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At least 145 records · Page 8

Reconfigurable unitary transformations of optical beam arrays

Spatial transformations of light are ubiquitous in optics, with examples ranging from simple imaging with a lens to quantum and classical information processing in waveguide meshes. Multi-plane light converter (MPLC) systems have emerged as a platform that promises completely general spatial transformations, i.e., a universal unitary. However, until now, MPLC systems have demonstrated transformations that are far from general, e.g., converting from a Gaussian to Laguerre-Gauss mode. Here, we demonstrate the promise of an MLPC, the ability to impose an arbitrary unitary transformation that can be reconfigured dynamically. Specifically, we consider transformations on superpositions of parallel free-space beams arranged in an array, which is a common information encoding in photonics. We experimentally test the full gamut of unitary transformations for a system of two parallel beams and make a map of their fidelity. We obtain an average transformation fidelity of 0.85 ± 0.03. This high-fidelity suggests that MPLCs are a useful tool for implementing the unitary transformations that comprise quantum and classical information processing.

47 OTHER INSTRUMENTATION↗

An ultra-compact x-ray free-electron laser

In the field of beam physics, two frontier topics have taken center stage due to their potential to enable new approaches to discovery in a wide swath of science. These areas are: advanced, high gradient acceleration techniques, and x-ray free electron lasers (XFELs). Further, there is intense interest in the marriage of these two fields, with the goal of producing a very compact XFEL. In this context, recent advances in high gradient radio-frequency cryogenic copper structure research have opened the door to the use of surface electric fields between 250 and 500 MV m -1 . Such an approach is foreseen to enable a new generation of photoinjectors with six-dimensional beam brightness beyond the current state-of-the-art by well over an order of magnitude. This advance is an essential ingredient enabling an ultra-compact XFEL (UC-XFEL). In addition, one may accelerate these bright beams to GeV scale in less than 10 m. Such an injector, when combined with inverse free electron laser-based bunching techniques can produce multi-kA beams with unprecedented beam quality, quantified by 50 nm-rad normalized emittances. The emittance, we note, is the effective area in transverse phase space (x, p x /m e c) or (y, p y /m e c) occupied by the beam distribution, and it is relevant to achievable beam sizes as well as setting a limit on FEL wavelength. These beams, when injected into innovative, short-period (1–10 mm) undulators uniquely enable UC-XFELs having footprints consistent with university-scale laboratories. We describe the architecture and predicted performance of this novel light source, which promises photon production per pulse of a few percent of existing XFEL sources. We review implementation issues including collective beam effects, compact x-ray optics systems, and other relevant technical challenges. To illustrate the potential of such a light source to fundamentally change the current paradigm of XFELs with their limited access, we examine possible applications in biology, chemistry, materials, atomic physics, industry, and medicine—including the imaging of virus particles—which may profit from this new model of performing XFEL science.

47 OTHER INSTRUMENTATION↗

Experimental Evidence of Free Carrier Generation in 2D Hybrid Organic–Inorganic Perovskites

Despite the significant potential of 2D hybrid organic–inorganic perovskites (2DHOIPs) for high-efficiency optoelectronics application-comparable to their 3D counterparts, the fundamental carrier photogeneration remains unclear. In contrast to conventional ultrafast optical property characterization, we use ultrafast photocurrent spectroscopy to investigate the early-time electrical properties of type-I and type-II 2DHOIPs by manipulating the quantum confinement and the dielectric quantum matching effect. We discovered that the high frequency dielectric quantum matching effect plays a major role in 2DHOIPs, demonstrated by their high carrier mobility (µ), near-unity photogeneration quantum yield (Φ), below-room temperature exciton binding energy (E b ), and approaching 3D space factor (DSF). Our work shows that the optoelectronic performances of 2DHOIPs are comparable to their counterparts of 3DHOIPs.

2D perovskite↗

Long-Range Dipole–Dipole Interactions in a Plasmonic Lattice

Spontaneous emission of quantum emitters can be enhanced by increasing the local density of optical states, whereas engineering dipole-dipole interactions requires modifying the two-point spectral density function. Here, we experimentally demonstrate long-range dipole-dipole interactions (DDIs) mediated by surface lattice resonances in a plasmonic nanoparticle lattice. Using angle-resolved spectral measurements and fluorescence lifetime studies, we show that unique nanophotonic modes mediate long-range DDI between donor and acceptor molecules. We observe significant and persistent DDI strengths for a range of densities that map to similar to 800 nm mean nearest-neighbor separation distance between donor and acceptor dipoles, a factor of similar to 100 larger than free space. Here, our results pave the way to engineer and control long-range DDIs between an ensemble of emitters at room temperature.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Entangled two-plasmon generation in carbon nanotubes and graphene-coated wires

