Browsing by Author "Sun, Quan"

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Chiral Second-Harmonic Generation from Monolayer WS2/Aluminum Plasmonic Vortex Metalens
(2020-04-08)
Guo, Wan-Ping
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Liang, Wei-Yun
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Cheng, Chang-Wei
;
Wu, Wei-Lin
;
Wang, Yen-Ting
Two-dimensional spiral plasmonic structures have emerged as a versatile approach to generate near-field vortex fields with tunable topological charges. We demonstrate here a far-field approach to observe the chiral second-harmonic generation (SHG) at designated visible wavelengths from a single plasmonic vortex metalens. This metalens comprises an Archimedean spiral slit fabricated on atomically flat aluminum epitaxial film, which allows for precise tuning of plasmonic resonances and subsequent transfer of two-dimensional materials on top of the spiral slit. The nonlinear optical measurements show a giant SHG circular dichroism. Furthermore, we have achieved an enhanced chiral SHG conversion efficiency (about an order of magnitude greater than the bare aluminum lens) from monolayer tungsten disulfide (WS2)/aluminum metalens, which is designed at the C-exciton resonance of WS2. Since the C-exciton is not a valley exciton, the enhanced chiral SHG in this hybrid system originates from the plasmonic vortex field-enhanced SHG under the optical spin-orbit interaction.
Control of plasmon dephasing time using stacked nanogap gold structures for strong near-field enhancement
(2019-03-01)
Ueno, Kosei
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Yang, Jinghuan
;
Sun, Quan
;
Aoyo, Daisuke
;
Yu, Han
The construction of metallic nanostructures with strong near-field enhancement is becoming increasingly significant for the practical use of plasmonic devices, such as plasmonic sensors and light-energy conversion systems. Importantly, the near-field enhancement effect depends on the plasmon dephasing time. Here, we propose a method for controlling plasmon dephasing time by utilizing plasmonic coupling for stronger near-field enhancement. Ordered arrays of stacked nanogap gold (Au) structures composed of a metal/insulator/metal nanostructure were fabricated by electron beam lithography and dry etching processes on a niobium-doped titanium dioxide substrate. The dark plasmon mode was excited by the near-field coupling between the upper and lower Au nanostructures separated by an alumina layer with a thickness of 15 nm. A strong near-field enhancement effect was induced by the localization of the electromagnetic field between the upper and lower Au nanostructures and the longer plasmon dephasing time based on the excitation of the dark plasmon mode. It is noteworthy that the dephasing time of the dark plasmon mode measured by time-resolved photoemission electron microscopy was extended 3-fold compared with that of the plasmon mode of the Au nanoblock, which can be controlled by the structural design of the stacked nanogap Au structures. (C) 2018 Elsevier Ltd. All rights reserved.
Correlation between Near-Field Enhancement and Dephasing Time in Plasmonic Dimers
(2020-04-24)
Li, Yaolong
;
Sun, Quan
;
Zu, Shuai
;
Shi, Xu
;
Liu, Yunquan
Near-field enhancement and dephasing time play critical roles in several applications of localized surface plasmon resonance. Here, using an example gold dimer system, we reveal the correlation between the near-field enhancement and dephasing time via time-resolved photoemission electron microscopy. Compared with isolated particles, dimers with small gap sizes show stronger near-field enhancement and shorter dephasing times. These results are well reproduced by numerical simulations and further explained by a coupled dipole approximation model. The roles of near- and far-field coupling and plasmon localization in balancing near-field enhancement and dephasing time are also unveiled.
Dissecting the Few-Femtosecond Dephasing Time of Dipole and Quadrupole Modes in Gold Nanoparticles Using Polarized Photoemission Electron Microscopy
(2016-03)
Sun, Quan
;
Yu, Han
;
Ueno, Kosei
;
Kubo, Atsushi
;
Matsuo, Yasutaka
Dipole and quadrupole modes are the two lowest orders of localized surface plasmon resonance (LSPR) eigenmodes in metallic nanoparticles. Of these two modes, the quadrupole mode is forbidden for symmetric metallic nanoparticles excited by linearly polarized light at normal incidence. Here, we demonstrate excitation of the quadrupole mode in symmetrical gold (Au) nanoblocks shined with s -polarized light at oblique incidence. In particular, we probe the near -field LSPR in Au nanoblocks using photoemission electron microscopy (PEEM) and find that at oblique incidence, the dipole and quadrupole modes can be selectively excited, in terms of near -field enhancement, by manipulating the light polarization state. More importantly, by time -resolved PEEM measurements, we experimentally demonstrate that the quadrupole mode in symmetrical Au nanoblocks has longer dephasing time than that of the dipole mode.
