arXiv subjects

Takumi Sannomiya

Publications and source records attributed to Takumi Sannomiya.

At least 19 recordsLinked to original sources

arXiv2026

Cathodoluminescence Wavefront Retrieval

Free-electron-based nanoscopy enables the study of optical excitations in materials with deep-subwavelength spatial resolution, with cathodoluminescence (CL) being one of the most useful resulting signals. When combined with an optical collection system, CL measurements can access multidimensional information of light; yet the phase of the emitted optical fields has remained largely elusive. Here, we demonstrate a reference-free phase retrieval approach for far-field CL wavefronts using the Gerchberg-Saxton algorithm implemented with real-space and angular-space CL intensity data. Applying this approach to representative nanostructures, including a planar surface, nanosphere, plasmonic crystal, and nanowire, we reconstruct distinct phase distributions that reveal their underlying radiation mechanisms. This reference-free framework offers a robust and flexible route for retrieving the phase of electron-beam-excited optical fields without relying on a reference wave, making it readily extendable to a wide range of nanostructures.

physics.optics↗

arXiv2026

Multi-Angle Beam Scanning Transmission Electron Microscopy for Diffraction-Contrast-Free Magnetic Imaging

Recent development of the differential phase contrast (DPC) scanning transmission electron microscopy (STEM) technique has significantly advanced materials science supported by high-sensitivity detectors and powerful data processing. Especially the 4D-STEM technique, employing a pixelated camera as a STEM detector, enables extensive information acquisition through post-processing of large datasets. However, magnetic or electric field imaging using DPC is often disturbed by diffraction contrasts intrinsic to the crystalline material. In this paper, we demonstrate elimination of the diffraction contrasts for magnetic field imaging by using angularly distributed multiple electron beams generated by a multi-hole aperture within the 4D-STEM framework. This multi-angle beam configuration suppresses irrelevant crystalline contrast and yields direct magnetic information with high sensitivity from the specimen. Furthermore, we performed various image analysis to extract and interpret magnetic domain structures and domain walls.

physics.ins-det↗

arXiv2026

Electron-Photon Spatial Entanglement in Coherent Cathodoluminescence

Electron--photon quantum entanglement in an electron microscope paves the way for a new quantum platform, enabling the integration of quantum functionalities into electron microscopy and opening opportunities for quantum imaging and quantum sensing at the nanoscale. To realize such a platform, it is crucial to understand the degree and nature of electron--photon entanglement in cathodoluminescence (CL). However, its dependence on electron-beam properties, particularly transverse coherence, remains unclear. Here, we present a theoretical framework describing the quantum state of an electron--photon pair generated in coherent CL from a system with translational invariance in the plane perpendicular to the electron beam, as can be realized, for example, in transition radiation at a planar interface. By expressing the scattered state directly in terms of the luminescence spectrum, we evaluate the entanglement using both subsystem purity and an Einstein--Podolsky--Rosen-type criterion. These two measures enable a clear distinction among wave-like, particle-like, and classical regimes in terms of spatial and momentum entanglement in the electron--photon system. Our analysis identifies the roles of the electron's transverse and longitudinal coherence, as well as the photon's spectral width, and reveals the conditions under which strong spatial entanglement emerges. This unified perspective clarifies the nature of electron--photon quantum correlations in coherent CL and advances the development of quantum-enabled functionalities in electron microscopy.

quant-ph↗

arXiv2026

Drift Correction of Scan Images by Snapshot Referencing

Reliable quantitative analysis in scanning (transmission) electron microscopy (S(T)EM) is often hindered by image drift during long-duration spectral mapping for elemental analysis or for various material functions. We here present snapshot-referencing (SSR) drift correction, a retrospective approach to eliminate spatial distortion based on the temporal nature of the scanning process. A continuous drift vector for every pixel is calculated for a normalized time-field of the scan pattern (e.g., serpentine or raster) utilizing a high-signal, fast-scan "snapshot" as a drift-free reference to guide the correction of simultaneously acquired analytical maps. To describe the drift, we employed Bezier basis functions to model smooth thermal or mechanical drifts and piece-wise linear basis for high-frequency "spiky" shifts such as those caused by charging. We demonstrate the efficacy of this approach on experimental cathodoluminescence (CL) datasets, showing that it effectively restores spatial integrity to hyperspectral data cubes without the need for specialized hardware. This flexible, software-based solution is broadly applicable to any probe-based analytical technique where a fast imaging signal can be recorded alongside slow spectroscopic data.

