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At least 1,369 records · Page 76

Conversion of Classical Light Emission from a Nanoparticle‐Strained WSe 2 Monolayer into Quantum Light Emission via Electron Beam Irradiation

Abstract Solid‐state single photon emitters (SPEs) within atomically thin transition metal dichalcogenides (TMDs) have recently attracted interest as scalable quantum light sources for quantum photonic technologies. Among TMDs, WSe 2 monolayers (MLs) are promising for the deterministic fabrication and engineering of SPEs using local strain fields. The ability to reliably produce isolatable SPEs in WSe 2 is currently impeded by the presence of numerous spectrally overlapping states that occur at strained locations. Here nanoparticle (NP) arrays with precisely defined positions and sizes are employed to deterministically create strain fields in WSe 2 MLs, thus enabling the systematic investigation and control of SPE formation. Using this platform, electron beam irradiation at NP‐strained locations transforms spectrally overlapped sub‐bandgap emission states into isolatable, anti‐bunched quantum emitters. The dependence of the emission spectra of WSe 2 MLs as a function of strain magnitude and exposure time to electron beam irradiation is quantified and provides insight into the mechanism for SPE production. Excitons selectively funnel through strongly coupled sub‐bandgap states introduced by electron beam irradiation, which suppresses spectrally overlapping emission pathways and leads to measurable anti‐bunched behavior. The findings provide a strategy to generate isolatable SPEs in 2D materials with a well‐defined energy range.

2D material↗

Spin Emitters beyond the Point Dipole Approximation in Nanomagnonic Cavities

Control over transition rates between spin states of emitters is crucial in a wide variety of fields ranging from quantum information science to the nanochemistry of free radicals. We present an approach to drive both electric and magnetic dipole-forbidden transitions of a spin emitter by placing it in a nanomagnonic cavity, requiring a description of both the spin emitter beyond the point dipole approximation and the vacuum magnetic fields of the nanomagnonic cavity with a large spatial gradient over the volume of the spin emitter. We specifically study the silicon vacancy (SiV – ) defect in diamond, whose Zeemansplit ground states comprise a logical qubit for solid-state quantum information processing, coupled to a magnetic nanoparticle serving as a model nanomagnonic cavity capable of concentrating microwave magnetic fields into deeply subwavelength volumes. Through first-principles modeling of the SiV – spin orbitals, we calculate the spin transition densities of magnetic dipole-allowed and -forbidden transitions and calculate their coupling rates to various multipolar modes of the nanomagnonic cavity. We envision using such a framework for manipulation of quantum spin states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Spectrochemical Series for Electron Spin Relaxation

Controlling the rate of electron spin relaxation in paramagnetic molecules is essential for contemporary applications in molecular magnetism and quantum information science. However, the physical mechanisms of spin relaxation remain incompletely understood, and new spectroscopic observables play an important role in evaluating spin dynamics mechanisms and structure–property relationships. Here, we use cryogenic magnetic circular dichroism (MCD) spectroscopy and pulse electron paramagnetic resonance (EPR) in tandem to examine the impact of ligand field (d–d) excited states on spin relaxation rates. We employ a broad scope of square-planar Cu(II) compounds with varying ligand field strength, including CuS 4 , CuN 4 , CuN 2 O 2 , and CuO 4 first coordination spheres. An unexpectedly strong correlation exists between spin relaxation rates and the average d–d excitation energy (R 2 = 0.97). The relaxation rate trends as the inverse 11th power of the excited-state energies, whereas simplified theoretical models predict only an inverse second power dependence. These experimental results directly implicate ligand field excited states as playing a critical role in the ground-state spin relaxation mechanism. Furthermore, ligand field strength is revealed to be a particularly powerful design principle for spin dynamics, enabling formation of a spectrochemical series for spin relaxation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Engineering chirality at wafer scale with ordered carbon nanotube architectures

Creating artificial matter with controllable chirality in a simple and scalable manner brings new opportunities to diverse areas. Here we show two such methods based on controlled vacuum filtration - twist stacking and mechanical rotation - for fabricating wafer-scale chiral architectures of ordered carbon nanotubes (CNTs) with tunable and large circular dichroism (CD). By controlling the stacking angle and handedness in the twist-stacking approach, we maximize the CD response and achieve a high deep-ultraviolet ellipticity of 40 ± 1 mdeg nm -1 . Our theoretical simulations using the transfer matrix method reproduce the experimentally observed CD spectra and further predict that an optimized film of twist-stacked CNTs can exhibit an ellipticity as high as 150 mdeg nm -1 , corresponding to a g factor of 0.22. Furthermore, the mechanical rotation method not only accelerates the fabrication of twisted structures but also produces both chiralities simultaneously in a single sample, in a single run, and in a controllable manner. The created wafer-scale objects represent an alternative type of synthetic chiral matter consisting of ordered quantum wires whose macroscopic properties are governed by nanoscopic electronic signatures and can be used to explore chiral phenomena and develop chiral photonic and optoelectronic devices.

