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At least 163 records · Page 9

Light cone dynamics in excitonic states of two-component Bose and Fermi gases

Herein we consider the non-equilibrium dynamics of two-component one dimensional quantum gases in the limit of extreme population imbalance where the minority species has but a single particle. We consider the situation where the gas is prepared in a state with a single spatially localized exciton: the single particle of the minority species is spatially localized while the density of the majority species in the vicinity of the minority particle sees a depression. Remarkably, we are able to consider cases where the gas contains on the order of $N$ = 100 particles, comparable to that studied in experiments on cold atomic gases. We are able to do so by exploiting the integrability of the gas together with the observation that the excitonic state can be constructed through a simple superposition of exact eigenstates of the gas. The number of states in this superposition, rather than being exponentially large in the number of particles, scales linearly with $N$. We study the evolution of such spatially localized states in both strongly interacting Bose and Fermi gases. The behavior of the light cones when the interaction strength and density of the gas is varied can be understood from exact results for the spin excitation spectrum in these systems. We argue that the light cone in both cases exhibits scaling collapse. However unique to the Bose gas, we show that the presence of gapped finite-momentum roton-like excitations provide the Bose gas dynamics with secondary light cones.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Excitons in Bilayer MoS 2 Displaying a Colossal Electric Field Splitting and Tunable Magnetic Response

van der Waals heterostructures composed of transition metal dichalcogenide monolayers (TMDCs) are characterized by their truly rich excitonic properties which are determined by their structural, geometric, and electronic properties: In contrast to pure monolayers, electrons and holes can be hosted in different materials, resulting in highly tunable dipolar many-particle complexes. However, for genuine spatially indirect excitons, the dipolar nature is usually accompanied by a notable quenching of the exciton oscillator strength. Via electric and magnetic field dependent measurements, we demonstrate that a slightly biased pristine bilayer MoS 2 hosts strongly dipolar excitons, which preserve a strong oscillator strength. We scrutinize their giant dipole moment, and shed further light on their orbital and valley physics via bias-dependent magnetic field measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Parton physics from a heavy-quark operator product expansion: Lattice QCD calculation of the fourth moment of the pion distribution amplitude

The pion light-cone distribution amplitude (LCDA) is an essential nonperturbative input for a range of high-energy exclusive processes in quantum chromodynamics. Building on our previous work, the continuum limit of the fourth Mellin moment of the pion LCDA is determined in quenched QCD using quark masses which correspond to a pion mass of 𝑚 𝜋 = 550 MeV. This calculation finds ⟨𝜉 2 ⟩ = 0.202⁢(8)⁢(9) and ⟨𝜉 4 ⟩ = 0.039⁢(28)⁢(11) where the first error indicates the combined statistical and systematic uncertainty from the analysis and the second indicates the uncertainty from working with Wilson coefficients computed to next-to-leading order. These results are presented in the $\overline{\textrm{MS}}$ scheme at a renormalization scale of 𝜇 = 2 GeV.

Detmold, William [Massachusetts Inst. of Technolog↗

Low temperature absolute internal quantum efficiency of InGaN-based light-emitting diodes

A method to reveal low temperature absolute internal quantum efficiency of an InGaN-based light-emitting diode (LED) is reported. Structural (via scanning electron and atomic force microscopies, x-ray diffraction, and Raman spectroscopy) and optical (via temperature- and power-dependent photoluminescence) properties of InGaN-based blue LEDs are coupled with a channel-based recombination model, which reveals the low temperature absolute internal quantum efficiency of the LED on traditional sapphire and emerging Si (111) substrates as 27.5% and 71.1%, respectively. High low-temperature absolute internal quantum efficiency of the former is attributed to its lower defect density and less strain. Furthermore, our results show assuming perfect (i.e., 100%) internal quantum efficiency in an InGaN-based LED at low temperatures could be misleading, and using negative thermal quenching properties of defect luminesce bands with a channel-based recombination model can be a method to quantify LED's less than ideal low temperature internal quantum efficiencies.

