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At least 181 records · Page 10

Identification of an Intrinsic Source of Doping Inhomogeneity in Vapor–Liquid–Solid-Grown Nanowires

The vapor-liquid-solid (VLS) process of semiconductor nanowire growth is an attractive approach to low-dimensional materials and heterostructures because it provides a mechanism to modulate, in situ, nanowire composition and doping, but the ultimate limits on doping control are ultimately dictated by the growth process itself. Under widely used conditions for the chemical vapor deposition growth of Si and Ge nanowires from a Au catalyst droplet, we find that dopants incorporated from the liquid are not uniformly distributed. Specifically, atom probe tomographic analysis revealed up to 100-fold enhancements in dopant concentration near the VLS tri-junction in both B-doped Si and P-doped Ge nanowires. We hypothesize that radial and azimuthal inhomogeneities arise from a faceted liquid-solid interface present during nanowire growth, and we present a simple model to account for the distribution. As the same segregation behavior was observed in two distinct semiconductors with different dopants, the observed inhomogeneity is likely to be present in other VLS grown nanowires.

Environmental Molecular Sciences Laboratory↗

Tuning the magnetoresistance symmetry of Pt on magnetic insulators with temperature and magnetic doping

We present a comparison study of the temperature dependence of the intriguing magnetoresistance (MR) in Pt/YIG (yttrium iron garnet), Pt/YIG BB (the YIG substrate has been bombarded with Ar + ), and Pt/SiO 2 (with different Fe doping levels). With decreasing temperature, the MRs in Pt/YIG and Pt/YIG BB change symmetry from R z = R x > R y at room temperature to R x > R z > R y at low temperature. A similar behavior in both Pt/YIG and Pt/YIG BB implies that the underlying physics is due to magnetic scattering, instead of the pure spin current across the interface. By changing the Fe doping level in the SiO 2 substrate, we can further systematically modulate the symmetry of MR in Pt/SiO 2 (Fe doped). The doping level dependent symmetry can also qualitatively explain the controversy over the MRs of Pt/YIG and similar structures at low temperature.

36 MATERIALS SCIENCE↗

Direct-Write Optical Patterning of P3HT Films Beyond the Diffraction Limit

Doping-induced solubility control is a patterning technique for semiconducting polymers, which utilizes the reduction in polymer solubility upon p-type doping to provide direct, optical control of film topography and doping level. In situ direct-write patterning and imaging are demonstrated, revealing sub-diffraction-limited topographic features. Here, photoinduced force microscopy shows that doping level can be optically modulated with similar resolution.

36 MATERIALS SCIENCE↗

Ionic Tunability of Conjugated Polyelectrolyte Solutions

Conjugated polyelectrolytes (CPEs), which combine a π-conjugated polymer backbone with pendant ionic functionalities, offer an opportunity for electrostatic control of materials properties. In this work, the mesoscale morphology and physical properties of a high-mobility conjugated polyelectrolyte are tuned by the addition of salt, variation of the charge-compensating counterion, and complexation with an oppositely charged polyelectrolyte containing the same π-conjugated backbone. In systems with a single polyelectrolyte species, added ions screen the electrostatic repulsions stabilizing the gel-phase, resulting in the dissolution of ionic cross-links and hydrophobic collapse. Further, exchanging the charge compensating counterion is found to enable finer structural control of the solution behavior and modulation of the self-doping behavior. Finally, novel CPE–CPE complexes resulting in dense solutions and gels of semiconductive material are produced by combination of oppositely charged polyelectrolytes. Such concentrated CPE formulations should be useful materials for mixed electronic–ionic conduction and pseudocapacitative energy storage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A broken translational symmetry state in an infinite-layer nickelate

A defining signature of strongly correlated electronic systems is a rich phase diagram, which consists of multiple broken symmetries, such as magnetism, superconductivity, and charge order. In the recently discovered nickelate superconductors a large antiferromagnetic exchange energy has been reported, which implies the existence of strong electronic correlations. However, signatures of a broken-symmetry state other than superconductivity have not yet been observed. Here, we observe charge ordering in infinite-layer nickelates La 1-x Sr x NiO 2 using resonant x-ray scattering. The parent compound orders along the Ni-O bond direction with an incommensurate wave vector, distinct from the stripe order observed in other nickelates that propagates along a direction 45º to the Ni-O bond. The resonance profile we measure indicates that ordering originates from the nickelate layers and induces a parasitic charge modulation of lanthanum electrons. After doping, the charge order diminishes and its wave vector shifts toward commensurate, indicating that strong electronic correlations are likely to be responsible for the ordered state. Our results suggest that the existence of charge order and its potential interplay with antiferromagnetic fluctuations and superconductivity are important themes in nickel-based superconductors.

