Electrochemical (EC) reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique...Electrochemical (EC) reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique for chemical analysis, yet its application to EC reactions is hindered by the strong attenuation of infrared (IR) light in both electrodes and electrolytes. Here we demonstrate that by incorporating appropriate sub-wavelength plasmonic structures at the metal electrode, the IR field at the EC interface can be greatly enhanced via the excitation of surface plasmon. This scheme facilitates in situ vibrational spectroscopic studies, especially using the surface-specific sum-frequency generation technique.展开更多
We investigate tunneling electron induced luminescence from isolated single porphyrin molecules that are decoupled by striped-phase self-assembled monolayer of octanethiol from the underneath Au(111) substrate. Intr...We investigate tunneling electron induced luminescence from isolated single porphyrin molecules that are decoupled by striped-phase self-assembled monolayer of octanethiol from the underneath Au(111) substrate. Intrinsic single-molecule electroluminescence has been realized by such decoupling at both bias polarities. The photon emission intensity acquired from the molecular lobe is found stronger than that from the molecular center. These re- sults provide useful information on the understanding of electroluminescent behavior and mechanism in molecular tunnel junctions.展开更多
We have investigated the self-assembly and light emission properties of organic α- sexithiophene (α-6T) molecules on Ag(100) under different coverage by scanning tunneling microscopy (STM). At very low coverag...We have investigated the self-assembly and light emission properties of organic α- sexithiophene (α-6T) molecules on Ag(100) under different coverage by scanning tunneling microscopy (STM). At very low coverage, the α-6T molecules form a unique enantiomer by grouping four molecules into a windmill supermolecular structure. As the coverage is increased,α-6T molecules tend to pack side by side into a denser stripe structure. Further increase of the coverage will lead to the layer-by-layer growth of molecules on Ag(100) with the lower-layer stripe pattern serving as a template. Molecular fluorescence for α-6T molecules on Ag(100) at a coverage of five monolayers has been detected by light excitations, which indicates a well decoupled electronic states for the top-layer α-6T molecules. However, the STM induced luminescent spectra for the same sample reveal only plasmonic-like emission. The absence of intramolecular fluorescence in this case suggests that the electronic decoupling is not a sufficient condition for generating photon emission from molecules. For intramolecular fluorescence to occur, the orientation of the dynamic dipole moment of molecules and the energy-level alignment at the molecule-metal interface are also important so that molecules can be effectively excited through efficient dipolar coupling with local plasmons and by injecting holes into the molecules.展开更多
We study surface plasmon polaritons excited on two-dimensional three-order dendritic structures. Previous studies show that split ring resonators (SRRs) can be used to obtain magnetic resonance, thus sustairdng surf...We study surface plasmon polaritons excited on two-dimensional three-order dendritic structures. Previous studies show that split ring resonators (SRRs) can be used to obtain magnetic resonance, thus sustairdng surface waves behaving like surface plasmon polaritons (SPPs). In this paper, we obtain detailed results on surface plasmon polaritons of several different grating structures and theoretically prove that this kind of structures can sustain SPPs. Besides, since dendritic structures can be fabricated by double template-assisted electrochemical deposition, it is worth noting that fabrication of SPP-based materials might be much easier.展开更多
By using the random phase approximation (RPA) in many-body perturbation theory,we calculate thepolarization function of the electron gas in graphene at finite temperature.Based on this,we calculate the temperaturedepe...By using the random phase approximation (RPA) in many-body perturbation theory,we calculate thepolarization function of the electron gas in graphene at finite temperature.Based on this,we calculate the temperaturedependent dielectric function ∈(q).The thermal effect on ∈(q) in various q regions is discussed.The temperaturedependence is found to be quadratic.We also investigate the plasmon dispersion relation at finite temperature,with thezero-temperature relation as a special case.The result is in good agreement with recent experimental data.展开更多
The optical embedded diffraction gratings with the internal refractive index modification in BK-7 glass plates were demonstrated using low-density plasma formation excited by a high-intensity femtosecond (130 fs) Ti...The optical embedded diffraction gratings with the internal refractive index modification in BK-7 glass plates were demonstrated using low-density plasma formation excited by a high-intensity femtosecond (130 fs) Ti: sapphire laser (λp=790 rim). The refractive index modifications with diameters ranging from 400 nm to 4 gm were photoinduced after plasma formation occurred upon irradiation with peak intensities of more than 1 ×10^13 W/cm2. The graded refractive index profile was fabricated to be a symmetric around the center of the point at which low-density plasma occurred. The maximum refractive index change (An) was estimated to be 1.5x10 2. Several optical embedded gratings in BK-7 glass plate were demonstrated with refractive index modification induced by the scanning of low-density plasma formation.展开更多
