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At least 289 records · Page 16

Frenkel excitons in heat-stressed supramolecular nanocomposites enabled by tunable cage-like scaffolding

Delocalized Frenkel excitons—coherently shared excitations among chromophores—are responsible for the remarkable efficiency of supramolecular light-harvesting assemblies within photosynthetic organisms. The translation of nature’s design principles to applications in optoelectronic devices has been limited by the fragility of the supramolecular structures used and the delicate nature of Frenkel excitons, particularly under mildly changing solvent conditions and elevated temperatures and upon deposition onto solid substrates. Here, we overcome those functionalization barriers through composition of stable supramolecular light-harvesting nanotubes enabled by tunable (~4.3–4.9 nm), uniform (±0.3 nm) cage-like scaffolds. High-resolution cryogenic electron microscopy, combined with scanning electron microscopy, broadband femtosecond transient absorption spectroscopy and near-field scanning optical microscopy revealed that excitons within the cage-like scaffolds are robust, even under extreme heat stress, and control over nanocomposite dimensions is maintained on solid substrates. Our bio-inspired nanocomposites provide a general framework for the development of next-generation organic devices made from stable supramolecular materials.

14 SOLAR ENERGY↗

Active galactic nucleus feedback in NGC 3982

The energetic feedback from supermassive black holes can influence star formation at the centres of galaxies. Observational evidence for active galactic nucleus (AGN) impact on star formation can be searched for in galaxies by combining ultraviolet imaging and optical integral field unit data. The ultraviolet flux directly traces recent star formation, and the integral field unit data can reveal dust attenuation, gas ionisation mechanisms, and gas kinematics from the central regions of the galaxy disk. A pilot study on NGC 3982 shows star formation suppression in the central regions of the galaxy, likely due to negative AGN feedback, and enhanced star formation in the outer regions. The case of NGC 3982 could be observational evidence of AGN feedback operating in a Seyfert galaxy.

79 ASTRONOMY AND ASTROPHYSICS↗

Non-uniform longitudinal current density induced power saturation in GaAs-based high power diode lasers

The output power of modern 975 nm GaAs-based broad area diode lasers is limited by increasing carrier and photon losses at high bias. Here, we use experiment and one-dimensional calculations on these devices to reveal that higher current densities (and hence higher local recombination rates and higher losses) arise near the front facet due to spatial hole burning and that the non-uniformity is strongly affected by laser geometry, which is more severe for longer resonators and less severe for higher front facet reflectivity. Specifically, we use devices with a segmented p-contact to directly measure the current distribution along the resonator and compare this with laser simulation. Devices with a 6 mm resonator show 29% more current at the front than back, twice as large as the 15% current non-uniformity in devices with a 3 mm resonator. In contrast, increased front facet reflectivity (20% rather than 0.8%) is shown to almost halve the current non-uniformity from 29% to 18% in devices with a 6 mm resonator and reduces power saturation. Although the magnitude of current non-uniformity in experiment and theory is broadly consistent, in experiment, an additional divergence is seen in current flow (and hence recombination rate) near the facets, and earlier power saturation occurs. Finally, we discuss the possible saturation mechanisms that are not included in the simulation.

47 OTHER INSTRUMENTATION↗

Ultrafast valley polarization in bilayer graphene

We study theoretically the interaction of a bilayer graphene with a circularly polarized ultrafast optical pulse of a single oscillation at an oblique incidence. The normal component of the pulse breaks the inversion symmetry of the system and opens up a dynamical bandgap due to which a valley-selective population of the conduction band becomes sensitive to the angle of incident of the pulse. We show that the magnitude of the valley polarization can be controlled by the angle of incidence, the amplitude, and the angle of in-plane polarization of the chiral optical pulse. Subsequently, a sequence of a circularly polarized pulse followed by a linearly polarized femtosecond-long pulse can be used to control and probe the valley polarization created by the preceding pulse. Our protocol provides a favorable platform to design ultrafast all-optical valleytronic information processing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Diagnosing the pedestal magnetic field and magnetohydrodynamics radial structure with pedestal–scrape of layer electron cyclotron emission radiation inversion in H-mode plasma (invited)