physics.ins-det↗

arXiv2026

Modulation of Spin Angular Momentum of Emission in Symmetric 1D Plasmonic Crystals by Cathodoluminescence

The spin angular momentum (SAM) of light has become a cornerstone of numerous photonic applications, including optical communication and chiral photonics. Because SAM is inherently associated with circularly polarized light (CPL), the ability to modulate CPL in a controlled and efficient manner is essential not only for advancing fundamental studies of light-matter interactions but also for enabling next-generation photonic technologies. However, such modulation is commonly realized by structurally chiral systems, which inherently limits the feasibility of dynamic tuning. Here, we demonstrate that one-dimensional plasmonic crystals (1D PlCs), despite their structural symmetry, can serve as a platform for controllable CPL generation. By employing an electron beam in scanning transmission electron microscopy (STEM), we coherently excite transition radiation and emission from 1D PlC modes. Their interference produces energy- and momentum- (emission angle-) resolved CPL, which clearly reveals its dispersion and spatial dependence at the nanoscale, providing direct guidance for its manipulation and offering insights into the design of plasmonic devices including the phase information. Furthermore, interference with surface plasmon polariton scattering at the structural boundary enables the efficiency modulation of CPL generation via the excitation position along the terrace.

physics.optics↗

arXiv2026

Room Temperature Collective Blinking and Photon Bunching from CsPbBr3 Quantum Dot Superlattice

Development of quantum light sources and search for quantum systems capable of supporting collective many-body states are crucial for further progress of modern quantum technologies. Metal halide perovskite quantum dots (QDs) have emerged as a promising candidate for quantum light sources, as individual QDs are reliable single photon emitters even at room temperature. However, photon bunching, a key signature of collective many-body states, has been so far largely observed at cryogenic temperatures in perovskite materials, limiting their applications under ambient conditions. Here, we report the observation of collective blinking and photon bunching in perovskite QD superlattices at room temperature. Sub-wavelength-sized (100 - 500 nm) CsPbBr3 QD superlattices, fabricated via a self-assembly process, exhibit an unusual two-level blinking behavior similar to that of single QDs, and demonstrate photon bunching with a degree of up to 2.75. Time-resolved photoluminescence (PL) measurements and super-resolution imaging reveal that the superlattices have a significantly longer PL lifetime than individual QDs and that their emission is spatially confined to regions tens of nanometers in size. These observations suggest long-range exciton migration to a localized energy trap within the superlattice. Excitation power dependent degree of bunching and analysis of the bunching dynamics indicate that the photon bunching originates from exciton-biexciton cascade emission, a key mechanism for generating entangled photons. These findings establish perovskite QD superlattices as a promising platform for room-temperature collective optical phenomena and quantum light generation, advancing scalable quantum photonic technologies.

physics.optics↗

arXiv2026

Electron Recoil via Sample Momentum Transfer under Optical-Mode Excitation

The interaction between free electrons and optical modes underlies a variety of quantum and nanoscale light-matter phenomena, yet the associated momentum exchange with the sample largely remained overlooked. Here, we experimentally demonstrate the momentum transfer from free electrons to planar samples during optical mode excitation using momentum-resolved electron energy-loss spectroscopy. The momentum transfer to the sample modifies the apparent dispersion relation which is significant when the planner sample is tilted. Under specific conditions, the sample receives momentum opposite to the electron beam direction.

physics.optics↗

arXiv2026

Compressive multi-beam scanning transmission electron microscopy

We demonstrate a multi-beam scanning transmission electron microscopy (STEM) imaging that integrates down-sampling with super-resolution image reconstruction via a compressive sensing framework. A custom condenser aperture with six randomly positioned circular holes is employed to produce a multi-beam STEM probe, with the beam shape and distribution tuned through defocus. While the raw multi-beam images exhibit overlapping patterns, reconstruction using Adam optimization and total variation normalization yields high-fidelity images that closely reproduce the original sample structures, even from substantially down-sampled data. The proposed approach offers a pathway toward significant acceleration of such techniques through multibeam sparse sampling and computational reconstruction potentially useful for the analytical scanning methods in general.

