arXiv subjects

Adam Alfrey

Publications and source records attributed to Adam Alfrey.

11 recordsLinked to original sources

arXiv2026

Inhomogeneous saturation of excitons in monolayer transition-metal dichalcogenides

We observe that the apparent inhomogeneous broadening, as measured by two-dimensional coherent spectroscopy (2DCS), of the exciton resonance in transition-metal dichalcogenide monolayers depends on the excitation strength. A key strength of 2DCS is the ability to separate inhomogeneous broadening, which primarily contributes to the diagonal linewidth, from homogeneous broadening, which dominates the cross-diagonal linewidth. We show that the fluence dependence of the diagonal linewidth arises from the effective saturation fluence varying with the exciton's resonance energy, i.e., inhomogeneous saturation. These results are critical for interpreting the exciton linewidths, which are often used as a measure of sample quality.

cond-mat.mes-hall↗

arXiv2026

Separation of Homogeneous and Inhomogeneous Broadening using Two-Dimensional Coherent Spectroscopy

Separating the contributions of homogeneous dephasing from inhomogeneous broadening in spectral linewidths is essential for connecting optical spectra to microscopic dissipation and disorder mechanisms. Voigt fits to one-dimensional spectra, such as photoluminescence, yield strongly correlated Gaussian and Lorentzian widths, so that neither width can be determined independently with confidence. We quantitatively show that two-dimensional coherent spectroscopy (2DCS) reduces this degeneracy by providing orthogonal spectral slices, diagonal and cross-diagonal, with complementary sensitivity to homogeneous and inhomogeneous broadening processes. As a demonstration, we measure the exciton resonance in hBN-encapsulated MoSe$_2$ at 8 K. A joint uncertainty-weighted fit maps the full $\chi^2(\sigma,\gamma)$ landscape to quantify parameter covariance. Compared with linear Voigt analysis, 2DCS yields more compact confidence regions and markedly reduced parameter correlation, enabling reliable separation of the contributions to the excitonic linewidth.

physics.optics↗

arXiv2026

Revealing Strain and Disorder in Transition-Metal Dichalcogenides Using Hyperspectral Photoluminescence Imaging

Hyperspectral photoluminescence (HSPL) imaging provides spatially resolved spectral information for monolayer transition-metal dichalcogenides (TMDs), enabling the detection of subtle variations in excitonic features that are not accessible with conventional optical or photoluminescence intensity imaging. We employ HSPL to map the microscopic spatial distribution of strain and disorder in hBN-encapsulated MoSe$_2$ and WSe$_2$ samples. Quantitative extraction of exciton, trion, and biexciton energies and linewidths reveals strain gradients and localized deformations, such as wrinkles and ripples. The technique allows for characterization of regions with uniform optical properties and identification of areas affected by micro-scale disorder, which may be missed by optical microscopy. Measurements on samples with different device architectures and fabrication processes demonstrate the general utility of hyperspectral PL imaging for assessing spatial heterogeneity and optoelectronic quality in two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2025

Magneto-Moir\'e Excitons in Twisted Bilayer CrSBr

Moir\'e superlattices in van der Waals materials have revolutionized the study of electronic and excitonic systems by creating periodic electrostatic potentials. Extending this concept to magnetic materials promises new pathways in merging spintronics with photonics. While moir\'e magnetism has been revealed with near-field probes and nonlinear optical techniques, the coupling of these magnetic textures to optical excitations - magneto-moir\'e excitons - remains unexplored. Here, we report the observation of magneto-moir\'e excitons in twisted bilayer CrSBr, correlated with moir\'e spin textures that emerge below a critical twist angle of ~2{\deg}. The nanoscale moir\'e spin texture imprints distinct signatures onto the optical spectrum, shifting the exciton energy via a periodic magnetic exchange field. First-principles calculations corroborate that these signatures arise from one-dimensional spin textures governed by the balance of exchange interactions and domain wall energy. Our results demonstrate that moir\'e magnetism can be used to engineer nanoscale excitonic energy landscapes, providing a new platform for magneto-optical sensing, quantum transduction, and control of non-collinear magnetism and topology through light.

cond-mat.mes-hall↗

arXiv2025

Twist Engineering of Anisotropic Excitonic and Optical Properties of a Two-Dimensional Magnetic Semiconductor

Two dimensional (2D) van der Waals (vdW) magnetic semiconductors are a new class of quantum materials for studying the emergent physics of excitons and spins in the 2D limit. Twist engineering provides a powerful tool to manipulate the fundamental properties of 2D vdW materials. Here, we show that twist engineering of the anisotropic ferromagnetic monolayer semiconductor, CrSBr, leads to bilayer magnetic semiconductors with continuously tunable magnetic moment, dielectric anisotropy, exciton energy and linear dichroism. We furthermore provide a model for exciton energy in the media with tunable anisotropy. These results advance fundamental studies on 2D vdW materials and open doors to applications to nano-optics, twistronics, and spintronics.

cond-mat.mes-hall↗

arXiv2024

Large Exciton Binding Energy in the Bulk van der Waals Magnet CrSBr

Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid state systems. Excitons and their associated many-body physics are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving their stability are still relatively unexplored. Here, we report an exceptionally large exciton binding energy in single crystals of the bulk van der Waals antiferromagnet CrSBr. Utilizing state-of-the-art angle-resolved photoemission spectroscopy and self-consistent ab-initio GW calculations, we present direct spectroscopic evidence that robust electronic and structural anisotropy can significantly amplify the exciton binding energy within bulk crystals. Furthermore, the application of a vertical electric field enables broad tunability of the optical and electronic properties. Our results indicate that CrSBr is a promising material for the study of the role of anisotropy in strongly interacting bulk systems and for the development of exciton-based optoelectronics.

