arXiv subjects

Minoru Fujii

Publications and source records attributed to Minoru Fujii.

15 recordsLinked to original sources

arXiv2026

Revealing time characteristics of optical excitations in dielectric and plasmonic structures through cathodoluminescence interferometry

Cathodoluminescence (CL) spectroscopy provides access to optical excitations with nanometer spatial resolution, but direct time-resolved measurements of optical resonances remain challenging. Here, we demonstrate that CL interferometry provides access to the temporal response, phase behavior, and modal spectral structure of resonant nanoscale scatterers without requiring ultrafast pump-probe schemes. We develop an analytical framework in which Fourier transformation angle- and frequency-resolved CL interferograms yields the decay time of optical resonances governed by the linear optical response. Multimode resonators exhibit characteristic temporal CL beating signatures associated with spectral mode splitting. By exploiting transition radiation emitted from a nearby metallic surface as a broadband reference, we further demonstrate phase retrieval and cross-correlation measurements between instantaneous and resonant emission processes. Experimental measurements on Au nanoparticles, broadband plasmonic emitters, Au nanostars, and Si nanospheres supporting multipolar Mie resonances confirm the theoretical predictions, and decay times in the range 1-10 fs are derived for each system. Our results establish CL interferometry as a powerful approach for accessing spectral, spatial, and phase information within a single nanoscale measurement with fs resolution.

cond-mat.mes-hall↗

arXiv2026

Probe- and Substrate-Dependent Visibility of Mie Resonances in Silicon Nanospheres

Silicon nanospheres are high-quality optical resonators and promising building blocks for Mie-tronic devices. While the Mie resonances of an isolated sphere are well understood, practical implementations require substrates that inevitably modify the measured optical response. Here, we investigate how substrates alter the observable spectrum of individual nanospheres, focusing on three fundamentally different cases: a thin silicon nitride membrane, that emulates a free-standing particle, bulk silicon, which is common in experiments, and gold, where mirror charges lead to hybrid optical modes. Cathodoluminescence and dark-field spectroscopy, combined with electrodynamic simulations, show that the measured resonances are not intrinsic to the particle but depend strongly on the environment and the excitation mechanism. We find that substrate-induced effects and probe-specific selection rules can suppress, enhance, or even invert the spectral signatures of electric and magnetic modes. These results provide practical guidelines for interpreting and designing substrate-supported dielectric resonators for Mie-tronic applications.

physics.optics↗

arXiv2025

Color Routing and Beam Steering of Single-Molecule Emission with a Spherical Silicon Nanoantenna

Single-photon emitters radiate as electric dipoles, which limits light collection efficiency and complicates integration into flat photonic devices. Developing nanophotonic structures capable of directing photon emission with tunable angular distributions in the visible spectrum has been pursued for applications ranging from integrated optical systems to discrimination of molecular species. To date, such directional control has been achieved using components whose overall footprint is larger than the emission wavelength and often rely on lossy plasmonic components. Here, we employ the DNA origami technique for deterministic nanoscale assembly, positioning single fluorophores in nanometric proximity to a single silicon spherical nanoparticle and demonstrate unidirectional emission with forward-to-backward intensity ratios up to ~7 dB. Furthermore, we show that a single silicon nanosphere antenna can function as a color router or a beam steerer depending on its size, emitter spectral range and emitter-nanoparticle distance.

physics.optics↗

arXiv2025

Polymer-Shell Coating of Mie-Resonant Silicon Nanospheres for Controlled Fabrication of Self-Assembled Monolayer

A polymer shell offers a unique opportunity to tailor structural and optical properties of optically functional nanoparticles and their ensembles. Here, we develop a process to coat Mie-resonant silicon nanospheres (Si NSs) with a thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) hydrogel shell. We show formation of a PNIPAM shell of controlled thickness from the change of the hydrodynamic diameter and study the effect of thermoresponsive shrinkage and expansion of the shell on the Mie resonance of a Si NS. We then demonstrate that Si NSs with PNIPAM shells enable fabrication of cluster-free, self-assembled monolayers of Si NSs, in which distances between NSs are controlled by the PNIPAM shell thickness.

