arXiv subjects

Marc A. Baldo

Publications and source records attributed to Marc A. Baldo.

9 recordsLinked to original sources

arXiv2024

Triplet Exciton Sensitization of Silicon Mediated by Defect States in Hafnium Oxynitride

Singlet exciton fission has the potential to increase the efficiency of crystalline silicon solar cells beyond the conventional single junction limit. Perhaps the largest obstacle to achieving this enhancement is uncertainty about energy coupling mechanisms at the interfaces between silicon and exciton fission materials such as tetracene. Here, the previously reported silicon-hafnium oxynitride-tetracene structure is studied and a combination of magnetic-field-dependent silicon photoluminescence measurements and density functional theory calculations is used to probe the influence of the interlayer composition on the triplet transfer process across the hafnium oxynitride interlayer. It is found that hafnium oxide interlayers do not show triplet exciton sensitization of silicon, and that nitrogen content in hafnium oxynitride layers is correlated with enhanced sensitization. Calculation results reveal that defects in hafnium oxynitride interlayers with higher nitrogen content introduce states close to the band-edge of silicon, which can mediate the triplet exciton transfer process. Some defects introduce additional deleterious mid-gap states, which may explain observed silicon photoluminescence quenching. These results show that band-edge states can mediate the triplet exciton transfer process, potentially through a sequential charge transfer mechanism.

cond-mat.mtrl-sci↗

arXiv2024

Closed Loop Superparamagnetic Tunnel Junctions for Reliable True Randomness and Generative Artificial Intelligence

Physical devices exhibiting stochastic functions with low energy consumption and high device density have the potential to enable complex probability-based computing algorithms, accelerate machine learning tasks, and enhance hardware security. Recently, superparamagnetic tunnel junctions (sMTJs) have been widely explored for such purposes, leading to the development of sMTJ-based systems; however, the reliance on nanoscale ferromagnets limits scalability and reliability, making sMTJs sensitive to external perturbations and prone to significant device variations. Here, we present an experimental demonstration of closed loop three-terminal sMTJs as reliable and potentially scalable sources of true randomness in the field-free regime. By leveraging dual-current controllability and incorporating feedback, we stabilize the switching operation of superparamagnets and reach cryptographic-quality random bitstreams. The realization of controllable and robust true random sMTJs underpin a general hardware platform for computing schemes exploiting the stochasticity in the physical world, as demonstrated by the generative artificial intelligence example in our experiment.

cond-mat.mtrl-sci↗

arXiv2024

Exciton Fission Enhanced Silicon Solar Cell

While silicon solar cells dominate global photovoltaic energy production, their continued improvement is hindered by the single junction limit. One potential solution is to use molecular singlet exciton fission to generate two electrons from each absorbed high-energy photon. We demonstrate that the long-standing challenge of coupling molecular excited states to silicon solar cells can be overcome using sequential charge transfer. Combining zinc phthalocyanine, aluminum oxide, and a shallow junction crystalline silicon microwire solar cell, the peak charge generation efficiency per photon absorbed in tetracene is (138 +- 6)%, comfortably surpassing the quantum efficiency limit for conventional silicon solar cells and establishing a new, scalable approach to low cost, high efficiency photovoltaics.

cond-mat.mtrl-sci↗

arXiv2019

Triplet-sensitization by lead halide perovskite thin films for near-infrared-to-visible upconversion

Lead halide-based perovskite thin films have attracted great attention due to the explosive increase in perovskite solar cell efficiencies. The same optoelectronic properties that make perovskites ideal absorber materials in solar cells are also beneficial in other light-harvesting applications and make them prime candidates as triplet sensitizers in upconversion via triplet-triplet annihilation in rubrene. In this contribution, we take advantage of long carrier lifetimes and carrier diffusion lengths in perovskite thin films, their high absorption cross sections throughout the visible spectrum, as well as the strong spin-orbit coupling owing to the abundance of heavy atoms to sensitize the upconverter rubrene. Employing bulk perovskite thin films as the absorber layer and spin-mixer in inorganic/organic heterojunction upconversion devices allows us to forego the additional tunneling barrier owing from the passivating ligands required for colloidal sensitizers. Our bilayer device exhibits an upconversion efficiency in excess of 3% under 785 nm illumination.

physics.app-ph↗

arXiv2016

Designing a Broadband Pump for High-Quality Micro-Lasers via Modified Net Radiation Method

