arXiv subjects

Søren Raza

Publications and source records attributed to Søren Raza.

At least 19 recordsLinked to original sources

arXiv2026

Enriching molecular Raman spectroscopy with vibrational strong coupling

Raman spectroscopy is widely used for molecular identification in biological samples, but spectral congestion often obscures key molecular fingerprints. Strategies to enrich vibrational spectra with additional controllable features are therefore desirable. We theoretically show that vibrational strong coupling (VSC) can reshape Raman spectra by reorganizing vibrational energies and intensities. Near-resonant coupling enables the resolution of quasi-degenerate vibrational modes and redistributes Raman activity among molecular vibrations, brightening otherwise Raman-inactive modes. Off-resonant coupling mediates effective interactions between vibrations, leading to tunable intensity reorganizations and spectral shifts via cavity-controlled vibrational mixing. Using a microscopic theory of Raman scattering, we show that observing Raman signals from collective VSC polaritons requires appropriate geometries for the scattering setup, the sample, and the cavity environment, helping to explain why polaritonic Raman signatures have remained challenging to observe experimentally.

physics.chem-ph↗

arXiv2026

A sulfonitride transparent conductive thin film with ultra-high refractive index

With the rise of AI-assisted materials screening, extraordinary properties are now frequently predicted in experimentally uncharted material systems, highlighting the need to develop new synthesis methods for unconventional materials beyond the classic bulk powder form. Here, we establish the first thin-film growth route for any metal sulfonitride compound by realizing Zr2SN2 films with a rare and compelling combination of optical and electrical properties. Zr2SN2 is transparent across most of the visible range while exhibiting a very high average refractive index of 2.95 in the visible, exceeding expectations based on conventional refractive index-bandgap scaling. Importantly, the same Zr2SN2 film shows degenerate n-type conductivity with carrier density above 10^20 cm-3 and intragrain mobility above 8 cm2V-1s-1, approaching those of established transparent conductive oxides. Zr2SN2 thus demonstrates that strong light-matter interaction, optical transparency and electrical conductivity can be reconciled within a single material platform, revealing a new class of high-refractive-index transparent conductors.

cond-mat.mtrl-sci↗

arXiv2026

Large-scale Integration of Experimental and Computational Data for 2D Materials

The past decade has seen rapid growth in the number of experimentally realized two-dimensional (2D) materials with diverse chemical and physical properties. However, information on their crystal structure, synthesis routes, and measured or predicted properties, remains scattered across thousands of publications. Here we consolidate this fragmented knowledge by establishing X2DB - an open infrastructure that integrates experimental and computational data on 2D materials. Using extensive literature mining and direct community uploads, we identify 370 unique 2D materials that have been realized in monolayer or few-layer form, and link them to their digital counterparts in computational databases, enabling consistent ab initio characterization of their properties across monolayer, bilayer and bulk forms. We describe the structure and content of the database highlighting its support for community uploads, illustrate how it can be used to generate new scientific insight and introduce a hierarchical classification of the known set of 2D materials. Our work provides a foundation for the integration and cross-fertilization of experimental and theoretical knowledge, opening new avenues for data-driven, predictive synthesis of novel 2D materials.

cond-mat.mtrl-sci↗

arXiv2026

Breaking the Moss rule

Photonic devices depend critically on the dielectric materials from which they are made, with higher refractive indices and lower absorption losses enabling new functionalities and higher performance. However, these two material properties are intrinsically linked through the empirical Moss rule, which states that the refractive index of a dielectric decreases as its band gap energy increases. Materials that surpass this rule, termed super-Mossian dielectrics, combine large refractive indices with wide optical transparency and are therefore ideal candidates for advanced photonic applications. This Review surveys the expanding landscape of high-index dielectric and semiconductor materials, with a particular focus on those that surpass the Moss rule. We discuss how electronic band structures with a large joint density of states near the band edge give rise to super-Mossian behavior and how first-principles computational screening can accelerate their discovery. Finally, we establish how the refractive index sets the performance limits of nanoresonators, waveguides, and metasurfaces, highlighting super-Mossian dielectrics as a promising route toward the next performance leap in photonic technologies.

