arXiv subjects

Carl P. Romao

Publications and source records attributed to Carl P. Romao.

17 recordsLinked to original sources

arXiv2026

Intercalation of Alkali Metal into WTe2, the Crystal Structure of A0.5WTe2 and Observation of a Metal-to-Semiconductor Transition

We explore the cationic intercalation of tungsten ditelluride (WTe2) with potassium (K), rubidium (Rb), and cesium (Cs), yielding intercalation compounds of the form A0.5WTe2 (A = K, Rb, Cs). Structural characterization was performed using powder X-ray diffraction (PXRD), while diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy and temperature-dependent conductivity measurements were employed to investigate the electronic properties. Density functional theory (DFT) calculations were carried out to support the experimental findings and to provide insight into the intercalation mechanisms and the resulting material characteristics. All synthesized compounds display semiconducting behavior with narrow band gaps, emphasizing the influence of alkali metal intercalation on the electronic structure and transport properties of WTe2. These results advance the fundamental understanding of property modulation in transition-metal dichalcogenides (TMDCs) and highlight their potential for electronic device applications.

cond-mat.mtrl-sci↗

arXiv2026

Dynamical multiferroicity in framework materials

Dynamical multiferroicity, which describes the magnetic fields generated by circularly polarized phonons in materials, is an established mechanism for optical control of magnetism. Here we perform ab initio calculations of dynamical multiferroicity in inorganic and organic framework materials, with the goal of identifying materials which enable the generation of large magnetic fields by light. We find the metal--organic framework material Zn(NH$_4$)(formate)$_3$ to have modes with magnetic moments almost twice that of SrTiO$_3$; these modes involve circular motions of NH$_4^+$ hydrogen ions with high gyromagnetic ratios. The complex structure and flexibility of framework materials can allow such angular momentum localization, and also increase the maximum light-induced magnetization permitted by the Lindemann melting criterion.

cond-mat.mtrl-sci↗

arXiv2026

Zero Indirect Band Gap and Flat Bands in a Niobium Oxyiodide Cluster Material

Explorative chemistry in a reaction system composed of NbI$_4$, Li$_2$(CN$_2$), and Li$_2$O has led to the discovery of a number of niobium oxyiodide cluster compounds. During this reaction, the formation of solid phases was detected alongside with gaseous phases, resulting in a range of products with cluster cores of varying shapes. After several niobium oxyiodide cluster compounds have already been identified within this reaction system, two additional compounds, Nb$_6$O$_3$I$_{15}$ and Nb$_{11}$O$_6$I$_{24}$, are discovered and structurally characterized by single-crystal X-ray diffraction. Both structures are based on the butterfly-shaped, oxygen-capped niobium cluster [Nb$_4$O], which is extended to larger cluster fragments. The [Nb$_4$O] cluster core in Nb$_6$O$_3$I$_{15}$is extended by two [NbO] units to form a three-dimensional framework, and Nb$_{11}$O$_6$I$_{24}$ contains two connected [Nb$_4$O] units, which form chiral units within an antiferrochiral hexagonal packing of strings. The striking string-like character of Nb$_{11}$O$_6$I$_{24}$ was investigated in terms of its electronic structure and properties. DFT calculations showed Nb$_{11}$O$_6$I$_{24}$ to possess a zero indirect band gap, with a pair of 3-dimensional flat bands surrounding the Fermi level. These unusual features of the electronic band structure suggest the presence of strongly correlated inter-cluster singlet electron states, arising from the helical shape of the clusters, the hexagonal packing of the strings, and the delocalized nature of cluster electron wavefunctions.

cond-mat.str-el↗

arXiv2026

Lattice excitations with finite polarization and magnetization

Ferrons are a type of quasiparticle corresponding to elementary excitations of the ferroelectric order. Analogously to how magnons modulate and transport magnetization, ferrons modulate and transport electric polarization. Here, we introduce multiferrons as elementary excitations with both electric and magnetic character. Multiferrons lead to a tilt and elliptical precession of the polarization and at the same time create a magnetization through the mechanism of dynamical multiferroicity. Using first-principles calculations for LiNbO$_3$, we show that the electric polarization of multiferrons is perpendicular to the equilibrium ferroelectric polarization, whereas the magnetization is parallel to it. Our calculations further demonstrate that multiferrons carry net electric and magnetic quadrupole and octupole moments, which we term multipolons. These multipolons could couple to internal multipolar degrees of freedom, for example in altermagnets, or to external probes such as neutrons, leading to potentially experimentally observable phenomena following coherent or thermal excitation of multiferrons.

cond-mat.mtrl-sci↗

arXiv2026

Electric field switching of chiral phonons

Lattice vibrations carrying angular momentum, known as chiral phonons, have emerged as a promising route to control and understand complex material properties, yet their deterministic manipulation remains largely unexplored. Here we demonstrate electric-field switching of phonon angular momentum in the technologically relevant ferroelectric BaTiO3. Using circularly dichroic resonant inelastic X-ray scattering (CD-RIXS) at the oxygen K edge, we directly probe the phonon angular momentum and compare the measured dichroism with first-principles predictions of phonon-mode chirality. We find excellent agreement, revealing a momentum-dependent circular-dichroism contrast that exhibits a reversible gyroelectric effect, stable for at least 15 hours. Our results establish a robust mechanism for non-volatile control of chiral phonons and point towards new opportunities for phonon-based information and energy technologies.

cond-mat.mtrl-sci↗

arXiv2026

Structural Evolution during Reversible Halogen Intercalation into WTe2: Commensurate-Incommensurate WTe2I and Multistage WTe2Brx (x = 0.5, 1.0 and 1.25)