High-quality micro-lasers are key ingredients in non-linear optics, communication, sensing and low-threshold solar-pumped lasers. However, such micro-lasers exhibit negligible absorption of free-space broadband pump light. Recently, this limitation was lifted by cascade energy transfer, in which the absorption and quality factor are modulated with wavelength, enabling non-resonant pumping of high-quality micro-lasers and solar-pumped laser to operate at record low solar concentration. Here, we present a generic theoretical framework for modeling the absorption, emission and energy transfer of incoherent radiation between cascade sensitizer and laser gain media. Our model is based on linear equations of the modified net radiation method and is therefore robust, fast converging and has low complexity. We apply this formalism to compute the optimal parameters of low-threshold solar-pumped lasers. It is revealed that the interplay between the absorption and self-absorption of such lasers defines the optimal pump absorption below the maximal value, which is in contrast to conventional lasers for which full pump absorption is desired. Numerical results are compared to experimental data on a sensitized Nd:YAG cavity, and quantitative agreement with theoretical models is found. Our work modularizes the gain and sensitizing components and paves the way for the optimal design of broadband-pumped high-quality micro-lasers and efficient solar-pumped lasers.

physics.optics↗

arXiv2015

Plexcitons: Dirac points and topological modes

Plexcitons are polaritonic modes that result from the strong coupling between excitons and plasmons. We consider plexcitons emerging from the interaction of excitons in an organic molecular layer with surface plasmons in a metallic film. We predict the emergence of Dirac cones in the two-dimensional bandstructure of plexcitons due to the inherent alignment of the excitonic transitions in the organic layer. These Dirac cones may open up in energy by simultaneously interfacing the metal with a magneto-optical layer and subjecting the whole system to a perpendicular magnetic field. The resulting energy gap becomes populated with topologically protected one-way modes which travel at the interface of this plexcitonic system. Our theoretical proposal suggests that plexcitons are a convenient and simple platform for the exploration of exotic phases of matter as well as of novel ways to direct energy flow at the nanoscale.

cond-mat.mes-hall↗

arXiv2015

360° Domain Walls: Stability, Magnetic Field and Electric Current Effects

The formation of 360° magnetic domain walls (360DWs) in Co and Ni80Fe20 thin film wires was demonstrated experimentally for different wire widths, by successively injecting two 180° domain walls (180DWs) into the wire. For narrow wires (less than 50 nm wide for Co), edge roughness prevented the combination of the 180DWs into a 360DW, and for wide wires (200 nm for Co) the 360DW collapsed, but over an intermediate range of wire widths, reproducible 360DW formation occurred. The annihilation and dissociation of 360DWs was demonstrated by applying a magnetic field parallel to the wire, showing that annihilation fields were several times higher than dissociation fields in agreement with micromagnetic modeling. The annihilation of a 360DW by current pulsing was demonstrated.

cond-mat.mes-hall↗

arXiv2013

Room temperature triplet state spectroscopy of organic semiconductors

Organic light emitting devices and solar cells are machines that create, manipulate and destroy excited states in organic semiconductors. It is crucial to characterize these excited states, or excitons, to optimize device performance in applications like displays and solar energy harvesting. This is complicated if the excited state is a triplet because the electronic transition is dark with a vanishing oscillator strength. As a consequence, triplet state spectroscopy must usually be performed at cryogenic temperatures to reduce competition from non-radiative rates. Here, we control non-radiative rates by engineering a solid-state host matrix containing the target molecule, allowing the observation of phosphorescence at room temperature and alleviating constraints of cryogenic experiments. We test these techniques on a wide range of materials with functionalities spanning multi-exciton generation (singlet exciton fission), organic light emitting device host materials, and thermally activated delayed fluorescence type emitters. Control of non-radiative modes in the matrix surrounding a target molecule may also have broader applications in light emitting and photovoltaic devices.

cond-mat.mtrl-sci↗

arXiv2013

Highly efficient, dual state emission from an organic semiconductor

We report highly efficient, simultaneous fluorescence and phosphorescence (74% yield) at room temperature from a single molecule ensemble of (BzP)PB dispersed into a polymer host. The slow phosphorescence (208 ms lifetime) is very efficient (50%) at room temperature and only possible because the non-radiative rate for the triplet state is extremely low. The ability of an organic molecule to function as an efficient dual state emitter at room temperature is unusual and opens new fields of applications including the use as broadband down-conversion emitters, optical sensors and attenuators, exciton probes, and spin-independent intermediates for Förster resonant energy transfer.

cond-mat.mtrl-sci↗