36 MATERIALS SCIENCE↗

Room‐Temperature Phosphorescent Platinum(II) Alkynyls with Microsecond Lifetimes Bearing a Strong‐Field Pincer Ligand

Abstract The use of organometallic triplet emitters in organic light emitting diodes (OLEDs) is motivated by the premise of efficient intersystem crossing leading to unit internal quantum efficiencies. However, since most devices are based on solid‐state components, an inherent limitation to square‐planar platinum(II) phosphors is their tendency toward aggregation‐based quenching. Here, a new class of emissive, four‐coordinate Pt II species based on the bisimidazolyl carbazolide (BIMCA) ligand is introduced, which displays highly efficient, long‐lived solid‐state phosphorescence at room temperature. A set of four BIMCAPt phenyl acetylides were synthesized that emit in the green ( λ max =507–540 nm) with >60 % quantum yield and millisecond lifetimes. The structures of the resulting species reveal a non‐planar structure imposed by steric clashes between BIMCA and the iodo or alkynyl co‐ligand. Ground‐state and photophysical characterization are presented. Density functional theory calculations indicate that the BIMCA ligand dominates the frontier orbitals along with the first Franck–Condon singlet and triplet excited states.

Liska, Tadeas↗

Creating Hydride Rim Structures in Zircaloy 4 Cladding Tubes to Mimic High Burnup

During their long service in commercial light water reactors, zirconium alloy cladding tubes are subject to oxidation and subsequent hydrogen pickup which can degrade the materials mechanical properties [1]. These degradations can lead to premature cladding ruptures during reactor power transients [2] as well as negatively impact the claddings post quench ductility following high temperature steam oxidation in thermal hydraulic transients [3]. Hydrogen has low solid solubility in zirconium and usually precipitates as brittle zirconium hydride platelets in the cladding metal matrix. Due to temperature driven diffusion (Soret effect) and the grain texture of stress relieved zirconium metal tubes, these hydrides precipitate with a circumferential orientation near the outer surface of the cladding tubes forming a hydride rim which can serve as a site for crack initiation during circumferential ‘hoop’ loading of the cladding [4rim formation][5]. In order to better understand the effect of hydride rims on the fracture behavior of stress relieved zirconium alloy cladding tubes a procedure to produce these rim-like structures is being developed at Idaho National Laboratory (INL).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Compositional texture engineering for highly stable wide-bandgap perovskite solar cells

The development of highly stable and efficient wide-bandgap (WBG) perovskite solar cells (PSCs) based on bromine-iodine (Br–I) mixed-halide perovskite (with Br greater than 20%) is critical to create tandem solar cells. However, issues with Br–I phase segregation under solar cell operational conditions (such as light and heat) limit the device voltage and operational stability. This challenge is often exacerbated by the ready defect formation associated with the rapid crystallization of Br-rich perovskite chemistry with antisolvent processes. We combined the rapid Br crystallization with a gentle gas-quench method to prepare highly textured columnar 1.75–electron volt Br–I mixed WBG perovskite films with reduced defect density. Here, with this approach, we obtained 1.75–electron volt WBG PSCs with greater than 20% power conversion efficiency, approximately 1.33-volt open-circuit voltage (V oc ), and excellent operational stability (less than 5% degradation over 1100 hours of operation under 1.2 sun at 65°C). When further integrated with 1.25–electron volt narrow-bandgap PSC, we obtained a 27.1% efficient, all-perovskite, two-terminal tandem device with a high V oc of 2.2 volts.

14 SOLAR ENERGY↗

Restricting electron flow at cytochrome b6f when downstream electron acceptors are severely limited

