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Gabriel Nagamine

Publications and source records attributed to Gabriel Nagamine.

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Profiling THz Beams With Off-Label Use of Infrared Microbolometric Cameras

Visualizing the spatial profile of light beams is essential for evaluating irradiance, characterizing beam quality, and achieving precise alignment. In the optical spectral range, this is readily performed using silicon-based CCD and CMOS cameras. In the terahertz (THz) range, however, it typically requires specialized detectors with prohibitive costs. Here, we show that an infrared (IR) camera can be used outside of its labeled specifications to achieve similar performance as a dedicated microbolometric THz camera, at under 1% of the THz camera's cost. We compared the cameras by characterizing THz beam profiles from two sources: a pulsed broadband THz beam produced through optical rectification in organic crystals, and a narrowband quasi-continuous-wave (quasi-CW) THz beam emitted by a quantum cascade laser. For the broadband THz radiation, the beam width measured by the two cameras differed by only ~ 6%, well within the pixel resolution limit, and in the narrowband quasi-CW case by just ~ 1.3%. Additionally, the IR camera exhibits a lower minimum detectable power (down to 1.5 THz) than the THz camera, while also maintaining a linear and polarization-independent responsivity. These results expand the applicability of conventional IR cameras to the THz range, suggesting that they will become routine tools for high-fidelity THz beam diagnostics and imaging in scientific and industrial applications.

physics.optics

Electronic excitations in the Shastry-Sutherland compound SrCu$_2$(BO$_3$)$_2$

SrCu2(BO3)2 (SCBO) is a paradigmatic realization of the Shastry-Sutherland model, hosting geometrically frustrated spin dimers and a variety of quantum magnetic phases and phenomena. Although its magnetic properties have been extensively studied, the high-energy electronic excitations that determine the crystal-field environment and Cu-O hybridization have remained largely unexplored. Here we combine Cu L3-edge resonant inelastic x-ray scattering (RIXS), broadband optical spectroscopy, and electronic-structure calculations to determine the relevant local and interband excitation energy scales in SCBO. RIXS resolves a well-defined manifold of localized Cu2+ d-d excitations between 1.8 and 2.4 eV, whose energies and polarization dependence are well reproduced by multireference quantum-chemistry calculations. In contrast, optical spectroscopy identifies charge-transfer excitations with an absorption onset near 1.2-1.6 eV and a broader higher-energy structure around 4.5 eV, which are qualitatively captured by DFT+U calculations. Taken together, these results define the characteristic energy scales of d-d and CT excitations, offering quantitative benchmarks for computational frameworks and providing essential input for refining superexchange-based magnetic models of this prototypical frustrated quantum antiferromagnet.

cond-mat.str-el

All-optical control of second-harmonic generation in $β$-BaB$_2$O$_4$ via coherent, terahertz-driven acentric lattice displacement

Dynamical control of the nonlinear optical properties of solids -- with light itself -- will be essential for future ultrafast photonic technologies. Previously, methods to modulate nonlinear processes including second-harmonic generation (SHG) have relied primarily on non-resonant light-matter interaction or photo-generation of hot electrons in nanoscale materials. However, these approaches are typically constrained by limited interaction lengths and the initial frequency conversion is relatively weak under equilibrium conditions. Here, an approximately 30\% modulation of efficient phase-matched SHG in bulk beta-barium borate (beta-BaB2O4) is achieved through transient lattice deformation by intense terahertz (THz) pulses that are tuned to resonance with an infrared-active phonon mode. The effect originates from modification of the index of refraction ellipsiod and the corresponding nonlinear phase-matching conditions, rather than from direct modulation of the nonlinear susceptibility through THz-mediated chi^(3) processes. This mechanism, of resonant selective lattice excitation, points toward novel THz-control schemes to tune the nonlinear optical response in materials.

physics.optics

Fourier pixels for reciprocal light control

Digital cameras and displays utilise picture elements (pixels) that perform a single function: detecting or emitting light intensity. To exploit the full information content of electromagnetic waves, more advanced elements are required. This has driven the development of multifunctional components, which for example, simultaneously detect and emit intensity or extract intensity and spectral information. However, no pixel exists that both senses and generates optical wavefronts with full control over amplitude, phase, and polarisation, limiting reciprocal control and feedback of sophisticated light fields. Here we present a route to such pixels by demonstrating a versatile platform of miniaturised diffractive elements based on Fourier optics. We exploit plasmonic surface waves, which propagate coherently and efficiently across metallic surfaces. When these plasmons are launched towards wavy microstructures designed with simple Fourier analysis, arbitrary and background-free optical wavefronts are generated. Conversely, incoming light can be sensed and its amplitude, phase, and polarisation fully characterised. By combining or superposing several such components, we create multifunctional 'Fourier pixels' that provide compact and accurate control over the optical field. Our approach, which could also use photonic waveguide modes, establishes a scalable, universal architecture for vectorially programmable pixels with applications in adaptive optics, holographic displays, optical communication, and quantum-information processing.

