arXiv subjects

Matthew C. Beard

Publications and source records attributed to Matthew C. Beard.

11 recordsLinked to original sources

arXiv2026

Morphology control and low-temperature magnetotransport in chiral 2D perovskite R-(MBA)$_2$PbI$_4$

Two-dimensional chiral hybrid perovskites, such as R/S-(MBA)\textsubscript{2}PbI\textsubscript{4}, are leading candidates for realizing and studying chirality-dependent charge and spin transport. However, their prohibitive in-plane resistance has precluded the electrical characterization. Here, we overcome this bottleneck by engineering the thin-film morphology of the chiral perovskite $R\text{-(MBA)}_2\text{PbI}_4$, enabling the first robust lateral device integration. In Hall-bar geometries, we demonstrate Hall measurements under dark conditions, unambiguously identifying p-type conduction with a Hall mobility of $\sim 0.2 \text{cm}^2 \text{V}^{-1} \text{s}^{-1}$ and a carrier density of $\sim 3\times10^{14} \text{ cm}^{-2}$, parameters previously inaccessible in this class of materials. Furthermore, we observe enhanced magnetoresistance along transport paths crossing grain boundaries, highlighting the strong influence of morphology on in-plane transport. This work demonstrates in-plane magnetotransport, enabling future investigations of the fundamental mechanisms of chirality-induced spin selectivity (CISS) and accelerating the integration of chiral materials into functional spintronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Chirality-induced magnetoresistance in hybrid organic-inorganic perovskite semiconductors

The combination of semiconducting properties and synthetically tunable chirality in chiral metal halide semiconductors (CMHS) offer a compelling platform for room temperature control over electronic spin properties, leveraging effects such as chirality-induced spin selectivity (CISS) for the development of new opto-spintronic functionalities. We report room-temperature CISS-induced magnetoresistance (CISS-MR) exceeding 100% for spin valves in a configuration consisting of a ferromagnet (FM), tunneling barrier, and CMHS. The high CISS-MR is attributed to interfacial spin-selective tunneling barrier induced by the chirality, which can produce current dissymmetry factors that surpass the limit imposed by the Julli\`ere model governed by the intrinsic spin polarization of the adjacent FM contact. The CISS-MR exhibits a strong dependence on the CMHS composition, revealing a structure-property relationship between CISS and structural chirality. The observed exceptionally large tunneling MR response differentiates from a subtle anisotropic MR arising from the proximity effect at the FM/CMHS interface in the absence of a tunneling barrier. Our study provides insights into charge-to-spin interconversion in chiral semiconductors, offering materials design principles to control and enhance CISS response and utilize it in functional platforms.

cond-mat.mtrl-sci↗

arXiv2025

Equilibrium Spin Polarization Arising From Chirality

Chirality-induced spin selectivity (CISS) describes how chiral molecules and materials generate spin polarization even at thermal equilibrium. This observation has challenged established principles of microscopic reversibility and Onsager reciprocity. We resolve this paradox by formulating a pseudo-Hermitian quantum framework in which structural chirality and electron correlations are sufficient to produce CISS observables. Chirality enters through a non-local metric that couples spin and spatial motion, leading to real spectra, unitary evolution, and thermodynamic consistency. The framework predicts a chirality-induced spin magnetic ordering characterized by a spin--displacement order $\langle σ\cdot x \rangle$, which reconciles equilibrium spin polarization with detailed balance and explains the persistence of CISS in materials composed of light elements. We also derive generalized Onsager-Casimir relations that respect the observed parity ($\mathcal{P}$) and time-reversal ($\mathcal{T}$) breaking, while preserving combined $\mathcal{PT}$-symmetry. This approach establishes a coherent foundation for equilibrium CISS and provides a route to link chemical chirality with measurable spin-to-charge conversion effects.