Electron-boson interaction is fundamental to a thorough understanding of various exotic properties emerging in many-body physics. In photoemission spectroscopy, photoelectron emission due to photon absorption would tr...Electron-boson interaction is fundamental to a thorough understanding of various exotic properties emerging in many-body physics. In photoemission spectroscopy, photoelectron emission due to photon absorption would trigger diverse collective excitations in solids, including the emergence of phonons,magnons, electron-hole pairs, and plasmons, which naturally provides a reliable pathway to study electron-boson couplings. While fingerprints of electron–phonon/-magnon interactions in this state-ofthe-art technique have been well investigated, much less is known about electron-plasmon coupling,and direct observation of the band renormalization solely due to electron-plasmon interactions is extremely challenging. Here by utilizing integrated oxide molecular-beam epitaxy and angle-resolved photoemission spectroscopy, we discover the long sought-after pure electron-plasmon couplinginduced low-lying plasmonic-polaron replica bands in epitaxial semimetallic SrIrO_(3) films, in which the characteristic low carrier concentration and narrow bandwidth combine to provide a unique platform where the electron-plasmon interaction can be investigated kinematically in photoemission spectroscopy. This finding enriches the forms of electron band normalization on collective modes in solids and demonstrates that, to obtain a complete understanding of the quasiparticle dynamics in 5 d electron systems, the electron-plasmon interaction should be considered on equal footing with the acknowledged electron–electron interaction and spin–orbit coupling.展开更多
The coupling of upconversion nanophosphors (UCNPs) with the surface plasmonic resonance (SPR) of noble metals is a promising way to improve luminescent efficiency of UCNPs; however, it is still a challenge to achi...The coupling of upconversion nanophosphors (UCNPs) with the surface plasmonic resonance (SPR) of noble metals is a promising way to improve luminescent efficiency of UCNPs; however, it is still a challenge to achieve stable, reproducible and effective upconversion luminescence (UCL) enhancement through such coupling. In this work, we present a novel strategy to improve UCL of NaYF4:ybB,Er3. UCNPs, by combining the near-field coupling of SPR of silver and the far-field coupling of poly(methyl methacrylate) (PMMA) opal photonic crystals (OPCs) with the UCNPs. In order to control the effective interaction distance between the UCNPs and the SPR, a porous silver film consisting of randomly distributed silver nanoparticles (NPs) (〉 100 nm) was prepared which demonstrated strong SPR over a broad wavelength range, and its coupling to the UCNPs was found to be much stronger than that of a dense film. In the far-field coupling of OPCs, the photonic stop band (PSB) of the PMMA OPCs was tuned to 980 nm, matching exactly the excitation light. By modulating the particle size of the UCNPs, and the direction and excitation power of the incident light, a maximum enhancement of 60-fold was observed, which is an important advance for metaMnduced UCL enhancement systems.展开更多
Aiming to enhance the luminescence yield of carbon nanotubes, we introduce a new class of hybrid nanoplasmonic colloidal systems (π-hybrids). Nanotubes dispersed in gold nanorod colloidal suspensions yield hybrid s...Aiming to enhance the luminescence yield of carbon nanotubes, we introduce a new class of hybrid nanoplasmonic colloidal systems (π-hybrids). Nanotubes dispersed in gold nanorod colloidal suspensions yield hybrid structures exhibiting enhanced luminescence up to a factor of 20. The novelty of the proposed enhancement mechanism relies on including metal proximity effects in addition to its localized surface plasmons. This simple, robust and flexible technique enhances the luminescence of nanotubes with chiralities whose enhancement has never reported before, for example the (8,4) tube.展开更多
We investigate theoretically the intervalley plasmon excitations(IPEs) in graphene monolayer within the random-phase approximation. We derive an analytical expression of the real part of the dielectric function. We fi...We investigate theoretically the intervalley plasmon excitations(IPEs) in graphene monolayer within the random-phase approximation. We derive an analytical expression of the real part of the dielectric function. We find a lowenergy plasmon mode with a linear anisotropic dispersion which depends on the Fermi energy and the dielectric constant of substrate. The IPEs show strongly anisotropic behavior, which becomes significant around the zigzag crystallographic direction. More interestingly, the group velocity of IPE varies from negative to positive, and vanishes at special energy.展开更多
文摘Electrochemical (EC) reactions play vital roles in many disciplines, and its molecular-level understanding is highly desired, in particular under reactions. The vibration spectroscopy is a powerful in situ technique for chemical analysis, yet its application to EC reactions is hindered by the strong attenuation of infrared (IR) light in both electrodes and electrolytes. Here we demonstrate that by incorporating appropriate sub-wavelength plasmonic structures at the metal electrode, the IR field at the EC interface can be greatly enhanced via the excitation of surface plasmon. This scheme facilitates in situ vibrational spectroscopic studies, especially using the surface-specific sum-frequency generation technique.
