arXiv subjects

Donglai Feng

Publications and source records attributed to Donglai Feng.

At least 19 recordsLinked to original sources

arXiv2026

Dimensional crossover and local strain induced deflection of the spin spiral state in multiferroic NiI2

Low-dimensional multiferroics hold great promise for integrated magnetoelectric devices. Spin spiral state has recently been shown to induce ferroelectricity in single-layer van der Waals (vdW) material NiI2. However, how this state evolves and can be tuned towards the two-dimensional limit remain unclear. Here, we combine spin-polarized scanning tunneling microscopy, layer-by-layer film growth, and multi-scale theoretical modeling to investigate the spin spirals in NiI2 thin films. As the film thickness increases from 1 to 7 monolayers, we observed a continuous increase of spin-spiral wavelength and a rotation of wavevector from near [110] to [1-10] direction, which evidences a dimensional crossover primarily driven by enhanced interlayer exchange energy. Moreover, we find that the film wrinkles can cause deflection of the spin spiral wavevector, which is caused by local curvature induced modification of exchange interactions. Our findings establish thickness and local strain as two tuning methods for engineering non-collinear helical magnetism and accompanied electric polarization in vdW multiferroics.

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arXiv2026

A Disconnected Superconducting Regime at the Parent Limit of Infinite-Layer Nickelates

Infinite-layer nickelates have been widely viewed as cuprate analogs in which superconductivity emerges and forms a superconducting dome centered around 10-20% cation substitution. Here we show that pristine and stoichiometric PrNiO2, without cation substitution, exhibits intrinsic superconductivity characterized by zero resistance and diamagnetism in uncapped films. Through heterostructure engineering, we further exclude an interfacial origin of the superconductivity. Remarkably, zero-resistance superconductivity is consistently observed in trivalent-substituted PrNiO2, whereas it is rapidly suppressed by dilute divalent substitution. Combined with angle-resolved photoemission studies, these results indicate that such a new superconducting regime is confined to within 3% additional hole doping from pristine PrNiO2. Furthermore, this phase is separated from the previously established superconducting dome around ~ 20% divalent doping by a non-superconducting region in the phase diagram, and is further distinguished by a remarkably stronger upper-critical-field anisotropy. These findings establish a unique separated superconducting regime, suggesting that infinite-layer nickelates are not merely cuprate analogs but host distinct superconducting physics.

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arXiv2026

Marginal-Fermi-Liquid-like Behavior without Pseudogap in Infinite-Layer Nickelates

Pseudogap formation, strange-metal behavior and unconventional superconductivity are closely intertwined in hole-doped cuprates, yet their relationship remains unresolved. Infinite-layer nickelates offer a distinct 3d9-derived platform to address this question by combining a cuprate-like Ni dx2-y2 Fermi surface with multiband electronic degrees of freedom. Here we use angle-resolved photoemission spectroscopy to resolve the low-energy spectral function of superconducting La0.8Ca0.2NiO2 and parent LaNiO2 thin films. In La0.8Ca0.2NiO2, the electronic self-energy Im Sigma(omega) is approximately linear in energy and its slope increases from (pi/2, pi/2) to (pi, 0), revealing momentum-dependent marginal-Fermi-liquid-like scattering. Both films show a progressive suppression of low-energy spectral weight from the diagonal direction toward (pi, 0), with stronger suppression in parent LaNiO2. However, finite Fermi-level spectral weight persists around the entire Fermi surface, with no leading-edge shift or back-bending indicative of pseudogap formation in either the electron pocket or the cuprate-like hole band. Our results demonstrate that momentum-selective correlations and marginal-Fermi-liquid-like scattering can occur without a detectable cuprate-like pseudogap, providing a benchmark for identifying the essential normal-state electronic ingredients of high-temperature superconductivity.