physics.ins-det↗

arXiv2025

Nano light-source generation by electron beam irradiation of CsPbBr3/Cs4PbBr6 composites

Precise allocation of nano light-sources in photonic integrated circuits is essential for the development of next-generation optical technologies such as optical nano-circuits, quantum information processing, and quantum communication. However, controlling the position of such light sources is a challenging task. We here show that halide perovskite nanoparticle light sources can be generated at the desired positions by electron beam. We applied cathodoluminescence spectroscopy to CsPbBr3/Cs4PbBr6 composite produced by thermal evaporation and discovered that the intensity of green light emission from the CsPbBr3 nanoparticles increased with electron beam irradiation. Changes in the cathodoluminescence spectrum associated with the electron beam irradiation suggest CsPbBr3 nanoparticle formations. Furthermore, by taking advantage of the high spatial resolution and controllability of the electron beam, we demonstrate nano-light source patterning on the film.

physics.optics↗

arXiv2025

Roadmap for Quantum Nanophotonics with Free Electrons

Over the past century, continuous advancements in electron microscopy have enabled the synthesis, control, and characterization of high-quality free-electron beams. These probes carry an evanescent electromagnetic field that can drive localized excitations and provide high-resolution information on material structures and their optical responses, currently reaching the sub-ångström and few-meV regime. Moreover, combining free electrons with pulsed light sources in ultrafast electron microscopy adds temporal resolution in the sub-femtosecond range while offering enhanced control of the electron wave function. Beyond their exceptional capabilities for time-resolved spectromicroscopy, free electrons are emerging as powerful tools in quantum nanophotonics, on par with photons in their ability to carry and transfer quantum information, create entanglement within and with a specimen, and reveal previously inaccessible details on nanoscale quantum phenomena. This Roadmap outlines the current state of this rapidly evolving field, highlights key challenges and opportunities, and discusses future directions through a collection of topical sections prepared by leading experts.

cond-mat.mes-hall↗

arXiv2025

Unveiling the nature of cathodoluminescence from photon statistics

Cathodoluminescence (CL), the emission of light induced by accelerated free electrons, has been extensively utilized in various applications, such as displays, streak cameras, and high-spatial-resolution analysis of optical material, surpassing the diffraction limit of light. Despite its long history, the photon statistics of CL have only recently been examined, revealing unexpectedly large bunching of photons. Here we find that this peculiar photon bunching contains information of intervening excitation processes before the photon emission, which can be extracted from the photon statistics within each excitation event by a single free electron. Using this approach, we experimentally unveiled the statistical differences of coherent CL involving a single electromagnetic interaction process and incoherent CL involving multiple excitation processes. The developed formulation is universally applicable for particle generation processes in general to investigate the nature of cascade reactions.

physics.optics↗

arXiv2024

Semicircular-aperture illumination scanning transmission electron microscopy

Scanning transmission electron microscopy (STEM) provides high-resolution visualization of atomic structures as well as various functional imaging modes utilizing phase contrast. In this study we introduce a semicircular aperture in STEM bright field imaging, which gives a phase contrast transfer function that becomes complex and includes both lower and higher spatial frequency contrast transfer. This approach offers significant advantages over conventional phase plate methods, having no charge accumulation, degradation, or unwanted background noise, which are all problematic in the phase plate material. Also compared to the differential phase contrast or ptychography equipment, this semicircular aperture is far less costly. We apply this approach to visualization of polymer, biological and magnetic samples.

physics.optics↗

arXiv2023

Controllable chiral light generation and vortex field investigation using plasmonic holes revealed by cathodoluminescence