36 MATERIALS SCIENCE↗

Anomalous nanoclusters, anisotropy, and electronic nematicity in the doped manganite L a 1 / 3 C a 2 / 3 Mn O 3

In doped manganites, a superlattice (SL) modulation associated with charge/orbital ordering is accepted as a key component in understanding many intriguing properties. It has been reported that the SL modulation always appears on the a axis of the crystals. Here in this study, by using multiple transmission electron microscopic techniques, we observe a type of anomalous nanocluster in which the SL modulation appears on the c axis of La 1/3 Ca 2/3 MnO 3 . By correlating the thermal evolution of the anomalous nanoclusters to other property measurements, we suggest that strain is responsible for the formation of the anomalous nanoclusters. The phase separation and phase transition scenario in La 1/3 Ca 2/3 MnO 3 are also described using electronic-liquid-crystal (ELC) phases. Lastly, an ELC phase diagram in La 1/3 Ca 2/3 MnO 3 is constructed as a function of temperature based on our observations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Helical muon beam cooling channel engineering design

The Helical Cooling Channel (HCC) achieves effective ionization cooling of the six-dimensional (6d) phase space of a muon beam by means of a series of 21st century inventions. In the HCC, hydrogen-pressurized RF cavities enable high RF gradients in strong external magnetic fields. The theory of the HCC, which requires a magnetic field with solenoid, helical dipole, and helical quadrupole components, demonstrates that dispersion in the gaseous hydrogen energy absorber provides effective emittance exchange to enable longitudinal ionization cooling. The 10-year development of a practical implementation of a muon-beam cooling device has involved a series of technical innovations and experiments that imply that an HCC of less than 300 m length can cool the 6d emittance of a muon beam by six orders of magnitude. We describe the design and construction plans for a prototype HCC module based on oxygen-doped hydrogen-pressurized RF cavities that are loaded with dielectric, fed by magnetrons, and operate in a superconducting helical solenoid magnet. The first phase of this project saw the development of a conceptual design for the integration of 805 MHz RF cavities into a 10 T Nb 3 Sn-based HS test section. Two very novel ideas are required to realize the design. The first idea is the use of dielectric inserts in the RF cavities to make them smaller for a given frequency so that the cavities and associated plumbing easily fit inside the magnet cryostat. Calculations indicate that heat loads will be tolerable, while RF breakdown of the dielectric inserts will be suppressed by the pressurized hydrogen gas. The second new idea is the use of a multi-layer Nb 3 Sn helical solenoid. The technology demonstrations for the two aforementioned key components of a 10T, 805 MHz HCC were begun in this project. The work load in the Fermilab Technical Division made it difficult to test a multi-layer Nb 3 Sn solenoid as originally planned. Instead, a complementary project was approved by the DOE Technical Topic Manager to develop magnets for the Mu2e experiment that fit well into the Fermilab Technical Division availability. The difference between the MCC helical solenoid and the Mu2e bent solenoid described in Appendix I is that the helical solenoid is made of coils that are in parallel planes with offset centers, while the coils in the bent solenoid follow the central particle trajectory and look much like a “slinky” toy. The muon-beam cooling-channel technologies developed in this project will enable a muon collider, the next step toward the energy frontier, Higgs/neutrino/Z-factories, and rare muon decay experiments. Commercial uses of the beams made possible by the cooling techniques developed in this project include scanning for nuclear contraband, studies of material properties with spin resonance techniques, and muon-catalyzed fusion.

43 PARTICLE ACCELERATORS↗

Muon Beam Helical Cooling Channel Design

The Helical Cooling Channel (HCC) achieves effective ionization cooling of the six-dimensional (6d) phase space of a muon beam by means of a series of 21st century inventions. In the HCC, hydrogen-pressurized RF cavities enable high RF gradients in strong external magnetic fields. The theory of the HCC, which requires a magnetic field with solenoid, helical dipole, and helical quadrupole components, demonstrates that dispersion in the gaseous hydrogen energy absorber provides effective emittance exchange to enable longitudinal ionization cooling. The 10-year development of a practical implementation of a muon-beam cooling device has involved a series of technical innovations and experiments that imply that an HCC of less than 300 m length can cool the 6d emittance of a muon beam by six orders of magnitude. We describe the design and construction plans for a prototype HCC module based on oxygen-doped hydrogen-pressurized RF cavities that are loaded with dielectric, fed by magnetrons, and operate in a superconducting helical solenoid magnet.