Here, we investigate the two-plasmon spontaneous decay of a quantum emitter near single-walled carbon nanotubes (SWCNTs) and graphene-coated wires (GCWs). We demonstrate efficient, enhanced generation of two-plasmon entangled states in SWCNTs due to the strong coupling between tunable guided plasmons and the quantum emitter. We predict two-plasmon emission rates more than twelve orders of magnitude higher than in free space, with average lifetimes of a few dozen nanoseconds. Given their low dimensionality, these systems could be more efficient for generating and detecting entangled plasmons in comparison to extended graphene. Indeed, we achieve a tunable spectrum of emission in GCWs, where sharp resonances occur precisely at the plasmons' minimum excitation frequencies. We show that by changing the material properties of the GCW's dielectric core, one could tailor the dominant modes and frequencies of the emitted entangled plasmons while keeping the decay rate ten orders of magnitude higher than in free space. By unveiling the unique properties of two-plasmon spontaneous emission processes in the presence of low-dimensional carbon-based nanomaterials, our findings set the basis for a novel material platform with applications to on-chip quantum information technologies.

36 MATERIALS SCIENCE↗

Robust finite-temperature many-body scarring on a quantum computer

Mechanisms for suppressing thermalization in disorder-free many-body systems, such as Hilbert space fragmentation and quantum many-body scars, have recently attracted much interest in foundations of quantum statistical physics and potential quantum information processing applications. However, their sensitivity to realistic effects such as finite temperature remains largely unexplored. Here, we have utilized IBM's Kolkata quantum processor to demonstrate an unexpected robustness of quantum many-body scars at finite temperatures when the system is prepared in a thermal Gibbs ensemble. We identify such robustness in the PXP model, which describes quantum many-body scars in experimental systems of Rydberg atom arrays and ultracold atoms in tilted Bose-Hubbard optical lattices. By contrast, other theoretical models which host exact quantum many-body scars are found to lack such robustness and their scarring properties quickly decay with temperature. Our study sheds light on the important differences between scarred models in terms of their algebraic structures, which impacts their resilience to finite temperature. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Celestial gluon amplitudes from the outside in

We show that, given a two-dimensional realization of the celestial OPE in self-dual Yang-Mills, we can find a scalar source around which scattering amplitudes replicate correlation functions computed from the 2D ‘gluon’ operators in a limit where a dynamic massless scalar decouples. We derive conditions on the two-dimensional three-point correlation function so that such a source exists and give two particular examples of this construction, one in which gluons are constructed from vertex operators in the semiclassical limit of Liouville theory and another in which the soft gluons arise from generalized free fields. Finally, we identify a bulk dual to the level of the boundary Kac-Moody algebra and discuss moving beyond the decoupling limit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Long-range cooperative resonances in rare-earth ion arrays inside photonic resonators

Engineering arrays of active optical centers to control the interaction Hamiltonian between light and matter has been the subject of intense research recently. Collective interaction of atomic arrays with optical photons can give rise to directionally enhanced absorption or emission, which enables engineering of broadband and strong atom-photon interfaces. Here, we report on the observation of long-range cooperative resonances in an array of rare-earth ions controllably implanted into a solid-state lithium niobate micro-ring resonator. We show that cooperative effects can be observed in an ordered ion array extended far beyond the light’s wavelength. We observe enhanced emission from both cavity-induced Purcell enhancement and array-induced collective resonances at cryogenic temperatures. Engineering collective resonances as a paradigm for enhanced light-matter interactions can enable suppression of free-space spontaneous emission. The multi-functionality of lithium niobate hosting rare-earth ions can open possibilities of quantum photonic device engineering for scalable and multiplexed quantum networks.

42 ENGINEERING↗

First-principles study of L -shell iron and chromium opacity at stellar interior temperatures

Recently developed free-energy density functional theory (DFT)-based methodology for optical property calculations of warm dense matter has been applied for studying L-shell opacity of iron and chromium at T = 182 eV. We use Mermin–Kohn–Sham density functional theory with a ground-state and a fully temperature-dependent generalized gradient approximation exchange-correlation (XC) functionals. It is demonstrated that the role of XC at such a high-T is negligible due to the total free-energy of interacting system being dominated by the noninteracting free-energy term in agreement with estimations for the homogeneous electron gas. Furthermore, our DFT predictions are compared to the radiative emissivity and opacity of dense plasmas model, to the real-space Greens function method, and to experimental measurements. Good agreement is found between all three theoretical methods, and in the bound–continuum region for Cr when compared to the experiment, while the discrepancy between direct DFT calculations and the experiment for Fe remains essentially the same as for plasma-physics models.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Vertical-cavity surface-emitting phase shifter

