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Commentary: Nanoarchitectonics— Think about NANO againKatsuhiko Ariga, Yusuke Yamauchi, and Masakazu Aono Citation: APL Materials 3, 061001 (2015); doi: 10.1063/1.4922549 View online: http://dx.doi.org/10.1063/1.4922549 View Table of Contents: http://scitation.aip.org/content/aip/journal/aplmater/3/6?ver=pdfcov Published by the AIP Publishing Articles you may be interested in Commentary: What I think about Now Phys. Today 67, 8 (2014); 10.1063/PT.3.2290 Thinking About Bernoulli Phys. Teach. 45, 379 (2007); 10.1119/1.2768700 Thinking about the Universe Phys. Part. Nucl. 29, 213 (1998); 10.1134/1.953066 Thinking small about energy Phys. Today 31, 87 (1978); 10.1063/1.3001841 Enchanting things to think about Phys. Teach. 15, 296 (1977); 10.1119/1.2339636

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APL MATERIALS 3, 061001 (2015)

Commentary: Nanoarchitectonics—Think about NANO again

Katsuhiko Ariga, Yusuke Yamauchi, and Masakazu AonoWorld Premier International (WPI) Research Center for Materials Nanoarchitectonics(MANA), National Institute for Materials Science (NIMS), 1-1 Namiki,Tsukuba 305-0044, Japan

(Received 9 May 2015; accepted 3 June 2015; published online 16 June 2015)

[http://dx.doi.org/10.1063/1.4922549]

Undoubtedly, nanotechnology has been a key concept in the scientific community since thelate 20th century and has significantly promoted the current science and technology. However, ifwe want to further develop materials science, we need to think about NANO again, as nanoscalephenomena appear to be more complex than we have expected. Based on the rapid progress ofobservation tools, such as various probe microscopes, we can now observe, analyze, and evenmanipulate objects at the nanoscale level. We can fabricate microscopic objects under conditionssimilar to the macroscopic regime, because in the micrometer-scale, objects are basically free fromuncertainties such as thermal and statistical fluctuations or quantum effects. The control and assem-bly of nanoscale objects are, however, not fully mastered yet, and their behaviors are still not wellunderstood.1 The control over these components at the nanometer scale requires the combinationof physical and chemical interactions. The ways to handle nano-materials should be different fromthose known for microtechnology. We must discard our initial expectations to establish nano-scaletechnology by a simple extension of microtechnology.

The stimulation of a paradigm shift and/or the creation of a new path of research are ofteneffectively induced through the proposal of new concepts. For example, the single term nanotech-nology undoubtedly successfully motivated current extensive research trends in small-scale scienceand technology. Although we only recognized the importance of nanotechnologies in the past fewdecades, theories, observation apparatuses, and fabrication tools related to the nanoscale worldhave been well innovated before the popularization of the term nanotechnology. All these separateefforts were combined into a bigger flow, united by this single concept, quoting, for example,words from Richards Feynman, proposals from Kim Eric Drexler, and politic statements from BillClinton. These historical facts indicate that clarifying a key concept, such as nanotechnology, cansuccessfully activate, facilitate, and motivate the development of science and technology.

The “post-nanotechnology era” now requires new concepts to be proposed. For example, aparadigm shift in house and building construction from carpenter work, such as cutting materialsand attaching parts, to architectonics was achieved in our living world. A similar conceptual changehas to be initiated in the nanoscale world, from nanotechnology to nanoarchitectonics.2 The termi-nology of this concept was first proposed by Masakazu Aono in the year 2000 at the 1st Interna-tional Symposium on Nanoarchitectonics Using Suprainteractions in Tsukuba, Japan. This involvesthe preparation of functional materials and fabrication of advanced systems by the harmonizationof various actions, including accurate control of atomic and molecular arrangements, chemistry-based (reaction-based) materials conversion, spontaneous self-assembly/organization, and controlover the structure through the application of various physical stimuli. The obtained materials wouldthen sometimes show unexpected properties due to mutual interactions between the componentsand various nanoscale uncertainties.

As mentioned above, nanoarchitectonics is a basic concept that covers a wide range of sci-ence and technology. Recent literature on nanoarchitectonics deals with various research sub-jects, including (i) materials innovation such as supramolecular assemblies,3 nanostructured mate-rials,4 and nanocarbons,5 (ii) fabrication of nanostructures with both organic and inorganic compo-nents,6 (iii) advanced applications such as sensing,7 batteries,8 catalysis,9 and capacitors,10 and

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061001-2 Ariga, Yamauchi, and Aono APL Mater. 3, 061001 (2015)

FIG. 1. Functional systems with nanoarchitectonic design at various dimensions: (a) atomic-level, (b) materials level, and(c) dimension-bridging.