cond-mat.mtrl-sci↗

arXiv2025

Distance dependent interaction between a single emitter and a single dielectric nanoparticle using DNA origami

Optical nanoantennas can manipulate light-matter interactions at the nanoscale, modifying the emission properties of nearby single photon emitters. To date, most optical antennas are based on metallic nanostructures that exhibit unmatched performance in terms of electric field enhancement but suffer from substantial ohmic losses that limit their applications. To circumvent these limitations, there is a growing interest in alternative materials. In particular, high-refractive-index dielectrics have emerged as promising candidates, offering negligible ohmic losses, and supporting both electric and magnetic resonances in the visible and near-infrared range that can unlock novel effects. Currently, the few available studies on dielectric nanoantennas focus on ensemble measurements. Here, we exploit the DNA origami technique to study the interaction between silicon nanoparticles and organic fluorophores at the single molecule level, in controlled geometries and at different spectral ranges within the visible spectrum. We characterize their distance-dependent interaction in terms of fluorescence intensity and lifetime, revealing a significant modification of the decay rate together with minimal quenching and a high fluorescence quantum yield even at short distances from the dielectric nanoparticle. This work demonstrates the advantages of dielectric nanoantennas over their metallic counterparts and paves the way for their applications in single-molecule spectroscopy and sensing.

physics.optics↗

arXiv2024

Routing Light Emission from Monolayer MoS$_2$ by Mie Resonances of Crystalline Silicon Nanospheres

A dielectric Mie-resonant nanoantenna is capable of controlling the directionality of the emission from nearby quantum emitters through the excitation of multiple degenerate Mie resonances. A crystalline silicon nanosphere (Si NS) is a promising candidate for a dielectric nanoantenna because crystalline Si has a large refractive index (3.8 at 650 nm) and the small imaginary part of a complex refractive index (0.015 at 650 nm) as an optical material. In this work, we control the emission directionality of excitons supported by monolayer transition metal dichalcogenides (1L-TMDCs) using a Si NS. We first discuss the condition to extract the emission preferentially towards the Si NS side from the analytical calculations. We then study the photoluminescence (PL) of 1L-TMDCs on which differently sized single Si NSs are placed. We show that the PL spectral shape strongly depends on the emission direction, and that the emission toward the Si NS side (top) with respect to the opposite side (bottom) is the largest at wavelengths between the magnetic dipole and electric dipole Mie resonances of a Si NS. Finally, we quantitatively discuss the spectral shape of the top-to-bottom ratio from numerical simulations.

physics.optics↗

arXiv2023

Universal click-chemistry approach for the DNA functionalization of nanoparticles

Nanotechnology has revolutionized the fabrication of hybrid species with tailored functionalities. A milestone in this field is the DNA conjugation of nanoparticles, introduced almost 30 years ago, which typically exploits the affinity between thiol groups and metallic surfaces. Over the last decades, developments in colloidal research have enabled the synthesis of an assortment of non-metallic structures, such as high-index dielectric nanoparticles, with unique properties not previously accessible with traditional metallic nanoparticles. However, to stabilize, integrate and provide further functionality to non-metallic nanoparticles, reliable techniques for their functionalization with DNA will be crucial. Here, we combine well-established dibenzylcyclooctyne-azide click-chemistry with a simple freeze-thaw method to achieve the functionalization of silica and silicon nanoparticles, which form exceptionally stable colloids with a high DNA surface density of 0.2 molecules/nm2. Furthermore, we demonstrate that these functionalized colloids can be self-assembled into high-index dielectric optical antennas with a yield of up to 78% via the use of DNA origami. Finally, we extend this method to functionalize other important nanomaterials, including oxides, polymers, core-shell and metal nanostructures. Our results indicate that the method presented herein serves as a crucial complement to conventional thiol functionalization chemistry and thus greatly expands the toolbox of DNA-functionalized nanoparticles currently available.