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arXiv2026

Direct observation of interfacial exchange coupling in a magnetic tunnel junction through spin-polarized quasiparticle interference

Interfacial exchange coupling plays a critical role in enabling novel phenomena in magnetic heterostructures, such as spin triplet superconductivity, quantum anomalous Hall effect (QAHE), and advanced spintronic functionalities. While microscopic characterization of this coupling is essential for elucidating the underlying mechanism, it remains technically challenging. Here, using spin-polarized scanning tunneling microscopy (SP-STM) and quasiparticle interference, we directly observed interfacial exchange coupling in a magnetic tunnel junction formed by an Fe coated tip and a Cr(001) surface. We found the ferromagnetic tip induces significant energy shift (up to 10 meV) in the spin-polarized surface state of Cr(001). This shift is highly sensitive to the tip-surface distance and the spin-alignment between Fe tip and Cr surface, which can be switched by external magnetic field. Our results demonstrate that extended 2D surface states can mediate strong exchange coupling across a heterojunction, enabling local control of interfacial exchange interaction induced phenomena.

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arXiv2026

Electronic Origin of Ferromagnetic Excitations in the Candidate Spin-Triplet Superconductor CeSb2

The origin of quasi-one-dimensional (q1D) ferromagnetic (FM) excitations in the candidate spin-triplet superconductor CeSb$_2$ has remained unclear. Here we report an electronic mechanism for emergent q1D magnetism in the quasi-two-dimensional lattice of CeSb$_2$, revealed by angle-resolved photoemission spectroscopy (ARPES). High-resolution ARPES resolves no spin-density-wave gap on the dispersive Fermi pockets, disfavoring a nesting-driven mechanism for the q1D FM excitations. Instead, resonant ARPES reveals a pronounced selective enhancement of Ce 4$f$ spectral weight on the $C_2$-distributed Fermi pockets aligned with the Ce ladder. This observation signifies band-selective Kondo coupling that generates strongly anisotropic magnetic exchange interactions, which can naturally account for both the q1D ferromagnetic excitations and the competing magnetic orders. Our results identify a band-selective Kondo coupling mechanism for emergent low-dimensional magnetism in correlated $f$-electron systems.

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arXiv2026

$3d_{z^2}$ orbital delocalization and magnetic collapse in superconducting (La,Pr)$_3$Ni$_2$O$_{7-\delta}$ films

The recent discovery of Ruddlesden--Popper (RP) nickelate thin-film superconductors has opened a new frontier in unconventional superconductivity. Its realization requires both compressive epitaxial strain and highly oxidative growth conditions, yet the microscopic pathway from the parent phase to the superconducting phase remains elusive. Here, X-ray absorption spectra and resonant inelastic X-ray scattering are employed to track this evolution by independently tuning strain and oxygen content in (La,Pr)$_3$Ni$_2$O$_{7-\delta}$ thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge in the same way upon two independent tunings: Spectral weight transfers from a ''Upper Hubbard''-like peak to the hole-like peak associated with O $2p_z$ state, and in parallel, the initially localized Ni $3d_{z^2}$ orbital becomes more itinerant followed by the broadening and weakening of $dd$ orbital excitations. Second, as itinerancy increases, long-range spin-density-wave (SDW) order is suppressed in both intensity and correlation length, indicating direct competition with superconductivity. Yet, short-range magnons persist: they become damped but their bandwidth stays unchanged. Our results paint a coherent picture that both strain and oxygenation drive the RP bilayer nickelates towards the superconducting instability, where the O $2p_z$ and Ni $3d_{z^2}$ orbitals become delocalized. Concomitantly, the long-range magnetic order loses coherence and gets suppressed. These findings establish an orbital-selective route to RP nickelate superconductivity, in which the delocalization of the $2p_z$ and $3d_{z^2}$ orbitals and the robust short-range magnons upon the melting of SDW order are prerequisites, providing strong constraints for theory and the roadmap for designing nickelate superconductors.