This study proposes a novel technique for a 2D beam steering system using hybrid plasmonic phase shifters with a cylindrical configuration in a 2D periodic array suitable for LIDAR applications. A nanoscale VCSEP design facilitates a sub-wavelength spacing between individual phase shifters, yielding an expanded field of view and side lobes suppression. The proposed design includes a highly doped sub-micron silicon pillar covered by a thin layer of nonlinear material and an additional conductive metal layer. Characterization of a single VCSEP demonstrated a Free Spectral Range (FSR) of 53.28 ± 2.5 nm and a transmission variation of 3 dB, with V π L equal to 0.075 V-mm.

47 OTHER INSTRUMENTATION↗

Experimental decoy-state Bennett-Brassard 1984 quantum key distribution through a turbulent channel

In free-space quantum key distribution (QKD) in turbulent conditions, scattering and beam wandering cause intensity fluctuations which decrease the detected signal-to-noise ratio. This effect can be mitigated by rejecting received bits when the channel's transmittance is below a threshold. Thus, the overall error rate is reduced and the secure key rate increases despite the deletion of bits. In this work, we implement recently proposed selection methods focusing on the prefixed-threshold real-time selection (P-RTS) where a cutoff can be chosen prior to data collection and independently of the transmittance distribution. We perform finite-size decoy-state Bennett-Brassard 1984 QKD in a laboratory setting where we simulate the atmospheric turbulence using an acousto-optical modulator. We show that P-RTS can yield considerably higher secure key rates for a wide range of the atmospheric channel parameters. In addition, we evaluate the performance of the P-RTS method for a realistically finite sample size. We demonstrate that a near-optimal selection threshold can be predetermined even with imperfect knowledge of the channel transmittance distribution parameters.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Engineering the radiative dynamics of thermalized excitons with metal interfaces

As a platform for optoelectronic devices based on exciton dynamics, monolayer transition metal dichalcogenides (TMDCs) are often placed near metal interfaces or inside planar cavities. While the radiative properties of point dipoles at metal interfaces has been studied extensively, those of excitons, which are delocalized and exhibit a temperature-dependent momentum distribution, lack a thorough treatment. Here, we analyze the emission properties of excitons in TMDCs near planar metal interfaces and explore their dependence on exciton center-of-mass momentum, transition dipole orientation, and temperature. Defining a characteristic energy scale k B T c = ($\hbar k$) 2 /2m (k being the radiative wavevector and m the exciton mass), we find that at temperatures T $\gg$ T c and low densities where the momentum distribution can be characterized by Maxwell-Boltzmann statistics, the modified emission rates (normalized to free space) behave similarly to point dipoles. This similarity in behavior arises due to the broad nature of wavevector components making up the exciton and point dipole emission. On the other hand, the narrow momentum distribution of excitons for T < T c can result in significantly different emission behavior as compared to point dipoles. These differences can be further amplified by considering excitons with a Bose Einstein distribution at high phase space densities, such as in a condensate phase. We find suppression or enhancement of emission relative to the point dipole case by several orders of magnitude. These insights can help optimize the performance of optoelectronic devices that incorporate 2D semiconductors near metal electrodes and can inform future studies of exciton radiative dynamics at low temperatures. Additionally, these studies show that nanoscale optical cavities are a viable pathway to generating long-lifetime exciton states in TMDCs.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Revealing Nanoscale Confinement Effects on Hyperbolic Phonon Polaritons with an Electron Beam

Hyperbolic phonon polaritons (HPhPs) in hexagonal boron nitride (hBN) enable the direct manipulation of mid-infrared light at nanometer scales, many orders of magnitude below the free-space light wavelength. High-resolution monochromated electron energy-loss spectroscopy (EELS) facilitates measurement of excitations with energies extending into the mid-infrared while maintaining nanoscale spatial resolution, making it ideal for detecting HPhPs. The electron beam is a precise source and probe of HPhPs, which allows the observation of nanoscale confinement in HPhP structures and directly extract hBN polariton dispersions for both modes in the bulk of the flake and modes along the edge. The measurements reveal technologically important nontrivial phenomena, such as localized polaritons induced by environmental heterogeneity, enhanced and suppressed excitation due to 2D interference, and strong modification of high-momenta excitations such as edge-confined polaritons by nanoscale heterogeneity on edge boundaries. Finally, the work opens exciting prospects for the design of real-world optical mid-infrared devices based on hyperbolic polaritons.

