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At least 955 records · Page 53

Towards higher frequencies in a compact prebunched waveguide THz-FEL

Free-electron-lasers fill a critical gap in the space of THz-sources as they can reach high average and peak powers with spectral tunability. Using a waveguide in a THz FEL significantly increases the coupling between the relativistic electrons and electromagnetic field enabling large amounts of radiation to be generated in a single passage of electrons through the undulator. In addition to transversely confining the radiation, the dispersive properties of the waveguide critically affect the velocity and slippage of the radiation pulse which determine the central frequency and bandwidth of the generated radiation. In this paper, we characterize the spectral properties of a compact waveguide THz FEL including simultaneous lasing at two different frequencies and demonstrating tuning of the radiation wavelength in the high frequency branch by varying the beam energy and ensuring that the electrons injected into the undulator are prebunched on the scale of the resonant radiation wavelength.

Experimental particle physics↗

Purcell enhancement of directional edge photocurrent in a van der Waals self-cavity

Cavities provide a means to manipulate the optical and electronic responses of quantum materials by selectively enhancing light-matter interaction at specific frequencies and momenta. While cavities typically involve external structures, exfoliated flakes of van der Waals (vdW) materials can form intrinsic self-cavities due to their small finite dimensions, confining electromagnetic fields into plasmonic cavity modes, characterized by standing-wave current distributions. While cavity-enhanced phenomena are well-studied at optical frequencies, the impact of self-cavities on nonlinear electronic responses—such as directional photocurrent—remains largely unexplored, particularly in the terahertz regime, critical for emerging ultrafast optoelectronic technologies. Here, we report a self-cavity-induced Purcell enhancement of directional photocurrents in the vdW semimetal WTe 2 . Using ultrafast optoelectronic circuitry, we measured coherent near-field THz emission resulting from nonlinear photocurrents excited at the sample edges. We observed enhanced emission at finite frequencies, tunable via excitation fluence and sample geometry, which we attribute to plasmonic interference effects controlled by the cavity boundaries. We developed an analytical theory that captures the cavity resonance conditions and spectral response across multiple devices. Our findings establish WTe 2 as a bias-free, geometry-tunable THz emitter and demonstrate the potential of self-cavity engineering for controlling nonlinear, nonequilibrium dynamics in quantum materials.

condensed-matter physics↗

Flow and extraction of energy and charge carriers in hybrid plasmonic nanostructures

Strong interactions of electromagnetic fields with plasmonic nanomaterials have been exploited in various applications. These applications have centred on plasmon-enhanced scattering rates in nearby molecules or plasmon-induced heating. A question that has emerged recently is whether it is possible to use plasmonic nanostructures in a range of hot electron (hole) applications, including photocatalysis, photovoltaics and photodetection. These applications require coupling of a plasmonic component, which amplifies the interaction of light with the material, to an attached non-plasmonic component that extracts this energy in the form of electronic excitations to perform a function. Here, in this Perspective, we discuss recent work in the emerging field of hybrid plasmonics. We focus on fundamental questions related to the nanoscopic flow of energy and excited charge carriers in these multicomponent materials. We also address critical misconceptions, challenges and opportunities that require more attention.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tunable spin and valley excitations of correlated insulators in Γ-valley moiré bands

Moiré superlattices formed from transition metal dichalcogenides (TMDs) have been shown to support a variety of quantum electronic phases that are highly tunable using applied electromagnetic fields. While the valley character of the low-energy states dramatically affects optoelectronic properties in the constituent TMDs, this degree of freedom has yet to be fully explored in moiré systems. Here, we establish twisted double bilayer WSe 2 as an experimental platform to study electronic correlations within Γ-valley moiré bands. Through a combination of local and global electronic compressibility measurements, we identify charge-ordered phases at multiple integer and fractional moiré band fillings ν. By measuring the magnetic field dependence of their energy gaps and the chemical potential upon doping, we reveal spin-polarized ground states with novel spin polaron quasiparticle excitations. In addition, an applied displacement field allows us to realize a new mechanism of metal-insulator transition at ν=–1 driven by tuning between Γ- and K-valley moiré bands. Together, our results demonstrate control over both the spin and valley character of the correlated ground and excited states in this system.

