DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
  1. Phonon Modulation of Strongly Coupled Gold Tetrahedral Plasmonic Nanoparticles and a Carbocyanine J-Aggregate

    Coupling exciton and plasmon excitations to form polaritons are of high interest for manipulating energy transfer at the nanoscale via the formation of hybrid light-matter states. In this study, we successfully couple gold tetrahedral nanoparticles with the J-aggregate forming dye 5,5′,6,6′-tetrachloro-1,1′-diethyl-3,3′-di(4–sulfobutyl) -benzimidazolocarbocyanine (TDBC) to form a strongly coupled colloidal polariton system with Rabi splitting energies of ~250 meV. These gold tetrahedra exhibit coherent phonon modes upon photoexcitation, which produce transient oscillations of the LSRP energy for isolated tetrahedra. Transient absorption measurements of the polariton system were performed and show how these coherent phonon modes influence coupling between plasmon and excitonmore » resonances. We find that the oscillation period is increased from 22.89 to 23.38 ps upon surface deposition of TDBC dye, indicating sensitivity for mass sensing applications. Shifts in the plasmon resonance due to the coherent phonon modes transiently alters LSPR alignment with the J-aggregate exciton peak, resulting in shifts of the hybrid polariton states’ oscillator strength.« less
  2. Search for the isospin-violating decays χ c J Λ Σ ¯ 0 + c . c . and η c Λ Σ ¯ 0 + c . c .

    Using a sample of ( 2712.4 ± 14.3 ) × 10 6     ψ ( 3686 ) events collected with the BESIII detector, we perform a search for the isospin-violating decays χ c J → Λ Σ ¯   0 + c . c . ( J = 0 , 1 , 2 ) and η c → Λ Σ ¯   0 + c . c . No significant signal for χ c J or η c is observed in the Λ Σ ¯   0 invariant mass distribution. The upper limits on the branching fractions at the 90% confidencemore » level are set to be B ( χ c 0 → Λ Σ ¯   0 + c . c . ) < 1.5 × 10 − 6 , B ( χ c 1 → Λ Σ ¯   0 + c . c . ) < 1.6 × 10 − 6 , B ( χ c 2 → Λ Σ ¯   0 + c . c . ) < 1.7 × 10 − 6 , and B ( η c → Λ Σ ¯   0 + c . c . ) < 6.2 × 10 − 5 for the first time.« less
  3. Statistics of base polytopes in F-theory

    We propose a new statistical ensemble of toric bases for elliptic Calabi-Yaus used in F-theory models, by focusing on only the convex hull of the base, i.e., the base polytope. This physically motivated coarse-graining greatly simplifies the combinatorial complexity of the part of the 4d F-theory landscape with toric bases. We develop a Monte Carlo approach that randomly samples the base polytopes within fixed boxes, with proper statistical weights. We first apply the algorithm to the set of 2d base polytopes, generating an enlarged set of toric 2d bases that include certain types of codimension-two (4,6) points, and we validatemore » our approach against exact numbers. We then explore the set of 3d base polytopes which fit in a set of “maximal” 3d boxes, and estimate the total number of inequivalent 3d base polytopes to be 1085 –1090. We provide statistical data such as the distribution of non-Higgsable gauge groups on these bases. Amusingly, a similar method can also be applied to generate reflexive polytopes in various dimensions. In both the reflexive and base polytope cases, the number of relevant polytopes obeys a Gaussian distribution as a function of the number of vertices, which can be understood in terms of other results on random polytopes in the math literature.« less
  4. 3D analysis of abnormal grain growth in calcia doped alumina in the presence of large pores

