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Steven J. Gomez Alvarado

Publications and source records attributed to Steven J. Gomez Alvarado.

12 recordsLinked to original sources

Dynamical many-body control of high harmonic generation in a Mott insulator

High harmonic generation (HHG) has emerged as a powerful probe of ultrafast electron dynamics in solids. However, in strongly correlated materials, where electronic excitations arise from many-body interactions rather than single-particle band dispersion, the field remains in its infancy. Here, we report HHG up to the 23$^{rd}$ order in the prototypical Mott insulator La$_2$CuO$_4$. We observe a robust 4 eV cutoff that is independent of driving field strength, revealing an intrinsic energy scale defined by the Hubbard bands. Using time-resolved high harmonic spectroscopy, we disentangle the distinct contributions of carrier creation, intraband acceleration, and interband recombination to the nonequilibrium radiation spectrum. We demonstrate that photo-doping triggers a fundamental reorganization of the many-body manifolds above a critical excitation density, a process that renormalizes the band curvature and suppresses nonlinear intraband currents, thereby directly imprinting the signature of many-body band reconstruction onto the harmonic emission. These results establish HHG as a sensitive probe of subtle correlation-driven electronic reconstructions and highlight that many-body interactions enable extreme nonlinear optical responses that are highly tunable in nonequilibrium states.

cond-mat.str-el↗

Crystal electric field excitations and an effective-spin-$1/2$ ground doublet in the hyperkagome magnet Yb$_3$Sc$_2$Ga$_3$O$_{12}$

We use inelastic neutron scattering (INS) to determine the crystal electric field (CEF) excitations of Yb$^{3+}$ in the rare-earth hyperkagome magnet Yb$_3$Sc$_2$Ga$_3$O$_{12}$. Three nearly dispersionless magnetic excitations are observed near 58, 68, and 74~meV, corresponding to transitions from the ground-state Kramers doublet to the three excited doublets of the $J=7/2$ multiplet. A Stevens-operator analysis constrained by the local $222$ ($D_2$) symmetry reproduces the excitation energies and spectral weights and yields an Ising-type ground-state $g$ tensor. The first excited doublet lies approximately 58~meV above the ground state, establishing a well-isolated effective $J_{\mathrm{eff}}=1/2$ degree of freedom over the low-temperature regime relevant to collective magnetism. Notably, the directly measured CEF spectrum substantially revises the level scheme previously inferred from bulk measurements, while preserving the essential low-energy pseudospin description. Two independent fitting protocols give consistent excitation energies, ground-doublet wave functions, and $g$ tensors, despite the nonuniqueness of the individual CEF parameters. The resulting single-ion model also reproduces the characteristic susceptibility, magnetization, and field evolution of the Schottky anomaly in specific heat. These results establish the microscopic single-ion basis needed to construct an effective exchange Hamiltonian and to interpret future measurements of low-energy collective excitations in Yb$_3$Sc$_2$Ga$_3$O$_{12}$.

cond-mat.str-el↗

Evidence for itinerant electron-local moment interaction in Li-doped $α$-MnTe

We use inelastic neutron scattering (INS) and angle-resolved photoemission spectroscopy (ARPES) to study the impact of Li doping on the semiconducting altermagnet $α$-MnTe. Introducing Li results in a spin reorientation from in-plane to out-of-plane direction and increases the density of itinerant carriers. While our ARPES measurements do not indicate any notable doping-induced changes in the electronic band structure or the magnitude of the altermagnetic band splitting, our INS measurements reveal an abrupt carrier-induced decrease in the spin wave lifetime near the zone boundary at high energies. This finding is consistent with a new magnon decay channel driven by doping-induced subtle changes in the band structure and enhanced interactions between Mn$^{2+}$ local moments and itinerant electrons. By extracting the local dynamic susceptibility from INS spectra and applying the total moment sum rule, we find that both undoped and Li-doped $α$-MnTe exhibit the full expected Mn$^{2+}$ local moment of $\approx5.9~μ_\mathrm{B}$ with $S=5/2$. These findings suggest that $α$-MnTe hosts robust local-moment altermagnetism which shows a breakdown at high energies upon addition of itinerant carriers, highlighting the importance of carrier-spin coupling in magneto-transport and spin dynamic properties of altermagnets even in the dilute-carrier limit.

cond-mat.str-el↗

Interplay between charge correlations and superconductivity across the superconducting domes of CsV$_{3}$Sb$_{5-x}$Sn$_x$

The kagome metal CsV$_3$Sb$_5$ shows an unconventional interplay between charge density wave (CDW) order and superconductivity. Tuning the band filling is known to rapidly suppress long-range CDW order and drive the formation of two superconducting ``domes" upon increasing hole concentration. Here we determine the detailed evolution of charge correlations across this phase diagram and resolve their interplay with the superconducting state. Upon light hole-doping, the suppression of a metastable $2\times 2\times 4$ CDW state coincides with the suppression of superconducting fluctuations present in the parent CsV$_3$Sb$_5$ compound. Continued doping suppresses long-range $2\times 2\times 2$ CDW order, leaving remnant short-range, quasi-1D correlations that persist across the second superconducting dome. These higher temperature charge correlations are seemingly essential to the lower temperature superconducting state, as charge correlations vanish coincident with superconductivity as a function of hole-doping. A multidomain model of short-range V-V dimer formation within the kagome plane is proposed in the second superconducting dome, where rotational and translational symmetry remain locally broken even in the absence of long-range CDW order.