Abstract Photosynthetic organisms frequently experience abiotic stress that restricts their growth and development. Under such circumstances, most absorbed solar energy cannot be used for CO2 fixation and can cause the photoproduction of reactive oxygen species (ROS) that can damage the photosynthetic reaction centers of PSI and PSII, resulting in a decline in primary productivity. This work describes a biological “switch” in the green alga Chlamydomonas reinhardtii that reversibly restricts photosynthetic electron transport (PET) at the cytochrome b6f (Cyt b6f) complex when the capacity for accepting electrons downstream of PSI is severely limited. We specifically show this restriction in STARCHLESS6 (sta6) mutant cells, which cannot synthesize starch when they are limited for nitrogen (growth inhibition) and subjected to a dark-to-light transition. This restriction represents a form of photosynthetic control that causes diminished electron flow to PSI and thereby prevents PSI photodamage but does not appear to rely on a ΔpH. Furthermore, when electron flow is restricted, the plastid alternative oxidase (PTOX) becomes active, functioning as an electron valve that dissipates some excitation energy absorbed by PSII and allows the formation of a proton motive force (PMF) that would drive some ATP production (potentially sustaining PSII repair and nonphotochemical quenching [NPQ]). The restriction at the Cyt b6f complex can be gradually relieved with continued illumination. This study provides insights into how PET responds to a marked reduction in availability of downstream electron acceptors and the protective mechanisms involved.

Plant Sciences↗

Physiological Responses of Populus trichocarpa to Warming

This data set contains empirical physiological, morphological, and chemical data collected over time on Western Black Cottonwood (Populs trichocarpa Torr. & A.Gray ex Hook., Salicaceae) clones, between July and December 2019 at Oak Ridge National Lab. The project was designed to experimentally warm P. trichocarpa clones and assess their physiological acclimation of leaves versus roots. Branch cuttings of the Nisqually-1 genotype were obtained from the US Department of Energy Joint Genome Institute (JGI) in Stanford, California, and propagated in leach tubes. Ninety genetically identical clones were planted into specially constructed mesocosm growth boxes and grown for an initial six weeks in the greenhouse, and then grown at three temperature treatments for ten weeks. The daytime air temperatures of treatments were approximately 25°C, 29°C, and 33°C. Measurements on plant physiology and growth were conducted at various intervals throughout the experiment. This dataset contains nine data files in comma separate (*.csv) format.

54 ENVIRONMENTAL SCIENCES↗

Förster Resonance Energy Transfer and Enhanced Emission in Cs 4 PbBr 6 Nanocrystals Encapsulated in Silicon Nano-Sheets for Perovskite Light Emitting Diode Applications

Encapsulating Cs 4 PbBr 6 quantum dots in silicon nano-sheets not only stabilizes the halide perovskite, but also takes advantage of the nano-sheet for a compatible integration with the traditional silicon semiconductor. Here, we report the preparation of un-passivated Cs 4 PbBr 6 ellipsoidal nanocrystals and pseudo-spherical quantum dots in silicon nano-sheets and their enhanced photoluminescence (PL). For a sample with low concentrations of quantum dots in silicon nano-sheets, the emission from Cs 4 PbBr 6 pseudo-spherical quantum dots is quenched and is dominated with Pb 2+ ion/silicene emission, which is very stable during the whole measurement period. For a high concentration of Cs 4 PbBr 6 ellipsoidal nanocrystals in silicon nano-sheets, we have observed Förster resonance energy transfer with up to 87% efficiency through the oscillation of two PL peaks when UV excitation switches between on and off, using recorded video and PL lifetime measurements. In an area of a non-uniform sample containing both ellipsoidal nanocrystals and pseudo-spherical quantum dots, where Pb 2+ ion/silicene emissions, broadband emissions from quantum dots, and bandgap edge emissions (515 nm) appear, the 515 nm peak intensity increases five times over 30 min of UV excitation, probably due to a photon recycling effect. This irradiated sample has been stable for one year of ambient storage. Cs 4 PbBr 6 quantum dots encapsulated in silicon nano-sheets can lead to applications of halide perovskite light emitting diodes (PeLEDs) and integration with traditional semiconductor materials.

36 MATERIALS SCIENCE↗

Brightening of a dark monolayer semiconductor via strong light-matter coupling in a cavity

Engineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe 2 with spin-forbidden, optically dark ground state. In our experiments, we harness the strong light-matter coupling between cavity photon and the high energy, spin-allowed bright exciton, and thus creating two bright polaritonic modes in the optical bandgap with the lower polariton mode pushed below the WSe 2 dark state. We demonstrate that in this regime the commonly observed luminescence quenching stemming from the fast relaxation to the dark ground state is prevented, which results in the brightening of this intrinsically dark material. We probe this effective brightening by temperature-dependent photoluminescence, and we find an excellent agreement with a theoretical model accounting for the inversion of the band ordering and phonon-assisted polariton relaxation.