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arXiv2026

Microscopic evidence of spin-driven multiferroicity and topological spin textures in monolayer NiI2

In type II multiferroics, noncollinear spin textures are expected to induce electric polarization directly, leading to strong magnetoelectric coupling. Realizing such spin driven multiferroicity in two-dimensional systems, and elucidating the interplay between local spins and electric polarization, are of both fundamental and technological importance. Here, using vectorial spin polarized scanning tunneling microscopy, we investigated the spin-driven multiferroicity in monolayer NiI2 at atomic scale. We identify a canted spin-spiral state with fully determined spin rotation plane, accompanied by a 2Q charge modulation. At spin spiral domain walls, we discover topological spin textures that composed of meron/antimeron pairs. These textures are associated with distinct charge pattern and notable band shifts, indicating local bound charges induced by variations of ferroelectricity at domain wall. Our observations are well captured by a realistic spin model incorporating Kitaev interactions and generalized spin-current model of type II multiferroicity. The findings provide microscopic evidence of spin-driven multiferroicity in an extreme 2D system and establish a platform for low-dissipation, electric-field control of topological spin textures.

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arXiv2026

Dissecting superconductivity in the Ruddlesden-Popper nickelates: The role of electron correlation and interlayer magnetic exchange

The discovery of superconductivity in the Ruddlesden-Popper (RP) nickelates has opened a new chapter in the search for high superconducting transition temperatures ($T_\mathrm{c}$) materials. A central and puzzling feature of this family is the wide variation in $T_\mathrm{c}$ despite their common NiO$_2$ building blocks, as highlighted by the recent observation of superconductivity at $\sim$ 30 K in trilayer $\mathrm{La_4Ni_3O_{10}}$, significantly lower than 80 K reported in bilayer $\mathrm{La_3Ni_2O_7}$. Understanding the factors that control $T_\mathrm{c}$ in this family is therefore of paramount importance. Here, we use resonant inelastic x-ray scattering (RIXS) to investigate the electronic and magnetic excitations of $\mathrm{La_4Ni_3O_{10}}$ in direct comparison with its bilayer counterpart. Our results reveal a markedly different landscape. $\mathrm{La_4Ni_3O_{10}}$ exhibits a more itinerant character, evidenced by broader Ni $dd$ orbital excitations and a strong Ni 3$d$ fluorescence continuum, suggesting weaker electronic correlations than in the bilayer. Despite this, well-defined collective spin excitations persist, including dispersive acoustic and optical magnon branches alongside an incommensurate spin density wave. Using linear spin wave theory, we extract the interlayer superexchange interaction ($J_z$) to be $\sim$ 22 meV, much smaller than that in $\mathrm{La_3Ni_2O_7}$. The weaker correlation and reduced interlayer exchange together provide a consistent explanation for the substantially lower $T_\mathrm{c}$ in the trilayer compound. Our findings establish interlayer magnetic coupling and electronic correlation as key parameters governing superconductivity in layered nickelates and offer critical constraints for understanding the pairing mechanism in this emerging family.

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arXiv2026

Anisotropic Electronic Correlations in the Spin Density Wave State of La$_3$Ni$_2$O$_7$

The bilayer nickelate superconductor La$_3$Ni$_2$O$_7$ undergoes a density wave transition near 150 K that has attracted intensive scrutiny, yet its microscopic origin remains elusive. Here we report polarization-resolved electronic Raman scattering measurements on high-quality single crystals of La$_3$Ni$_2$O$_7$. Below 150\,K, we observe a pronounced, symmetry-dependent redistribution of spectral weight in B$_{1g}$ and B$_{2g}$ channels, consistent with the formation of spin-density-wave (SDW) gaps. Quantitative analysis reveals momentum-selective SDW gap amplitudes, with intermediate-to-strong coupling near X/Y points of the Brillouin zone and weaker coupling along the diagonal direction, indicating an unconventional SDW driven by anisotropic electronic correlations. Our results establish the electronic character of the SDW in La$_3$Ni$_2$O$_7$, and provide a microscopic foundation for understanding the emergence of high-temperature superconductivity under pressure in nickelates.