2D materials↗

Average nonlinear dynamics of particles in gravitational pulses: Effective Hamiltonian, secular acceleration, and gravitational susceptibility

Particles interacting with a prescribed quasimonochromatic gravitational wave (GW) exhibit secular (average) nonlinear dynamics that can be described by Hamilton’s equations. We derive the Hamiltonian of this “ponderomotive” dynamics to the second order in the GW amplitude for a general background metric. For the special case of vacuum GWs, we show that our Hamiltonian is equivalent to that of a free particle in an effective metric, which we calculate explicitly. We also show that already a linear GW pulse displaces a particle from its unperturbed trajectory by a finite distance that is independent of the GW phase and proportional to the integral of the pulse intensity.This effect is independent from the nonlinear memory effects that has been known. We calculate the particle displacement analytically and show that our result is in agreement with numerical simulations. We also show how the Hamiltonian of the nonlinear averaged dynamics naturally leads to the concept of the linear gravitational susceptibility of a particle gas with an arbitrary phase-space distribution. We calculate this susceptibility explicitly to apply it, in a follow-up paper, toward studying self-consistent GWs in inhomogeneous media within the geometrical-optics approximation

79 ASTRONOMY AND ASTROPHYSICS↗

Chemistry, Structure, and Function of Lone Pairs in Extended Solids

The lone pair has been a known feature of the electronic structure of molecules for over 100 years. Beginning with the pioneering work of Lewis and others that was later developed into useful guidelines for predicting molecular structure, lone pairs and their steric consequences are now taught at the very earliest stages of a chemistry education. In the crystalline solid state, lone pairs have perhaps had a less visible yet equally consequential role, with a significant impact on a range of properties and functionalities. Important properties associated with s 2 electron-derived lone pairs include their role in creating conditions favorable for ion transport, in the formation and correlation of local dipoles and the resulting polar behavior leading to ferroics and multiferroics, in increasing the refractive index of glass, in reducing the thermal conductivity of thermoelectric materials, and in breaking local symmetry permitting second-harmonic light generation.. In recent years, the role of the lone pair in developing the electronic structure of some topological quantum materials has also been recognized. While structural distortions due to lone pairs have traditionally been characterized through their crystallography, recent advances in scattering and spectroscopy have revealed the presence of local lone pair-driven distortions that do not correlate over long length scales. The role of these crystallographically “hidden” lone pairs, their detection, and their impact on properties have become a growing body of work in the literature. Hidden lone pairs are an effective argument for considering a role for lone pairs that goes beyond their being objects that occupy space in the coordination polyhedra of cations. This Account introduces the chemistry of lone pairs in extended crystalline solids, including a discussion of when they are stereochemically active, how they manifest in the structure, and how their chemistry can be tuned by the chemical environment around them. Eventually, all of these factors work in unison to help develop and tune properties of interest. Certain specific examples of structure–property relationships in materials that are driven by lone pair behavior are described here, including the potential impact of lone pairs on the optical and electronic properties of hybrid halide perovskite compounds that are relevant to their photovoltaic applications. Here, we highlight the role of lone pairs in the dielectric behavior of geometrically frustrated pyrochlores, the temperature-dependent optoelectronic behavior of halide perovskites, the polar phase transitions in lead-free ferroelectric perovskites, and the compositional insulator-to-metal transition in ruthenium pyrochlores. The theme underpinning this Account is that the lone pair can be considered to be a powerful design element for a broad range of material function.

36 MATERIALS SCIENCE↗

Structural Diversity and Magnetic Properties of Hybrid Ruthenium Halide Perovskites and Related Compounds

There has been a great deal of recent interest in extended compounds containing Ru 3+ and Ru 4+ in light of their range of unusual physical properties. Many of these properties are displayed in compounds with the perovskite and related structures. Here we report an array of structurally diverse hybrid ruthenium halide perovskites and related compounds: MA 2 RuX 6 (X=Cl or Br), MA 2 MRuX 6 (M=Na, K or Ag; X=Cl or Br) and MA 3 Ru 2 X 9 (X=Br) based upon the use of methylammonium (MA=CH 3 NH 3 + ) on the perovskite A site. The compounds MA 2 RuX 6 with Ru 4+ crystallize in the trigonal space group R3¯m and can be described as vacancy-ordered double-perovskites. The ordered compounds MA 2 MRuX 6 with M + and Ru 3+ crystallize in a structure related to BaNiO 3 with alternating MX 6 and RuX 6 face-shared octahedra forming linear chains in the trigonal P3¯m space group. The compound MA 3 Ru 2 Br 9 crystallizes in the orthorhombic Cmcm space group and displays pairs of face-sharing octahedra forming isolated Ru 2 Br 9 moieties with very short Ru–Ru contacts of 2.789 Å. The structural details, including the role of hydrogen bonding and dimensionality, as well as the optical and magnetic properties of these compounds are described. The magnetic behavior of all three classes of compounds is influenced by spin–orbit coupling and their temperature-dependent behavior has been compared with the predictions of the appropriate Kotani models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Deep-ultraviolet ptychographic pocket-scope (DART): mesoscale lensless molecular imaging with label-free spectroscopic contrast

