arXiv subjects

Ilija Zeljkovic

Publications and source records attributed to Ilija Zeljkovic.

At least 19 recordsLinked to original sources

arXiv2026

Unmodeled states and uncertain action outcomes in agentic scanning tunneling microscopy

In physical experiments, interventions can alter hidden experimental states in ways that cannot be predicted in advance. Autonomous scientific agents must therefore interpret the consequences of their interventions while operating with incomplete knowledge of the experimental state. Here we investigate this problem using scanning tunneling microscopy (STM) tip conditioning, traditionally a human-expert-intensive task governed by inaccessible tip apex conditions and uncertain action outcomes. We introduce quailbot, an agent harness that places the LLM inside the instrument feedback loop by linking physical interventions with experimental readbacks. After a brief apprenticeship with a human expert, frontier LLM agents autonomously completed end-to-end tip conditioning on an STM and passed an independent verification. The contingencies that arose during the experiments further exposed the limits of LLM agentic autonomy when relevant experimental states or dynamics were hidden or unmodeled. Our results show that future autonomous physical experimentation requires agents to infer hidden and unmodeled experimental states, track the outcomes of their actions, and operate within the observability and action limits of real instruments.

cond-mat.mes-hall↗

arXiv2026

Phase-shifted multicomponent spin-charge nematicity in an altermagnet

Altermagnets host spin-split Fermi surfaces without net magnetization. This intrinsically multicomponent electronic setting raises the possibility that familiar correlated electron phases acquire unconventional spin-charge structure. Here we report the discovery of altermagnetic nematicity in Co0.25NbSe2. Using spectroscopic-imaging scanning tunneling microscopy and spin-polarized scanning tunneling microscopy, we find that the three nominally C3-related directions lose rotational equivalence in the zero-field state, in both charge and spin-sensitive tunneling channels. Strikingly, the dominant spin-sensitive component is shifted by one C3 sector relative to the dominant charge component, revealing a phase-shifted spin-charge nematic response. A phenomenological theory shows that altermagnetic order favors a finite relative phase between the charge and spin-sensitive nematic components -- C3 lattice pinning frustrates this preferred offset and selects the observed phase locking. These results establish altermagnetic nematicity as a new form of multicomponent electronic liquid-crystal order and point to a potentially generic route by which altermagnets can transform conventional correlated phases into symmetry-engineered spin-charge orders.

cond-mat.str-el↗

arXiv2026

Robust spin splitting and fermiology in a layered altermagnet

Altermagnetism defies conventional classifications of collinear magnetic phases, standing apart from ferromagnetism and antiferromagnetism with its unique combination of spin-dependent symmetries, net-zero magnetization, and anomalous Hall transport. Although altermagnetic states have been realized experimentally, their integration into functional devices has been hindered by the structural rigidity and poor tunability of existing materials. First, through cobalt intercalation of the superconducting 2H-NbSe$_2$ polymorph, we induce and stabilize a robust altermagnetic phase and using both theory and experiment, we directly observe the lifting of Kramers degeneracy. Additionally, we present spectroscopic insight into a previously hinted low-temperature phase, and provide evidence of its electronic origin. While shedding light on overlooked aspects of altermagnetism, these findings open pathways to spin-based technologies and lay a foundation for advancing the emerging field of altertronics.

cond-mat.str-el↗

arXiv2025

Pervasive electronic nematicity as the parent state of kagome superconductors

Kagome superconductors $A$V$_3$Sb$_5$ ($A$ = Cs, K, Rb) have developed into an exciting playground for realizing and exploring exotic solid state phenomena. Abundant experimental evidence suggests that electronic structure breaks rotational symmetry of the lattice, but whether this may be a simple consequence of the symmetry of the underlying 2 $\times$ 2 charge density wave phase or an entirely different mechanism remains intensely debated. We use spectroscopic imaging scanning tunneling microscopy to explore the phase diagram of the prototypical kagome superconductor CsV$_3$Sb$_5$ as a function of doping. We intentionally suppress the charge density wave phase with chemical substitutions selectively introduced at two distinct lattice sites, and investigate the resulting system. We discover that rotational symmetry breaking of the electronic structure -- now present in short-range nanoscale regions -- persists in all samples, in a wide doping range long after all charge density waves have been suppressed. As such, our experiments uncover ubiquitous electronic nematicity across the $A$V$_3$Sb$_5$ phase diagram, unrelated to the 2 $\times$ 2 charge density wave. This further points towards electronic nematicity as the intrinsic nature of the parent state of kagome superconductors, under which other exotic low-temperature phenomena subsequently emerge.