36 MATERIALS SCIENCE↗

Tucana B: A Potentially Isolated and Quenched Ultra-faint Dwarf Galaxy at $D$ ≈ 1.4 Mpc*

We report the discovery of Tucana B, an isolated ultra-faint dwarf galaxy at a distance of $D$ = 1.4 Mpc. Tucana B was found during a search for ultra-faint satellite companions to the known dwarfs in the outskirts of the Local Group, although its sky position and distance indicate the nearest galaxy to be ~500 kpc distant. Deep ground-based imaging resolves Tucana B into stars, and it displays a sparse red giant branch consistent with an old, metal-poor stellar population analogous to that seen in the ultra-faint dwarf galaxies of the Milky Way, albeit at fainter apparent magnitudes. Tucana B has a half-light radius of 80 ± 40 pc and an absolute magnitude of ${M}_{V}=-{6.9}_{-0.6}^{+0.5}$ mag (${L}_{V}=({5}_{-2}^{+4})\times {10}^{4}$ L⊙), which is again comparable to the Milky Way's ultra-faint satellites. There is no evidence for a population of young stars, either in the optical color–magnitude diagram or in GALEX archival ultraviolet imaging, with the GALEX data indicating $\mathrm{log}({\mathrm{SFR}}_{\mathrm{NUV}}/{M}_{\odot }\,{\mathrm{yr}}^{-1})\lt -5.4$ for star formation on ≲100 Myr timescales. Given its isolation and physical properties, Tucana B may be a definitive example of an ultra-faint dwarf that has been quenched by reionization, providing strong confirmation of a key driver of galaxy formation and evolution at the lowest mass scales. It also signals a new era of ultra-faint dwarf galaxy discovery at the extreme edges of the Local Group.

79 ASTRONOMY AND ASTROPHYSICS↗

Comparing Pr 3+ and Nd 3+ for deactivating the Er 3+ : 4 I 13/2 level in lanthanum titanate glass

Erbium lanthanum titanate glasses were prepared by levitation melting for the spectroscopic study of ways to promote the mid-infrared fluorescence. Two series of heavily erbium doped glasses (15 wt%) were prepared with the addition of either Pr 3+ or Nd 3+ in amounts relative to Er 3+ of 0.05, 0.1, and 0.2. Both ions quench the lower Er 3+ laser level with the Pr 3+ doing so more rapidly. Although high co-dopant concentrations result in higher energy transfer, as clearly evidenced in upconversion and downconversion fluorescence measurements, the mid-infrared lifetime also suffers a reduction and, therefore, a balance must be struck in the co-dopant concentration. Lifetime and spectral measurements indicate that, at a fixed relative co-dopant amount, Pr 3+ is more effective than Nd 3+ at removing the bottleneck of the Er 3+ 4 I 13/2 level. Moreover, consideration of the lifetimes alongside the absorption data of the individual ions indicates that despite the large absorption cross-section of Nd 3+ at 808 nm, the concentration needed to yield more absorbed power than utilizing direct 976 nm excitation of Er 3+ results in unfavorable lifetimes of the mid-infrared transition. In the end, Pr 3+ prevails as the superior co-dopant in terms of the effects on fluorescence lifetimes as well as potential laser system design considerations. In a unique self-doping approach, a reducing melt atmosphere of Ar instead of O 2 creates a small fraction of Ti 3+ . In 5Er 2 O 3 -12La 2 O 3 -83TiO 2 glass, the presence of Ti 3+ quenches the 4 I 13/2 emission about 2.6 times more than the 4 I 11/2 when lifetimes are compared to an O 2 melt environment. As an additional means of increasing the mid-infrared emission, the effect of temperature on the mid- and near- infrared lifetimes of a lightly doped lanthanum titanate composition is investigated between 77-300 K. The mid-infrared lifetime increases by ∼30% while the near-infrared lifetime increases by ∼10%, which suggests in addition to co-doping, active cooling of the gain media will further enhance performance.

