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At least 415 records · Page 23

A characterization of quantum Kerr optical frequency combs

Quantum Kerr optical frequency combs are generated by pumping a high-Q microresonator with a continuous wave resonant laser. Below threshold, two pump photons are symmetrically up- and down-converted as twin photons via spontaneous four-wave mixing, thereby generating up to a hundred paired channels. Furthermore, these chipscale, high-dimensional and room-temperature systems are expected to play a major role in quantum engineering. However, their theoretical description is still unclear. Here, we present an explicit description of this quantum system via a frequency-bin state and its density operator, and explore the properties of the eigenkets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Resonance Effect in Brunel Harmonic Generation in Thin Film Organic Semiconductors

Abstract Nonlinear optical properties of organic semiconductors (OSCs) have been extensively investigated in the perturbative regime, while strong light induced high‐order processes in solid‐state OSCs are less studied. Here, below‐threshold harmonic generation is examined, both experimentally and theoretically, in two solid‐state thin film OSCs, that is, tetraphenylporphyrin and zinc tetraphenylporphyrin. Results show that the π–π* excitations of the porphyrin ring system generate the harmonic emission. The contribution of the Brunel harmonic to the 5th harmonic emission is uncovered, where the resonant 5‐photon transition ( S 0 → S 2 transition) is found to lead to an early onset of non‐perturbative behavior. A similar resonance effect is expected in Brunel harmonic generation in other organic materials.

36 MATERIALS SCIENCE↗

Cosmic axions revealed via amplified modulation of the ellipticity of a laser

We propose a new axion dark matter detection strategy that employs optical readout of laser beam ellipticity modulations caused by axion-induced electric fields in a microwave cavity, using electro-optic (EO) crystals, enhanced by externally injected radio-frequency (rf) power. Building upon the variance-based probing method [Phys. Rev. D 107, 103005 (2023).], we extend this concept to the optical domain: A weak probe laser interacts with an EO crystal coupled to the resonant microwave cavity field at cryogenic temperatures, and the axion-induced electric field is revealed through induced ellipticity. The injected rf signal coherently interferes with that of the axion field, amplifying the optical response and significantly improving sensitivity. While our EO-based method employs a Fabry-Pérot resonator, we do not require Michelson interferometers. Our method, hence, enables compact, high-frequency axion searches, across the 0.5–50 GHz range. Operating at cryogenic temperatures not only suppresses thermal backgrounds, but, critically, allows the probing method to mitigate the quantum noise. This approach offers a scalable path forward for axion detection over the ∼(few−200) μ⁢eV mass range—covering the preferred parameter space for the postinflationary Peccei-Quinn axion dark matter—using compact, tunable systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Point-localized, site-specific membrane potential optical recording by single fluorescent nanodiscs

Nanodisc technology was implemented as a platform for voltage nanosensors. A fluorescence (Förster) resonance energy transfer (FRET)-based voltage-sensing scheme employing fluorescent nanodiscs and the hydrophobic ion dipicrylamine was developed and utilized to optically record membrane potentials on the single-nanodisc level. Ensemble and single-nanosensor recordings were demonstrated for HEK293 cells and primary cortical neuron cells. Conjugation of nanodiscs to anti-GABA A antibodies allowed for site-specific membrane potential measurements from postsynaptic sites.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Mitigating photorefractive effect in thin-film lithium niobate microring resonators

Thin-film lithium niobate is an attractive integrated photonics platform due to its low optical loss and favorable optical nonlinear and electro-optic properties. However, in applications such as second harmonic generation, frequency comb generation, and microwave-to-optics conversion, the device performance is strongly impeded by the photorefractive effect inherent in thin-film lithium niobate. In this paper, we show that the dielectric cladding on a lithium niobate microring resonator has a significant influence on the photorefractive effect. By removing the dielectric cladding layer, the photorefractive effect in lithium niobate ring resonators can be effectively mitigated. Our work presents a reliable approach to control the photorefractive effect on thin-film lithium niobate and will further advance the performance of integrated classical and quantum photonic devices based on thin-film lithium niobate.