cond-mat.str-el↗

arXiv2025

Kagome metals

Three important driving forces for creating qualitatively new phases in quantum materials are the topology of the materials' electronic band structures, frustration in the electrons' motion or magnetic interactions, and strong correlations between their charge, spin, and orbital degrees of freedom. In very few material systems do all of these aspects come together to contribute on an equal footing to stabilize new electronic states with unprecedented properties; however the search for such systems can be guided by models of configurational motifs or key sublattices that can host such physics. One of the most fascinating structural motifs for realizing this rich interplay of frustration, electronic topology, and electron correlation effects is the kagome lattice. In this review, we provide an overview of the theoretical underpinnings driving the physics of kagome lattices, and we then discuss experimental progress in realizing novel states enabled by kagome networks in crystalline materials. Different material classes are discussed with an emphasis on the phenomenologies of their electronic states and how they map to interactions arising from their kagome lattices.

cond-mat.str-el↗

arXiv2025

Frieze charge-stripes in a correlated kagome superconductor CsCr$_3$Sb$_5$

Kagome metals have developed into a vibrant playground for materials physics, where geometric frustration, electronic correlations and band topology come together to create a variety of exotic phenomena. Recently synthesized CsCr$_3$Sb$_5$ has provided a rare opportunity to explore unconventional superconductivity in a strongly correlated kagome system with hints of frustrated magnetism and quantum criticality. Using spectroscopic imaging scanning tunneling microscopy, we reveal a cascade of density wave transitions with different symmetries in bulk single crystals of CsCr$_3$Sb$_5$. In particular, we discover a new electronic state $-$ a unidirectional density wave that breaks all mirror symmetries akin to a chiral density wave, but in contrast retains a mirror-glide symmetry. We term this state a frieze charge-stripe order phase, because its symmetry properties agree with one of the fundamental frieze symmetry groups. A combination of high-resolution imaging, Fourier analysis and theoretical simulations uncovers the crucial role of sublattice degrees of freedom in forming this phase, with internal chiral textures of opposite handedness. Our experiments reveal that superconductivity in CsCr$_3$Sb$_5$ develops from a new type of a unidirectional density wave, and set the foundation for exploring electronic states with frieze symmetry groups in quantum materials.

cond-mat.str-el↗

arXiv2025

Limitations of detecting structural changes and time-reversal symmetry breaking in scanning tunneling microscopy experiments

The family of kagome superconductors $A$V$_3$Sb$_5$ ($A$=K, Cs, Rb) is an exciting playground for investigating various density waves, unusual superconductivity and a surprising time-reversal symmetry breaking despite the absence of spin magnetism. The origin of time-reversal symmetry breaking has been of particular interest, and conflicting results have been intensely debated. Scanning tunneling microscopy (STM) provided crucial evidence by the observation that apparent chirality associated with the 2 $\times$ 2 charge density wave (CDW) may be modified by the direction of magnetic field, a phenomenon observed in select sample areas in some experiments, but not others. Related to this, Xing et al. investigated the effects of magnetic and electric fields on the 2 $\times$ 2 CDW state and the lattice structure of kagome superconductor RbV$_3$Sb$_5$. They report a $\sim$ 1% change in the in-plane lattice constants, concomitant with the CDW intensities modification, controlled by the field direction. This was interpreted as a rare case of piezomagnetism. Here we show how the apparent magnetic field induced lattice and CDW intensity change is a consequence of two independent experimental artifacts: reconfiguration of atoms at the STM tip apex that alter the amplitudes of CDW modulations, and piezo creep, hysteresis, and thermal drift that artificially distort STM topographs. We find no evidence supporting that magnetic field leads to intrinsic changes in the sample, which challenges reported piezomagnetism.

cond-mat.supr-con↗

arXiv2025

Discovery of magnetic-field-tunable density waves in a layered altermagnet

Altermagnets recently came into the spotlight as a new class of magnetic materials, arising as a consequence of specific crystal symmetries. They are characterized by a spin-polarized electronic band structure similar to ferromagnets, but with net zero magnetization, and touted as a promising platform to host a slew of exotic properties, many of which are yet to be explored. Here we study a new layered triangular lattice altermagnet, Co-intercalated NbSe$_2$ using scanning tunneling microscopy and spectroscopy (STM/S). Differential conductance dI/dV spectra at low temperature reveal a surprising partial gap opening centered at the Fermi level, which is not captured by density functional theory calculations of the system in the pure altermagnetic state. Spatial mapping using spectroscopic-imaging STM and spin-polarized STM further reveals emergent tri-directional charge and spin density modulations with a 2a$_0$ wave length. Interestingly, we discover that out-of-plane magnetic field can serve as a knob to tune the amplitudes of the modulations as well as alter the overall electronic density-of-states in a manner that is strongly dependent on the field direction and strength. This can be attributed to the tilting of spins by the external magnetic field, which can have profound implications on the electronic properties of the altermagnet. By providing elusive atomic-scale insights, our work uncovers a tunable density wave accompanied by concomitant changes in the electronic band structure, and sets the foundation for studies of correlated electronic phenomena in altermagnets.