Control of the angular momentum of light is a key technology for next-generation nano-optical devices and optical communications, including quantum communication and encoding. We propose an approach to controllably generate circularly polarized light from a circular hole in a metal film using an electron beam by coherently exciting transition radiation and light scattering from the hole through surface plasmon polaritons. The circularly polarized light generation is confirmed by fully polarimetric four-dimensional cathodoluminescence mapping where angle-resolved spectra are simultaneously obtained. The obtained intensity and Stokes maps show clear interference fringes as well as almost fully circularly polarized light generation with controllable parities by electron beam position. By applying this approach to a metal film with three holes, a vortex field with a phase singularity is visualized in the middle of the holes.

physics.optics↗

arXiv2023

Time-correlated electron and photon counting microscopy

Electron microscopy based on high-energy electrons allows nanoscopic analytical imaging taking advantage of secondarily generated particles. Especially for cathodoluminescence, the correlation between primary incident electrons and emitted photons includes information on the entire interaction process. However, electron-photon time correlation tracking the relaxation dynamics of luminescent materials has so far not been achieved. In this work, we propose time-correlated electron and photon counting microscopy, where coincidence events of primary electrons and generated photons are counted after interaction. The electron-photon time correlation enables extracting a unique lifetime of the emitter independent of the photon state, accounting for coherent and incoherent photon generation processes. We also introduce a correlation factor and discuss the correlation between electrons and generated coherent photons. Through momentum selection, we observe correlation changes indicating the presence of pair correlation originated from the electron-photon entanglement. The present work lays the foundation for developing next-generation electron microscopy based on quantum correlation.

physics.ins-det↗

arXiv2023

Superbunching in cathodoluminescence: a master equation approach

We propose a theoretical model of a master equation for cathodoluminescence (CL). The master equation describes simultaneous excitation of multiple emitters by an incoming electron and radiative decay of individual emitters. We investigate the normalized second-order correlation function, $g^{(2)}(τ)$, of this model. We derive the exact formula for the zero-time delay correlation, $g^{(2)}(0)$, and show that the model successfully describes giant bunching (superbunching) in the CL. We also derive an approximate form of $g^{(2)}(τ)$, which is valid for small excitation rate. Furthermore, we discuss the state of the radiation field of the CL. We reveal that the superbunching results from a mixture of an excited photon state and the vacuum state and that this type of state is realized in the CL.

cond-mat.mes-hall↗

arXiv2022

Simultaneous nanoscale excitation and emission mapping by cathodoluminescence

Free-electron-based spectroscopies can reveal the nanoscale optical properties of semiconductor materials and nanophotonic devices with a spatial resolution far beyond the diffraction limit of light. However, the retrieved spatial information is constrained to the excitation space defined by the electron beam position, while information on the delocalization associated with the spatial extension of the probed optical modes in the specimen has so far been missing, despite its relevance in ruling the optical properties of nanostructures. In this study, we demonstrate a cathodoluminescence method that can access both excitation and emission spaces at the nanoscale, illustrating the power of such simultaneous excitation and emission mapping technique by revealing a sub-wavelength emission position modulation as well as by visualizing electromagnetic energy transport in nanoplasmonic systems. Besides the fundamental interest of these results, our technique grants us access into previously inaccessible nanoscale optical properties.

physics.optics↗

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↗

arXiv2021

Chiral Light Emission from a Sphere Revealed by Nanoscale Relative Phase Mapping

Circularly polarized light (CPL) is currently receiving much attention as a key ingredient for next-generation information technologies, such as quantum communication and encryption. CPL photon generation for such applications is commonly realized by coupling achiral optical quantum emitters to chiral nanoantennas. Here, we explore a different strategy consisting in exciting a nanosphere -- the ultimate symmetric structure -- to produce all-directional CPL emission. Specifically, we demonstrate chiral emission from a silicon nanosphere induced by an electron beam based on two different strategies: dissolving the degeneracy of orthogonal dipole modes, and interference of electric and magnetic modes. We prove these concepts by visualizing the phase and polarization using a newly developed polarimetric four-dimensional cathodoluminescence method. Besides their fundamental interest, our results support the use of free-electron-induced light emission from spherically symmetric systems as a versatile platform for the generation of chiral light with on-demand control over the phase and degree of polarization.

physics.optics↗