physics.optics

Band-Edge Carrier Trapping Limits Light Emission in WSe$_2$

Monolayers of transition metal dichalcogenides (TMDs) exhibit bright photoluminescence, a desirable property for light-emitting diodes and single-photon emitters. Because the emission intensity is heavily influenced by factors such as defect density and oxidation, it is critical to understand how they affect photoluminescence efficiency. However, due to the time-consuming process of identifying individual monolayers, studies of high-quality exfoliated TMDs have been limited to only a few samples. Here, we present an investigation of excited-state lifetimes and spectra for over 200 WSe$_2$ exfoliated monolayers at room temperature. We find a linear correlation between photoluminescence lifetime and intensity across hundreds of monolayers and within individual monolayers. Results from intentional photooxidation experiments indicate that this correlation is due to photoinduced band-edge carrier traps, which introduce a nonradiative decay pathway that competes with exciton emission. Our work highlights the importance of controlling such traps, as they are the primary limitation of bright photoluminescence.

cond-mat.mes-hall

Diffraction of Light from Optical Fourier Surfaces

Diffractive surfaces shape optical wavefronts for applications in spectroscopy, high-speed communication, and imaging. The performance of these structures is primarily determined by how precisely they can be patterned. Fabrication constraints commonly lead to square-shaped, "binary" profiles that contain unwanted spatial frequencies that contaminate the diffraction. Recently, "wavy" surfaces (known as optical Fourier surfaces, OFSs) have been introduced that include only the desired spatial frequencies. However, the optical performance and reliability of these structures have not yet been experimentally tested with respect to models and simulations. Such a quantitative investigation could also provide previously unobtainable information about the diffraction process from the most fundamental diffractive surfaces$\unicode{x2014}$sinusoidally pure profiles. Here, we produce and study two classes of reflective OFSs: (i) single-sinusoidal profiles of varying depth and (ii) double-sinusoidal profiles with varying relative phase. After refining our fabrication procedure to obtain larger and deeper OFSs at higher yields, we find that the measured optical responses from our OFSs agree quantitatively with full electrodynamic simulations. In contrast, our measurements diverge from analytical scalar diffraction models routinely used by researchers to describe diffraction. Overall, our results confirm that OFSs provide a precise and powerful platform for Fourier-spectrum engineering, satisfying the growing demand for intricately patterned interfaces for applications in holography, augmented reality, and optical computing.

physics.optics

Spectroscopy of Single CdSe Magic-Sized Nanocrystals

Chemical syntheses that provide nanocrystals (NCs) with narrow distributions in size and shape are critical for NC research. This has led to the investigation of magic-sized NCs (MSNCs), a class of semiconductor crystallites that grow in discrete steps, potentially offering a single size and shape (i.e., monodispersity). However, the photoluminescence (PL) spectra of CdSe MSNCs measured at room temperature have been reported to be broader than those of state-of-the-art quantum dots. This difference could be due to the smaller size of MSNCs, which broadens their line widths, or due to their residual size dispersity. To better understand the optical performance of MSNCs, here we perform single-particle spectroscopy. Our results show that, while CdSe MSNCs do exhibit particle-to-particle variations that lead to modest broadening of their ensemble emission spectra, the largest contribution comes from the single-particle line width. By examining MSNCs with different sizes and shells, we conclude that this single-particle broadening is consistent with exciton coupling to acoustic phonons from the NC surface. Because of their small size, this coupling and the role of residual size dispersity have a larger impact on the ensemble emission line widths. Notably, when small (<2.7 nm diameter) MSNCs and quantum dots are compared, the ensemble PL line widths of MSNCs are actually sharper. Due to their small size, MSNCs also exhibit strong anti-bunching $[g^{(2)}(0) \sim 0.05]$ at room temperature. Thus, MSNCs represent a bright, spectrally pure class of quantum emitter, useful for applications in optoelectronic and quantum-information technologies where strong three-dimensional confinement is required.

