4th – 5th of March 2024
Okazaki Conference CenterWelcome to NanospecFY2023. This conference is organized collaboratively by threecommunities (SPring-8 User Community: Micro and Nano Materials Science ResearchGroup, Japan Surface Science Society: Synchrotron Radiation Surface Science Research
Division and Probe Microscopy Research Division). It aims to discuss cutting-edge
material analyses at the nanoscale to facilitate active discussion and exchange. The
conference covers a wide range of topics in physics, chemistry, and biology, including theelectronic states, structures, and physical properties of condensed matter, as well as
catalysis, surface chemistry, electrochemistry, and biophysics. We hope this conference
will contribute to active interaction within the communities and foster future developmentof international research cooperation.
Organizing committee
Conference chair
Takashi Kumagai (Institute for Molecular Science)
Research Group of Nanospectroscopy and Materials Science, SPring-8 Users
Community
Hirokazu Fukidome (Tohoku Univ.), Takuo Ohkochi (Univ. of Hyogo), Akinobu
Yamaguchi (Univ. of Hyogo)
The Japan Society of Vacuum and Surface Science, Synchrotron Radiation Surface
Science Division
Jun Yoshinobu (ISSP, Univ. of Tokyo), Kenichi Ozawa (KEK), Ryo Toyoshima (KeioUniv.)The Japan Society of Vacuum and Surface Science, Scanning Probe Microscopy
Division
Yukio Hasegawa (ISSP, Univ. of Tokyo), Hiroshi Onishi (Kobe Univ.)
Joint sponsorship
Institute for Molecular Science
The Japan Society of Vacuum and Surface Science Chubu Division
UNISOKU Co., Ltd.
Quantum Design Japan

Access to Okazaki Conference Center
Please get off at Meitetsu Higashi Okazaki Station. Turn left (south) at the ticket gate in
the basement and exit the station. The OCC is a 10-minute walk up the hill.
See more details: https://www.orion.ac.jp/occ-e/
From Meitetsu Higashi-Okazaki station

Venue Guide⚫

The talk session is held in Ohsumi Hall.

⚫

The poster session is held in Conference Room B/Foyer b⚫

The Opinion Exchange Event is held in Conference Room B⚫

Luncheon seminar is held in:
Conference Room B (Quantum Design Japan) and C (UNISOKU)

Day 1 (March 4th)
12:00-

Registration

13:00-13:05

Opening remarks

13:05-14:05

Martin Wolf (Plenary Lecture)
Ultrafast light-matter interaction probed in momentum and real space

14:05-14:35

Masahiro Shibuta (Invited talk)
Ultrafast Spatial and Temporal Evolutions of Photoexcited Electrons at
Functional Organic Surfaces and Interfaces

14:35-14:50

Break

14:50-15:20

Satoshi Kera (Invited talk)
Many body effects define the material properties of molecular solids

15:20-15:50

Masaki Hada (Invited talk)Atomic or molecular motions in solids observed by ultrafast time-resolved
electron diffraction

15:50-16:20

Masanori Sakamoto (Invited talk)Chemical energy conversion process using infrared light

16:20-16:30

Break

16:30-17:00

Yasumitsu Miyata (Invited talk)
In-plane heterostructures based on 2D transition metal dichalcogenides

17:00-17:20

Yuki Tsujikawa (Contributed Talk)
Study of a novel copper boride surface on Cu(110) with a one-dimensional
quasi-periodic growth

17:20-17:40

Hiroaki Ooe (Contributed talk)
Lattice-conserved polymerization of self assembled Br2-HPB molecules on
Au(111)

17:40-18:00

Can Liu (Contributed Talk)
Diffusion and adsorbate-adsorbate interaction of methoxy intermediates
adsorbed on Ti sites of a Pt/TiO2(110) surface

18:00-19:30

Poster session

19:30-21:00

Opinion Exchange EventDay 2 (March 5th)
8:50-9:20

Yasuo Seto (Invited talk)
Development of latent fingerprint detection by synchrotron soft X-ray
microimaging

9:20-9:50

Masato Kotsugi (Invited talk)Feature extended Landau free energy model: extracting hidden informationfrom magnetic domain image

9:50-10:20

Kiyohiro Adachi (Invited talk)Multi-scale structure analysis of white smoker chimney collected from theMariana Trench using multiple synchrotron radiation techniques

10:20-10:40

Wang Zi (Contributed Talk)
In situ soft-X-ray absorption spectroscopy study of photoexcited hole transfer
in the cocatalyst-loaded SrTiO3:Al photocatalyst under UV irradiation

10:40-11:00

Break

11:00-11:30

Noriyuki Kodera (Invited talk)Video imaging of biological molecules in action by high-speed AFM

11:30-12:00

Kyoung-Duck Park (Invited talk)Tip-induced control of strong quantum light-matter interactions at thenanoscale

12:00-12:30

Chi Chen (Invited talk)Near-field Spectroscopic Imaging of Mesoscopic Photophysics: 2D
Semiconductors and Lipid Bilayers

12:30-13:30

Lunch (Luncheon seminar by UNISOKU and QDJ)

13:30-14:00

Miyabi Imai (Invited talk)Atomic-scale visualization of single-molecule photocurrent channels by
Photon-STM

14:00-14:30

Valeria Sheina (Invited talk)Atom by atom Electron spin resonance: coherence of Ti spins on ultra-thin
MgO layers

14:30-15:00

Chun-Liang Lin (Invited talk)
Tomography Scan of Charge Density Wave in NbSe2

15:00-15:20

Shota Takahashi (Contributed talk)
Pioneering tip-enhanced nonlinear optics and spectroscopy

15:20-15:30

Closing remarks

15:50-

Lab tour at IMSNanospecFY2023

Plenary Lecture

Ultrafast light-matter interaction probed in momentum and real space
Martin Wolf*
Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195 Berlin, Germany
Interaction of quantum matter with ultrashort light pulses may lead to emergent phenomena away fromequilibrium. Examples are light harvesting in molecular semiconductors, exciton fission or ultrafast
phase transitions in solids. Ultrafast laser spectroscopy provides a rich toolbox to study non-equilibrium
dynamics of the underlying elementary excitations in the time-domain, but typically lacks spatial
resolution. In order to obtain a complete picture of complex spatial-temporal dynamics of quantum
matter, nanoscale spectro-microscopy should be combined with ultrafast temporal resolution. In thistalk, I will discuss several complementary approaches to study the dynamics of elementary excitations
from a momentum and real space perspective.
Recent advances in time-resolved photoemission spectroscopy (trARPES) combined with
momentum space microscopy allow direct probing of excited states throughout the complete Brillouinzone. 2D materials and their heterostructures provide a vast playground to obtain a mechanistic
understanding of exciton dynamics and probing the spatial extend of excitons in momentum-space. We
also investigate the primary step of singlet fission in crystalline pentacene using orbital tomography anddecompose energetically overlapping states on the basis of their orbital character. Our results show acharge-transfer mediated mechanism with hybridization of Frenkel and charge transfer states for fissionof the singlet exciton [1].
Ultrafast scanning tunneling microscopy (STM) pushes spatial resolution to atomic scales. THzlightwave-driven STM (THz-STM) and photon-assisted STM (ph-STM) are two approaches to probe thedynamics of charge, orbital and lattice degrees of freedom at the atomic scale [2]. While THz-STM uses
single-cycle THz pulses to drive tunneling via classical rectification, ph-STM is based on photon
absorption-induced tunneling. Here we use ph-STM to probe coherent phonons in ultrathin
ZnO/Ag(111) via their coupling to an electronic resonance that enhances photon-assisted tunneling [3].
On the other hand, we can study the charge density wave (CDW) phase in 1T-TaS2 using THz-STM,
and probe locally the photoinduced Mott collapse and the coherent CDW amplitude motion (see Figure1). Our results demonstrate the ability of ultrafast STM to reveal inhomogeneous non-equilibrium
dynamics at atomic scales, previously obscured in spatially-averaged spectroscopy.

