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At least 163 records · Page 9

Photo‐Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room‐Temperature Diamond

Abstract The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV 0 to SiV ‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV ‒ , on the other hand, yields only fractional recombination into SiV 2‒ , a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characterizations of two-photon absorption process induced by defects in aluminum nitride using Z-scan method

Abstract In this work, we reported two-photon absorption (TPA) measurements for aluminum vacancies in Aluminum nitride single crystals. We measured the linear transmission and identified the defect levels. Using the Z-scan method, we measured the TPA coefficients of the transitions between defect levels from 380 nm to 735 nm. The transition occurs between the aluminum vacancies defect levels. Furthermore, the power dependence shows good linear fitting, confirming the TPA mechanism. These results will be helpful for the design and fabrication of ultra-low loss waveguides and integrated photonics in the ultraviolet spectral range.

Engineering↗

Single-Particle Spectroscopy as a Versatile Tool to Explore Lower-Dimensional Structures of Inorganic Perovskites

The remarkable defect tolerant nature of inorganic cesium halide perovskites leading to near unity photoluminescence (PL) quantum yield (QY) and narrow emission linewidth across the entire visible spectrum, have provided a tantalizing platform for a development of a plethora of light-emitting applications. Recently, lower dimensional (2D, 1D, and 0D) perovskites have attracted further attention due to the enhanced thermal, photo and chemical stability as compared to their three-dimensional (3D) analogues. Combination of the external size quantization and internal octahedral organization provides a unique opportunity to study and harness “multidimensional” electronic properties engineered both on atomic scale and the nanoscale. However, crucial research to understand the elementary charge carrier dynamics in lower dimensional perovskites lags far behind the enormous effort to incorporate them into optoelectronic devices. In this Perspective, we provide a review of recent developments that focus on studies of the dynamics of excitonic complexes in Cs-based perovskite nanocrystals using single-particle time-resolved PL spectroscopy and photon correlation measurements. Single photon statistical studies not only offer the unprecedented level of detail to directly assess various recombination pathways but also provide insights into specifics of carrier’s localization. Further, we discuss the underlying physicochemical processes that govern PL emission and draw attention to a number of attributes within this class of the materials, especially lower-dimensional perovskites that may indicate the common origin of the PL emission, as well as provide a route map for the vast unexplored territories where single particle spectroscopy can be a powerful tool to unravel crucial information.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Azimuthal single- and double-spin asymmetries in semi-inclusive deep-inelastic lepton scattering by transversely polarized protons

A comprehensive set of azimuthal single-spin and double-spin asymmetries in semi-inclusive leptoproduction of pions, charged kaons, protons, and antiprotons from transversely polarized protons is presented. These asymmetries include the previously published HERMES results on Collins and Sivers asymmetries, the analysis of which has been extended to include protons and antiprotons and also to an extraction in a three-dimensional kinematic binning and enlarged phase space. They are complemented by corresponding results for the remaining four single-spin and four double-spin asymmetries allowed in the one-photon-exchange approximation of the semi-inclusive deep-inelastic scattering process for target-polarization orientation perpendicular to the direction of the incoming lepton beam. Among those results, significant non-vanishing cos ( Φ–Φ S ) modulations provide evidence for a sizable worm-gear (II) distribution, ${g}_{1\mathrm{T}}^q\left(x,{\mathrm{p}}_T^2\right)$. Most of the other modulations are found to be consistent with zero with the notable exception of large sin ( Φ S ) modulations for charged pions and K + .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Quantum interferometry and pathway selectivity in the nonlinear response of photosynthetic excitons

We propose a time–frequency resolved spectroscopic technique which employs nonlinear interferometers to study exciton–exciton scattering in molecular aggregates. A higher degree of control over the contributing Liouville pathways is obtained as compared to classical light. We show how the nonlinear response can be isolated from the orders-of-magnitude stronger linear background by either phase matching or polarization filtering. Both arise due to averaging the signal over a large number of noninteracting, randomly oriented molecules. We apply our technique to the Frenkel exciton model which excludes charge separation for the photosystem II reaction center. We show how the sum of the entangled photon frequencies can be used to select two-exciton resonances, while their delay times reveal the single-exciton levels involved in the optical process.