    Abnormal grain growth has been previously found to increase with the inclusion of large pores (∼60 µm in diameter) in 80 ppm calcium doped alumina. However, the two-dimensional analysis could not accurately describe the proximity of the abnormal grains and pores to establish a correlation. This study uses laboratory-based diffraction contrast tomography and x-ray computed tomography to spatially map the pores and abnormal grains in 3D. A preference towards the formation of abnormal grains near large pores is found when compared to all potential sites. This finding supports that the pores may be a nucleation site for complexion transitions thatmore » promote abnormal grain growth. The growth of the abnormal grains in a subsequent heat treatment at 1600°C for 16 hrs was also studied. The elongation along the principal axes is similar for both small and large grains, again supporting that abnormal grain growth was facilitated by a complexion transition.« less
  5. Revealing ultrafast proton-transfer mediated autoionization as a source of low energy electrons in hydrogen-bonded systems

    This study combines theory and experiment to probe ultrafast relaxation and dissociation in water dimers following inner- and outer-valence photoionization. By tracking electron and nuclear motion simultaneously, we reveal competing fragmentation pathways that produce low-energy electrons, which are key agents in radiation-induced chemistry, including DNA damage. While low-energy electrons are known to arise via intermolecular Coulombic decay, here we identify a faster relaxation mechanism gated by proton transfer following inner-valence ionization, which we call proton-transfer-mediated autoionization.
  6. Data-Driven Discovery of Bimetallic Nanoparticles Catalysts for the Hydrogenolysis of Polyethylene

    Supported platinum nanoparticles are known to convert polyolefins to high-quality liquid hydrocarbons with hydrogen under relatively mild conditions. However, no systematic study has been undertaken using bimetallic catalysts for polyethylene upcycling. Specifically, a total of 98 monometallic and bimetallic combinations (Ag, Cr, Co, Cu, Fe, Ga, In, Mn, Ni, Pd, Pt, Rh, Ru, Zr) on alumina were synthesized utilizing surface organometallic chemistry (SOMC) technique via robotic platform. These were investigated at a small scale (10 mg of catalyst and 50 mg of polyethylene) for their activity for the hydrogenolysis of polyethylene in a high-throughput batch reactor. Combinations of Ni andmore » Co were selected as candidates with high activity toward conversion into paraffin oils. Reaction conditions were optimized with Ni/Co/Al2O3 catalyst at a larger scale (300 mg catalyst and 3 g polyethylene) to obtain a high yield (93.1%) of paraffin wax with desired properties (Mn = 380 Da) and low polydispersity (Đ = 1.2). Ni/Co/Al2O3 was compared against Co/Ni/Al2O3 to understand the role of the deposition sequence. When Co is deposited before Ni, a layer of cobalt aluminate is formed upon reduction, stabilizing the deposition of 5 nm metallic Ni particles. When nickel is deposited before Co, particles are larger (average >20 nm) and more oxidized (Niδ+ in NiAl2O4), decreasing the availability of the catalytically active metallic Ni. In conclusion, the difference in electronic environments was also described by DFT calculations, which revealed that smaller 3D clusters of Ni are preferred on CoAl2O4 over the 3D clusters on NiAl2O4 and that these smaller clusters are more reducible, as confirmed experimentally.« less
  7. Partial wave analysis of 𝑒+⁢𝑒 → 𝜋+⁢𝜋⁢𝐽/𝜓 and cross section measurement of 𝑒+⁢𝑒 → 𝜋 ± ⁢𝑍𝑐⁢(3900) from 4.1271 to 4.3583 GeV

    Based on 12.0 fb−1 of 𝑒+⁢𝑒 collision data samples collected by the BESIII detector at center-of-mass energies from 4.1271 to 4.3583 GeV, a partial wave analysis is performed for the process 𝑒+⁢𝑒 → 𝜋+⁢𝜋⁢𝐽/𝜓. The cross sections for the subprocesses 𝑒+⁢𝑒 → 𝜋+⁢𝑍𝑐⁢(3900) + c.c. → 𝜋+⁢𝜋⁢𝐽/𝜓, 𝑓0⁡(980)⁢(→ 𝜋+⁢𝜋)⁢𝐽/𝜓, and (𝜋+⁢𝜋)S−wave⁢𝐽/𝜓 are measured for the first time. The mass and width of the 𝑍𝑐⁢(3900)± are determined to be 3884.6 ± 0.7 ± 3.3 MeV/𝑐2 and 37.2 ± 1.3 ± 6.6 MeV, respectively. The first errors are statistical and the second systematic. The final state (𝜋+⁢𝜋)S−wave⁢𝐽/𝜓 dominates the process 𝑒+⁢𝑒more » 𝜋+⁢𝜋⁢𝐽/𝜓. By analyzing the cross sections of 𝜋±⁢𝑍𝑐⁢(3900) and 𝑓0⁡(980)⁢𝐽/𝜓, 𝑌⁡(4220) has been observed. Its mass and width are determined to be 4225.7 ± 4.1 ± 3.4 MeV/𝑐2 and 57.5 ± 9.4 ± 12.1 MeV, respectively.« less
  8. Measurement of the phase between strong and electromagnetic amplitudes in the decay J/ψ → ϕη