physics.optics↗

arXiv2025

Enhanced and directional light emission from two-dimensional excitons using Mie voids

Controlling light emission at the nanoscale has important applications in solid-state lighting, displays, and quantum light sources. Achieving this control requires both enhanced local electromagnetic fields to boost emission intensity and engineered radiation patterns to direct photons efficiently. Mie voids, consisting of an air cavity surrounded by a high-index semiconductor, are particularly suited for this purpose because they expose their strongest fields in an accessible region for nearby emitters while supporting resonances that shape directional emission through interference. Here, we demonstrate an all-van der Waals nanophotonic platform that couples excitons in atomically thin WS$_2$ to Mie void resonators formed in WSe$_2$. Guided by electromagnetic simulations, we identify void geometries that maximize photoluminescence through synergistic enhancement of excitation and emission processes. We also develop a two-step fabrication strategy that enables independent control of void diameter and depth, providing a route to systematically tune the optical response. Experimentally, we observe up to a 600-fold increase in photoluminescence intensity from monolayer WS$_2$ placed on individual voids compared to on an unstructured WSe$_2$, along with pronounced out-of-plane beaming of light that yields a forward-to-off-axis enhancement of 2.6 dB. Our results establish Mie voids in van der Waals semiconductors as a new platform for controlling light-matter interactions and realizing compact, directional, and efficient nanoscale light sources.

physics.optics↗

arXiv2025

Reflectivity-based refractive index measurement of van der Waals materials

We present a reflectivity-based method for measuring the in-plane refractive index of transparent van der Waals (vdW) materials. The approach enables the characterization of as small as $3 \times 3$~{\textmu}m$^2$ exfoliated flakes on a non-transmissive substrate without assuming any specific spectral shape of the refractive index. Exfoliated flakes are most commonly obtained through mechanical exfoliation, which generally produces vdW flakes with tens-of-micron lateral dimensions. As a result, conventional ellipsometry - which depends on large, uniform areas and specific spectral models - becomes challenging to apply. Our method determines the refractive index directly from the spectral position of reflectivity minima, provided the flake thickness and the substrate complex refractive index are known. We demonstrate the technique on hafnium disulfide (HfS$_2$), a vdW semiconductor with high refractive index and low absorption, retrieving its in-plane refractive index across the visible range. The results both validate previous ellipsometry measurements and establish this method as an accessible and spectral-model-free alternative for refractive index characterization of vdW materials.

physics.optics↗

arXiv2025

Apparent Resonance Splitting in Self-Coupled Excitonic Systems

Thin films of high-refractive-index excitonic materials enable self-coupling by simultaneously supporting intrinsic excitonic transitions and optical resonances. These optical resonances take the form of Fabry-Perot resonances in thick films and absorption resonances in ultrathin films placed on metallic substrates. Here, we investigate whether these optical resonances lead to true exciton-photon hybridization. Using far-field reflectance and spectrally resolved photocurrent measurements, we study tungsten disulfide (WS$_2$) flakes on both metallic and dielectric substrates across a range of thicknesses. While reflectance spectra for ultrathin flakes exhibit resonance splitting between excitons and absorption resonances, our photocurrent measurements reveal only excitonic peaks, indicating that no polaritons are formed. In contrast, thicker flakes exhibit Fabry-Perot resonances that strongly couple to excitons, resulting in clear splitting in both reflectance and photocurrent spectra, and providing evidence of polariton formation. We further show that the polariton resonances can be tuned through the reflection phase at the WS$_2$-substrate interface by changing the substrate material. In addition to coupling with the strong A-exciton, we observe polariton formation involving the weaker B-exciton at shorter wavelengths, as well as higher-order hybridization where both excitons interact simultaneously with a single Fabry-Perot resonance. These findings clarify the distinction between apparent and true strong coupling in excitonic materials and demonstrate how reflection phase and flake thickness can be used to engineer light-matter interactions.

