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88 records · Page 5

Large-scale efficient mid-wave infrared optoelectronics based on black phosphorus ink

The mid-wave infrared (MWIR), ranging from 2 to 5 micrometers, is of substantial interest for chemical sensing, imaging, and spectroscopy. Black phosphorus (bP)–based MWIR light emitters and detectors have been shown to outperform the state-of-the-art for commercial devices due to the low Auger recombination coefficient of bP. However, the scalability of these devices remains a challenge. Here, we report a bP ink formula that preserves the exceptional MWIR optoelectronic properties of bP to deposit centimeter-scale, uniform, and pinhole free films with a photoluminescence quantum yield higher than competing III-V and II-VI semiconductors with similar bandgaps at high excitation regime. As a proof of concept, we use bP ink as a “phosphor” on a red commercial light-emitting diode to demonstrate bright MWIR light emission. We also show that these films can be integrated into heterostructure device architectures with electron and hole selective contacts for direct-injected light emission and detection in MWIR.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum Interference in Two-Atom Resonant X-ray Scattering of an Intense Attosecond Pulse

We theoretically investigate resonant x-ray scattering from two noninteracting Ne+ ions driven by an intense attosecond pulse using a nonrelativistic, QED-based time-dependent framework. Our model includes Rabi oscillations, photoionization, Auger decay, and quantum interference among elastic scattering and resonance fluorescence pathways. We analyze how the total scattering signal depends on pulse intensity, atomic configuration, and initial electronic state. We find that the total resonant scattering yield exceeds its nonresonant counterpart; the angular dependence of the signal qualitatively resembles a two-atom structure factor; and the visibility of interference fringes is sensitive to pulse area and the initial electronic state. Only a subset of final states reached via resonance fluorescence exhibits interference, determined by the indistinguishability of photon emission pathways. Fringe visibility is maximized in the linear scattering regime, where ionization is minimal and resonance fluorescence pathways can be largely indistinguishable. These results highlight optimal conditions for applying ultrafast resonant x-ray scattering to single-particle imaging.

Venkatesh, Akilesh↗

Efficiency Improvement Progress in Green, Yellow and Red III Nitride LEDs

Large improvements in the efficiencies of visible light emitting diodes (LEDs) have been realized over the last decade. Extending the range of wavelengths over which efficient emission can be realized continues to be a goal of active research. Efficiency droop refers to a non-thermal decrease in internal quantum efficiency with increasing current density that affects III-nitride LEDs in general, but more severely those with longer emission wavelengths. The so-called green gap is mainly related to the wavelength dependence of efficiency droop. The peak EQE in commercial green LEDs exceeds 60% but corresponds to a current density that is an order of magnitude lower than required for applications. In this presentation, we will review some of the underlying physics that contribute to the wavelength dependence of droop. We will discuss some challenges in the development of long wavelength III-nitride LEDs and possible strategies to mitigate efficiency droop based on the understanding that nonradiative Auger recombination is the root cause. One general strategy is to engineer the multi-quantum well active region to minimize the average carrier density. Another approach is to design wells with a more favorable balance between the radiative and Auger coefficients. Finally, we will present the current status of the performance of green, yellow and red III-Nitride LEDs.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Role of weak interlayer coupling in ultrafast exciton-exciton annihilation in two-dimensional rhenium dichalcogenides

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS 2 ), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS 2 is still lacking. In this work, we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS 2 . Additionally, we directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS 2 . We attribute this distinct feature in ReS 2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS 2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.

36 MATERIALS SCIENCE↗

Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics

Antimony-119 ( 119 Sb) is one of the most attractive Auger-electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris-catecholate ligand TREN-CAM. Through a combination of radiolabeling, spectroscopic, solid-state, and computational studies, the radiochemistry and structural chemistry of TREN-CAM with 1XX/nat Sb(V) were established. The resulting [ 1XX Sb]Sb–TREN-CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117 Sb, the diagnostic analogue of 119 Sb. These studies revealed marked differences in the uptake and distribution of activity in mice administered unchelated [ 117 Sb]Sb(OH) 6 – versus [ 117 Sb]Sb–TREN-CAM, suggesting that 117 Sb is largely retained by TREN-CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no-carrier-added 1XX Sb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. In conclusion, our results also establish the feasibility of 117 Sb as an elementally matched partner to 119 Sb for theranostic applications.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Electron emission from fluorene (C 13 H 10 ) upon 3.5 MeV/u Si 8+ ion impact: double differential distributions