36 MATERIALS SCIENCE↗

Tri-molybdenum phosphide (Mo 3 P) and multi-walled carbon nanotube junctions for volatile organic compounds (VOCs) detection

Detection and analysis of volatile organic compounds' (VOCs) biomarkers lead to improvement in healthcare diagnosis and other applications such as chemical threat detection and food quality control. Here, we report on tri-molybdenum phosphide (Mo3P) and multiwalled carbon nanotube (MWCNT) junction-based vapor quantum resistive sensors (vQRSs), which exhibit more than one order of magnitude higher sensitivity and superior selectivity for biomarkers in comparison to pristine MWCNT junctions based vQRSs. Transmission electron microscope/scanning tunneling electron microscope with energy dispersive x-ray spectroscopy, x-ray diffraction, and x-ray photoelectron spectroscopy studies reveal the crystallinity and the presence of Mo and P elements in the network. The presence of Mo3P clearly enhanced the performance of vQRS as evidenced in sensitivity and selectivity studies. The vQRSs are stable over extended periods of time and are reproducible, making them a potential candidate for sensing related applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnon-mediated qubit coupling determined via dissipation measurements

Controlled interaction between localized and delocalized solid-state spin systems offers a compelling platform for on-chip quantum information processing with quantum spintronics. Hybrid quantum systems (HQSs) of localized nitrogen-vacancy (NV) centers in diamond and delocalized magnon modes in ferrimagnets—systems with naturally commensurate energies—have recently attracted significant attention, especially for interconnecting isolated spin qubits at length-scales far beyond those set by the dipolar coupling. However, despite extensive theoretical efforts, there is a lack of experimental characterization of the magnon-mediated interaction between NV centers, which is necessary to develop such hybrid quantum architectures. Here, we experimentally determine the magnon-mediated NV–NV coupling from the magnon-induced self-energy of NV centers. Our results are quantitatively consistent with a model in which the NV center is coupled to magnons by dipolar interactions. This work provides a versatile tool to characterize HQSs in the absence of strong coupling, informing future efforts to engineer entangled solid-state systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structure and electronic tunability of acene alkylamine based layered hybrid organic-inorganic perovskites from first principles

Twelve layered hybrid organic-inorganic perovskites combining oligoacene derivatives [phenylmethylammonium (PMA), naphthylmethylammonium (NMA), anthrylmethylammonium (AMA), and tetrylmethylammonium (TMA)] and lead halides (Cl - , Br - , and I - anions) are investigated by first-principles density functional theory (DFT), showing broad, rational tunability of band gap, quantum well type, and spin-dependent energy band properties. Six compounds are known from previous syntheses and are used to devise a computational search space for likely low-energy structures. Among the six known compounds, a refined structure is identified for (NMA) 2 ⁢ PbCl 4 and a new, lower-energy structure is suggested for (AMA) 2 ⁢PbCl 4 . The DFT based search methodology is next applied to predict the likely structures for the six unknown compounds. Computationally predicted energy levels for all 12 compounds from spin-orbit coupled hybrid DFT reveal tunable type I quantum well alignments, with frontier orbitals located on the inorganic component, on the organic component, or on both, as controlled by cation and anion selection. In conclusion, several structures spontaneously break local and global inversion symmetry, causing strong spin splitting of the conduction bands [up to 0.12 eV for (PMA) 2 ⁢PbCl 4 ] and showing potential for spin-dependent transport properties and future spintronic and tunable chiroptical applications.

