arXiv subjects

Robert L. Z. Hoye

Publications and source records attributed to Robert L. Z. Hoye.

At least 19 recordsLinked to original sources

arXiv2026

Computing at the Edge Enabled by Indoor Photovoltaics and Ferroelectrics

The exponential, pervasive rise of artificial intelligence (AI), hosted in large data centres, will test the limits of the underpinning infrastructure, including electricity and water supplies, which are becoming increasingly precious resources. Rather than performing all AI computations in centralized servers, for many functionalities, these can be performed locally across a network of billions of small, autonomous nodes, saving substantial energy costs associated with communication. This alternative paradigm is known as edge computing, or distributed intelligence (DI), but has been held back by the lack of availability of reliable local energy supplies matching the energy requirements of the computational infrastructure. Opportunities to address this challenge are emerging with rapid advances in high-performance indoor photovoltaics (IPVs) for local energy harvesting, as well as reductions in computational cost through neuromorphic or in-memory computing devices. In this perspective, we discuss the requirements of IPVs for DI, the extent to which emerging materials fulfil these requirements, and how current gaps could be addressed. We make the case that (anti)ferroelectric materials can surpass bottlenecks for both electrostatic energy storage and low-power in-memory neuromorphic computing. The core theme of this perspective is that co-creation between energy harvesting, storage and computing is essential for making DI a reliable and more sustainable alternative to centralized AI.

cond-mat.mtrl-sci↗

arXiv2026

Carrier Localization in Pnictogen-Based Chalcohalides from Defect-Bound Hot Polarons

Pnictogen-based solar absorbers have gained prominence as promising nontoxic and stable alternatives to lead-halide perovskites (LHPs), but are severely limited by carrier localization, preventing their performance from approaching those of LHPs. Recent efforts have uncovered routes to overcome carrier localization, but these early efforts only considered intrinsic factors. Herein, we push beyond these limited early efforts, examining the role of defects, not only on cold carriers but also hot carriers. Focusing on the structurally one-dimensional pnictogen chalcohalide BiSBr, we find that whilst this material intrinsically does not exhibit carrier localization, vacancies introduced during synthesis or post-treatment lead to pronounced extrinsic self-trapping via the formation of defect-bound hot polarons-excited charge-carriers strongly coupled to local defect-induced vibrational modes. These above-gap defect states divert hot carriers from cooling to the band edge, thus depleting the mobile carrier population. Our findings establish the key role of defect-bound hot polarons in mediating extrinsic localization and offer new mechanistic insights into the interplay between defects, lattice coupling, and excited-state charge-carrier transport, which are critical to designing efficient perovskite-inspired solar absorbers.

cond-mat.mtrl-sci↗

arXiv2026

Rapid Atmospheric Vapor Deposition of H:In2O3 Transparent Conducting Oxide Thin Films

Transparent conducting oxides (TCOs) are essential for the optoelectronics industry, but there is a critical gap in cost-effective methods to rapidly deposit low sheet resistance, high transmittance films without damaging delicate materials, including emerging soft semiconductors like metal-halide perovskites. In this work, atmospheric pressure chemical vapor deposition (AP-CVD) is used to synthesise H:In2O3 films with 7.20+/-0.01 Ohm/sq sheet resistance (0.50+/-0.06 mOhm.cm resistivity) and transmittance up to 89% in the near-infrared (NIR), surpassing commercial sputter-deposited indium tin oxide. The growth rate is 40x higher than atomic layer deposition (ALD), and the AP-CVD films are fully processed under atmospheric conditions at only 140 C. Comparison of secondary ion mass spectrometry and time-of-flight elastic recoil detection analysis with changes in carrier concentration indicate that H dopants are introduced from the water oxidant. There is an increase in mobility form 40+/-10 cm2/Vs to 160+/-30 cm2/Vs when changing from O2 to H2O as the oxidant, which is attributed to H dopants passivating oxygen vacancies that act as carrier scattering centers. This work establishes AP-CVD as a promising method for manufacturing high figure-of-merit TCOs in a rapid, scalable and cost-effective manner, using mild growth conditions compatible with thermally-sensitive materials.

cond-mat.mtrl-sci↗

arXiv2026

Circularity in Perovskite-Based Tandem Photovoltaics for Terawatt-Scale Deployment