Science & Technology - Other Topics↗

Attosecond Intramolecular Scattering and Vibronic Delays

We study the temporal and vibrational signature of the universal nuclear recoil associated with the electron emission and intramolecular scattering that accompanies the photoelectric effect. We illustrate these phenomena in the photoionization of the CO molecule from the C-1s orbital using an analytical model that reproduces the entangled character of the nuclear and electronic motion in this process. We show that the photoelectron emission delay can be decomposed into its localization and resonant-confinement components. Photoionization by a broadband x-ray pulse results in a coherent vibrational ionic state delayed compared to the classical sudden-photoemission limit.

74 ATOMIC AND MOLECULAR PHYSICS↗

Search for anomalous neutral current coherent-like single-photon production in MicroBooNE

This note describes progress towards the first experimental search for neutrino-induced neutral current coherent single-photon production (NC coherent 1γ). The search makes use of data from the MicroBooNE’s 85-tonne active mass liquid argon time projection chamber detector, situated in Fermilab’s Booster Neutrino Beam, with an average neutrino energy of $\langle$E ν $\rangle$ ~ 0.8 GeV. A selection targeted on candidate neutrino interactions with a single photon-like electromagnetic shower in the final state and no visible vertex activity was developed to search for this rare NC coherent 1γ process.

43 PARTICLE ACCELERATORS↗

First Search for Neutral Current Coherent Single-Photon Production in MicroBooNE

This article presents the first search for neutrino-induced neutral current coherent single-photon production (NC coherent 1$\gamma$). The search makes use of data from the MicroBooNE 85-tonne active volume liquid argon time projection chamber detector, situated in the Fermilab Booster Neutrino Beam (BNB), with an average neutrino energy of $\langle E_{\nu}\rangle \sim 0.8$ GeV. A targeted selection of candidate neutrino interactions with a single photon-like electromagnetic shower in the final state and no visible vertex activity was developed to search for the NC coherent 1$\gamma$ process, along with two auxiliary selections used to constrain the dominant background from NC$\pi^0$ production. With an integrated exposure of $6.87 \times 10^{20}$ protons on target delivered by the BNB, we set the world's first limit for this rare process, corresponding to an upper limit on the flux-averaged cross section of $\sigma<1.49 \times 10^{-41}\text{cm}^2$ at 90% C.L.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

A non-Markovian model of avalanche gain statistics for a solid-state photomultiplier

A solid-state photomultiplier (SSPM) capable of continously detecting individual photons of wavelength between 0.4 and 28 microns has recently been disclosed (Petroff et al., 1987). The initial response of the SSPM to single photon is a fast, high-amplitude current pulse of between 10,000 and 100,000 electrons. A phenomenological model of the SSPM avalanche process is presented which successfully predicts the shape of the observed pulse-amplitude distribution by including small history-dependent effects on the carrier transport. The model clarifies the consequences of the electric field strength and the scattering of the electrons for the development of the avalanche in the SSPM.

Laviolette, Randall A.↗

A long-range laser velocimeter for the National Full-Scale Aerodynamics Complex: New developments and experimental application

A long-range laser velocimeter (LV) developed for remote operation from within the flow fields of the large wind tunnels of the National Full-Scale Aerodynamics Complex is described. Emphasis is placed on recent improvements in optical hardware as well as recent additions to data acquisition and processing techniques. The system has been upgraded from a dual-beam, single-color LV with focal range to 10 m, to a dual-beam, two-color LV with focal range to 20 m. At the new extended measurement range (between 10 and 20 m), signals are photon-resolved, and a photon correlation technique is applied to acquire and process the LV signals. This technique permits recovery of the velocity probability distributions at a particular measurement location from which the mean components of velocity and the corresponding normal stress components of turbulence are obtained. The method used for data reduction is outlined in detail, and a discussion of measurement accuracy is made. To study the performance of the LV and verify the measurement accuracy, laboratory measurements were made in the flow field of a 10 cm-diameter, 30-m/sec axisymmetric jet. A discussion of the requirements and techniques used to seed the flow is made, and boundary-layer surveys of mean velocity and turbulence intensity of the streamwise component and the component normal to the surface are presented.