cond-mat.str-el↗

arXiv2024

Pomeranchuk instability from electronic correlations in CsTi$_3$Bi$_5$ kagome metal

Among many-body instabilities in correlated quantum systems, electronic nematicity, defined by the spontaneous breaking of rotational symmetry, has emerged as a critical phenomenon, particularly within high-temperature superconductors. Recently, this behavior has been identified in CsTi$_3$Bi$_5$, a member of the AV$_3$Sb$_5$ (A = K, Rb, Cs) kagome family, recognized for its intricate and unconventional quantum phases. Despite accumulating indirect evidence, the fundamental mechanisms driving nematicity in CsTi$_3$Bi$_5$ remain inadequately understood, sparking ongoing debates. In this study, we employ polarization-dependent angle-resolved photoemission spectroscopy to reveal definitive signatures of an orbital-selective nematic deformation in the electronic structure of CsTi$_3$Bi$_5$. This direct experimental evidence underscores the pivotal role of orbital degrees of freedom in symmetry breaking, providing new insights into the complex electronic environment. By applying the functional renormalization group technique to a fully interacting ab initio model, we demonstrate the emergence of a finite angular momentum ($d$-wave) Pomeranchuk instability in CsTi$_3$Bi$_5$, driven by the concomitant action of electronic correlations within specific orbital channels and chemical potential detuning away from Van Hove singularities. By elucidating the connection between orbital correlations and symmetry-breaking instabilities, this work lays a crucial foundation for future investigations into the broader role of orbital selectivity in quantum materials, with far-reaching implications for the design and manipulation of novel electronic phases.

cond-mat.str-el↗

arXiv2024

Quantifying magnetic field driven lattice distortions in kagome metals at the femto-scale using scanning tunneling microscopy

A wide array of unusual phenomena has recently been uncovered in kagome solids. The charge density wave (CDW) state in the kagome superconductor AV3Sb5 in particular intrigued the community -- the CDW phase appears to break the time-reversal symmetry despite the absence of spin magnetism, which has been tied to exotic orbital loop currents possibly intertwined with magnetic field tunable crystal distortions. To test this connection, precise determination of the lattice response to applied magnetic field is crucial, but can be challenging at the atomic-scale. We establish a new scanning tunneling microscopy based method to study the evolution of the AV3Sb5 atomic structure as a function of magnetic field. The method substantially reduces the errors of typical STM measurements, which are at the order of 1% when measuring an in-plane lattice constant change. We find that the out-of-plane lattice constant of AV3Sb5 remains unchanged (within 10^-6) by the application of both in-plane and out-of-plane magnetic fields. We also reveal that the in-plane lattice response to magnetic field is at most at the order of 0.05%. Our experiments provide further constraints on time-reversal symmetry breaking in kagome metals, and establish a new tool for higher-resolution extraction of the field-lattice coupling at the nanoscale applicable to other quantum materials.

cond-mat.str-el↗

arXiv2024

Alternate cleavage structure and electronic inhomogeneity in Ca-doped YBa$_2$Cu$_3$O$_{7-δ}$

YBa$_2$Cu$_3$O$_{7-δ}$ (YBCO) has favorable macroscopic superconducting properties of $T_\mathrm{c}$ up to 93 K and $H_{c2}$ up to 150 T. However, its nanoscale electronic structure remains mysterious because bulk-like electronic properties are not preserved near the surface of cleaved samples for easy access by local or surface-sensitive probes. It has been hypothesized that Ca-doping at the Y site could induce an alternate cleavage plane that mitigates this issue. We use scanning tunneling microscopy (STM) to study both Ca-free and 10% Ca-doped YBCO, and find that the Ca-doped samples do indeed cleave on an alternate plane, yielding a spatially-disordered partial (Y,Ca) layer. Our density functional theory calculations support the increased likelihood of this new cleavage plane in Ca-doped YBCO. On this surface, we image a superconducting gap with average value 24 $\pm$ 3 meV and characteristic length scale 1-2 nm, similar to Bi-based high-$T_\mathrm{c}$ cuprates, but the first map of gap inhomogeneity in the YBCO family.

cond-mat.supr-con↗

arXiv2023

Nanoscale strain manipulation of smectic susceptibility in kagome superconductors