physics.chem-ph↗

arXiv2021

Ultraviolet Mie resonances in computationally discovered boron phosphide nanoparticles

Controlling ultraviolet light at the nanoscale using optical Mie resonances holds great promise for a diverse set of applications, such as lithography, sterilization, and biospectroscopy. However, Mie resonances hosted by dielectric nanoantennas are difficult to realize at ultraviolet wavelengths due to the lack of both suitable materials and fabrication methods. Here, we systematically search for improved materials by computing the frequency dependent optical permittivity of 338 binary semiconductors and insulators from first principles, and evaluate their potential performance as high refractive index materials using Mie theory. Our analysis reveals several interesting candidate materials among which boron phosphide (BP) appears particularly promising. We then prepare BP nanoparticles and demonstrate that they support Mie resonances at visible and ultraviolet wavelengths using both far-field optical measurements and near-field electron energy-loss spectroscopy. We also present a laser reshaping method to realize spherical Mie-resonant BP nanoparticles. With a refractive index above 3 and low absorption losses, BP nanostructures advance Mie optics to the ultraviolet.

physics.optics↗

arXiv2021

Disentangling cathodoluminescence spectra in nanophotonics: particle eigenmodes vs transition radiation

Cathodoluminescence spectroscopy performed in an electron microscope has proven a versatile tool for analysing the near- and far-field optical response of plasmonic and dielectric nanostructures. Nevertheless, the transition radiation produced by electron impact is often disregarded in the interpretation of the spectra recorded from resonant nanoparticles. Here we show, experimentally and theoretically, that transition radiation can by itself generate distinct resonances which, depending on the time of flight of the electron beam inside the particle, can result from constructive or destructive interference in time. Superimposed on the eigenmodes of the investigated structures, these resonances can distort the recorded spectrum and lead to potentially erroneous assignment of modal characters to the spectral features. We develop an intuitive analogy that helps distinguish between the two contributions. As an example, we focus on the case of silicon nanospheres, and show that our analysis facilitates the unambiguous interpretation of experimental measurements on Mie-resonant nanoparticles.

cond-mat.mes-hall↗

arXiv2021

Optical Spin Sorting Chain

Transverse spin angular momentum of light is a key concept in recent nanophotonics to realize unidirectional light transport in waveguides by spin-momentum locking. Herein we theoretically propose subwavelength nanoparticle chain waveguides that efficiently sort optical spins with engineerable spin density distributions. By arranging high-refractive-index nanospheres of different sizes in a zigzag manner, directional optical spin propagation is realized. The origin of the efficient spin transport is revealed by analyzing the dispersion relation and spin angular momentum density distributions. In contrast to conventional waveguides, the proposed asymmetric waveguide can spatially separate up- and down-spins and locate one parity inside and the other outside the structure. Moreover, robustness against bending the waveguide and its application as an optical spin sorter are presented. Compared to previous reports on spatial engineering of local spins in photonic crystal waveguides, we achieved substantial miniaturization of the entire footprint down to subwavelength scale.

physics.optics↗

arXiv2020

MENP: An Open-Source MATLAB Implementation of Multipole Expansion for Applications in Nanophotonics

In modern nanophotonics, multipolar interference plays an indispensable role to realize novel optical devices represented by metasurfaces with unprecedented functionalities. Not only to engineer sub-wavelength structures that constitute such devices but also to realize and interpret unnatural phenomena in nanophotonics, a program that efficiently carries out multipole expansion is highly demanded. MENP is a MATLAB program for computation of multipole contributions to light scattering from current density distributions induced in nanophotonic resonators. The main purpose of MENP is to carry out post-processing of a rigid multipole expansion for full-field simulations which in principle provide the information of all near- and far-field interactions (e.g. as a total scattering cross section). MENP decomposes total scattering cross sections into partial ones due to electric and magnetic dipoles and higher-order terms based on recently developed exact multipole expansion formulas. We validate the program by comparing results for ideal and realistic nanospheres with those obtained with the Mie theory. We also demonstrate the potential of MENP for analysis of anapole states by calculating the multipole expansion under the long-wavelength approximation which enables us to introduce toroidal dipole moments.