(iv) fundamentals and applications in bio- and medical fields.11 In order to exemplify innovativetopics initiated by nanoarchitectonics, three challenges are briefly explained below.

Atomic-level nanoarchitectonic switch designs have been developed based on nanoscopicarrangements of metal and semiconductor materials and atomic diffusion upon electrochemicalreactions (Figure 1(a)).12 They include non-volatile three-terminal atomic transistor, on-demandfunction-selectable atomic switch, and synapse-like atomic switch junction. These switches oftenshow unusual behaviour that is totally different from what is observed in macroscopic electri-cal switches. Moreover, they are not based on simple ON/OFF operations. For example, thesynapse-like atomic switch junction can show two types of plasticity: short-term plasticity andlong-term potentiation. Their operation is based on non-digital chemical reactions, and their switch-ing behaviour is far from linear. For example, the junction remains switched off if the voltage pulsesare input at low frequencies, while it switches on when several voltage pulses with a sufficientlyhigh frequency are used. The observed switching behaviour is conceptually close to brain functionsin contrast to conventional artificial switches. This stimulates further developments toward newartificial neuromorphic computational systems without any pre-programming.

Typical features to architect materials with nanosized components can be seen in materialssynthesis from various kinds of nanosheets. In these strategies, nanosheets with different prop-erties can be assembled into layer-structured materials with a specific sequence, which oftenshows novel functions in individual components.13 In addition, controlling the inter-sheet dis-tance upon appropriate physical/chemical inputs, such as swelling,14 can lead to the fabrication of




FIG. 2. FWCI of research institutions in the world. Source: SciVal database, Elsevier B.V. (downloaded at the beginning of2015).

structure-controlled soft-materials, such as sheet-included polymer gels.15 The example illustratedin Figure 1(b) is an architected gel composite with oriented nanosheet components, which exhibithighly anisotropic mechanical properties. Applying a strong magnetic field induces the alignmentof titanate charged nanosheets inside the polymer gel. This special orientation can be fixed bycross linking. The compression of the composite can be suppressed when an orthogonal force isapplied, while lateral deformation can be easily induced through parallel shear forces. Surpris-ingly, this exotic material is constructed from rather simple components, nanosheets and polymers,through harmonizing multiple kinds of physical principles, self-organization, alignment in externalmagnetic field, and chemical reaction.

Architecting functional components makes it possible to control dynamically harmonized ac-tions of functional objects such as molecular machines. In the example of Figure 1(c), molecularmachines were placed at the dynamic air-water interface, where macroscopic mechanical stimuli(compression and expansion) can be applied only in a lateral direction and induce harmonizedmotion of the molecular machines within a two-dimensional plane.16 In this quasi-two-dimensionalarchitecture, in-plane directions of molecularly thin films have macroscopically visible dimensions,but the film thickness is restricted to the molecular scale. This two-dimensional nanoarchitecton-ics actually connects macroscopic mechanical motions and molecular-level functionalities. In thisparticular case, molecular machines such as reversible capture and release of guest molecules canbe operated by macroscopic operations such as hand-level motions. Similar systems enable us tofinely tune molecular receptor structures upon mechanical motions to realize precise discrimina-tions of amino acids17 and nucleotides.18 These unusual techniques can bridge systems within abillionth-of-a-meter length scale, which is why they are named as hand-operating nanotechnol-ogies.19

Finally, the impact of proposing nanoarchiectonics is here measured from indirect-researchviewpoints using statistical parameters. Recently, Elsevier introduced a new indicator called Field-Weighted Citation Impact (FWCI) that can normalize citation counts depending on the level offocus in corresponding fields. By using this parameter, comparing the quality of papers of individual




research centers in different fields becomes possible. As expected, top-ranked universities suchas Massachusetts Institute of Technology (MIT), University of California Berkeley, and HarvardUniversity show high FWCI values (Figure 2). For example, the calculated FWCI values for MITand Research Center for Materials Nanoarchitectonics (MANA) are both around 2.5, which meansthat the papers published from these institutes are cited almost 150% more than expected from theworld average (FWCI = 1). The presented statistical data provide evidence that approaches basedon nanoarchitectonics have successfully created a world-top-level research impact within these lastfew years. The elaboration of this new research concept in the research community has now becomean accomplishment that is hard to ignore. In nano-research, nanoarchitectonics has provided a newparadigm that goes beyond the previously established concepts of nanotechnology. Let us thinkabout NANO again with nanoarchitectonics.1 M. Magoga and C. Joachim, Phys. Rev. B 59, 16011 (1999); U. M. B. Marconi, A. Puglisi, L. Rondoni, and A. Vulpiani, Phys.