physics.optics↗

arXiv2025

Experimental demonstration of a beam shaping non-imaging metasurface

Light emitting diodes have superior performance over most other light sources, but the need for secondary optics to shape their illumination for specific applications yield bulky lighting products. Here, we present an approach to shaping light from incoherent sources, such as light emitting diodes, using non-imaging metasurfaces. We present a theoretical framework and a numerical tool for designing the metasurface phase, and use it to construct a proof-of-principle beam shaping metasurface. We demonstrate the optical performance of the fabricated sample, and perform numerical experiments to investigate the quality of the metasurface design. Our approach bridges the fields of non-imaging optics and metaoptics, and may enable metasurface applications for shaping coherent and incoherent light.

physics.optics↗

arXiv2025

Computational discovery of high-refractive-index van der Waals materials: The case of HfS$_2$

New high-refractive-index dielectric materials may enhance many optical technologies by enabling efficient manipulation of light in waveguides, metasurfaces, and nanoscale resonators. Van der Waals materials are particularly promising due to their excitonic response and strong in-plane polarizability. Here we combine ab initio calculations and experiments to discover new high-refractive-index materials. Our screening highlights both known and new promising optical materials, including hafnium disulfide (HfS$_2$), which shows an in-plane refractive index above 3 and large anisotropy in the visible range. We confirm these theoretical predictions through ellipsometry measurements and investigate the photonic potential of HfS$_2$ by fabricating nanodisk resonators, observing optical Mie resonances in the visible spectrum. Over the course of seven days, we observe a structural change in HfS$_2$, which we show can be mitigated by storage in either argon-rich or humidity-reduced environments. This work provides a comparative overview of high-index van der Waals materials and showcases the potential of HfS$_2$ for photonic applications in the visible spectrum.

physics.optics↗

arXiv2025

Fourier-Tailored Light-Matter Coupling in van der Waals Heterostructures

Dielectric structures can support low-absorption optical modes, which are attractive for engineering light-matter interactions with excitonic resonances in two-dimensional (2D) materials. However, the coupling strength is often limited by the electromagnetic field being confined inside the dielectric, reducing spatial overlap with the active excitonic material. Here, we demonstrate a scheme for enhanced light-matter coupling by embedding excitonic tungsten disulfide (WS$_2$) within dielectric hexagonal boron nitride (hBN), forming a van der Waals (vdW) heterostructure that optimizes the field overlap and alignment between excitons and optical waveguide modes. To tailor diffractive coupling between free-space light and the waveguide modes in the vdW heterostructure, we fabricate Fourier surfaces in the top hBN layer using thermal scanning-probe lithography and etching, producing sinusoidal topographic landscapes with nanometer precision. We observe the formation of exciton-polaritons with a Rabi splitting indicating that the system is at the onset of strong coupling. These results demonstrate the potential of Fourier-tailored vdW heterostructures for exploring advanced optoelectronic and quantum devices.

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↗

arXiv2024

Quantitative mapping of smooth topographic landscapes produced by thermal scanning-probe lithography

Scanning probe microscopy (SPM) is a powerful technique for mapping nanoscale surface properties through tip-sample interactions. Thermal scanning-probe lithography (tSPL) is an advanced SPM variant that uses a silicon tip on a heated cantilever to sculpt and measure polymer films with nanometer precision. The surfaces produced by tSPL-smooth topographic landscapes-allow mathematically defined contours to be fabricated on the nanoscale, enabling sophisticated functionalities for photonic, electronic, chemical, and biological technologies. Evaluating the physical effects of a landscape requires fitting arbitrary mathematical functions to SPM datasets, however, this capability does not exist in standard analysis programs. Here, we provide an open-source software package (FunFit) to fit analytical functions to SPM data and develop a fabrication and characterization protocol based on this analysis. We demonstrate the benefit of this approach by patterning periodic and quasiperiodic landscapes in a polymer resist with tSPL, which we transfer to hexagonal boron nitride (hBN) flakes with high fidelity via reactive-ion etching. The topographic landscapes in polymers and hBN are measured with tSPL and atomic force microscopy (AFM), respectively. Within the FunFit program, the datasets are corrected for artefacts, fit with analytical functions, and compared, providing critical feedback on the fabrication procedure. Beyond application to tSPL, this protocol can improve analysis, reproducibility, and process development for a broad range of SPM experiments. The protocol can be performed within a working day by an inexperienced user, where fabrication and characterization take a few hours and software analysis takes a few minutes.