36 MATERIALS SCIENCE↗

Flexoelectricity and New Phenomena

It is easy to miss the scientific implications of our recent work on Triboelectricity. Everyone knows that rubbing and contact can produce static electricity; less appreciated is that the thermodynamic driver has been an open question since static electricity was first observed by Thales of Miletus around 585 BC. People think they understand it, for instance one common explanation that can still be found in the current literature is that differences in the work function drives charge transfer, often called the Volta-Helmholtz hypothesis. As summarized in 1967 by Harper, this fails to explain many experimental observations, for instance that charging can occur when two pieces of the same material are rubbed against each other. We are the first to place triboelectricity on a solid foundation rooted in quantum mechanics – the flexoelectric effect. We were able to explain a significant number of previously unexplained phenomena: 1) Bipolar tribocurrents associated with stick-slip, due to the change in sign of the strain gradients. 2) A one-third power scaling of tribocurrents with indentation force. 3) Tribocharging when two identical materials are used, these being due to local variations in the asperities so there are usually local potential differences. 4) Inhomogeneous charging of insulators, related to the statistical nature of asperities. 5) An experimentally observed reversal in the sign of charge transfer for negative and positive curvature, which is related to a change in the sign of the strain gradient. Exploiting our DOE prior funded work on flexoelectricity, we obtained semi-quantitative matching to existing experimental measurements of the surface charge in triboelectric experiments. The work has been well received in the literature. The work has been the focus of a number of popular science press articles, and also formed the basis for a Podcast for children 6-10 “The Rise and Fall of Static Man” posted in December 2019 by NPR as part of their “Wow in the World” series. I was also briefly interviewed by the Chicago PBS station in January 2020. This work are significant for a wide range of energy applications; to quote from an independent source: "Triboelectric power has plenty of potential, says Wenzhuo Wu, an assistant professor of engineering at Purdue. If the basics of static electricity are better understood, we could maximize the efficiency of wind or wave power generators, Wu says. The body's own movement could be used to power internal medical devices. Imagine being able to create a roof shaped to harness the power of a raindrop — the friction of the rain passing over the surface — to generate triboelectricity, powering the building below it." This is the start of new science, some of which we already partially understand such as the role of band bending in charge transfer. We need to understand charge transfer combining elasticity, quantum mechanics, band bending and defect states. These directly involve several of the DOE Grand Challenges: "How do we control material processes at the level of electrons? How do remarkable properties of matter emerge from complex correlations of the atomic or electronic constituents and how can we control these properties? How do we characterize and control matter away—especially very far away— from equilibrium?" I will argue that this work truly falls into the class of disruptive science; it is not just a simple extension, linear science. Not everyone will accept the approach. Since we explain far more about triboelectricity than anyone before, the preponderance of evidence supports the model. The feedback I have received is that many agree with the work, to quote: "The model makes sense, says Michael McAlpine, a professor of engineering at the University of Minnesota. "It's such a simple explanation, I was surprised I didn't put my finger on that," McAlpine says." The proposal received strong reviews. It was also publicized on the Department of Energy Web Site.

16 TIDAL AND WAVE POWER↗

Erbium quantum memory platform with long optical coherence via back-end-of-line deposition on foundry-fabricated photonics

Realizing scalable quantum interconnects necessitates the integration of solid-state quantum memories with foundry photonics processes. While prior photonic integration efforts have relied upon specialized, laboratory-scale fabrication techniques, this work demonstrates the monolithic integration of a quantum memory platform with low-loss foundry photonic circuits via back-end-of-line deposition. We deposited thin films of titanium dioxide (Ti⁢O 2 ) doped with erbium (Er) onto silicon nitride nanophotonic waveguides and studied Er optical coherence at subkelvin temperatures with photon echo techniques. Furthermore, we suppressed optical dephasing through ex-situ oxygen annealing and optimized measurement conditions, which yielded an optical coherence time of 64 μ⁢s (a 5-kHz homogeneous linewidth) and slow spectral diffusion of 27 kHz over 4 ms, results that are comparable to state-of-the-art Er nanophotonic devices. Combined with second-long electron spin lifetimes and demonstrated electrical control of Er emission, our findings establish Er:Ti⁢O 2 on foundry photonics as a manufacturable platform for ensemble and single-ion quantum memories.

Electro-optic effects↗

Many-Electron System on Helium and Color Center Spectroscopy

Electrons on the helium surface display sharp resonant absorption lines related to the transitions between the subbands of quantized motion transverse to the surface. A magnetic field parallel to the surface strongly affects the absorption spectrum.We show that the effect results from admixing the intersubband transitions to the in-plane quantum dynamics of the strongly correlated electron liquid or a Wigner crystal. This is similar to the admixing of electron transitions in color centers to phonons. Furthermore, the spectrum permits a direct characterization of the many-electron dynamics and also enables testing the theory of color centers in a system with controllable coupling.