cond-mat.mes-hall

High-Throughput Identification and Statistical Analysis of Atomically Thin Semiconductors

Transition metal dichalcogenides (TMDs) are layered two-dimensional semiconductors explored for various optoelectronic applications, ranging from light-emitting diodes to single-photon emitters. To interact strongly with light, such devices require monolayer TMDs, which exhibit a direct bandgap. These atomically thin sheets are typically obtained through mechanical exfoliation followed by manual identification with a brightfield optical microscope. While this traditional procedure provides high-quality crystals, the identification step is time-intensive, low-throughput, and prone to human error, creating a significant bottleneck for TMD research. Here, we report a simple and fully automated approach for high-throughput identification of TMD monolayers using photoluminescence microscopy. Compared to a manual search and verification, our methodology offers a four-orders-of-magnitude decrease in the time a researcher must invest per identified monolayer. This ability enables us to measure geometric and photoluminescence-intensity features of more than 2,400 monolayers and bilayers of WSe$_2$, MoSe$_2$, and MoS$_2$. Due to these large numbers, we can study and quantify material properties previously inaccessible. For example, we show that the mean photoluminescence intensity from a monolayer correlates with its size due to reduced emission from its edges. Further, we observe large variations in brightness (up to 10$\times$) from WSe$_2$ monolayers of different batches produced by the same supplier. Therefore, our automated approach not only increases fabrication efficiency but also enhances sample quality for optoelectronic devices of atomically thin semiconductors.

cond-mat.mes-hall

Towards Engineering Intrinsic Linewidths and Line-Broadening in Perovskite Nanoplatelets

Perovskite nanoplatelets possess extremely narrow absorption and emission linewidths, which are crucial characteristics for many optical applications. However, their underlying intrinsic and extrinsic line-broadening mechanisms are poorly understood. Here, we apply multi-dimensional coherent spectroscopy to determine the homogeneous line-broadening of colloidal perovskite nanoplatelet ensembles. We demonstrate control of not only their intrinsic linewidths, but also control of various broadening mechanisms by tuning the platelet geometry. Remarkably, we find that decreasing nanoplatelet thickness by a single polyhedral layer results in a 2-fold reduction of the inhomogeneous linewidth and a 3-fold reduction of the intrinsic homogeneous linewidth to the sub-meV regime. In addition, our measurements suggest homogeneously broadened exciton resonances in 3-layer (but not necessarily 4-layer) nanoplatelets at room-temperature.

physics.optics

Partially-Bright Triplet Excitons in Perovskite Nanocrystals

Advances in opto-electronics require the development of materials with novel and engineered characteristics. A class of materials that has garnered tremendous interest is metal-halide perovskites, stimulated by meteoric increases in photovoltaic efficiencies of perovskite solar cells. In addition, recent advances have applied perovskite nanocrystals (NCs) in light-emitting devices. It was discovered recently that, for cesium lead-halide perovskite NCs, their unusually efficient light-emission may be due to a unique excitonic fine-structure composed of three bright triplet states that minimally interact with a proximal dark singlet state. To study this fine-structure without isolating single NCs, we use multi-dimensional coherent spectroscopy at cryogenic temperatures to reveal coherences involving triplet states of a CsPbI$_3$ NC ensemble. Picosecond timescale dephasing times are measured for both triplet and inter-triplet coherences, from which we infer a unique exciton fine-structure level-ordering comprised of a dark state energetically positioned within the bright triplet manifold.

cond-mat.mtrl-sci

Effect of Dimensionality on the Optical Absorption Properties of CsPbI$_3$ Perovskite Nanocrystals

The band-gaps of CsPbI$_3$ perovskite nanocrystals are measured by absorption spectroscopy at cryogenic temperatures. Anomalous band-gap shifts are observed in CsPbI$_3$ nanocubes and nanoplatelets, which are modeled accurately by band-gap renormalization due to lattice vibrational modes. We find that decreasing dimensionality of the CsPbI$_3$ lattice in nanoplatelets greatly reduces electron-phonon coupling, and dominant out-of-plane quantum confinement results in a homogeneously broadened absorption lineshape down to cryogenic temperatures. An absorption tail forms at low-temperatures in CsPbI$_3$ nanocubes, which we attribute to shallow defect states positioned near the valence band-edge.

physics.app-ph