Fig. 1. Left: Charge density wave in TaS2 imaged in constant height STM and THz-STM image of thesame area (VDC = +50 mV UTHz= 450 mV). Right: Rectified THz current versus time delay acquired on topof a selected CDW cluster. The periodic oscillations (t > 1ps) arise from the CDW amplitude mode (V DC =-100 mV UTHz= 450 mV).
References[1] A. Neef et al., Orbital-resolved observation of singlet fission, Nature 616, 275 (2023).
[2] M. Müller, Imaging surfaces at the space-time limit: New perspectives of time-resolved scanningtunneling micro-scopy for ultrafast surface science, Prog. Surf. Sci. 100727 (2023)[3] S. Liu et al., Nanoscale Coherent Phonon Spectroscopy, Science Advances 8, eabq5682 (2022).
* Acknowledgements: This work was performed in collaboration with A. Neef, S. Beaulieu, S. Dong, J.
Maklar, T. Pincelli, P. Xian, L. Rettig, J. Pflaum, R. Ernstorfer and S. Liu, A. Hammud, I. Hamada, T.
Kumagai and M. Müller

NanospecFY2023

Invited Talk

Ultrafast Spatial and Temporal Evolutions of Photoexcited Electrons at Functional
Organic Surfaces and Interfaces
Masahiro Shibuta
Department of Engineering, Osaka Metropolitan University, Japan
Understanding of the ultrafast electron dynamics at organic surfaces and interfaces is of highimportance because it governs the functionalities of photoconversion devices. Since the growth ofthe organic layer exhibits inhomogeneity, time-resolved spectroscopy should be combined withmicroscopic way to observe the local phenomena. Two-photon photoemission spectroscopy (2PPES) is a powerful method for studying the ultrafast electron dynamics, in which a first photon
excites an electron in a targeted system and the excited electron is extracted by the aftercoming
second photon. Using the optics for photoelectron emission microscopy as 2P-PEEM, the local
excited-state dynamics can also be resolved with ~100 nm resolution [1].
On the fullerene C60 layer, our 2P-PES and 2P-PEEM characterized the ultrafast dynamics
of photocarrier generation in the C60 layers with high energy, spatial, and temporal resolutions [1,2].
In addition, momentum-resolved 2P-PES showed a variety of highly-dispersive conduction bands
in a well-assembled C60 film; the nearly free-electron-like character originates from the diffuse
superatomic molecular orbitals of C60 [3].
In case of the pentacene layer, 2P-PEEM reflects the lateral distribution of excitons confinedin the nanocrystal anisotropically grown on a substrate. Importantly, time-resolved 2P-PEEM
captured the evolution of hot electrons dissipated into the substrate in 1 ps or sub μm ranges [4].
We have also demonstrated that 2P-PES and 2P-PEEM are valuable to observe plasmonic
phenomena, which enhance the functionalities of organic system. By depositing atomically sizeselected silver nanoclusters on C60 layer, 2P-photoemission was drastically enhanced by plasmoninduced hot electrons [5]. Using a plasmon-active gold (Au)
substrate for C60 deposition, we clearly visualized andevaluated the propagating surface plasmon polaritons (SPPs)
generated at the C60/Au interface [6]. These spectroscopic
and microscopic methodologies probing 2P-photoemission

Two-Photon Photoemission

have high potential to reveal the optical and plasmonic
properties of various functional nanoscale systems.
References[1] M. Shibuta, A. Nakajima, J. Phys. Chem. Lett. 14, 3285-3295 (2023).
[2] M. Shibuta et. al., Sci. Rep. 6, 35853 (2016)., Appl. Phys. Lett. 109, 203111 (2016).
[3] M. Shibuta et. al., J. Phys. Chem. C 124, 734 (2020)[4] M. Shibuta et. al., in revision[5] M. Shibuta, et al., ACS Nano 15, 1199 (2021).
[6] M. Shibuta, et al., ACS Nano 14, 2044 (2020).

NanospecFY2023

Invited Talk

Many body effects define the material properties of molecular solids
Satoshi Kera
Institute for Molecular Science
Understanding the impacts of weak electronic interaction on the electron delocalization is required
to discuss the rich functionalities of organic molecular materials. Moreover, the temporal and spatial
effects of the strong coupling of phonon (collective lattice vibration) and/or local molecular vibration
to electron must be unveiled. Angle-resolved ultraviolet photoelectron spectroscopy (ARUPS) is
known to be a powerful technique to study the valence electronic structure. The frontier orbital of
HOMO state can offer a wide variety of key information, that is essential to comprehend chargehopping transport (small-polaron related transport) in the ordered monolayer film [1] as well as tocoherent band transport in the molecular single crystal [2,3]. However, the experimental study of
ARUPS fine features of the HOMO state has not been progressed till recently due to difficulty inthe sample preparation, charging effects, irradiation damages, and so on [4,5]. We present thelatest development for the ARUPS measurements of electronic states for rubrene (C42H28) single
crystal by using low-energy excited and high-resolution experimental station at BL7U of UVSOR
synchrotron facility. We demonstrate how the HOMO band is observed differently against theprevious results in theory [6] for the orthorhombic crystal structure of rubrene. To understand theeffects of polaron formation on the electronic structure, a partially dressed polaron model that
accounts for the electron–phonon interaction with frequency-dependent coupling constants basedon Debye relaxation was proposed recently [7]. The precise experiments of the temperaturedependence and 2D momentum-energy scanning for the ARUPS shed light on the problem ofdescribing the characteristics of the electronic structure of organic materials, and thus the results
would provide a perspective for the design of organic semiconductor devices.
References[1] S. Kera et. al., Prog. Surf. Sci., 84, 135 (2009).
[2] N. Ueno et. al., Prog. Surf. Sci., 83, 135 (2008).
[3] Y. Nakayama et. al., J. Mater. Chem. C., 8, 9090 (2020).
[4] S. Machida et. al., Phys. Rev. Lett. 104, 156401 (2010).
[5] F. Bussolotti et. al., Nat. Comm, 8, 173 (2017).
[6] Y. Li et. al., J. Phys. Chem. Lett. 3, 3325 (2012).
[7] H. Sato et. al., Nat. Mater. 21, 910 (2022).

NanospecFY2023

Invited Talk

Atomic or molecular motions in solids observed
by ultrafast time-resolved electron diffraction
Masaki Hada
University of Tsukuba
In the last two decades, methods have been developed to directly observe the light-driven
atomic and molecular motions of materials in real time. This progress is currently being made in
elucidating the mechanisms of photoreactions or photoinduced phase transition phenomena inmolecules or materials. [1,2]. These methodologies generally have a time resolution of 10–14 to 10–
12 seconds (10 femtoseconds to 1 picosecond) and are called ultrafast measurements. Among theultrafast measurement techniques, I will discuss ultrafast time-resolved electron diffraction
measurements on solid-state materials in this presentation. Ultrafast time-resolved electron
diffraction uses techniques like ultrafast time-resolved x-ray diffraction to measure thephotoinduced changes of atomic or molecular coordinates.
The presentation shows the recent combined investigation of ultrafast time-resolved
electron diffraction measurements, ultrafast transient absorption measurements, and firstprinciples calculations on a one-dimensional van der Waals heterostructure. The heterostructure
contains carbon nanotubes (CNTs) as an inner core and boron nitride nanotubes (BNNTs) as anouter core. We found peculiar charge transfer channels between CNTs and BNNTs through theheterostructures.
References[1] S. Koshihara, T. Ishikawa, Y. Okimoto, K. Onda, R. Fukaya, M. Hada, Y. Hayashi, S. Ishihata,
T. Luty, Physics Reports 942, 1 –61 (2022).
[2] M. Hada, Y. Nishina, T. Kato, Accounts of Chemical Research 54, 731–743 (2021).

NanospecFY2023

Invited Talk

Chemical energy conversion process using infrared light
Masanori Sakamoto
Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011, Japan
Solar radiation is the most abundant renewable energy source; however, its overall utilization
remains inefficient as half of the energy is in the form of infrared (IR) light, which cannot beharnessed due to its low energy.
The presenter has been investigated the materials and method for converting the infrared light,
an unused renewable energy source, into an energy resource. Localized surface plasmon
resonance (LSPR) band can be tuned over a wide spectral range enabling solar energy utilizationfrom ultraviolet (UV) to infrared (IR) regions. This excellent light-harvesting ability provide thetechnologies which convert wide range of light including IR region to chemical or electronicenergies. However, the low conversion efficiency has been major drawbacks of LSPR-induced
energy conversion.
LSPR materials of compound semiconductors, copper chalcogenide nanocrystals have shown
unique carrier dynamics which demonstrate the efficient IR-responsive photocatalysts and device
including IR sensor. The unique carrier transfer induced by LSPR excitation overcomes thelimitation of low efficiency of plasmonic energy conversion realizing the efficient IR light to chemicalenergy conversion.
In this lecture, presenter will introduce the materials and mechanism of energy conversion of
infrared light and applications for IR-responsive photocatalyst and devices.

