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A valence analytical end point complete a the complete aught provides a altered case for the abstraction of a breakthrough adaptation of the able body aberration at the Widom band in the supercritical fluids. Although atypical allegation and alternate dynamics are adapted apparently to adapt the cyberbanking anatomy significantly, breaking bottomward the accepted quasi-particle picture, this has never been accepted experimentally to date. We accommodate the aboriginal empiric affirmation that the adjacency to breakthrough valence criticality leads to a bright breakdown of Fermi aqueous behavior. Our abundant abstraction of the alloyed valence admixture α-YbAlB4 reveals that a baby actinic barter induces a aciculate valence crossover, accompanied by a arresting non–Fermi aqueous behavior characterized by a aberrant able accumulation and abnormal T/B ascent in the magnetization.

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The supercritical aqueous accompaniment a the liquid-gas analytical point has been a aloft accountable in abridged bulk physics for its abstruse appliance and for its accurate acceptation (1, 2). One of the important goals is to accompany bottomward the analytical temperature and pressure, which are commonly abundant college than ambient conditions. By contrast, in the cyberbanking versions of these analytical points, there are some cases area the temperature calibration may be bargain decidedly bottomward to near-zero temperatures so that one may beam breakthrough analytical phenomena in the agnate “supercritical” states. Aberrant metal behaviors accept been apparent in activated electron systems as a aftereffect of adjacency to a breakthrough analytical end point of a first-order alteration such as a metamagnetic alteration and a Mott alteration (3–5). Another applicant for the body alternation that may apparently drive atypical breakthrough criticality (QC) is valence alteration (6–9). A its associated breakthrough analytical end point, atypical fluctuations of valence (which includes charge, spin, and alternate degrees of freedom) and its coupling with thermodynamic quantities are accepted to advance to a able abuse of Fermi aqueous (FL) behavior. Similar to the Widom band in the supercritical aqueous (10, 11), fluctuations abide able a the valence crossover line. Although a valence crossover at low temperatures has been appear in a array of abstracts (12–19), the associated QC has not been accepted to date.

For the abstraction of QC, abounding prototypal abstracts accept been begin amid heavy-fermion 4f intermetallic compounds, because fine-tuning of adapted activity scales is accessible appliance high-purity crystals (20, 21). In this chic of materials, QC has been admired to appear from a antagonism amid bounded moment allure and advice electron screening of the bounded moments (the Kondo effect), as originally discussed by Doniach (22). Thus, the studies accept focused on the systems with an about basic valence that stabilizes the bounded moments.

Breaking this pattern, β-YbAlB4 is the aboriginal actual that exhibits arresting QC admitting its able alloyed valency (23–25). An ultrapure audible bright of the actual exhibits atypical behavior afterwards tuning, namely, beneath aught acreage and ambient pressure, such as a aberrant access of the susceptibility ~T−1/2 and aberrant T3/2 assurance of the resistivity, both of which are acutely acute to alien acreage B. T/B ascent of the magnetization empiric over four decades of T/B pinpoints the analytical acreage to 0 ± 0.1 mT and reveals an anarchistic anatomy of the QC. Moreover, a contempo burden abstraction begin that this QC is afar from an antiferromagnetic (AF) actualization that appears beneath burden and extends up to Pc ~ 0.4 GPa, advertence the actuality of a aberrant metal actualization (26).

β-YbAlB4 has a locally isostructural polymorph α-YbAlB4 (27). At aerial temperatures, the two phases allotment about the aforementioned concrete backdrop (24, 28). For example, both accept alloyed valence beneath than 2.8 (25) and adherence temperatures of ~200 to 250 K (23, 28). Moreover, admitting the alloyed valency, both actualization an Yb ion bounded moment behavior accepted for a Kondo filigree (24, 28). In the arena state, however, they accept cogent differences; in adverse to the QC behavior in β-YbAlB4, α-YbAlB4 forms a abundant FL at low temperatures with a specific calefaction accessory of γ ~ 130 mJ/mol K2. On the added hand, a contempo abstraction appear that several percentages of Fe barter at the Al armpit abet Yb antiferromagnetism (29). Here, we actualization on the abject of our complete abstraction that the antiferromagnetism appears through a first-order actualization alteration beyond a actual baby bulk of Fe barter of xc= 1.4% in α-YbAl1−xFexB4. We begin a aciculate valence crossover at the analytical absorption xc accompanied by anarchistic QC, which cannot be explained by the accepted approach based on spin-density beachcomber (SDW) fluctuations (30, 31) but, instead, can be accounted for by the valence QC.

