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At least 253 records · Page 14

Embedding PbS Quantum Dots (QDs) in Pb-Halide Perovskite Matrices: QD Surface Chemistry and Antisolvent Effects on QD Dispersion and Confinement Properties

Hybrid materials of metal chalcogenide colloidal quantum dots (QDs) embedded in metal halide perovskites (MHPs) have led to composites with synergistic properties. Here, we investigate how QD size, surface chemistry, and MHP film formation methods affect the resulting optoelectronic properties of QD/MHP “dot-in-matrix” systems. We monitor the QD absorption and photoluminescence throughout synthesis, ligand exchange, and transfer into the MHP ink, and we characterize the final QD/MHP films via electron microscopy and transient absorption. In addition, we are the first to globally map how PbS QDs are distributed on the micrometer scale within these dot-in-matrix systems, using three-dimensional (3D) tomography time-of-flight secondary ion mass spectrometry. The surface chemistry imparted during synthesis directly affects the optical properties of the dot-in-matrix composites. Pb-halide passivation leads to QD/MHP dot-in-matrix samples with optical properties that are well-described by a theoretical model, based on a Type I finite-barrier heterostructure between the PbS QD and the MHP matrix. Samples without Pb-halide passivation show complicated size-dependent behavior, indicating a transition from a Type I heterostructure between the PbS QD wells and MHP barriers for small-sized QDs to PbS QDs that are electronically decoupled from the MHP matrix for larger QDs. Furthermore, the choice in perovskite antisolvent crystallization method leads to a difference in the spatial QD distribution within the perovskite matrix, differences in carrier lifetime, and photoluminescence shifts of up to 180 meV for PbS in methylammonium lead iodide. This work establishes an understanding of such emerging synergistic systems relevant for technologies such as photovoltaics, infrared emitters and detectors, and other unexplored technological applications.

92 SC - Basic Energy Sciences (BES) (SC-22)↗

Enhanced quantum state transfer by circumventing quantum chaotic behavior

The ability to realize high-fidelity quantum communication is one of the many facets required to build generic quantum computing devices. In addition to quantum processing, sensing, and storage, transferring the resulting quantum states demands a careful design that finds no parallel in classical communication. Existing experimental demonstrations of quantum information transfer in solid-state quantum systems are largely confined to small chains with few qubits, often relying upon non-generic schemes. Here, by using a superconducting quantum circuit featuring thirty-six tunable qubits, accompanied by general optimization procedures deeply rooted in overcoming quantum chaotic behavior, we demonstrate a scalable protocol for transferring few-particle quantum states in a two-dimensional quantum network. These include single-qubit excitation, two-qubit entangled states, and two excitations for which many-body effects are present. Our approach, combined with the quantum circuit’s versatility, paves the way to short-distance quantum communication for connecting distributed quantum processors or registers, even if hampered by inherent imperfections in actual quantum devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Superluminescent diodes in the spectral range of 1.5 – 1.6 μm based on strain-compensated AlGaInAs/InP quantum wells

Superluminescent diodes based on AlGaInAs/InP separate-confinement double heterostructures with strain-compensated quantum wells are investigated. The influence of elastic strains in the active region on the output characteristics of the devices is analysed. It is shown that such a design of a superluminescent diode allows an optical power of more than 5 mW, a radiation spectrum width of more than 60 nm, a degree of output radiation polarisation up to 30 dB to be obtained at the output of a single-mode fibre, and has a great potential for further improvement. (paper)

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Achieving extreme light confinement in low-index dielectric resonators through quasi-bound states in the continuum

Obtaining large field enhancement in low-refractive-index dielectric materials is highly relevant to many photonic and quantum optics applications. However, confining light in these materials is challenging, owing to light leakage through coupling to continuum modes in the surrounding environment. Here, we investigate the possibility of achieving high quality factors in low-index dielectric resonators through the bound states in the continuum (BIC). Our simulations demonstrate that destructive interference between leaky modes can be achieved by tuning the geometrical parameters of the resonator arrays, leading to the emergence of quasi-BIC in resonators that have a small index contrast to the underlying substrates. The resultant large field enhancement gives rise to giant quality factors and Purcell effects. By introducing vertical mirror symmetry, the quasi-BIC can be tuned into an ideal BIC. In addition, the quasi-BIC can modify the emission patterns of the coupled emitters, rendering highly directional and focused far-field emission. These findings may provide a path for the practical implementation of photonic and quantum devices based on low-index dielectric materials.

