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At least 811 records · Page 45

Optically pumped spin polarization as a probe of many-body thermalization

Disorder and many body interactions are known to impact transport and thermalization in competing ways, with the dominance of one or the other giving rise to fundamentally different dynamical phases. Here we investigate the spin diffusion dynamics of 13 C in diamond, which we dynamically polarize at room temperature via optical spin pumping of engineered color centers. We focus on low-abundance, strongly hyperfine-coupled nuclei, whose role in the polarization transport we expose through the integrated impact of variable radio-frequency excitation on the observable bulk 13 C magnetic resonance signal. Unexpectedly, we find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength, which we attribute to effective carbon-carbon interactions mediated by the electronic spin ensemble. In particular, observations across the full range of hyperfine couplings indicate the nuclear spin diffusion constant takes values up to two orders of magnitude greater than that expected from homo-nuclear spin couplings.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Valley-Mediated Singlet- and Triplet-Polaron Interactions and Quantum Dynamics in a Doped WSe 2 Monolayer

In doped transition metal dichalcogenides, optically created excitons (bound electron-hole pairs) can strongly interact with a Fermi sea of electrons to form Fermi polaron quasiparticles. When there are two distinct Fermi seas, as is the case in WSe 2 , there are two flavors of lowest-energy (attractive) polarons—singlet and triplet—where the exciton is coupled to the Fermi sea in the same or opposite valley, respectively. Using two-dimensional coherent electronic spectroscopy, we analyze how their quantum decoherence evolves with doping density and determine the condition under which stable Fermi polarons form. Because of the large oscillator strength associated with these resonances, intrinsic quantum dynamics of polarons as well as valley coherence between coupled singlet- and triplet polarons occur on subpicosecond timescales. Surprisingly, we find that a dark-to-bright state conversion process leads to a particularly long-lived singlet polaron valley polarization, persisting up to 200–800 ps. Valley coherence between the singlet- and triplet polaron is correlated with their energy fluctuations. In conclusion, our finding provides valuable guidance for the electrical and optical control of spin and valley indexes in atomically thin semiconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Local microwave sensing of excitons and their electrical environment

Excitons in atomically thin transition metal dichalcogenides (TMDs) possess intriguing optical properties, drawing interest for both technology and fundamental research. However, as the demands for nanodevice applications and the exploration of fundamental physics push toward smaller, subwavelength scales, studying them locally is challenging. In this work, we introduce a cryogenic scanning probe photoelectrical sensing technique, termed exciton-resonant microwave impedance microscopy (ER-MIM), to measure the excitonic responses in a monolayer MoSe 2 device at 1.5K. From the microwave signal changes, we identify exciton polarons and their Rydberg states. Building on these observations, we systemically reveal the local and nonlocal effects of carrier density, inhomogeneous electric fields, as well as dielectric screening on excitons, beyond the reach of conventional probes. By further integrating deep learning techniques, we precisely extracted the electrical parameters surrounding excitons, demonstrating a quantified, exciton-assisted nanoscale electrometry. Our results provide new insight into exciton-environment interactions, establish ER-MIM as a powerful optoelectronic sensing platform, and open avenues for exciton-based quantum control and device technologies.

scanning probe microscopy↗

Using resonant energy X-ray diffraction to extract chemical order parameters in ternary semiconductors

II–IV–V 2 materials, ternary analogs to III–V materials, are emerging for their potential applications in devices such as LEDs and solar cells. Controlling cation ordering in II–IV–V 2 materials offers the potential to tune properties at nearly fixed compositions and lattice parameters. While tuning properties at a fixed lattice constant through ordering has the potential to be a powerful tool used in device fabrication, cation ordering also creates challenges with characterization and quantification of ordering. In this work, we investigate two different methods to quantify cation ordering in ZnGeP 2 thin films: a stretching parameter calculated from lattice constants , and an order parameter determined from the cation site occupancies ( S ). We use high resolution X-ray diffraction (HRXRD) to determine and resonant energy X-ray diffraction (REXD) to extract S . REXD is critical to distinguish between elements with similar Z -number ( e.g. Zn and Ge). We found that samples with a corresponding to the ordered chalcopyrite structure had only partially ordered S values. The optical absorption onset for these films occurred at lower energy than expected for fully ordered ZnGeP 2 , indicating that S is a more accurate descriptor of cation order than the stretching parameter. Since disorder is complex and can occur on many length scales, metrics for quantifying disorder should be chosen that most accurately reflect the physical properties of interest.