Forward modeling is used to interpret inversion patterns of the pedestal–Scrape of Layer (SOL) Electron Cyclotron Emission (ECE) in DIII-D H-mode experiments. The modeling not only significantly improves the ECE data interpretation quality but also leads to the potential measurements of (1) the magnetic field strength |B| at the separatrix, (2) the pedestal |B| evolution during an inter-Edge Localized Mode (ELM) period, and (3) the pedestal Magnetohydrodynamics (MHD) radial structure. The ECE shine-through effect leads to three types of pedestal–SOL radiation inversions that are discussed in this paper. The first type of inversion is the non-monotonic T e,rad profile with respect to the major radius. Using the ECE frequency at the minimum T e,rad , the inversion can be applied to measure the magnetic field |B| at the separatrix and calibrate the mapping of the ECE channels with respect to the separatrix. The second type of inversion refers to the opposite phase between the radiation fluctuations δT e,rad at the pedestal and SOL. This δT e,rad phase inversion is sensitive to density and temperature fluctuations at the pedestal foot and, thus, can be used to qualitatively measure the MHD radial structure. The third type of inversion appears when the pedestal and SOL T e,rad evolve in an opposite trend, which can be used to infer the pedestal |B| field change during an inter-ELM period. Finally, the bandwidth effect on measuring δT e,rad due to pedestal MHD is also investigated in the radiation modeling.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Lightwave-driven electron emission for polarity-sensitive terahertz beam profiling

The full exploitation of advanced light sources in the terahertz (THz) frequency range requires versatile experimental tools to fully characterize the spatial, temporal, and spectral shapes of the THz electric field. Several techniques for passive THz beam profiling exist that offer information about the temporally integrated intensity. Thus, any information about the electric field itself is lost. Here, we show that a UV–visible light emission produced via a lightwave-driven field emission from single-layer metasurfaces can be used to visualize the peak electric field distribution of THz beams in real time. Our technique is scalable up to frequencies approaching the plasma frequency of the metal used for the metasurface. Uniquely, our device is sensitive to the absolute polarity of the THz lightwave. These findings demonstrate a general pathway to designing metamaterial-based field-sensitive optical detectors suitable for the entire THz and IR spectral region.

42 ENGINEERING↗

Tailoring light-induced charge transfer and intersystem crossing in FeCO using time-dependent spin–orbit configuration interaction

Real-time (RT) electronic structure methods provide a natural framework for describing light–matter interactions in arbitrary time-dependent electromagnetic fields (EMF). Optically induced excited state transitions are of particular interest, which require tuned EMF to drive population transfer to and from the specific state(s) of interest. Intersystem crossing, or spin-flip, may be driven through shaped EMF or laser pulses. These transitions can result in long-lived “spin-trapped” excited states, which are especially useful for materials requiring charge separation or protracted excited state lifetimes. Time-dependent configuration interaction (TDCI) is unique among RT methods in that it may be implemented in a basis of eigenstates, allowing for rapid propagation of the time-dependent Schrödinger equation. The recent spin–orbit TDCI (TD-SOCI) enables a real-time description of spin-flip dynamics in an arbitrary EMF and, therefore, provides an ideal framework for rational pulse design. The present study explores the mechanism of multiple spin-flip pathways for a model transition metal complex, FeCO, using shaped pulses designed to drive controlled intersystem crossing and charge transfer. These results show that extremely tunable excited state dynamics can be achieved by considering the dipole transition matrix elements between the states of interest.

