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Abstract The potential energy landscape (PEL) formalism is a powerful tool within statistical mechanics to study the thermodynamic properties of classical low-temperature liquids and glasses. Recently, the PEL formalism has been extended to liquids/glasses that obey quantum mechanics, but applications have been limited to atomistic model liquids. In this work, we extend the PEL formalism to liquid/glassy water using path-integral molecular dynamics (PIMD) simulations, where nuclear quantum effects (NQE) are included. Our PIMD simulations, based on the q-TIP4P/F water model, show that the PEL of quantum water is both Gaussian and anharmonic. Importantly, the ring-polymers associated to the O/H atoms in the PIMD simulations, collapse at the local minima of the PEL (inherent structures, IS) for both liquid and glassy states. This allows us to calculate, analytically, the IS vibrational density of states (IS-VDOS) of the ring-polymer system using the IS-VDOS of classical water (obtained from classical MD simulations). The role of NQE on the structural properties of liquid/glassy water at various pressures are discussed in detail. Overall, our results demonstrate that the PEL formalism can effectively describe the behavior of molecular liquids at low temperatures and in the glass states, regardless of whether the liquid/glass obeys classical or quantum mechanics. 

Abstract The challenge of fabricating transparent and conductive (T/C) films and patterns for applications in flexible electronics, touch screens, solar cells, and smart windows remains largely unsolved. Traditional fabrication techniques are complex, costly, time‐consuming, and struggle to achieve the necessary precision and accuracy over electronic and optical properties. Here, hypersurface photolithography (HP), which integrates microfluidics, a digital micromirror device, and photochemical surface‐initiated polymerizations is used to create polymer brush patterns. The high‐throughput optimization enabled by HP provides conditions to fabricate patterns composed of cross‐linked polymer brushes containing Au‐binding 2‐vinylpyrrolidine (2VP) groups with precise control over the height and the composition at each pixel. Au nanoparticles (AuNPs) are incorporated into the polymer brush patterns through in situ reduction of Au ions, resulting in T/C composite AuNP/polymer brush patterns. The sheet resistance at 100 mA of a 2VP‐AuNP‐functionalized patterns on a glass substrate is 0.42 Ω sq⁻¹with 86% transmittance of visible light. Additional patterns demonstrate multiplexing by copatterning rhodamine B functionalized fluorescent polymer brushes and AuNP/polymer brush conductive domains. This work solves the challenge of creating T/C films by forming metal‐polymer composites from polymer brush patterns, offering a scalable solution for electronic and optical device development and fabrication. 

Abstract Establishing connections between material impurities and charge transport properties in emerging electronic and quantum materials, such as wide‐bandgap semiconductors, demands new diagnostic methods tailored to these unique systems. Many such materials host optically‐active defect centers which offer a powerful in situ characterization system, but one that typically relies on the weak spin‐electric field coupling to measure electronic phenomena. In this work, charge‐state sensitive optical microscopy is combined with photoelectric detection of an array of nitrogen‐vacancy (NV) centers to directly image the flow of charge carriers inside a diamond optoelectronic device, in 3D and with temporal resolution. Optical control is used to change the charge state of background impurities inside the diamond on‐demand, resulting in drastically different current flow such as filamentary channels nucleating from specific, defective regions of the device. Conducting channels that control carrier flow, key steps toward optically reconfigurable, wide‐bandgap optoelectronics are then engineered using light. This work might be extended to probe other wide‐bandgap semiconductors (SiC, GaN) relevant to present and emerging electronic and quantum technologies. 

Abstract Amorphous ices are usually classified as belonging to low-density or high-density amorphous ice (LDA and HDA) with densitiesρ_LDA ≈ 0.94 g/cm³andρ_HDA ≈ 1.15−1.17 g/cm³. However, a recent experiment crushing hexagonal ice (ball-milling) produced amedium-density amorphous ice (MDA,ρ_MDA ≈ 1.06 g/cm³) adding complexity to our understanding of amorphous ice and the phase diagram of supercooled water. Motivated by the discovery of MDA, we perform computer simulations where amorphous ices are produced by isobaric cooling and isothermal compression/decompression. Our results show that, depending on the pressure employed, isobaric cooling can generate a continuum of amorphous ices with densities that expand in between those of LDA and HDA (briefly, intermediate amorphous ices, IA). In particular, the IA generated atP ≈ 125 MPa has a remarkably similar density and average structure as MDA, implying that MDA is not unique. Using the potential energy landscape formalism, we provide an intuitive qualitative understanding of the nature of LDA, HDA, and the IA generated at different pressures. In this view, LDA and HDA occupy specific and well-separated regions of the PEL; the IA prepared atP = 125 MPa is located in the intermediate region of the PEL that separates LDA and HDA. 

