Resonant Excitation Research Articles

Probing Interlayer Interactions and Commensurate-Incommensurate Transition in Twisted Bilayer Graphene through Raman Spectroscopy.

Twisted 2D layered materials have garnered much attention recently as a class of 2D materials whose interlayer interactions and electronic properties are dictated by the relative rotation/twist angle between the adjacent layers. In this work, we explore a prototype of such a twisted 2D system, artificially stacked twisted bilayer graphene (TBLG), where we probe, using Raman spectroscopy, the changes in the interlayer interactions and electron-phonon scattering pathways as the twist angle is varied from 0° to 30°. The long-range Moiré potential of the superlattice gives rise to additional intravalley and intervalley scattering of the electrons in TBLG, which has been investigated through their Raman signatures. Density functional theory (DFT) calculations of the electronic band structure of the TBLG superlattices were found to be in agreement with the resonant Raman excitations across the van Hove singularities in the valence and conduction bands predicted for TBLG due to hybridization of bands from the two layers. We also observe that the relative rotation between the graphene layers has a marked influence on the second order overtone and combination Raman modes signaling a commensurate-incommensurate transition in TBLG as the twist angle increases. This serves as a convenient and rapid characterization tool to determine the degree of commensurability in TBLG systems.

Beyond single-molecule chemistry for electrified interfaces using molecule polaritons

Abstract This review introduces the preparation, observation, and characterization of systems of molecule polaritons. We summarize recent progress by our group on the control of molecular properties in the spaces of various optical cavities, such as plasmonic metal nanostructures and Fabry–Perot mirrors. After stating our motivations, we introduce topics on single-molecule observations based on surface-enhanced Raman scattering (SERS) spectroscopy. Our original findings are not limited to the ultrasensitive detection of molecules/materials, but include unique resonant enhancements of SERS through exotic electronic excitation processes at electrified interfaces. Comprehensive analyses of SERS spectra provide novel routes to electronic excitation using plasmonic metal nanostructures. This behavior leads to the distinct photoenergy conversion based on excited electrons and holes with anomalous electrochemical potentials. Such unique resonant electronic excitation emerges as a large optical force that can be used to manipulate small single molecules on surfaces in solution, even at room temperature. We also introduce systems for examining unique interactions between molecules and the optical modes of cavities, from single molecules to molecular ensembles. Plasmonic surface lattices and Fabry–Perot mirrors allow the formation of electronic and vibrational strong coupling states, respectively, showing unique properties of molecule polaritons, even under dark conditions, i.e. without photoillumination.

Research on ionization characteristics of atmospheric pressure pulse-modulated microwave He/air plasma jet

The atmospheric pressure pulsed microwave He plasma jet has the advantages of high electron density and abundant active particles, but its shrinking on the discharge electrode morphology limits its application range. In order to modulate a He plasma jet with a longer plume and study its ionization development characteristics, we constructed a dual-channel pulsed microwave coaxial discharge device. He and air were, respectively, injected into the inner and outer gas channels of the resonator to generate a double-layer atmospheric pressure microwave plasma jet with a longer plume. It is observed that the bifurcation of the stratified plasma jet will occur by changing the gas flow. The ionization development of plasma jet was observed by using enhanced charge-coupled device and microwave Rayleigh scattering apparatus measured the space-time evolution of plasma and observed the three times ionization enhancement process of plasma jet development. The spectral lines of the active products associated with Penning ionization were observed by using a fiber optic spectrometer. A fluid model was constructed to simulate and analyze that under the condition of sufficient He flow rate (He flow rate is above 0.6 slm), there will be sufficient and stable He mole fraction (64%) at the stratification of the plasma jet. The experimental and simulation results show that the jet profile of the microwave He plasma is related to the inlet structure of the discharger and He flow rate. Stratified intake structure can produce stratified He plasma jet, and the unique appearance of bifurcation of jet can be produced by changing the flow rate of He. In the bifurcation process of the plasma jet, the product of Penning ionization inhibits the development of the main branch of the plasma jet, and the secondary electron avalanche of the local electric field promotes the formation of the branch of the plasma jet and is accompanied by the enhancement of the second ionization. The ionization mechanism of microwave He plasma is the resonance excitation of local enhanced electric field, the advance of ionizing waves, and the interaction between the spatially distributed active particles.

