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- ItemA faux hawk fullerene with PCBM-like properties(Cambridge : Royal Society of Chemistry, 2014) San, Long K.; Bukovsky, Eric V.; Larson, Bryon W.; Whitaker, James B.; Deng, S.H.M.; Kopidakis, Nikos; Rumbles, Garry; Popov, Alexey A.; Chen, Yu-Sheng; Wang, Xue-Bin; Boltalina, Olga V.; Strauss, Steven H.Reaction of C60, C6F5CF2I, and SnH(n-Bu)3 produced, among other unidentified fullerene derivatives, the two new compounds 1,9-C60(CF2C6F5)H (1) and 1,9-C60(cyclo-CF2(2-C6F4)) (2). The highest isolated yield of 1 was 35% based on C60. Depending on the reaction conditions, the relative amounts of 1 and 2 generated in situ were as high as 85% and 71%, respectively, based on HPLC peak integration and summing over all fullerene species present other than unreacted C60. Compound 1 is thermally stable in 1,2-dichlorobenzene (oDCB) at 160 °C but was rapidly converted to 2 upon addition of Sn2(n-Bu)6 at this temperature. In contrast, complete conversion of 1 to 2 occurred within minutes, or hours, at 25 °C in 90/10 (v/v) PhCN/C6D6 by addition of stoichiometric, or sub-stoichiometric, amounts of proton sponge (PS) or cobaltocene (CoCp2). DFT calculations indicate that when 1 is deprotonated, the anion C60(CF2C6F5)− can undergo facile intramolecular SNAr annulation to form 2 with concomitant loss of F−. To our knowledge this is the first observation of a fullerene-cage carbanion acting as an SNAr nucleophile towards an aromatic C–F bond. The gas-phase electron affinity (EA) of 2 was determined to be 2.805(10) eV by low-temperature PES, higher by 0.12(1) eV than the EA of C60 and higher by 0.18(1) eV than the EA of phenyl-C61-butyric acid methyl ester (PCBM). In contrast, the relative E1/2(0/−) values of 2 and C60, −0.01(1) and 0.00(1) V, respectively, are virtually the same (on this scale, and under the same conditions, the E1/2(0/−) of PCBM is −0.09 V). Time-resolved microwave conductivity charge-carrier yield × mobility values for organic photovoltaic active-layer-type blends of 2 and poly-3-hexylthiophene (P3HT) were comparable to those for equimolar blends of PCBM and P3HT. The structure of solvent-free crystals of 2 was determined by single-crystal X-ray diffraction. The number of nearest-neighbor fullerene–fullerene interactions with centroid⋯centroid (⊙⋯⊙) distances of ≤10.34 Å is significantly greater, and the average ⊙⋯⊙ distance is shorter, for 2 (10 nearest neighbors; ave. ⊙⋯⊙ distance = 10.09 Å) than for solvent-free crystals of PCBM (7 nearest neighbors; ave. ⊙⋯⊙ distance = 10.17 Å). Finally, the thermal stability of 2 was found to be far greater than that of PCBM.
- ItemTowards low-temperature processing of efficient γ-CsPbI3 perovskite solar cells(London [u.a.] : RSC, 2023) Zhang, Zongbao; Ji, Ran; Hofstetter, Yvonne J.; Deconinck, Marielle; Brunner, Julius; Li, Yanxiu; An, Qingzhi; Vaynzof, YanaInorganic cesium lead iodide (CsPbI3) perovskite solar cells (PSCs) have attracted enormous attention due to their excellent thermal stability and optical bandgap (∼1.73 eV), well-suited for tandem device applications. However, achieving high-performance photovoltaic devices processed at low temperatures is still challenging. Here we reported a new method for the fabrication of high-efficiency and stable γ-CsPbI3 PSCs at lower temperatures than was previously possible by introducing the long-chain organic cation salt ethane-1,2-diammonium iodide (EDAI2) and regulating the content of lead acetate (Pb(OAc)2) in the perovskite precursor solution. We find that EDAI2 acts as an intermediate that can promote the formation of γ-CsPbI3, while excess Pb(OAc)2 can further stabilize the γ-phase of CsPbI3 perovskite. Consequently, improved crystallinity and morphology and reduced carrier recombination are observed in the CsPbI3 films fabricated by the new method. By optimizing the hole transport layer of CsPbI3 inverted architecture solar cells, we demonstrate efficiencies of up to 16.6%, surpassing previous reports examining γ-CsPbI3 in inverted PSCs. Notably, the encapsulated solar cells maintain 97% of their initial efficiency at room temperature and under dim light for 25 days, demonstrating the synergistic effect of EDAI2 and Pb(OAc)2 in stabilizing γ-CsPbI3 PSCs.