References[1] M. Sakamoto*, M. Hada*, W. Ota, F. Uesugi, and T. Sato “Localised surface plasmon
resonance inducing cooperative Jahn–Teller effect for crystal phase-change in a nanocrystal”
Nat. Commun, 2023, 14, 4471.
[2] G. T. Mario, L. Zichao, C. Boiko, M. Sakamoto,* A. Douhal* “Hot Hole Transfer at Plasmonic
Semiconductor/Semiconductor Interface” Nanoscale, 2023,15, 657-666.
[3] Z. Lian, and M. Sakamoto* et. al., “Harnessing infrared solar energy with plasmonic energy
upconversion” Nat. Sustain, 2022, 5, 1092–1099.
[4] Z. Lian, and M. Sakamoto* et. al., "Plasmonic p-n Junction for Infrared Light to Chemical
Energy Conversion" J. Am. Chem. Soc. 2019, 141, 2446-2450.
[5] Z. Lian, and M. Sakamoto* et. al., “Near infrared light induced plasmonic hole transfer at a
nano-heterointerface” Nat. Commun. 2018, 9, 2314.

NanospecFY2023

Invited Talk

In-plane heterostructures based on 2D transition metal dichalcogenides
Yasumitsu Miyata
Department of Physics, Tokyo Metropolitan University, Hachioji, Tokyo, Japan
Transition metal dichalcogenides (TMDs) are attractive materials with atomically-thin layered
structures and unique physical properties. Recent advances in growth techniques have facilitated
the fabrication of various TMD-based heterostructures. In particular, the edges of TMD single
crystals can serve as platforms for the epitaxial growth of other TMDs. In this talk, we will present
our recent progress in the chemical vapor deposition (CVD) and applications of such in-plane
heterostructures (Figure 1) [1-5]. For example, two-step CVD process allows the formation of inplane heterostructures with atomically sharp interfaces and nanometer-wide quantum wires[1,2,5]. In addition, tuning the precursor supply rates facilitates the realization of a compositionally
graded TMD alloy [3,4]. We have demonstrated diverse functionalities of these heterostructures,
including chiral or wavelength tunable electroluminescence [2,3], directional exciton energy
transport [4], and band-to-band tunneling [5]. These TMD-based heterostructures would provide
opportunities to investigate low-dimensional physics and explore applications in future devices.

Figure 1 (a) Schematic illustrations of the heteroepitaxial growth of TMD in-plane heterostructure.
(b) Optical images of WSe2/WS2 in-plane heterostructures. (c) Examples of various TMD-based
in-plane heterostructures.
References[1] Y. Kobayashi, et al., ACS Nano, 13 (2019) 7527.
[2] N. Wada, et al., Adv. Func. Mater., 32 (2022) 2203602.
[3] J. Pu, et al., Adv. Mater. 34 (2022) 2203250.
[4] M. Shimasaki, et al., ACS Nano, 16 (2022) 8205.
[5] H. Ogura, et al., ACS Nano 17 (2023) 6545.

NanospecFY2023

Contributed Talk

Study of a novel copper boride surface on Cu(110) with a one-dimensional quasiperiodic growth
Yuki TsujikawaA, Xiaoni ZhangA, Kazuki YamaguchiA, Masahiro HazeA, Takeru
NakashimaB, Arpita VaradwajC, Yusuke SatoA, Masafumi HorioA, Yukio
HasegawaA, Fumio KomoriA, Masaki OshikawaA, Masato KotsugiC, Yasunobu
AndoB, Takahiro KondoD, and Iwao MatsudaA
AISSP, The University of Tokyo, BCDF-Mat, AIST, CFaculty of Advanced Engineering,Tokyo University of Science, DFaculty of Pure and Applied Sciences, University ofTsukuba
A new surface compound material, copper boride (Cu-boride), has recently beenachieved in a two-dimensional (2D) form on the Cu(111) surface [1-4]. Compounds with thiscombination of elements were previously not known to synthesize in a 3D bulk form due to thesmall difference in electronegativities and large difference in atomic sizes. However, it was found
to exist in a 2D form, exhibiting a unique 1D boron chain configuration combined with the Cu
atoms. The combination of molecular orbitals of boron chains and hybridization with Cu enables
the synthesis of this exotic compound.
Here, we report a new Cu-boride surface synthesized on the anisotropic Cu(110)substrate [5]. The B/Cu(110) surface displayed 1D growth, with atomic chains periodically aligned
parallel to one another. The chains grew in a self-assembled manner, extending over hundreds ofnanometers, even crossing the surface steps. Intriguingly, the 1D structure of the chains showedno average lattice, resulting in a quasi-periodic order of two lengths, verified through Fouriertransform analysis. The observed long-range formation of a quasi-periodic 1-D structure wastheoretically modeled under a 1-D quasi-crystal condition, and the predicted conditions alignedwith the structural parameters determined experimentally. This quasi-periodic 1-D copper boride
system serves as a unique platform for studying 1-D quasi-crystallinity in an actual material,
ensuring the rich nature of structures and bindings in the boron system [6].
References[1] Y. Tsujikawa et al., Physical Review B 106, 205406 (2022).
[2] C. Yue et al., Fundamental Research 1, 482 (2021).
[3] X.-J. Weng et al., Physical Review Materials 4, 074010 (2020).
[4] Y. Tsujikawa et al., e-Journal of Surface Science and Nanotechnology, Advance online
publication, https://doi.org/10.1380/ejssnt.2023-058[5] Y. Tsujikawa et al., Surface Science 732, 122282 (2023).
[6] Y. Tsujikawa et al., Nano letters, acceptedNanospecFY2023

Contributed Talk

Lattice-conserved polymerization of self-assembled Br2-HPB molecules on Au(111)
Hiroaki OOE and Takashi YOKOYAMA
Yokohama City University

The bottom-up construction of covalent nanostructures has been achieved through on-surface
polymerization of tailor-made precursors.[1] Recently, the influence of precursor self-assembly on
the on-surface polymerization reactions has also been reported. The polymerization of selfassembled precursor molecules has been generally understood as that the restricted molecular
diffusion leads to the formation of covalent bonding between closely adjacent reaction sites.[2]Nevertheless, the detailed influence of self-assembled structure has not been clear.
In this study, we focus upon the influence of self-assembly on the polymerization reaction. As areaction precursor, dibromo-substituted hexaphenylbenzene (Br2-HPB; Figure 1) is used. In ourprevious report, as well as the Br2-HPB precursors, covalently bonded HPB polymer chainsproduced by the on-surface polymerization also exhibited a long-range ordering on Au(111), as
shown in Figure 2a and 2b.[3] This indicate that, during the polymerization process, the orderedself-assembly has been maintained apparently. Nevertheless, the structural disordering is expectedby the sequential polymerization reactions due to the molecular size difference between Br2-HPB
precursor and HPB polymer. To clarify why the ordered self-assembly has been maintained, we
have investigated the partially polymerized mixture phase, which is achieved by short annealing.
After the short annealing at 200 °C, we have observed an well-ordered structure composed ofboth Br2-HPB precursors and HPB polymers. The ordered mixture phase suggests that thepolymerization of Br2-HPB proceeds without the disruption of ordered self-assembly. From thedetailed analysis of the mixture phase, we find that the polymerization of Br2-HPB is accompaniedby the molecular rotation to conserve the self-assembled array of Br2-HPB. After higher
temperature annealing at 400 °C, the finally produced hexabenzocoronene (HBC) nanographene
chains show a tendency to align their orientation, as shown in Figure 2c. This orientation alignment
should be attributed to the ordered structure of HPB polymers. Thus, we have clarified that the selfassembled ordering of Br2-HPB precursor molecules influences on the molecular arrangements
not only after the polymerization process but also even after the cyclodehydrogenation process.

References[1] C. Cai et al., Nature, 466 (2010) 470. [2] J. Huang et al., ACS NANO 15 (2021) 4617.
[3] H. Ooe, K. Ikeda, and T. Yokoyama, J. Phys. Chem. C, 127 (2023) 7659.