We aboriginal present a actualization diagram accustomed on the abject of our magnetothermal and carriage abstracts with a ambit artifice of the resistivity backer α authentic by ρ = ρ0 A′Tα in Fig. 1A. Upon doping, antiferromagnetism due to Yb 4f moments appears rather aback at x = 1.5% with the Néel temperature TN of 1.2 K, admitting it is suppressed beneath 25 mK at xc = 1.4%. The alluring susceptibility shows history assurance amid the zero-field–cooled (ZFC) and field-cooled (FC) sequences beneath TN due to the apostate of the alluring moments with the ad-lib moment forth the c arbor (Fig. 2A) (29). This AF acclimation additionally exhibits a bright aberration in the temperature assurance of the specific calefaction (Fig. 2B). Note that Fe itself does not backpack any alluring moment, as axiomatic from the baby diamagnetism begin in the Lu analog, α-LuAl1−xFexB4 (Fig. 2A and fig. S3). Arresting non-FL (NFL) behavior with α ~ 1.6 was empiric about xc = 1.4% (Fig. 1A). Added backdrop of the NFL will be discussed afterwards in detail.

(A) Actualization diagram of temperature (vertical axis) against Fe absorption x (horizontal axis) for α-YbAl1−xFexB4 with the ambit artifice map of the ability law backer α = ∂ln(ρa(T) − ρa(0))/∂lnT of the a arbor resistivity. TN denotes the AF Néel point bent by magnetization (closed circles), specific calefaction (closed squares), and resistivity (closed triangles). The burst vertical band indicates the analytical absorption xc = 1.4% for the valence crossover and the first-order AF transition. (B) Doping assurance of the Yb valence estimated from adamantine x-ray photoemission spectroscopy (HAXPES) at 20 K (left axis) and doping assurance of the assemblage corpuscle aggregate abstinent by crumb x-ray diffraction at 273, 175, and 17 K (right axis). (C) HAXPES spectra of Yb 3d5/2 amount akin in YbAl1−xFexB4 with x = 1.3 and 4.2% (top) and the aberration of these spectra from x = 1.3 to 4.2% (bottom). (D) Schematic actualization diagram for the valence QC mechanism, which is apparent as a action of temperature T, alluring acreage B, and the actinic burden P for an Yb-based arrangement (8). Valence crossover (blue) and the AF adjustment (green) are both shown. Valence crossover (magenta) and first-order valence alteration (FOVT) (red) apparent are about fatigued beneath 0 K. Valence crossover apparent (blue) evolves into a actualization aals due to a basic FOVT in the abrogating temperature. The analytical end band at the bound amid FOVT and the crossover apparent touches 0 K, basic a breakthrough analytical point (QCP). a.u. approximate units.

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(A) T assurance of the c arbor basic of the DC susceptibility M/B for α-YbAl1−xFexB4 with assorted x and the nonmagnetic analog α-LuAl1−xFexB4. Both zero-field-cooling (ZFC) (open syms) and field-cooling (FC) (closed syms) sequences were used. (B) Temperature assurance of the 4f cyberbanking accession to the specific calefaction disconnected by T, C4f/T, which is acquired afterwards adding the nonmagnetic accession estimated appliance the specific calefaction of α-LuAlB4 (see the Supplementary Abstracts for details).

Strikingly, a aciculate valence crossover was empiric at xc by adamantine x-ray photoemission spectroscopy (HAXPES) at 20 K, area the valence exhibits a abrupt access by 0.03 (corresponding to a 3% access of 4f aperture density) (Fig. 1B). Typical Yb 3d5/2 amount akin spectra for x = 1.3% and x = 4.2% are apparent in Fig. 1C (top), which exhibits a bright break amid the peaks associated with Yb2 and Yb3 states. Here, the valence is estimated appliance the arrangement of the areas for these two peaks (see the Supplementary Abstracts for details). As apparent in Fig. 1C (bottom), the aberration spectrum acquired by adding the x = 1.3% spectrum from the 4.2% spectrum shows that the Yb3 (Yb2 ) basic grows (diminishes) by accretion x. Correspondingly, the able moment μeff estimated from the low T susceptibility beneath 15 K shows a baby access beyond xc (fig. S4). Note that the empiric 3% change in 4f aperture absorption is ample and amounts to added than ~20% of those begin at the first-order valence alteration (FOVT) in the prototypal systems such as Ce and YbInCu4 [10 to 15% of 4f electrons/holes (32–34)].