Johnson, Rolland↗

Modeling of the metal–insulator transition temperature in alio-valently doped VO 2 through symbolic regression

The correlated semiconductor vanadium dioxide (VO 2 ) exhibits an insulator–metal transition (IMT) near room temperature, which is of interest in various device applications. Precise IMT temperature control is crucial to determine the use cases across technologies such as thermochromic windows, actuators for robots or neuronal oscillators. Doping the cation or anion sites can modulate the IMT by several tens of degrees and control hysteresis. However, modeling the effects of control parameters (e.g., doping concentration, type of dopants) is challenging due to complex experimental procedures and limited data, hindering the use of traditional data-driven machine learning approaches. Symbolic regression (SR) can bridge this gap by identifying nonlinear expressions connecting key input parameters to target properties, even with small data sets. In this work, we develop SR models to capture the IMT trends in VO 2 influenced by different dopant parameters. Using experimental data from the literature, our study reveals a dual nature of the IMT temperature with varying tungsten (W) doping concentrations. The symbolic model captures data trends and accounts for experimental variability, providing a complementary approach to first-principles calculations. Our feature-driven analysis across a broader class of dopants informs selectivity and provides qualitative insights into tuning phase transition properties valuable for neuromorphic computing and thermochromic windows.

36 MATERIALS SCIENCE↗

P-Type Doping of Mixed Tin–Lead Halide Perovskites Using Electron Transfer to Mo(tfd-COCF3) 3 and F 4 TCNQ

Mixed tin-lead halide perovskites are emerging as promising candidates to address the toxicity issues of lead-based perovskites and to provide additional bandgap tunability for optoelectronic applications. Electron-transfer doping offers a prospective pathway to modulate electronic properties of metal-halide perovskites, while not disturbing the underlying crystal structure. However, limited research exists comparing molecular dopants for these systems. Here, our study investigates the p-type electron-transfer doping of the mixed tin-lead halide perovskite MAPb 0.5 Sn 0.5 I 3 (MA = methylammonium) using a sequential deposition approach (perovskite film followed by dopant incorporation) and the molecular dopants F 4 TCNQ and Mo(tfd-COCF 3 ) 3 . Up to 3 orders of magnitude higher carrier density and up to 2 orders of magnitude greater conductivity are achieved relative to the undoped samples, with F 4 TCNQ and Mo(tfd-COCF 3 ) 3 demonstrating similar doping efficiencies (associated with the ratio of mobile charges added to the number of dopant molecules incorporated) of 0.031(3) % and 0.024(3) %, respectively. Differences in the doping effectiveness for a given molarity doping solution likely follow from variations in dopant incorporation within the film during the spin coating deposition step.

14 SOLAR ENERGY↗

Cubic to tetragonal phase transition of Tm{sup 3+} doped nanocrystals in oxyfluoride glass ceramics

Tm{sup 3+} ions doped β-PbF{sub 2} nanocrystals in oxyfluoride glass ceramics with different doping concentrations and thermal temperatures are prepared by a traditional melt-quenching and thermal treatment method to investigate the structure and the phase transition of Tm{sup 3+} doped nanocrystals. The structures are characterized by X-ray diffraction Rietveld analysis and confirmed with numerical simulation. The phase transitions are proved further by the emission spectra. Both of the doping concentration and thermal temperature can induce an O{sub h} to D{sub 4h} site symmetry distortion and a cubic to tetragonal phase transition. The luminescence of Tm{sup 3+} doped nanocrystals at 800 nm was modulated by the phase transition of the surrounding crystal field.

