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“Highly Crystalline Multimetallic Nanoframes with Three Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces Chen Chen et al. Science 343, 1339 (2014); DOI: 10.1126/science.1249061 This copy is for your personal, non-commercial use only. If you wish to distribute this article to others, you can order high-quality copies for your colleagues, clients, or customers by clicking here. Permission to republish or repurpose articles or portions of articles can be obtained by following the guidelines here. The following resources related to this article are available online at www.sciencemag.org (this information is current as of June 10, 2014 ): Updated information and services, including high-resolution figures, can be found in the online on June 10, 2014 version of this article at: http://www.sciencemag.org/content/343/6177/1339.full.html Supporting Online Material can be found at: http://www.sciencemag.org/content/suppl/2014/02/26/science.1249061.DC1.html A list of selected additional articles on the Science Web sites related to this article can be found at: http://www.sciencemag.org/content/343/6177/1339.full.html#related www.sciencemag.org This article cites 38 articles, 9 of which can be accessed free: http://www.sciencemag.org/content/343/6177/1339.full.html#ref-list-1 This article has been cited by 1 articles hosted by HighWire Press; see: http://www.sciencemag.org/content/343/6177/1339.full.html#related-urls This article appears in the following subject collections: Chemistry http://www.sciencemag.org/cgi/collection/chemistry Downloaded from Science (print ISSN 0036-8075; online ISSN 1095-9203) is published weekly, except the last week in December, by the American Association for the Advancement of Science, 1200 New York Avenue NW, Washington, DC 20005. Copyright 2014 by the American Association for the Advancement of Science; all rights reserved. The title Science is a registered trademark of AAAS. REPORTS directions. At low T, in the present classical theory magnetic spin fluctuations (16, 17): With decreasing 23. See supplementary materials on Science Online. 24. M. Le Tacon et al., Nat. Phys. 10,52–58 (2014). without randomness, SF vanishes as T → 0; doping, there is a zero-field quantum critical point x 25. L. Nie, G. Tarjus, S. A. Kivelson, http://arxiv.org/abs/1311.5580. however, pinning of the charge order by impurities to the onset of antiferromagnetic order (38), and 26. D. R. Nelson, J. M. Kosterlitz, Phys. Rev. Lett. 39, is likely responsible for the observed SFx (24, 25). this indicates that our present model will have to 1201–1205 (1977). At high T, our assumption of a T-independent bare be extended to explicitly include spin fluctuations 27. L. Li et al., Phys. Rev. B 81, 054510 (2010). 28. I. Kokanović, D. J. Hills, M. L. Sutherland, R. Liang, rs starts failing at T ≈ 2Tc, and we expect a cross- (39) to apply at such densities. J. R. Cooper, Phys. Rev. B 88, 060505(R) (2013). over to a theory with substantial amplitude fluc- 29. A. Larkin, A. Varlamov, Theory of Fluctuations in tuations and smaller SFx with increasing T. References and Notes Superconductors (Clarendon, Oxford, 2005). Next, we examined the superconducting cor- 1. G. Ghiringhelli et al., Science 337, 821–825 (2012). 30. V. Oganesyan, D. A. Huse, S. L. Sondhi, Phys. Rev. B 73, relations by computing the associated helicity 2. J. Chang et al., Nat. Phys. 8, 871–876 (2012). 094503 (2006). 3. A. J. Achkar et al., Phys. Rev. Lett. 109, 167001 (2012). modulus (Fig. 4). This allows us to determine 31. D. Podolsky, S. Raghu, A. Vishwanath, Phys. Rev. Lett. 99, 4. A. J. Achkar et al., http://arxiv.org/abs/1312.6630. 117004 (2007). Tc by comparing against the expected universal 5. Y. Endoh et al., Phys. Rev. B 37, 7443–7453 (1988). 32. K. Sarkar, S. Banerjee, S. Mukerjee, T. V. Ramakrishnan, – jump (26). We find a Tc below the peak in SFx. 6. B. Keimer et al., Phys. Rev. B 46, 14034 14053 (1992). http://arxiv.org/abs/1309.3776. This is consistent with the arguments in (10), which 7. In La2CuO4, there is long-range antiferromagnetic order 33. V. J. Emery, S. A. Kivelson, Nature 374, 434–437 (1995). below 325 K, but this is entirely due to the interlayer predicted a monotonic decrease in charge order 34. J. Corson, R. Mallozzi, J. Orenstein, J. N. Eckstein, exchange interactions. I. Bozovi, Nature 398, 221 (1999). through Tc: Evidently those computations only 8. S. Chakravarty, B. I. Halperin, D. R. Nelson, Phys. Rev. Lett. 35. Z. A. Xu, N. P. Ong, Y. Wang, T. Kakeshita, S. Uchida, – apply in a narrow window about Tc.Wehavenot 60, 1057 1060 (1988). Nature 406, 486–488 (2000). accounted for interlayer couplings in our two- 9. A. M. Polyakov, Phys. Lett. B 59,79–81 (1975). 