This abrupt and connected valence change may appear either from a aciculate crossover or from a actualization break due to a anemic first-order alteration at xc. In the closing case, aggregate fractions of the phase-separated regions with audible assemblage corpuscle ambit may be accepted to advance beyond xc, which is absurd as we altercate here. Aboriginal of all, our crumb x-ray diffraction abstraction at 17 K finds no adorning of x-ray diffraction spectra but, instead, a connected aggregate abbreviating agnate to the valence change (figs. S5A and S6). Low-temperature manual electron microscopy detects no agreement change in the filigree anatomy beyond xc (figs. S7 and S8). In addition, the assemblage corpuscle aggregate is begin to be proportional to the valence over the complete ambit including the analytical arena if we decrease the filigree allotment due to actinic doping (fig. S5B). All these observations announce that there is no actualization separation. This should additionally be the case at temperatures far beneath 17 K because no signature of a alluring adjustment induced by actualization break has been detected bottomward to the everyman temperature of our measurements, that is, 25 mK. The associated assemblage corpuscle aggregate change was begin alike at animated temperatures of 175 and 273 K beyond xc (Fig. 1B). This shows that the activity calibration of the valence crossover is abundant college than the calibration for the antiferromagnetism, advertence the ascendant role of the valence fluctuations rather than circuit fluctuations on the QC empiric at xc.

If the valence fluctuations drive the QC, again the associated schematic actualization diagram should attending like the one accustomed in Fig. 1D (8, 14, 35). Namely, the FOVT is suppressed bottomward to aught or alike abrogating temperature in the actualization diagram. At bound temperatures, the arrangement is controlled from a “mixed-valent regime” (MV) to a “Kondo regime” through a valence crossover apparent by affability either actinic burden P or corpuscle aggregate (−ΔV > 0). This is due to the actuality that the ambit is abate for the alluring Yb3 ion than for the nonmagnetic Yb2 . Back the arrangement moves into the Kondo regime, a alluring adjustment may appear as a first-order alteration as a action of P. At aerial temperatures, the alluring amount of abandon finer decreases the entropic chargeless energy, appropriately stabilizing the Kondo administration rather than the MV, which defines the abruptness of the valence crossover surface.

To added appraise the agent of the QC, we altercate the NFL behaviors begin at xc in detail. Figure 2 represents the alluring susceptibility M/B = χ and the 4f cyberbanking accession to the specific calefaction disconnected by T (C4f/T), for samples with altered x, respectively. Here, C4f is acquired afterwards adding the nonmagnetic accession and nuclear Schottky accession (see the Supplementary Abstracts for details). As apparent in the figures, both χ and C4f/T are best aberrant at xc = 1.4%. The T assurance of C4f/T shows a logarithmic access on cooling. Note that there is a accessible crossover from the logarithmic to a ability law behavior with a apportioned backer β ~ 0.5, namely, C4f/T ~ T−β beneath about 100 mK as accepted from the Maxwell affiliation and the T/B ascent begin for the magnetization as apparent below. However, the accession of the ample nuclear accession makes it adamantine to actuate whether such a crossover exists (see the Supplementary Abstracts for details). Notably, in either case, our after-effects announce the alteration of quasi-particle accumulation at xc.

Significantly, the acreage change of M/B in anemic fields beneath 50 mT follows the T/B scaling, the aforementioned as that begin in β-YbAlB4 (24). As apparent in Fig. 3A, the analytical acreage assurance of M/B can be burst assimilate a audible ascent action φ(T/B) at T < 2 K; that is(1)(2)with α = 3/2. This indicates that χ(T) diverges at B → 0 with a T−1/2 assurance and forth that the analytical acreage Bc associated with the QC is aing to zero. Note that if Bc is finite, again the ascent should be with account to T/(B − Bc) rather than T/B. A analytical change from a zero-field NFL to a field-induced FL behavior at xc was additionally accepted by the T assurance of the resistivity. The ambit artifice of the ability law backer α indicates an aberrant ability law assurance at zero-field (T beeline at 5 K > T > 1 K and T1.6 able-bodied beneath 1 K), which crossovers to the FL with α ~ 2 in a alluring acreage (Fig. 3B, see additionally fig. S10, A and C).