- ItemTopological boundaries between helical domains as a nucleation source of skyrmions in the bulk cubic helimagnet Cu2OSeO3(College Park, MD : APS, 2022) Leonov, A.O.; Pappas, C.Cu2OSeO3 represents a unique example in the family of B20 cubic helimagnets with a tilted spiral and a low-temperature skyrmion phase arising for magnetic fields applied along the easy crystallographic (100) axes. Although the stabilization mechanism of these phases can be accounted for by cubic magnetic anisotropy, the skyrmion nucleation process is still an open question, since the stability region of the skyrmion phase displays strongly hysteretic behavior with different phase boundaries for increasing and decreasing magnetic fields. Here, we address this important point using micromagnetic simulations and come to the conclusion that skyrmion nucleation is underpinned by the reorientation of spiral domains occurring near the critical magnetic fields of the phase diagrams: HC1, the critical field of the transition between the helical and conical/tiled spiral phase, and HC2, the critical field between the conical/tiled spiral and the homogenous phase. By studying a wide variety of cases we show that domain walls may have a 3D structure. Moreover, they can carry a finite topological charge stemming from half-skyrmions (merons) also permitting along-the-field and perpendicular-to-the-field orientation. Thus, domain walls may be envisioned as nucleation source of skyrmions that can form thermodynamically stable and metastable lattices as well as skyrmion networks with misaligned skyrmion tubes. The results of numerical simulations are discussed in view of recent experimental data on chiral magnets, in particular, for the bulk cubic helimagnet Cu2OSeO3.
- ItemMicrostructure and elastic deformation behavior of β-type Ti-29Nb-13Ta-4.6Zr with promising mechanical properties for stent applications(Amsterdam : Elsevier B.V., 2019) Plaine, A.H.; Silva, M.R.D.; Bolfarini, C.In this paper, an attempt was made to combine theoretical composition design and thermo-mechanical treatments to produce a metastable β-type titanium alloy with mechanical compatibility for self-expandable stent applications. Metastable β-type Ti-29Nb-13Ta-4.6â»Zr (wt.%) thin-wires with an elastic modulus of 46â»GPa and a yield strength of 920â»MPa were successfully fabricated by cold rolling and low temperature aging. This combination of high yield strength and comparatively low elastic modulus resulted in enhanced elastic recoverable strain of 1.9%, which is much higher than that of the conventional metallic stent materials. The microstructure responsible for the much sought-after mechanical properties was observed to be mainly consisted of a homogeneous distribution of nanometer-sized α-precipitates in a β-phase matrix obtained via a spinodal decomposition of the pre-existed α″-martensite phase through α″â»→â»α″ leanâ»+â»α″ richâ»→â»αâ»+â»β. The α-precipitates increase the strength of the material by hindering the motion of dislocations (spinodal hardening) while the β-matrix with relatively low content of β-stabilizers gives rise to the observed low elastic modulus. More broadly, these findings could be extended to developing advanced metastable β-type titanium alloys for implant and other engineering applications.
- ItemElectrodeposition of nanocrystalline Fe-P coatings: Influence of bath temperature and glycine concentration on structure, mechanical and corrosion behavior(Basel : MDPI AG, 2019) Kovalska, N.; Tsyntsaru, N.; Cesiulis, H.; Gebert, A.; Fornell, J.; Pellicer, E.; Sort, J.; Hansal, W.; Kautek, W.A detailed electrochemical study and investigation of a Fe-P glycine bath as a function of the temperature and glycine concentrations and current density, and their resulting corrosion and mechanical behavior is presented. A low addition of glycine to the electrolyte led to a drastic increase of the P content. At low Fe-P deposition rates, heterogeneous rough deposits with morphological bumps and pores were observed. By increasing the Fe-P deposition rate, the number of pores were reduced drastically, resulting in smooth coatings. Increasing the P content led to the formation of nanocrystalline grains from an "amorphous-like" state. Coatings with higher P contents exhibited better corrosion resistance and hardening, most likely attributed to grain boundary strengthening.
