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岡安 悟; 針井 一哉*; 小畠 雅明; 吉井 賢資; 福田 竜生; 石田 真彦*; 家田 淳一; 齊藤 英治
Journal of Applied Physics, 128(8), p.083902_1 - 083902_7, 2020/08
The ion-irradiation tolerance of thermoelectric devices based on the spin Seebeck effect (SSE) was investigated by using 320 MeV gold ion (Au
) beams modeling cumulative damages due to fission products emitted from the surface of spent nuclear fuels. For this purpose, prototypical Pt/Y
Fe
O
/GdGaO SSE elements were irradiated with varying the dose level at room temperature and measured the SSE voltage of them. We confirmed that the thermoelectric and magnetic properties of the SSE elements are not affected by the ion-irradiation up to 
ions/cm
fluence and that the SSE signal is extinguished around 
ions/cm, in which the ion tracks almost fully cover the sample surface. We also performed the hard X-ray photoemission spectroscopy (HAXPES) measurements to understand the effects at the interface of Pt/YFeO. The HAXPES measurements suggest that the chemical reaction that diminishes the SSE signals is enhanced with the increase of the irradiation dose. The present study demonstrates that SSE-based devices are applicable to thermoelectric generation even in harsh environments for a long time period.
Fe
O小畠 雅明; 吉井 賢資; 福田 竜生; 川崎 郁斗; 岡根 哲夫; 山上 浩志; 矢板 毅; 針井 一哉; 家田 淳一; 岡安 悟; et al.
JPS Conference Proceedings (Internet), 30, p.011192_1 - 011192_6, 2020/03
スピンゼーベック効果を示す系として注目されているPt/YFeO(YIG)系に対し、放射光を用いた硬X線光電子分光(HAXPES)により表面及び界面の電子状態測定を行った。本系ではスピンゼーベック効果のほかに特異な性質を示すことが報告されている。例えば、外部磁場が存在しない状況でもホール効果を発現する。この起源として、YIG中のFe
イオンがPt膜に染み出し、磁性を持つ金属間化合物を生成している可能性が提案されている。そこでHAXPESの分析深さを利用し、界面近傍の鉄イオン等の電子状態を測定した。Ptの厚みが2nm, 5nm, 8nm, 10nmの試料を測定したところ、2nmと5nmの試料において鉄イオンの分析を行うことができた。Fe 1s光電子スペクトルからは、鉄イオンが3+のものと金属的な0価に近い2つの状態が存在することが判明し、上記の可能性を支持する結果が得られた。Pt 4fやO 1sスペクトルなども測定しており、詳しい結果は当日報告する。
Kim, J.*; 山中 暁*; 村山 一郎*; 加藤 孝典*; 坂本 友和*; 川崎 卓郎; 福田 竜生; 関野 徹*; 中山 忠親*; 武田 雅敏*; et al.
Sustainable Energy & Fuels (Internet), 4(3), p.1143 - 1149, 2020/03
被引用回数：1 パーセンタイル：100(Chemistry, Physical)Waste heat is a potentially exploitable energy source but remains a problem awaiting a solution. To explore solutions for automobile applications, we investigate pyroelectric power generation from the temperature variation of exhaust gas using a novel electro-thermodynamic cycle. Niobium-doped lead zirconate titanate stannate (PNZST) ceramics were applied as pyroelectric materials, and their structural characteristics were investigated. In the driving cycle assessments (JC-08) using real exhaust gas, the maximum power generated was identified as 143.9 mW cm
(777.3 J L
per 1 cycle) over a temperature range of 150-220 
C and an electric field of 13 kV cm-1. The net mean generating power of the total driving cycle was 40.8 mW cm, which is the most enhanced result in our power generating systems to date and 314 times greater than our first report. Materials with sharp transition behaviors with the temperature and electric field are worthy of study with regard to pyroelectric energy harvesting materials, and their corresponding crystal and domain structures were investigated to optimize performance.