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arXiv2026

Direct Observation of Unidirectional Density Wave and Band splitting in a Single-Domain Trilayer Nickelate Pr$_4$Ni$_3$O$_{10}$

Unraveling the interplay between density-wave (DW) instabilities and multi-orbital physics is critical for understanding superconductivity in Ruddlesden-Popper nickelates, yet intrinsic electronic features have been persistently obscured by material inhomogeneity and thus the multi-domain averaging effect. Here, we employ micro-focused angle-resolved photoemission spectroscopy ($\mu$-ARPES) on single-domain Pr$_4$Ni$_3$O$_{10}$ to disentangle the complex hierarchy of intrinsic and back-folded bands, explicitly identifying the electronic states driving the DW phase transition. We provide decisive spectroscopic evidence that the low-energy reconstruction is governed by inter-orbital nesting between the $\alpha$ and $\beta$ bands. Specifically, we resolve a orbital-dependent gap of $\sim44$ meV on the $\alpha$ pocket, a value quantitatively consistent with prior measurements, unifying previously conflicting experimental reports regarding the locus and magnitude of the DW gap. Furthermore, we reveal strong orbital-selective mass renormalization in the $d_{z^2}$ states and successfully resolve the long-sought intrinsic trilayer $\beta$-band splitting, establishing a critical lower bound for the outer-layer hopping. These results define a coherent microscopic fingerprint for the trilayer nickelates, identifying the specific nesting channels and correlation effects that underpin the phase diagram.

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arXiv2026

Contrasting Momentum-Selective Spin-Density-Wave Gaps in Bilayer and Trilayer Nickelates

Resolving where the density-wave gap opens in momentum space is essential for identifying the microscopic origin of the instability in layered nickelates. Using polarization-resolved electronic Raman scattering, we map the momentum selectivity of the spin-density-wave (SDW) gap in trilayer La4Ni3O10. We observe a SDW-induced redistribution of spectral weight on both the $\alpha$ pocket at the Brillouin-zone centre and a portion of the $\beta$ pocket near the zone boundary, characterized by gap energies of approximately 55~meV. In contrast, no comparable spectral weight suppression is observed along the diagonal region of $\beta$ pockets, implying little or no gap opening. This gap topology contrasts sharply with that in La3Ni2O7, where anisotropic SDW gaps open solely on the $\beta$ pocket. Our results establish a distinct momentum-space gap topology between bilayer and trilayer nickelates, placing new constraints on the ordering wave vector and the mechanism of the density-wave instability relevant to superconductivity.

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arXiv2025

Thermoelectricity evidence for quantum criticality in clean infinite-layer nickelate films

We investigate the Seebeck coefficient ($S$) in infinite-layer nickelate films with different disorder levels. The disordered NdNiO$_{2}$ film exhibits a flat $S/T$ curve, whereas cleaner samples display a logarithmic divergence with decreasing temperature, followed by a pronounced ``hump'' near 25 K. These distinct behaviors reveal a disorder-driven transition from band-structure-dominated transport to quantum-critical-dominated transport. Below the ``hump'' temperature, four-fold symmetry breaking is observed in the in-plane angular magnetoresistance, indicating the presence of short-range antiferromagnetic order in parent infinite-layer nickelate films. Furthermore, the logarithmic divergence in $S/T$ is also observed in a clean superconducting Sm$_{0.73}$Ca$_{0.05}$Eu$_{0.22}$NiO$_{2}$ film, where it coexists with linear-in-temperature resistivity over the same temperature range. These findings demonstrate the existence of quantum criticality over a wide doping range in clean infinite-layer nickelate films, similar to cuprates, which highlights the central role of antiferromagnetic spin correlations in their superconducting pairing mechanisms.

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arXiv2025

Observation of superconductivity-induced leading-edge gap in Sr-doped $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films