Rep. 461, 111 (2008); P. Haenggi and F. Marchesoni, Rev. Mod. Phys. 81, 387 (2009); H. Vazquez, R. Skouta, S. Schneebeli,M. Kamenetska, R. Breslow, L. Venkataraman, and M. S. Hybertsen, Nat. Nanotechnol. 7, 663 (2012); P. Karagiannis, Y.Ishii, and T. Yanagida, Chem. Rev. 114, 3318 (2014).

2 M. Aono, Sci. Technol. Adv. Mater. 12, 040301 (2011); K. Ariga, M. Li, G. J. Richards, and J. P. Hill, J. Nanosci. Nanotech-nol. 11, 1 (2011); K. Ariga, Q. Ji, W. Nakanishi, J. P. Hill, and M. Aono, “Nanoarchitectonics: A new materials horizon fornanotechnology,” Mater. Horiz. (in press).

3 M. Ramanathan, L. K. Shrestha, T. Mori, Q. Ji, J. P. Hill, and K. Ariga, Phys. Chem. Chem. Phys. 15, 10580 (2013); M.Ramanathan, K. L. Hong, Q. Ji, Y. Yonamine, J. P. Hill, and K. Ariga, J. Nanosci. Nanotechnol. 14, 390 (2014); H. Hamoudi,Nanoscale. Res. Lett. 9, 287 (2014); M. Pandeeswar and T. Govindaraju, J. Inorg. Organomet. Polym. Mater. 25, 293 (2015).

4 S. Hecht, Angew. Chem. Int. Ed. 42, 24 (2003); K. Ariga, A. Vinu, Y. Yamauchi, Q. Ji, and J. P. Hill, Bull. Chem. Soc. Jpn.85, 1 (2012); L. Zerkoune, A. Angelova, and S. Lesieur, Nanomaterials 4, 741 (2014).

5 L. K. Shrestha, Q. Ji, T. Mori, K. Miyazawa, Y. Yamauchi, J. P. Hill, and K. Ariga, Chem. - Asian J. 8, 1662 (2013); H.Hamoudi, RSC Adv. 4, 22035 (2014); H. Pan, S. Zhu, and L. Mao, J. Inorg. Organomet. Polym. Mater. 25, 179 (2015).

6 K. Wang, K. Galatsis, R. Ostroumov, A. Khitun, Z. Zhao, and S. Han, Proc. IEEE 96, 212 (2008); K. Ariga, M. V. Lee, T.Mori, X.-X. Yu, and J. P. Hill, Adv. Colloid Interface Sci. 154, 20 (2010); K. Ariga, Q. Ji, J. P. Hill, Y. Bando, and M. Aono,NPG Asia Mater. 4, e17 (2012); T. Govindaraju and M. B. Avinash, Nanoscale 4, 6102 (2012); T. Mori, K. Sakakibara, H.Endo, M. Akada, K. Okamoto, A. Shundo, M. V. Lee, Q. Ji, T. Fujisawa, K. Oka, M. Matsumoto, H. Sakai, M. Abe, J. P. Hill,and K. Ariga, Langmuir 29, 7239 (2013); K. Ariga, T. Mori, and J. P. Hill, ibid. 29, 8459 (2013); K. Ariga, Y. Yamauchi, G.Rydzek, Q. Ji, Y. Yonamine, K. C.-W. Wu, and J. P. Hill, Chem. Lett. 43, 36 (2014); S. Cordier, F. Grasset, Y. Molard, M.Amela-Cortes, R. Boukherroub, S. Ravaine, M. Mortier, N. Ohashi, N. Saito, and H. Haneda, J. Inorg. Organomet. Polym.Mater. 25, 189 (2015).