文摘We investigate tunneling electron induced luminescence from isolated single porphyrin molecules that are decoupled by striped-phase self-assembled monolayer of octanethiol from the underneath Au(111) substrate. Intrinsic single-molecule electroluminescence has been realized by such decoupling at both bias polarities. The photon emission intensity acquired from the molecular lobe is found stronger than that from the molecular center. These re- sults provide useful information on the understanding of electroluminescent behavior and mechanism in molecular tunnel junctions.
基金Author to whom correspondence should be addressed. E-mail: zcdong@ustc.edu.cn, FAX: +86-551-3600103 This work was supported by the National Basic Research Program of China (No.2006CB922003 and No.2011CB921402), the Chinese Academy of Sciences (No.KJCX2.YW.H06), and the National Natural Science Foundation of China (No.91021004, No.10574117, and No.10974186).
文摘We have investigated the self-assembly and light emission properties of organic α- sexithiophene (α-6T) molecules on Ag(100) under different coverage by scanning tunneling microscopy (STM). At very low coverage, the α-6T molecules form a unique enantiomer by grouping four molecules into a windmill supermolecular structure. As the coverage is increased,α-6T molecules tend to pack side by side into a denser stripe structure. Further increase of the coverage will lead to the layer-by-layer growth of molecules on Ag(100) with the lower-layer stripe pattern serving as a template. Molecular fluorescence for α-6T molecules on Ag(100) at a coverage of five monolayers has been detected by light excitations, which indicates a well decoupled electronic states for the top-layer α-6T molecules. However, the STM induced luminescent spectra for the same sample reveal only plasmonic-like emission. The absence of intramolecular fluorescence in this case suggests that the electronic decoupling is not a sufficient condition for generating photon emission from molecules. For intramolecular fluorescence to occur, the orientation of the dynamic dipole moment of molecules and the energy-level alignment at the molecule-metal interface are also important so that molecules can be effectively excited through efficient dipolar coupling with local plasmons and by injecting holes into the molecules.
基金Supported by the National Natural Science Foundation of China under Grants Nos. 10974030 and 10574027
文摘We study surface plasmon polaritons excited on two-dimensional three-order dendritic structures. Previous studies show that split ring resonators (SRRs) can be used to obtain magnetic resonance, thus sustairdng surface waves behaving like surface plasmon polaritons (SPPs). In this paper, we obtain detailed results on surface plasmon polaritons of several different grating structures and theoretically prove that this kind of structures can sustain SPPs. Besides, since dendritic structures can be fabricated by double template-assisted electrochemical deposition, it is worth noting that fabrication of SPP-based materials might be much easier.
基金Supported by National Natural Science Foundation of China under Grant No.10474001
文摘By using the random phase approximation (RPA) in many-body perturbation theory,we calculate thepolarization function of the electron gas in graphene at finite temperature.Based on this,we calculate the temperaturedependent dielectric function ∈(q).The thermal effect on ∈(q) in various q regions is discussed.The temperaturedependence is found to be quadratic.We also investigate the plasmon dispersion relation at finite temperature,with thezero-temperature relation as a special case.The result is in good agreement with recent experimental data.
基金Projects(2010-0001-226, 2010-0008-277) supported by NCRC(National Core Research Center) Program through the National Research Foundation of Korea funded by the Ministry of Education, Science and Technology
文摘The optical embedded diffraction gratings with the internal refractive index modification in BK-7 glass plates were demonstrated using low-density plasma formation excited by a high-intensity femtosecond (130 fs) Ti: sapphire laser (λp=790 rim). The refractive index modifications with diameters ranging from 400 nm to 4 gm were photoinduced after plasma formation occurred upon irradiation with peak intensities of more than 1 ×10^13 W/cm2. The graded refractive index profile was fabricated to be a symmetric around the center of the point at which low-density plasma occurred. The maximum refractive index change (An) was estimated to be 1.5x10 2. Several optical embedded gratings in BK-7 glass plate were demonstrated with refractive index modification induced by the scanning of low-density plasma formation.