As photovoltaics (PVs) scale from one to multiple terawatts over the next decade, ensuring sustainable deployment is urgently required. Crystalline silicon (c-Si) PVs, the current industry standard, will generate an estimated 160 million tonnes of waste by 2050, and there remains complex technoeconomic challenges associated with their recycling. Metal-halide perovskite (MHP)-based tandem PVs not only promise higher power conversion efficiencies than single-junction c-Si devices, but also offer intrinsic advantages for circularity, including simpler device architectures, low-temperature processing, and more accessible materials recovery routes. At this pivotal juncture when perovskite PVs begin to enter the market, this review examines the critical circularity challenges that must be addressed: substitution of scarce raw materials, scalable recycling protocols, cost-effective stack delamination, safe lead sequestration, and policy frameworks to encourage circularity across the device lifecycle with effective incentives. By integrating the materials, technoeconomic and policy dimensions that go beyond conventional lifecycle assessments, we outline actionable strategies to co-optimize device performance and sustainability. This review aims to guide researchers, policymakers, and industry stakeholders in steering perovskite-based tandem PVs towards a circular and responsible commercialization pathway within the global clean-energy transition.

cond-mat.mtrl-sci↗

arXiv2026

Band-Like Transport and Cation Off-Centring in Ag/Bi-Based Solar Absorbers

Ag(I)-Bi(III)-based semiconductors have gained substantial attention as nontoxic, stable alternatives to lead-halide perovskites for optoelectronics, but are widely limited by carrier localization, which severely restricts diffusion lengths. The most efficient Ag/Bi solar absorber is AgBiS2, but diffusion lengths in nanocrystal films are <50 nm. Carrier localization in this rock-salt (Fm-3m) system is believed to arise from cation disorder, and so we herein investigate the layered cation-ordered analogue. Through beyond-DFT simulations combined with neutron and X-ray powder diffraction, we reveal that off-centring of Ag+ and Bi3+ cations is energetically-favoured in this cation-ordered phase. Despite local distortions in the AgS6 and BiS6 octahedra, band-like transport takes place, which, surprisingly, also occurs in the cation-disordered rock-salt phase when these materials are made as bulk powders. The cubic-phase powders have the same degree of cation disorder as the nanocrystals that have carrier localization, which suggests that extrinsic factors play a determining role. We ascribe the intrinsic band-like transport of both phases of AgBiS2 to its close packing, ensuring high electronic dimensionality. These insights offer pathways for designing solar absorbers avoiding carrier localization limitations, and call for future efforts to enhance the efficiency of AgBiS2 photovoltaics to focus on large-grained thin films, or improved nanocrystal surface passivation.

cond-mat.mtrl-sci↗

arXiv2026

Ligand Engineering for Precise Control of Ultrathin CsPbI3 Nanoplatelet Superlattices for Efficient Light-Emitting Diodes

Strongly-confined perovskite nanoplatelets (PeNPLs) offer opportunities not found in conventional isotropic nanocubes, especially in producing linearly polarized light, as well as enhancing outcoupling through control over the transition dipole moment. But this requires ultrathin nanoplatelets with three or fewer monolayers of PbI6 octahedra across the thickness, which are challenging to synthesise uniformly, and their luminescence is strongly affected by surface defects. Together, these limit the performance of ultrathin PeNPLs in light-emitting diodes (LEDs). Here, we address these challenges with an ancillary ligand engineering strategy. We demonstrate that ligands with phosphoryl functional groups strongly bind to the perovskite surface, while having an organic backbone that is not sterically bulky ensures high ligand density. By modulating nucleation and growth, these ancillary ligands lead to monodisperse PeNPLs that stack more uniformly when self-assembled into superlattices, with suppressed agglomeration. As a result, from edge-up PeNPL superlattices, we achieve enhanced degree of polarization, while from face-down PeNPL superlattices, we achieve enhanced outcoupling that results in LEDs with 13.1% external quantum efficiency, the highest reported for ultrathin PeNPL LEDs. This work establishes ancillary ligand-induced synthesis as a decisive route to achieve uniform nanoplatelets with robust orientation control, enabling full utilization of the multifunctionality of anisotropic PeNPLs.

physics.optics↗

arXiv2025

Breaking the 800 mV open-circuit voltage barrier in antimony sulfide photovoltaics

Sb2S3 is a promising material for low-toxicity, high-stability next-generation photovoltaics. Despite high optical limits in efficiency, progress in improving its device performance has been limited by severe voltage losses. Recent spectroscopic investigations suggest that self-trapping occurs in Sb2S3, limiting the open-circuit voltage (Voc) to a maximum of approximately 800 mV, which is the level the field has asymptotically approached. In this work, we surpass this voltage barrier through reductions in the defect density in Sb2S3 thin films by modulating the growth mechanism in chemical bath deposition using citrate ligand additives. Deep level transient spectroscopy identifies two deep traps 0.4-0.7 eV above the valence band maximum, and, through first-principles calculations, we identify these to likely be S vacancies, or Sb on S anti-sites. The concentrations of these traps are lowered by decreasing the grain boundary density from 1114+/-52 nm/um2 to 585+/-10 nm/um2, and we achieve a Voc of 824 mV, the record for Sb2S3 solar cells. This work addresses the debate in the field around whether Sb2S3 is limited by defects or self-trapping, showing that it is possible to improve the performance towards the radiative limit through careful defect engineering.