村井 直樹; 福田 竜生; 中島 正道*; 河村 光晶*; 石川 大介*; 田島 節子*; Baron, A. Q. R.*
Physical Review B, 101(3), p.035126_1 - 035126_6, 2020/01
被引用回数：0 パーセンタイル：100(Materials Science, Multidisciplinary)非弾性X線散乱を用いたFeSe超伝導体のフォノン研究について報告する。実験的に決定したフォノン分散と非磁性相の密度汎関数理論(DFT)とを比較を行うと、両所の間には顕著な不一致が見られた。FeSeは磁気秩序を示さないにもかかわらず、スピン偏極DFTを用いることによって初めて実験結果は再現される。この解析は、強いスピン揺らぎを内在した常時性状態における近似を与える。
Fe
平賀 晴弘*; 矢野 真一郎*; 福田 竜生
Journal of Magnetism and Magnetic Materials, 469, p.629 - 632, 2019/01
被引用回数：0 パーセンタイル：100(Materials Science, Multidisciplinary)Low-energy magnetic excitation of spin-density wave (SDW) in a single crystal of CrFe was measured using cold neutron triple-axis spectroscopy. Because of the unchanged incommensurability and the constant line width in 2.5 
6 meV, the magnetic excitation could not be explained with a conventional dispersion of 
. In this paper, we conjectured the presence of standing waves, which would be excited in local spin matrices. The effectively vertical dispersion was attributed to the longitudinal spin fluctuation in the spin matrices. A series of low-energy magnetic excitations in Cr alloys could be understood with the coexistence of the standing waves and progressive waves such as spin waves.
Kim, J.*; 山中 暁*; 中島 啓*; 加藤 孝典*; Kim, Y.*; 福田 竜生; 吉井 賢資; 西畑 保雄; 馬場 将亮*; 武田 雅敏*; et al.
Advanced Sustainable Systems (Internet), 2(11), p.1800067_1 - 1800067_8, 2018/11
被引用回数：1 パーセンタイル：82.39(Green & Sustainable Science & Technology)An innovative electrothermodynamic cycle (pyroelectric effect with an external electric field) was recently presented, which is based on temporal temperature variations in wasted heat from engine exhaust gas. In this paper, for further improvement, a generating mechanism of the cycle is investigated using in-operando time-resolved synchrotron X-ray diffraction with generating assessment. The polarizations of the sample are gained from both crystal/domain changes and simultaneous electrical measurements. Three types of materials are prepared: soft and hard types of lead zirconate titanate (PZT) and lead magnesium niobate-lead titanate (PMN-PT). Among them, PMN-PT has the highest generating power. When an external electric field is applied, the PMN-PT exhibits only 180
domain rotations, whereas PZTs exhibit both 90 and 180 rotations. A strong driving force for 180 rotation depresses rotations in other angles and increases polarization changes. The results show that the material development, which has only 180 switching domains, has potential for use in the establishment of a high-efficiency waste heat recovery system.
茂呂 拓哉*; Kim, J.*; 山中 暁*; 村山 一郎*; 加藤 孝典*; 中山 忠親*; 武田 雅敏*; 山田 昇*; 西畑 保雄; 福田 竜生; et al.
Journal of Alloys and Compounds, 768, p.22 - 27, 2018/11
被引用回数：6 パーセンタイル：33.7(Chemistry, Physical)Relaxor-based ternary Pb(In
Nb)O-Pb(Mg
Nb
)O-PbTiO (PIN-PMN-PT) ceramics near a morphotropic phase boundary were grown, and their electrical properties at various temperatures were investigated in the electrothermodynamic cycle for the future environment-friendly automotive applications. Structural disordering, depending on the PIN content, influenced the diffuse phase transition between the tetragonal and cubic structures and contributed to the power-generating behavior. The net power-generating energies (P
) were 2.43-3.01 mW/cm
at temperatures above 200C and were maintained at above 1 mW/cm over a temperature range of approximately 100 degrees. Therefore, the PIN-PMN-PT system has a possibility of a wider usage temperature range, the disordering of the perovskite crystal structure can be controlled, and it will be a candidate for the application of pyroelectric energy conversion system.
