研究者詳細 - 中嶋　敦

論文 - 中嶋　敦

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Photoexcited Electron Transfer Properties at C₆₀ Film on Graphite and on Au(111) Interfaces Studied by Two-Photon Photoemission Spectroscopy

M. Shibuta, K. Yamamoto, K. Yamagiwa, T. Eguchi, A. Nakajima

Chemistry Letters （Chemical Society of Japan） 46 （ 10 ） 1528 - 1531 2017年08月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り

Geometric and electronic properties of Si-atom doped Al clusters: Robustness of binary superatoms against charging

M. Akutsu, K. Koyasu, J. Atobe, K. Miyajima, M. Mitsui, H. Tsunoyama, A. Nakajima

Physical Chemistry Chemical Physics （Royal Society of Chemistry） 19 （ 31 ） 20401 - 20411 2017年07月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 14639076

The geometric and electronic properties of silicon-atom-doped aluminum clusters, AlnSim (n = 7-30, m = 0-2), were investigated experimentally. The size dependences of the ionization energy and electron affinity of AlnSim show that the stability of AlnSim is governed by the total number of valence electrons in the clusters, where Al and Si atoms behave as trivalent and tetravalent atoms, respectively. Together with theoretical calculations, it has been revealed that neutral Al10Si and Al12Si have a cage-like geometry with central Si atom encapsulation and closed electronic structures of superatomic orbitals (SAOs), and also that they both exhibit geometric robustness against reductive and oxidative changes as cage-like binary superatoms of Si@Al10 and Si@Al12. As well as the single-atom-doped binary superatoms, the effect of symmetry lowering was examined by doping a second Si atom toward the electron SAO closing of 2P SAO, forming Al11Si2. The corresponding anion and cation clusters keep their geometry of the neutral intact, and the ionization energy is low compared to others, showing that Al11Si2 is characterized to be, Si@Al11Si as an alkaline-like binary superatom. For Al21Si2, a face-sharing bi-icosahedral structure was identified to be the most stable as dimeric superatom clusters.

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A designer ligand field for blue-green luminescence of organoeuropium(II) sandwich complexes with cyclononatetraenyl ligands

K. Kawasaki, R. Sugiyama, T. Tsuji, T. Iwasa, H. Tsunoyama, Y. Mizuhata, N. Tokitoh, A. Nakajima

Chemical Communications （Royal Society of Chemistry） 53 （ 49 ） 6557 - 6560 2017年05月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 1359-7345

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Two-Photon Photoelectron Emission Microscopy for Surface Plasmon Polaritons at the Au(111) Surface Decorated with Alkanethiolate Self-Assembled Monolayers

K. Yamagiwa, M. Shibuta, A. Nakajima

Phys. Chem. Chem. Phys. （Royal Society of Chemistry） 19 （ 21 ） 13455 - 13461 2017年05月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り

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Photoexcited State Confinement in Two-Dimensional Crystalline Anthracene Monolayer at Room Temperature

M. Shibuta, N. Hirata, T. Eguchi, A. Nakajima

ACS Nano （American Chemical Society） 11 （ 4 ） 4307 - 4314 2017年04月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 1936-0851

Organic thin film electronics place a high demand on bottom-up technology to form a two-dimensionally (2D) functional unit consisting of a single molecular crystalline layer bound to a layered structure. As the strong interaction between a substrate and molecules makes it difficult to evaluate the electronic properties of organic films, the nature of electronic excited states has not been elucidated. Here, we study a 2D crystalline anthracene monolayer electronically decoupled by alkanethiolates on a gold substrate using scanning tunneling microscopy and time-resolved two-photon photoemission spectroscopy and unravel the geometric/electronic structures and excited electron dynamics. Our data reveal that dispersive 2D excited electrons on the surface can be highly coupled with an annihilation of nondispersive excitons that facilitate electron emission with vibronic interaction. Our results provide a fundamental framework for understanding photoexcited anthracene monolayer and show how the coupling between dispersive and nondispersive excited states may assist charge separation in crystalline molecular layers.