Exotic quantum solids can host electronic states that spontaneously break rotational symmetry of the electronic structure, such as electronic nematic phases and unidirectional charge density waves (CDWs). When electrons couple to the lattice, uniaxial strain can be used to anchor and control this electronic directionality. Here we reveal an unusual impact of strain on unidirectional "smectic" CDW orders in kagome superconductors AV3Sb5 using spectroscopic-imaging scanning tunneling microscopy. We discover local decoupling between the smectic electronic director axis and the direction of anisotropic strain. While the two are generally aligned along the same direction in regions of small CDW gap, the two become misaligned in regions where CDW gap is the largest. This in turn suggests nanoscale variations in smectic susceptibility, which we attribute to a combination of local strain and electron correlation strength. Overall, we observe an unusually high decoupling rate between the smectic electronic director of the 3-state Potts order and anisotropic strain, revealing weak smecto-elastic coupling in the CDW phase of kagome superconductors. This is phenomenologically different from the extensively studied nemato-elastic coupling in the Ising nematic phase of Fe-based superconductors, providing a contrasting picture of how strain can control electronic unidirectionality in different families of quantum materials.

cond-mat.supr-con↗

arXiv2023

Colossal orbital Zeeman effect driven by tunable spin-Berry curvature in a kagome metal

Berry phase and the related concept of Berry curvature can give rise to many unconventional phenomena in solids. In this work, we discover colossal orbital Zeeman effect of topological origin in a newly synthesized bilayer kagome metal TbV6Sn6. We use spectroscopic-imaging scanning tunneling microscopy to study the magnetic field induced renormalization of the electronic band structure. The nonmagnetic vanadium d-orbitals form Dirac crossings at the K point with a small mass gap and strong Berry curvature induced by the spin-orbit coupling. We reveal that the magnetic field leads to the splitting of gapped Dirac dispersion into two branches with giant momentum-dependent g factors, resulting in the substantial renormalization of the Dirac band. These measurements provide a direct observation of the magnetic field controlled orbital Zeeman coupling to the enormous orbital magnetic moments of up to 200 Bohr magnetons near the gapped Dirac points. Interestingly, the effect is increasingly non-linear, and becomes gradually suppressed at higher magnetic fields. Theoretical modeling further confirms the existence of orbital magnetic moments in TbV6Sn6 produced by the non-trivial spin-Berry curvature of the Bloch wave functions. Our work provides the first direct insight into the momentum-dependent nature of topological orbital moments and their tunability by magnetic field concomitant with the evolution of the spin-Berry curvature. Significantly large orbital magnetic moments driven by the Berry curvature can also be generated by other quantum numbers beyond spin, such as the valley in certain graphene-based structures, which may be unveiled using the same tools highlighted in our work.

cond-mat.mes-hall↗

arXiv2023

YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$, vanadium-based kagome metals with Yb$^{2+}$ and Eu$^{2+}$ zig-zag chains

Here we present YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$, two new compounds exhibiting slightly distorted vanadium-based kagome nets interleaved with zig-zag chains of divalent Yb$^{2+}$ and Eu$^{2+}$ ions. Single crystal growth methods are reported alongside magnetic, electronic, and thermodynamic measurements. YbV$_3$Sb$_4$ is a nonmagnetic metal with no collective phase transitions observed between 60mK and 300K. Conversely, EuV$_3$Sb$_4$ is a magnetic kagome metal exhibiting easy-plane ferromagnetic-like order below $T_\text{C}$=32K with signatures of noncollinearity under low field. Our discovery of YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$ demonstrate another direction for the discovery and development of vanadium-based kagome metals while incorporating the chemical and magnetic degrees of freedom offered by a rare-earth sublattice.

cond-mat.mtrl-sci↗

arXiv2023

Inhomogeneous high temperature melting and decoupling of charge density waves in spin-triplet superconductor UTe2

Periodic spatial modulations of the superfluid density, or pair density waves, have now been widely detected in unconventional superconductors, either as the primary or the secondary states accompanying charge density waves. Understanding how these density waves emerge, or conversely get suppressed by external parameters, provides an important insight into their nature. Here we use spectroscopic imaging scanning tunneling microscopy to study the evolution of density waves in the heavy fermion spin-triplet superconductor UTe2 as a function of temperature and magnetic field. We discover that charge modulations, composed of three different wave vectors gradually weaken but persist to a surprisingly high temperature T_CDW ~ 10-12 K. By tracking the local amplitude of modulations, we find that these modulations become spatially inhomogeneous, and form patches that shrink in size with higher temperature or with applied magnetic field. Interestingly, one of the density wave vectors along the mirror symmetry has a slightly different temperature onset, thus revealing an unexpected decoupling of the three-component CDW state. Importantly, T_CDW determined from our work matches closely to the temperature scale believed to be related to magnetic fluctuations, providing the first possible connection between density waves observed by surface probes and bulk measurements. Combined with magnetic field sensitivity of the modulations, this could point towards an important role of spin fluctuations or short-range magnetic order in the formation of the primary charge density wave.