42 ENGINEERING↗

Intrinsic donor-bound excitons in ultraclean monolayer semiconductors

The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe 2 . These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns). Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellites' photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.

36 MATERIALS SCIENCE↗

Imaging plasma formation in isolated nanoparticles with ultrafast resonant scattering

We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Surface plasmon enhanced fast electron emission from metallised fibre optic nanotips

Physical mechanisms of electron emission from fibre optic nanotips, namely, tunnelling, multi-photon, and thermionic emission, either prevent fast switching or require intense laser fields. Time-resolved electron emission from nano-sized sources finds applications ranging from material characterisation to fundamental studies of quantum coherence. We present a nano-sized electron source capable of fast-switching (≤1 ns) that can be driven with low-power femtosecond lasers. The physical mechanism that can explain emission at low laser power is surface plasmon enhanced above-threshold photoemission. An electron emission peak is observed and provides support for resonant plasmonic excitation. The electron source is a metal-coated optical fibre tapered into a nano-sized tip. The fibre is flexible and back illuminated facilitating ease of positioning. The source operates with a few nJ per laser pulse, making this a versatile emitter that enables nanometrology, multisource electron-lithography and scanning probe microscopy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Polarized Resonant X-ray Scattering to Measure Molecular Orientation and Conformation in Organic Nanostructures

The ordering of organic (carbon-based) molecules into nanostructures drives useful materials properties for applications such as organic light emitting diodes, flexible batteries, and polymer nanocarriers. However, there is a current lack of techniques to measure this ordering. X-ray scattering techniques involving molecular resonances have shown promise in identifying molecular types, locations, and orientation. However, resonant soft X-ray scattering (RSoXS) techniques have not been developed even lacking basic optical models. The objectives achieved by this research were the development of methods, models, and analysis techniques that harness these resonant phenomena in X-ray scattering measurements to quantitatively probe ordering of organic molecules within devices and nanostructures. This award resulted in 11 peer reviewed publications with two others soon to be submitted. New physical models for X-ray scattering that accurately describe these complex molecular resonances enable measurements of how molecules assemble, orient and conform at the nanometer scale. These new techniques were applied to both organic electronic devices and aqueous nanoparticles being developed for hydrocarbon sequestration. This new measurement capability will enable characterization of structure-property relationships that lead to disruptive technologies of printable, stretchable, and biocompatible devices based on organic materials.

14 SOLAR ENERGY↗

Toward radiative-limited coherence of erbium dopants in a nanophotonic resonator

Atomic-like emitters in the solid state serve as important resources in the advancement of future quantum networks. In particular, intra-4f optical transitions of rare earth ions exhibit excellent coherence properties thanks to the shielding effect of outer electrons. Still, the presence of various dephasing channels in solid state hosts introduces additional decoherence beyond the radiative decay, causing the coherence time of most rare earth doped materials to be over an order of magnitude lower than the radiative limit. Such obstacle prevents the emission of indistinguishable photons from rare earth ions, which is an essential requirement for various quantum applications. In this work, we perform optical coherence study on erbium ions doped in thin-film lithium niobate by patterning photonic crystal resonators with quality factor around 100 k and sub-λ3 mode volume. Leveraging the combination of long coherence and strong Purcell enhancement in the cavity, we show that the coherence time measured with photon echo approaches the radiative limit (80%), representing a 50-fold improvement compared to the waveguide case. Our results present promising prospects toward utilizing rare earth doped materials as quantum repeaters and sources of indistinguishable photons.