cond-mat.mes-hall↗

arXiv2024

Encapsulated void resonators in lossy dielectric van der Waals heterostructures

Dielectric optical resonators traditionally rely on materials with the combination of high refractive indices and low optical losses. Such materials are scarce for operation in visible spectrum and shorter wavelengths. This limitation can be circumvented by relaxing the requirement of low losses. We demonstrate that highly lossy dielectric materials can be structured to support optical resonances that confine light in air voids. We theoretically design void resonances in the visible spectrum and identify resonant modes supported by void arrays. Experimentally, we fabricate void arrays in tungsten diselenide and characterize the confined resonances using far-field reflectance measurements and scanning near-field optical microscopy. Using van der Waals heterostructure assembly, we encapsulate the voids with hexagonal boron nitride which reduces the void volume causing a large spectral blue shift of the void resonance exceeding 150 nm. Our work demonstrates a versatile optical platform for lossy materials, expanding the range of suitable materials and the spectral range of photonic devices.

physics.optics↗

arXiv2024

Quality factor of dielectric optical resonators

We show analytically that the quality ($Q$) factor of magnetic and electric Mie modes in a lossless dielectric spherical resonator with high refractive index ($n \gg 1$) scales as $n^{2j+1}$ and $n^{2j+3}$ respectively, where $j$ denotes the multipolar order. We numerically validate these results and show that our high-$n$ analytical relation is accurate for the dipolar modes when $n>5$. For higher multipolar orders, the analytical relation becomes valid for increasingly lower $n$. We study the dependence of the $Q$ factor on absorption losses and determine a general functional form that describes the $Q$ factor for all Mie modes for any complex refractive index. Finally, we observe that this functional form predicts a multipolar-dependent singular value of optical gain which gives rise to a lasing condition with an infinite $Q$ factor.

physics.optics↗

arXiv2023

Non-imaging metasurface design for collimated beam shaping

Non-imaging optical lenses can shape the light intensity from incoherent sources to a desired target intensity profile, which is important for applications in lighting, solar light concentration, and optical beam shaping. Their surface curvatures are designed to ensure optimal transfer of energy from the light source to the target. The performance of such lenses is directly linked to their asymmetric freeform surface curvature, which is challenging to manufacture. Metasurfaces can mimic any surface curvature without additional fabrication difficulty by imparting a spatially-dependent phase delay using optical antennas. As a result, metasurfaces are uniquely suited to realize non-imaging optics, but non-imaging design principles have not yet been established for metasurfaces. Here, we take an important step in connecting non-imaging optics and metasurface optics, by presenting a phase-design method for beam shaping based on the concept of optimal transport. We establish a theoretical framework that enables a collimated beam to be redistributed by a metasurface to a desired output intensity profile. The optimal transport formulation leads to metasurface phase profiles that transmit all energy from the incident beam to the output beam, resulting in an efficient beam shaping process. Through a variety of examples, we show that our approach accommodates a diverse range of different input and output intensity profiles. Last but not least, a full field simulation of a metasurface has been done to verify our phase-design framework.

physics.optics↗

arXiv2022

Nanoscale engineering of optical strong coupling inside metals

Optical polaritons appear when a material excitation strongly couples to the optical mode. Such strong coupling between molecular transitions and optical cavities results in far-reaching opportunities in modifying fundamental properties of chemical matter. More recently an exciting prospect of cavity-free polaritons has emerged by matter sustaining the optical mode with its geometry. Here we show how strong coupling of the interband transition and surface plasmons can be engineered in nickel at the nanoscale to realize cavity-free optical polaritons inside metals. Using electron energy-loss spectroscopy, we demonstrate that in thin films and nanoantennas the propagation and radiation losses result in a broadening of the plasmon linewidth and a transition from strong to weak coupling. Further, higher-order plasmon resonances couple to the interband transition, and the multipolar coupled states acquire the field profile of the plasmon. Our results provide a fundamental understanding of plasmon-interband coupling in metals and establish the base for the design of unforeseen photocatalytic and magneto-optical nanosystems.

physics.optics↗

arXiv2022

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

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↗