cond-mat.mtrl-sci↗

arXiv2025

Enhanced Stability and Linearly Polarized Emission from CsPbI$_3$ Perovskite Nanoplatelets through A-site Cation Engineering

The anisotropy of perovskite nanoplatelets (PeNPLs) opens up many opportunities in optoelectronics, including enabling the emission of linearly polarized light. But the limited stability of PeNPLs is a pressing challenge, especially for red-emitting CsPbI$_3$. Herein, we address this limitation by alloying FA into the perovskite cuboctahedral site. Unlike Cs/FA alloying in bulk thin films or nonconfined nanocubes, FA incorporation in nanoplatelets requires meticulous control over the reaction conditions, given that nanoplatelets are obtained in kinetically-driven growth regimes instead of thermodynamically-driven conditions. Through in-situ photoluminescence (PL) measurements, we find that excess FA leads to uncontrolled growth, where phase-impurities and nanoplatelets of multiple thicknesses co-exist. Restricting the FA content to up to 25% Cs substitution enables monodisperse PeNPLs, and increases the PL quantum yield (from 53% to 61%), exciton lifetime (from 18 ns to 27 ns), and stability in ambient air (from ~2 days to >7 days) compared to CsPbI$_3$. This arises due to hydrogen bonding between FA and the oleate and oleylammonium ligands, anchoring them to the surface to improve optoelectronic properties and stability. The reduction in non-radiative recombination, improvement in the nanoplatelet aspect ratio, and higher ligand density lead to FA-containing PeNPLs more effectively forming edge-up superlattices, enhancing the PL degree of linear polarization from 5.1% (CsPbI$_3$) to 9.4% (Cs$_{0.75}$FA$_{0.25}$PbI$_3$). These fundamental insights show how the stability limitations of PeNPLs could be addressed, and these materials grown more precisely to improve their performance as polarized light emitters, critical for utilizing them in next-generation display, bioimaging and communications applications.

cond-mat.mtrl-sci↗

arXiv2024

Multifaceted nature of defect tolerance in halide perovskites and emerging semiconductors

Lead-halide perovskites (LHPs) have shot to prominence as efficient energy conversion materials that can be processed using cost-effective fabrication methods. A widely-quoted reason for their exceptional performance is their ability to tolerate defects, enabling long charge-carrier lifetimes despite high defect densities. Realizing defect tolerance in broader classes of materials would have a substantial impact on the semiconductor industry. Significant effort has been made over the past decade to unravel the underlying origins of defect tolerance to design stable alternatives to LHPs comprised of nontoxic elements. However, it has become clear that understanding defect tolerance in LHPs is far from straightforward. This review discusses the models proposed for defect tolerance in halide perovskites, evaluating the experimental and theoretical support for these models, as well as their limitations. We cover attempts to apply these models to identify materials beyond the lead-halide system that could also exhibit defect tolerance, and the successes and pitfalls encountered over the past decade. Finally, a discussion is made of some of the important missing pieces of information required for a deeper understanding and predictive models that enable the inverse design of defect tolerant semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

Additive engineering for Sb$_2$S$_3$ indoor photovoltaics with efficiency exceeding 17%

Indoor photovoltaics (IPVs) have attracted increasing attention for sustainably powering Internet of Things (IoT) electronics. Sb$_2$S$_3$ is a promising IPV candidate material with a bandgap of ~1.75 eV, which is near the optimal value for indoor energy harvesting. However, the performance of Sb$_2$S$_3$ solar cells is limited by nonradiative recombination, closely associated with the poor-quality absorber films. Additive engineering is an effective strategy to improved the properties of solution-processed films. This work shows that the addition of monoethanolamine (MEA) into the precursor solution allows the nucleation and growth of Sb$_2$S$_3$ films to be controlled, enabling the deposition of high-quality Sb$_2$S$_3$ absorbers with reduced grain boundary density, optimized band positions and increased carrier concentration. Complemented with computations, it is revealed that the incorporation of MEA leads to a more efficient and energetically favorable deposition for enhanced heterogeneous nucleation on the substrate, which increases the grain size and accelerates the deposition rate of Sb$_2$S$_3$ films. Due to suppressed carrier recombination and improved charge-carrier transport in Sb$_2$S$_3$ absorber films, the MEA-modulated Sb$_2$S$_3$ solar cell yields a power conversion efficiency (PCE) of 7.22% under AM1.5G illumination, and an IPV PCE of 17.55% under 1000 lux white light emitting diode (WLED) illumination, which is the highest yet reported for Sb$_2$S$_3$ IPVs. Furthermore, we construct high performance large-area Sb$_2$S$_3$ IPV modules to power IoT wireless sensors, and realize the long-term continuous recording of environmental parameters under WLED illumination in an office. This work highlights the great prospect of Sb$_2$S$_3$ photovoltaics for indoor energy harvesting.