36 MATERIALS SCIENCE↗

Radiative dynamics and delayed emission in pure and doped InP/ZnSe/ZnS quantum dots

We have used time-correlated single photon counting to elucidate the radiative dynamics of InP/ZnSe/ZnS core/shell/shell quantum dots (QDs) that differ in the amount and distribution of excess indium. Stoichiometric QDs having an In:P atom ratio very near unity exhibit simple luminescence kinetics. The photoluminescence (PL) rises with the 40 ps instrument response function and exhibits a decay that is close to a single exponential with a time constant that decreases from 32 to 28 ns with increasing shell thickness. QDs having excess indium (In:P ratio of 1.15–1.63) show a significant component of a slower rise time assigned to transient population of indium-based hole traps in the ZnSe shell. They also have a slower PL decay, attributed to an equilibrium between these traps, which are optically dark, and the emissive valence-band state. This results in a radiative lifetime that increases from 32 to 48 ns with increasing shell thickness. Different treatments of the InP cores prior to shell deposition result in different core/shell interfaces as indicated by resonance Raman spectroscopy, as well as differences in the amplitude and timescale of the slow PL rise and the PL decay time. These are interpreted in terms of different radial distributions of the indium-based hole traps, which can be related to differences in the interfacial lattice strain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanophotonic waveguide chip-to-world beam scanning

A seamless chip-to-world photonic interface enables broad advancements in optical ranging, display, communication, computation and quantum information science. The ideal solution enables two-dimensional scanning of a diffraction-limited beam from anywhere on a photonic integrated circuit to a large number of resolvable spots. Current beam-scanning technologies are limited by a fundamental trade-off: photonic-integrated-circuits with diffractive optics offer scalability but have poor mode quality, whereas inertially limited micromechanical scanners provide high-quality beams but lack scalable integration. Here we report a photonic ski-jump—a nanoscale waveguide monolithically integrated on a piezoelectric cantilever—to overcome these limitations. It passively curls ~90° out-of-plane within a less-than-0.1 mm 2 footprint, emits a submicrometre, broadband diffraction-limited beam, and exhibits kilohertz-rate mechanical resonances with quality factors of over 10,000. Fabricated in a volume complementary metal–oxide–semiconductor (CMOS) foundry, our device enables scalable two-dimensional beam scanning. Driven on-resonance at CMOS-level voltages, it achieves a footprint-adjusted spot rate of 68.6 mega spots s –1 mm–², exceeding state-of-the-art micro-electro-mechanical systems mirrors by more than 50-fold, which is sufficient for one million pixels at 100 Hz from an approximately 1.5 mm diameter footprint. We demonstrate full-colour image and video projection, and single-photon initialization and readout from silicon vacancy centres in diamond. Finally, by demonstrating uniformity across a 64 ski-jump array, we establish a pathway to achieving greater than one gigaspot resolution at kilohertz rates within a sub-5-cm-diameter footprint, creating a seamless optical pipeline between integrated photonic processors and the free-space world.

Displays↗

Trapping light in air with membrane metasurfaces for vibrational strong coupling

Optical metasurfaces can manipulate electromagnetic waves in unprecedented ways at ultra-thin engineered interfaces. Specifically, in the mid-infrared (mid-IR) region, metasurfaces have enabled numerous biochemical sensing, spectroscopy, and vibrational strong coupling (VSC) applications via enhanced light-matter interactions in resonant cavities. However, mid-IR metasurfaces are usually fabricated on solid supporting substrates, which degrade resonance quality factors (Q) and hinder efficient sample access to the near-field electromagnetic hotspots. Besides, typical IR-transparent substrate materials with low refractive indices, such as CaF 2 , NaCl, KBr, and ZnSe, are usually either water-soluble, expensive, or not compatible with low-cost mass manufacturing processes. Here, we present novel free-standing Si-membrane mid-IR metasurfaces with strong light-trapping capabilities in accessible air voids. We employ the Brillouin zone folding technique to excite tunable, high-Q quasi-bound states in the continuum (qBIC) resonances with our highest measured Q-factor of 722. Leveraging the strong field localizations in accessible air cavities, we demonstrate VSC with multiple quantities of PMMA molecules and the qBIC modes at various detuning frequencies. Our new approach of fabricating mid-IR metasurfaces into semiconductor membranes enables scalable manufacturing of mid-IR photonic devices and provides exciting opportunities for quantum-coherent light-matter interactions, biochemical sensing, and polaritonic chemistry. The authors introduce a mid-IR metasurface fabricated by decorating a free-standing Si-membrane with air holes. The enhanced light-matter interactions in such air cavities enable vibrational strong coupling and advanced biochemical sensing.