cond-mat.supr-con↗

Magnetic dilution in the triangular lattice antiferromagnet NaYb$_{1-x}$Lu$_{x}$O$_2$

The delafossite-like compound NaYbO$_2$ hosts a triangular lattice of Yb$^{3+}$ moments and is a promising candidate for the realization of a quantum spin liquid ground state -- an exotic, quantum-disordered magnetic phase featuring long-range entanglement of spins. Tuning this system away from this quantum-disordered regime toward classical order or spin freezing is a powerful approach to shed light on the nature of the parent ground state. Here we leverage the substitution of nonmagnetic Lu$^{3+}$ onto the Yb$^{3+}$ sites to study the effects of magnetic disorder in NaYbO$_2$ using low-temperature ac susceptibility, heat capacity, and muon spin relaxation ($μ$SR) measurements. Our $μ$SR measurements reveal resilient, correlated magnetic fluctuations that persist to at least 15\% dilution, precluding conventional spin freezing and magnetic inhomogeneity. Heat capacity and magnetic susceptibility resolve a rapid suppression of the field-induced ``up-up-down'' magnetic order upon dilution and a crossover in the power-law behavior of the low-temperature magnetic excitations associated with the zero-field quantum disordered ground state. Taken together, these results support the notion of a robust network of entangled moments in NaYbO$_2$, and provides experimental validation of several models of a Heisenberg triangular lattice antiferromagnet in the presence of disorder.

cond-mat.str-el↗

Hidden frustration in the triangular-lattice antiferromagnet NdCd3P3

We report a study of the magnetic ground state and crystal electric field (CEF) scheme in the triangular-lattice antiferromagnet NdCd$_3$P$_3$. Combined neutron scattering, magnetization, and heat capacity measurements demonstrate that the Nd$^{3+}$ moments occupying the triangular lattice in this material harbor hidden signs of frustration not detected in typical Curie-Weiss-based parameterization of the frustration index ($f=Θ_{CW} / T_N$). This is evidenced by a zero-field splitting of the Kramers' ground state and first excited state doublets at temperatures far in excess of $T_N$ as well as signatures of low-energy fluctuations for $T>>T_N$. A suppression of the zero-field ordered moment relative to its field saturation value is observed, and the impacts of this magnetic frustration as well as the coexisting bond frustration in the CdP honeycomb network on the physical properties of NdCd$_3$P$_3$ are discussed.

cond-mat.str-el↗

Evolution of charge correlations in the hole-doped kagome superconductor CsV$_{3-x}$Ti$_x$Sb$_5$

The interplay between superconductivity and charge correlations in the kagome metal CsV$_3$Sb$_5$ can be tuned by external perturbations such as doping or pressure. Here we present a study of charge correlations and superconductivity upon hole doping via Ti substitution on the V kagome sites in CsV$_{3-x}$Ti$_x$Sb$_5$ via synchrotron x-ray diffraction and scanning SQUID measurements. While the superconducting phase, as viewed via the vortex structure, remains conventional and unchanged across the phase diagram, the nature of charge correlations evolves as a function of hole-doping from the first superconducting dome into the second superconducting dome. For Ti doping in the first superconducting dome, competing $2\times 2 \times 2$ and $2\times 2 \times 4$ supercells form within the charge density wave state and are suppressed rapidly with carrier substitution. In the second superconducting dome, no charge correlations are detected. Comparing these results to those observed for CsV$_3$Sb$_{5-x}$Sn$_x$ suggests important differences between hole doping via chemical substitution on the V and Sb sites, particularly in the disorder potential associated with each dopant.

cond-mat.supr-con↗

Stability frontiers in the AM$_6$X$_6$ kagome metals: The LnNb$_6$Sn$_6$ (Ln:Ce-Lu,Y) family and density-wave transition in LuNb$_6$Sn$_6$