Materials Science↗

Reductive Dynamic and Static Excited State Quenching of a Homoleptic Ruthenium Complex Bearing Aldehyde Groups

A new homoleptic Ru polypyridyl complex bearing two aldehyde groups on each bipyridine ligand, [Ru(dab) 3 ](PF 6 ) 2 , where dab is 4,4′-dicarbaldehyde-2,2′-bipyridine, was synthesized, characterized, and utilized for iodide photo-oxidation studies. In acetonitrile (CH 3 CN) solution, the complex displayed an intense metal-to-ligand charge transfer (MLCT) absorbance maximum at 475 nm (ε = 22,000 M –1 cm –1 ) and an infrared (IR) band at 1712 cm –1 assigned to the pendent aldehyde groups. Visible light excitation in air-saturated solution resulted in room temperature photoluminescence (PL) with a maximum at 675 nm, a quantum yield, ϕ PL = 0.048, and an excited state lifetime, τ ο = 440 ns, from which radiative and nonradiative relaxation rate constants were extracted, k r = 9.1 × 10 4 s –1 and knr = 1.8 × 10 6 s –1 . Pulsed visible light excitation yielded transient UV–vis and IR absorption spectra consistent with an MLCT excited state; relaxation occurred with the maintenance of two isosbestic points in the visible region, and a lifetime that agreed with that measured by time-resolved PL. Cyclic voltammetry studies in a CH 3 CN solution with 0.1 M TBAPF 6 electrolyte revealed a quasi-reversible oxidation, E°(Ru III/II ) = +1.25 V vs. Fc +/0 , and three sequential one-electron reductions at −1.10, −1.25, and −1.54 V vs. Fc +/0 . Here, an excited state reduction potential of E°(Ru *2+/+ ) = +0.89 V vs. Fc +/0 was estimated with the Rehm–Weller expression. Titration of tetrabutylammonium iodide, TBAI, into a CD 3 CN solution of [Ru(dab) 3 ](PF 6 ) 2 resulted in significant shifts in the aldehyde H atom and 3,3′-biypridyl resonances that were analyzed with a 1:1 equilibrium model, from which K eq = 460 M –1 was extracted, increasing to 5800 M –1 when the solvent was changed to acetone-d 6 . Iodide titrations resulted in a significant quenching of the [Ru(dab) 3 ] *2+ lifetime and quantum yield in both CH 3 CN and acetone solvents. In CH 3 CN, the quenching was mainly dynamic and well described by the Stern–Volmer model, from which a quenching rate constant, k q , of 4.5 × 10 10 M –1 s –1 and an equilibrium constant, K eq , of 8.3 × 10 3 M –1 were obtained. In acetone, the static quenching pathway by iodide was greatly enhanced, with a K eq of 1.2 × 10 4 M –1 and a higher k q of 9.2 × 10 10 M –1 s –1 .

Aldehydes↗

Understanding the Nature of an Unusual Post-starburst Quasar with Exceptionally Strong Ne v Emission

We present a z = 0.94 quasar, SDSS J004846.45-004611.9, discovered in the Sloan Digital Sky Survey III (SDSS-III) BOSS survey. A visual analysis of this spectrum reveals highly broadened and blueshifted narrow emission lines, in particular, [Ne v] λ3426 and [O III ] λ5007, with outflow velocities of 4000 km s -1 , along with unusually large [Ne v] λ3426/[Ne III ] λ3869 ratios. The gas shows higher ionization at higher outflow velocities, indicating a connection between the powerful outflow and the unusual strength of the high ionization lines. The spectral energy distribution and the i – W3 color of the source reveal that it is likely a core extremely red quasar (ERQ); a candidate population of young active galactic nuclei (AGN) that are violently blowing out gas and dust from their centers. The dominance of host galaxy light in its spectrum and its fortuitous position in the SDSS S82 region allows us to measure its star formation history and investigate variability for the first time in an ERQ. Our analysis indicates that SDSS J004846.45-004611.9 underwent a short-lived starburst phase 400 Myr ago and was subsequently quenched, possibly indicating a time lag between star formation quenching and the onset of AGN activity. We also find that the strong extinction can be uniquely attributed to the AGN and does not persist in the host galaxy, contradicting a scenario where the source has recently transitioned from being a dusty submillimeter galaxy. In our relatively shallow photometric data, the source does not appear to be variable at 0.24–2.4 μm in the rest frame, most likely due to the dominant contribution of host galaxy starlight at these wavelengths.