Engineering Ultrafast Carrier Dynamics at the Graphene/GaAs Interface by Bulk Doping Level
(2019-10-01)
Yang, Jinghuan
;
Sun, Quan
;
Liu, Wei
;
Zhang, Zhibin
;
Hu, Xiaoyong
Carrier dynamics, the most fundamental process in electronics and optoelectronics, has drawn great attentions owing to its crucial role in property engineering of materials. Exploration and regulation of carrier dynamics are essential for designing devices with specific functions and optimizing their performances. However, the lack of conventional tools with simultaneous ultrafast temporal and ultrasmall spatial resolution has impeded direct observation and manipulation of carrier dynamics at both the femtosecond and nanometer scale. In this study, the direct observation and modulation of ultrafast carrier dynamics at the graphene/gallium arsenide (GaAs) interface is achieved by tuning the doping level of bulk GaAs. This successful characterization is performed using advanced in situ photoemission electron microscopy combined with the ultrafast pump-probe technique. It is found that a change in the doping level in GaAs can change its band bending and switch the hot-carrier transfer direction at the graphene/GaAs interface with a lifetime reduction of nearly six times. This work paves the way of engineering ultrafast carrier dynamics at 2D interfaces by modifying the 3D bulk properties, and also provides a platform for fundamental studies of ultrafast physics with high spatial resolution.
Enhanced water splitting under modal strong coupling conditions
(2018-10-01)
Shi, Xu
;
Ueno, Kosei
;
Oshikiri, Tomoya
;
Sun, Quan
;
Sasaki, Keiji
Strong coupling between plasmons and optical modes, such as waveguide or resonator modes, gives rise to a splitting in the plasmon absorption band. As a result, two new hybrid modes are formed that exhibit near-field enhancement effects. These hybrid modes have been exploited to improve light absorption in a number of systems. Here we show that this modal strong coupling between a Fabry-Perot nanocavity mode and a localized surface plasmon resonance (LSPR) facilitates water splitting reactions. We use a gold nanoparticle (Au-NP)/TiO2/Au-film structure as a photoanode. This structure exhibits modal strong coupling between the Fabry-Perot nanocavity modes of the TiO2 thin film/Au film and LSPR of the Au NPs. Electronic excitation of the Au NPs is promoted by the optical hybrid modes across a broad range of wavelengths, followed by a hot electron transfer to TiO2. A key feature of our structure is that the Au NPs are partially inlaid in the TiO2 layer, which results in an enhancement of the coupling strength and water-oxidation efficiency. We observe an 11-fold increase in the incident photon-to-current conversion efficiency with respect to a photoanode structure with no Au film. Also, the internal quantum efficiency is enhanced 1.5 times under a strong coupling over that under uncoupled conditions.
Exotic Mode Suppression in Plasmonic Heterotrimer System
(2019-01-17)
Song, Hanfa
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Sun, Quan
;
Li, Jie
;
Yang, Fan
;
Yang, Jinghuan
We investigate the far- and near-field properties of plasmonic heterotrimers with small detuning of the eigenfrequency numerically, theoretically, and experimentally. In our simulations, we find that the dipolar mode of the middle nanorod in the trimer system is greatly suppressed in both far and near fields. This phenomenon is confirmed by our subsequent experiments. The far-field suppression can be interpreted by the destructive interference due to the antiphase dipolar response of the respective nanorod. To deeply understand the underlying physics, an analytical model considering both the near-field-mediated direct coupling and radiative-field-mediated indirect coupling is adopted. We determine that the radiative field coupling, which is stronger in the trimer system with a smaller detuning, plays an essential role in mode suppression in the near field. Our work will provide new thoughts on the fundamental mechanisms of plasmon coupling and plasmon-based applications.