42 ENGINEERING↗

Site-Controlled Quantum Emitters in Monolayer MoSe 2

Atomically thin semiconductors provide a highly attractive platform for quantum emitters (QEs): They can be combined with arbitrary substrates, can be spatially aligned with photonic structures, and can be electrically driven. All QEs reported to date in these materials have, however, relied on nominally spin-forbidden transitions, with radiative rates falling substantially below those of other solid-state QE systems. In this work, we employ strain confinement in monolayer MoSe 2 to produce engineered QEs, as confirmed in photon antibunching measurements. We discuss spin-allowed versus spin-forbidden transitions based on magneto- and time-resolved photoluminescence measurements. We calculate a radiative rate for spin-allowed quantum emission greater than 1 ns –1 , which exceeds reported radiative rates of WSe 2 QEs by 2 orders of magnitude.

2D materials↗

Electronic Probing and Manipulation of Low-Dimensional Magnets (Final Report)

We investigate the effects of reduced dimensionality of nanomagnets on the dynamical properties at low temperatures where quantum effects such as confinement, coherence, decoherence, and environmental coupling may be important. The experimental focus is on low-temperature transport measurements of such nanomagnets and cryogenic preamplification, followed by theoretical modeling of magnetic dynamics. In addition, we explore quantum effects in magnetic dynamics for their potential as quantum sensors of spin. We are particularly interested in the regime of strong environmental coupling, where novel phases of magnetic matter such as spin-boson may develop. The key new results are improved signal-to-noise ratio of magnetic tunneling junctions through low temperature preamplification that enables us to find the spin-dependent component of the current noise; a new powerful technique to simulate magnetic dynamics in the quantum coherent regime using the master equation formalism; and, finally, experimental hint of a novel state of matter in rare-earth doped permalloy ferromagnetic samples.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Perturbative stability of non-Abelian electric field solutions

We consider SU(2) gauge theory with a scalar field in the fundamental representation. The model is known to contain electric field solutions sourced by the scalar field that are distinct from embedded Maxwell electric fields. We examine the perturbative stability of the solution and identify a region of parameter space where the solution is stable. In the regime where the scalar field has a negative mass squared, the solution has two branches, and we identify an instability in one of the branches.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Collection of fluorescence from an ion using trap-integrated photonics

Spontaneously emitted photons are entangled with the electronic and nuclear degrees of freedom of the emitting atom, so interference and measurement of these photons can entangle separate matter-based quantum systems as a resource for quantum information processing. Since confinement in a single-mode facilitates the photon interference needed for generating entanglement, the dipole emission patterns relevant in spontaneous emission present a mode-matching challenge. Current demonstrations rely on bulk photon-collection and manipulation optics that suffer from large component size and system-to-system variability—factors that impede scaling to the large numbers of entangled pairs needed for quantum information processing. To address these limitations, we demonstrate a collection method that enables passive phase stability, straightforward photonic manipulation, and intrinsic reproducibility. Specifically, we engineer a waveguide-integrated grating to couple photons emitted from a trapped ion into a single optical mode within a microfabricated ion-trap chip. Using the integrated collection optic, we characterize the collection efficiency, image the ion, and detect the ion’s quantum state. The integrated optic covers 2.18% of the solid angle and collects 1.97 ± 0.3% of the spontaneously emitted light incident on the grating for a total collection efficiency of 0.043% into a single-mode waveguide. This proof-of-principle demonstration lays the foundation for leveraging the inherent stability and reproducibility of integrated photonics to create, manipulate, and measure multipartite quantum states in arrays of quantum emitters.