In this work, we have studied the electron emission from one of the polycyclic aromatic hydrocarbon (PAH) molecules namely, fluorene (C13H10), upon 3.5 MeV/u Si8+ ion impact. The experimentally measured absolute double differential cross sections (DDCS) are compared with the continuum distorted wave-eikonal initial state (CDW-EIS) model and the first Born approximation including correct boundary conditions (CB1). The measurements are carried out in the ejected e⁻-energy range of 1 eV–400 eV and in the angular range of 20°–160°. We have obtained the single differential and the total cross sections (TCSs) of e⁻-emission as well. The CB1 calculation largely underestimates the data. The CDW-EIS model, which is applied for the PAH molecule for the first time, provides an overall better agreement with the double differential, single differential and TCS data. The DDCS data for fluorene has also been compared with that for CH4 molecule, at a few angles. The forward–backward angular asymmetry shows a relatively flatter distribution compared to the theoretical predictions. The contribution due to the giant plasmon resonance could not be clearly observed except a mild indication in the asymmetry parameter. The angular distribution of the carbon KLL Auger electron cross section shows certain variations. The study of the KLL hyper-satellite component indicates the double K-ionization cross section is about 8.6% of the single K-ionization one.

74 ATOMIC AND MOLECULAR PHYSICS↗

Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics

Abstract Antimony‐119 ( 119 Sb) is one of the most attractive Auger‐electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris‐catecholate ligand TREN‐CAM. Through a combination of radiolabeling, spectroscopic, solid‐state, and computational studies, the radiochemistry and structural chemistry of TREN‐CAM with 1XX/nat Sb(V) were established. The resulting [ 1XX Sb]Sb–TREN‐CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117 Sb, the diagnostic analogue of 119 Sb. These studies revealed marked differences in the uptake and distribution of activity in mice administered unchelated [ 117 Sb]Sb(OH) 6 – versus [ 117 Sb]Sb–TREN‐CAM, suggesting that 117 Sb is largely retained by TREN‐CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no‐carrier‐added 1XX Sb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. Our results also establish the feasibility of 117 Sb as an elementally matched partner to 119 Sb for theranostic applications.

Olson, Aeli P. [Department of Medical Physics Univ↗

Colloidal quantum dot lasers

We report semiconductor nanocrystals represent a promising class of solution-processable optical-gain media that can be manipulated via inexpensive, easily scalable colloidal techniques. Due to their extremely small sizes (typically <10 nm), their properties can be directly controlled via effects of quantum confinement; therefore, they are often termed colloidal quantum dots (CQDs). In addition to size-tunable emission wavelengths, CQDs offer other benefits for lasing applications, including low optical-gain thresholds and high temperature stability of lasing characteristics. Recent progress in understanding and practical control of processes impeding light amplification in CQDs has resulted in several breakthroughs, including the demonstration of optically pumped continuous-wave lasing, the realization of optical gain with direct current electrical injection and the development of dual-function electroluminescent devices that also operate as optically pumped lasers. The purpose of this Review is to assess the status of the field of CQD lasing and discuss the existing challenges and opportunities. A particular focus is on approaches for suppressing nonradiative Auger recombination, novel optical-gain concepts enabled by strong exciton-exciton interactions and controlled CQD charging, effects of nanocrystal form factors on light amplification and practical architectures for realizing electrically pumped CQD lasers. This overview suggests that the accumulated knowledge, along with the approaches developed for manipulating the optical-gain properties of colloidal nanostructures, perfectly position the CQD field for successfully addressing a long-standing challenge: the realization of CQD-based laser diodes. Colloidal quantum dots are promising materials for realizing versatile, wavelength-tunable, solution-processed lasers. This Review surveys recent advances in colloidal quantum dot lasing, provides an in-depth analysis of outstanding challenges and discusses a path forward to implementing technologically viable lasing devices.