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(A) Ascent empiric for the magnetization M in the T < 2 K and B < 50 mT. The abstracts can be adapted to the ascent action φ(t) = Λt(A t2)−n with t = T/B, a anatomy called to amuse the adapted attached behaviors in the FL administration (24). The solid band is the adapted abstracts for β-YbAlB4 (24). The inset is the T assurance of the DC susceptibility M/B for xc in α-YbAl1−xFexB4 beneath assorted fields (solid line). Abstracts at x = 4.2% beneath B = 3.5 T are additionally apparent (broken line). (B) Ambit artifice of the ability law backer α = ∂ln(ρ(T) − ρ(0))/∂lnT of the a arbor resistivity ρa(T) in the B-T actualization diagram of α-YbAl1−xFexB4 at xc.

A abrupt actualization of TN > 1.2 K with alone a actual baby change in Fe absorption from xc = 1.4% to x = 1.5% indicates the first-order actualization of the AF transition, which suggests the accessory role of the allure and associated circuit fluctuations for the QC begin at xc. To added authenticate this, in the following, we analyze the zero-field QC at xc with a field-induced AF QC for the samples at x = 4.2%. In general, appliance of the alluring acreage stabilizes the Kondo administration with college valence. As apparent schematically in Fig. 1D, the valence crossover apparent will move to the abate x, that is, the abate P beneath alluring field. Therefore, for the sample able-bodied central the AF actualization at zero-field, the field-induced AF QCP will be afar from the valence instability. This allows us to abstraction the QC associated alone with AF appliance the sample at x = 4.2%.

Figure 4A provides the actualization diagram for x = 4.2%, bent by magnetothermal and carriage measurements, accumulated with a ambit artifice of α, assuming that TN vanishes at the alteration acreage BN ~ 3.5 T. A fan-shaped NFL arena with α ~ 1.6 is acutely apparent at BN, which systematically crossovers to FL (α = 2) at lower and college fields (see additionally fig. S10B). In aciculate adverse to the zero-field QC begin at xc, the alluring susceptibility does not actualization a aberrant behavior against the field-induced QCP at BN. As apparent in Fig. 4B, the bifurcation amid FC and ZFC abstracts disappears aloft BN = 3.5 T. Correspondingly, the magnetization disconnected by the acreage M/B at 80 mK peaks at BN (Fig. 4D), and dM/dB forms a ample aiguille at 2.9 T < BN (Fig. 4C). This is in aciculate adverse to the abundant bluff and beyond aiguille in dM/dB accepted at 80 mK by ascent Eq. 1 at BN (broken band in Fig. 4C). The ascertainment discriminates the anarchistic anatomy of the zero-field QC at xc from the one at the field-induced AF instability. The T1.6 assurance of the resistivity and the nondivergent temperature dependences of the susceptibility (broken band in the inset of Fig. 3A) are all connected with the behaviors predicted for an AF SDW alternation (30, 31). At the aforementioned time, this allegory artlessly leads us to achieve that the zero-field QC accompanied by the aciculate valence crossover at xc is induced not by the AF alternation but by the adjacency to a breakthrough valence instability.

(A) Field-temperature actualization diagram of the antiferromagnetism. Ambit artifice of the ability law backer α = ∂ln(ρ(T) − ρ(0))/∂lnT of the a arbor resistivity ρa(T) in the B-T actualization diagram of α-YbAl1−xFexB4 (x = 4.2%). The Néel credibility bent by the specific calefaction C (circles), magnetization M (diamonds), and the resistivity ρ (squares) abstracts are shown. (B) T assurance of the DC susceptibility M/B beneath assorted fields aing to the alteration acreage BN. Both ZFC (open syms) and FC (closed syms) sequences were used. (C) Magnetization ambit abstinent at T = 80 mK (right axis) and its acreage acquired ∂M/∂B (left axis). The burst band is affected from ascent Eq. 1 appliance the ambit bent for the applicable to the abstracts of α-YbAl1−xFexB4 at xc = 1.4%. Note that, here, the analytical acreage Bc is confused from aught acreage to BN ~ 3.5 T. (D) Magnetization disconnected by the alluring acreage M/B at T = 80 mK as a action of B. The red arrow indicates BN = 3.5 T, area M/B starts to be suppressed with abbreviating B. Consistently, the DC susceptibility exhibits bifurcation amid FC and ZFC beneath BN, as apparent in (B).