36 MATERIALS SCIENCE↗

Symmetry-protected electronic metastability in an optically driven cuprate ladder

Optically excited quantum materials exhibit non-equilibrium states with remarkable emergent properties, but these phenomena are usually transient, decaying on picosecond timescales and limiting practical applications. Advancing the design and control of non-equilibrium phases requires the development of targeted strategies to achieve long-lived, metastable phases. Here, in this study, we report the discovery of symmetry-protected electronic metastability in the model cuprate ladder Sr 14 Cu 24 O 41 . Using femtosecond resonant X-ray scattering and spectroscopy, we show that this metastability is driven by a transfer of holes from chain-like charge reservoirs into the ladders. This ultrafast charge redistribution arises from the optical dressing and activation of a hopping pathway that is forbidden by symmetry at equilibrium. Relaxation back to the ground state is, hence, suppressed after the pump coherence dissipates. Our findings highlight how dressing materials with electromagnetic fields can dynamically activate terms in the electronic Hamiltonian, and provide a rational design strategy for non-equilibrium phases of matter.

36 MATERIALS SCIENCE↗

Laser cooling of antihydrogen atoms

The photon—the quantum excitation of the electromagnetic field—is massless but carries momentum. A photon can therefore exert a force on an object upon collision 1 . Slowing the translational motion of atoms and ions by application of such a force 2,3 , known as laser cooling, was first demonstrated 40 years ago 4,5 . It revolutionized atomic physics over the following decades 6–8 , and it is now a workhorse in many fields, including studies on quantum degenerate gases, quantum information, atomic clocks and tests of fundamental physics. However, this technique has not yet been applied to antimatter. Here we demonstrate laser cooling of antihydrogen 9 , the antimatter atom consisting of an antiproton and a positron. By exciting the 1S–2P transition in antihydrogen with pulsed, narrow-linewidth, Lyman-α laser radiation 10,11 , we Doppler-cool a sample of magnetically trapped antihydrogen. Although we apply laser cooling in only one dimension, the trap couples the longitudinal and transverse motions of the anti-atoms, leading to cooling in all three dimensions. We observe a reduction in the median transverse energy by more than an order of magnitude—with a substantial fraction of the anti-atoms attaining submicroelectronvolt transverse kinetic energies. We also report the observation of the laser-driven 1S–2S transition in samples of laser-cooled antihydrogen atoms. The observed spectral line is approximately four times narrower than that obtained without laser cooling. The demonstration of laser cooling and its immediate application has far-reaching implications for antimatter studies. A more localized, denser and colder sample of antihydrogen will drastically improve spectroscopic 11–13 and gravitational 14 studies of antihydrogen in ongoing experiments. Furthermore, the demonstrated ability to manipulate the motion of antimatter atoms by laser light will potentially provide ground-breaking opportunities for future experiments, such as anti-atomic fountains, anti-atom interferometry and the creation of antimatter molecules.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Emerging supersolidity in photonic-crystal polariton condensates

A supersolid is a counter-intuitive phase of matter in which its constituent particles are arranged into a crystalline structure, yet they are free to flow without friction. This requires the particles to share a global macroscopic phase while being able to reduce their total energy by spontaneous, spatial self-organization. The existence of the supersolid phase of matter was speculated more than 50 years ago1, 2, 3–4. However, only recently has there been convincing experimental evidence, mainly using ultracold atomic Bose–Einstein condensates (BECs) coupled to electromagnetic fields. There, various guises of the supersolid were created using atoms coupled to high-finesse cavities5,6, with large magnetic dipole moments7, 8, 9, 10, 11, 12–13, and spin–orbit-coupled, two-component systems showing stripe phases14, 15–16. Here we provide experimental evidence of a new implementation of the supersolid phase in a driven-dissipative, non-equilibrium context based on exciton–polaritons condensed in a topologically non-trivial, bound state in the continuum (BiC) with exceptionally low losses, realized in a photonic-crystal waveguide. We measure the density modulation of the polaritonic state indicating the breaking of translational symmetry with a precision of several parts in a thousand. Direct access to the phase of the wavefunction allows us to also measure the local coherence of the supersolid. We demonstrate the potential of our synthetic photonic material to host phonon dynamics and a multimode excitation spectrum.