36 MATERIALS SCIENCE↗

Role of the junction voltage on the overflow current in light-emitting diodes

Quantum-well (QW)-based light emitters, such as light-emitting diodes (LEDs) and lasers, of various semiconductor materials experience a reduction in their efficiency when operating at higher temperatures, a phenomenon referred to as “thermal droop.” Among the various claims on the origins of thermal droop, an increased overflow current with increasing temperatures is a common contender. Since overflow of carriers can only occur when the junction voltage 𝑉 Junction approaches the built-in voltage 𝑉 BI of any diodes, we develop a simple method relating the difference between 𝑉 Junction and 𝑉 BI to approximate the upper limit of overflow occurring in QW-based light-emitting diodes. The measured difference between 𝑉 Junction and 𝑉 BI of state-of-the-art commercial blue and green In⁢Ga⁢N-based LEDs at temperatures up to ∼450 K suggests negligible overflow. To further experimentally verify the absence of overflow, we perform temperature-dependent electron emission spectroscopy on the same commercial blue and green LEDs and find no evidence of thermally enhanced overflow carriers up to ∼450 K. In agreement with our claims that 𝑉 Junction must approach 𝑉 BI for overflow to occur, two-dimensional temperature-dependent electrical simulations of violet, blue, and green LEDs including alloy disorder and V-defects demonstrate that overflow can be significant in violet LEDs, where the small band offset between the In⁢Ga⁢N QW and Ga⁢N cladding layers due to the larger QW bandgap requires larger 𝑉 Junction to reach standard operating current densities, thereby approaching 𝑉 BI . By contrast, simulations indicate that overflow is negligible in blue and green LEDs, whose smaller QW bandgaps result in smaller quasi-Fermi levels difference to reach significant carrier injection, resulting in a 𝑉 Junction much smaller than 𝑉 BI up to large operating current densities. Considering that overflow is negligible in blue and longer-wavelength LEDs, and our observations of the large thermal droop occurring at low current densities, where Shockley-Read-Hall (SRH) recombination dominates, we conclude that thermally enhanced SRH processes are the most significant contributor to thermal droop. Finally, we also simulate the carrier densities in the different QWs of a multiple-QW LED and observe a reduction in the total carrier density at a given operating current density, which results in a decrease in the total Auger-Meitner current of the LED from just the thermally enhanced carrier redistribution among QWs without taking any possible additional temperature dependence of their recombination coefficients. Taking all this into account, minimizing thermal droop effects in LEDs can be achieved by a reduction in defect density, using wider band gap p-n junction-defining cladding layers, and operating at higher currents.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of Quantum Dot Loading on the Radioluminescence Efficiency in Quantum-Dot-Embedded Composites

Nanoparticle-embedded plastic scintillators are an emerging technology for fast, large-area, high-resolution radiation detection and imaging. Here, this study investigates the properties of such composites, focusing on the effects of the quantum dot (QD) concentration on the radioluminescence (RL) intensity, spectra, and dynamics. Experiments using CdSe/CdS QDs in a polymer reveal a superlinear increase in RL with the QD concentration despite optical losses from inner filtering and interparticle interactions. When corrected for inner filtering, RL shows a quadratic concentration dependence, consistent with simple analytical models of improving the secondary electron capture. Practically, the benefits of high QD concentrations are muted by optical losses, but the findings apply to other systems with insulating hosts. In addition to manipulating emission for large effective Stokes shifts, future improvements may come from hosts with higher stopping power and better charge transport, which enable more effective funneling of excitations but without concomitant optical losses associated with high nanoparticle concentrations.

Auger recombination↗

Constraining models for the origin of ultra-high-energy cosmic rays with a novel combined analysis of arrival directions, spectrum, and composition data measured at the Pierre Auger Observatory

The combined fit of the measured energy spectrum and shower maximum depth distributions of ultra-high-energy cosmic rays is known to constrain the parameters of astrophysical models with homogeneous source distributions. Studies of the distribution of the cosmic-ray arrival directions show a better agreement with models in which a fraction of the flux is non-isotropic and associated with the nearby radio galaxy Centaurus A or with catalogs such as that of starburst galaxies. Here, we present a novel combination of both analyses by a simultaneous fit of arrival directions, energy spectrum, and composition data measured at the Pierre Auger Observatory. The model takes into account a rigidity-dependent magnetic field blurring and an energy-dependent evolution of the catalog contribution shaped by interactions during propagation. We find that a model containing a flux contribution from the starburst galaxy catalog of around 20% at 40 EeV with a magnetic field blurring of around 20° for a rigidity of 10 EV provides a fair simultaneous description of all three observables. The starburst galaxy model is favored with a significance of 4.5σ (considering experimental systematic effects) compared to a reference model with only homogeneously distributed background sources. By investigating a scenario with Centaurus A as a single source in combination with the homogeneous background, we confirm that this region of the sky provides the dominant contribution to the observed anisotropy signal. Models containing a catalog of jetted active galactic nuclei whose flux scales with the γ-ray emission are, however, disfavored as they cannot adequately describe the measured arrival directions.