Theoretically, breakthrough valence criticality has been advised by assorted authors (6–9). In particular, the mode-coupling approach predicts the exact behaviors experimentally empiric beneath aught acreage at xc, that is, T−1/2 alteration of the alluring susceptibility (and additionally T/B scaling) and the crossover from T beeline to T3/2 assurance of the resistivity as T → 0 (8, 36). These NFL backdrop appear from the alteration of the cyberbanking able accumulation and the bounded actualization of the valence fluctuations (8). In addition, the accessory alluring alternation at a valence crossover is apparently accepted to aftereffect in a first-order alluring transition, connected with our beginning observations (35). On the added hand, cogent affinity to the QC in authentic β-YbAlB4 indicates an another possibility, area a topological actualization alteration of the Fermi apparent occurs in a topologically nontrivial amphitheater metal, assuming alteration in χ with T−1/2 assurance and T/B ascent (37). A decidedly absorbing achievability is that a topological amphitheater metal could accommodate a accustomed way for valence fluctuations to become breakthrough analytical as the f akin alcove at the Fermi energy. Note that both scenarios crave a fine-tuning of the arrangement to the QCP at B = 0 to amuse the T/B scaling. Another absorbing achievability would be the actualization of a second-order alteration basic a QCP back the FOVT hits the complete aught from the abrogating temperature side. Finally, our ascertainment of breakthrough valence criticality provides a specific archetype of how breakthrough fluctuations may affect a supercritical aqueous accompaniment by suppressing the analytical temperature to near-zero temperatures.

Single crystals of α-YbAl1−xFexB4 (x ≤ 4.2%) were developed by the aluminum self-flux adjustment (27, 29). The Fe absorption was estimated by inductively accompanying claret spectroscopy with resolution of 0.01%. Crumb x-ray diffraction abstracts were agitated out from allowance temperature bottomward to 16 K appliance a bartering x-ray diffraction arrangement (RINT2100, Rigaku) in the bend ambit amid 10° ≤ 2θ ≤ 90°. α-YbAl1−xFexB4 and a silicon accepted (standard advertence actual 640c, National Institute of Standards and Technology) were abstinent accompanying to annihilate the altitude absurdity due to the optical agreement of the x-ray system. We analyzed diffraction patterns to actuate the bright anatomy and filigree connected appliance the Rietveld assay affairs PDXL (Rigaku) and begin no birthmark actualization or structural alteration from the authentic system. Electron diffraction patterns for x = 0 and x = 4.2 % at 300 and 13 K were acquired appliance a manual electron microscope (JEM-2010F, JEOL Ltd.) operating at a voltage of 200 kV.

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We abstinent the electrical resistivity, DC magnetization, and specific calefaction of α-YbAl1−xFexB4. The electrical resistivity was abstinent by the accepted four-probe adjustment appliance a capricious temperature admit aloft 2 K and by appliance a concoction refrigerator aloft 50 mK. The magnetization M aloft 2 K was abstinent appliance a bartering SQUID magnetometer, Breakthrough Design Alluring Property Altitude Arrangement in the acreage alignment from 0.02 to 1 T. At low temperatures, the magnetization beneath 0.05 T was abstinent by a magnetometer fabricated appliance DC-SQUID probes (Tristan Technologies) in affiliation with a 3He-4He concoction refrigerator bottomward to 25 mK. Earth’s alluring acreage was alone by appliance a Nb superconducting absorber covered with a μ-metal tube. Aloft 3 T, the magnetization was abstinent appliance the Faraday adjustment in a concoction refrigerator bottomward to 80 mK (38). The specific calefaction was abstinent by a thermal alleviation technique. The Breakthrough Design Concrete Property Altitude Arrangement was acclimated for the abstracts aloft 0.4 K. For abstracts at lower temperatures bottomward to 30 mK, a home-made specific calefaction corpuscle installed in a 3He-4He concoction refrigerator was used.

HAXPES abstracts were performed at the RIKEN Coherent X-ray Optics Beamline (BL29XU) in the SPring-8 synchrotron ability (39, 40). Photoelectrons aflame by a 7.94-keV x-ray were analyzed appliance a Scienta R4000-10kV hemispherical electron spectrometer. The absolute activity resolution was set to ΔE = 250 meV. Clean bright surfaces were acquired by fracturing in situ beneath the abject burden of ~ 10−8 Pa at allowance temperature. All spectra were acquired at the sample temperature of 20 K. The Fermi akin EF was bent by barometer the Fermi bend of an evaporated Au blur electrically contacted to the sample.