Physics↗

Simultaneous Brillouin and piezoelectric coupling to a high-frequency bulk acoustic resonator

Bulk acoustic resonators support robust, long-lived mechanical modes, capable of coupling to various quantum systems. In separate works, such devices have achieved strong coupling to both superconducting qubits, via piezoelectricity, and optical cavities, via Brillouin interactions. In this work, we present a hybrid microwave–optical platform capable of coupling to bulk acoustic waves through cavity-enhanced piezoelectric and photoelastic interactions. The modular, tunable system achieves fully resonant and well-mode-matched interactions among a 3D microwave cavity, a high-frequency bulk acoustic resonator, and a Fabry–Perot cavity. We realize this piezo–Brillouin interaction in x-cut quartz, demonstrating the potential for strong optomechanical interactions and high cooperativity using optical cavity enhancement. We further show how this device functions as a bidirectional electro–opto–mechanical transducer, with transduction efficiency exceeding 10 − <#comment/> 8 , and a feasible path towards unity conversion efficiency. The high optical sensitivity and ability to apply a large resonant microwave field in this system also offers a tool for probing anomalous electromechanical couplings, which we demonstrate by investigating (nominally centrosymmetric) C a F 2 and revealing a parasitic piezoelectricity of 83 am/V. Such studies are an important topic for emerging quantum technologies, and highlight the versatility of this hybrid platform.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Moiré Exchange Effect in Twisted WSe 2 /WS 2 Heterobilayer

Moiré superlattices of layered transition metal dichalcogenides are proven to host periodic electron crystals due to strong correlation effects. These electron crystals can also be intertwined with intricate magnetic phenomena. Here, in this Letter, we present our findings on the moiré exchange effect, resulting from the modulation of local magnetic moments by electron crystals within well-aligned WSe 2 /WS 2 heterobilayers. Employing polarization-resolved magneto-optical spectroscopy, we unveil a high-energy excitonic resonance near one hole per moiré unit cell (v=–1), which possesses a giant g factor several times greater than the already very large g factor of the WSe 2 A exciton in this heterostructure. Supported by continuum model calculations, these high-energy states are found to be dark excitons brightened through Umklapp scattering from the moiré mini-Brillouin zone. When the carriers form a Mott insulating state near v=–1, the Coulomb exchange between doped carriers and excitons forms an effective magnetic field with moiré periodicity. This moiré exchange effect gives rise to the observed giant g factor for the excitonic Umklapp state.

36 MATERIALS SCIENCE↗

Optically Active Spin Defects in Few-Layer Thick Hexagonal Boron Nitride

Optically active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this Letter, we first demonstrate that the electron spin resonance frequencies of boron vacancy centers ($V$$^{–}_{B}$) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of $V$$^{–}_{B}$ centers with the hBN thickness with a focus on (i) the zero-field splitting parameters, (ii) the optically induced spin polarization rate and (iii) the longitudinal spin relaxation time. Furthermore, this Letter provides important insights into the properties of $V$$^{–}_{B}$ centers embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Understanding the p-doping of spiroOMeTAD by tris(pentafluorophenyl)borane

The solid-state organization of photoabsorber, hole and electron transporting layers, and interfaces between them plays an important role in governing the performance and stability of emerging optoelectronic devices such as perovskite solar cells (PSCs). The molecular organic semiconductor (OSC) 2,2' ,7,7' -tetrakis [N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (spiroOMeTAD) is a promising hole-transporting material (HTM) for PSCs, which is p-doped by molecular dopants to augment the charge carrier mobility. Here, the p-type doping of spiroOMeTAD by tris(pentafluorophenyl)borane (BCF) is investigated by a combination of techniques including optical spectroscopy, X-ray diffraction, Fourier transform infrared (FTIR), solid-state (ss)NMR, and electron paramagnetic resonance (EPR) spectroscopy. BCF molecules interact with traces of water molecules to form BCF-water complexes. Optical spectroscopy analysis suggests that the BCF/BCF-water complexes oxidize spiroOMeTAD molecules and facilitate p-type doping of spiroOMeTAD molecules. The different distributions of BCF and BCF-water molecules in doped spiroOMeTAD are characterized by FTIR and 11B NMR spectroscopy. An NMR crystallography approach which combines two-dimensional (2D) ssNMR and crystallography modeling is employed to unravel the packing interactions in spiroOMeTAD, and this analysis is extended to probe the morphological and structural changes in spiroOMeTAD:BCF blends. The hyperfine interactions are characterized by 2D hyperfine sub-level correlation (HYSCORE) spectroscopy. In this way, insight into the complex spiroOMeTAD:BCF blend morphology is obtained and compared for different dopant concentrations. Further, molecular-level analysis of doped HTMs enabled by this study has much wider relevance for further investigation, for example, chemical design and interfacial engineering of p-type doped HTMs for stable and efficient hybrid perovskite photovoltaics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High resolution x-ray emission spectrometer for multiple hard x-ray emission lines: Demonstration for Cu Kα and Kβ emissions