79 ASTRONOMY AND ASTROPHYSICS↗

Large-scale Cosmic-ray Anisotropies with 19 yr of Data from the Pierre Auger Observatory

Results are presented for the measurement of large-scale anisotropies in the arrival directions of ultra–high-energy cosmic rays detected at the Pierre Auger Observatory during 19 yr of operation, prior to AugerPrime, the upgrade of the observatory. The 3D dipole amplitude and direction are reconstructed above 4 EeV in four energy bins. Besides the established dipolar anisotropy in R.A. above 8 EeV, the Fourier amplitude of the 8–16 EeV energy bin is now also above the 5σ discovery level. No time variation of the dipole moment above 8 EeV is found, setting an upper limit to the rate of change of such variations of 0.3% yr$^{−1}$ at the 95% confidence level. Additionally, the results for the angular power spectrum are shown, demonstrating no other statistically significant multipoles. The results for the equatorial dipole component down to 0.03 EeV are presented, using for the first time a data set obtained with a trigger that has been optimized for lower energies. Finally, model predictions are discussed and compared with observations, based on two source emission scenarios obtained in the combined fit of spectrum and composition above 0.6 EeV.

79 ASTRONOMY AND ASTROPHYSICS↗

Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy

Attosecond four-wave mixing (FWM) spectroscopy using an extreme ultraviolet (XUV) pulse and two noncollinear near-infrared (NIR) pulses is employed to measure Rydberg wave packet dynamics resulting from XUV excitation of a 3s electron in atomic argon into a series of autoionizing 3s –1 np Rydberg states ~29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the FWM emission signals of each individually detected state. A wave packet decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s –1 (n + 1) p states to the observed 3s –1 np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. Finally, the theory highlights that coherent amplitude transfer is driven nonresonantly to the 3s –1 np states by the NIR light through 3s –1 (n + 1)s and 3s –1 (n – 1)d dark states during the FWM process.

74 ATOMIC AND MOLECULAR PHYSICS↗

2D Semiconductor Nanosheets Supported on Colloidal Quantum Cubes

Two-dimensional (2D) colloidal nanocrystals bridge the physics of epitaxial quantum wells with the synthetic scalability of solution-processed nanomaterials, making them an attractive platform for future LEDs, lasers, and photodetectors. However, their strongly anisotropic 2D morphology complicates the formation of close-packed films required for electrically interfaced devices. Here, we address this limitation by introducing semiconductor quantum cubes (QCs) in which 2D CdSe nanosheets are conformally grown on six faces of CdS cubic scaffolds. This architecture preserves excitonic physics of quasi-2D nanosheets while leveraging the mechanical rigidity and self-assembly of nanocubes, enabling close-packed films with improved electronic coupling and electrical conductivity. By extending CdS/CdSe QCs into a CdS/CdSe/CdS core/shell/shell structure, we realize 2D quantum wells that exhibit unusual multiexciton behavior. In particular, CdS/CdSe/CdS QCs show repulsive exciton–exciton interactions, which decouple CdSe facets into quasi-independent emitters. This leads to the suppressed Auger recombination, long multiexciton lifetimes, and broadband optical gain. The demonstrated combination of unusual multiexciton photophysics and favorable film self-assembly characteristics in QCs presents opportunities for solution-processed optoelectronic devices.

perovskites↗

Study of scintillation light collection, production and propagation in a 4 tonne dual-phase LArTPC

The 3×1×1 m3 demonstrator is a dual phase liquid argon time projection chamber that has recorded cosmic rays events in 2017 at CERN. The light signal in these detectors is crucial to provide precise timing capabilities. The performance of the photon detection system, composed of five PMTs, are discussed. The collected scintillation and electroluminescence light created by passing particles has been studied in various detector conditions. In particular, the scintillation light production and propagation processes have been analyzed and compared to simulations, improving the understanding of some liquid argon properties.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