Authorship：Lead author   Publishing type：Research paper (scientific journal)   Publisher：AIP Publishing  

Arrays and ensembles of chiral nanostructures have potential applications in the field of enantioselective sensors, metamaterials, and metasurfaces. In particular, chiral nanostructures fabricated through chemical and bottom-up approaches have attracted much attention from the viewpoint of cost and scalability, but the heterogeneity of the unit nanostructure constituting the array or ensemble often deteriorates its chiroptical responses. Here, we report that their deteriorated responses can be recovered or even enhanced further by interparticle plasmon coupling. We employed chiral silver (Ag) hexamers as models for electromagnetic simulations and investigated the effect of their parameters, such as interparticle spacing, chiral purity, and enantiomeric excess, on their g-factor, which is an index for chiroptical responses. The maximum value of g-factor (gmax) of the Ag hexamer surpasses that of the chiral monomer and augments with decreasing interparticle spacing. This enhancement in g-factor is observed even when chiral purity and enantiomeric excess are less than 100%, showing the potent role of plasmon coupling in amplifying chiroptical responses. Furthermore, our research highlights the amplification of the effect of plasmon coupling on the gmax value of infinite periodic chiral nanostructures. These results corroborate the potential of plasmon coupling to improve chiroptical responses by precisely controlling the interparticle spacing of chiral plasmonic nanostructures, thus mitigating the loss of g-factor caused by low purity and enantiomeric excess of the nanostructures fabricated by chemical and bottom-up approaches.

DOI： 10.1063/5.0185286

Authorship：Lead author,　Corresponding author   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acs.jpcc.3c07566

Publishing type：Research paper (scientific journal)  

DOI： 10.1103/PhysRevB.109.035428

Authorship：Lead author   Publishing type：Research paper (scientific journal)   Publisher：AIP Publishing  

Chiral plasmonic nanostructures, which would be applied to enantioselective sensors and metasurfaces, can be prepared in an enantioselective manner by irradiation with circularly polarized light (CPL). However, their resonance sites have been covered with non-plasmonic, dielectric moieties. Here, we prepared all-silver chiral plasmonic nanostructures on a glass plate in one-step by irradiating 380–450 nm right- or left-CPL to an aqueous solution containing Ag+ and citrate ions. Achiral or racemic Ag nanoparticles with anisotropic geometry are deposited on a glass plate by photochemical electron transfer from citrate to Ag+ in the initial phase. The deposited nanoparticles are grown into chiral structures under CPL via generation of an electric field with chiral distributions. An achiral Ag nanoplate array was also grown under 600–700 nm CPL into chiral nanostructure arrays on the basis of hot electron reduction of Ag+.

DOI： 10.1063/5.0155834

Publishing type：Research paper (scientific journal)   Publisher：Wiley  

DOI： 10.1002/cnma.202300096

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：AIP Publishing  

Nanofabrication of three-dimensional chiral plasmonic structures has been a challenging research topic. In the present study, we shaped dielectric caps on plasmonic gold nanocubes (AuNCs) into three-dimensional nanospiroids by circularly polarized light (CPL) as the chirality source, without using lithographic methods or chiral molecules. AuNCs adsorbed on a TiO₂ substrate were irradiated with right or left CPL in the presence of Pb²⁺ for the deposition of PbO₂ on AuNCs. The Au–PbO₂ nanocomposites, thus, obtained are the first spiral plasmonic nanostructures prepared by CPL. They exhibit strong and sharp signals of circular dichroism, and the signs of the signals are reversed by changing the rotation direction of the CPL used. Their g-factor values are highest among the chiral plasmonic nanostructures fabricated by CPL.