Exploring Coupled Plasmonic Nanostructures in the Near Field by Photoemission Electron Microscopy
(2016-11)
Yu, Han
;
Sun, Quan
;
Ueno, Kosei
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Oshikiri, Tomoya
;
Kubo, Atsushi
The extraordinary optical properties of coupled plasmonic nanostructures make these materials potentially useful in many applications; thus, they have received enormous attention in basic and applied research. Coupled plasmon modes have been characterized predominantly using far-field spectroscopy. In near-field spectroscopy, the spectral response of local field enhancement in coupled plasmonic nanostructures remains largely unexplored, especially experimentally. Here, we investigate the coupled gold dolmen nanostructures in the near field using photoemission electron microscopy, with wavelength tunable femtosecond laser pulses as an excitation source. The spatial evolution of near-field mapping of an individual dolmen structure with the excitation wavelength was successfully obtained. In the near field, we spatially resolved an anti-bonding mode and a bonding mode as the result of plasmon hybridization. Additionally, the quadrupole plasmon mode that could be involved in the formation of a Fano resonance was also revealed by spatially resolved near-field spectra, but it only contributed little to the total near-field enhancement. On the basis of these findings, we obtained a better understanding of the near-field nanostructures, where the plasmon hybridization and the plasmonic Fano resonance were mixed.
Exploring the Near-Field of Strongly Coupled Waveguide-Plasmon Modes by Plasmon-Induced Photocurrent Generation Using a Gold Nanograting-Loaded Titanium Dioxide Photoelectrode
(2017-10-05)
Guo, Jingchun
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Ueno, Kosei
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Yang, Jinghuan
;
Shi, Xu
;
Li, Jie
Near-field spectrum measurement techniques, including near-field scanning optical microscopy, electron energy loss spectroscopy, and multiphoton photoemission electron microscopy, are powerful means to investigate near-field interactions directly on closely spaced metallic nanoparticles or a metallic nanostructure coupled with optical modes, such as whispering gallery mode and waveguide mode, which are called coupled plasmonic systems. In the present study, we have successfully measured the near-field spectra of coupled plasmonic systems using a simple photoelectrochemical measurement based on plasmon-induced water oxidation. Coupling was explored between the localized surface plasmon resonance (LSPR.) mode and waveguide mode of periodic gold nanogratings patterned on a thin titanium dioxide waveguide film. It is known that the far-field reflection spectrum of this waveguide-LSPR coupling system shows a complicated shape with multiple peaks, and the coupling has been explored by numerical electromagnetic simulations so far. However, in this study, it was clearly elucidated that an internal quantum efficiency (IQE) spectrum observed in the plasmon-induced photocurrent generation has successfully reproduced the near-field spectrum predicted by electromagnetic simulations under the coupling conditions. The photocurrent generation based on the plasmon-induced charge separation is due to the near-field effect, and it can be considered that the IQE spectrum corresponds to the near-field spectrum. This study paves a new way to indirectly measure the near-field spectrum of plasmonic systems.
Interplay of hot electrons from localized and propagating plasmons
(2017-10-03)
Chung V. Hoang
;
Hayashi, Koki
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Ito, Yasuo
;
Gorai, Naoki
;
Allison, Giles
Plasmon-induced hot-electron generation has recently received considerable interest and has been studied to develop novel applications in optoelectronics, photovoltaics and green chemistry. Such hot electrons are typically generated from either localized plasmons in metal nanoparticles or propagating plasmons in patterned metal nanostructures. Here we simultaneously generate these heterogeneous plasmon-induced hot electrons and exploit their cooperative interplay in a single metal-semiconductor device to demonstrate, as an example, wavelength-controlled polarity-switchable photoconductivity. Specifically, the dual-plasmon device produces a net photocurrent whose polarity is determined by the balance in population and directionality between the hot electrons from localized and propagating plasmons. The current responsivity and polarity-switching wavelength of the device can be varied over the entire visible spectrum by tailoring the hot-electron interplay in various ways. This phenomenon may provide flexibility to manipulate the electrical output from light-matter interaction and offer opportunities for biosensors, long-distance communications, and photoconversion applications.