physics.optics↗

arXiv2016

Phenomenological theory of optical broadening in zero-dimensional systems applied to silicon nanocrystals

We develop a phenomenological theory of inhomogeneous broadening in zero-dimensional systems and apply it to study photoluminescence (PL) spectra of silicon nanocrystals measured at helium and room temperatures. The proposed approach allowed us to explain experimentally observed PL peak asymmetry, linear dependence of the peak width on its maximum and anomalous alteration of spectral characteristics with temperature increase.

cond-mat.mes-hall↗

arXiv2012

Ultra-broad near-infrared photoluminescence from crystalline (K-crypt)2Bi2 containing [Bi2]2- dimers

For the first time, we report that a single crystal of (K-crypt)2Bi2 containing [Bi2]2+ displays ultra-broad near-infrared photoluminescence (PL) peaking at around 1190 nm and having a full width at the half maximum of 212 nm, stemming from the inherent electronic transitions of [Bi2]2+.The results not only add to the number of charged Bi species with luminescence, but also deepen the understanding of Bi-related near-infrared emission behavior and lead to the reconsideration of the fundamentally important issue of Bi-related PL mechanisms in some material systems such as bulk glasses, fibers, and conventional optical crystals.

cond-mat.mtrl-sci↗

arXiv2012

Photoluminescence from Bi5(GaCl4)3 molecular crystal

Bi5(GaCl4)3 sample has been synthesized through the oxidation of Bi metal by gallium chloride (GaCl3) salt. Powder X-ray diffraction as well as micro-Raman scattering results revealed that, in addition to crystalline Bi5(GaCl4)3 in the product, amorphous phase containing [GaCl4]- and [Ga2Cl7]- units also exist. The thorough comparison of steady-state and time-resolved photoluminescent behaviors between Bi5(GaCl4)3 product and Bi5(AlCl4)3 crystal leads us to conclude that Bi53+ is the dominant emitter in the product, which gives rise to the ultrabroad emission ranging from 1 to 2.7 micrometer. Detailed quantum chemistry calculation helps us assign the observed excitations to some electronic transitions of Bi53+ polycation, especially at shorter wavelengths. It is believed that our work shown here not only is helpful to solve the confusions on the luminescent origin of bismuth in other material systems, but also serves to develop novel broadband tunable laser materials.

cond-mat.mtrl-sci↗

arXiv2012

Near-infrared photoluminescence from molecular crystals containing tellurium

We report the observation of near-infrared photoluminescence from Te4(Ga2Cl7)2 and Te4(Al2Cl7)2 molecular crystals containing Te42+ polycations. The experimental and theoretical results clearly revealed that Te42+ polycation is one smart near-infrared emitter with characteristic emission peaks at 1252 and 1258 nm for Te4(Ga2Cl7)2 and Te4(Al2Cl7)2 crystals, respectively, resulting from the intrinsic electronic transitions of Te42+. Furthermore, it was also found that the emissions strongly depend on the excitation wavelengths for both Te4(Ga2Cl7)2 and Te4(Al2Cl7)2 samples, most possibly owing to the co-existence of other Te-related optically active centers. This research not only enriches the species of luminescent charged p-block element polyhedra and deepens the understanding of Te-related photophysical behaviors, but also may stimulate efforts for designing novel material systems using such active centers. It is also greatly expected that these sub-nanometer optically active species could exist in other systems such as glasses, polymers, and bulk optical crystals, and the stabilization of these centers in widely used hosts will pave the way for their practical applications.

cond-mat.mtrl-sci↗