36 MATERIALS SCIENCE↗

Radioluminescence characterization of in situ x-ray nanodosimeters: Potential real-time monitors and modulators of external beam radiation therapy

Europium-doped yttrium oxide (Y{sub 2}O{sub 3}:Eu) has garnered considerable interest recently for its use as a highly efficient, red phosphor in a variety of lighting applications that include fluorescent lamps, plasma, and field emission display panels, light emitting diodes (LEDs), and lasers. In the present work, we describe the development of Y{sub 2}O{sub 3}:Eu nanoparticles for a very different application: in situ, in vivo x-ray dosimetry. Spectroscopic analyses of these nanoparticles during x-ray irradiation reveal surprisingly bright and stable radioluminescence at near-infrared wavelengths, with markedly linear response to changes in x-ray flux and energy. Monte Carlo modeling of incident flux and broadband, wide-field imaging of mouse phantoms bearing both Y{sub 2}O{sub 3}:Eu nanoparticles and calibrated LEDs of similar spectral emission demonstrated significant transmission of radioluminescence, in agreement with spectroscopic studies; with approximately 15 visible photons being generated for every x-ray photon incident. Unlike the dosimeters currently employed in clinical practice, these nanodosimeters can sample both dose and dose rate rapidly enough as to provide real-time feedback for x-ray based external beam radiotherapy (EBRT). The technique's use of remote sensing and absence of supporting structures enable perturbation-free dosing of the targeted region and complete sampling from any direction. With the conjugation of pathology-targeting ligands onto their surfaces, these nanodosimeters offer a potential paradigm shift in the real-time monitoring and modulation of delivered dose in the EBRT of cancer in situ.

36 MATERIALS SCIENCE↗

Scalable bottom-up synthesis of Co-Ni–doped graphene

Introducing heteroatoms into graphene is a powerful strategy to modulate its catalytic, electronic, and magnetic properties. At variance with the cases of nitrogen (N)– and boron (B)–doped graphene, a scalable method for incorporating transition metal atoms in the carbon (C) mesh is currently lacking, limiting the applicative interest of model system studies. This work presents a during-growth synthesis enabling the incorporation of cobalt (Co) alongside nickel (Ni) atoms in graphene on a Ni(111) substrate. Single atoms are covalently stabilized within graphene double vacancies, with a Co load ranging from 0.07 to 0.22% relative to C atoms, controllable by synthesis parameters. Structural characterization involves variable-temperature scanning tunneling microscopy and ab initio calculations. The Co- and Ni-codoped layer is transferred onto a transmission electron microscopy grid, confirming stability through scanning transmission electron microscopy and electron energy loss spectroscopy. This method holds promise for applications in spintronics, gas sensing, electrochemistry and catalysis, and potential extension to graphene incorporation of similar metals.

Science & Technology - Other Topics↗

TU-F-12A-06: BEST IN PHYSICS (IMAGING) - A Novel Catheter-Based Radionuclide Imaging System to Characterize Atherosclerotic Plaque

Purpose: Atherosclerosis underlies coronary artery diseases, the leading cause of death in the United States and worldwide. In this study, we developed a novel catheter-based radionuclide imaging (CRI) system to image 18F-fluorodeoxyglucose (18F-FDG), a radionuclide, a marker of vascular inflammation, in murine carotid arteries and characterized the system for spatial resolution from multiple scintillating materials. Methods: The catheter system includes 35 mm and 8 mm fixed focal length lenses, which are subsequently connected to a CMOS camera and fiber holder. The distal ferrule of an image bundle is terminated with a wide-angle lens. The novelty of this system is a scintillating balloon with a crystal tip in the front of the wide angle lens to image light from the decay of 18F-FDG emission signal. The scintillating balloon is fabricated from 1mL of silicone RTV catalyst mixed with 1 mL base and 50 mg/mL calcium fluoride doped with Europium (CaF2:Eu). To identify the optimal scintillating materials with respect to resolution, we calculated modulation transfer function (MTF) of Yttrium Aluminum Garnet doped with Cerium (YAG:Ce), anthracene, and CaF2:Eu phosphors using a thin line optical phantom (Fig. 1a-1b). Macrophage-rich FVB murine atherosclerotic carotid plaque model (n = 4) was used in ex vivo experiments. Confirmatory imaging was also performed by an external optical imaging system (IVIS-200). Results: Analysis of the different phosphors (Fig 1b) showed that CaF2:Eu enabled the best resolution of 1.2μm. The CRI system visualized 18F-FDG in atherosclerotic plaques (Fig. 1d). The ligated left carotid (LR) artery exhibited 4× higher 18F-FDG signal intensity compared to the non-ligated right carotid (negative control) artery (1.65×10{sup 2} ±4.07×10{sup 1} vs. 4.44×10{sup 1}±2.17×10{sup 0}, A.U., p = 0.005) and confirmed with IVIS-200 (Fig. 1d). Conclusion: This CRI system enables high-resolution and sensitive detection of 18F-FDG uptake by murine atherosclerotic plaques.