NanospecFY2023

Contributed Talk

Diffusion and adsorbate-adsorbate interaction of methoxy intermediates
adsorbed on Ti sites of a Pt/TiO2(110) surface
Can Liu1, Bang Lu1, Hiroko Ariga Miwa2, Min Gao1, Jun-ya Hasegawa1, Ken-ichi
Shimizu1, Kiyotaka Asakura1, Satoru Takakusagi1
1Hokkaido University, 2The University of Electro-Communications
Understanding the dynamic behavior of intermediate adsorbates on a catalyst surface is crucial
because it significantly influences the catalytic performance. We have recently reported that thethermal decomposition property of methoxy intermediates adsorbed on the Ti sites of a Pt/TiO2(110)
surface was controlled by their diffusion and reverse spillover.1,2 It has been well known that themobility of the intermediate adsorbates is affected by the adsorbate-substrate and adsorbateadsorbate interactions. In this study, we examined the diffusion mechanism and adsorbateadsorbate interaction of the methoxy intermediates on the Pt/TiO2(110) surface by scanningtunneling microscopy (STM), density functional theory (DFT) calculation and space-correlation
analysis.

(a)(b) CH3OH → CH3O-Ti5c+

Figure 1 shows a typical STM image

[001]

H-Obr

of the Pt/TiO2(110) surface after exposure tomethanol vapor at room temperature. The
methoxy adsorbates were present on theTi5c sites of the TiO2(110) after they werecreated on the Pt nanoparticles and then

Ti

O

C

H

2
spilled over to the TiO2 surface. The Figure 1. (a) STM image (7.4×7.4 nm ) of the Pt/TiO2(110)saturation

coverageofthemethoxy surface after exposure to 5 L methanol vapor. (b) Atomic

intermediates was 0.14 ML (1ML= 5.2×1018 model of methoxy adsorbate adsorbed at the Ti5c site.
/m2). Sequential STM imaging showed that, the methoxy adsorbates were mobile at room
temperature and diffused both along the [001] and [11̅0] directions. DFT calculations of a single
methoxy adsorbate on a TiO2(110) surface showed that the conversion to methanol-likeintermediate is a key for facile diffusion on the TiO2(110) surface. Along the [001] direction, themethanol-like intermediate diffuses to the nearest Ti5c site with an energy barrier of 0.68 eV. Alongthe [11̅0] direction, the barrier could be lowered to 0.64 eV with the presence of an additional HObr.
The collective behavior of the methoxy species was also studied by space correlation analysis. The
neighboring distance between the two methoxy adsorbates along the [001] direction was more than
3 lattice constants, indicating a repulsive interaction between them which may limit the saturation
coverage of the methoxy intermediates and act as a driving force for their diffusion along the [001]direction.
References[1] S. Takakusagi, K.-i. Fukui, R. Tero, K. Asakura, Y. Iwasawa, Langmuir 2010, 26, 16392.
[2] C. Liu, B. Lu, H. Ariga-Miwa, S. Ogura, T. Ozawa, K. Fukutani, M. Gao, J.-y. Hasegawa, K.-i.
Shimizu, K. Asakura, S. Takakusagi, J. Am. Chem. Soc. 2023, 145, 19953.

NanospecFY2023

Invited Talk

Development of latent fingerprint detection by synchrotron soft X-ray microimaging
Yasuo SetoA, Masahisa TakatsuA, Hiroyuki FujiwaraA, Shimpei WatanabeA,
Seiji MuratsuA, Toshio NakanishiA, Hideya OkadaA, Satoru HamamotoA,
Takuo OhkochiBAC, Masaki OuraA
ARIKEN SPring-8 Center, BUniv. Hyogo, CJASRI
Fingerprint (FP) examination is key forensic technology. FP is composed of secretion of sweat
and sebaceous glands, as well as contaminations which were adhesive to the fingers. Inclusionsof FP are water, organic compounds such as amino acids, proteins, carbohydrates, organic acid,fatty acids and lipids, inorganic compounds such as alkali metals and halogens, and also
contaminants such as cosmetics. Matching of ridge pattern taken from latent FP left on crime
scene surface with those of reference FP, leads to personal identification, like forensic DNA
typing. Analysis of FP components provide personal information and history; age, gender, bodystatus, time between fingerprint adhesion and sampling, and special action such as handling of
explosives. Many FP detection and enhancement methods have been used in real criminal
investigation, such as ninhydrin method and cyanoacrylate method. Fourier-transform infra-red(FT/IR) spectroscopy, mass spectrometry and electrochemical method are also developed.
However, it is difficult to get ridge pattern from unclear latent FP. Especially, in fire scenes FPs
are severely deteriorated by heating, which cause FP visualization impossible. In this research,
synchrotron soft X-ray microimaging technique was compared with conventional optical
microscopy, FT/IR microimaging and scanning electron microscopy with energy dispersive X-ray
spectroscopy (SEM-EDX). for visualizing heated FP.
Index fingers were pushed on various substrates (silicone, glass, stainless steel, aluminum,
brass) to form FPs, and sealed FPs were treated by heating (400℃ for 3 h). Untreated andheated FPs were subject to scanning soft-X-ray fluorescent microscopy (SXFM) andphotoemission electron microscopy (PEEM) at SPring-8 BL17SU, and also laboratory analysis.
Untreated FPs showed images of assembles of ridge streaks (several hundred m width, about 1
m height) separated each other by few hundred m under optical microscopy observation, but
after heating, FP ridge pattern could not be clearly observed. Micro FT/IR spectroscopy showed
spectrum composed of absorption peaks derived from sweat and sebaceous gland inclusion for
untreated FPs, but after heating, characteristic IR absorption could not be observed. By SEMEDX measurement, clear FP ridge patters could not be observed for heated FPs, but aggregatesof about 1 m NaCl particles were observed on silicone substrate. SXFM (0.5 m size, photon
energy 2 keV, 40 m step scanning) clearly visualized FP ridge streaks on all the substrates for
untreated FPs by observing Na K, O K and elastic peaks, but for heated FPs, SXFM visualized
FP ridge streaks only on silicone, stainless steel and brass substrates by detecting Na K peak.
PEEM successfully visualized positive particles which formed FP ridge streaks at Na K-edge forheated FPs on all the substrates, where in magnified field of view, about 1 m-size Na particles
were observed.

NanospecFY2023

Invited Talk

Feature extended Landau free energy model: extracting hidden information frommagnetic domain image
Masato Kotsugi,
Tokyo University of Science
Microscopic materials analysis is essential to achieve desirable performance in next-generation
nanoelectronic devices, such as low power consumption and high speeds. However, themagnetic materials involved in such devices often exhibit incredibly complex interactions between
nanostructures and magnetic domains. This, in turn, makes functional design challenging.
Traditionally, researchers have performed a visual analysis of the microscopic image data.
However, this often makes the interpretation of such data qualitative and highly subjective. Whatis lacking is a causal analysis of the mechanisms underlying the complex interactions in
nanoscale magnetic materials.
We carried out in automating the interpretation of the microscopic image data. This was achieved
using an “extended Landau free-energy model” that we developed using a combination of
topology, data science, and free energy1-6. The model could illustrate the physical mechanism aswell as the critical location of the magnetic effect, and proposed an optimal structure for a nanodevice. The model used physics-based features to draw energy landscapes in the information
space, which could be applied to understand the complex interactions at the nanoscales in a wide
variety of materials.
References[1] S. Kunii, K. Masuzawa, A. L. Fogiatto, C. Mitsumata & M. Kotsugi, Sci. Rep. 12, 19892 (2022)[2] A. L. Foggiatto, S. Kunii, C. Mitsumata & M. Kotsugi, Communications Physics 5, 277 (2022)[3] S. Kunii, A. L. Foggiatto, C. Mitsumata & M. Kotsugi, Sci. Tech. and Adv. Mater. Methods, 2445-459 (2022)[4] C. Mitsumata, M. Kotsugi, J. Magn. Soc. Jpn, 46, (2022) pp. 90-96[5] K. Masuzawa, S. Kunii, A. Foggiatto, C. Mitsumata, M. Kotsugi, T. Magn. Soc. Japan. 6(2022), 1-9.
[6] T. Nishio, M. Yamamoto, T. Ohkochi, D. Nanasawa, A. Foggiatto, M. Kotsugi, Sci. Tech. andAdv. Mater. Methods, 2, pp 345-354, (2022)

NanospecFY2023

Invited Talk

Multi-scale structure analysis of white smoker chimney collected from the Mariana
Trench using multiple synchrotron radiation techniques
Kiyohiro Adachi
RIKEN Center for Emergent Matter Science (CEMS)
What is the origin of life? –– This is a question that has long intrigued mankind. Microorganisms
are engaged in chemosynthesis in deep-sea hydrothermal vents (HVs), which may hold the key
to the elucidation of the origin of life. Scientists once believed that light was necessary for life.
However, the discovery in 1979 of microorganisms swarming around deep-sea HVs changed theconventional wisdom. Following the discovery of Black Smoker HVs, a giant HV (White Smoker
Chimney), which emitted alkaline pH hydrothermal water was discovered.
Remarkable progress in extreme environment science continues to expand the frontiers ofscience on the origin of life. However, studies on HVs have been conducted mainly from theviewpoints of microbiology and geology, and the structural order and function are unexploredissues.
We have been working to elucidate the structure and function of White Smoker Chimney
from multiple perspectives using multiple synchrotron radiation techniques. White Smoker
Chimney has a hierarchical structure, consisting of water channels (~100 μm), walls (~10 μm),
nanochannels (nm-scale), and Brucite layers (sub nm-scale). The White Smoker Chimney
sample was collected by Shinkai 6500 from the Mariana Trench. The orientation of Brucite layers
and alignment of walls were analyzed by WAXS and SAXS using a focused X-ray beam at
BL32XU and BL38B1, respectively. To reveal the function of Chimney in deep sea, the state ofwater inside the Chimney was further analyzed by IR and XAS at BL43IR and BL17SU,
respectively. Further details on the experiments and results were explained in the presentation.