The discovery of high-temperature superconductivity in pressurized bulk $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ has ignited significant interest in nickelate superconductors. Unlike cuprates, where superconductivity predominantly originates from the $\mathrm{3}d_{x^2-y^2}$ orbital, nickelates exhibit additional complexities involving contributions from the $\mathrm{3}d_{z^2}$ orbital, prompting fundamental questions about their pairing mechanisms. Despite recent progress in stabilizing superconductivity in $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films at ambient pressure, direct spectroscopic evidence of the superconducting gap opening remains elusive. Here, we present an in-situ angle-resolved photoemission spectroscopy study of Sr-doped superconducting $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films. Fermi surface mapping reveals Ni-$\mathrm{3}d_{x^2-y^2}$-derived $\alpha$ and $\beta$ pockets, with orbital fillings of 0.11$\pm$0.02 electrons and 0.66$\pm$0.03 holes per Ni, respectively, resulting in a total of 0.45$\pm$0.04 electrons for each Ni. These bands exhibit moderate electron correlations, characterized by a band renormalization factor of 3-4. Notably, both $\alpha$ and $\beta$ bands exhibit leading-edge shifts across the superconducting transition, with gap magnitude of ~1-2 meV at Fermi momenta along the Brillouin zone diagonal and slightly away from the zone diagonal, deviating from the conventional $d_{x^2-y^2}$-wave gap structure. Additionally, the Ni-$\mathrm{3}d_{z^2}$-derived $\gamma$ band lies ~75 meV below the Fermi level, indicating a $\mathrm{3}d_{x^2-y^2}$-dominated fermiology in this compound.

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arXiv2025

Observation of Electride-like $s$ States Coexisting with Correlated $d$ Electrons in NdNiO$_2$

Despite exhibiting a similar $d_{x^2-y^2}$ band character to cuprates, infinite-layer nickelates host additional electron pockets that distinguish them from single-band cuprates. The elusive orbital origin of these electron pockets has led to competing theoretical scenarios. Here, using polarization-dependent and resonant angle-resolved photoemission spectroscopy (ARPES), we determine the orbital character of the Fermi surfaces in NdNiO$_2$. Our data reveal that the electron-like pocket arises predominantly from interstitial $s$ states, with negligible contributions from rare-earth 5$d$ and 4$f$ orbitals near the Fermi level. The observation of well-defined quantum well states indicates a uniform distribution of these interstitial electrons throughout the film thickness. By comparing with electronic structure of LaNiO$_2$, we find that the rare-earth element modulates the Ni-derived bands and hopping integrals through a chemical pressure effect. These findings clarify the role of rare-earth elements in shaping the low-energy electronic structure and establish the presence of electride-like interstitial $s$ states in a correlated oxide system, where electrons occupy lattice voids rather than atomic orbitals. The electride-like character offer new insight into the self-doping and superconductivity in infinite-layer nickelates.

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arXiv2025

High Temperature Superconductivity Dominated by Inner Underdoped CuO$_2$ Planes in Quadruple-Layer Cuprate (Cu,C)Ba$_2$Ca$_3$Cu$_4$O$_{11+\delta}$

The superconducting transition temperature ($T_{\mathrm{c}}$) of trilayer or quadruple-layer cuprates typically surpasses that of single-layer or bilayer systems. This observation is often interpreted within the ``composite picture", where strong proximity effect between inner CuO$_2$ planes (IPs) and outer CuO$_2$ planes (OPs) is crucial. Albeit intriguing, a straightforward scrutinization of this composite picture is still lacking. In this study, using angle-resolved photoemission spectroscopy to investigate (Cu,C)Ba$_2$Ca$_3$Cu$_4$O$_{11+\delta}$ (CuC-1234) with a high $T_{\mathrm{c}}$ of 110~K, we found that the OPs are not superconducting at the $T_{\mathrm{c}}$ of the material. Instead, the large pairing strength and phase coherence concurrently emerge at the underdoped IPs, suggesting that the high $T_{\mathrm{c}}$ is primarily driven by these underdoped IPs. Given that the $T_{\mathrm{c}}$ of CuC-1234 is comparable to other trilayer or quadruple-layer cuprates, our findings suggest that the conventional ``composite picture" is not universally required for achieving high $T_{\mathrm{c}}$. More importantly, we demonstrate that CuO$_2$ planes free of apical oxygen can support superconductivity up to 110~K even at a doping level of 0.07 holes per Cu, a level that lies deep in the underdoped regime of single- and bilayer cuprates. These findings provide new insights into the origin of high $T_{\mathrm{c}}$ in multilayer cuprates.