-site randomness on the antiferroelectric/relaxor nature of the ground state; Diffuse and inelastic X-ray scattering study of Pb(InNb)O大和田 謙二*; 塚田 慎也*; 福田 竜生; 筒井 智嗣*; Baron, A. Q. R.*; 水木 純一郎*; 大和 英弘*; 安田 直彦*; 寺内 暉*
Physical Review B, 98(5), p.054106_1 - 054106_10, 2018/08
被引用回数：0 パーセンタイル：100(Materials Science, Multidisciplinary)The effect of -site randomness on the antiferroelectric/relaxor nature of the ground state was investigated by studying diffuse and inelastic X-ray scattering from ordered and disordered Pb(InNb)O (O- and D-PIN) single crystals. The diffuse scattering measurement of O-PIN (antiferroelectric at 
) shows the existence of ferroelectrically interactive local polarization above 
. Inelastic X-ray scattering shows that the transverse-acoustic (TA) and transverse-optic (TO) modes are dominant at 
800 K, while the central peak (CP) and TA modes are coupled and majorly contribute to the critical behavior of the diffuse scattering at . Upon these results, the -site randomness is discussed in terms of suppressing the antiferroelectric instability and enhancing the polarization fluctuation.
by tuning nematicity and magnetism in FeSe
S
superconductors松浦 康平*; 水上 雄太*; 新井 佑基*; 杉村 優一*; 前島 尚行*; 町田 晃彦*; 綿貫 徹*; 福田 竜生; 矢島 健*; 広井 善二*; et al.
Nature Communications (Internet), 8, p.1143_1 - 1143_6, 2017/10
被引用回数：33 パーセンタイル：10.25(Multidisciplinary Sciences)A fundamental issue concerning iron-based superconductivity is the roles of electronic nematicity and magnetism in realising high transition temperature (). To address this issue, FeSe is a key material, as it exhibits a unique pressure phase diagram involving nonmagnetic nematic and pressure-induced antiferromagnetic ordered phases. However, as these two phases in FeSe have considerable overlap, how each order affects superconductivity remains perplexing. Here we construct the three-dimensional electronic phase diagram, temperature (
) against pressure (
) and iso-valent S-substitution (
), for FeSeS. By simultaneously tuning chemical and physical pressures, against which the chalcogen height shows a contrasting variation, we achieve a complete separation of nematic and antiferromagnetic phases. In between, an extended nonmagnetic tetragonal phase emerges, where shows a striking enhancement. The completed phase diagram uncovers that high- superconductivity lies near both ends of the dome-shaped antiferromagnetic phase, whereas remainslow near the nematic critical point.
Kim, J.*; 山中 暁*; 中島 啓*; 加藤 孝典*; Kim, Y.*; 福田 竜生; 吉井 賢資; 西畑 保雄; 馬場 将亮*; 武田 雅敏*; et al.
Ferroelectrics, 512(1), p.92 - 99, 2017/08
被引用回数：6 パーセンタイル：49.21(Materials Science, Multidisciplinary)We have been investigating a novel electrothermodynamic cycle based on temporal temperature variations using the pyroelectric effect to utilize the waste heat as renewable energy. An improved generating performance with relaxer ferroelectric ceramics was achieved using 75Pb(MgNb)O-25PbTiO which is well known for the high dielectric and pyroelectric properties. The potential was evaluated by using the hysteresis loops and generating properties are analyzed both in laboratory and engine dynamometer. Results showed 0.48 mW/cm in engine dynamometer assessment, which is 3 times larger than the previous study using Pb(Zr,Ti)O.
山中 暁*; Kim, J.*; 中島 啓*; 加藤 孝典*; Kim, Y.*; 福田 竜生; 吉井 賢資; 西畑 保雄; 馬場 将亮*; 山田 昇*; et al.
Advanced Sustainable Systems (Internet), 1(3-4), p.1600020_1 - 1600020_6, 2017/04
我々がプロジェクトとして取り組んできている自動車排ガスを用いた温度変化発電に関し、変換素子の材料選定等に重要となる性能指数について、素子の物理量の温度変化の測定を行うことで調べた。測定結果を用い、これまで提案されていたいくつかの性能指数の温度変化を詳しく調べて比較することで、
と呼ばれる指数が最も発電量との相関が高いことを示した。この指数には唯一誘電正接(
)が含まれており、誘電体内での電気エネルギー損失が重要であることを示唆する結果となっている。
-XRD with synchrotron radiation甕 聡子*; 向井 広樹*; 綿貫 徹; 大和田 謙二; 福田 竜生; 町田 晃彦; 倉又 千咲*; 菊池 亮佑*; 矢板 毅; 小暮 敏博*
Journal of Mineralogical and Petrological Sciences, 111(5), p.305 - 312, 2016/10
被引用回数：11 パーセンタイル：36.63(Mineralogy)福島土壌粒子から放射能をもつ粒子を選び出し、50ミクロン程度の粒子一粒ごとに鉱物種の同定を放射光X線回折によって行った。板状の風化雲母の粒については様々な度合のバーミキュライト化されたものが見出された。ごく微粒子の塊である土壌粒子からは、長石や石英に加えてスメクタイト状の粘土鉱物が検出された。
As using high-resolution inelastic X-ray scattering村井 直樹*; 福田 竜生; 小林 達也*; 中島 正道*; 内山 裕士*; 石川 大介*; 筒井 智嗣*; 中村 博樹; 町田 昌彦; 宮坂 茂樹*; et al.