Manipulation of the dephasing time by strong coupling between localized and propagating surface plasmon modes
(2018-11-19)
Yang, Jinghuan
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Sun, Quan
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Ueno, Kosei
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Shi, Xu
;
Oshikiri, Tomoya
Strong coupling between two resonance modes leads to the formation of new hybrid modes exhibiting disparate characteristics owing to the reversible exchange of information between different uncoupled modes. Here, we realize the strong coupling between the localized surface plasmon resonance and surface plasmon polariton Bloch wave using multilayer nanostructures. An anticrossing behavior with a splitting energy of 144 meV can be observed from the far-field spectra. More importantly, we investigate the near-field properties in both the frequency and time domains using photoemission electron microscopy. In the frequency domain, the near-field spectra visually demonstrate normal-mode splitting and display the extent of coupling. Importantly, the variation of the dephasing time of the hybrid modes against the detuning is observed directly in the time domain. These findings signify the evolution of the dissipation and the exchange of information in plasmonic strong coupling systems and pave the way to manipulate the dephasing time of plasmon modes, which can benefit many applications of plasmonics.
Near-field spectral properties of coupled plasmonic nanoparticle arrays
(2017-03-20)
Yu, Han
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Sun, Quan
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Yang, Jinghuan
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Ueno, Kosei
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Oshikiri, Tomoya
We investigated the grating effect in complex gold dolmen structures, in which multiple plasmon modes are present due to plasmon hybridization, experimentally from both the far field and the near field. In particular, the near-field properties were investigated using photoemission electron microscopy, and it was demonstrated that two hybridized plasmon modes on the dolmen structures could be influenced by the grating effect. For comparison, we also investigated the grating effect in arrays of simple nanoblocks and heptamer structures, which were supposed to support a strong bright plasmon mode and a strong dark plasmon mode, respectively, in the near field. We found that the spectral responses of the two hybridized modes on the dolmen structures as the pitch size changed evolved in a manner similar to that of the bright dipole mode on the nanoblocks, whereas the dark mode on the heptamer structures is less sensitive to the pitch size. (C) 2017 Optical Society of America
Optical Characterization of Gold Nanoblock Dimers: From Capacitive Coupling to Charge Transfer Plasmons and Rod Modes
(2018-08-09)
Su, Man-Nung
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Sun, Quan
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Ueno, Kosei
;
Chang, Wei-Shun
;
Misawa, Hiroaki
The optical properties of plasmonic dimers consisting of two adjacent metal nanoparticles can be tuned over a broad spectral range by changing only slightly the dimer geometry. Most drastic are the changes in the smallest interparticles distances, and often only optical spectroscopy together with electromagnetic simulations yields insights into the geometry of the junction. Here, we study the coupling of gold nanoblock dimers, two square nanoantennas with different nanogaps between their closest corners. We identify three different coupling regimes-capacitively coupled, conductively bridged, and fused dimers-and optically characterize the transitions between them. By combining sample array fabrication, single-particle hyperspectral measurements, and electromagnetic simulations, we were able to examine in detail the effects of junction geometry on the resonance energy and intensity of the plasmon modes supported by gold nanoblock dimers.
Solid-State Plasmonic Solar Cells
(2018-03-28)
Ueno, Kosei
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Oshikiri, Tomoya
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Sun, Quan
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Shi, Xu
;
Misawa, Hiroaki
Metallic nanoparticles such as silver and gold show localized surface plasmon resonances (LSPRs), which are associated with near-field enhancement effects in the vicinity of nanoparticles. Therefore, strong light-matter interaction is induced by the near-field enhancement effects of LSPRs. Because the resonant wavelength of LSPRs can be easily controlled by the size and shape of the metallic nanoparticles in the visible and near-infrared wavelength range, LSPRs have received considerable attention as optical antennae for light energy conversion systems such as solar cells. LSPRs decay very quickly as a result of light scattering and excitation of electron-hole pairs in the metal itself. However, in addition to the near-field enhancement effect, this light scattering and electron-hole pair excitation, which are known to cause loss of LSPRs, can be utilized as a solar cell enhancement mechanism. Here, we focus on plasmonic solid-state solar cells. The mechanisms of the light scattering by LSPRs, near-field enhancement, and plasmon-induced charge separation based on electron-hole pair excitations can be clarified. We review the related studies from the viewpoint of these mechanisms rather than material science.