The mesoscale characterization of biological specimens has traditionally required compromises between resolution, field-of-view, depth-of-field, and molecular specificity, with most approaches relying on external labels. Here we present the Deep-ultrAviolet ptychogRaphic pockeT-scope (DART), a handheld platform that transforms label-free molecular imaging through intrinsic deep-ultraviolet spectroscopic contrast. By leveraging biomolecules’ natural absorption fingerprints and combining them with lensless ptychographic microscopy, DART resolves down to 308-nm linewidths across centimeter-scale areas while maintaining millimeter-scale depth-of-field. The system’s virtual error-bin methodology effectively eliminates artifacts from limited temporal coherence and other optical imperfections, enabling high-fidelity molecular imaging without lenses. Through differential spectroscopic imaging at deep-ultraviolet wavelengths, DART quantitatively maps nucleic acid and protein distributions with femtogram sensitivity, providing an intrinsic basis for explainable virtual staining. We demonstrate DART’s capabilities through imaging of tissue sections, cytopathology specimens, blood cells, and neural populations, revealing detailed molecular contrast without external labels. The combination of high-resolution molecular mapping and broad mesoscale imaging in a portable platform opens new possibilities from rapid clinical diagnostics, tissue analysis, to biological characterization in space exploration.

60 APPLIED LIFE SCIENCES↗

N-Terminal Decarboxylation as a Probe for Intramolecular Contact Formation in $γ$-Glu-(Pro) n -Met Peptides

The kinetics of intramolecular-contact formation between remote functional groups in peptides with restricted conformational flexibility were examined using designed peptides with variable-length proline bridges. As probes for this motion, free radicals were produced using the • OH-induced oxidation at the C-terminal methionine residue of γ-Glu-(Pro) n -Met peptides ( n = 0–3). The progress of the radicals’ motion along the proline bridges was monitored as the radicals underwent reactions along the peptides’ backbones. Of particular interest was the reaction between the sulfur atom located in the side chain of the oxidized Met residue and the unprotonated amino group of the glutamic acid moiety. Interactions between them were probed by the radiation-chemical yields (expressed as G values) of the formation of C-centered, α-aminoalkyl radicals (αN) on the Glu residue. These radicals were monitored directly or via their reaction with p -nitroacetophenone (PNAP) to generate the optically detected PNAP •– radical anions. The yields of these αN radicals were found to be linearly dependent on the number of Pro residues. A constant decrease by 0.09 μM J –1 per spacing Pro residue of the radiation-chemical yields of G (αN) was observed. Previous reports support the conclusion that the αN radicals in these cases would have to result from (S$\therefore$N) + -bonded cyclic radical cations that arose as a result from direct contact between the ends of the peptides. Furthermore, by analogy with the rate constants for the formation of intramolecularly (S$\therefore$S) + -bonded radical cations in Met-(Pro) n -Met peptides ( J. Phys. Chem. B 2016 , 120 , 9732), the rate constants for the formation of intramolecularly (S$\therefore$N) + -bonded radical cations are activated to the same extent for all of the γ-Glu-(Pro) n -Met peptides. Thus, the continuous decrease of G (αN) with the number of Pro residues (from 0 to 3) suggests that the formation of a contact between the S-atom in the C-terminal Met residue and the N-atom of a deprotonated N-terminal amino group of Glu is controlled in peptides with 0 to 3 Pro residues by the relative diffusion of the S •+ and unoxidized N-atom. The overall rate constants of cyclization to form the (S$\therefore$N)-bonded radical cations were estimated to be 3.8 × 10 6 , 1.8 × 10 6 , and 8.1 × 10 5 s –1 for peptides with n = 0, 1, and 2 Pro residues, respectively. If activation is the same for all of the peptides, then these rate constants are a direct indication for the end-to-end dynamics along the chain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