    The first direct measurement of the relative phase between the strong and electromagnetic amplitudes for a J/ψ decaying into a vector-pseudoscalar final state is performed using 26 energy points of e+e annihilation data between 3.00 GeV and 3.12 GeV. The data sets were collected by the BESIII detector with a total integrated luminosity of 452 pb−1. By investigating the interference pattern in the cross section lineshape of e+e → ϕη, the relative phase between the strong and electromagnetic amplitudes of J/ψ decay is determined to be within [133°, 228°] at 68% confidence level.
  9. Doping Effects on the Ductility of a Lightweight Refractory High-Entropy Alloy: Grain Boundary and Bulk Lattice Aspects

    Doping elements in small amounts often segregate to grain boundaries (GBs) in alloys and can significantly impact mechanical properties and performance. Refractory high-entropy alloys (RHEAs) are known for their poor ductility, especially at low temperatures. Promoting GB cohesion through segregation can be an effective approach to mitigate embrittlement. Here, in this study, first-principles density functional theory (DFT) calculations were performed to examine the effects of important interstitial dopants (O, B, C, and N) and substitutional dopants (Cr, Y, La, and Ce) on the Σ5(310) [001] tilt GB of a lightweight RHEA Nb32.5Ti27.5Mo22.5Ta12.5Hf2.5Zr2.5. The DFT calculations reveal that certain dopants, suchmore » as B, C, Cr, N, and Y, exhibit favorable GB strengthening effects by improving bonding interactions with the bulk alloy. The impact of doping on the ductility parameter of the bulk lattice, defined as the ratio of surface energy to unstable stacking fault energy for the {110} <111> slip system, was also studied; and the results show that doping reduces the intrinsic ductility of the alloy, decreasing the D-parameter from 2.90 to 2.55, depending on the specific dopant. The present findings provide a foundational understanding at atomic level of the effect of representative dopants on mechanical properties of RHEAs and can be used to guide future alloy design for improved mechanical properties.« less
  10. Superstructural phase transitions in polymer-grafted nanooctahedra

    Superlattices of polyhedral nanocrystals exhibit emergent properties defined by their structural arrangements, but native nanocrystal ligands often limit their programmability. Polymeric ligands address this limitation by enabling tunable nanocrystal softness through modifications of polymer molecular weight and grafting density. Here, we investigate phase transitions in polymer-grafted nanooctahedra by varying polymer length, nanocrystal size, truncation, and ligand density. In two-dimensional superlattices, longer polymers or smaller nanooctahedra induce a transition from orientationally ordered to hexagonal rotator lattices. In three-dimensional superlattices, increasing polymer length drives transitions from Minkowski to body-centered cubic and plastic hexagonal close-packed phases, while higher grafting densities further enable transitionsmore » to simple hexagonal phases. Polymer brush and thermodynamic perturbation theories, supported by Monte Carlo simulations, uncover the entropic and enthalpic forces that govern these transitions. This work highlights the versatility of polymer-grafted anisotropic nanocrystals as building blocks for designing hierarchical superstructures and metamaterials with customizable properties.« less
...

Search for:
All Records
Creator / Author
"Wang, Yi"

Refine by:
Article Type
Availability
Journal
Creator / Author
Publication Date
Research Organization