Spatial evolution of the near-field distribution on planar gold nanoparticles with the excitation wavelength across dipole and quadrupole modes
(2017-06-01)
Yang, Jinghuan
;
Sun, Quan
;
Yu, Han
;
Ueno, Kosei
;
Misawa, Hiroaki
We investigate the superposition properties of the dipole and quadrupole plasmon modes in the near field both experimentally, by using photoemission electron microscopy (PEEM), and theoretically. In particular, the asymmetric near-field distributions on gold (Au) nanodisks and nanoblocks under oblique incidence with different polarizations are investigated in detail. The results of PEEM measurements show that the evolutions of the asymmetric near-field distributions are different between the excitation with s-polarized and p-polarized light. The experimental results can be reproduced very well by numerical simulations and interpreted as the superposition of the dipole and quadrupole modes with the help of analytic calculations. Moreover, we hypothesize that the electrons collected by PEEM are mainly from the plasmonic hot spots located at the plane in the interface between the Au particles and the substrate in the PEEM experiments. (C) 2017 Chinese Laser Press
Surface plasmon optical antennae in the infrared region with high resonant efficiency and frequency selectivity
(2016-08-08)
Ueno, Kosei
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Sun, Quan
;
Mino, Masahiro
;
Itoh, Takumi
;
Oshikiri, Tomoya
Infrared light has received attention for sensor applications, including fingerprint spectroscopy, in the bioengineering and security fields. Surface plasmon physics enables the operation of a light harvesting optical antenna. Gold nanochains exhibit localized surface plasmon resonance (LSPR) in the infrared region with high frequency selectivity. However, a feasible design for optical antennae with a higher resonant efficiency and frequency selectivity as a function of structural design and periodicity is still unknown. In the present study, we investigated the relationship between the resonant efficiency and frequency selectivity as a function of the structural design of gold nanochains and explored structural periodicity for obtaining highly frequency-selective optical antennae. An optical antenna design with higher resonant efficiency is proposed on the basis of its efficient interaction with non-polarized light. (C) 2016 Optical Society of America
Twisted Surface Plasmons with Spin-Controlled Gold Surfaces
(2019-04-01)
Tsai, Wei-Yi
;
Sun, Quan
;
Hu, Guangwei
;
Wu, Pin Chieh
;
Lin, Ren Jie
Twisted photon, associated with orbital angular momentum (OAM), is a physical notion that has long captivated the intriguing imagination and wide applications. Owing to the native orthogonality between different topological charges of the vortices, it will be of significant value to generate, access, and discriminate the vortex on integrated chips. Archimedean spirals or multiple split gratings are commonly employed to generate OAMs on plasmonic films. However, the single-crystalline plasmonic surface sets a very stringent condition of probing the on-chip OAM dynamics at sub-femtosecond scale. In previous reports, spins of the incident light and actual topological charge of the on-chip OAM generator are also hybridized due to the intrinsic spin-to-orbital angular momentum conversion, making the direct discrimination of plasmonic vortex impossible. Here, a paradigm of generating twisted surface plasmons is presented in a fully spin-controlled fashion. With the two-photon photoemission electron microscopy, the dynamics of OAM formation is demonstrated at subwavelength spatial resolution and sub-femtosecond temporal resolution simultaneously, revealing its OAM-dependent angular velocity. In addition, this scheme of twisting on-chip plasmons shows that the challenging crystalline requirement of the thin film can be significantly alleviated. The results open up a distinct way to multiplex, record, and read the information with plasmons.