7 K. Ariga, Y. Yamauchi, Q. Ji, Y. Yonamine, and J. P. Hill, APL Mater. 2, 030701 (2014); S. Ishihara, J. Labuta, W. VanRossom, D. Ishikawa, K. Minami, J. P. Hill, and K. Ariga, Phys. Chem. Chem. Phys. 16, 9713 (2014).

8 K. Takada, Langmuir 29, 7538 (2013); K. Takada, N. Ohta, and Y. Tateyama, J. Inorg. Organomet. Polym. Mater. 25, 205(2015).

9 C.-M. Puscasu, E. M. Seftel, M. Mertens, P. Cool, and G. Carja, J. Inorg. Organomet. Polym. Mater. 25, 259 (2015).10 R. Rajendran, L. K. Shrestha, K. Minami, M. Subramanian, R. Jayavel, and K. Ariga, J. Inorg. Organomet. Polym. Mater.

25, 18480 (2015); R. Rajendran, L. K. Shrestha, R. M. Kumar, R. Jayavel, J. P. Hill, and K. Ariga, ibid. 25, 267 (2015).11 K. Ariga, Q. Ji, M. J. McShane, Y. M. Lvov, A. Vinu, and J. P. Hill, Chem. Mater. 24, 728 (2012); S. Howorka, Langmuir 29,

7244 (2013); K. Ariga, Q. Ji, T. Mori, M. Naito, Y. Yamauchi, H. Abe, and J. P. Hill, Chem. Soc. Rev. 42, 6322 (2013); A. P.Pandey, N. M. Girase, M. D. Patil, P. O. Patil, D. A. Patil, and P. K. Deshmukh, J. Nanosci. Nanotechnol. 14, 828 (2014); W.Nakanishi, K. Minami, L. K. Shrestha, Q. Ji, J. P. Hill, and K. Ariga, Nano Today 9, 378 (2014); K. Ariga, K. Kawakami, M.Ebara, Y. Kotsuchibashi, Q. Ji, and J. P. Hill, New J. Chem. 38, 5149 (2014); M. B. Avinash and T. Govindaraju, Nanoscale6, 13348 (2014).

12 T. Hasegawa, K. Terabe, T. Tsuruoka, and M. Aono, Adv. Mater. 24, 252 (2012); S. Tappertzhofen, I. Valov, T. Tsuruoka,T. Hasegawa, R. Waser, and M. Aono, ACS Nano 7, 6396 (2013); T. Ohno, T. Hasegawa, T. Tsuruoka, K. Terabe, J. K.Gimzewski, and M. Aono, Nat. Mater. 10, 591 (2011); T. Hino, T. Hasegawa, H. Tanaka, T. Tsuruoka, K. Terabe, T. Ogawa,and M. Aono, Nanotechnology 24, 384006 (2013).

13 R. Ma, X. Liu, J. Liang, Y. Bando, and T. Sasaki, Adv. Mater. 26, 4173 (2014).14 F. Geng, R. Ma, A. Nakamura, K. Akatsuka, Y. Ebina, Y. Yamauchi, N. Miyamoto, Y. Tateyama, and T. Sasaki, Nat. Commun.

4, 1632 (2013).15 M. Liu, Y. Ishida, Y. Ebina, T. Sasaki, T. Hikima, M. Takata, and T. Aida, Nature 517, 68 (2015).16 K. Ariga, T. Mori, and J. P. Hill, Adv. Mater. 24, 158 (2012); K. Ariga, H. Ito, J. P. Hill, and H. Tsukube, Chem. Soc. Rev.

41, 5800 (2012); K. Ariga, T. Mori, and J. P. Hill, Soft Matter 8, 15 (2012).17 T. Michinobu, S. Shinoda, T. Nakanishi, J. P. Hill, K. Fujii, T. N. Player, H. Tsukube, and K. Ariga, J. Am. Chem. Soc. 128,

14478 (2006); Phys. Chem. Chem. Phys. 13, 4895 (2011).18 T. Mori, K. Okamoto, H. Endo, J. P. Hill, S. Shinoda, M. Matsukura, H. Tsukube, Y. Suzuki, Y. Kanekiyo, and K. Ariga, J.

Am. Chem. Soc. 132, 12868 (2010).19 K. Ariga, Y. Yamauchi, T. Mori, and J. P. Hill, Adv. Mater. 25, 6477 (2013); K. Ariga, T. Mori, S. Ishihara, K. Kawakami,

and J. P. Hill, Chem. Mater. 26, 519 (2014).


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