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Highly Ordered Self-Assembled Monolayers of Carboxy- and Ester-Terminated Alkanethiols on Au(111): Infrared Absorption and Hyperthermal-Deposition Experiments with Cr(benzene)₂ Ions

N. Hirata, S. Suga, Y. Noguchi, M. Shibuta, H. Tsunoyama, T. Eguchi, A. Nakajima

Journal of Physical Chemistry C （American Chemical Society） 121 （ 12 ） 6736 - 6747 2017年03月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 19327447

The physical and chemical properties of carboxy- and ester-terminated alkanethiolate self-assembled monolayers (SAMs) on a gold (Au) substrate (Au(111)), which were prepared in a one-pot reaction, were investigated by means of infrared reflection absorption spectroscopy (IRAS) and hyperthermal-deposition experiments with Cr(benzene)2 ions. IRAS spectra showed that the vibrational modes of hydrogen-bonded COOH and CH2 wagging are sensitive to the flatness and cleanness of Au substrates for COOH-SAM and COOMe-/COOEt-SAM, respectively. The intensities of CH2 wagging modes are temperature dependent, which is relevant to the alkyl chain ordering in the highly ordered SAM. The terminal groups of the highly ordered SAM are dissociated by hyperthermal collision events of gas-phase-synthesized Cr(benzene)2 sandwich complex ions, and the adsorption properties of deposited Cr(benzene)2 are discussed in relation to IRAS and temperature-programmed desorption (TPD) measurements.

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Adiabatic electron affinity of pentacene and perfluoropentacene molecules studied by anion photoelectron spectroscopy: Molecular insights into electronic properties

T. Masubuchi, Y. Sugawara, A. Nakajima

Journal of Chemical Physics （American Institute of Physics） 145 （ 24 ） 244306 2016年12月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 00219606

Pentacene (C22H14, PEN) and perfluoropentacene (C22F14, PFP) are considered promising building blocks of organic semiconductors. Using gas-phase anion photoelectron spectroscopy, the adiabatic electron affinity of PEN and PFP molecules is determined to be 1.43 ± 0.03 and 2.74 ± 0.03 eV, respectively, and the S0-T1 transition energies of PEN and PFP are evaluated to be 0.96 ± 0.06 and 0.72 ± 0.05 eV, respectively. Photoelectron spectra indicate that the vibronic coupling in PFP is stronger than that in PEN. Quantum chemistry calculations demonstrate that the strong vibronic coupling originates from significant structural displacement upon electron injection to PFP.

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Fabrication and Characterization of Floating Memory Devices Based on Thiolate-Protected Gold Nanoclusters

N. Hirata, M. Sato, E. Tsunemi, Y. Watanabe, H. Tsunoyama, M. Nakaya, T. Eguchi, Y. Negishi, A. Nakajima

Journal of Physical Chemistry C （American Chemical Society） 121 （ 20 ） 10638 - 10644 2016年11月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 1932-7447

The floating memory properties of thiolate-protected gold (Au:SR) nanoclusters, Au25(SR)18, Au38(SR)24, Au144(SR)60, and Au333(SR)79 (R = C12H25), and Au colloids were investigated using four-probe measurements in vacuum. Uniform and monolayer films of Au:SR nanoclusters or Au colloids were formed as floating memory layers on p-type Si substrates by Langmuir-Blodgett method. The fluoropolymer (CYTOP, ∼15 nm thick) was spin-coated on top to form a hydrophobic insulating layer. Using Au dot (∼40 nm thick) as the anode electrode, the capacitance-voltage (C-V) measurements were performed using the Au and Cu plate electrodes as contact points for the two probes. Clockwise hysteresis curves originating from the Au:SR nanoclusters or Au colloids were observed, and the hysteresis width was dependent on the size of the Au:SR nanoclusters and the sample temperature. In particular, for the Au38(SR)24 nanocluster, multiple phases were observed in the C-V curve, implying their application in multivalued memory devices.