Figure1. Hierarchical structure of the White Smoker Chimney
References[1] Lee H-E, Okumura T, Ooka H, Adachi K, et al. Osmotic Energy Conversion in Deep-Sea
Hydrothermal Vents. ChemRxiv, (doi:10.26434/chemrxiv-2023-v9nc6).

NanospecFY2023

Contributed Talk

In situ soft-X-ray absorption spectroscopy study of photoexcited hole transfer in the
cocatalyst-loaded SrTiO3:Al photocatalyst under UV irradiation
Zi WangA, Ryo ToyoshimaA, Masaaki YoshidaB, Kazuhiko MaseC, Hiroshi KondohA
A Department of Chemistry, Keio University, 3-14-1 Hiyoshi, Yokohama 223-8522,
Japan
B Department of Applied Chemistry, Yamaguchi University, 2-16-1 Tokiwadai, Ube755-0097, Japan
C Institute of Materials Structure Science, High Energy Accelerator Research
Organization, 1-1 Oho, Tsukuba, Ibaraki 305-0801, Japan
Photocatalytic water splitting is one promising way to providing clean hydrogen as energy
source. Recently, Al doped SrTiO3 (STO) with co-catalysts loading which Rh/Cr2O3 as hydrogen
evolution reaction (HER) site and CoOOH as oxygen evolution reaction (OER) site gives up to 96
per cent of quantum efficiency at a UV-light wavelength range [1]. During the photocatalytic water
splitting reaction, photoexcited charge carriers transfer to the OER and HER co-catalysts have notbeen observed yet. In this work, the oxidation process of the Co-containing OER site is observedwith in situ soft-X-ray absorption spectroscopy (SXAS) technique [2].
A newly modified cell using the conversion electron yield (CEY) mode was used to conduct insitu SXAS measurements at beamline 13A at the Photon Factory, with which UV-Vis lights can bedelivered onto sample surfaces under ambient pressure conditions and surface-sensitive
information on photoinduced chemical states changes of the co-catalysts are obtained. In situ CoL SXAS measurements have been conducted for the STO photocatalyst with the both co-catalysts
loaded. Under UV irradiation without water vapor (He flow only), the Co species in CoOOH was
reduced as evidenced by increasing of Co2+ component. However, when saturated water vapor
was introduced, the Co2+ component drastically diminished, showing oxidation from Co2+ to Co3+,and the Co3+ peak top further shifts to the higher energy side with UV irradiation time, which
provides evidence for that UV-induced hole carriers transport to the Co species, and oxidize towardhigher oxidation states. DFT simulations indicate photoexcited holes are not localized on a specific
Co atom but tend to be gathering on the topmost surface layer of CoOOH. Interestingly, a STO
photocatalyst with only CoOOH co-catalyst loaded (without HER site) exhibits no oxidation but
reduction of Co, indicating that the HER site, thus, Rh/Cr2O3, is crucial to act as an electron sink totrap photoinduced electrons and promote efficient hole transfer to the CoOOH site to oxidize Co.
We conclude that water atmosphere and the presence of HER site are essentially important for thephotoinduced hole transfer to the CoOOH site and resultant oxidation of Co.
References[1]

Takata, T. et al. Nature 581, 411–414 (2020).

[2]

Shimizu, H. et al Phys. Chem. Chem. Phys. 24, 2988–2996 (2022).

NanospecFY2023

Invited Talk

Video imaging of biological molecules in action by high-speed AFM
Noriyuki Kodera
WPI-Nano Life Science Institute, Kanazawa University
High-speed atomic force microscopy (high-speed AFM) is a unique microcopy that allows direct
real-time visualization of biological macromolecules in action under near-physiological conditions,
without any chemical labeling. Typically, the temporal resolution is sub-100 ms, and the spatial
resolution is 2–3 nm in the lateral direction and ~0.1 nm in the vertical direction [1]. A wide range of
biomolecular systems and their dynamic processes have been studied by high-speed AFM,
providing deep mechanistic insights into how biomolecules function. Notably, high-speed AFM is
particularly powerful in visualizing large and flexible biomolecular systems, which conventional
structural biology methods are unable to visualize. These unique features of high-speed AFM are
well demonstrated in recent research results that visualize the structural dynamics of intrinsicallydisordered regions, single polypeptide
chains with height of ~0.5 nm in a
protein (Fig. 1a) [2], the gathering oftranslation

factorsaroundtheribosomal stalk complex (Fig. 1b) [3],and the long-range DNA degradationof CRISPR-Cas3 driven by its helicase
and nuclease activities (Fig. 1c) [4]. In
the presentation, after overviewing theprinciples and performance of highspeed AFM, movies showing dynamic
behaviors of biomolecules will beshown. In addition, our recent efforts toimprove the speed performance ofhigh-speed AFM will be discussed [5].

Fig. 1 Typical high-speed AFM images showing biomolecules in action. (a) An intrinsically disordered protein
involved in chromatin remodeling. (b) Ribosomal stalkcomplex (SB) with two structural states. (c) DNA
degradation by CRISPR-Cas3 enzyme.

[References][1] Ando, T.; Uchihashi, T.; Kodera, N., High-speed AFM and applications to biomolecular systems.
Anuu. Rev. Biophys. 2013, 42, 393-414.
[2] Kodera, N.; Noshiro, D., Dora, S. K.; …; Longhi, S.; Ando T., Structural and dynamics analysis
of intrinsically disordered proteins by high-speed atomic force microscopy. Nat. Nanotechnol.
2021, 16, 181-189.
[3] Imai, H.; Uchiumi, T.; Kodera, N., Direct visualization of translational GTPase factor pool
formed around the archaeal ribosomal P-stalk by high-speed AFM. PNAS 2020, 117, 3238632394.
[4] Yoshimi, K.; Takeshita, K.; Kodera, N.; …; Mashimo, T., Dynamic mechanisms of CRISPR
interference by Escherichia coli CRISPR-Cas3. Nat. Commun. 2022, 13, 4917.
[5] Umeda, K.; McArthur, S. J.; Kodera, N., Spatiotemporal resolution in high-speed atomic force
microscopy for studying biological macromolecules in action. Microscopy 2023, 72, 151-161.

NanospecFY2023

Invited Talk

Tip-induced control of strong quantum light-matter interactions at the nanoscale
Kyoung-Duck Park
Department of Physics, University of Science and Technology (POSTECH),
Pohang 37673, Republic of Korea
The tunability of the bandgap, radiative emission, and energy transfer in transition metal
dichalcogenide (TMD) monolayers provides a new class of functions for a wide range of ultrathin
photonic devices. Additionally, understanding and controlling the nanoscale transport of excitonic
quasiparticles, such as excitons and trions, in atomically thin 2D semiconductors are crucial toproduce highly efficient nano-excitonic devices. In this work, we present a dynamic nanomechanical strain-engineering of naturally-formed wrinkles in a WSe2 monolayer, with real-time
investigation of nano-spectroscopic properties using tip-enhanced cavity-spectroscopy [1-4]. We
reveal the modified nano-excitonic properties by the induced tensile strain at the wrinkle apex,
exhibiting the exciton funneling phenomenon. In addition, we demonstrate a nanogap device toselectively confine excitons or trions of 2D TMDs at the nanoscale, facilitated by the drift-dominant
exciton funneling into the strain-induced local spot. Furthermore, we present a method for the alloptical control of the exciton-to-trion conversion process and its spatial distributions in a MoS2
monolayer. We exploit propagating surface plasmon polaritons (SPPs) to localize hot electrons in
a 2D TMD transferred on a metal–insulator–metal (MIM) waveguide. Our work provides a new
strategy for robust, tunable, and ultracompact nano-excitonic devices using atomically thinsemiconductors.
References[1] Yeonjeong Koo et al., Advanced Materials 33, 2008234 (2021).
[2] Hyeongwoo Lee et al., Advanced Functional Materials 31, 2102893 (2021).
[3] Hyeongwoo Lee et al., Science Advances 8, eabm5236 (2022).
[4] Hyeongwoo Lee et al., Nature Communications 14, 1891 (2023).