cond-mat.str-el↗

arXiv2025

Non-Hermitian Exchange as the Origin of Chirality-Induced Spin Selectivity

For over two decades, the role of structural chirality in spin polarization has been widely investigated, with implications for the origins of life, catalysis, and quantum phenomena. Yet, it remains unclear whether all chirality-induced spin selectivity (CISS) effects arise from a common mechanism. We show that breaking all mirror symmetries in structurally chiral electron systems enforces a twin-pair electron exchange, inherently violating both parity P and time-reversal T symmetry while preserving combined PT-symmetry of the Hamiltonian. This exchange produces chiral quantum states where electron spin and motion are intrinsically linked, a key feature of CISS. At interfaces, these states drive spin and charge accumulation via spin-momentum locking. Our findings establish a new paradigm connecting quantum statistics, non-Hermitian physics, and spin transport with structural chirality. This framework unifies all observed CISS effects and provides guiding principles for designing chiral materials for spintronic and quantum applications.

cond-mat.mes-hall↗

arXiv2024

Optical activity of chiral excitons

Recent activity in the area of chiroptical phenomena has been focused on the connection between structural asymmetry, electron spin configuration and light matter interactions in chiral semiconductors. In these systems, spin-splitting phenomena emerge due to inversion symmetry breaking and the presence of extended electronic states, yet the connection to chiroptical phenomena is lacking. Here, we develop an analytical effective mass model of chiral excitons, parameterized by density functional theory. The model accounts for parity mixing of the band edge Bloch functions resulting from polar distortions, resulting in magnetic dipole allowed transitions. Through the study of a prototypical chiral 2D hybrid perovskite semiconductor, we show that circular dichroism of the chiral exciton and its interband continuum emerges from spin-splitting via cross coupling of Rashba-like and chiral/helical spin-texture components. As a counterpoint, we apply our model to describe chiroptical properties of excitons in perovskite nanocrystals that occur without chiral lattice distortions.

cond-mat.mes-hall↗

arXiv2024

Hot Carrier Dynamics in Operational Metal Halide Perovskite Solar Cells

One of the main approaches to inhibit carrier cooling in semiconductor systems enabling the study of hot carrier solar cell protocols is the use of concentrated illumination to obtain high power densities and create a phonon bottleneck. This, however, typically also increases the lattice temperature of the solar cells significantly. Accordingly, the solar cells subject to high concentration illumination also need to withstand high operating temperatures. Having previously demonstrated the high temperature tolerance of the triple halide perovskite (FA0.8Cs0.2Pb1.02I2.4Br0.6Cl0.02) solar cells, here the hot carrier relaxation dynamics are studied in these devices using high power transient absorption (TA) measurements. In addition to monitoring TA spectra obtained at different time delays, the thermalization mechanisms of hot carriers is mapped with power dependent TA to extract the carrier cooling time in this system under in-operando conditions at various bias conditions that reflect the Jsc, Vmax and Voc of these structures, and subsequently deconvolve the underlying physics of carrier relaxation; as well as track the dynamics of the thermalization close to working conditions of the solar cells. These measurements uncover a complex interaction of hot carrier thermalization involving the temporal carrier density, transport, and extraction, and apparent non-equivalent contributions with respect to non-equilibrium photogenerated electrons and holes in these metal halide perovskite solar cell architectures.

cond-mat.mtrl-sci↗

arXiv2024

High-temperature observation of intralayer, interlayer, and Rydberg excitons in bulk van der Waals alloy single crystals

Transition metal dichalcogenides (TMDs) exhibit remarkable optical properties due to the diverse number of strongly bound excitons, which can be fine-tuned by alloying. Despite a flurry of research activity in characterizing these excitons, a comprehensive and profound understanding of their behavior with temperature is lacking. Here, we report the rich spectrum of excitonic features within bulk van der Waals alloy Mo$_{0.5}$W$_{0.5}$S$_2$ and Mo$_{0.5}$W$_{0.5}$Se$_2$ single crystals through temperature-dependent reflectance spectroscopy and first-principle calculations. We observed Rydberg excitons and interlayer excitons in both the single crystals. Notably, we provide the first experimental evidence of highly energetic A$^\prime$ and B$^\prime$ excitons in Mo$_{0.5}$W$_{0.5}$S$_2$ at room temperature. The strong carrier-phonon scattering significantly broadens the A$^\prime$, B$^\prime$ and interlayer excitons at room temperature in bulk Mo$_{0.5}$W$_{0.5}$S$_2$ single crystal compared to its selenide. Our findings, supported by density functional theory and Bethe-Salpeter equation calculations, signify the crucial role of carrier-phonon interactions. These results open pathways for next-generation optoelectronic devices and quantum technologies operating at high temperature.