Optical physics↗

Single-photon superradiance in individual caesium lead halide quantum dots

The brightness of an emitter is ultimately described by Fermi’s golden rule, with a radiative rate proportional to its oscillator strength times the local density of photonic states. As the oscillator strength is an intrinsic material property, the quest for ever brighter emission has relied on the local density of photonic states engineering, using dielectric or plasmonic resonators. By contrast, a much less explored avenue is to boost the oscillator strength, and hence the emission rate, using a collective behaviour termed superradiance. Recently, it was proposed that the latter can be realized using the giant oscillator-strength transitions of a weakly confined exciton in a quantum well when its coherent motion extends over many unit cells. Here we demonstrate single-photon superradiance in perovskite quantum dots with a sub-100 picosecond radiative decay time, almost as short as the reported exciton coherence time. The characteristic dependence of radiative rates on the size, composition and temperature of the quantum dot suggests the formation of giant transition dipoles, as confirmed by effective-mass calculations. The results aid in the development of ultrabright, coherent quantum light sources and attest that quantum effects, for example, single-photon emission, persist in nanoparticles ten times larger than the exciton Bohr radius.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum real-time evolution of entanglement and hadronization in jet production: Lessons from the massive Schwinger model

The possible link between entanglement and thermalization, and the dynamics of hadronization are addressed by studying the real-time response of the massive Schwinger model coupled to external sources. This setup mimics the production and fragmentation of quark jets, as the Schwinger model and quantum chromodynamics (QCD) share the properties of confinement and chiral symmetry breaking. By using simulations of quantum dynamics on classical hardware, we study the entanglement between the produced jets, and observe the growth of the corresponding entanglement entropy in time. This growth arises from the increased number of contributing eigenstates of the reduced density matrix with sufficiently large and close eigenvalues. We also investigate the physical nature of these eigenstates, and find that at early times they correspond to fermionic Fock states. We then observe the transition from these fermionic Fock states to mesonlike bound states as a function of time. In other words, we observe how hadronization develops in real time. At late times, the local observables at midrapidity (such as the fermion density and the electric field) approach approximately constant values, suggesting the onset of equilibrium and approach to thermalization. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ultra-high aspect ratio pores milled in diamond via laser, ion and electron beam mediated processes

Microfabrication techniques are critical for the rapid prototyping and development of applications for cutting edge materials. Recently diamond has gained considerable interest for quantum photonic, biosensing, inertial confinement fusion and magnetometer applications. In this article, ultra-high aspect ratio milling of diamond micropores by photon, ion and electron based methods is reported. A multiphoton absorption laser ablation approach is revealed to rapidly produce sub-10 μm diameter micropores in diamond with an aspect ratio of 14:1 and a tapered profile at the surface interface. Chemically active, oxygen focused ion beam milling produces high-aspect ratio pores in diamond with an aspect ratio of 65:1 and minimal tapering over the length of the pore, overcoming the physical interaction volume limitations imposed in conventional gallium based focused ion beam milling and laser ablation methods. Oxygen-mediated electron beam induced etching is revealed to negate the limitations imposed by physical sputtering mechanisms utilized in focused ion beam milling via the direct initiation of chemical reactions at the receding surface, producing aspect ratios on the order of 200:1. Numerical simulations reveal the physical basis for the superior aspect-ratio pore milling of the oxygen focused ion beam milling and electron beam induced etching methods. Our results demonstrate direct-write methods for the fabrication of ultra-high aspect micropores in diamond and provide insight into the underlying mechanisms of these physical processes. The three methods demonstrated here can be interchanged for applications based on the desired characteristic aspect ratio and process throughput.