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Imaging and spectromicroscopy of photocarrier electron dynamics in C₆₀ fullerene thin films

M. Shibuta, K. Yamagiwa, T. Eguchi, A. Nakajima

Applied Physics Letters （American Institute of Physics） 109 （ 20 ） 203111 2016年11月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 00036951

We have employed a two-photon photoelectron emission microscopy (2P-PEEM) to observe the photocarrier electron dynamics in an organic thin film of fullerene (C60) formed on a highly oriented pyrolytic graphite with a spatial resolution of ca. 135 nm. In this approach, photocarrier electrons in C60 single-layer islands generated by the first pump photon are detected by the second probe photon. These spectromicroscopic observations conducted over a 100 × 100 nm2 region of C60 islands consistently reproduced the macroscopic two-photon photoemission spectrum of fully covered C60 monolayer film, where the energy of photocarrier electron in the islands was +0.9 eV relative to the Fermi level. Time-resolved 2P-PEEM revealed that the photocarrier electron decayed from the monolayered C60 islands into the substrate with a time constant of 470 ± 30 fs.

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Direct observation of photocarrier electron dynamics in C₆₀ films on graphite by time-resolved two-photon photoemission

M. Shibuta, K. Yamamoto, T. Ohta, M. Nakaya, T. Eguchi, A. Nakajima

Scientific Reports （Springer Nature） 6 35853 2016年10月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 2045-2322

Time-resolved two-photon photoemission (TR-2PPE) spectroscopy is employed to probe the electronic states of a C60 fullerene film formed on highly oriented pyrolytic graphite (HOPG), acting as a model two-dimensional (2D) material for multi-layered graphene. Owing to the in-plane sp 2-hybridized nature of the HOPG, the TR-2PPE spectra reveal the energetics and dynamics of photocarriers in the C60 film: after hot excitons are nascently formed in C60 via intramolecular excitation by a pump photon, they dissociate into photocarriers of free electrons and the corresponding holes, and the electrons are subsequently detected by a probe photon as photoelectrons. The decay rate of photocarriers from the C60 film into the HOPG is evaluated to be 1.31 × 1012 s-1, suggesting a weak van der Waals interaction at the interface, where the photocarriers tentatively occupy the lowest unoccupied molecular orbital (LUMO) of C60. The photocarrier electron dynamics following the hot exciton dissociation in the organic thin films has not been realized for any metallic substrates exhibiting strong interactions with the overlayer. Furthermore, the thickness dependence of the electron lifetime in the LUMO reveals that the electron hopping rate in C60 layers is 3.3 ± 1.2 × 1013 s-1.

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Multiple-decker and ring sandwich formation of manganese-benzene organometallic cluster anions: Mn_nBz_n^- (n = 1-5 and 18)

T. Masubuchi, T. Iwasa, A. Nakajima

Physical Chemistry Chemical Physics （Royal Chemical of Society） 18 （ 37 ） 26049 - 26056 2016年09月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 14639076

Organometallic multiple-decker sandwich clusters are topics of great interest due to their unique electronic and magnetic properties originating from anisotropic structures. We report a joint anion photoelectron spectroscopic and computational study on a new family of manganese (Mn)-benzene (Bz) anionic clusters MnnBzn-. In stark contrast to the most widely studied vanadium-Bz sandwich clusters, it is found that MnnBzn- (n = 1-5) clusters exhibit unprecedented multiple-decker structures with a tilted Mn-Bz stacking and a monotonically increasing behavior of their high spin multiplicities. Furthermore, a couple of closed ring forms of Mn18Bz18- and its neutral state are computationally anticipated as an intriguing "cluster of Mn1Bz1 clusters" in which the neutral Mn18Bz18 has extremely high C18h symmetry with an uncommon spin state of 2S + 1 = 55. The extensively delocalized electron environment of Mn18Bz18 allows the simple Hückel model to reveal the strong intra-atomic exchange interactions within the Mn 3d electrons.