DOI： 10.1063/5.0146579

Publishing type：Research paper (scientific journal)   Publisher：The Electrochemical Society of Japan  

DOI： 10.5796/electrochemistry.22-00046

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acsanm.2c00509

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.apsusc.2021.148932

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1039/d0nr08552a

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acs.jpcc.0c07267

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acsnano.9b10216

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acs.jpcc.9b09738

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acs.jpcc.9b08923

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acs.jpcc.8b07986

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acsanm.8b01829

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1246/cl.170707

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1039/c7sc00031f

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.apsusc.2017.01.304

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

DOI： 10.1039/c6nr01531j

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.2116/analsci.32.275

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：The Materials Research Society of Japan  

DOI： 10.14723/tmrsj.40.253

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.vibspec.2014.04.002

Publisher：The Electrochemical Society  

Chiral plasmonic nanostructures attract attention because those could be applied to enantioselective chemical sensors, optical isolators, light sources for circularly polarized light (CPL), metasurfaces, and metamaterials. In many cases, chiral plasmonic nanostructures are fabricated by a top-down method such as electron beam lithography (EBL). Since EBL is time-consuming and expensive, we have developed photoelectrochemical methods in which a site-selective reaction is driven by optical near field generated around anisotropic metal nanoparticles under right- or left-CPL. As anisotropic metal precursors for preparation of chiral nanoparticles, we have used gold or silver nanocuboids, nanorods, nanocubes, and triangular or hexagonal nanoplates so far.^1-5 In the present work we demonstrate that laterally isotopic, circular nanodisks can also be used as precursors for the preparation of chiral nanostructures.

We prepared ensembles of circular gold nanodisks on a glass plate by a nanosphere lithography method. A glass plate was coated with a gold thin film, and an array of polystyrene spheres (500 nm diameter) was prepared on the gold film. The polystyrene spheres were etched by oxygen plasma, and the exposed gold film was etched by argon ion milling. As a result, an ensemble of gold nanodisks (~200 nm diameter) was obtained. Each nanodisk was capped with a polystyrene cone, and the cap was removed by sonication in toluene if necessary. We used both capped and uncapped nanodisk ensembles. The ensemble was irradiated with visible right- or left-CPL in the presence of silver ions and sodium citrate. The obtained Au-Ag nanostructures exhibited circular dichroism (CPL), indicating that the nanostructures have chirality. Initial deposition at arbitrary site may break the geometric symmetry, resulting in the growth into chiral structures. Saito, K.; Tatsuma, T. Nano Lett. 2018, 18, 3209–3212.

Morisawa, K.; Ishida, T.; Tatsuma, T. ACS Nano 2020, 14, 3603–3609.

Shimomura, K.; Nakane, Y.; Ishida, T.; Tatsuma, T. Appl. Phys. Lett. 2023, 122, 151109.

Homma, T.; Sawada, N.; Ishida, T.; Tatsuma, T. ChemNanoMat 2023, 9, e202300096.

Ishida, T.; Isawa, A.; Kuroki, S.; Kameoka, Y.; Tatsuma, T. Appl. Phys. Lett. 2023, 123, 061111.

DOI： 10.1149/ma2024-01131099mtgabs

Other Link： https://iopscience.iop.org/article/10.1149/MA2024-01131099mtgabs/pdf

Publisher：The Electrochemical Society  

Chiral plasmonic nanostructures attracts attention because they are potentially applicable to optical materials such as enantioselective sensors and metamaterials, as well as photoelectrochemical devices. Chiral nanostructures are often prepared by electron beam lithography or synthesis based on DNA templates. We have recently developed a photoelectrochemical method, in which handedness of the chiral nanostructure can be controlled by right- or left- circularly polarized light.

The photoelectrochemical method is based on plasmon-induced charge separation (PICS),^1,2 in which electrons are injected from a plasmonic metal nanoparticle to a semiconductor such as titania in direct contact. In PICS, anodic reactions often occur at the resonance sites of the plasmonic nanoparticle, at which electron oscillation is localized.^3,4 Energetic electron-hole pairs generate at the resonance site, and holes are used for the local anodic reaction, probably via trap sites. On the basis of the mechanisms, we have demonstrated site-selective etching of silver nanoparticles and site-selective deposition of lead oxide on gold nanoparticles.

