arXiv subjects

Michael P. Nielsen

Publications and source records attributed to Michael P. Nielsen.

16 recordsLinked to original sources

arXiv2026

Multiplexing approaches to thermoradiative signatureless communications

Using mid-infrared emission from semiconductor devices for covert communications remains a relatively unexplored and yet promising opportunity. The phenomenon of negative luminescence allows for a method of signatureless covert communications where the net infrared emission of an emitting optoelectronic device is balanced to be identical to the ambient thermal background. In this work we provide a practical demonstration of covert data transfer over a thermoradiative channel with data rates up to 100 kbps. In addition, we demonstrate several additional multiplexing techniques that make the proposed thermoradiative communications method more secure against interception by achieving zero instantaneous optical emission, while remaining detectable if a sufficiently spatially or spectrally discerning observation is utilised. Finally, we discuss various application scenarios in which the proposed methods can be used to achieve secure signatureless communications.

physics.app-ph↗

arXiv2026

Silicon Solar Cell Design for >30% Efficiency via Singlet Fission

Singlet fission (SF) materials convert high-energy photons into multiple charge carriers, providing a route to exceed the efficiency limits of single-junction silicon solar cells without many of the complexities of multi-junction tandem designs. Following the first demonstration of an SF-enhanced silicon solar cell in 2025, there is a need to understand how SF materials can be effectively integrated into high-efficiency industrial silicon devices and translated from proof of concept to a manufacturable technology. Using coupled optical and electrical simulations, we assess the efficiency potential of several industrially relevant silicon cell architectures combined with SF materials. Interdigitated back-contact (IBC) cells offer the greatest potential for improvement due to unrestricted front-surface access and can achieve efficiencies exceeding 33%. However, performance is highly sensitive to front-surface passivation quality. Appropriate silicon design, particularly controlled surface doping and fixed interfacial charge, can mitigate recombination losses and relax passivation requirements for ultra-thin exciton-transfer layers.

cond-mat.mtrl-sci↗

arXiv2026

Thermal history controls the optoelectronic response of lead halide perovskites through structure and dynamics

Lead halide perovskites are promising optoelectronic materials for photovoltaics, light emission and detection. Their efficiencies in PV now approach the detailed-balance limit, leaving stability as the principal barrier. The intrinsic instabilities studied to date centre on ionic motion within a fixed, homogeneous lattice. Here we identify a further source of intrinsic structural instability, hidden in the lattice dynamics. Mapping caesium, methylammonium and formamidinium-based compositions with Cl, Br, I and mixed X-sites through all accessible phases, using single crystal X-ray and neutron diffuse scattering, machine-learning-assisted molecular dynamics, a phenomenological octahedral tilt model and hyperspectral photoluminescence, we find that nearly every composition hosts equilibrium local structural fluctuations: dynamic nanodomains of correlated octahedral tilts, a few nanometres in size, that locally break the crystallographic symmetry. Three complementary levers control them. The A-site cation sets their symmetry, shape and anisotropy, from sparse, isotropic and tetragonal in formamidinium-based compositions to dense, anisotropic and orthorhombic in nominally cubic caesium-based ones, the most locally disordered we studied. The halide controls the dynamic disorder and the phase-transition sequence. Thermal history is the third: different ramp rates drive nominally identical compositions into distinct crystallographic phases, each with its own hidden local order. In MAPbI3, the heating rate alone changes the photoluminescence quantum efficiency across the phase transition. Because these transitions lie within device operating ranges, from terrestrial thermal cycling to the extremes of space, thermal history may shape the local structure, and hence the optoelectronic response, throughout fabrication and operation, establishing it as a design variable alongside composition.

cond-mat.mtrl-sci↗

arXiv2026

Visible Imaging of Incoherent 1200-nm Light via Triplet--Triplet Annihilation Upconversion

Upconversion of low-energy photons to higher-energy photons provides an opportunity to surpass traditional limitations in fields such as 3D printing, photovoltaics, and photocatalysis. Triplet--triplet annihilation upconversion (TTA-UC) is particularly appealing for such applications as it can efficiently upconvert low-intensity, incoherent light. However, previously demonstrated thin-film TTA systems are simultaneously constrained by modest efficiencies and limited reach into the near infrared (NIR). Here, we design a single-layer thin-film bulk heterojunction that integrates PbS quantum dots (QDs) as tunable NIR absorbers within an organic semiconductor matrix of TES-ADT, achieving large anti-Stokes shifts up to 500 nm and high internal quantum efficiencies across the NIR-I and NIR-II windows (800-1200 nm). Through the incorporation of 5-tetracene carboxylic acid ligands on the PbS QD surface, the yield of sensitized triplets was boosted, as confirmed by transient absorption and time-resolved photoluminescence measurements. The resulting films demonstrated a 15-fold improvement in UC efficiency. Furthermore, we demonstrate visible imaging of incoherent 1200 nm light via thin-film TTA-UC at incident intensities at the imaging mask as low as 20 mWcm$^2$, marking a significant advance toward practical implementation of solid-state NIR-to-visible upconversion.