cond-mat.supr-con↗

arXiv2023

Unidirectional coherent quasiparticles in the high-temperature rotational symmetry broken phase of AV3Sb5 kagome superconductors

Kagome metals AV3Sb5 (where the A can stand for K, Cs, or Rb) display a rich phase diagram of correlated electron states, including superconductivity and density waves. Within this landscape, recent experiments revealed signs of a transition below approximately 35 K attributed to an electronic nematic phase that spontaneously breaks rotational symmetry of the lattice. Here, we show that rotational symmetry breaking initiates universally at a high temperature in these materials, toward the 2 x 2 charge density wave transition temperature. We do this via spectroscopic-imaging scanning tunneling microscopy and study atomic-scale signatures of electronic symmetry breaking across several materials in the AV3Sb5 family: CsV3Sb5, KV3Sb5 and Sn-doped CsV3Sb5. Below a significantly lower temperature of about 30 K, we measure quantum interference of quasiparticles, a key signature for the formation of a coherent electronic state. These quasiparticles display a pronounced unidirectional feature in reciprocal space that strengthens as the superconducting state is approached. Our experiments reveal that high-temperature rotation symmetry breaking and the charge ordering states are separated from the superconducting ground state by an intermediate-temperature regime with coherent unidirectional quasiparticles. This picture is phenomenologically different compared to that in high-temperature superconductors, shedding light on the complex nature of rotation symmetry breaking in AV3Sb5 kagome superconductors.

cond-mat.str-el↗

arXiv2023

Electronic nematicity without charge density waves in titanium-based kagome metal

Layered crystalline materials that consist of transition metal atoms on a kagome network have emerged as a versatile platform to study unusual electronic phenomena. For example, in the vanadium-based kagome superconductors AV3Sb5 (where A can stand for K, Cs, or Rb) there is a parent charge density wave phase that appears to simultaneously break both the translational and the rotational symmetry of the lattice. Here, we show a contrasting situation where electronic nematic order - the breaking of rotational symmetry without the breaking of translational symmetry - can occur without a corresponding charge density wave. We use spectroscopic-imaging scanning tunneling microscopy to study the kagome metal CsTi3Bi5 that is isostructural to AV3Sb5 but with a titanium atom kagome network. CsTi3Bi5 does not exhibit any detectable charge density wave state, but comparison to density functional theory calculations reveals substantial electronic correlation effects at low energies. Comparing the amplitudes of scattering wave vectors along different directions, we discover an electronic anisotropy that breaks the six-fold symmetry of the lattice, arising from both in-plane and out-of-plane titanium-derived d orbitals. Our work uncovers the role of electronic orbitals in CsTi3Bi5, suggestive of a hexagonal analogue of the nematic bond order in Fe-based superconductors.

cond-mat.str-el↗

arXiv2023

Nanoscale visualization of the thermally-driven evolution of antiferromagnetic domains in FeTe thin films

Antiferromagnetic order, being a ground state of a number of exotic quantum materials, is of immense interest both from the fundamental physics perspective and for driving potential technological applications. For a complete understanding of antiferromagnetism in materials, nanoscale visualization of antiferromagnetic domains, domain walls and their robustness to external perturbations is highly desirable. Here, we synthesize antiferromagnetic FeTe thin films using molecular beam epitaxy. We visualize local antiferromagnetic ordering and domain formation using spin-polarized scanning tunneling microscopy. From the atomically-resolved scanning tunneling microscopy topographs, we calculate local structural distortions to find a high correlation with the distribution of the antiferromagnetic order. This is consistent with the monoclinic structure in the antiferromagnetic state. Interestingly, we observe a substantial domain wall change by small temperature variations, unexpected for the low temperature changes used compared to the much higher antiferromagnetic ordering temperature of FeTe. This is in contrast to electronic nematic domains in the cousin FeSe multilayer films, where we find no electronic or structural change within the same temperature range. Our experiments provide the first atomic-scale imaging of perturbation-driven magnetic domain evolution simultaneous with the ensuing structural response of the system. The results reveal surprising thermally-driven modulations of antiferromagnetic domains in FeTe thin films well below the Neel temperature.

cond-mat.str-el↗