Resonant excitation of terahertz surface magnetoplasmons by optical rectification over a rippled surface of n-type indium antimonide

We analysed the excitation of a surface magnetoplasmon wave by the mode conversion of a p-polarized laser beam over a rippled semiconductor (n-type)-free space interface. The pump surface magnetoplasmon wave exerts a ponderomotive force on the free electrons in the semiconductor, imparting a linear oscillatory velocity at the laser modulation frequency to them. This linear oscillatory velocity couples with the modulated electron density to produce a current density, which develops a resonant surface magnetoplasmon wave in the terahertz region. The amplitude of the terahertz surface magnetoplasmon wave can be tuneable with an external magnetic field and the semiconductor's temperature.

Plasmonic‐assisted Electrocatalysis for CO2 Reduction Reaction

AbstractIntegrating plasmonic features as an emerging strategy for enhancing electrocatalysis for the carbon dioxide reduction reaction (CO2RR). The key parameters responsible for the enhanced electrocatalysis performance are the local heating, the hot carriers, and near‐field enhancement induced by localized surface plasmon resonance (LSPR, that is, plasmonic) excitation. This review provides a concise overview of the fundamental mechanism of CO2RR, detailing the generation and decay of plasmonic and the energy transfer dynamics between plasmonic nanostructures and adsorbates. It further involves recent progress in plasmonic‐assisted electrocatalysis for CO2RR, including experimental and theoretical research to decipher plasmonic mechanisms. Finally, it ends with an insightful discussion of the existing challenges and potential future directions in this field.

Wide angle anapole excitation in stacked resonators.

In the search for resonances with high localized field strengths in all-dielectric nanophotonics, novel states such as anapoles, hybrid anapoles and bound states in the continuum have been realized. Of these, the anapoles are the most readily achievable. Interaction between vertically stacked disks supporting anapole resonances increases the field localization further. When fabricated from materials with high non-linear coefficients, such stacked disk pillars can be used as non-linear antennas. The excitation of such 3D pillars often includes off normal incidence when using focusing optics. Therefore, it is important to evaluate the angular and polarization response of such pillars. In the paper we fabricate pillars with three AlGaAs disks in a stack separated by stems of GaAs. The angular and polarization responses are evaluated experimentally with integrating sphere measurements and numerically through simulation, multipole decomposition and quasi-normal modes. We find that the stacked geometry shows hybridized anapole excitation for a broad span of incidence angles, with tunability of the individual multipolar response up to octupoles, including an electric octupole anapole, and we show how the average enhanced confined energy varies under angled excitation. The results show that the vertical stacked geometry can be used with highly focusing optics for efficient in-coupling to the hybridized anapole.

On-Demand Generation of Indistinguishable Photons in the Telecom C-Band Using Quantum Dot Devices.

Semiconductor quantum dots (QDs) enable the generation of single and entangled photons, which are useful for various applications in photonic quantum technologies. Specifically for quantum communication via fiber-optical networks, operation in the telecom C-band centered around 1550 nm is ideal. The direct generation of QD-photons in this spectral range with high quantum-optical quality, however, remained challenging. Here, we demonstrate the coherent on-demand generation of indistinguishable photons in the telecom C-band from single QD devices consisting of InAs/InP QD-mesa structures heterogeneously integrated with a metallic reflector on a silicon wafer. Using pulsed two-photon resonant excitation of the biexciton-exciton radiative cascade, we observe Rabi rotations up to pulse areas of 4π and a high single-photon purity in terms of g(2)(0) = 0.005(1) and 0.015(1) for exciton and biexciton photons, respectively. Applying two independent experimental methods, based on fitting Rabi rotations in the emission intensity and performing photon cross-correlation measurements, we consistently obtain preparation fidelities at the π-pulse exceeding 80%. Finally, performing Hong-Ou-Mandel-type two-photon interference experiments, we obtain a photon-indistinguishability of the full photon wave packet of up to 35(3)%, representing a significant advancement in the photon-indistinguishability of single photons emitted directly in the telecom C-band.