physics.optics↗

arXiv2026

Anomalous Platinum and Oxygen Transport during Electroforming of NbOx Memristors

Electroforming of metal-oxide-metal memristors is generally attributed to the creation of oxygen-vacancy filaments within the oxide, with noble metal electrodes such as Pt and Au remaining chemically inert. Here, we demonstrate that electroforming and subsequent operation of Pt/NbOx/Nb2O5/Pt devices can induce an unexpected and highly correlated redistribution of both oxygen and platinum. Time-of-flight secondary ion mass spectrometry reveals a filamentary pathway characterized by micrometer-scale oxygen enrichment extending from the Nb2O5 layer through NbOx and deep into the Pt top electrode. Surprisingly, this is accompanied by the formation of a Pt-rich filament penetrating the oxide stack along the same filamentary path. Finite-element and lumped-element modelling show that current-controlled negative-differential-resistance operation produces localized Joule heating and high-frequency thermal cycling, which strongly enhances oxygen migration and enables thermally assisted Pt diffusion along vacancy-rich pathways. These findings reveal a previously unrecognized metal-ion transport mechanism in NbOx memristors and highlight the critical role of post-forming electrical dynamics in determining filament chemistry, stability, and device reliability.

cond-mat.mtrl-sci↗

arXiv2025

Mitigating Singlet Exciton Back-Transfer using 2D Spacer Layers for Perovskite-Sensitised Upconversion

Photon upconversion has potential applications in light-emitting diodes, photocatalysis, bio-imaging, microscopy, 3D printing, and photovoltaics. Bulk lead-halide perovskite films have emerged as promising sensitisers for solid-state photon upconversion via triplet-triplet annihilation due to their excellent optoelectronic properties. In this system, a perovskite sensitiser absorbs photons and subsequently generates triplet excitons in an adjacent emitter material, where triplet-triplet annihilation can occur allowing for the emission of higher energy photons. However, a major loss pathway in perovskite-sensitised upconversion is the back-transfer of singlet excitons from the emitter to the sensitiser via Förster Resonance Energy Transfer. In this investigation we introduce a 2D perovskite spacer layer between the bulk perovskite sensitiser and a rubrene emitter to mitigate back-transfer of singlet excitons from rubrene to the bulk perovskite sensitiser. This modification reveals the inherent balance between efficient triplet exciton transfer across the interface with a potential barrier versus the mitigation of near-field back-transfer by increasing the distance between the sensitiser and singlet excitons in the emitter. Notably, the introduction of this spacer layer enhances the relative upconversion efficiency at lower excitation power densities while also sustaining performance over extended timescales. This work represents significant progress toward the practical applications of perovskite-sensitised photon upconversion.

cond-mat.mtrl-sci↗

arXiv2025

Liquid Metal-Exfoliated SnO$_2$-Based Mixed-dimensional Heterostructures for Visible-to-Near-Infrared Photodetection

Ultra-thin two-dimensional (2D) materials have gained significant attention for making next-generation optoelectronic devices. Here, we report a large-area heterojunction photodetector fabricated using a liquid metal-printed 2D $\text{SnO}_2$ layer transferred onto CdTe thin films. The resulting device demonstrates efficient broadband light sensing from visible to near-infrared wavelengths, with enhanced detectivity and faster photo response than bare CdTe photodetectors. Significantly, the device shows a nearly $10^5$-fold increase in current than the dark current level when illuminated with a 780 nm laser and achieves a specific detectivity of around $10^{12} \, \text{Jones}$, nearly two orders of magnitude higher than a device with pure CdTe thin film. Additionally, temperature-dependent optoelectronic testing shows that the device maintains a stable response up to $140^\circ \text{C}$ and generates distinctive photocurrent at temperatures up to $80^\circ \text{C}$, demonstrating its thermal stability. Using band structure analysis, density functional theory (DFT) calculations, and photocurrent mapping, the formation of a $p$-$n$ junction is indicated, contributing to the enhanced photo response attributed to the efficient carrier separation by the built-in potential in the hetero-junction and the superior electron mobility of 2D $\text{SnO}_2$. Our results highlight the effectiveness of integrating liquid metal-exfoliated 2D materials for enhanced photodetector performance.