Physical Review B, 93(2), p.020301_1 - 020301_5, 2016/01
被引用回数：6 パーセンタイル：55.84(Materials Science, Multidisciplinary)Phonon spectra of detwinned SrFeAs crystals, as measured by inelastic X-ray scattering, show clear anisotropyaccompanying the magnetostructural transition at 200 K. We model the mode splitting using magnetic DFT calculations, including a phenomenological reduction in force-constant anisotropy that can be attributed to magnetic fluctuations. This serves as a starting point for a general model of phonons in this material applicable to both the antiferromagnetically ordered phase and the paramagnetic phase. Using this model, the measured splitting in the magnetic phase below T
, and the measured phonon linewidth, we set a lower bound on the mean magnetic fluctuation frequency above T at 210 K.
伊藤 晋一*; 横尾 哲也*; 益田 隆嗣*; 吉澤 英樹*; 左右田 稔*; 池田 陽一*; 井深 壮史*; 川名 大地*; 佐藤 卓*; 南部 雄亮*; et al.
JPS Conference Proceedings (Internet), 8, p.034001_1 - 034001_6, 2015/09
Since the installation of the High Resolution Chopper Spectrometer, HRC, experiments using the HRC are being conducted to observe the dynamics in wide range of physics. Scientific results during the period since the initial construction are summarized.
Kim, Y.*; Kim, J.*; 山中 暁*; 中島 啓*; 小川 孝*; 芹沢 毅*; 田中 裕久*; 馬場 将亮*; 福田 竜生; 吉井 賢資; et al.
Advanced Energy Materials, 5(13), p.1401942_1 - 1401942_6, 2015/07
空中に廃棄されている自動車排ガスの廃熱の再利用は、現在社会のエネルギー問題の重要な位置を占めるが、その一つとして強誘電体(焦電体)の誘電・焦電効果を応用したエネルギー回生技術の研究が進められている。焦電体を自動車排ガス中に設置するとともに、エンジン運転に伴う熱振動に同期した電場を外部から加えることで、回生エネルギーは大幅に上昇する。本研究ではこの時用いる取り出し電気回路の改良を行うとともに、典型的な焦電体PbZrTiO(PZT)を用いて実際に有効活用できる回生エネルギーが非常に小さいながらもプラスであることを初めて確認した。また回生運転と同時測定した時分割X線回折により、焦電体の結晶構造の変化やドメイン比といったミクロな機構に関する知見を得るとともに、さらに実機エンジンを用いた試験でも実際に有効活用できる回生エネルギーの取得を確認できた。
福田 竜生; Baron, A. Q. R.*; 内山 裕士*; 中村 博樹; 石角 元志*; 町田 昌彦; 社本 真一
SPring-8/SACLA利用研究成果集(Research Report) (インターネット), 3(2), p.290 - 293, 2015/07
Using inelastic X-ray scattering (IXS), we investigated acoustic phonons of PrFeAsO precisely in order to select between two different models based on first principles calculations: the in-plane soft and clipped model. These models predict slightly different phonon intensities, and, in particular, different contamination of the longitudinal acoustic (LA) phonon spectra by transverse acoustic (TA) phonon modes. We were able to reduce the contamination with improved 
resolution, but the data quality was not sufficient to clearly decide between our models. Based on 
dependence there appears to be slightly better agreement with the in-plane soft model at room temperature.
Si利根川 翔*; 笠原 成*; 福田 竜生; 杉本 邦久*; 安田 伸広*; 鶴原 悠悟*; 渡邊 大樹*; 水上 雄太*; 芳賀 芳範; 松田 達磨*; et al.