36 MATERIALS SCIENCE↗

Controlled Organization of Inorganic Materials Using Biological Molecules for Activating Therapeutic Functionalities

Precise control over the assembly of biocompatible three-dimensional (3D) nanostructures would allow for programmed interactions within the cellular environment. Nucleic acids can be used as programmable crosslinkers to direct the assembly of quantum dots (QDs) and tuned to demonstrate different interparticle binding strategies. In this work, morphologies of self-assembled QDs are evaluated via gel electrophoresis, transmission electron microscopy, small-angle X-ray scattering, and dissipative particle dynamics simulations, with all results being in good agreement. The controlled assembly of 3D QD organizations is demonstrated in cells via the colocalized emission of multiple assembled QDs, and their immunorecognition is assessed via enzyme-linked immunosorbent assays. RNA interference inducers are also embedded into the interparticle binding strategy to be released in human cells only upon QD assembly, which is demonstrated by specific gene silencing. The programmability and intracellular activity of QD assemblies offer a strategy for nucleic acids to imbue the structure and therapeutic function into the formation of complex networks of nanostructures, while the photoluminescent properties of the material allow for optical tracking in cells in vitro.

36 MATERIALS SCIENCE↗

Dancing the Quantum Waltz: Compiling Three-Qubit Gates on Four Level Architectures

Superconducting quantum devices are a leading technology for quantum computation, but they face several challenges. Gate errors, coherence errors and a lack of connectivity all contribute to low fidelity results. In particular, connectivity restrictions enforce a gate set that requires three-qubit gates to be decomposed into one- or two-qubit gates. This substantially increases the number of two-qubit gates that need to be executed. However, many quantum devices have access to higher energy levels. We can expand the qubit abstraction of |0〉 and |1〉 to a ququart which has access to the |2〉 and |3〉 state, but with shorter coherence times. This allows for two qubits to be encoded in one ququart, enabling increased virtual connectivity between physical units from two adjacent qubits to four fully connected qubits. This connectivity scheme allows us to more efficiently execute three-qubit gates natively between two physical devices.We present direct-to-pulse implementations of several three-qubit gates, synthesized via optimal control, for compilation of three-qubit gates onto a superconducting-based architecture with access to four-level devices with the first experimental demonstration of four-level ququart gates designed through optimal control. We demonstrate strategies that temporarily use higher level states to perform Toffoli gates and always use higher level states to improve fidelities for quantum circuits. We find that these methods improve expected fidelities with increases of 2x across circuit sizes using intermediate encoding, and increases of 3x for fully-encoded ququart compilation.

Litteken, Andrew↗

Quantum random number generator

A system and method are provided to yield a QRNG based on homodyne detection of quantum noise (e.g., vacuum noise measured as shot noise) generated from a local oscillator, such as an LED. In one embodiment, a QRNG may be provided that is adjustable based on a control input to produce a random output that can be translated to one or more random data bits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum defects in carbon nanotubes as single-photon sources

Single-photon emitters are essential components of emerging quantum technologies, including secure communication and quantum computing. Single-walled carbon nanotubes (SWCNTs) have emerged as a promising platform for quantum light sources due to their quasi-one-dimensional excitonic host structure and compatibility with telecom photonic systems. Recent advances in deterministic defect engineering—most notably the development of organic color centers (OCCs)—have enabled stable, chemically controllable, and spectrally tunable single-photon emission. OCC-based emitters have demonstrated single-photon purity exceeding 99% and, more recently, room-temperature photon indistinguishability, placing them among the few solid-state systems with quantum-grade performance under ambient conditions. This review surveys progress in the field from three complementary perspectives: chemical synthesis and quantum defect engineering, computational studies of structure-property relationships and excitonic behavior, and experimental investigations of quantum optical properties. We also discuss alternative approaches, including air-suspended SWCNTs and hybrid van der Waals heterostructures, highlighting opportunities and open challenges for scalable integration into quantum photonic platforms.