cond-mat.mtrl-sci↗

arXiv2024

Dynamic Nanodomains Dictate Macroscopic Properties in Lead Halide Perovskites

Empirical A-site cation substitution has advanced the stability and efficiency of hybrid organic-inorganic lead halide perovskites solar cells and the functionality of X-ray detectors. Yet, the fundamental mechanisms underpinning their unique performance remain elusive. This multi-modal study unveils the link between nanoscale structural dynamics and macroscopic optoelectronic properties in these materials by utilising X-ray diffuse scattering, inelastic neutron spectroscopy and optical microscopy complemented by state-of-the-art machine learning-assisted molecular dynamics simulations. Our approach uncovers the presence of dynamic, lower-symmetry local nanodomains embedded within the higher-symmetry average phase in various perovskite compositions. The properties of these nanodomains are tunable via the A-site cation selection: methylammonium induces a high density of anisotropic, planar nanodomains of out-of-phase octahedral tilts, while formamidinium favours sparsely distributed isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. The observed variations in the properties of dynamic nanodomains are in agreement with our simulations and are directly linked to the differing macroscopic optoelectronic and ferroelastic behaviours of these compositions. By demonstrating the influence of A-site cation on local nanodomains and consequently, on macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics, and X-ray imaging.

cond-mat.mtrl-sci↗

arXiv2024

Long-Lived Coherent Acoustic Phonons in Epitaxially Grown III-V Adiabatic Cavities

We provide evidence of strongly confined coherent acoustic phonons inside high quality factor phononic cavities that exhibit tailoredphonon potentials. Using GaAs/AlAs quasiperiodic superlattices, these functional phonon potentials are realized by adiabatically changing the layer thicknesses along the growth direction. Room temperature ultrafast vibrational spectroscopy reveals discrete phonon levels in the range of $\approx 96-101$ GHz. Additionally, we confirm that phononic cavities significantly retard the energy loss rate of the photoexcited carriers as evidenced by time-resolved photoluminescence measurements. These results highlight the potential of opto-phononic devices that can bridge the divide between phononics and optoelectronics by concurrently engineering electronic and phononic properties.

physics.app-ph↗

arXiv2022

Identifying optimal photovoltaic technologies for underwater applications

Improving solar energy collection in aquatic environments would allow for superior environmental monitoring and remote sensing, but the identification of optimal photovoltaic technologies for such applications is challenging as evaluation requires either field deployment or access to large water tanks. Here, we present a simple bench-top characterization technique that does not require direct access to water and therefore circumvents the need for field testing during initial trials of development. Employing LEDs to simulate underwater solar spectra at various depths, we compare Si and CdTe solar cells, two commercially available technologies, with GaInP cells, a technology with a wide band gap close to ideal for underwater solar harvesting. We use this method to show that while Si cells outperform both CdTe and GaInP under terrestrial AM1.5G solar irradiance, both CdTe and GaInP outperform Si at depths > 2 m, with GaInP cells operating with underwater efficiencies exceeding 51%.

physics.app-ph↗

arXiv2022

Acceleration and adiabatic expansion of multi-state fluorescence from a nanofocus

Since Purcell's seminal report 75 years ago, electromagnetic resonators have been used to control light-matter interactions to make brighter radiation sources and unleash unprecedented control over quantum states of light and matter. Indeed, optical resonators such as microcavities and plasmonic nanostructures offer excellent control but only over a limited spectral range. Strategies to tune both emission and the resonator are often required, which preclude the possibility of enhancing multiple transitions simultaneously. In this letter, we report a more than 590-fold radiative emission enhancement across the telecommunications emission band of Erbium-ions in silica using a single non-resonant plasmonic waveguide. Our plasmonic waveguide uses a novel reverse nanofocusing approach to efficiently collect emission, making these devices brighter than all non-plasmonic control samples considered. Remarkably, the high broadband Purcell factor allows us to resolve the Stark-split electric dipole transitions, which are typically only observed under cryogenic conditions. Simultaneous Purcell enhancement of multiple quantum states is of interest for photonic quantum networks as well as on-chip data communications.

physics.optics↗

arXiv2022

Singlet Fission Photovoltaics: Progress and Promising Pathways

Singlet fission is a form of multiple exciton generation which occurs in organic chromophores when a high energy singlet exciton separates into two lower energy triplet excitons, each with approximately half the singlet energy. Since this process is spin-allowed it can proceed on an ultrafast timescale of less than several picoseconds, outcompeting most other loss mechanisms and reaching quantitative yields approaching 200%. Due to this high quantum efficiency, the singlet fission process shows promise as a means of reducing thermalisation losses in photovoltaic cells. This would potentially allow for efficiency improvements beyond the thermodynamic limit in a single junction cell. Efforts to incorporate this process into solar photovoltaic cells have spanned a wide range of device structures over the past decade. In this review we compare and categorise these attempts in order to assess the state of the field and identify the most promising avenues of future research and development.

physics.app-ph↗

arXiv2022

Electronic and optical properties of Si$_{x}$Ge$_{1-x-y}$Sn$_{y}$ alloys lattice-matched to Ge