基金This work was supported by the National Key R&D Program of the MOST of China(2016YFA0300204)the National Natural Science Foundation of China(11574337,11874199,and 11874263)+2 种基金supported by the National Basic Research Program of China(2015CB654901)Part of this research used Beamline 03U of the Shanghai Synchron Radiation Facility,which is supported by ME2 project(11227902)from the National Natural Science Foundation of Chinasupported by‘‘Award for Outstanding Member in Youth Innovation Promotion Association CAS”。
文摘Electron-boson interaction is fundamental to a thorough understanding of various exotic properties emerging in many-body physics. In photoemission spectroscopy, photoelectron emission due to photon absorption would trigger diverse collective excitations in solids, including the emergence of phonons,magnons, electron-hole pairs, and plasmons, which naturally provides a reliable pathway to study electron-boson couplings. While fingerprints of electron–phonon/-magnon interactions in this state-ofthe-art technique have been well investigated, much less is known about electron-plasmon coupling,and direct observation of the band renormalization solely due to electron-plasmon interactions is extremely challenging. Here by utilizing integrated oxide molecular-beam epitaxy and angle-resolved photoemission spectroscopy, we discover the long sought-after pure electron-plasmon couplinginduced low-lying plasmonic-polaron replica bands in epitaxial semimetallic SrIrO_(3) films, in which the characteristic low carrier concentration and narrow bandwidth combine to provide a unique platform where the electron-plasmon interaction can be investigated kinematically in photoemission spectroscopy. This finding enriches the forms of electron band normalization on collective modes in solids and demonstrates that, to obtain a complete understanding of the quasiparticle dynamics in 5 d electron systems, the electron-plasmon interaction should be considered on equal footing with the acknowledged electron–electron interaction and spin–orbit coupling.
文摘The coupling of upconversion nanophosphors (UCNPs) with the surface plasmonic resonance (SPR) of noble metals is a promising way to improve luminescent efficiency of UCNPs; however, it is still a challenge to achieve stable, reproducible and effective upconversion luminescence (UCL) enhancement through such coupling. In this work, we present a novel strategy to improve UCL of NaYF4:ybB,Er3. UCNPs, by combining the near-field coupling of SPR of silver and the far-field coupling of poly(methyl methacrylate) (PMMA) opal photonic crystals (OPCs) with the UCNPs. In order to control the effective interaction distance between the UCNPs and the SPR, a porous silver film consisting of randomly distributed silver nanoparticles (NPs) (〉 100 nm) was prepared which demonstrated strong SPR over a broad wavelength range, and its coupling to the UCNPs was found to be much stronger than that of a dense film. In the far-field coupling of OPCs, the photonic stop band (PSB) of the PMMA OPCs was tuned to 980 nm, matching exactly the excitation light. By modulating the particle size of the UCNPs, and the direction and excitation power of the incident light, a maximum enhancement of 60-fold was observed, which is an important advance for metaMnduced UCL enhancement systems.
文摘Aiming to enhance the luminescence yield of carbon nanotubes, we introduce a new class of hybrid nanoplasmonic colloidal systems (π-hybrids). Nanotubes dispersed in gold nanorod colloidal suspensions yield hybrid structures exhibiting enhanced luminescence up to a factor of 20. The novelty of the proposed enhancement mechanism relies on including metal proximity effects in addition to its localized surface plasmons. This simple, robust and flexible technique enhances the luminescence of nanotubes with chiralities whose enhancement has never reported before, for example the (8,4) tube.
基金Supported by the National Basic Research Program of China(973 Program)under Grant No.2013CB934001the State Key Laboratory of Software Development Environment under Grant No.SKLSDE-2013ZX-28
文摘We investigate theoretically the intervalley plasmon excitations(IPEs) in graphene monolayer within the random-phase approximation. We derive an analytical expression of the real part of the dielectric function. We find a lowenergy plasmon mode with a linear anisotropic dispersion which depends on the Fermi energy and the dielectric constant of substrate. The IPEs show strongly anisotropic behavior, which becomes significant around the zigzag crystallographic direction. More interestingly, the group velocity of IPE varies from negative to positive, and vanishes at special energy.