arXiv subjects

Nathan Giles-Donovan

Publications and source records attributed to Nathan Giles-Donovan.

6 recordsLinked to original sources

arXiv2026

Twinning of domains and spin anisotropy in K$_5$Fe$_4$Ag$_6$Te$_{10}$

The Fe-based superconductors are derived from metallic parent compounds with nematic and stripe magnetic orders, which lead to two types of magnetic domains. Recently it was found that K$_5$Fe$_4$Ag$_6$Te$_{10}$ (KFAT), an Fe-based semiconductor, exhibits similar nematic and stripe magnetic orders, and is thus an analogue to the Fe-based superconductors in the limit of localized electrons. In this work, the superstructure and magnetic domains of KFAT are elucidated by fully mapping the reciprocal space using time-of-flight single crystal neutron diffraction. In KFAT, Fe and Ag atoms order to form a $\sqrt{5}\times\sqrt{5}$ superstructure containing $2\times2$ Fe blocks, which leads to two superstructure domains with identical main Bragg peaks but distinct superstructure peaks. Below $T_{\rm N}\approx35$~K, magnetic and nematic orders break in-plane rotational symmetry of the tetragonal $\sqrt{5}\times\sqrt{5}$ superstructure, and further give rise to two magnetic domains. These four equally populated domains account for the complex scattering pattern observed in our time-of-flight elastic neutron scattering measurements. Using polarized neutron scattering, we demonstrate a prominent spin anisotropy with an easy-plane spanned by the $c$-axis and the intra-block antiferromagnetic Fe-Fe bond direction. Such an anisotropy at ${\bf q}\neq0$ persists well above $T_{\rm N}$, accounts for the in-plane ${\bf q}=0$ magnetic anisotropy observed in uniaxial-strained KFAT, and offers an indicator for discovering similar piezomagnetic effects in other materials.

cond-mat.str-el↗

arXiv2026

Selective coupling of high-order phonons in La2-xSrxCuO4

In crystals and molecules with strong coupling between the charge carriers and atomic vibrations, high order harmonics of the vibrational excitations can be observed with intensity following the Franck-Condon envelope. Here, we uncover a new regime of electron-phonon coupling in La2-xSrxCuO4 using resonant inelastic X-ray scattering. In the undoped compound, we find sharp peaks at approximately 85$\pm$5 meV, 180$\pm$7 meV, and 330$\pm$5 meV with no observable dispersion, and an absence of appreciable intensity from other modes observed in Raman spectroscopy in this energy range. The 180 meV and 330 meV excitations have energies approximately consistent with two-phonon and four-phonon in-plane Cu-O bond stretching mode, suggesting that the resonantly excited valence electrons strongly couple to this mode. These excitations exhibit significant doping dependence, eventually becoming unresolvable at 10% hole doping, where the low energy charge excitations are dominated by dispersive plasmons. The observation of selective coupling to even-ordered phonons and stark contrast with the Raman spectra indicate anomalous electron-phonon coupling beyond the Franck-Condon picture. One intriguing possibility is the existence of locally paired quasiparticles in insulating cuprates.

cond-mat.str-el↗

arXiv2026

Spectroscopic evidence for a molecular orbital Kondo insulator

A Kondo insulator (KI) is a prototypical example of a highly entangled phase of matter, where many-body interactions between local moments and delocalized electrons engender the non-magnetic insulating ground state. Conventionally, the local moments arise from atomic multiplet states with a narrow bandwidth, limiting Kondo coherence to low temperatures. Here, we realize a new paradigm for constructing the KI state with hybridized molecular orbitals in FeSb2. Resonant inelastic X-ray scattering (RIXS) at the Fe L-edge reveals distinct signatures of band-like continuum states and localized states. Comparisons with first-principles calculations establish a mixed-configuration ground state with hybridized Fe d-Sb p molecular orbitals as basis states. By systematically investigating the RIXS momentum, temperature, and doping dependences, we find propagating collective modes commensurate with many-body charge and spin excitations. Our results pave the way for understanding the emerging class of unconventional d electron insulators and engineering high temperature Kondo many-body states.

cond-mat.str-el↗

arXiv2026

Strongly-coupled hybrid lattice-plasmons in layered cuprates

Metallic systems with delocalized valence electrons host collective charge density oscillations known as plasmons. On the other hand, conventional insulators do not have free electrons and the low energy charge degrees of freedom are pinned to the ions. The fate of the collective charge excitations in the intermediate regime is an outstanding question. This problem is especially important for strongly correlated systems such as the layered cuprates, where unconventional superconductivity and other emergent phenomena arise from valence electrons on the border between Mott localization and itinerancy. Using resonant inelastic X-ray scattering, we track this evolution in the prototypical electron-doped cuprate Nd2-xCexCuO4. We find a continuous transformation of the low-energy charge response: from an acoustic plasmon in the metallic regime, to a gapped hybrid mode at intermediate doping, and finally to a nearly dispersionless 139 meV excitation at half filling. Remarkably, the 139 meV excitation has approximately twice the energy of the oxygen breathing phonon responsible for the dispersion kink observed in angle-resolved photoemission spectroscopy, and is consistent with a putative 2-phonon excitation observed in Raman spectroscopy. These results establish a unified picture of collective charge excitations across the phase diagram of electron-doped cuprates, showing that such modes persist across the Mott transition via strong coupling to lattice degrees of freedom and revealing a missing link in the charge dynamics of carrier doped Mott insulators.

cond-mat.str-el↗

arXiv2024

Spontaneously formed phonon frequency combs in van der Waals solid CrXTe$_3$ (X=Ge,Si)

Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. In this study, we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe$_3$ (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest $A_g$ mode in CrGeTe$_3$ splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 100K before decaying. These modes correspond to localized oscillations of Ge$_2$Te$_6$ clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe$_3$, demonstrating the generalizability of this phenomenon. Our findings reveal that Raman scattering effectively probes high-frequency nonlinear phonon modes, providing new insight into generating long-lived, tunable phonon frequency combs with applications in ultrafast material control and phonon-based technologies.

cond-mat.mes-hall↗

arXiv2024

Charge Density Fluctuations with Enhanced Superconductivity at the Proposed Nematic Quantum Critical Point

A quantum critical point (QCP) represents a continuous phase transition at absolute zero. At the QCP of an unconventional superconductor, enhanced superconducting transition temperature and magnetic fluctuations strength are often observed together, indicating magnetism-mediated superconductivity. This raises the question of whether quantum fluctuations in other degrees of freedom, such as charge, could similarly boost superconductivity. However, because charge is frequently intertwined with magnetism, isolating and understanding its specific role in Cooper pair formation poses a significant challenge. Here, we report persistent charge density fluctuations (CDF) down to 15 K in the non-magnetic superconductor Sr$_{0.77}$Ba$_{0.23}$Ni$_{2}$As$_{2}$, which lies near a proposed nematic QCP associated with a six-fold enhancement of superconductivity. Our results show that the quasi-elastic CDF does not condense into resolution-limited Bragg peaks and displays non-saturated strength. The CDF completely softens at 25 K, with its critical behavior described by the same mathematical framework as the antiferromagnetic Fermi liquid model, yielding a fitted Curie-Weiss temperature of $θ\approx 0$ K. Additionally, we find that the nematic fluctuations are not lattice-driven, as evidenced by the absence of softening in nematic-coupled in-plane transverse acoustic phonons. Our discovery positions Sr$_{x}$Ba$_{1-x}$Ni$_{2}$As$_{2}$ as a promising candidate for charge-fluctuation-driven nematicity and superconductivity.

cond-mat.supr-con↗