Chemistry↗

Manipulation of Localized Excitons in CrPS4 by Temperature and Magnetic Field

Layered van der Waals magnetic semiconductors provide a versatile platform for exploring excitonic phenomena intertwined with spin and lattice degrees of freedom, enabling excitons to act as sensitive probes of magnetic order. CrPS4 is a layered antiferromagnetic semiconductor that hosts rich excitonic features whose microscopic origin and connection to magnetic ordering remain incompletely understood. Here, we investigate the electronic and excitonic properties of bulk CrPS4 using a combination of many-body perturbation theory, dynamical mean-field theory, and photoluminescence-based experiments. Our calculations establish CrPS4 as a direct-gap semiconductor with a bandgap of 2.48 eV in the antiferromagnetic phase. Several subbandgap excitonic transitions are predicted by theory, comprising multiple spin-allowed excitons and an additional spin-flip excitation, predominantly localized on the Cr3+ ions. Temperature- and magnetic-field-dependent optical measurements reveal thermally driven exciton redistribution among localized states and identify characteristic energy shifts that provide clear optical signatures of magnetic phase transitions in CrPS4. These results provide insights into the excitonic transitions of antiferromagnets and suggest potential routes for all-optical sensing and light-driven control of their magnetic order.

2D materials↗

The metallicity’s fundamental dependence on both local and global galactic quantities

ABSTRACT We study the scaling relations between gas-phase metallicity, stellar mass surface density (Σ*), star formation rate surface density (ΣSFR), and molecular gas surface density ($\Sigma _{{\rm H}_2}$) in local star-forming galaxies on scales of a kpc. We employ optical integral field spectroscopy from the Mapping Nearby Galaxies at Apache Point Observatory (MaNGA) survey, and ALMA data for a subset of MaNGA galaxies. We use partial correlation coefficients and Random Forest regression to determine the relative importance of local and global galactic properties in setting the gas-phase metallicity. We find that the local metallicity depends primarily on Σ* (the resolved mass–metallicity relation, rMZR), and has a secondary anticorrelation with ΣSFR (i.e. a spatially resolved version of the ‘Fundamental Metallicity Relation’, rFMR). We find that $\Sigma _{{\rm H}_2}$ is less important than ΣSFR in determining the local metallicity. This result indicates that gas accretion, resulting in local metallicity dilution and local boosting of star formation, is unlikely to be the primary origin of the rFMR. The local metallicity depends also on the global properties of galaxies. We find a strong dependence on the total stellar mass (M*) and a weaker (inverse) dependence on the total SFR. The global metallicity scaling relations, therefore, do not simply stem out of their resolved counterparts; global properties and processes, such as the global gravitational potential well, galaxy-scale winds and global redistribution/mixing of metals, likely contribute to the local metallicity, in addition to local production and retention.

79 ASTRONOMY AND ASTROPHYSICS↗

Superconducting coherence peak in near-field radiative heat transfer

Enhancement and peaks in near-field radiative heat transfer (NFRHT) typically arise due to surface phonon-polaritons, plasmon-polaritons, and electromagnetic (EM) modes in structured materials. However, the role of material quantum coherence in enhancing near-field radiative heat transfer remains unexplored. Here, we unravel that NFRHT in superconductor-ferromagnetic systems displays a unique peak at the superconducting phase transition that originates from the quantum coherence of Bogoliubov quasiparticles in superconductors. Our theory takes into account evanescent EM radiation emanating from fluctuating currents related to Cooper pairs and Bogoliubov quasiparticles in stark contrast to the current-current correlations induced by free electrons in conventional materials. Our proposed NFRHT configuration exploits ferromagnetic resonance at frequencies deep inside the superconducting band gap to isolate this superconducting coherence peak. Furthermore, we reveal that Cooper pairs and Bogoliubov quasiparticles have opposite effects on near-field thermal radiation and isolate their effects on many-body radiative heat transfer near superconductors. As a result, our proposed phenomenon can have applications for developing thermal isolators and heat sinks in superconducting circuits.