cond-mat.mtrl-sci↗

arXiv2024

Extending the Defect Tolerance of Halide Perovskite Nanocrystals to Hot Carrier Cooling Dynamics

Defect tolerance is a critical enabling factor for efficient lead-halide perovskite materials, but the current understanding is primarily on band-edge (cold) carriers, with significant debate over whether hot carriers (HCs) can also exhibit defect tolerance. Here, this important gap in the field is addressed by investigating how internationally-introduced traps affect HC relaxation in CsPbX3 nanocrystals (X = Br, I, or mixture). Using femtosecond interband and intraband spectroscopy, along with energy-dependent photoluminescence measurements and kinetic modelling, it is found that HCs are not universally defect tolerant in CsPbX3, but are strongly correlated to the defect tolerance of cold carriers, requiring shallow traps to be present (as in CsPbI3). It is found that HCs are directly captured by traps, instead of going through an intermediate cold carrier, and deeper traps cause faster HC cooling, reducing the effects of the hot phonon bottleneck and Auger reheating. This work provides important insights into how defects influence HCs, which will be important for designing materials for hot carrier solar cells, multiexciton generation, and optical gain media.

physics.app-ph↗

arXiv2024

Factors Enabling Delocalized Charge-Carriers in Pnictogen-Based Solar Absorbers: In-depth Investigation into CuSbSe2

Inorganic semiconductors based on heavy pnictogen cations (Sb3+ and Bi3+) have gained significant attention as potential nontoxic and stable alternatives to lead-halide perovskites for solar cell applications. A limitation of these novel materials, which is being increasingly commonly found, is carrier localization, which substantially reduces mobilities and diffusion lengths. Herein, the layered příbramite CuSbSe2 is investigated and discovered to have delocalized free carriers, as shown through optical pump terahertz probe spectroscopy and temperature-dependent mobility measurements. Using a combination of theory and experiment, it is found that the underlying factors are: 1) weak coupling to acoustic phonons due to low deformation potentials, as lattice distortions are primarily accommodated through rigid inter-layer movement rather than straining inter-atomic bonds, and 2) weak coupling to optical phonons due to the ionic contributions to the dielectric constant being low compared to electronic contributions. This work provides important insights into how pnictogen-based semiconductors avoiding carrier localization could be identified.

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

Roadmap on Photovoltaic Absorber Materials for Sustainable Energy Conversion

Photovoltaics (PVs) are a critical technology for curbing growing levels of anthropogenic greenhouse gas emissions, and meeting increases in future demand for low-carbon electricity. In order to fulfil ambitions for net-zero carbon dioxide equivalent (CO 2 eq) emissions worldwide, the global cumulative capacity of solar PVs must increase by an order of magnitude from 0.9 TWp in 2021 to 8.5 TWp by 2050 according to the International Renewable Energy Agency, which is considered to be a highly conservative estimate. In 2020, the Henry Royce Institute brought together the UK PV community to discuss the critical technological and infrastructure challenges that need to be overcome to address the vast challenges in accelerating PV deployment. Herein, we examine the key developments in the global community, especially the progress made in the field since this earlier roadmap, bringing together experts primarily from the UK across the breadth of the photovoltaics community. The focus is both on the challenges in improving the efficiency, stability and levelized cost of electricity of current technologies for utility-scale PVs, as well as the fundamental questions in novel technologies that can have a significant impact on emerging markets, such as indoor PVs, space PVs, and agrivoltaics. We discuss challenges in advanced metrology and computational tools, as well as the growing synergies between PVs and solar fuels, and offer a perspective on the environmental sustainability of the PV industry. Through this roadmap, we emphasize promising pathways forward in both the short- and long-term, and for communities working on technologies across a range of maturity levels to learn from each other.

physics.app-ph↗

arXiv2023

Fast near-infrared photodetectors based on nontoxic and solution-processable AgBiS2