Under right-circularly polarized light (CPL), distribution of the resonance sites could be the mirror image of that under left-CPL.⁵ Therefore, we performed site-selective deposition of lead oxide on gold nanocuboids on titania under right- or left-CPL.⁶ As a result, lead oxide was deposited on the gold nanocuboids in a chiral geometry. The nanostructures thus obtained exhibited circular dichroism (CD), and the CD spectrum obtained for the structure prepared under right-CPL was opposite to that obtained for the structure prepared under left-CPL. Reversible switching of the handedness of the chiral plasmonic nanostructures can also be possible.⁷ This method also allows us to fabricate spiral nanostructures. 1. Y. Tian and T. Tatsuma, J. Am. Chem. Soc., 127, 7632 (2005). 2. T. Tatsuma, H. Nishi, and T. Ishida, Chem. Sci., 8, 3325 (2017) [review]. 3. I. Tanabe and T. Tatsuma, Nano Lett., 12, 5418 (2012). 4. T. Tatsuma and H. Nishi, Nanoscale Horiz., 5, 597 (2020) [review]. 5. S. Hashiyada, T. Narushima, and H. Okamoto, J. Phys. Chem. C, 118, 22229 (2014). 6. K. Saito and T. Tatsuma, Nano Lett., 18, 3209 (2018). 7. K. Morisawa, T. Ishida, and T. Tatsuma, ACS Nano, 14, 3603 (2020).

DOI： 10.1149/ma2022-0113929mtgabs

Other Link： https://iopscience.iop.org/article/10.1149/MA2022-0113929mtgabs/pdf

Publisher：The Electrochemical Society  

Plasmon-induced charge separation (PICS)^1,2 involves electron transfer from plasmonic noble metal nanoparticles or compound nanoparticles to an n-type semiconductor such as TiO₂. Oxidation reactions involved in PICS are based on a charge accumulation mechanism (Figure a) or a hole ejection mechanism (Figure b).³ The latter enables nanoscale local oxidation at relatively positive potentials.^4-7 This can be applied to photoinduced nanofabrication beyond the diffraction limit of light. For instance, chiral plasmonic nanostructures can be prepared by PICS under right or left circularly polarized light (Figure c).^8,9 Some other applications of the plasmonic hole ejection will also be mentioned. Enhancement of PICS with hole ejection through plasmon coupling¹⁰ and its application to photocatalysis will also be described.

References Y. Tian and T. Tatsuma, J. Am. Chem. Soc., 127, 7632 (2005).

T. Tatsuma, H. Nishi, and T. Ishida, Chem. Sci., 8, 3325 (2017) [review].

T. Tatsuma and H. Nishi, Nanoscale Horiz., 5, 597-606 (2020) [review].

E. Kazuma, N. Sakai, and T. Tatsuma, Chem. Commun., 47, 5777 (2011).

I. Tanabe and T. Tatsuma, Nano Lett., 12, 5418 (2012).

K. Saito, I. Tanabe, and T. Tatsuma, J. Phys. Chem. Lett., 7, 4363 (2016).

H. Nishi, M. Sakamoto, and T. Tatsuma, Chem. Commun., 54, 11741 (2018).

K. Saito and T. Tatsuma, Nano Lett., 18, 3209 (2018).

K. Morisawa, T. Ishida, and T. Tatsuma, ACS Nano, 14, 3603 (2020).

T. Ishida and T. Tatsuma, J. Phys. Chem. C, 122, 26153 (2018).





Figure 1

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DOI： 10.1149/ma2020-02613099mtgabs

Other Link： https://iopscience.iop.org/article/10.1149/MA2020-02613099mtgabs/pdf

Publisher：The Electrochemical Society  

Plasmon-induced charge separation (PICS)^1-3 involves electron transfer from plasmonic nanoparticles of Au, Ag, or Cu to a semiconductor, typically TiO₂.^1-4 The electron transfer is caused by external photoelectric effects (including hot carrier injection) or interfacial electron transition.³ We have reported that oxidation of Ag to Ag⁺ occurs at the Ag nanoparticle surface in PICS of Ag-TiO₂ systems,⁵ and this reaction occurs preferentially at the sites where optical near field is localized.^6-8 This can be explained in terms of ejection of energetic holes from the nanoparticles as Ag⁺ ions.^8,9 This possibility has been further investigated on the basis of other anodic reactions. For a system with isolated Au nanoparticles on TiO₂, the interface mode may be more important than the full-surface mode. However, plasmon coupling between two nanoparticles, which enhances full-surface mode but not necessarily enhances the interface mode, increases the PICS efficiency. This could also indicate that not only injection of electrons from Au nanoparticles into TiO₂ but also ejection of holes from Au nanoparticles play an important role in those PICS systems. Y. Tian and T. Tatsuma, J. Am. Chem. Soc., 127, 7632 (2005).