Ultrasensitive Upconversion Nanoparticle Immunoassay for Human Serum Cardiac Troponin I Detection Achieved with Resonant Waveguide Grating.

Selective detection of biomarkers at low concentrations in blood is crucial for the clinical diagnosis of many diseases but remains challenging. In this work, we aimed to develop an ultrasensitive immunoassay that can detect biomarkers in serum with an attomolar limit of detection (LOD). We proposed a sandwich-type heterogeneous immunosensor in a 3 × 3 well array format by integrating a resonant waveguide grating (RWG) substrate with upconversion nanoparticles (UCNPs). UCNPs were used to label a target biomarker captured by capture antibody molecules immobilized on the surface of the RWG substrate, and the RWG substrate was used to enhance the upconversion luminescence (UCL) of UCNPs through excitation resonance. The LOD of the immunosensor was greatly reduced due to the increased UCL of UCNPs and the reduction of nonspecific adsorption of detection antibody-conjugated UCNPs on the RWG substrate surface by coating the RWG substrate surface with a carboxymethyl dextran layer. The immunosensor exhibited an extremely low LOD [0.24 fg/mL (9.1 aM)] and wide detection range (1 fg/mL to 100 pg/mL) in the detection of cardiac troponin I (cTnI). The cTnI concentrations in human serum samples collected at different times during cyclophosphamide, epirubicin, and 5-fluorouracil (CEF) chemotherapy in a breast cancer patient were measured by an immunosensor, and the results showed that the CEF chemotherapy did cause cardiotoxicity in the patient. Having a higher number of wells in such an array-based biosensor, the sensor can be developed as a high-throughput diagnostic tool for clinically important biomarkers.

Highly Indistinguishable Single Photons from Droplet-Etched GaAs Quantum Dots Integrated in Single-Mode Waveguides and Beamsplitters.

Integration of on-demand quantum emitters into photonic integrated circuits (PICs) has drawn much attention in recent years, as it promises a scalable implementation of quantum information schemes. A central property for several applications is the indistinguishability of the emitted photons. In this regard, GaAs quantum dots (QDs) obtained by droplet etching epitaxy show excellent performances, making the realization of these QDs into PICs highly appealing. Here, we show the first implementation in this direction, realizing the key passive elements needed in PICs, i.e., single-mode waveguides (WGs) with integrated GaAs-QDs and beamsplitters. We study the statistical distribution of wavelength, linewidth, and decay time of the excitonic line, as well as the quantum optical properties of individual emitters under resonant excitation. We achieve single-photon purities as high as 1 - g(2)(0) = 0.929 ± 0.009 and two-photon interference visibilities of up to VTPI = 0.953 ± 0.032 for consecutively emitted photons.

Design and simulation of a rectangular planar printed circuit board coil for nuclear magnetic resonance, radio frequency energy harvesting, and wireless power transfer devices

AbstractIn this study, a planar printed circuit board (PCB) coil with FR4 substrate was designed and simulated using the finite element method, and the results were analyzed in the frequency domain. This coil can be used in wireless power transfer (WPT) as a transmitter or receiver, eliminating wires. It can also be used as the receiver in radio frequency energy‐harvesting (RF‐EH) systems by optimizing the planar PCB coil to convert radio‐wave energy into electricity, and it can be employed as an excitation (transmitter) or receiver coil in nuclear magnetic resonance (NMR) spectroscopy. This PCB coil can replace the conventional coil, yielding a reduced occupied volume, a fine‐tuned design, reduced weight, and increased efficiency. Based on the calculated gain, power, and electromagnetic and electric field results, this planar PCB coil can be implemented in WPT, NMR spectroscopy, and RF‐EH devices with minor changes. In applications such as NMR spectroscopy, it can be used as a transceiver planar PCB coil. In this design, at frequencies of 915 MHz and 40 MHz with 5 mm between coils, we received powers of 287.3 W and 480  W, respectively, which are suitable for an NMR coil or RF‐EH system.