Trypogeorgos, Dimitrios↗

Nanoscale transfer of angular momentum mediated by the Casimir torque

Casimir interactions play an important role in the dynamics of nanoscale objects. Here, we investigate the noncontact transfer of angular momentum at the nanoscale through the analysis of the Casimir torque acting on a chain of rotating nanoparticles. We show that this interaction, which arises from the vacuum and thermal fluctuations of the electromagnetic field, enables an efficient transfer of angular momentum between the elements of the chain. Working within the framework of fluctuational electrodynamics, we derive analytical expressions for the Casimir torque acting on each nanoparticle in the chain, which we use to study the synchronization of chains with different geometries and to predict unexpected dynamics, including a “rattleback”-like behavior. Our results provide insights into the Casimir torque and how it can be exploited to achieve efficient noncontact transfer of angular momentum at the nanoscale, and therefore have important implications for the control and manipulation of nanomechanical devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

First-principles theory of the rate of magnetic reconnection in magnetospheric and solar plasmas

Abstract The rate of magnetic reconnection is of the utmost importance in a variety of processes because it controls, for example, the rate energy is released in solar flares, the speed of the Dungey convection cycle in Earth’s magnetosphere, and the energy release rate in harmful geomagnetic substorms. It is known from numerical simulations and satellite observations that the rate is approximately 0.1 in normalized units, but despite years of effort, a full theoretical prediction has not been obtained. Here, we present a first-principles theory for the reconnection rate in non-relativistic electron-ion collisionless plasmas, and show that the same prediction explains why Sweet-Parker reconnection is considerably slower. The key consideration of this analysis is the pressure at the reconnection site (i.e., the x-line). We show that the Hall electromagnetic fields in antiparallel reconnection cause an energy void, equivalently a pressure depletion, at the x-line, so the reconnection exhaust opens out, enabling the fast rate of 0.1. If the energy can reach the x-line to replenish the pressure, the exhaust does not open out. In addition to heliospheric applications, these results are expected to impact reconnection studies in planetary magnetospheres, magnetically confined fusion devices, and astrophysical plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

X-ray free-electron lasing in a flying-focus undulator

Laser-driven free-electron lasers (LDFELs) replace magnetostatic undulators with the electromagnetic fields of a laser pulse. Because the undulator period is half the wavelength of the laser pulse, LDFELs can amplify X rays using lower electron energies and over shorter interaction lengths than a traditional free-electron laser. In LDFELs driven by conventional laser pulses, the undulator uniformity required for high gain necessitates large laser-pulse energies. Here, we show that a flying-focus pulse provides the undulator uniformity required to reach high gain with a substantially lower energy than a conventional pulse. The flying-focus pulse features an intensity peak that travels in the opposite direction of its phase fronts. This enables an LDFEL configuration where an electron beam collides head-on with the phase fronts and experiences a near-constant undulator strength as it co-propagates with the intensity peak. Three-dimensional simulations of this configuration demonstrate the generation of megawatts of coherent X-ray radiation with 20 × less energy than a conventional laser pulse.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nanoscale mapping of plasmon and exciton in ZnO tetrapods coupled with Au nanoparticles

Metallic nanoparticles can be used to enhance optical absorption or emission in semiconductors, thanks to a strong interaction of collective excitations of free charges (plasmons) with electromagnetic fields. Herein we present direct imaging at the nanoscale of plasmon-exciton coupling in Au/ZnO nanostructures by combining scanning transmission electron energy loss and cathodoluminescence spectroscopy and mapping. The Au nanoparticles (~30 nm in diameter) are grown in-situ on ZnO nanotetrapods by means of a photochemical process without the need of binding agents or capping molecules, resulting in clean interfaces. Interestingly, the Au plasmon resonance is localized at the Au/vacuum interface, rather than presenting an isotropic distribution around the nanoparticle. Moreover, on the contrary, a localization of the ZnO signal has been observed inside the Au nanoparticle, as also confirmed by numerical simulations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Plasmonic Au nanoparticles embedding enhances the activity and stability of CdS for photocatalytic hydrogen evolution