NanospecFY2023

Invited Talk

Near-field Spectroscopic Imaging of Mesoscopic Photophysics:
2D Semiconductors and Lipid Bilayers.
Chi Chen
Research Center for Applied Sciences, Academia Sinica, Taipei, 115, Taiwan
chenchi@sinica.edu.tw
Scanning near-field optical microscopy (SNOM) is a scanning probe technique thatcombines optics with atomic force microscopy (AFM) to achieve subdiffraction-limit opticalresolution. We employed near-field photoluminescence (NF-PL) to study the atomically sharp 1Dinterfaces between WS2 and MoS2 [1]. With an optical resolution of 68 nm, a 105 nm-wide region
for quenched PL was confirmed using NF-PL imaging, which resolved the narrowest quenchingregion thus far. For low-quantum-yield materials, we developed the near-field broadband
transmission (NF-tr) method, which provides abbreviation-free and nanoscale-resolution imaging
capabilities for the entire conduction band over a highly lateral inhomogeneity [2]. Both bandgap
evolutions with varying compositions and bilayer coupling effects were visualized in real space witha spatial resolution of 135 nm.
With further instrumentation challenges [3], we developed a liquid-phase SNOM system forlateral distribution and phase segregation of supported lipid bilayers (SLB). Surprisingly, the SNOM
tip can manipulate local lipid molecules from the gel phase to the fluid phase and vice versa, whichcauses the fluorescence contrast to flip the opposite. This demonstrates that there was no particularpartition of the fluorescence tag in the fluid or gel phases. Our results reveal the fundamental
mechanisms and offer a practical guide for interpreting the partitioning of fluorescent tags.

References[1] H.-C. Chou et al., Nanoscale 14, 6323 (2022).
[2] P.-W. Tang et al., ACS Nano, 16, 5, 7503 (2022).
[3] J.-R. Yu et al., Rev. Sci. Instrum. 91, 073703 (2020).

NanospecFY2023

Invited Talk

Atomic-scale visualization of single-molecule photocurrent channels by Photon-STM
Miyabi Imai-ImadaA, B
ASISL RIKEN, BJST PRESTO
Photoinduced electron transfer (PET) from excited molecules plays central roles in various lightenergy conversion systems, and therefore it has been widely studied using optical spectroscopy
and photocurrent measurement. To understand the detailed insights into PET, as an initial processof photocurrent generation, microscopic techniques for photocurrent measurement have beendeveloped by combining scanning probe microscopes (SPMs) and optical systems. These
techniques have allowed the efficiency of photocurrent generation to be correlated to local
morphology of molecular films on the nanoscale, far below the diffraction limit of the light. However,the spatial resolution of these techniques is still not enough to distinguish individual molecules, andobserved PET signals are often obscured by ensemble-averaging over inhomogeneous local
structures. Since electron transfer between two substances depends on the direct overlap of theirelectron wavefunctions, atomic-scale geometric changes can profoundly affect the efficiency of thisprocess. Consequently, it would be highly desirable to develop a photocurrent measurement
technique with atomic spatial resolution that could reveal the fundamental physics governing the
PET process.
In this study, we achieve atomic-scale visualization of photocurrent channels of a single freebase phthalocyanine (FBPc) molecule [1] using a scanning tunneling microscope (STM) combinedwith a narrow-width tunable laser (Figures a, b) [2-4]. PET from the single FBPc molecule in thefirst singlet excited state was clearly detected via the photoinduced tunneling current through the
STM tip. Depending on the applied bias voltage, not only the direction but also the spatial
distribution of the photocurrent changes remarkably. The atomically resolved photocurrent images
allowed us to discover multiple counterflowing photocurrent channels even at a voltage where theaveraged photocurrent is almost zero. Moreover, we found direct evidence of competition between
PET and photoluminescence (PL), and demonstrated the controllability of their branching ratio
during energy relaxation by positioning the STM tip with three-dimensional, atomic precision. Ourfindings present that specific photocurrent channels can be selectively promoted or suppressed bytuning the coupling between molecular orbitals and metal wavefunctions, which provides a newperspective for improving the energy conversion efficiency by atomic-scale electronic andgeometric engineering of molecular interfaces.

References[1] M. Imai-Imada et al., Phys. Rev. B 98, 201403(R) (2018).
[2] M. Imai-Imada et al., Nature 603, 829 (2022).
[3] H. Imada, M. Imai-Imada et al., J. Chem. Phys. 157, 104302 (2022).
[4] H. Imada, M. Imai-Imada et al., Science 373, 95 (2021).

NanospecFY2023

Invited Talk

Atom by atom Electron spin resonance: coherence of Ti spins on ultra-thin MgO layers
Valeria Sheina, Hong T. Bui, We-hyo Seo, Yaowu Liu, Andreas Heinrich,
Soo-hyon Phark*
Center for Quantum Nanoscience, Institute for Basic Science, Seoul 03760, Korea
Department of Physics, Ewha Womans University, Seoul 03760, Korea
Email (Valeria Sheina): sheina.valeria@qns.science

Scanning tunneling microscopy (STM) combined with electron spin resonance (ESR) enables acoherent control of atomic spins on surfaces. However, the two metallic electrodes, i.e., tip andsubstrate, and tunneling electrons, inducing scattering of the spins, significantly limits the coherenceof their quantum states [1]. Recently, introduction of a 'remote' spin [2], which is free from the tunnelinginduced scattering, has shown a coherence time (T2), reaching the theoretical limit as determined only
by its spin relaxation time (T1) [3]. Here, we report an ESR-STM study on the spin relaxation andquantum coherence of single Ti atoms (S = 1/2) on 2 and 3 ML MgO, Ti(2) and Ti(3), respectively. First,
Ti(3) in the tunnel junction showed a T2 that is longer by the factor of ~5 than Ti(2), indicative of aconsiderably suppressed coupling with the substrate on 3 ML. In addition, both Ti(2) and Ti(3) showedlinear dependence of decoherence rates (1/T2) on the tunneling current, with the same slopes, which
revealed the effect of the tunneling electron on the spin dynamics, contributing independent of thedecoupling layer thickness, and thus allowed a quantitative understanding on it. A remote Ti(3) showed
T1 of ~10 s, longer by 2 orders of magnitude than Ti(2), which is well understood by the enhanced
decoupling from the substrate. However, T2 of a remote Ti(3) remained similar to that of Ti(2), implying
existence of a significant decoherence process as revealed by free induction decay time (T*2)
measurement, probably due to the spin fluctuation of the single atom magnet in its proximity [4]. This
work serves as a quantitative insight, pointing at the importance of decoupling the spins from thesubstrate as well as the tunneling electrons and shedding light on the on-surface spins as a noble
atomic-scale qubit platform [3].
References:[1] W. Paul et al. Nature Phys. 13, 403–407 (2017).
[2] S. Phark et al. ACS Nano 17, 14144–14151 (2023).
[3] Y. Wang et al. Science 382, 6666 (2023).
[4] S. Phark et al. Adv. Sci. 10, 2302033 (2023).

NanospecFY2023

Invited Talk

Tomography Scan of Charge Density Wave in NbSe2
Chun-Liang Lin
Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu,
TaiwanCharge density wave (CDW) resulting from a periodic distortion in the lattice creates new orders
beyond the original lattice. In 2H-NbSe2, one of the layered transition metal dichalcogenides (TMD),
the 3×3 charge order appears in two-dimensional (2D) layers. Although CDW can be observed bydifferent techniques, the spatial distribution within a 2D layer has never been systematicallyvisualized. Here, by using scanning tunneling microscopy (STM) and density functional theory(DFT), we monitored the evolution of CDW along the c-axis and realized a tomography scan of
CDW of the topmost layer. The results show that the appearance of the CDW varies while tuning
the tunneling current and undergoes a transition from the outermost Se level to Nb level. The
calculation of orbital charge distributions shows that both CDW intensity modulation and thetransition are strongly correlated with the distribution of Se 4p orbitals and Nb 4d orbitals.