Ultrafast Electron Cooling and Decay in Monolayer WS2 Revealed by Time- and Energy-Resolved Photoemission Electron Microscopy
(2020-05-13)
Li, Yaolong
;
Liu, Wei
;
Wang, Yunkun
;
Xue, Zhaohang
;
Leng, Yu-Chen
A comprehensive understanding of the ultrafast electron dynamics in two-dimensional transition metal dichalcogenides (TMDs) is necessary for their applications in optoelectronic devices. In this work, we contribute a study of ultrafast electron cooling and decay dynamics in the supported and suspended monolayer WS2 by time- and energy-resolved photoemission electron microscopy (PEEM). Electron cooling in the Q valley of the conduction band is clearly resolved in energy and time, on a time scale of 0.3 ps. Electron decay is mainly via a defect trapping process on a time scale of several picoseconds. We observed that the trap states can be produced and increased by laser illumination under an ultrahigh vacuum, and the higher local optical-field intensity led to the faster increase of trap states. The enhanced defect trapping could significantly modify the carrier dynamics and should be paid attention to in photoemission experiments for two-dimensional materials.
Versatile plasmonic-effects at the interface of inverted perovskite solar cells
(2017)
Shalan, Ahmed Esmail
;
Oshikiri, Tomoya
;
Sawayanagi, Hiroki
;
Nakamura, Keisuke
;
Ueno, Kosei
Plasmonics is a highly promising approach to enhancing the light-harvesting properties of hybrid organic/ inorganic perovskite solar cells. In the present work, our cells have a p-i-n inverted planar structure. An ultrathin NiO film with two different thicknesses of 5 and 10 nm prepared by a pulsed laser deposition process on an ITO substrate with a faceted and furrowed surface enabled the formation of a continuous and compact layer of well-crystallized CH3NH3PbI3 via an anti-solvent chlorobenzene process. The coverage mechanism of the NiO film on the ITO was clearly demonstrated through the J-V and external quantum efficiency (EQE) curves. Moreover, the results demonstrated that the gold nanoislands (Au NIs) increased the power conversion efficiency to 5.1%, almost double that of the samples without Au NIs. This result is due to the excitation of surface plasmons, which is characterized by strong scattering and enhancement of the electric field in the vicinity of the Au NIs loaded at the interface between the NiO and perovskite films. Additionally, we observed an enhancement of the EQE at wavelengths shorter than the plasmon resonance peak. In the current state, we speculate that the plasmoelectric potential effect is considered to be a good explanation of the photocurrent enhancement at the off-resonance region. Our work provides good guidance for the design and fabrication of solar-energy-related devices employing NiO electrodes and plasmonic Au NIs.
Versatile plasmonic-effects at the interface of inverted perovskite solar cells
(2017)
Shalan, Ahmed Esmail
;
Oshikiri, Tomoya
;
Sawayanagi, Hiroki
;
Nakamura, Keisuke
;
Ueno, Kosei
Plasmonics is a highly promising approach to enhancing the light-harvesting properties of hybrid organic/ inorganic perovskite solar cells. In the present work, our cells have a p-i-n inverted planar structure. An ultrathin NiO film with two different thicknesses of 5 and 10 nm prepared by a pulsed laser deposition process on an ITO substrate with a faceted and furrowed surface enabled the formation of a continuous and compact layer of well-crystallized CH3NH3PbI3 via an anti-solvent chlorobenzene process. The coverage mechanism of the NiO film on the ITO was clearly demonstrated through the J-V and external quantum efficiency (EQE) curves. Moreover, the results demonstrated that the gold nanoislands (Au NIs) increased the power conversion efficiency to 5.1%, almost double that of the samples without Au NIs. This result is due to the excitation of surface plasmons, which is characterized by strong scattering and enhancement of the electric field in the vicinity of the Au NIs loaded at the interface between the NiO and perovskite films. Additionally, we observed an enhancement of the EQE at wavelengths shorter than the plasmon resonance peak. In the current state, we speculate that the plasmoelectric potential effect is considered to be a good explanation of the photocurrent enhancement at the off-resonance region. Our work provides good guidance for the design and fabrication of solar-energy-related devices employing NiO electrodes and plasmonic Au NIs.