36. T. Wu et al., Nat. Commun. 4, 2113 (2013). dimensional theory: These can raise T and yield 10. S. Sachdev, E. Demler, Phys. Rev. B 69, 144504 (2004). 37. S. Banerjee, S. Zhang, M. Randeria, Nat. Commun. 4,1700 c 11. O. Zachar, S. A. Kivelson, V. J. Emery, Phys. Rev. B 57, (2013). a cusplike singularity in the charge order at Tc. 1422–1426 (1998). 38. T. Wu et al., Phys. Rev. B 88, 014511 (2013). One of the fundamental aspects of our theory 12. E. W. Carlson, V. J. Emery, S. A. Kivelson, D. Orgad, in 39. S. Blanco-Canosa et al., Phys. Rev. Lett. 110, 187001 (2013). is that the same set of parameters used above to The Physics of Superconductors Vol II: Superconductivity describe x-ray scattering experiments also predict in Nanostructures, High-Tc and Novel Superconductors, Acknowledgments: We thank A. Chubukov, A. Georges, Organic Superconductors, K. H. Bennemann, J. B. Ketterson, M.-H. Julien, B. Keimer, S. Kivelson, J. Orenstein, and the strength of superconducting fluctuations above Eds. (Springer, Berlin, 2004), pp. 275–452. A. Yacoby for useful discussions. This research was supported Tc. The latter are detectable in diamagnetism mea- 13. S. Sachdev, Rev. Mod. Phys. 75, 913–932 (2003). by the NSF under grant DMR-1103860 and the Natural surements, and indeed YBa2Cu3O6+x shows substan- 14. S. Sachdev, R. La Placa, Phys. Rev. Lett. 111, 027202 (2013). Sciences and Engineering Research Council of Canada. This tial fluctuation diamagnetism (27, 28) over the range 15. S. A. Kivelson, E. Fradkin, V. J. Emery, Nature 393, research was also supported in part by Perimeter Institute 550–553 (1998). of temperatures that x-ray experiments measure for Theoretical Physics; research at Perimeter Institute is 16. M. A. Metlitski, S. Sachdev, Phys. Rev. B 82, 075128 (2010). supported by the Government of Canada through Industry charge-order fluctuations. We compute the dia- 17. K.B.Efetov,H.Meier,C.Pépin,Nat. Phys. 9,442–446 (2013). Canada and by the Province of Ontario through the Ministry magnetic susceptibility in the N = ∞ theory (23). 18. H. Meier, M. Einenkel, C. Pépin, K. B. Efetov, Phys. Rev. B of Research and Innovation. R.G.M. and S.S. acknowledge the Such a theory has effectively Gaussian supercon- 88, 020506(R) (2013). John Templeton Foundation for support. 19. I. Affleck, Z. Zou, T. Hsu, P. W. Anderson, Phys. Rev. B Supplementary Materials ducting fluctuations, albeit with a T dependence 38, 745–747 (1988). www.sciencemag.org/content/343/6177/1336/suppl/DC1 of the superconducting coherence length, which 20. E. Dagotto, E. Fradkin, A. Moreo, Phys. Rev. B 38, Supplementary Text is different from the standard Landau-Ginzburg 2926–2929 (1988). References (40–42) form (29). An absolute comparison of this theory 21. P. A. Lee, N. Nagaosa, X.-G. Wen, Rev. Mod. Phys. 78, 17–85 (2006). 23 September 2013; accepted 21 February 2014 with the observations (28) yields the value of a, 22. S.-C. Zhang, Science 275, 1089–1096 (1997). 10.1126/science.1246310 which is found to differ by about 33% from the value obtained from the charge-order correlation length. Considering the simplicity of the N = ∞ theory, the possible differences in the x-ray and Highly Crystalline Multimetallic diamagnetism samples, and the absence of fitting to determine l and w, this result is encouraging. For a sharper comparison, a Monte Carlo study of the Nanoframes with Three-Dimensional crossover into a vortex-dominated regime (30–32) is needed. Eventually, with a complete study that Electrocatalytic Surfaces also includes the effects of disorder and more 1,2,3 4 1,2 1,2 1,2 2 detailed measurements of charge order and super- Chen Chen, * Yijin Kang, * Ziyang Huo, Zhongwei Zhu, Wenyu Huang, Huolin L. Xin, Joshua D. Snyder,4 Dongguo Li,4 Jeffrey A. Herron,5 Manos Mavrikakis,5 Miaofang Chi,6 Karren L. More,6 conducting correlations on the same sample, we 3 4 1,2 1,2,7,8† 4† expect to be able to more tightly constrain the Yadong Li, Nenad M. Markovic, Gabor A. Somorjai, Peidong Yang, Vojislav R. Stamenkovic values of ga2, wa2, l,anda. Control of structure at the atomic level can precisely and effectively tune catalytic properties of Although we have only applied the theory to materials, enabling enhancement in both activity and durability. We synthesized a highly active and a doping where charge order is most pronounced, durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) we argue that it is characteristic of the entire bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by pseudogap phase. The dominant paradigms for the interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular pseudogap have been phase-fluctuating super- accessibility.
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