36 MATERIALS SCIENCE↗

Biasing topological charge injection in topological matter

Here we explore the interplay between topologies in the momentum and real spaces to formulate a thermodynamic description of nonequilibrium injection of topological charges under external bias. We show that the edge modes engendered by the momentum-space topology can play a functional role of connecting the external reservoirs to the bulk transport of topological charges in the real space. We illustrate our general results with two examples: the spin-torque injection of skyrmions in an electrically biased integer quantum Hall system, and the vortex injection in a topological $p + ip$ superconductor coupled to heat reservoirs. Based on the universal fractional entropy of the Majorana zero modes bound to the vortices, their controllable injection proposed in this work could provide a route for creating and manipulating Majorana fermions.

36 MATERIALS SCIENCE↗

Submonolayer Quantum Dot Infrared Photodetector

A method has been developed for inserting submonolayer (SML) quantum dots (QDs) or SML QD stacks, instead of conventional Stranski-Krastanov (S-K) QDs, into the active region of intersubband photodetectors. A typical configuration would be InAs SML QDs embedded in thin layers of GaAs, surrounded by AlGaAs barriers. Here, the GaAs and the AlGaAs have nearly the same lattice constant, while InAs has a larger lattice constant. In QD infrared photodetector, the important quantization directions are in the plane perpendicular to the normal incidence radiation. In-plane quantization is what enables the absorption of normal incidence radiation. The height of the S-K QD controls the positions of the quantized energy levels, but is not critically important to the desired normal incidence absorption properties. The SML QD or SML QD stack configurations give more control of the structure grown, retains normal incidence absorption properties, and decreases the strain build-up to allow thicker active layers for higher quantum efficiency.

Ting, David Z.↗

Unveiling horizons in quantum critical collapse

Critical gravitational collapse offers a unique window into regimes of arbitrarily high curvature, culminating in a naked singularity arising from smooth initial data — thus providing a dynamical counterexample to weak cosmic censorship. Near the critical regime, quantum effects from the collapsing matter are expected to intervene before full quantum gravity resolves the singularity. Despite its fundamental significance, a self-consistent treatment has so far remained elusive. In this work, we perform a one-loop semiclassical analysis using the robust anomaly-based method in the canonical setup of Einstein gravity minimally coupled to a free, massless scalar field. Focusing on explicitly solvable near-critical solutions in both 2 + 1 and 3 + 1 dimensions, we analytically solve the semiclassical Einstein equations and obtain controlled, quantitative results for several long-standing questions within the dominant s-wave sector. We find that regularity uniquely selects a Boulware-like quantum state, encoding genuine vacuum polarization effects from the collapsing matter. Remarkably, the resulting quantum corrections manifest as a growing mode. Horizon-tracing analyses, incorporating both classical and quantum modes, reveal the emergence of a finite mass gap, signaling a phase transition from classical Type II to quantum-modified Type I behavior, thereby providing a quantum enforcement of the weak cosmic censorship. The most non-trivial aspect of our analysis involves dealing with non-conformal matter fields in explicitly time-dependent critical spacetimes. Along the way, we uncover intriguing and previously underexplored features of quantum field theory in curved spacetime.

2D Gravity↗

Decorrelated singlet and triplet exciton delocalization in acetylene-bridged Zn-porphyrin dimers

The controlled delocalization of molecular excitons remains an important goal towards the application of organic chromophores in processes ranging from light-initiated chemical transformations to classical and quantum information processing. In this study, we present a methodology to couple optical and magnetic spectroscopic techniques and assess the delocalization of singlet and triplet excitons in model molecular chromophores. By comparing the steady-state and time-resolved optical spectra of Zn-porphyrin monomers and weakly coupled dimers, we show that we can use the identity of substituents bound at specific positions of the macromolecules' rings to control the inter-ring delocalization of singlet excitons stemming from their B states through acetylene bridges. While broadened steady-state absorption spectra suggest the presence of delocalized B state excitons in mesityl-substituted Zn-tetraphenyl porphyrin dimers (Zn 2 U-D), we confirm this conclusion by measuring an enhanced ultrafast non-radiative relaxation from these inter-ring excitonic states to lower lying electronic states relative to their monomer. In contrast to the delocalized nature of singlet excitons, we use time-resolved EPR and ENDOR spectroscopies to show that the triplet states of the Zn-porphyrin dimers remain localized on one of the two macrocyclic sub-units. We use the analysis of EPR and ENDOR measurements on unmetallated model porphyrin monomers and dimers to support this conclusion. The results of DFT calculations also support the interpretation of localized triplet states. These results demonstrate researchers cannot conclude triplet excitons delocalize in macromolecular based on the presence of spatially extended singlet excitons, which can help in the design of chromophores for application in spin conversion and information processing technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