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Charge Transfer Complexation of Ta-Encapsulating Ta@Si₁₆ Superatom with C₆₀

T. Ohta, M. Shibuta, H. Tsunoyama, T. Eguchi, A. Nakajima

Journal of Physical Chemistry C （American Chemical Society） 120 （ 28 ） 15265 - 15271 2016年07月

研究論文（学術雑誌）, 最終著者, 責任著者, 査読有り, ISSN 19327447

The tantalum-encapsulating Si16 cage nanocluster superatom (Ta@Si16) has been a promising candidate for a building block of nanocluster-based functional materials. Its chemical states of Ta@Si16 deposited on an electron acceptable C60 fullerene film were evaluated by X-ray and ultraviolet photoelectron spectroscopies (XPS and UPS, respectively). XPS results for Si, Ta, and C showed that Ta@Si16 combines with a single C60 molecule to form the superatomic charge transfer (CT) complex, (Ta@Si16)+C60-. The high thermal and chemical robustness of the superatomic CT complex has been revealed by the XPS and UPS measurements conducted before and after heat treatment and oxygen exposure. Even when heated to 720 K or subjected to ambient oxygen, Ta@Si16 retained its original framework, forming oxides of Ta@Si16 superatom.

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Extended Smoluchowski Model for the Formation of Size-Selected Silver Nanoclusters Generated via Modulated Pulsed Power Magnetron Sputtering

C.-H. Zhang, H. Tsunoyama, Y. Feng, A. Nakajima

Journal of Physical Chemistry C （American Chemical Society） 120 （ 10 ） 5667 - 5672 2016年03月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 1932-7447

Size-selected silver nanoclusters (NCs) were generated using a modulated pulsed power magnetron sputtering (MPP-MSP) system coupled with a mass spectrometer, and their formation mechanism was investigated by applying an extended Smoluchowski model. Attractive interactions between NC cations and anions were incorporated into the conventional Smoluchowski equations to explain the origin of the size tuning of Ag NCs prepared via MPP-MSP. Bunches overlapped as the repetition rate (f) and peak power (Pp) increased, resulting in the initial formation of large ionic nanoclusters, ultimately causing a reduction in the size of the NC ions due to neutralization via NC cation-anion charge recombination and the formation of aggregates.

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Interplay between experiments and calculations for organometallic clusters and caged clusters

A. Nakajima

AIP Conference Proceedings （American Institute of Physics） 1702 090031-1 - 090031-6 2015年12月

研究論文（国際会議プロシーディングス）, 単著, 筆頭著者, 最終著者, 責任著者, 査読有り, ISSN 0094-243X

Clusters consisting of 10-1000 atoms exhibit size-dependent electronic and geometric properties. In particular, composite clusters consisting of several elements and/or components provide a promising way for a bottom-up approach for designing functional advanced materials, because the functionality of the composite clusters can be optimized not only by the cluster size but also by their compositions. In the formation of composite clusters, their geometric symmetry and dimensionality are emphasized to control the physical and chemical properties, because selective and anisotropic enhancements for optical, chemical, and magnetic properties can be expected. Organometallic clusters and caged clusters are demonstrated as a representative example of designing the functionality of the composite clusters. Organometallic vanadium-benzene forms a one dimensional sandwich structure showing ferromagnetic behaviors and anomalously large HOMO-LUMO gap differences of two spin orbitals, which can be regarded as spin-filter components for cluster-based spintronic devices. Caged clusters of aluminum (Al) are well stabilized both geometrically and electronically at Al12X, behaving as a "superatom".

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Chemical Characterization of an Alkali-Like Superatom Consisting of a Ta-Encapsulating Si₁₆ Cage

M. Shibuta, T. Ohta, M. Nakaya, H. Tsunoyama, T. Eguchi, A. Nakajima

Journal of the American Chemical Society （American Chemical Society） 137 （ 44 ） 14015 - 14018 2015年10月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 00027863