36 MATERIALS SCIENCE↗

Si/SiGe QuBus for single electron information-processing devices with memory and micron-scale connectivity function

The connectivity within single carrier information-processing devices requires transport and storage of single charge quanta. Single electrons have been adiabatically transported while confined to a moving quantum dot in short, all-electrical Si/SiGe shuttle device, called quantum bus (QuBus). Here we show a QuBus spanning a length of 10 μm and operated by only six simply-tunable voltage pulses. We introduce a characterization method, called shuttle-tomography, to benchmark the potential imperfections and local shuttle-fidelity of the QuBus. The fidelity of the single-electron shuttle across the full device and back (a total distance of 19 μm) is (99.7 ± 0.3) %. Using the QuBus, we position and detect up to 34 electrons and initialize a register of 34 quantum dots with arbitrarily chosen patterns of zero and single-electrons. The simple operation signals, compatibility with industry fabrication and low spin-environment-interaction in 28 Si/SiGe, promises long-range spin-conserving transport of spin qubits for quantum connectivity in quantum computing architectures.

97 MATHEMATICS AND COMPUTING↗

Improved Radiative Recombination in AlInGaP LEDs

Direct-emitting red and amber LEDs based on the AlInGaP material system offer a higher efficacy potential than phosphor-converted (pc) red and amber LEDs due to the absence of Stokes losses. Direct red LEDs (~610-620nm) are increasingly used in color-mixed and color-tunable illumination applications, where they have a significant advantage over pc-red LEDs, with high power conversion efficiency (PCE) and narrower emission enabling higher luminous efficacy of radiation (LER). Still, adoption is limited as the complexities associated with mixing different emitters offset the value of the efficacy gain. Adoption of direct amber LEDs (~580-595nm) in illumination applications is virtually non-existent due to their lower PCE and the availability of very efficient pc-amber emitters, which suffer less from Stokes loss and LER penalties associated with the broader bandwidth than pc-red. Further improvement in PCE of direct red and amber LEDs is needed to achieve wider adoption and ultimately enable more energy savings than possible with pc-LEDs. In this project, Lumileds has developed improved high-power amber and red LEDs incorporating tensile-strain barriers into the active region to improve carrier confinement and thereby increase external quantum efficiency (EQE). This approach is most beneficial for the short (amber) end of the AlInGaP wavelength range where carrier confinement is lowest. An EQE of 22% was achieved for amber LEDs, exceeding the project target of 20%

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Confinement, reduced entanglement, and spin-glass order in a random quantum spin-ice model

In this work, we study an effective spin model derived perturbatively from a random transverse-field Ising model on the pyrochlore lattice. The model consists of spin configurations on the pyrochlore lattice, restricted to the spin-ice subspace, with spins interacting with random Ising exchange couplings as well as ring exchanges along the hexagons of the lattice. This model is studied by exact diagonalization up to N=64 site systems. Furthermore, we calculate spin-glass correlation functions and local entanglement entropy S T between spins in a single tetrahedron and the rest of the system. We find that the model undergoes two phase transitions. At weak randomness the model is in a quantum spin-ice phase where S T =ln 6. Increasing randomness, at low transverse fields, first leads to a frozen phase, with long-range spin-glass order and S T =ln 2 corresponding to the Cat states associated with Ising order. Further increase in randomness leads to a random resonating-hexagon phase with a frozen backbone of spins and a broad distribution of entanglement entropies. The implications of these studies for non-Kramers rare-earth pyrochlores are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Single molecule tracking of bacterial cell surface cytochromes reveals dynamics that impact long-distance electron transport

Using a series of multiheme cytochromes, the metal-reducing bacterium Shewanella oneidensis MR-1 can perform extracellular electron transfer (EET) to respire redox-active surfaces, including minerals and electrodes outside the cell. While the role of multiheme cytochromes in transporting electrons across the cell wall is well established, these cytochromes were also recently found to facilitate long-distance (micrometer-scale) redox conduction along outer membranes and across multiple cells bridging electrodes. Recent studies proposed that long-distance conduction arises from the interplay of electron hopping and cytochrome diffusion, which allows collisions and electron exchange between cytochromes along membranes. However, the diffusive dynamics of the multiheme cytochromes have never been observed or quantified in vivo, making it difficult to assess their hypothesized contribution to the collision-exchange mechanism. Here, we use quantum dot labeling, total internal reflection fluorescence microscopy, and single-particle tracking to quantify the lateral diffusive dynamics of the outer membrane-associated decaheme cytochromes MtrC and OmcA, two key components of EET in S. oneidensis. We observe confined diffusion behavior for both quantum dot-labeled MtrC and OmcA along cell surfaces (diffusion coefficients D MtrC = 0.0192 ± 0.0018 µm 2 /s, D OmcA = 0.0125 ± 0.0024 µm 2 /s) and the membrane extensions thought to function as bacterial nanowires. We find that these dynamics can trace a path for electron transport via overlap of cytochrome trajectories, consistent with the long-distance conduction mechanism. The measured dynamics inform kinetic Monte Carlo simulations that combine direct electron hopping and redox molecule diffusion, revealing significant electron transport rates along cells and membrane nanowires.