Dipole approximation↗

Minimally entangled state preparation of localized wave functions on quantum computers

Initializing a single site of a lattice scalar field theory into an arbitrary state with support throughout the quantum register requires $O(2^{nQ})$ entangling gates on a quantum computer with $n_Q$ qubits per site. It is conceivable that instead initializing to functions that are good approximations to states may have utility in reducing the number of required entangling gates. In the case of a single site of a noninteracting scalar field theory, initializing to a symmetric exponential wave function requires $n_Q – 1$ entangling gates, the minimal number necessary to create an entangled state of all $n_Q$ qubits. This is compared with the $2^{nQ – 1} + n_Q – 3 + δ_{nQ, 1}$ required for a symmetric Gaussian wave function. In this work, we explore the initialization of one-site $(n_Q = 4)$, two-site $(n_Q = 3)$, and three-site ( n Q = 3 ) noninteracting scalar field theories with symmetric exponential wave functions using IBM's quantum simulators and quantum devices (Poughkeepsie and Tokyo). With the digitizations attainable with $n_Q = 3,4$, these tensor-product wave functions are found to have large overlap with a Gaussian wave function and provide a suitable low-noise initialization for improvement and Somma inflation. Further, in performing these simulations, we have employed a workflow that interleaves calibrations to mitigate systematic errors in production. The calibrations allow tolerance cuts on gate performance including the fidelity of the symmetrizing Hadamard gate, both in vacuum $(|\textbf{0}\gg^{\bigotimes nQ})$ and in medium ($n_Q –1$ qubits initialized to an exponential function). The results obtained in this work are relevant to systems beyond scalar field theories, such as the deuteron radial wave function, two- and three-dimensional Cartesian-space wave functions, and nonrelativistic multinucleon systems built on a localized eigenbasis.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Exact two-body expansion of the many-particle wave function

Progress toward the solution of the strongly correlated electron problem has been stymied by the exponential complexity of the wave function. Previous work established an exact two-body exponential product expansion for the ground-state wave function. By developing a reduced density-matrix analog of Dalgarno-Lewis perturbation theory, we prove here that (i) the two-body exponential product expansion is rapidly and globally convergent with each operator representing an order of a renormalized perturbation theory, (ii) the energy of the expansion converges quadratically near the solution, and (iii) the expansion is exact for both ground and excited states. The two-body expansion offers a reduced parametrization of the many-particle wave function as well as the two-particle reduced density matrix with potential applications on both conventional and quantum computers for the study of strongly correlated quantum systems. In this work, we demonstrate the result with the exact solution of the contracted Schrödinger equation for the molecular chains H 4 and H 5 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Imaging ring-current wave packets in the helium atom

We study the reconstruction of a wave packet and the corresponding electron dynamics in an atom via photoelectron angular distributions (PADs) in a pump-probe scheme as a function of time delay. The method is applied to the superposition of ground and one or two excited states in helium atom representing field-free charge migrations on the attosecond timescale in form of ring currents around the core. It is based on the interference between one- and two-photon transitions from ground and excited states into the continuum. In the reconstruction predictions of first- and second-order perturbation theory are used to determine the unknown phases and amplitudes from the PADs, which we simulate via solutions of the time-dependent Schrödinger equation in single-active-electron approximation. Results of calculations show that the reconstruction technique works well for peak laser intensities less than 10 13 W/cm 2 . Knowledge of the electric field of the probe pulse is required with shot-to-shot variations of carrier-to-envelope phase and peak intensity of up to 10% and 20%, respectively. The relevance of different one- and two-photon pathways for the reconstruction as a function of peak intensity and pulse duration is analyzed—specifically their role for ultrashort probe pulses with broad bandwidths.

74 ATOMIC AND MOLECULAR PHYSICS↗

Quantum states of cylindrical surface charge density for modeling plasmonic circuit elements: Nanowires, nanorods, cavities, and waveguides

Nanostructures in the form of ellipsoids, prolate spheroids, rings, and cylinders are known to exhibit resonant surface and cavity modes with applications in nanophotonics and plasmonics and, more recently, in novel quantum experiments, in which control of plasmons and their interactions with plasmons, photons, phonons, excitons, and quantum emitters are desired. Nanorods and nanowires are examples of plasmonic structures with spectral properties of potential use as interconnects and circuit components. Additionally, estimates of the surface properties of these components are needed in circuit design and integrated systems. Here, we present a quantum Hamiltonian for the cylindrical surface charge density. We then study the photon excitation of plasmons on the cylindrical surface and calculate their scattering and radiative decay rate. Nonradiative decay of plasmons induces an efficient heating of the nanoparticle and can photoacoustically excite mechanical oscillations. Computational calculations are also presented for the plasmonic modes and the ensuing excitations of nanomechanical eigenmodes of nanoparticles with near-cylindrical symmetries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strong-field ionization of plasmonic nanoparticles