Chemical characterization was performed for an alkali-like superatom consisting of a Ta-encapsulating Si16 cage, Ta@Si16, deposited on a graphite substrate using X-ray photoelectron spectroscopy (XPS) to element-specifically clarify the local electronic structure of the cage atoms. The XPS spectra derived from Ta 4f and Si 2p core levels have been well modeled with a single chemical component, revealing the formation of a symmetric Si cage around the Ta atom in the deposited nanoclusters. On chemical treatments by heating or oxygen exposure, it is found that the deposited Ta@Si16 is thermally stable up to 700 K and is also exceptionally less reactive toward oxygen compared to other Ta-Si nanoclusters, although some heat degradation and oxidation accompany the treatments. These results show the promising possibility of applying Ta@Si16 as a building block to fabricate cluster-assembled materials consisting of naked nanoclusters.

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Excitation and Relaxation Dynamics of Two-Dimensional Photoexcited Electrons on Alkanethiolate Self-Assembled Monolayers

M. Shibuta, N. Hirata, R. Matsui, M. Nakaya, T. Eguchi, A. Nakajima

Journal of Physical Chemistry C （American Chemical Society） 119 （ 40 ） 22945 - 22953 2015年09月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 1932-7447

The electron dynamics in alkanethiolate self-assembled monolayers (Cn-SAMs; n = 6-18, where n is the number of alkyl carbons) formed on Au(111) surfaces has been investigated by time- and angle-resolved two-photon photoemission spectroscopy. The time evolution of photoexcited electrons flowing down into image potential states (IPSs) formed on standing-up structure of SAMs is resolved two-dimensionally; the electron lifetime in the IPS increases with chain length, from sub-ps to 100 ps. The chain length dependence of the IPS lifetime is particularly marked at shorter chain lengths of n = 6-10, whereas it becomes milder at chain lengths above n = 10, whose alkyl layer thickness is ≈10 Å. This thickness dependence can be explained by two competitive channels for the decay of IPS electrons: one is electronic coupling of IPS with unoccupied bulk Au states and an interfacial state localized at the Au-S linkage, and the other is IPS electron decay to the Au substrate through a tunneling barrier of insulating alkyl chains. The former is most influential at shorter chain lengths, while the latter is solely dominant at longer chain lengths. In addition, the photon energy dependence of the IPS intensity revealed that electron injection into the IPS is mediated effectively by an electron excitation into interfacial resonance formed in the alkyl layer.

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Hard x-ray photoelectron spectroscopy using an environmental cell with silicon nitride membrane windows

E. Tsunemi, Y. Watanabe, H. Oji, Y. T. Cui, J. Y. Son, A. Nakajima

Journal of Applied Physics （American Institute of Physics） 117 （ 23 ） 234902 2015年06月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 0021-8979

We applied hard x-ray photoelectron spectroscopy (HAXPES) to a sample under ambient pressure conditions using an environmental cell with an approximately 24 nm-thick SiNx membrane window. As a model chemical substance, europium (II) iodide (EuI2) sealed in the cell with argon gas was investigated with HAXPES to identify the chemical species present inside the cell. The optical and morphological properties of the sample within the cell were measured with optical and fluorescent microscopy, scanning electron microscopy, cathodoluminescence, and energy dispersive x-ray spectrometry. We confirmed the effectiveness of the gas barrier properties of the cell with the SiNx window and demonstrated its applicability to various other optical and electron measurements as well as HAXPES.

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Heterodimerization via the covalent bonding of Ta@Si₁₆ nanoclusters and C₆₀ molecules

M. Nakaya, T. Iwasa, H. Tsunoyama, T. Eguchi, A. Nakajima

Journal of Physical Chemistry C （American Chemical Society） 119 （ 20 ） 10962 - 10968 2015年02月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 19327447