Thermal transport and optical anisotropy in CVD grown large area few-layer MoS2 over an FTO substrate

Atomically thin MoS2 is a promising candidate for its integration into devices due to its strikingly unique electronic, optical, and thermal properties. Here, we report the fabrication of a few-layer MoS2 thin film over a conducting fluorine-doped tin oxide-coated glass substrate via a one-step chemical vapor deposition method. We have quantitatively analyzed the nonlinear temperature-dependent Raman shift using a physical model that includes thermal expansion and three- and four-phonon anharmonic effects, which exhibits that the main origin of nonlinearity in both the phonon modes primarily arises from the three-phonon anharmonic process. We have also measured the interfacial thermal conductance (g) and thermal conductivity (ks) of the synthesized film using the optothermal Raman spectroscopy technique. The obtained values of g and ks are ∼7.218 ± 0.023 MW m−2 K−1 and ∼40 ± 2 W m−1 K−1, respectively, suggesting the suitability of thermal dissipation in MoS2 based electronic and optoelectronic devices. Furthermore, we performed a polarization study using the angle resolved polarized Raman spectroscopy technique under non-resonance and resonance excitations to reveal the electron–photon–phonon interaction in the prepared MoS2, based on the semi-classical theory that includes deformation potential and Fröhlich interaction. Our study provides much needed experimental information about thermal conductivity and polarization response in a few-layer MoS2 grown over the conducting substrate, which is relevant for applications in low power thermoelectric and optoelectronic devices.

High-resolution photoelectron spectroscopy of the very weakly bound MgNe molecule

ABSTRACT We report on the characterisation of the X + 2 Σ + ground electronic state of MgNe + by photoionisation, mass-analysed threshold-ionisation (MATI) and pulsed-field-ionisation zero-kinetic-energy photoelectron (PFI-ZEKE-PE) spectroscopy and the observation of the metastable a  3 Π 0 state of MgNe. Rotationally cold MgNe was generated in a laser-ablation supersonic-beam source in both the X 1 Σ + ( v ″ = 0 ) ground state and a 3 Π 0 ( v ″ = 0 ) metastable electronic state. PFI-ZEKE-PE spectra with full resolution of the vibrational structure and partial resolution of the rotational structure were recorded from the X 1 Σ + ground state following resonant ( 1 + 1 ′ ) two-photon excitation via selected rovibrational levels of the C 1 Π intermediate state and from the a  3 Π 0 metastable state following single-photon excitation. The lowest six vibrational levels of the X + 2 Σ + state were observed, covering 80% of the X + 2 Σ + potential-well depth. The experimental data were used to determine potential-energy functions, dissociation energies, and molecular constants for the X 1 Σ + , a 3 Π 0 and C 1 Π states of MgNe and the X + 2 Σ + state of MgNe + . With dissociation energies D 0 of 12(3) cm−1 and 10(3) cm−1, respectively, the X 1 Σ + and a 3 Π 0 states of 24 Mg 20 Ne are extremely weakly bound. In contrast, the X + 2 Σ + state of 24 Mg 20 Ne + has a dissociation energy D 0 of 185(3) cm − 1 and 12 bound vibrational levels. From the difference between the adiabatic ionisation energies of the X 1 Σ + (61 498.5(4) cm − 1 ) and the a 3 Π 0 (39 645.1(3) cm − 1 ) states, the term value of the a 3 Π 0 ground vibrational level is determined to be 21 853.4(5) cm − 1 . These results are compared with those of earlier experimental studies and ab initio quantum-chemical calculations.