We present a combined experimental and theoretical analysis of the evolution of the near-band gap electronic and optical properties of Si$_{x}$Ge$_{1-x-y}$Sn$_{y}$ alloys lattice-matched to Ge and GaAs substrates. We perform photoreflectance (PR) and photoluminescence (PL) measurements on Si$_{x}$Ge$_{1-x-y}$Sn$_{y}$ epitaxial layers grown via chemical vapour deposition, for Si (Sn) compositions up to $x =$ 9.6% ($y =$ 2.5%). Our measurements indicate the presence of an indirect fundamental band gap, with PL observed $\approx$ 200-250 meV lower in energy than the direct $E_0$ transition identified by PR measurements. The measured PL is Ge-like, suggesting that the alloy conduction band (CB) edge is primarily derived from the Ge L-point CB minimum. Interpretation of the PR and PL measurements is supported by atomistic electronic structure calculations. Effective alloy band structures calculated via density functional theory confirm the presence of an indirect fundamental band gap, and reveal the origin of the observed inhomogeneous broadening of the measured optical spectra as being alloy-induced band hybridisation occurring close in energy to the CB edge. To analyze the evolution of the band gap, semi-empirical tight-binding (TB) calculations are employed to enable calculations for large supercell sizes. TB calculations reveal that the alloy CB edge is hybridized in nature, consisting at low Si and Sn compositions of an admixture of Ge L-, $Γ$- and X-point CB edge states, and confirm that the alloy CB edge retains primarily Ge L-point CB edge character. Our experimental measurements and theoretical calculations confirm a direct transition energy close to 1 eV in magnitude for Si and Sn compositions $x =$ 6.8 - 9.6% and $y =$ 1.6 - 2.2%.

cond-mat.mtrl-sci↗

arXiv2020

Optoelectronic Reciprocity in Hot Carrier Solar Cells with Ideal Energy Selective Contacts

Hot carrier solar cells promise theoretical power conversion efficiencies far beyond the single junction limit. However, practical implementations of hot carrier solar cells have lagged far behind those theoretical predictions. Reciprocity relations for electro-luminescence from conventional single junction solar cells have been extremely successful in driving their efficiency ever closer to the theoretical limits. In this work, we discuss how the signatures of a functioning hot carrier device should manifest experimentally in electro-luminescence and dark $I-V$ characteristics. Hot carrier properties lead to deviations from the Shockley diode equation that is typical for conventional single junction solar cells. These deviations are directly linked to an increase in temperature of the carriers and therefore the temperature measured from electro-luminescence spectra. We also elucidate how the behaviour of hot carrier solar cells in the dark depends on whether Auger processes play a significant role, revealing a stark contrast between the regime of negligible Auger recombination (carrier conservation model) and dominant Auger recombination (Impact Ionization model) for hot carrier solar cells.

physics.app-ph↗

arXiv2019

Hybrid plasmonic waveguide coupling of photons from a single molecule

We demonstrate the emission of photons from a single molecule into a hybrid gap plasmon waveguide (HGPW). Crystals of anthracene, doped with dibenzoterrylene (DBT), are grown on top of the waveguides. We investigate a single DBT molecule coupled to the plasmonic region of one of the guides, and determine its in-plane orientation, excited state lifetime and saturation intensity. The molecule emits light into the guide, which is remotely out-coupled by a grating. The second-order auto-correlation and cross-correlation functions show that the emitter is a single molecule and that the light emerging from the grating comes from that molecule. The coupling efficiency is found to be $β_{WG}=11.6(1.5)\%$. This type of structure is promising for building new functionality into quantum-photonic circuits, where localised regions of strong emitter-guide coupling can be interconnected by low-loss dielectric guides.

quant-ph↗

arXiv2017

Efficient four-wave mixing at the nanofocus of integrated organic gap plasmon waveguides on silicon

Nonlinear optics, especially frequency mixing, underpins modern optical technology and scientific exploration in quantum optics, materials and life sciences, and optical communications. Since nonlinear effects are weak, efficient frequency mixing must accumulate over large interaction lengths restricting the integration of nonlinear photonics with electronics and establishing limitations on mixing processes due to the requirement of phase matching. In this work we report efficient four-wave mixing over micron-scale interaction lengths at telecoms wavelengths. We use an integrated plasmonic gap waveguide on silicon that strongly confines light within a nonlinear organic polymer in the gap. Our approach is so effective because the gap waveguide intensifies light by efficiently nanofocusing it to a mode cross-section of a few tens of nanometres, generating a nonlinear response so strong that efficient four-wave mixing accumulates in just a micron. This is significant as our technique opens up nonlinear optics to a regime where phase matching and dispersion considerations are relaxed, giving rise to the possibility of compact, broadband, and efficient frequency mixing on a platform that can be integrated with silicon photonics.

physics.optics↗