60 APPLIED LIFE SCIENCES↗

Modulation of oxygen vacancies assisted ferroelectric and photovoltaic properties of (Nd, V) co-doped BiFeO 3 thin films

We are reporting on the improved ferroelectric and photovoltaic properties of (Nd3+, V5+) co-doped (Bi0.95Nd0.05)(Fe-1 V-x(x))O-3 (BNFVO) (x = 0.01, 0.03) thin films grown by PLD. BNFVO thin films showed reduced leakage current, lower optical bandgap, and improved ferroelectricity compared to BFO films, which can be explained by valance change and extinguishing oxygen vacancies due to the doping effect. Piezoresponse force microscopy measurements showed an improved domain back switching in doped thin films indicating that the suppression of oxygen vacancies offset the effect of polarization flipping caused by doping. Further, we found a relatively stable and enhanced photovoltaic effect in BNFVO films with an order of magnitude higher photocurrent and almost doubled photovoltage in comparison to BFO films, which can be explained by less recombination between hopping electrons and oxygen vacancies. Our results demonstrate the significance of dopant selection to suppress the oxygen vacancies for improved ferroelectric and photovoltaic properties of BFO films.

Agarwal, Radhe (ORCID:0000000289449423)↗

Studies of anisotropy of iron based superconductors

To study the electronic anisotropy in iron based superconductors, the temperature dependent London penetration depth, Δλ (T), have been measured in several compounds, along with the angular dependent upper critical field, H c2 (T). Study was undertaken on single crystals of Ba(Fe 1-x Co x ) 2 As 2 with x=0.108 and x=0.127, in the overdoped range of the doping phase diagram, characterized by notable modulation of the superconducting gap. Heavy ion irradiation with matching field doses of 6 T and 6.5 T respectively, were used to create columnar defects and to study their effect on the temperature Δλ (T). The variation of the low-temperature penetration depth in both pristine and irradiated samples was fitted with a power-law function Δλ (T) = AT n . Irradiation increases the magnitude of the pre-factor A and decreases the exponent n, similar to the effect on the optimally doped samples. This finding supports the universal s ± scenario for the whole doping range. Knowing that the s ± gap symmetry exists across the superconducting dome for the electron doped systems, we next looked at λ (T), in optimally - doped, SrFe 2 (As 1-x P x ) 2 , x =0.35. Both, as-grown (T c ~ 25 K) and annealed (T c ~ 35 K) single crystals of SrFe 2 (As 1-x P x ) 2 were measured. Annealing decreases the absolute value of the London penetration depth from λ(0) = 300 ± 10 nm in as-grown samples to λ (0) = 275±10 nm. At low temperatures, λ (T) ~ T indicates a superconducting gap with line nodes. Analysis of the full-temperature range superfluid density is consistent with the line nodes, but differs from the simple single-gap d-wave. The observed behavior is very similar to that of BaFe 2 (As 1-x P x ) 2 , showing that isovalently substituted pnictides are inherently different from the charge-doped materials. In-plane resistivity measurements as a function of temperature, magnetic field, and its orientation with respect to the crystallographic ab-plane were used to study the upper critical field, H c2 , of two overdoped compositions of Ba(Fe 1-x Ni x ) 2 As 2 , x=0.054 and x=0.072. Measurements were performed using precise alignment (with accuracy less than 0.1°) of the magnetic field with respect to the Fe-As plane. The dependence of the H c2 on angle θ between the field and the ab- plane was measured in isothermal conditions in a broad temperature range. We found that the shape of the H c2 vs. θ curve clearly deviates from the Ginzburg-Landau theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Studies of anisotropy of iron based superconductors

To study the electronic anisotropy in iron based superconductors, the temperature dependent London penetration depth, Δλ(T), have been measured in several compounds, along with the angular dependent upper critical field, H c2 (T). Study was undertaken on single crystals of Ba(Fe 1-x Co x ) 2 As 2 with x=0.108 and x=0.127, in the overdoped range of the doping phase diagram, characterized by notable modulation of the superconducting gap. Heavy ion irradiation with matching field doses of 6 T and 6.5 T respectively, were used to create columnar defects and to study their effect on the temperature Δλ(T). The variation of the low-temperature penetration depth in both pristine and irradiated samples was fitted with a power-law function Δλ(T) = AT n . Irradiation increases the magnitude of the pre-factor A and decreases the exponent n, similar to the effect on the optimally doped samples. This finding supports the universal s ± scenario for the whole doping range.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