79 ASTRONOMY AND ASTROPHYSICS↗

Single-Molecule Fluorescence Microscopy Reveals Energy Transfer Active versus Inactive Nanocrystal/Dye Conjugate Pairs

Defect-mediated energy transfer (EnT) is a radiative process that occurs between donor defect states in the forbidden bandgap of semiconductor nanocrystals (NCs) and dye molecules bound to their surfaces. The EnT efficiency depends on the number of dye molecules attached to each NC, the donor–acceptor distance, and the dipole orientation factor between the donor and acceptor, all of which vary across all individual NCs in a sample. While ensemble-level fluorescence spectroscopy measurements have provided average values for donor–acceptor distances, dye-to-NC ratios, and EnT rate constants, questions remain about the impact of donor/acceptor heterogeneity on observed EnT efficiencies. Notably, ensemble-level measurements cannot distinguish between bare NCs and EnT-active versus inactive NC/dye pairs in the same sample batch, limiting the ability to design systems with 100% EnT efficiency. To address this, we studied defect-mediated EnT between AlexaFluor 555 dye acceptors chemically bound to ZnO NC donors at the level of single molecules and single NCs. Interestingly, 20% of bound NC/dye pairs are EnT-inactive, likely contributing to residual defect photoluminescence (PL) observed in ensemble-level measurements and reducing overall EnT efficiency. Single particle-level ZnO defect PL and acceptor fluorescence trajectories exhibited distinct microfluctuations, which are absent in bare ZnO NCs. We hypothesized that our observations can be explained with a competitive dye fluorescence quenching pathway, possibly due to charge transfer between the excited state dye and the ZnO NC. Numerical simulations of single-molecule PL traces for this scenario produced microfluctuations consistent with the experimental results. These findings highlight the impact of sample heterogeneity on EnT processes and provide insights for designing light-harvesting systems with optimized EnT efficiency.

25 ENERGY STORAGE↗

Magnetic field frustration of the metal-insulator transition in V 2 O 3

Despite decades of efforts, the origin of metal-insulator transitions (MITs) in strongly correlated materials remains one of the main long-standing problems in condensed-matter physics. An archetypal example is V 2 O 3 , which undergoes simultaneous electronic, structural, and magnetic phase transitions. This remarkable feature highlights the many degrees of freedom at play in this material. In this work, acting solely on the magnetic degree of freedom, we reveal an anomalous feature in the electronic transport of V 2 O 3 : On cooling, the magnetoresistance changes from positive to negative values well above the MIT temperature, and shows divergent behavior at the transition. In this work, the effects are attributed to the magnetic field quenching antiferromagnetic fluctuations above the Néel temperature $T_N$, and preventing long-range antiferromagnetic ordering below $T_N$. In both cases, suppressing the antiferromagnetic ordering prevents the opening of the incipient electronic gap. This interpretation is supported by Hubbard model calculations which fully reproduce the experimental behavior. Our study sheds light on this classic problem providing a clear and physical interpretation of the nature of the metal-insulator transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Negative thermal quenching of photoluminescence in a copper–organic framework emitter

Negative thermal quenching (NTQ), an abnormal phenomenon that the intensity of photoluminescence (PL) increases with increasing temperature, has essentially been restricted to either bulk semiconductors or very low temperatures. Here, we report a delayed fluorescence copper–organic framework exhibiting negative thermal quenching (NTQ) of photoluminescence, which is driven by the fluctuation between the localized and delocalized form of its imidazole ligand. The process is completely reversible on cooling/heating cycles. This study opens a new avenue to explore the electronically switchable NTQ effect in coordination networks and further to develop the NTQ-based light-emitting diodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