We modeled strong-field ionization of metal nanoparticles by intense infrared laser pulses, accounting for and distinguishing in photoelectron (PE) momentum distributions the effects of PE correlation, PE–residual-charge interactions, PE rescattering and recombination, and transient laser-induced plasmonic fields. Our numerical results for 5-, 30-, and 70-nm-diameter gold nanospheres and peak laser-pulse intensities of 8.0×10 12 and 1.2×10 13 W/cm 2 show how PE velocity-map images are distinctly shaped by PE Coulomb repulsion, residual-charge accumulations, and plasmonic near fields. In contrast to gaseous atomic targets and dielectric nanoparticles, we find very large PE cutoff energies, for both directly emitted and rescattered PEs, that exceed the incident laser-pulse ponderomotive energy by two orders of magnitude.

74 ATOMIC AND MOLECULAR PHYSICS↗

Variational Self-Consistent Theory for Beam-Loaded Cavities

A new variational theory is presented for beam loading in microwave cavities. The beam{field interaction is formulated as a dynamical interaction whose stationarity according to Hamilton’s principle will naturally lead to steady-state solutions that indicate how a cavity’s resonant frequency, Q and optimal coupling coefficient will detune as a result of the beam loading. A driven cavity Lagrangian is derived from first principles, including the effects of cavity wall losses, input power and beam interaction. The general formulation is applied to a typical klystron input cavity to predict the appropriate detuning parameters required to maximize the gain (or modulation depth) in the average Lorentz factor boost, (Δ γ). Numerical examples are presented, showing agreement with the general detuning trends previously observed in the literature. The developed formulation carries several advantages for beam-loaded cavity structures. It provides a self-consistent model for the dynamical (nonlinear) beam{field interaction, a procedure for maximizing gain under beam-loading conditions, and a useful set of parameters to guide cavity-shape optimization during the design of beam-loaded systems. Enhanced clarity of the physical picture underlying the problem seems to be gained using this approach, allowing straightforward inclusion or exclusion of different field configurations in the calculation and expressing the final results in terms of measurable quantities. Two field configurations are discussed for the klystron input cavity, using finite magnetic confinement or no confinement at all. Formulating the problem in a language that is directly accessible to the powerful techniques found in Hamiltonian dynamics and canonical transformations may potentially carry an additional advantage in terms of analytical computational gains, under suitable conditions

43 PARTICLE ACCELERATORS↗

Thermodynamics of Light Management in Near-Field Thermophotovoltaics

We evaluate near-field thermophotovoltaic (TPV) energy-conversion systems focusing in particular on their open-circuit voltage (V OC ). Unlike previous analyses based largely on numerical simulations with fluctuational electrodynamics, here, we develop an analytic model that captures the physics of near-field TPV systems and can predict their performance metrics. Using our model, we identify two opportunities of TPV systems operating in the near field. First, we show analytically that enhancement of radiative recombination is a natural consequence of operating in the near field. Second, we note that, owing to photon recycling and minimal radiation leakage in near-field operation, the PV cell used in near-field TPV systems can be much thinner compared to those used in solar PV systems. Since nonradiative recombination is a volumetric effect, use of a thinner cell reduces nonradiative losses per unit area. The combination of these two opportunities leads to increasingly large values of V OC as the TPV vacuum gap decreases. Hence, although operation in the near-field was previously perceived to be beneficial for electrical power-density enhancement, here, we emphasize that thin-film near-field TPVs are also significantly advantageous in terms of V OC and consequently conversion efficiency as well as power density. We provide numerical results for an InAs-based thin-film TPV that exhibits efficiency >50% at an emitter temperature as low as 1100 K.

42 ENGINEERING↗