Nature Communications (Internet), 5, p.4188_1 - 4188_7, 2014/06
被引用回数：45 パーセンタイル：8.09(Multidisciplinary Sciences)We report on the observation of lattice symmetry breaking from the fourfold to twofold structure by high-resolution synchrotron X-ray diffraction measurements at zero field. Small orthorhombic symmetry-breaking distortion sets in at the transition temperature with a jump, uncovering the weakly first-order nature of the hidden-order transition. This distortion is observed only in ultra pure samples, implying a highly unusual coupling nature between the electronic pneumaticity and underlying lattice.
using resonant X-ray emission spectroscopy at the Ba-L and Ti K absorption edges吉井 賢資; 米田 安宏; Jarrige, I.*; 福田 竜生; 西畑 保雄; 鈴木 知史; 伊藤 嘉昭*; 寺嶋 孝仁*; 吉門 新三*; 福島 整*
Journal of Physics and Chemistry of Solids, 75(3), p.339 - 343, 2014/03
被引用回数：5 パーセンタイル：68.96(Chemistry, Multidisciplinary)強誘電体BaTiO3について、共鳴X線発光(RXES)及び部分蛍光法を用いたX線吸収分光(PFY-XAS)により電子状態を分析した。実験はSPring8の原子力機構ビームラインBL14B1と物質・材料研究機構ビームラインBL15XUで行った。Ba L吸収端でのPFY-XASスペクトルは、過去の文献とは異なり、キュリー点上下で変化しなかった。これは、Ba
イオンの位置はキュリー点で変位しないか変位が小さいことを示唆する。また、Ti K吸収端でのRXESスペクトルからは、発光ピークのエネルギーは入射光エネルギーによらずほぼ一定であった。この結果は、Ti 3d軌道が非局在的な性質を持っており、それによりTiイオンが変位して電気双極子の生成して強誘電体となるという、理論計算から提案された機構を支持することが分かった。
SrCuO
Park, S. R.*; 福田 竜生; Hamann, A.*; Lamago, D*; Pintschovius, L.*; 藤田 全基*; 山田 和芳*; Reznik, D.*
Physical Review B, 89(2), p.020506_1 - 020506_5, 2014/01
被引用回数：18 パーセンタイル：30.71(Materials Science, Multidisciplinary)In superconducting copper oxides, some Cu-O bond-stretching phonons around 70 meV show anomalous giant softening and broadening of electronic origin, and electronic dispersions have large renormalization kinks near the same energy. These observations suggest that phonon broadening originates from quasiparticle excitations across the Fermi surface and the electronic dispersion kinks originate from coupling to anomalous phonons. We measured the phonon anomaly in underdoped ( = 0.05) and overdoped ( = 0.20 and 0.25) LaSrCuO by inelastic neutron and X-ray scattering with high resolution. Combining these and previously published data, we found that doping dependence of the magnitude of the giant phonon anomaly is very different from that of the ARPES kink, i.e., the two phenomena are not connected. We show that these results provide indirect evidence that the phonon anomaly originates from novel collective charge excitations as opposed to interactions with electron-hole pairs. Their amplitude follows the superconducting dome so these charge modes may be important for superconductivity.
土居 篤典*; 藤岡 淳*; 福田 竜生; 筒井 智嗣*; 奥山 大輔*; 田口 康二郎*; 有馬 孝尚*; Baron, A. Q. R.*; 十倉 好紀*
Physical Review B, 90(8), p.081109_1 - 081109_4, 2014/01
被引用回数：15 パーセンタイル：34.63(Materials Science, Multidisciplinary)The phonon dynamics of spin-state crossover for perovskite LaCoO was investigated using infrared and inelastic X-ray spectroscopy. We observed that the Co-O bond stretching phonons couples to the thermally excited spin-state. The momentum dispersion of the optical mode is anomalously dispersionless (less than 3 meV), and this supports the spin-state disproportionation scenario. The steep enhancement of spin-state fluctuation compared to the charge gap suggests the density dependent spin state disproportionation; a simple low spin (LS)/high spin (HS)- or LS/intermediate spin (IS)-state disproportionation is realized at the initial stage with dilute HS- (or IS-) state density, while the complex spin-state disproportionation involving all of the LS-, IS- and HS-state is formed when the density of HS- (or IS-) state is enhanced.