Supplementary actual for this commodity is accessible at http://advances.sciencemag.org/cgi/content/full/4/2/eaao3547/DC1

Supplementary text

fig. S1. Yb 3d and Al 1s amount akin spectrum of α-YbAlB4.

fig. S2. Yb 3d amount akin applicable for HAXPES data.

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fig. S3. Temperature assurance of the alluring susceptibility acquired beneath a acreage of 0.1 T forth the c arbor for x = 0, 1.0, 1.4, and 1.7% and forth the ab even for x = 0 and 4.2%.

fig. S4. Temperature assurance of the changed alluring susceptibility acquired beneath a acreage of 0.1 T forth the c arbor for x = 0, 1.0, 1.4, 1.7, and 4.2%.

fig. S5. Fe body assurance of the filigree connected and its affiliation to the Yb valence change.

fig. S6. Normalized crumb x-ray diffraction abstracts at about 400 aiguille for α-YbAl1−xFexB4 (x = 0.5, 1.3, 1.4, 1.7, and 2.2%), area the acuteness and the drop bend 2θ are normalized by those ethics at the capital peak.

fig. S7. Electron diffraction patterns of x = 0 for [001] administration at 300 and 14 K (top) and for [010] administration at 300 and 13 K (bottom).

fig. S8. Electron diffraction patterns of x = 4.2% for [001] administration at 300 and 14 K (top) and for [3-10] administration at 300 and 13 K (bottom).

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fig. S9. The temperature assurance of the specific calefaction C disconnected by temperature T acquired at x = 0 and 1.4%.

fig. S10. Aberrant ability law temperature assurance of the a-axis resistivity at the zero-field breakthrough valence criticality and the field-induced antiferromagnetic instability.

References (41–49)

This is an open-access commodity broadcast beneath the agreement of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so continued as the resultant use is not for bartering advantage and provided the aboriginal assignment is appropriately cited.

Y. Arai, T. Sako, Y. Takebayashi, Supercritical Fluids (Springer, 2002).

T. Moriya, Circuit Fluctuations in Itinerant Electron Allure (Springer, 1985).

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S. Hüfner, Photoelectron Spectroscopy (Springer, ed. 3, 2003).

R. D. Cowan, The Approach of Atomic Anatomy and Spectra (University of California Press, 1981).

Acknowledgments: We acknowledge E. C. T. O’Farrell, N. Horie, S. Watanabe, and K. Ueda for abutment and advantageous discussions. Funding: This assignment was partially accurate by Grants-in-Aid for Accurate Analysis (16H02209) and Affairs for Advancing Strategic International Networks to Accelerate the Circulation of Talented Researchers (no. R2604) from the Japanese Society for the Promotion of Science; by Grants-in-Aids for Accurate Analysis on Innovative Areas (15H05882, 15H05883, and 26103002) of the Ministry of Education, Culture, Sports, Science, and Technology of Japan; and by the Amount Analysis for Evolutionary Science and Technology (JPMJCR15Q5), Japan Science and Technology Agency. The use of the accessories of the Abstracts Design and Assuming Laboratory at the Institute for Solid Accompaniment Physics, The University of Tokyo, is acknowledged. HAXPES abstracts were performed at BL29XU in SPring-8 with the approval of RIKEN (proposal nos. 20090041 and 20100057). Author contributions: K.K. and Y.M. contributed appropriately to this activity including sample preparation, thermodynamic and carriage measurements, and abstracts analysis/interpretation. M.O. conducted HAXPES abstracts and contributed to abstracts assay and interpretation. Y.T., M.M., R.E., M.T., A.C., S. Shin, K.T., Y.N., M.Y., and T.I. contributed to HAXPES measurements. S. Suzuki., K.S., and D.N.-H. contributed to structural analyses. Y.S., T.S., and Y.K. agitated out low-temperature magnetization measurements. S.N. conceived the activity and akin the analysis and contributed to bright growth, characterization, and abstracts interpretation. S.N., Y.M., and K.K. wrote the paper. All authors discussed the after-effects and commented on the manuscript. Aggressive interests: The authors acknowledge that they accept no aggressive interests. Abstracts and abstracts availability: All abstracts bare to appraise the abstracts in the cardboard are present in the cardboard and/or the Supplementary Materials. Additional abstracts accompanying to this cardboard may be requested from the authors.

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