In this work, we present a compact 3D printed x-ray emission spectrometer based on the von Hamos geometry that represents a significant upgrade to the existing von Hamos geometry-based miniature x-ray emission spectrometer (miniXES). The upgrades include the incorporation of a higher pixel density 500K detector for improved energy resolution and an enlarged sample area to accommodate a wider range of sample formats. The versatile spectrometer houses removable crystal holders that can be easily exchanged, as well as movable alignment eyelets that give flexibility in Bragg angle selection. Designed for ease of manufacture, all the components, except for the apertures, can be 3D printed and readily assembled. We describe its implementation in measurements of resonant and non-resonant Cu Kα and Kβ x-ray emission and report the theoretical and measured energy resolution and collected solid angle of the emission.

3D printing↗

Characterization of the Interfacial Orientation and Molecular Conformation in a Glass-Forming Organic Semiconductor

The ability to control structure in molecular glasses has enabled them to play a key role in modern technology; in particular, they are ubiquitous in organic light-emitting diodes. While the interplay between bulk structure and optoelectronic properties has been extensively investigated, few studies have examined molecular orientation near buried interfaces despite its critical role in emergent functionality. Direct, quantitative measurements of buried molecular orientation are inherently challenging, and many methods are insensitive to orientation in amorphous soft matter or lack the necessary spatial resolution. To overcome these challenges, we use polarized resonant soft X-ray reflectivity (pRSoXR) to measure nanometer-resolved, molecular orientation depth profiles of vapor-deposited thin films of an organic semiconductor Tris(4-carbazoyl-9-ylphenyl)amine (TCTA). Our depth profiling approach characterizes the vertical distribution of molecular orientation and reveals that molecules near the inorganic substrate and free surface have a different, nearly isotropic orientation compared to those of the anisotropic bulk. Comparison of pRSoXR results with near-edge X-ray absorption fine structure spectroscopy and optical spectroscopies reveals that TCTA molecules away from the interfaces are predominantly planar, which may contribute to their attractive charge transport qualities. Buried interfaces are further investigated in a TCTA bilayer (each layer deposited under separate conditions resulting in different orientations) in which we find a narrow interface between orientationally distinct layers extending across ≈1 nm. Coupling this result with molecular dynamics simulations provides additional insight into the formation of interfacial structure. This study characterizes the local molecular orientation at various types of buried interfaces in vapor-deposited glasses and provides a foundation for future studies to develop critical structure–function relationships.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Superposition of intra- and inter-layer excitons in twistronic MoSe 2 /WSe 2 bilayers probed by resonant Raman scattering

Abstract Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe 2 /WSe 2 heterostructures, strong hybridization of both single particle and excitonic states can occur via single particle tunnelling. Here we use resonance Raman scattering to provide direct evidence for the hybridisation of excitons in twistronic MoSe 2 /WSe 2 structures, by observing scattering of specific excitons by phonons in both WSe 2 and MoSe 2 . We also demonstrate that resonance Raman scattering spectroscopy opens up a wide range of possibilities for quantifying the layer composition of the superposition states of the exciton and the interlayer hybridisation parameters in heterostructures of two-dimensional materials.

Materials Science↗