Real-time hybrid model test to replicate high-rise building resonant vibration under wind loads

In May 2021, the 72-story Shenzhen Saige building experienced abnormal vibration that was strongly felt on many floors and triggered social panic. The tower was therefore closed for more than 2 months resulting in huge economic losses. A preliminary study consisting of field resonant excitation tests and a series of numerical simulations were carried out. It was concluded that the wind loads provoked the higher modes of the building vibration. Specifically, the vibration of the mast, which is located at the building top, induced this abnormal vibration. To validate this conclusion, real-time hybrid model (RTHM) tests was developed to reproduce this building vibration incident. This paper presents the details of the validation RTHM tests including testing design and result discussions. Structural vibration parameters obtained from the field tests were used in the numerical substructure building model, and the experimental substructures were the two scaled down mast models (the cantilever beam section of the masts). During RTHM test, the restoring force of the experimental substructure due to real wind loads induced by an air fan was measured and used in the numerical simulation to compute interface motions. A shaking table was then used to impose the interface motion back to the bottom of the mast model to reproduce the abnormal vibration incident. The demonstrated ability of the developed RTHM testing method to reproduce the resonant phenomenon of the wind-induced tower vibration provides an alternative experimental method to study vibration responses of high-rise buildings in future.

On the multiphoton ionisation photoelectron spectra of phenol.

The phenol molecule is a prototype for non-adiabatic dynamics and the excited-state photochemistry of biomolecules. In this article, we report a joint theoretical and experimental investigation on the resonance enhanced multiphoton ionisation photoelectron (REMPI) spectra of the two lowest ionisation bands of phenol. The focus is on the theoretical interpretation of the measured spectra using quantum dynamics simulations. These were performed by numerically solving the time-dependent Schrödinger equation using the multi-layer variant of the multiconfiguration time-dependent Hartree algorithm together with a vibronic coupling Hamiltonian model. The ionising laser pulse is modelled explicitly within the ionisation continuum model to simulate experimental femtosecond 1+1 REMPI photoelectron spectra. These measured spectra are sensitive to very short lived electronically excited states, providing a rigorous benchmark for our theoretical methods. The match between experiment and theory allows for an interpretation of the features of the spectra at different wavelengths and shows that there are features due to both 'direct' and 'indirect' ionisation, resulting from non-resonant and resonant excitation by the pump pulse.

New Injection Controls Environment for the Taiwan Light Source

Taiwan Light Source (TLS) has been service for user service since 1993. Several legacy systems have recently been updated in order to remove obsolescent parts and provide higher operating efficiency. Proprietary designed timing modules were recently replaced by an event based timing system. The magnets of the booster synchrotron were configured as three White circuits and driven by resonance excitation. The original control of the White circuits, which included an analogue amplitude loop and digital phase loop for regulation, has been replaced by full digital regulation loops. The successful upgrade of both systems has led to easy and smooth injection control with enhanced functionality and flexibility. The injection control includes foreground and background processes that coordinate the operation of e-gun, linear accelerator, booster synchrotron, and storage ring with the help of timing system. The injection control GUI provides an intuitive operation interface that includes parameter setting and all necessary information displays, such as various timing value, stored beam current/lifetime, injection efficiency, filling pattern, kickers waveform and so on. Energy saving mode of White circuits operation are supported and embedded into injection control to save electricity. Lifetime calculation of the storage ring is also synchronized with the injection process. Implementation details and operation experience will be presented.

X-ray induced ultrafast charge transfer in thiophene-based conjugated polymers controlled by core-hole clock spectroscopy.

We explore ultrafast charge transfer (CT) resonantly induced by hard X-ray radiation in organic thiophene-based polymers at the sulfur K-edge. A combination of core-hole clock spectroscopy with real-time propagation time-dependent density functional theory simulations gives an insight into the electron dynamics underlying the CT process. Our method provides control over CT by a selective excitation of a specific resonance in the sulfur atom with monochromatic X-ray radiation. Our combined experimental and theoretical investigation establishes that the dominant mechanism of CT in polymer powders and films consists of electron delocalisation along the polymer chain occurring on the low-femtosecond time scale.

MXene-antenna electrode with collective multipole resonances.