The kagome motif is a versatile platform for condensed matter physics, hosting rich interactions between magnetic, electronic, and structural degrees of freedom. In recent years, the discovery of a charge density wave (CDW) in the AV$_3$Sb$_5$ superconductors and structurally-derived bond density waves in FeGe and ScV$_6$Sn$_6$ have stoked the search for new kagome platforms broadly exhibiting density wave (DW) transitions. In this work, we evaluate the known AM$_6$X$_6$ chemistries and construct a stability diagram that summarizes the structural relationships between the $\approx$125 member family. Subsequently we introduce our discovery of the broader LnNb$_6$Sn$_6$ (Ln:Ce-Nd,Sm,Gd-Tm,Lu,Y) family of kagome metals and an analogous DW transition in LuNb$_6$Sn$_6$. Our X-ray scattering measurements clearly indicate a (1/3, 1/3, 1/3) ordering wave vector ($\sqrt{3}\times\sqrt{3}\times3$ superlattice) and diffuse scattering on half-integer $L$-planes. Our analysis of the structural data supports the ``rattling mode'' DW model proposed for ScV$_6$Sn$_6$ and paints a detailed picture of the steric interactions between the rare-earth filler element and the host Nb-Sn kagome scaffolding. We also provide a broad survey of the magnetic properties within the HfFe$_6$Ge$_6$-type LnNb$_6$Sn$_6$ members, revealing a number of complex antiferromagnetic and metamagnetic transitions throughout the family. This work integrates our new LnNb$_6$Sn$_6$ series of compounds into the broader AM$_6$X$_6$ family, providing new material platforms and forging a new route forward at the frontier of kagome metal research.

cond-mat.str-el↗

Characterization of Chromium Impurities in $β$-Ga$_2$O$_3$

Chromium is a common transition-metal impurity that is easily incorporated during crystal growth. It is perhaps best known for giving rise to the 694.3 nm (1.786 eV) emission in Cr-doped Al$_2$O$_3$, exploited in ruby lasers. Chromium has also been found in monoclinic gallium oxide, a wide-bandgap semiconductor being pursued for power electronics. In this work, we thoroughly characterize the behavior of Cr in Ga$_2$O$_3$ through theoretical and experimental techniques. $β$-Ga$_2$O$_3$ samples are grown with the floating zone method and show evidence of a sharp photoluminescence signal, reminiscent of ruby. We calculate the energetics of formation of Cr from first principles, demonstrating that Cr preferentially incorporates as a neutral impurity on the octahedral site. Cr possesses a quartet ground-state spin and has an internal transition with a zero-phonon line near 1.8 eV. By comparing the calculated and experimentally measured luminescence lineshape function, we elucidate the role of coupling to phonons and uncover features beyond the Franck-Condon approximation. The combination of strong emission with a small Huang-Rhys factor of 0.05 and a technologically relevant host material render Cr in Ga$_2$O$_3$ attractive as a quantum defect.

cond-mat.mtrl-sci↗

Advances in high-pressure laser floating zone growth: the Laser Optical Kristallmacher II

The optical floating zone crystal growth technique is a well-established method for obtaining large, high-purity single crystals. While the floating zone method has been constantly evolving for over six decades, the development of high-pressure (up to 1000 bar) growth systems has only recently been realized via the combination of laser-based heating sources with an all-metal chamber. While our inaugural high-pressure laser floating zone furnace design demonstrated the successful growth of new volatile and metastable phases, the furnace design faces several limitations with imaging quality, heating profile control, and chamber cooling power. Here, we present a second-generation design of the high-pressure laser floating zone furnace, "Laser Optical Kristallmacher II" (LOKII), and demonstrate that this redesign facilitates new advances in crystal growth by highlighting several exemplar materials: $α$-Fe$_2$O$_3$, $β$-Ga$_2$O$_3$, and La$_2$CuO$_{4+δ}$. Notably, for La$_2$CuO$_{4+δ}$, we demonstrate the feasibility and long-term stability of traveling solvent floating zone growth under a record pressure of 700 bar.

physics.app-ph↗

Revisiting spin ice physics in the ferromagnetic Ising pyrochlore Pr$_2$Sn$_2$O$_7$

Pyrochlore materials are characterized by their hallmark network of corner-sharing rare-earth tetrahedra, which can produce a wide array of complex magnetic ground states. Ferromagnetic Ising pyrochlores often obey the "two-in-two-out" spin ice rules, which can lead to a highly-degenerate spin structure. Large moment systems, such as Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, tend to host a classical spin ice state with low-temperature spin freezing and emergent magnetic monopoles. Systems with smaller effective moments, such as Pr$^{3+}$-based pyrochlores, have been proposed as excellent candidates for hosting a "quantum spin ice" characterized by entanglement and a slew of exotic quasiparticle excitations. However, experimental evidence for a quantum spin ice state has remained elusive. Here, we show that the low-temperature magnetic properties of Pr$_2$Sn$_2$O$_7$ satisfy several important criteria for continued consideration as a quantum spin ice. We find that Pr$_2$Sn$_2$O$_7$ exhibits a partially spin-frozen ground state with a large volume fraction of dynamic magnetism. Our comprehensive bulk characterization and neutron scattering measurements enable us to map out the magnetic field-temperature phase diagram, producing results consistent with expectations for a ferromagnetic Ising pyrochlore. We identify key hallmarks of spin ice physics, and show that the application of small magnetic fields ($μ_0 H_c \sim$0.75T) suppresses the spin ice state and induces a long-range ordered magnetic structure. Together, our work clarifies the current state of Pr$_2$Sn$_2$O$_7$ and encourages future studies aimed at exploring the potential for a quantum spin ice ground state in this system.

cond-mat.str-el↗

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↗