Y. Tian and T. Tatsuma, Chem. Commun., 2004, 1810.

T. Tatsuma, H. Nishi, and T. Ishida, Chem. Sci., 8, 3325 (2017) [review].

E. Kazuma and T. Tatsuma, Adv. Mater. Interfaces, 1, 1400066 (2014).

Y. Ohko, T. Tatsuma, T. Fujii, K. Naoi, C. Niwa, Y. Kubota, and A. Fujishima, Nat. Mater., 2, 29 (2003).

E. Kazuma, N. Sakai, and T. Tatsuma, Chem. Commun., 47, 5777 (2011).

I. Tanabe and T. Tatsuma, Nano Lett., 12, 5418 (2012).

K. Saito, I. Tanabe, and T. Tatsuma, J. Phys. Chem. Lett., 7, 4363 (2016).







Figure 1

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DOI： 10.1149/ma2018-01/11/931

Other Link： https://iopscience.iop.org/article/10.1149/MA2018-01/11/931/pdf

Publisher：The Electrochemical Society  

Plasmon-induced charge separation (PICS) occurs at the interface between plasmonic nanostructures of Au, Ag, or Cu and a semiconductor (e.g., TiO₂).^1-3 Carrier transfer from the nanostructure to the semiconductor due to external photoelectric effects (including hot carrier injection) or interfacial electron transition is responsible for PICS.⁴ We reported PICS for the first time more than 10 years ago^1,2 and studied its mechanisms^4,5 and applications.^1,3,6,7 In particular, we have reported effects of localized electric field on PICS. In the case of PICS-based oxidation of Ag nanoparticles, anodic reaction (i.e., oxidation of Ag to Ag⁺) occurs preferentially at the sites where optical near field is localized.^8-10 This may be explained in terms of ejection of energetic holes from the nanoparticles as Ag⁺ ions.¹⁰

1. Y. Tian and T. Tatsuma, J. Am. Chem. Soc., 127, 7632 (2005).

2. Y. Tian and T. Tatsuma, Chem. Commun., 2004, 1810.

3. T. Tatsuma, Bull. Chem. Soc. Jpn., 86, 1 (2013) [account].

4. E. Kazuma and T. Tatsuma, Adv. Mater. Interfaces, 1, 1400066 (2014).

5. H. Nishi and T. Tatsuma, Angew. Chem. Int. Ed., 55, 10771 (2016).

6. Y. Ohko, T. Tatsuma, T. Fujii, K. Naoi, C. Niwa, Y. Kubota, and A. Fujishima, Nat. Mater., 2, 29 (2003).

7. Y. Takahashi and T. Tatsuma, Appl. Phys. Lett., 99, 182110 (2011).

8. E. Kazuma, N. Sakai, and T. Tatsuma, Chem. Commun., 47, 5777 (2011).

9. I. Tanabe and T. Tatsuma, Nano Lett., 12, 5418 (2012).

10. K. Saito, I. Tanabe, and T. Tatsuma, J. Phys. Chem. Lett., 7, 4363 (2016).

DOI： 10.1149/ma2017-01/13/830

Other Link： https://iopscience.iop.org/article/10.1149/MA2017-01/13/830/pdf

Authorship：Lead author   Language：Japanese  

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プラズモニックなキラルナノ構造体は、局在表面プラズモン共鳴（LSPR）により強いキラル光学応答を示すため、キラル分子センサや負の屈折率を持つメタマテリアルへの応用が期待されている。しかし、可視域で負の屈折率を実現するには、光波長の1/10以下での精密な構造制御が必要である。我々は、円偏光をキラル源とした簡便なキラルナノ構造作製手法を開発し、熱正孔による酸化析出や熱電子による還元析出を用いてキラル構造体を作製してきた。本研究では、アキラルなAuナノ粒子に円偏光を照射してAgを析出させ、キラルナノ構造体を作製した。さらにFDTD電磁場解析法により、キラル形状化過程と光学応答の解析を行った。

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