Andreev reflection and order parameter symmetry in heavy-fermion superconductors: the case of CeCoIn5_5

We review the current status of Andreev reflection spectroscopy on the heavy fermions, mostly focusing on the case of CeCoIn$_5$, a heavy-fermion superconductor with a critical temperature of 2.3 K. This is a well-established technique to investigate superconducting order parameters via measurements of the differential conductance from nanoscale metallic junctions. Andreev reflection is clearly observed in CeCoIn$_5$ as in other heavy-fermion superconductors. The measured Andreev signal is highly reduced to the order of maximum $\sim$ 13% compared to the theoretically predicted value (100%). Analysis of the conductance spectra using the extended BTK model provides a qualitative measure for the superconducting order parameter symmetry, which is determined to be $d_{x^2-y^2}$-wave in CeCoIn$_5$. A phenomenological model is proposed employing a Fano interference effect between two conductance channels in order to explain both the conductance asymmetry and the reduced Andreev signal. This model appears plausible not only because it provides good fits to the data but also because it is highly likely that the electrical conduction occurs via two channels, one into the heavy electron liquid and the other into the conduction electron continuum. Further experimental and theoretical investigations will shed new light on the mechanism of how the coherent heavy-electron liquid emerges out of the Kondo lattice, a prototypical strongly correlated electron system. Unresolved issues and future directions are also discussed.Comment: Topical Review published in JPCM (see below), 28 pages, 9 figure

Faceting of Single-Crystal SrTiO₃ During Wet Chemical Etching

AbstractWe use an Atomic Force Microscope (AFM) to study changes in the surface of single-crystal SrTiO3 etched in HF-based solutions. Attention in this work has been focused upon observations of pyramidal pitting – both because of an interest in avoiding etch pits during substrate preparation prior to heteroepitaxial growth, and because of an interest in micromachining this highly polarizable material. We note that (110) SrTiO3 is surprisingly robust against the formation of pits, while pitting is significant on {100} surfaces. Particular etch rates have been measured, and we discuss anisotropies in the rates of dissolution. These data are combined to extract a macroscopic model describing processes relevant to the most extreme pitting, which we show to be associated with surface defects.</jats:p

Visible-Light-Responsive Graphitic Carbon Nitride: Rational Design and Photocatalytic Applications for Water Treatment

Graphitic carbon nitride (g-C₃N₄) has recently emerged as a promising visible-light-responsive polymeric photocatalyst; however, a molecular-level understanding of material properties and its application for water purification were underexplored. In this study, we rationally designed nonmetal doped, supramolecule-based g-C₃N₄ with improved surface area and charge separation. Density functional theory (DFT) simulations indicated that carbon-doped g-C₃N₄ showed a thermodynamically stable structure, promoted charge separation, and had suitable energy levels of conduction and valence bands for photocatalytic oxidation compared to phosphorus-doped g-C₃N₄. The optimized carbon-doped, supramolecule-based g-C₃N₄ showed a reaction rate enhancement of 2.3–10.5-fold for the degradation of phenol and persistent organic micropollutants compared to that of conventional, melamine-based g-C₃N₄ in a model buffer system under the irradiation of simulated visible sunlight. Carbon-doping but not phosphorus-doping improved reactivity for contaminant degradation in agreement with DFT simulation results. Selective contaminant degradation was observed on g-C₃N₄, likely due to differences in reactive oxygen species production and/or contaminant-photocatalyst interfacial interactions on different g-C₃N₄ samples. Moreover, g-C₃N₄ is a robust photocatalyst for contaminant degradation in raw natural water and (partially) treated water and wastewater. In summary, DFT simulations are a viable tool to predict photocatalyst properties and oxidation performance for contaminant removal, and they guide the rational design, fabrication, and implementation of visible-light-responsive g-C₃N₄ for efficient, robust, and sustainable water treatment

Fullerene-encapsulated Cyclic Ozone for the Next Generation of Nano-sized Propellants via Quantum Computation

Cyclic ozone additives have the potential to significantly increase the specific impulse of rocket fuel, which would lead to greater efficiency and reduced costs for space launches, allowing up to one third more payload per rocket. Although practical attempts to capture this isomer have not been successful, cyclic ozone might be stabilized within confined geometries. However, the required synthetic methods are challenging to design and need theory-driven inputs that exceed the capabilities of classical methods. Quantum computation could enable these calculations, but the hardware requirements for many practical applications are still unclear. We provide a comprehensive analysis of how quantum methods could aid efforts to isolate cyclic ozone using fullerene encapsulation. Our discussion goes beyond formal complexity analysis, offering both logical and physical overhead estimates for determining ground state energies based on quantum phase estimation (QPE). Together, these data outline a plausible scale for realistic, computationally-assisted molecular design efforts using fault-tolerant quantum computation

Singlet Fission in Dideuterated Tetracene and Pentacene

AbstractThe impact of molecular vibrations on singlet fission, which is the spontaneous fission of a singlet exciton into two triplet excitons, is studied using ultrafast optical spectroscopy for the prototypical singlet fission chromophores tetracene and pentacene. We modify the frequency of intramolecular vibrations by deuteration, without impacting thin film structure and molecular arrangement, and study the resulting changes in exo‐ and endothermic singlet fission rates by comparing the deuterated and parent chromophores. We find that changes in the frequency of the C−C deformation modes of Δω=6 cm−1 and the occurrence of C−D vibrational modes do not lead to significant modifications in the singlet fission time constants. We conclude that the changes in the frequency of phonon modes induced by deuteration are too small to significantly impact the electron–phonon coupling that drives the singlet fission process