Solution-processable near-infrared (NIR) photodetectors are urgently needed for a wide range of next-generation electronics, including sensors, optical communications and bioimaging. However, there is currently a compromise between low toxicity and slow (<300 kHz cut-off frequency) organic materials versus faster detectors (>300 kHz cut-off frequency) based on compounds containing toxic lead or cadmium. Herein, we circumvent this trade-off by developing solution-processed AgBiS2 photodetectors with high cut-off frequencies under both white light (>1 MHz) and NIR (approaching 500 kHz) illumination. These high cut-off frequencies are due to the short transit distances of charge-carriers in the AgBiS2 photodetectors, which arise from the strong light absorption of these materials, such that film thicknesses well below 120 nm are adequate to absorb >65% of near-infrared to visible light. By finely controlling the thickness of the photoactive layer, we can modulate the charge-collection efficiency, achieve low dark current densities, and minimize the effects of ion migration to realize fast photodetectors that are stable in air. These outstanding characteristics enable real-time heartbeat sensors based on NIR AgBiS2 photodetectors. # equal contribution, * corresponding authors

cond-mat.mtrl-sci↗

arXiv2023

Direct Linearly-Polarised Electroluminescence from Perovskite Nanoplatelet Superlattices

Polarised light is critical for a wide range of applications, but is usually generated by filtering unpolarised light, which leads to significant energy losses and requires additional optics. Herein, the direct emission of linearly-polarised light is achieved from light-emitting diodes (LEDs) made of CsPbI3 perovskite nanoplatelet superlattices. Through use of solvents with different vapour pressures, the self-assembly of perovskite nanoplatelets is achieved to enable fine control over the orientation (either face-up or edge-up) and therefore the transition dipole moment. As a result of the highly-uniform alignment of the nanoplatelets, as well as their strong quantum and dielectric confinement, large exciton fine-structure splitting is achieved at the film level, leading to pure-red LEDs exhibiting a high degree of linear polarisation of 74.4% without any photonic structures. This work unveils the possibilities of perovskite nanoplatelets as a highly promising source of linearly-polarised electroluminescence, opening up the development of next-generation 3D displays and optical communications from this highly versatile, solution-processable system.

physics.optics↗

arXiv2020

Identifying and reducing interfacial losses to enhance color-pure electroluminescence in blue-emitting perovskite nanoplatelet light-emitting diodes

Perovskite nanoplatelets (NPls) hold great promise for light-emitting applications, having achieved high photoluminescence quantum efficiencies (PLQEs) approaching unity in the blue wavelength range, where other metal-halide perovskites have typically been ineffective. However, the external quantum efficiency (EQE) of blue-emitting NPl light-emitting diodes (LEDs) have only reached 0.12%, with typical values well below 0.1%. In this work, we show that the performance of NPl LEDs is primarily hindered by a poor electronic interface between the emitter and hole-injector. Through Kelvin Probe and X-ray photoemission spectroscopy measurements, we reveal that the NPls have remarkably deep ionization potentials (>=6.5 eV), leading to large barriers for hole injection, as well as substantial non-radiative decay at the interface between the emitter and hole-injector. We find that an effective way to reduce these non-radiative losses is by using poly(triarylamine) interlayers. This results in an increase in the EQE of our blue LEDs emitting at 464 nm wavelength to 0.3%. We find that our results can be generalized to thicker sky-blue-emitting NPls, where we increase the EQE to 0.55% using the poly(triarylamine) interlayer. Our work also identifies the key challenges for further efficiency increases.

physics.optics↗

arXiv2020

Boosting tunable blue luminescence of halide perovskite nanoplatelets through post-synthetic surface trap repair

The easily tunable emission of halide perovskite nanocrystals throughout the visible spectrum makes them an extremely promising material for light-emitting applications. Whereas high quantum yields and long-term colloidal stability have already been achieved for nanocrystals emitting in the red and green spectral range, the blue region currently lags behind, with low quantum yields, broad emission profiles and insufficient colloidal stability. In this work, we present a facile synthetic approach for obtaining two-dimensional CsPbBr3 nanoplatelets with monolayer-precise control over their thickness, resulting in sharp photoluminescence and electroluminescence peaks with a tunable emission wavelength between 432 and 497 nm due to quantum confinement. Subsequent addition of a PbBr2-ligand solution repairs surface defects likely stemming from bromide and lead vacancies in a sub-ensemble of weakly emissive nanoplatelets. The overall photoluminescence quantum yield of the blue-emissive colloidal dispersions is consequently enhanced up to a value of 73+-2 %. Transient optical spectroscopy measurements focusing on the excitonic resonances further confirm the proposed repair process. Additionally, the high stability of these nanoplatelets in films and to prolonged UV light exposure is shown.

cond-mat.mes-hall↗