cond-mat.mtrl-sci↗

arXiv2023

Magnetic Exciton-Polariton with Strongly Coupled Atomic and Photonic Anisotropies

Anisotropy plays a key role in science and engineering. However, the interplay between the material and engineered photonic anisotropies has hardly been explored due to the vastly different length scales. Here we demonstrate a matter-light hybrid system, exciton-polaritons in a 2D antiferromagnet, CrSBr, coupled with an anisotropic photonic crystal (PC) cavity, where the spin, atomic lattice, and photonic lattices anisotropies are strongly correlated, giving rise to unusual properties of the hybrid system and new possibilities of tuning. We show exceptionally strong coupling between engineered anisotropic optical modes and anisotropic excitons in CrSBr, which is stable against excitation densities a few orders of magnitude higher than polaritons in isotropic materials. Moreover, the polaritons feature a highly anisotropic polarization tunable by tens of degrees by controlling the matter-light coupling via, for instance, spatial alignment between the material and photonic lattices, magnetic field, temperature, cavity detuning and cavity quality-factors. The demonstrated system provides a prototype where atomic- and photonic-scale orders strongly couple, opening opportunities of photonic engineering of quantum materials and novel photonic devices, such as compact, on-chip polarized light source and polariton laser.

physics.optics↗

arXiv2022

Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides

Transition metal dichalcogenides (TMDs) are regarded as a possible materials platform for quantum information science and related device applications. In TMD monolayers, the dephasing time and inhomogeneity are crucial parameters for any quantum information application. In TMD heterostructures, coupling strength and interlayer exciton lifetimes are also parameters of interest. However, many demonstrations in TMDs can only be realized at specific spots on the sample, presenting a challenge to the scalability of these applications. Here, using multi-dimensional coherent imaging spectroscopy (MDCIS), we shed light on the underlying physics - including dephasing, inhomogeneity, and strain - for a MoSe$_2$ monolayer and identify both promising and unfavorable areas for quantum information applications. We furthermore apply the same technique to a MoSe$_2$/WSe$_2$ heterostructure. Despite the notable presence of strain and dielectric environment changes, coherent and incoherent coupling, as well as interlayer exciton lifetimes are mostly robust across the sample. This uniformity is despite a significantly inhomogeneous interlayer exciton photoluminescence distribution that suggests a bad sample for device applications. This robustness strengthens the case for TMDs as a next-generation materials platform in quantum information science and beyond.

cond-mat.mtrl-sci↗

arXiv2021

Nanoscale trapping of interlayer excitons in a 2D semiconductor heterostructure

For quantum technologies based on single excitons and spins, the deterministic placement and control of a single exciton is a long-standing goal. MoSe2-WSe2 heterostructures host spatially indirect interlayer excitons (IXs) which exhibit highly tunable energies and unique spin-valley physics, making them promising candidates for quantum information processing. Previous IX trapping approaches involving moir\'e superlattices and nanopillars do not meet the quantum technology requirements of deterministic placement and energy tunability. Here, we use a nanopatterned graphene gate to create a sharply varying electric field in close proximity to a MoSe2-WSe2 heterostructure. The dipole interaction between the IX and the electric field creates an ~20 nm trap. The trapped IXs show the predicted electric field dependent energy, saturation at low excitation power, and increased lifetime, all signatures of strong spatial confinement. The demonstrated architecture is a crucial step towards deterministic trapping of single IXs, which has broad applications to scalable quantum technologies.

cond-mat.mes-hall↗

arXiv2020

Temperature dependent moir\'e trapping of interlayer excitons in MoSe2-WSe2 heterostructures

MoSe2-WSe2 heterostructures host strongly bound interlayer excitons (IXs) which exhibit bright photoluminescence (PL) when the twist-angle is near 0{\deg} or 60{\deg}. Over the past several years, there have been numerous reports on the optical response of these heterostructures but no unifying model to understand the dynamics of IXs and their temperature dependence. Here, we perform a comprehensive study of the temperature, excitation power, and time-dependent PL of IXs. We observe a significant decrease in PL intensity above a transition temperature that we attribute to a transition from localized to delocalized IXs. Astoundingly, we find a simple inverse relationship between the IX PL energy and the transition temperature, which exhibits opposite power dependent behaviors for near 0{\deg} and 60{\deg} samples. We conclude that this temperature dependence is a result of IX-IX exchange interactions, whose effect is suppressed by the moir\'e potential trapping IXs at low temperature.

physics.optics↗

arXiv2019

2D Semiconductor Nonlinear Plasmonic Modulators

A plasmonic modulator is a device that controls the amplitude or phase of propagating plasmons. In a pure plasmonic modulator, the presence or absence of a pump plasmonic wave controls the amplitude of a probe plasmonic wave through a channel. This control has to be mediated by an interaction between disparate plasmonic waves, typically requiring the integration of a nonlinear material. In this work, we demonstrate the first 2D semiconductor nonlinear plasmonic modulator based on a WSe2 monolayer integrated on top of a lithographically defined metallic waveguide. We utilize the strong coupling between the surface plasmon polaritons, SPPs, and excitons in the WSe2 to give a 73 percent change in transmission through the device. We demonstrate control of the propagating SPPs using both optical and SPP pumps, realizing the first demonstration of a 2D semiconductor nonlinear plasmonic modulator, with a modulation depth of 4.1 percent, and an ultralow switching energy estimated to be 40 aJ.

physics.app-ph↗