘Nitrogen-doped three-dimensional graphene(N-doped 3D-graphene)is a graphene derivative with excellent adsorption capacity,large specific surface area,high porosity,and optoelectronic properties.Herein,N-doped 3D-graphene/Si heterojunctions were grown in situ directly on silicon(Si)substrates via plasma-assisted chemical vapor deposition(PACVD),which is promising for surface-enhanced Raman scattering(SERS)substrates candidates.Combined analyses of theoretical simulation,incorporating N atoms in 3D-graphene are beneficial to increase the electronic state density of the system and enhance the charge transfer between the substrate and the target molecules.The enhancement of the optical and electric fields benefits from the stronger light-matter interaction improved by the natural nano-resonator structure of N-doped 3D-graphene.The as-prepared SERS substrates based on N-doped 3D-graphene/Si heterojunctions achieve ultra-low detection for various molecules:10^(-8)M for methylene blue(MB)and 10^(-9)M for crystal violet(CRV)with rhodamine(R6G)of 10^(10)M.In practical detected,10^(-8)M thiram was precisely detected in apple peel extract.The results indicate that N-doped 3D-graphene/Si heterojunctions based-SERS substrates have promising applications in low-concentration molecular detection and food safety.
基金support provided by the National Natural Science Foundation of China under Grant(No.62174093)Guangdong Provincial Key Laboratory of Computational Science and Material Design(2019B030301001)+1 种基金Fundamental Research Program of Shenzhen(JCYJ20190809174203802)K.C.Wong Magna Fund in Ningbo University and Natural Science Foundation of Ningbo under Grant(No.202003 N4097).
文摘Highly sensitive and uniform three-dimensional(3D)hybrid heterogeneous structures for use in surface-enhanced Raman scattering(SERS)experiments were fabricated by sequentially decorating high-quality,ultra-clean,graphene quantum dots(GQDs)and Ag nanoparticles(Ag-NPs)onto 3D-graphene.Finite-difference time-domain calculations and scanning Kelvin probe microscopy were used to verify that the Ag-NPs/GQDs/3D-graphene system facilitates substantial electromagnetic enhancement(due to the occurrence of two kinds of"gaps"between the Ag-NPs that form 3D"hot spots")and additional chemical enhancement(in detecting someπ-conjugated molecules).The SERS mechanism was explored in further detail via experimental analysis and confirmed by performing theoretical calculations.The large surface area of the 3D substrate(due to the large specific surface areas of the GQDs and 3D-graphene)results in a better enrichment effect which helps produce lower detection limits.In particular,the detection limits obtained using the Ag-NPs/GQDs/3D-graphene platform can reach 10^(-11)M for rhodamine 6G,10^(-10)M for methylene blue and dopamine,and 10^(-7)M for tetramethylthiuram disulfide and methyl parathion in apple juice(these are superior to most of the results reported using graphene-based SERS substrates).In summary,the 3D-platform Ag-NPs/GQDs/3D-graphene/Si shows outstanding SERS performance.It therefore has excellent application prospects in biochemical molecular detection and food safety monitoring.