- ItemFate of density waves in the presence of a higher-order van Hove singularity(College Park, MD : APS, 2023) Zervou, Alkistis; Efremov, Dmitry V.; Betouras, Joseph J.Topological transitions in electronic band structures, resulting in van Hove singularities in the density of states, can considerably affect various types of orderings in quantum materials. Regular topological transitions (of neck formation or collapse) lead to a logarithmic divergence of the electronic density of states (DOS) as a function of energy in two dimensions. In addition to the regular van Hove singularities, there are higher-order van Hove singularities (HOVHS) with a power-law divergence in DOS. By employing renormalization group techniques, we study the fate of a spin-density wave phase formed by nested parts of the Fermi surface, when a HOVHS appears in parallel. We find that the phase formation can be boosted by the presence of the singularity, with the critical temperature increasing by orders of magnitude, under certain conditions. We discuss possible applications of our findings to a range of quantum materials such as Sr3Ru2O7, Sr2RuO4, and transition metal dichalcogenides.
- ItemValence effect on the thermopower of Eu systems(College Park, MD : American Physical Society, 2020) Stockert, U.; Seiro, S.; Seiro, S.; Caroca-Canales, N.; Hassinger, E.; Hassinger, E.; Geibel, C.We investigated the thermoelectric transport properties of EuNi2P2 and EuIr2Si2 to evaluate the relevance of Kondo interaction and valence fluctuations in these materials. While the thermal conductivities behave conventionally, the thermopower curves exhibit large values with pronounced maxima as typically observed in Ce- and Yb-based heavy-fermion materials. However, neither the positions of these maxima nor the absolute thermopower values at low temperature are in line with the heavy-fermion scenario and the moderately enhanced effective charge carrier masses. Instead, we may relate the thermopower in our materials to the temperature-dependent Eu valence by taking into account changes in the chemical potential. Our analysis confirms that valence fluctuations play an important role in EuNi2P2 and EuIr2Si2.
- ItemPhononic-magnetic dichotomy of the thermal Hall effect in the Kitaev material Na2 Co2 TeO6(College Park, MD : APS, 2023) Gillig, Matthias; Hong, Xiaochen; Wellm, Christoph; Kataev, Vladislav; Yao, Weiliang; Li, Yuan; Büchner, Bernd; Hess, ChristianThe quest for a half-quantized thermal Hall effect of a Kitaev system represents an important tool to probe topological edge currents of emergent Majorana fermions. Pertinent experimental findings for α-RuCl3 are, however, strongly debated, and it has been argued that the thermal Hall signal stems from phonons or magnons rather than from Majorana fermions. Here, we investigate the thermal Hall effect of the Kitaev candidate material Na2Co2TeO6, and we show that the measured signal emerges from at least two components, phonons and magnetic excitations. This dichotomy results from our discovery that the longitudinal and transversal heat conductivities share clear phononic signatures, while the transversal signal changes sign upon entering the low-temperature, magnetically ordered phase. Our results demonstrate that uncovering a genuinely quantized magnetic thermal Hall effect in Kitaev topological quantum spin liquids such as α-RuCl3 and Na2Co2TeO6 requires disentangling phonon vs magnetic contributions, including potentially fractionalized excitations such as the expected Majorana fermions.
- ItemTransition to the quantum hall regime in InAs nanowire cross-junctions(Bristol : IOP Publ., 2019) Gooth, Johannes; Borg, Mattias; Schmid, Heinz; Bologna, Nicolas; Rossell, Marta D.; Wirths, Stephan; Moselund, Kirsten; Nielsch, Kornelius; Riel, HeikeWe present a low-temperature electrical transport study on four-terminal ballistic InAs nanowire cross-junctions in magnetic fields aligned perpendicular to the cross-plane. Two-terminal longitudinal conductance measurements between opposing contact terminals reveal typical 1D conductance quantization at zero magnetic field. As the magnetic field is applied, the 1D bands evolve into hybrid magneto-electric sub-levels that eventually transform into Landau levels for the widest nanowire devices investigated (width = 100 nm). Hall measurements in a four-terminal configuration on these devices show plateaus in the transverse Hall resistance at high magnetic fields that scale with (ve 2 /h) -1 . e is the elementary charge, h denotes Planck's constant and v is an integer that coincides with the Landau level index determined from the longitudinal conductance measurements. While the 1D conductance quantization in zero magnetic field is fragile against disorder at the NW surface, the plateaus in the Hall resistance at high fields remain robust as expected for a topologically protected Quantum Hall phase. © 2019 IOP Publishing Ltd.