Abstract The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV⁰to SiV^‐transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV^‒, on the other hand, yields only fractional recombination into SiV^2‒, a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms. 

Abstract Extending the coherence lifetime of a qubit is central to the implementation and deployment of quantum technologies, particularly in the solid state where various noise sources intrinsic to the material host play a limiting role. This study examines theoretically the coherent spin dynamics of a hetero‐spin system formed by a spin featuring a non‐zero crystal field and in proximity to a paramagnetic center . An analysis of the energy level structure of the dyad shows this system exhibits apair of levels separated by a magnetic‐field‐insensitive energy gap, which can be exploited to create long‐lived zero‐quantum coherences. It is found that these coherences are selectively sensitive to “local”—as opposed to “global”—magnetic field fluctuations, suggesting these spin dyads can serve as a nanoscale gradiometer for precision magnetometry. On the other hand, the distinct response of either spin species to electric or thermal stimuli allows one to implement alternative sensing protocols for magnetic‐noise‐free electrometry and thermometry. 

Abstract Coherent control and manipulation of quantum degrees of freedom such as spins forms the basis of emerging quantum technologies. In this context, the robust valley degree of freedom and the associated valley pseudospin found in two‐dimensional transition metal dichalcogenides is a highly attractive platform. Valley polarization and coherent superposition of valley states have been observed in these systems even up to room temperature. Control of valley coherence is an important building block for the implementation of valley qubit. Large magnetic fields or high‐power lasers have been used in the past to demonstrate the control (initialization and rotation) of the valley coherent states. Here, the control of layer–valley coherence via strong coupling of valley excitons in bilayer WS₂to microcavity photons is demonstrated by exploiting the pseudomagnetic field arising in optical cavities owing to the transverse electric–transverse magnetic (TE–TM)mode splitting. The use of photonic structures to generate pseudomagnetic fields which can be used to manipulate exciton‐polaritons presents an attractive approach to control optical responses without the need for large magnets or high‐intensity optical pump powers. 

Abstract The surface states of 3D topological insulators in general have negligible quantum oscillations (QOs) when the chemical potential is tuned to the Dirac points. In contrast, we find that topological Kondo insulators (TKIs) can support surface states with an arbitrarily large Fermi surface (FS) when the chemical potential is pinned to the Dirac point. We illustrate that these FSs give rise to finite-frequency QOs, which can become comparable to the extremal area of the unhybridized bulk bands. We show that this occurs when the crystal symmetry is lowered from cubic to tetragonal in a minimal two-orbital model. We label such surface modes as ‘shadow surface states’. Moreover, we show that the sufficient next-nearest neighbor out-of-plane hybridization leading to shadow surface states can be self-consistently stabilized for tetragonal TKIs. Consequently, shadow surface states provide an important example of high-frequency QOs beyond the context of cubic TKIs. 

Abstract Hydrogen, the smallest and most abundant element in nature, can be efficiently incorporated within a solid and drastically modify its electronic and structural state. In most semiconductors interstitial hydrogen binds to defects and is known to be amphoteric, namely it can act either as a donor (H⁺) or an acceptor (H⁻) of charge, nearly always counteracting the prevailing conductivity type. Here we demonstrate that hydrogenation resolves an outstanding challenge in chalcogenide classes of three-dimensional (3D) topological insulators and magnets — the control of intrinsic bulk conduction that denies access to quantum surface transport, imposing severe thickness limits on the bulk. With electrons donated by a reversible binding of H⁺ions to Te(Se) chalcogens, carrier densities are reduced by over 10²⁰cm⁻³, allowing tuning the Fermi level into the bulk bandgap to enter surface/edge current channels without altering carrier mobility or the bandstructure. The hydrogen-tuned topological nanostructures are stable at room temperature and tunable disregarding bulk size, opening a breadth of device platforms for harnessing emergent topological states. 

Abstract We report a novel glycan array architecture that binds the mannose‐specific glycan binding protein, concanavalin A (ConA), with sub‐femtomolar avidity. A new radical photopolymerization developed specifically for this application combines the grafted‐from thiol–(meth)acrylate polymerization with thiol–ene chemistry to graft glycans to the growing polymer brushes. The propagation of the brushes was studied by carrying out this grafted‐to/grafted‐from radical photopolymerization (GTGFRP) at >400 different conditions using hypersurface photolithography, a printing strategy that substantially accelerates reaction discovery and optimization on surfaces. The effect of brush height and the grafting density of mannosides on the binding of ConA to the brushes was studied systematically, and we found that multivalent and cooperative binding account for the unprecedented sensitivity of the GTGFRP brushes. This study further demonstrates the ease with which new chemistry can be tailored for an application as a result of the advantages of hypersurface photolithography.