59 BASIC BIOLOGICAL SCIENCES↗

Unconventional Hall response in the quantum limit of HfTe 5

Interacting electrons confined to their lowest Landau level in a high magnetic field can form a variety of correlated states, some of which manifest themselves in a Hall effect. Although such states have been predicted to occur in three-dimensional semimetals, a corresponding Hall response has not yet been experimentally observed. Here, we report the observation of an unconventional Hall response in the quantum limit of the bulk semimetal HfTe 5 , adjacent to the three-dimensional quantum Hall effect of a single electron band at low magnetic fields. The additional plateau-like feature in the Hall conductivity of the lowest Landau level is accompanied by a Shubnikov-de Haas minimum in the longitudinal electrical resistivity and its magnitude relates as 3/5 to the height of the last plateau of the three-dimensional quantum Hall effect. Our findings are consistent with strong electron-electron interactions, stabilizing an unconventional variant of the Hall effect in a three-dimensional material in the quantum limit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Valley-Tunable Even-Denominator Fractional Quantum Hall State in the Lowest Landau Level of an Anisotropic System

Fractional quantum Hall states (FQHSs) at even-denominator Landau level filling factors (v) are of prime interest as they are predicted to host exotic, topological states of matter. Here, we report here the observation of a FQHS at v = 1/2 in a two-dimensional electron system of exceptionally high quality, confined to a wide AlAs quantum well, where the electrons can occupy multiple conduction-band valleys with an anisotropic effective mass. The anisotropy and multivalley degree of freedom offer an unprecedented tunability of the v = 1/2 FQHS as we can control both the valley occupancy via the application of in-plane strain, and the ratio between the strengths of the short- and long-range Coulomb interaction by tilting the sample in the magnetic field to change the electron charge distribution. Thanks to this tunability, we observe phase transitions from a compressible Fermi liquid to an incompressible FQHS and then to an insulating phase as a function of tilt angle. We find that this evolution and the energy gap of the v = 1/2 FQHS depend strongly on valley occupancy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Conditional quantum plasmonic sensing

The possibility of using weak optical signals to perform sensing of delicate samples constitutes one of the main goals of quantum photonic sensing. Furthermore, the nanoscale confinement of electromagnetic near fields in photonic platforms through surface plasmon polaritons has motivated the development of highly sensitive quantum plasmonic sensors. Despite the enormous potential of plasmonic platforms for sensing, this class of sensors is ultimately limited by the quantum statistical fluctuations of surface plasmons. Indeed, the fluctuations of the electromagnetic field severely limit the performance of quantum plasmonic sensing platforms in which delicate samples are characterized using weak near-field signals. Furthermore, the inherent losses associated with plasmonic fields levy additional constraints that challenge the realization of sensitivities beyond the shot-noise limit. Here, we introduce a protocol for quantum plasmonic sensing based on the conditional detection of plasmons. We demonstrate that the conditional detection of plasmonic fields, via plasmon subtraction, provides a new degree of freedom to control quantum fluctuations of plasmonic fields. This mechanism enables improvement of the signal-to-noise ratio of photonic sensors relying on plasmonic signals that are comparable to their associated field fluctuations. Consequently, the possibility of using weak plasmonic signals to sense delicate samples, while preserving the sample properties, has important implications for molecule sensing, and chemical detection.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