cond-mat.mtrl-sci↗

arXiv2023

Roadmap on Perovskite Light-Emitting Diodes

In recent years, the field of metal-halide perovskite emitters has rapidly emerged as a new community in solid-state lighting. Their exceptional optoelectronic properties have contributed to the rapid rise in external quantum efficiencies (EQEs) in perovskite light-emitting diodes (PeLEDs) from <1% (in 2014) to approaching 30% (in 2023) across a wide range of wavelengths. However, several challenges still hinder their commercialization, including the relatively low EQEs of blue/white devices, limited EQEs in large-area devices, poor device stability, as well as the toxicity of the easily accessible lead components and the solvents used in the synthesis and processing of PeLEDs. This roadmap addresses the current and future challenges in PeLEDs across fundamental and applied research areas, by sharing the community's perspectives. This work will provide the field with practical guidelines to advance PeLED development and facilitate more rapid commercialization.

physics.optics↗

arXiv2023

Spin injection across a III-V/chiral perovskite interface enabling spin accumulation at room temperature

Spin accumulation in semiconductor structures at room temperature and without magnetic fields is key to enable a broader range of opto-electronic functionality. Current efforts are limited due to inherent inefficiencies associated with spin injection into semiconductor structures. Here, we demonstrate spin injection across chiral halide perovskite/III-V interfaces achieving spin accumulation in a standard semiconductor III-V (AlxGa1-x)0.5In0.5P multiple quantum well (MQW) light emitting diode (LED). The spin accumulation in the MQW is detected via emission of circularly polarized light with a degree of polarization of up to ~15%. The chiral perovskite/III-V interface was characterized with X-ray photoemission spectroscopy (XPS), cross sectional scanning Kelvin probe force microscopy, and cross section transmission electron microscopy (TEM) imaging, showing a clean semiconductor/semiconductor interface where the fermi-level can equilibrate. These findings demonstrate chiral perovskite semiconductors can transform well-developed semiconductor platforms to ones that can also control spin.

physics.app-ph↗

arXiv2023

Tunable Magnon-Photon Coupling by Magnon Band Gap in a Layered Hybrid Perovskite Antiferromagnet

Tunability of coherent coupling between fundamental excitations is an important prerequisite for expanding their functionality in hybrid quantum systems. In hybrid magnonics, the dipolar interaction between magnon and photon usually persists and cannot be switched off. Here, we demonstrate this capability by coupling a superconducting resonator to a layered hybrid perovskite antiferromagnet, which exhibits a magnon band gap due to its intrinsic Dzyaloshinskii-Moriya interaction. The pronounced temperature sensitivity of the magnon band gap location allows us to set the photon mode within the gap and to disable magnon-photon hybridization. When the resonator mode falls into the magnon band gap, the resonator damping rate increases due to the nonzero coupling to the detuned magnon mode. This phenomena can be used to quantify the magnon band gap using an analytical model. Our work brings new opportunities in controlling coherent information processing with quantum properties in complex magnetic materials.

cond-mat.mtrl-sci↗

arXiv2022

Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells

The presence of unreacted lead iodide in organic-inorganic lead halide perovskite solar cells is widely correlated with an increase in power conversion efficiency. We investigate the mechanism for this increase by identifying the role of surfaces and interfaces present between methylammonium lead iodide perovskite films and excess lead iodide. We show how type I and II band alignments arising under different conditions result in either passivation of surface defects or hole injection. Through first-principles simulations of solid-solid interfaces, we find that lead iodide captures holes from methylammonium lead iodide and modulates the formation of defects in the perovskite, affecting recombination. Using surface-sensitive optical spectroscopy techniques, such as transient reflectance and time-resolved photoluminescence, we show how excess lead iodide affects the diffusion and surface recombination velocity of charge carriers in methylammonium lead iodide films. Our coupled experimental and theoretical results elucidate the role of excess lead iodide in perovskite solar cells.

cond-mat.mtrl-sci↗