infrared spectroscopy↗

Integrating collapsible plasmonic gaps on near-field probes for polarization-resolved mapping of plasmon-enhanced emission in 2D material

Scanning near-field optical microscopy (SNOM) is an important technique used to study the optical properties of material systems at the nanoscale. In previous work, we reported on the use of nanoimprinting to improve the reproducibility and throughput of near-field probes including complicated optical antenna structures such as the ‘campanile’ probe. However, precise control over the plasmonic gap size, which determines the near-field enhancement and spatial resolution, remains a challenge. Here, we present a novel approach to fabricating a sub-20 nm plasmonic gap in a near-field plasmonic probe through the controlled collapse of imprinted nanostructures using atomic layer deposition (ALD) coatings to define the gap width. The resulting ultranarrow gap at the apex of the probe provides a strong polarization-sensitive near-field optical response, which results in an enhancement of the optical transmission in a broad wavelength range from 620 to 820 nm, enabling tip-enhanced photoluminescence (TEPL) mapping of 2-dimensional (2D) materials. We demonstrate the potential of this near-field probe by mapping a 2D exciton coupled to a linearly polarized plasmonic resonance with below 30 nm spatial resolution. This work proposes a novel approach for integrating a plasmonic antenna at the apex of the near-field probe, paving the way for the fundamental study of light-matter interactions at the nanoscale.

Zhou, Junze (ORCID:000000020682767X)↗

Ultrafast snapshots of terahertz electric potentials across ring-shaped quantum barriers

Probing the time evolution of the terahertz electric field within subwavelength dimensions plays a crucial role in observing the nanoscale lightwave interactions with fundamental excitations in condensed-matter systems and in artificial structures, such as metamaterials. Here, we propose a novel probing method for measuring terahertz electric potentials across nanogaps using a combination of optical and terahertz pulse excitations. To achieve this, we employ ring-shaped nanogaps that enclose a metallic island, allowing us to capture tunneling charges when subjected to terahertz electromagnetic pulse illumination. By controlling and manipulating the terahertz tunneling charges through a focused optical gate pulse, we can obtain the terahertz potential strength as a function of spatial coordinates and time delays between pulses. To accurately quantify the time evolution of terahertz electric potential across quantum barriers, we carefully calibrate the recorded nonlinear tunneling current. Its on-resonance and off-resonance behaviors are also discussed, providing valuable insights into the antenna’s characteristics and performance.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

KIPM Detector Characterization in QUIET

Kinetic Inductance Phonon‑Mediated (KIPM) detectors are superconducting microwave resonators on silicon that sense bursts of energy through tiny shifts in their resonance. In this work, we installed new devices in the QUIET facility's cryogenic test setup and used a network analyzer to drive them across a range of power levels. At each setting, we measured the transmitted signal and fit it to a simple notch‑filter model, allowing us to extract key performance metrics. And despite the increased noise at low power, our model consistently captured the resonance behavior. We observed that the resonant frequency stayed stable across most powers, the device s internal quality factor improved with stronger signals, and its coupling strength peaked mid‑range before leveling off. Overall, these findings confirm the detector s performance, laying groundwork for future work on energy calibration with pulsed optical sources.

Savitala, Akash [Washington U., Seattle; Fermilab]↗

The chemRIXS Instrument for Solution-Phase Resonant Inelastic X-ray Scattering at the Linac Coherent Light Source

The chemRIXS instrument at the Linac Coherent Light Source (LCLS) offers new opportunities for studying solution-phase systems with time-resolved soft X-ray spectroscopic methods such as resonant inelastic X-ray scattering (RIXS) using the recently commissioned high-repetition-rate LCLS-II X-ray free electron laser. The orders-of-magnitude X-ray flux improvement provided by the superconducting accelerator, combined with corresponding advances in the optical laser system and the liquid jet recirculation system, enables studies on dilute systems with high signal-to-noise compared to what was possible with the LCLS-I copper accelerator. These capabilities open up time-resolved X-ray absorption spectroscopy and RIXS to entirely new classes of samples, as well as enabling the development of new soft X-ray spectroscopic methods on liquid samples. An overview of the beamline components and the first LCLS-II commissioning results are presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interstitial Nature of Mn 2+ Doping in 2D Perovskites