Reinath, Michael S.↗

Mode Multiplexing for Scalable Cavity-Enhanced Operations in Neutral-Atom Arrays

Neutral-atom arrays provide a versatile platform for quantum information processing. However, in large-scale arrays, efficient photon collection remains a bottleneck for key tasks such as fast, nondestructive qubit readout and remote entanglement distribution. We propose a cavity-based approach that enables fast, parallel operations over many atoms using multiple modes of a single optical cavity. By selectively shifting the relevant atomic transitions, each atom can be coupled to a distinct cavity mode, allowing independent simultaneous processing. We present practical system designs that support cavity-mode multiplexing with up to 50 modes, enabling rapid mid-circuit syndrome extraction and significantly enhancing entanglement distribution rates between remote atom arrays. This approach offers a scalable solution to core challenges in neutral-atom arrays, advancing the development of practical quantum technologies.

Aqua, Ziv [Massachusetts Institute of Technology (↗

Rational design of efficient defect-based quantum emitters

Single-photon emitters are an essential component of quantum networks, and defects or impurities in semiconductors are a promising platform to realize such quantum emitters. Here, we present a model that encapsulates the essential physics of coupling to phonons, which governs the behavior of real single-photon emitters, and critically evaluate several approximations that are commonly utilized. Emission in the telecom wavelength range is highly desirable, but our model shows that nonradiative processes are greatly enhanced at these low photon energies, leading to a decrease in efficiency. Our results suggest that reducing the phonon frequency is a fruitful avenue to enhance the efficiency.

Optics↗

Investigation of coherence of niobium-based resonators enabled by a fast-sealing microwave cavity

Resonators and qubits with a niobium (Nb) base metal layer achieve some of the highest coherence times in superconducting quantum devices. The performance of such devices is often limited by loss associated with two-level systems, which are found primarily at material surfaces and interfaces. The metal-air (MA) interface is a major contributor to device loss. In this work, we develop a fast-sealing microwave cavity that enables devices to be placed under vacuum within five minutes of oxide removal, thereby significantly reducing the MA interface loss compared to common device processing and packaging approaches. Using coplanar stripline resonators, we demonstrate that devices sealed in such a cavity exhibit internal quality factors exceeding one million at single-photon power. After re-exposure to air, the devices show downward resonance frequency shifts and quality factor degradations, quantitatively consistent with a model of Nb oxide regrowth. The fast-sealing microwave cavity provides a practical and consistent method to mitigate MA interface loss and sustain high coherence in Nb devices, and establishes a controlled platform for studying metal oxide regrowth kinetics and dielectric properties, the understanding of which is critical to achieving high coherence in superconducting quantum devices.

Zhang, C. [Waterloo U., IQC; Waterloo U.]↗

Using double pulse laser ablation in air to enhance the strength of laser-driven shocks

In the process of multi-pulse laser ablation, inter-pulse delay time, Δ t , is known to be an important parameter for maximizing ablation efficiency as well as impulse imparted to the target. In this work, using photon Doppler velocimetry, we show that for single pairs of colinear pulses (1064 nm, 8 ns, ∼ 60 J cm -2 per pulse) in air, the peak free surface velocity of the back surface of an aluminum target (125 µm thick) is increased, by a factor of nearly 3, when Δ t = 10 microseconds, compared with both pulses arriving simultaneously (Δ t = 0). Fast imaging of the ablation process suggests this enhancement is due to rarefaction of the contiguous air in the passage of the leading shock produced by ablation, which then in turn allows a larger fraction of the energy of the second pulse to reach the target surface. This interpretation is strengthened by additional experiments in which the two pulses do not overlap on the target surface, but the shock strength is nevertheless enhanced. Given a fixed energy budget this work suggests a prescription for maximizing laser-driven shock strength by judicious choice of inter-pulse delay.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measuring signatures in photon angular spectra to distinguish nonlinear Compton scattering models