Reference:[1] Jyun-Yu Wu, Chun-Liang Lin* et al. arXiv:2303.12053v1

NanospecFY2023

Contributed Talk

Pioneering tip-enhanced nonlinear optics and spectroscopy
Shota TakahashiA, Atsunori SakuraiA, B, Tatsuto MochizukiA, B, Toshiki SugimotoA, B
A

Institute for Molecular Science, BGraduate Institute for Advanced Science, SOKENDAI
Plasmonic excitation at the nanogap between a metallic nanotip and a surface results inthe strong localization and enhancement of the electromagnetic field, thereby amplifying weak
spectroscopic signals from sub-diffraction-limited volumes. This mechanism of light compression
and amplification, when integrated with scanning probe microscopy, facilitates nanoscale opticalmapping of materials. While prior studies in tip-enhanced nanoscopy have largely focused on linear
optical responses such as light scattering and photoluminescence, recent years have seen
significant advancements in the nanoscale detection of nonlinear optical processes, achieving
notable sensitivity and spatial resolution [1-3]. A critical limitation in these studies on tip-enhanced
nonlinear optics, however, is the restricted wavelength range, which is typically limited to the visible
to near-infrared region. These wavelengths are too short to resonantly excite molecular vibrations,which typically resonate with mid-infrared light, thus preventing the application of tip-enhanced
nonlinear optics in molecular vibrational nanoscopy.
In this study, we directly tackle this issue. To exploit the tip-enhanced nonlinear opticalphenomena as an advanced molecular spectroscopic technique, we explore the nonlinear opticalproperties of tip-substrate nanocavities over a broader wavelength range, extending from thevisible to the mid-infrared region. We focus on tip-enhanced second-harmonic generation (TESHG)
induced by a wavelength-tunable femtosecond laser, demonstrating efficient tip-enhancement of
nonlinear optical effects across this extended wavelength range (Fig. 1) [4]. Furthermore, we showthat this TESHG response can be significantly modulated and controlled by an external electricfield. Leveraging these insights, we recently established nanoscale
tip-enhanced molecular spectroscopy by extending our TESHG
setup and developing a vibrational nanoscopic system based on tipenhanced sum-frequency generation (TESFG). By irradiating the tipsubstrate nanocavity with both mid- and near-infrared femtosecond
pulses, we successfully captured vibrational SFG nanoscopic signals
from an ultrathin molecular layer not only on (plasmonic) Au surfaces
but also on (non-plasmonic) Pt and Ni surfaces. Our results lay a new
foundation for understanding and precisely manipulating nonlinear Figure 1 Nonlinear optical
optical phenomena in plasmonic nanocavities, opening new avenues effectataplasmonic

for detailed exploration of correlated chemical and topographic nanogap between a tip
information through tip-enhanced nonlinear nanoscopy.

and a substrate.

[1] C.-F. Wang and P. Z. El-Khoury, J. Phys. Chem. Lett. 13, 7350 (2022). [2] C.-F. Wang and P. Z.
El-Khoury, J. Phys. Chem. Lett. 12, 10761 (2021). [3] V. Kravtsov et al., Nat. Nanotechnol. 11, 459(2016). [4] S. Takahashi et al., J. Phys. Chem. Lett. 14, 6919 (2023).

NanospecFY2023

PosterPoster presentation
Please be aware that No. 1 to 32 have been nominated for the Poster Award. We invite all participants
to select up to three posters that they found outstanding and to record their choices on the provided ballot.
Ballots will be distributed at the conference reception. After poster session, we kindly ask you to deposit
your completed ballot in the designated collection box.

1.

STM observation of the initial Ag overlayer formation on the Ni(110) surface
Aoi Mizuhara, Tsuneo Fukuda, Kenji Umezawa

2.

Using AFM Manipulation of Fluorescence On and Off to Reveal the Partition of Tags between Gel
and Fluid Phases
Jia-Ru Yu, He-Chun Chou, Wei-Ssu Liao, Chi Chen

3.

Clarifications of local interactions though image processing of the data acquired from energy
materials by scanning probe microscopy
Sota Tsubokura, Shoya Kawano, Yumiko Imai, Tadashi Ueda, Kei-ichi Nakamoto, Hirohisa Hioki,
Haruo Noma, Taketoshi Minato

4.

The Coulomb interaction between single MgNc molecules and insulating thin films on a metal
substrate -Controlling molecular optical properties from the substrateHiroki Nanbu, Hiroshi Imada, J. Ahn,M. Lee, X. Ouyang, Atuya Muranaka, J. Jung, H. Lim,
Yousoo Kim

5.

Analysis of Water Adsorption On TiO2(110)-(1x2) Surface By Scanning Tunneling Microscopy
Fengxua Li, Zhuo Diao, Daiki Katsube, Linfeng Hou, Hayato Yamashita, Masayuki Abe

6.

Chloride-Gated Electrical Switching of Single-Molecule Junction of Anion Receptor
Harunari Okura, Bui Okada, Hiromitsu Maeda, Tomoaki Nishino

7.

Visualization and Characterization of Surface Plasmon Polaritons Propagating at a Buried
Metal/Dielectric Interface Sensitized by Photofunctional Quantum Dots
Kazuki Kamada, DaeGwi Kim, Masahiro Shibuta

8.

STM study of anormaly CDW formation on layered material NbSe 2
Ryo Ichikawa, Toyokazu Yamada

9.

A Useful Method of Observing Diatom Frustules via Digital Holographic Microscopy
Makoto Saito, Masaki Kitamura, Yuki Ide, Minh Hieu Nguyen, Binh Duong Le, Anh Tuan Mai,
Daisuke Miyashiro, Shigeki Mayama, Kazuo Umemura

NanospecFY2023

Poster

10. Synthesis and spectroscopic measurements of large-area hydrogen boride sheets
Kazuki Yamaguchi, Masato Niibe, Toshihide Sumi, Xiaoni Zhang, Eiken Nakamura、Kiyohisa
Tanaka, Koji Nakanishi, Kazuhiro Kanda, Masafumi Horio, Takahiro Kondoh, Iwao Matsuda
11. In-situ Evaluation of Solid Layer Formation at Superconcentrated Electrolyte/Electrode Interface
Akito Kobayashi, Masanori Nagasaka, Taketoshi Minato, Katsuyoshi Ikeda, and Kenta
Motobayashi
12. Atomically demonstration of SnO2 (4x1) reconstruction by STM/AFM
L.Hou, D.Katsube, T.Ishibe, Y.Nakamura, H.Yamashita, M.Abe
13. Fabrication of plasmonic probes for tip-enhanced Raman spectroscopy using FIB
Kazunori Hirosawa, Kaifeng Zhang, Masanori Hara and Masamichi Yoshimura
14. Development of a high coherence and ultrafast electron source
Yui Iwasaki, Yuri Saida, Ryota Nishimori, Masaki Hada
15. Mechanism of Binary Conductance Switching of Fullerene Single Molecules in Break Junction
Experiments
Aoshi Yamane, Fujii Shintaro, Tomoaki Nishino
16. Development of integrated system for machine-learning automatic RHEED analysis and MBE
chamber
Toshiro Osawa, Asako Yoshinari, Masato Kotsugi, Naoka Nagamura
17. Development of automatic Fermi surfaces analysis using data science
Daichi Ishikawa, Kentaro Fuku, Yoshio Miura, Yasuhiko Igarashi, Yuma Iwasaki, Yuya Sakuraba,
Koichiro Yaji, Alexandre Lira Foggiatto, Arpita Varadwaj, Naoka Nagamura, Masato Kotsugi
18. Analysis of DMI Energy in the Formation Process of Skyrmions Using an Extended Landau Free
Energy Model
Yotaro Machida, Michiki Taniwaki, Alexandre Lira Foggiatto, Chiharu Mitsumata, Ippei Obayashi,
Yasuaki Hiraoka, Kyoko Ishizaka，Masato Kotsugi
19. Selective dehydrogenation of methanol on Cu(977) and Pd/Cu(977) surfaces
Yoshiko Sakaguchi, Wataru Osada, Kozo Mukai, Shunsuke Tanaka, Jun Yoshinobu
20. STM atom manipulation of single Ag atoms on Si(111)-(7×7) at room temperature
Junya Okuyama, Diao Zhuo, Masayuki Abe, Hayato Yamashita
21. Identify the Relationship between Crystal Structure and Electronic State of Boron Nitride Using
Density Functional Theory and Machine Learning
Reika Hasegawa, Arpita Varadwaj, Alexandre Lira Foggiatto, Masahito Niibe, Yasunobu Ando,
Iwao Matsuda, Masato Kotsugi