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arXiv2025

Unconventional band splitting of CeSb in the devil's staircase transition

The interplay between magnetism and electronic band structure is a central theme in condensed matter physics. CeSb, with its complex devil's staircase antiferromagnetic transition, offers a unique opportunity to explore this interplay. Using angle-resolved photoemission spectroscopy (ARPES), we investigate the electronic structure evolution across the devil's staircase transition. Upon entering the antiferromagnetic phase, we observe an intriguing band splitting of the electron pocket around the X point. The energy separation between the split bands changes abruptly with temperature, consistent with the characteristics of the first-order phase transition. However, their respective spectral weights behave gradually with temperature. Combined with our density functional theory (DFT) calculations, we suggest that this atypical behavior deviates from conventional magnetically induced band splitting and potentially arises from the intricate modulation of paramagnetic and antiferromagnetic layers within the devil's staircase transition. Our results provide insights into the complex relationship between electronic structure and magnetism in correlated electron systems.

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arXiv2025

Revealing the electron-spin fluctuation coupling by photoemission in CaKFe4As4

Electron-boson coupling in unconventional superconductors is one of the key parameters in understanding the superconducting pairing symmetry. Here, we report definitive photoemission evidence of electron-spin exciton coupling in the iron-based superconductor CaKFe4As4, obtained via high-resolution ARPES. Our study identifies a distinct kink structure on the {\alpha} band, observable only in the superconducting phase and closely linked with the superconductivity, indicative of strong electron-boson interactions. Notably, this kink structure corresponds to two distinct bosonic modes at 11 meV and 13 meV, aligning with spin resonance modes previously observed in inelastic neutron scattering experiments. This alignment underscores the significant role of antiferromagnetic fluctuations in the pairing mechanism of this superconductor. Furthermore, the unique momentum-dependent and orbital-selective properties of the coupling revealed by ARPES provide profound insights into the pairing symmetry, suggesting predominantly s_+- wave pairing facilitated by spin fluctuations. Our findings not only highlight the pivotal role of spin resonance in the superconductivity of CaKFe4As4 but also enhance understanding of the electron-spin exciton interactions in unconventional superconductors.

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arXiv2024

Revealing nanoscale structural phase separation in La$_{3}$Ni$_{2}$O$_{7-\delta}$ single crystal via scanning near-field optical microscopy

The discovery of superconductivity in La3Ni2O7-${\delta}$ under high pressure,with an onset critical temperature around 80 K, has sparked significant interest in the superconducting phases of Ruddlesden-Popper nickelates, Lan+1NinO3n+1. While La4Ni3O10 exhibits nearly 100% superconductivity with Tc~30 K under high pressure, magnetic susceptibility studies on La3Ni2O7-${\delta}$, however, reveal a more complex picture, indicating either filamentary superconductivity or that approximately 50% of crystal phase becomes superconducting in polycrystalline samples. In this study, we employed scattering-type scanning near-field optical microscopy to visualize nanoscale structural phase separation in La3Ni2O7-${\delta}$, identifying enhanced optical conductivity with stripes approximately 183 nm wide. These stripes run diagonally with respect to the Ni-O-Ni bond directions in the a-b plane, ruling out the possibility that they arise from impurity phases, like the '1313', '214' or '4310' structures. The dark regions and bright stripes exhibit optical conductivities ~ 22% and 29% of gold's, respectively. Additionally, we find that the bright stripes constitute about 38% of the total field of view, while the remainder consists of dark regions and the transitional region between dark regions and bright stripes. Our results suggest that optical conductivity stripes originate from nanoscale structural phase separation. In contrast, La4Ni3O10 exhibits uniform and higher optical conductivity with no observable evidence of phase separation. Thus, our study represents a pioneering effort to directly image nanoscale phase separation in Lan+1NinO3n+1 nickelates. This observation could provide crucial insights into the factors that limit the superconducting volume fraction of La3Ni2O7-${\delta}$, highlighting SNOM as a powerful probe for exploring nanoscale low-energy physics in correlated quantum materials.

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