Halide perovskites doped with magnetic impurities (such as the transition metals Mn 2+ , Co 2+ , Ni 2+ ) are being explored for a wide range of applications beyond photovoltaics, such as spintronic devices, stable light-emitting diodes, single-photon emitters, and magneto-optical devices. However, despite several recent studies, there is no consensus on whether the doped magnetic ions will predominantly replace the octahedral B-site metal via substitution or reside at interstitial defect sites. Here, by performing correlated nanoscale X-ray microscopy, spatially and temporally resolved photoluminescence measurements, and magnetic force microscopy on the inorganic 2D perovskite Cs 2 PbI 2 Cl 2 , we show that doping Mn 2+ into the structure results in a lattice expansion. The observed lattice expansion contrasts with the predicted contraction expected to arise from the B-site metal substitution, thus implying that Mn 2+ does not replace the Pb 2+ sites. Photoluminescence and electron paramagnetic resonance measurements confirm the presence of Mn 2+ in the lattice, while correlated nano-XRD and X-ray fluorescence track the local strain and chemical composition. Density functional theory calculations predict that Mn 2+ atoms reside at the interstitial sites between two octahedra in the triangle formed by one Cl – and two I – atoms, which results in a locally expanded structure. These measurements show the fate of the transition metal dopants, the local structure, and optical emission when they are doped at dilute concentrations into a wide band gap semiconductor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Energy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping

Abstract Selectively exciting target molecules to high vibrational states is inefficient in the liquid phase, which restricts the use of IR pumping to catalyze ground-state chemical reactions. Here, we demonstrate that this inefficiency can sometimes be solved by confining the liquid to an optical cavity under vibrational strong coupling conditions. For a liquid solution of 13 CO 2 solute in a 12 CO 2 solvent, cavity molecular dynamics simulations show that exciting a polariton (hybrid light-matter state) of the solvent with an intense laser pulse, under suitable resonant conditions, may lead to a very strong (>3 quanta) and ultrafast (<1 ps) excitation of the solute, even though the solvent ends up being barely excited. By contrast, outside a cavity the same input pulse fluence can excite the solute by only half a vibrational quantum and the selectivity of excitation is low. Our finding is robust under different cavity volumes, which may lead to observable cavity enhancement on IR photochemical reactions in Fabry–Pérot cavities.

74 ATOMIC AND MOLECULAR PHYSICS↗

Element-specific ultrafast lattice dynamics in FePt nanoparticles

Light–matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

36 MATERIALS SCIENCE↗

Plasmonically assisted channels of photoemission from metals

We analyze recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbar$ω p above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbar$ω p and nonlinear 2$\hbar$ω p electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Understanding and Manipulating Helical Nanofilaments in Binary Systems with Achiral Dopants

Here, in this paper, we report the relationship between helical pitch of the helical nanofilament (HNF) phase formed by bent-core molecule NOBOW and the concentration of achiral dopants 5CB and octane, using linearly polarized resonant soft X-ray scattering (RSoXS). Utilizing theory-based simulation, which fits well with the experiments, the molecular helices in the filament were probed and the superstructure of helical 5CB directed by groove of HNFs was observed. Quantitative pitch determination with RSoXS reveals that helical pitch variation is related to 5CB concentration with no temperature dependence. Doping rodlike immiscible 5CB led to a pitch shortening of up to 30%, which was attributed to a change in interfacial tension. By shedding light not only on phase behavior of binary systems but also enabling control over pitch length, our work may benefit various applications of HNF-containing binary systems, including optical rotation devices, circularly polarized light emitters, and chirality transfer agents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Control of spin dynamics in artificial honeycomb spin-ice-based nanodisks

In this paper, we report the experimental and theoretical characterization of the angular-dependent spin dynamics in arrays of ferromagnetic nanodisks arranged on a honeycomb lattice. The magnetic field and microwave frequency dependence, measured by broadband ferromagnetic resonance, reveal a rich spectrum of modes that is strongly affected by the microstate of the network. Based on symmetry arguments with respect to the external field, we show that certain parts of the ferromagnetic network contribute to the detected signal. A comparison of the experimental data with micromagnetic simulations reveals that different subsections of the lattice predominantly contribute to the high-frequency response of the array. This is confirmed by optical characterizations using microfocused Brillouin light scattering. Furthermore, we find indications that nucleation and annihilation of vortexlike magnetization configurations in the low-field range affect the dynamics, which is different from clusters of ferromagnetic nanoellipses. Our work opens up new perspectives for designing magnonic devices that combine geometric frustration in gyrotropic vortex crystals at low frequencies with magnonic crystals at high frequencies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