The collision of a high-energy electron beam with a laser pulse may be used to study radiation reaction and nonlinear Compton scattering among many other processes in strong-field quantum electrodynamics. Predictions from simulation and theory for these interactions rely on a number of approximations and assumptions that have not been experimentally tested. Here, experimentally measurable signatures are identified that might be able to distinguish between radiation reaction models, i.e., classical or quantum, or between the local constant field and local monochromatic approximations used to calculate the properties of the nonlinear Compton process. These signatures are considered through Monte Carlo simulations of various experimental conditions that are relevant to today's laser facilities. Potential detection schemes for measuring the signatures are proposed. We find that single-photon counting of keV photons to resolve harmonics and scintillator-based detection of MeV photons may allow us to validate nonlinear Compton scattering models and radiation reaction models respectively. This will require electron beams with divergence angles less than 2 mrad and less than 20% energy spread.

Russell, Brandon K↗

Superior photodynamic effect of single-walled carbon nanotubes in aprotic media: a kinetic study

It has been confirmed that single-walled carbon nanotubes (SWCNTs) could generate reactive oxygen species in aprotic media by utilizing photon energy. However, the impact of photon irradiation on SWCNTs and the kinetics of the generation process in aprotic media are still unclear, which significantly limits the yield performance. In this work, the kinetics for photodynamic effects has been investigated by performing characterizations on ultraviolet-treated SWCNTs using Raman spectroscopy, conductive atomic force microscope (in-situ), kelvin probe force microscope, and X-ray photoelectron spectroscopy. It is found that ultraviolet-treated SWCNTs are observed to have more defects, lower conductivity, and less surface charge after energy conversion. Starting from the fundamental intrinsic properties of SWCNTs, the kinetics and formation of these changes are thoroughly discussed. It turns out that the dispersion, chirality, and structural integrity of SWCNTs are important for achieving high-performance photodynamic effects, which are validated using several different SWCNTs as well as other carbon nanomaterials. A type of (6,5) s-SWCNTs exhibited the highest energy efficiency among a variety of other carbon nanomaterials. The yield rate is 2.15 mM/h, and the energy consumption is determined to be 2.79 W∙h/mM. This work is expected to help dramatically boost the energy efficiency of the photodynamic effect in aprotic media and pave the way for designing high-performance carbon nanomaterial-based photoinduced devices.

36 MATERIALS SCIENCE↗

Direct Exciton Harvesting from a Bound Triplet Pair

Abstract Singlet fission is commonly defined as the generation of two triplet excitons from a single absorbed photon. However, ambiguities within this definition arise due to the complexity of the various double triplet states that exist in SF chromophores and the corresponding interconversion processes. To clarify this process, singlet fission is frequently depicted as sequential two‐step conversion in which a singlet exciton decays into a bound triplet‐pair biexciton state that dissociates into two “free” triplet excitons. However, this model discounts the potential for direct harvesting from the coupled biexciton state. Here, it is demonstrated that individual triplet excitons can be extracted directly from a bound triplet pair. It is demonstrated that due to the requirement for geminate triplet–triplet annihilation in intramolecular singlet fission compounds, unique spectral and kinetic signatures can be used to quantify triplet‐pair harvesting yields. An internal quantum efficiency for triplet exciton transfer from the triplet pair of >50%, limited only by the solubility of the compounds is achieved. The harvesting process is not dependent on the net multiplicity of the triplet‐pair state, suggesting that an explicit, independent dissociation step is not a requirement for using triplet pairs to do chemical or electrical work.

Chemistry↗

Towards multi-qudit quantum processor using superconducting RF cavities

Superconducting radio-frequency (SRF) cavities made using high-purity Niobium can reach single photon lifetimes longer than a second with proper treatment [1]. These resonator cavities are thus an excellent choice for storing higher-dimensional quantum states. However, preparing and manipulating quantum states with larger photon numbers require a nonlinear component, like a transmon, with a sufficiently long coherence time. With the advancement in materials processing enabling coherence times for transmons exceeding hundreds of micro-seconds, one can encode and process quantum information using d-levels (qudit) of the resonators. In this talk, we will present preliminary results showing the control of a single-qudit and our progress toward building multi-qudit architecture using multi-mode SRF cavities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