NanospecFY2023

Poster

22. Observation of ZnO(0001) surface structure by scanning tunneling microscopy
Yamato Tashiro, Masayuki Abe , Hayato Yamashita
23. Preparation of a solution containing copper complexes with thiocyanate groups in a hydrophobic
solvent and solid-state transformation of the film formed using the solution into copper thiocyanate
Kota Kobayashi, Takeshi Tanaka, Yoichi Nakashima, and Takayo Moriuchi
24. Ultrafast dynamics of Charge-density wave in 1T-TiSe2
Yu Mizukoshi, Takumi Fukuda, Muneaki Hase
25. RHEED analysis methods using machine learning and application for film preparation
Asako Yoshinari, Toshiro Osawa, Shingo Takezawa, Shunsuke Sato, Yuma Iwasaki, Yasunobu
Ando, Tarojiro Matsumura, Rei Hobara, Shuji Hasegawa, Masato Kotsugi, Naoka Nagamura
26. Investigating energy transfer from Alq3 molecules to Si by pump-probe spectroscopy
Yu-Chan Tai, Wen-Yen Tzeng, Jhen-Dong Lin, Yi-Hou Kuo, Fu-Xiang Rikudo Chen, Ruei-Jhe Tu,
Ming-Yang Huang, Shyh-Shii Pai, Nick Weihan Chang, Sheng-Yang Tseng, Chi Chen, Chun-Liang
Lin, Atsushi Yabushita, Shun-Jen Cheng, Chih-Wei Luo
27. Monitoring of the Oxygen Partial Pressure inside the Gas Diffuision Layer of Polymer Electrolyte
Fuel Cells during High-Temperature Power Generation
Christopher Schreiber, Junji Inukai
28. Study on Metal-Supported Photocatalyst Materials Using High-Speed Atomic Force Microscopy
Ryotaro Tani, Hayato Yamashita, Masayuki Abe
29. Atomic-Level Patterning of Si(111) Surface using STM Lithography
Kensho Tsukuda, Masayuki Abe, Hayato Yamashita, Jo Onoda, Linfeng Hou
30. Visualization of friction distribution in stearic acid solution at cross-sectional direction using
simultaneous system of FM-AFM / LFM
Yuya Yamaguchi, Haruto Gato, Akinori Kogure, Hiroshi Arai, Masahiro Ota, Kaisei Sato, Shinya
Sasaki31. Study of hydrogen addition and desorption processes in iridium complex using transmission FT-IR
Tianle Wang, Wataru Osada, Kozo Mukai, Shunsuke Tanaka, Takanori Koitaya, Kenichi Fujita, Jun
Yoshinobu
32. Study on a method to grow self-assembled-monolayer covered tips for quantitative Atomic ForceMicrosocpoy
Koji Tomofuji, Toshikazu Kitagawa, Naruo Sasaki, Dai Kobayashi, Hideki Kawakatsu
33. TPD Study of Argon Hydride ArH from Argon Implanted Pd(111) Surfaces
Hayato Naka, Aruku Fukushima, Kohei Izawa, Tomotaka Hirano, Kazuo WatanabeNanospecFY2023

Poster

34. Selective coupling of coherent optical phonons in YBa2Cu3O7-δ with electronic transitions
Kunie Ishioka, Alexej Pashkin, Christian Bernhard, Hrvoje Petek, Xin Yao, and Jure Demsar
35. Construction of optics combined low temperature STM
Alexina Ollier, Pegah Farahi Shandiz, Jiyoon Lee, Alexina Ollier, Lei Fang, Minsu Seo, Soohyeong
Lee, Sangwon Yoon, Andreas J. Heinrich and Wonjun Jang
36. Visualization of Band Shifting and Interlayer Coupling in W xMo1−xS2 Alloys Using Near-Field
Broadband Absorption Microscopy
Po-Wen Tang, Shiue-Yuan Shiau, He-Chun Chou, Xin-Quan Zhang, Jia-Ru Yu, Chun-Te Sung, YiHsien Lee, and Chi Chen
37. Nanoscopic Observation and Control of Chiro-Optical Force
Junsuke Yamanishi, Hyo-Yong Ahn, and Hiromi Okamoto
38. Investigation of 3D-Fermi-surface by using the the angle-resolved photoelectron spectroscopy withthe synchrotron radiation
Shin-ichiro Tanaka, Shigemasa Suga, Keiji Ueno, Keisuke Fukutani, Seiji Makita, FumihikoMatsui, Kiyohisa Tanaka
39. Tip-enhanced Raman study of pentacene derivative on Ag surface: adsorption structure anddynamics
Norihiro Aiga, Takenori Nagasawa and Satoshi Takeuchi
40. Time-resolved photoemission study of photo-excited carrier dynamics in zinc phthalocyanine thinfilms grown on HOPG substrate
Isamu Yamamoto, Azuma Junpei, Masaki Imamura, Kazutoshi Takahashi
41. Development of Electronics for Low-temperature Scanning Near-Field Optical Microscopy
Tomonori Toyoda, Takashi Kumagai, Msasyuki Abe
42. Atomic-scale investigation for electronic properties of multiple resonance thermally activateddelayed fluorescence molecule
Jaehyun Bae, Miyabi Imai-Imada, Lee Minhui, Hyungsuk Kim, Hiroshi Imada, Youichi Tsuchiya,
Takuji Hatakeyama, Chihaya Adachi, Yousoo Kim
43. s-SNOM using kHz laser sources
Samuel Palato
44. Single molecule photonics for nanospectroscopy and beyond
Hiroshi Imada, Miyabi Imai-Imada, Yousoo Kim
45. In-situ Evaluation of Solid Layer Formation at Superconcentrated Electrolyte/Electrode Interface
Akito Kobayashi, Masanori Nagasaka, Taketoshi Minato, Katsuyoshi Ikeda, and Kenta
Motobayashi

NanospecFY2023

Poster

46. Quantum dynamics of a photoexcited electronic system coupled to an anharmonic oscillator
environment
Kuniyuki Miwa, Souichi Sakamoto, and Akihito Ishizaki
47. DNA Investigation by AFM and nano-FTIR
Chaweewan Sapcharoenkun, Jun Nishida, Akihiro Otomo, Taketoshi Minato, Ryota Iino, andTakashi Kumagai
48. Electrochemical Imaging of Hydrogen Evolution Reaction at Surface of MoS 2 Nanoribbons by
Scanning Electrochemical Cell Microscopy
Kaito Hirata, Kota Honda, Ma Zongpeng, Pablo Solís Fernández, Hiroki Ago, Yasufumi Takahashi
49. Metastability in the Insulator-Metal Transition for Individual VO2 Nanoparticles
K. Nishikawa, J. Nishida, T. Kumagai, Y. Watanabe
50. Nano-scale study of reaction film using zinc dialkyl dithiophosphates induced by shear stress
Kaisei Sato, Shinya Sasaki
51. Multimodal photoemission investigation of 1T-TaS2 chiral charge density wave phase transition bysoft X-ray/VUV photoelectron momentum microscope
Fumihiko Matsui, Kenta Hagiwara, Shigemasa Suga
52. Reaction Mechanisms at the Interfaces between Halogen Ions and Metal Electrodes in Liquid
Electrolytes Analyzed by Scanning Probe Microscopy
Yumiko Imai, Tadashi Ueda, Kei-ichi Nakamoto, Taketoshi Minato

Luncheon Seminar
Quantum Design Japan

Introduction of neaSCOPE that realize wavelength-independent nanoscale optical imaging &spectroscopy across THz, IR and visible spectral ranges by combining SPM with optics
The neaSCOPE was originally developed as a scattering-type scanning nea-field optical
microscope (s-SNOM). Owing to unique patented detection, neaSCOPE realize wavelengthindependent 10-20nm optical resolution imaging and spectroscopy across THz, IR and visible
spectral ranges without background. We can offer integrated system with light sources thatguarantee reliable data. Furthermore, it can be combined with your own light source such assynchrotron beam line. Over 10 neaSCOPEs has been installed at synchrotron facilities aroundthe world. These days, neaSCOPE is developed to support various measurement modes both
optical and mechanical for comprehensive and correlative nanoscale analytics.
I’m going to introduce principal of measurement, instrumentation and the latest applications.

UNISOKU Co., Ltd.

TBA