Two-dimensional transition metal carbides and nitrides (MXene-s) are the focus of extensive research due to their exceptional potential for practical applications. We study nanostructured MXene layers to design photodetector electrodes and increase their response through hot-electron generation. We demonstrate that the lattice arrangement plays a crucial role in exciting strong optical resonances in the nanostructured MXene, specifically Ti3C2Tx, despite its high loss and weak optical resonances in an isolated antenna. We use numerical simulations and analytical calculations with coupled dipole-quadrupole lattice sums for designing photodetector electrodes. We also provide proof-of-concept experimental demonstration of the enhanced resonances even for the case of lossy materials. We report on the excitation of strong lattice resonances of the MXene antenna array with enhanced absorption, resulting in a more efficient generation of hot electrons. Our findings reveal that a multi-period array of MXene antennas can improve narrowband and broadband photodetector functionality. We propose highly efficient absorbers based on MXene metasurfaces and transforming electrodes into hybrid photodetectors using MXene antennas to enhance their performance.

Plasmon-induced hot carrier distribution in a composite nanosystem: role of the adsorption site.

The generation of hot carriers (HCs) through the excitation of localized surface plasmon resonance (LSPR) in metal nanostructures is a fascinating phenomenon that fuels both fundamental and applied research. However, gaining insights into HCs at a microscopic level has posed a complex challenge, limiting our ability to create efficient nanoantennas that utilize these energized carriers. In this investigation, we employ real-time time-dependent density functional theory (rt-TDDFT) calculations to examine the creation and distribution of HCs within a model composite system consisting of a silver (Ag) nanodisk and a carbon monoxide (CO) molecule. We find that the creation and distribution of HCs are notably affected by the CO adsorption site. Particularly, when the CO molecule adsorbs onto the hollow site of the Ag nanodisk, it exhibits the highest potential among various composite systems in terms of structural stability, enhanced orbital hybridization, and HC generation and transfer. Utilizing a Gaussian laser pulse adjusted to match the LSPR frequency, we observe a marked buildup of hot electrons and hot holes on the C and O atoms. Conversely, the region encompassing the C-O bond exhibits a depletion of hot electrons and hot holes. We believe that these findings could have significant implications in the field of HC photocatalysis.

Electrodynamic approach for calculating the absorption spectra of plasmons in a rectangle with a two-dimensional electron gas excited by an incident electromagnetic wave

The purpose of this research is to develop an electrodynamic method for calculating the plasmon spectrum in a three-dimensional structure with a two-dimensional electron gas excited by an incident electromagnetic wave. Methods. The developed method is based on solving integral equations formed with respect to induced currents in the conducting parts of a three-dimensional structure. Results. The convergence of the method and the calculation time were studied. The conditions for the convergence of calculations of higher plasmon resonances in a rectangular structure with a two-dimensional electron gas are determined. The normal incidence of an arbitrarily polarized electromagnetic wave on a rectangle with a two-dimensional gas is studied. The spectra of the absorption, extinction, forward and back scattering cross sections of the incident wave are calculated. Conclusion. It is found that in a rectangular structure containing a two-dimensional electron gas, the spectrum of plasmon resonances is modified in comparison with established by two-dimensional models of problem formulation, in which the structure is assumed to be infinite and homogeneous in one of the directions. It has been established that the incident wave most effectively excites fundamental plasmon modes. Plasmonic modes exhibit strong charge accumulation at the edges of the rectangle, which significantly affects the resonant excitation frequencies of plasmonic modes.

New event based timing system for the Taiwan Light Source

The Taiwan Light Source (TLS) is a third generation synchrotron light source that has been in operation since 1993. However, the legacy timing system is obsolete and needs to be upgraded to an event based timing system. This upgrade is intended to replace obsolete components and improve functionality. The new timing system must coordinate the operation of the linac, the White circuit based booster synchrotron, and the storage ring for beam generation, injection, extraction, and accumulation, while also supporting top up operation of the storage ring. To achieve this, a cPCI (CompactPCI) based EPICS IOC (Input Output Controller) and expandable fanless embedded computers have been adopted for the new TLS timing system, replacing the existing VME-based ILC (Intelligent Local Controller) to provide an easy to maintain control environment. However, the resonant excitation of the booster magnets with the event system requires special attention in the design and implementation phases. This paper summarizes the design ideas and implementation process for addressing this issue.