A composite photocatalyst of embedding plasmonic Au nanoparticle into CdS (Au@CdS) was prepared with a cysteine-assisted hydrothermal approach. This structure could take fully advantage of electromagnetic fields at the surface of the Au nanoparticles under visible light illumination. The photocatalytic hydrogen evolution activity of CdS could be significantly improved. Without the use of any other metal or metal oxide as cocatalysts, the quantum efficiency can reach 12.1 % over 0.5%Au@CdS at 420 nm. When using 0.1%Pt as a cocatalyst, the quantum efficiency of 0.5%Au@CdS can be further improved to 45.6%. This efficiency can be maintained more than 100 h in the test 12 days, exhibiting a relatively high stability. Photoluminescence (PL) characterization shows that the formation rate of photoexcited e-/h+ was dramatically increased when Au nanoparticles were embedded into CdS. Time-resolved PL measurement shows that Au@CdS also has a longer luminescence lifetime than that of CdS, reflecting that the photoexcited electrons in Au@CdS be with much longer lifetime to reduce H+ forming H2. All these enhancements can be attributed to the effective energy transfer between the Au surface and CdS due to the well matched composite nanostructure. Dr. Xiang Wang gratefully acknowledges the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division for the support of this work.

Au nanoparticles↗

Imaging out-of-plane polarized emission patterns on gap mode SERS substrates: from high molecular coverage to the single molecule regime

Gap mode surface-enhanced Raman scattering (SERS) substrates are created when a single nanoparticle is deposited on a thin metal film, creating a region of significant electromagnetic field enhancement in the gap between the nanoparticle and the film due to excitation of a vertically-oriented, out-of-plane dipole plasmon mode, e.g. the gap plasmon. When molecules are located in the gap and couple to the gap plasmon mode, the resulting emission is polarized perpendicular to the thin film, generating SERS emission patterns that have a characteristic donut shape. We analyze these SERS emission patterns using a dipole emission model and extract out-of-plane and in-plane emission angles associated with the gap plasmon mode. Fluctuations in both of these angles reveal dynamic heterogeneity due to molecular motion within the hot spot that changes as a function of molecular coverage. We also reveal static heterogeneity associated with structural defects in the thin film component of the gap mode substrates, indicating that even nanometer-scale surface roughness can impact the quality of gap mode emission.

Chemistry↗

Angle-resolved polarimetry of hybrid perovskite emission for photonic technologies

Coupling between light and matter strongly depends on the polarization of the electromagnetic field and the nature of excitations in a material. As hybrid perovskites emerge as a promising class of materials for light-based technologies such as LEDs, LASERs, and photodetectors, it is critical to understand how their microstructure changes the intrinsic properties of the photon emission process. While the majority of optical studies have focused on the spectral content, quantum efficiency and lifetimes of emission in various hybrid perovskite thin films and nanostructures, few studies have investigated other properties of the emitted photons such as polarization and emission angle. Here, we use angle-resolved cathodoluminescence microscopy to access the full polarization state of photons emitted from large-grain hybrid perovskite films with spatial resolution well below the optical diffraction limit. In this work, mapping these Stokes parameters as a function of the angle at which the photons are emitted from the thin film surface, we reveal the effect of a grain boundary on the degree of polarization and angle at which the photons are emitted. Such studies of angle- and polarization-resolved emission at the single grain level are necessary for future development of perovskite-based flat optics, where effects of grain boundaries and interfaces need to be mitigated.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Quantitative resonant soft x-ray reflectivity of ultrathin anisotropic organic layers: Simulation and experiment of PTCDA on Au

Resonant soft X-ray reflectivity at the carbon K edge, with linearly polarized light, was used to derive quantitative information of film morphology, molecular arrangement, and electronic orbital anisotropies of an ultrathin 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) film on Au(111). The experimental spectra were simulated by computing the propagation of the electromagnetic field in a trilayer system (vacuum/PTCDA/Au), where the organic film was treated as an anisotropic medium. Optical constants were derived from the calculated (through density functional theory) absorption cross sections of the single molecule along the three principal molecular axes. These were used to construct the dielectric tensor of the film, assuming the molecules to be lying flat with respect to the substrate and with a herringbone arrangement parallel to the substrate plane. Resonant soft X-ray reflectivity proved to be extremely sensitive to film thickness, down to the single molecular layer. The best agreement between simulation and experiment was found for a film of 1.6 nm, with flat laying configuration of the molecules. The high sensitivity to experimental geometries in terms of beam incidence and light polarization was also clarified through simulations. The optical anisotropies of the organic film were experimentally determined and through the comparison with calculations, it was possible to relate them to the orbital symmetry of the empty electronic states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