Initial products prepared via the surface immobilization of Ta-atom-encapsulated Si16 cage (Ta@Si16) nanoclusters on solid surfaces terminated with monolayer films of C60 molecules were investigated using scanning tunneling microscopy (STM). The STM results indicated that marked aggregation and desorption of surface-immobilized Ta@Si16 nanoclusters were not induced, even after thermal annealing at -500 K, whereas the local vertical and lateral positions of the Ta@Si16 nanoclusters with respect to neighboring adsorption sites in the C60 film were modified. This local positional transition occurred on C60 monolayer films weakly bonded (via van der Waals forces) to substrates such as highly oriented pyrolytic graphite (HOPG) but did not occur on C60 monolayer films covalently bonded to substrates such as Si(111)7 × 7. These results indicated that the heterodimer consisting of a Ta@Si16 nanocluster and a C60 molecule, Ta@Si16-C60, was formed as an initial product via covalent bonding, which inhibited wide-range surface migration of the Ta@Si16 nanoclusters but allowed them to locally change their positions via thermally activated precessional motion. In addition, the transition temperature of the local positional shift was found to decrease as the area density of the surface-immobilized Ta@Si16 nanoclusters increased, indicating that the barrier height of the precessional motion of the Ta@Si16-C60 heterodimer was decreased due to accumulation of the elastic strain energy generated in the C60 films.

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Experimental and theoretical studies of the structural and electronic properties of vanadium-benzene sandwich clusters and their anions: V_nBz_n^0/- (n = 1-5) and V_nBz_n-1^0/- (n = 2-5)

T. Masubuchi, T. Iwasa, A. Nakajima

Journal of Chemical Physics （American Institute of Physics） 141 （ 21 ） 214304 2014年12月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 00219606

One end open VnBzn- (n = 1-5; Bz = benzene) and both ends open VnBzn-1- (n = 2-5) vanadium-benzene cluster anions were studied using anion photoelectron spectroscopy and density functional calculations. The smaller (n ≤ 3) VnBzn and VnBzn-1 clusters and corresponding anions were found to have structural isomers, whereas full-sandwiched VnBzn+1 clusters preferred to form multiple-decker sandwich structures. Several isomeric V2Bz2 structures were identified theoretically and the anion photoelectron spectra of V2Bz20/- were explained well by the coexistence of two isomeric structures: (1) a V2-core structure sandwiched between benzene molecules and (2) an alternating sandwich structure with the spin state strongly dependent on the structure. The adiabatic electron affinity of both VnBzn and VnBzn-1 was found to increase with the cluster size at larger sizes (n = 4 or 5) and approaches to that of VnBzn+1. The evolution of the structural and electronic properties of VnBzm and VnBzm- (m = n and n - 1) with size is discussed in comparison with VnBzn+1 and VnBzn+1-.

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Formation of a superatom monolayer using gas-phase-synthesized Ta@Si₁₆ nanocluster ions

M. Nakaya, T. Iwasa, H. Tsunoyama, T. Eguchi, A. Nakajima

Nanoscale （Royal Society of Chemistry） 6 （ 24 ） 14702 - 14707 2014年10月

研究論文（学術雑誌）, 共著, 最終著者, 責任著者, 査読有り, ISSN 20403364

The controlled assembly of superatomic nanocluster ions synthesized in the gas phase is a key technology for constructing a novel series of functional nanomaterials. However, it is generally difficult to immobilize them onto a conductive surface while maintaining their original properties owing to undesirable modifications of their geometry and charge state. In this study, it has been shown that this difficulty can be overcome by controlling the donor-acceptor interaction between nanoclusters and surfaces. Cations of Ta-atom-encapsulated Si16 cage nanoclusters (Ta@Si16) behaving as rare-gas-like superatoms are synthesized in the gas phase and deposited on conductive surfaces terminated with acceptor-like C60 and donor-like α-sexithiophene (6T) molecules. Scanning tunneling microscopy and spectroscopy have demonstrated that Ta@Si16 cations can be densely immobilized onto C60-terminated surfaces while retaining their cage shape and positive charge, which is realized by creating binary charge transfer complexes (Ta@Si16+-C60-) on the surfaces. The Ta@Si16 nanoclusters exhibit excellent thermal stability on C60-teminated surfaces similar to those in the gas phase, whereas the nanoclusters destabilize at room temperature on 6T-terminated surfaces owing to the loss of electronic closure via a change in the charge state. This journal is

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論文 - 中嶋　敦