Halogen intercalation into the layered material tungsten ditelluride (WTe2) provides a unique pathway to tune its structural and electronic properties. In this study, we detail the synthesis and characterization of the new bromine-intercalated phases WTe2Brx (x = 0.5, 1.0, and 1.25), and reinvestigate the iodine-intercalated analogue, WTe2I. A defining feature of the bromine system is its rapid and reversible "breathing" behavior at room temperature, allowing guest molecules to be absorbed or released from the van der Waals gaps under ambient conditions. Structural analysis shows that the bromine-poor phase WTe2Br0.5 crystallizes in the orthorhombic space group Pmmn, thereby maintaining a uniform stacking sequence. In contrast, the bromine-rich WTe2Br1.25 phase (space group Imm2) adopts an architecture where two distinct types of bromine layers alternate between the host layers. For the iodine system, the compound WTe2I exhibits both incommensurate and commensurate (3+1)D modulated variants in the superspace group P21/m(α0γ)00. In the commensurate polytype, the structural modulation locks into a rational vector, q = (1/2, 0, 1/6), which can be described also as a 3D supercell. Electronic structure calculations show WTe2Br0.5 and commensurately modulated WTe2I to be metals with flat bands at the Fermi energy arising from the intercalation. These findings demonstrate the unusual stability and structural flexibility of anionic intercalation in a transition metal dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2026

Anomalous phonon magnetic moments

Circularly polarized phonons conventionally carry an angular momentum and a magnetic moment arising from circular motions of the atoms. Here, we present three anomalous cases that lead to phonon magnetic moments, which cannot be described in the conventional framework: rotationless axial phonons, which exhibit magnetic responses despite only carrying pseudo angular momentum, divergent gyromagnetic ratios of phonons, in which a magnetic moment is produced despite vanishing angular momentum, and anisotropic gyromagnetic ratios of phonons, which make the phonon angular momentum and magnetic moment noncollinear. Our results shed light on the origin and nature of phonon magnetism and suggest the existence of phononomagnetic hidden order.

cond-mat.mtrl-sci↗

arXiv2025

Chiral phonons in metal-organic frameworks as quantum sensors for the direct detection of dark matter

We investigate a new quantum sensor for dark matter direct detection with sub-eV sensitivity, focusing on several candidate materials that potentially host chiral phonons with large magnetic moments that can be directly read out with an external magnetometer. We focus on metal-organic frameworks (MOFs) as possible candidate materials for single chiral phonon detection due to their noncentrosymmetric structure, tunability, and the ability to host these excitations in stable acoustic bands. We identify several promising candidates and compare their projected dark matter detection sensitivity for all possible interactions identified within effective field theory. We establish that the expected sensitivity does not depend heavily on the specific choice of the MOF, enabling us to tailor the final material composition to facilitate the magnetic readout. We then propose a prototype setup able to test the direct readout of a chiral phonon sensor with a surface-integrated magnetometer.

hep-ph↗

arXiv2025

Hubbard dimer physics and the magnetostructural transition in the correlated cluster material Nb$_3$Cl$_8$

We present a combined computational and experimental study of Nb$_3$Cl$_8$, a correlated layered material containing Nb trimers, through the lens of competing intra- and intercluster interactions. Different proposed explanations for its magnetostructural transition such as charge disproportionation, antiferromagnetic quenching, and interlayer singlet formation are investigated in light of the various reported low-temperature structures. Our findings rule out the previously proposed charge-disproportionation, suggest an intricate interplay between Mott physics and the formation of interlayer singlets, and also hint at a possible explanation of the observed intratrimer scissoring distortion. We suggest that the physics of Nb$_3$Cl$_8$ should be understood in the context of weakly coupled Hubbard dimers.

cond-mat.str-el↗

arXiv2025

Tuning chirality amplitude at ultrafast timescales

Chirality is a fundamental symmetry concept describing discrete states, i.e., left-handed, right-handed, or achiral, and existing at disparate scales and in many categories of scientific fields. Even though symmetry breaking is indispensable for describing qualitatively distinct phenomena, symmetry cannot quantitatively predict measurable quantities. One can continuously distort an object, introducing the concept of chirality amplitude, similar to representing magnetization as the amplitude of time-reversal symmetry breaking. Considering the role of magnetization in emergent phenomena with time-reversal symmetry breaking, chirality amplitude is intuitively a key quantity for controlling chirality-related emergent phenomena. Here, we propose two types of chiral lattice distortions and demonstrate the tunability of their amplitude in ultrafast timescales. Resonant X-ray diffraction with circular polarization is an established technique to measure crystal chirality directly. We quantify the ultrafast change in chirality amplitude in real time after an optical excitation. Using instead a THz excitation, we observe oscillations in the resonant diffraction intensities corresponding to specific phonon frequencies. This indicates the creation of additional asymmetry, which could also be described as an enhancement in chirality amplitude. Our proposed concept of chirality amplitude and its ultrafast control may lead to a unique approach to control chirality-induced emergent phenomena in ultrafast timescales.

cond-mat.str-el↗

arXiv2025

Chiral phonons in polar LiNbO3

Quasiparticles describe collective excitations in many-body systems, and their symmetry classification is of fundamental importance because they govern physical processes on various timescales, e.g., excited states, transport phenomena, and phase transitions. Recent studies have revealed that quasiparticles can possess chirality and that this degree of freedom leads to various important phenomena. Among them, chiral phonons have recently attracted significant interest because of their intrinsic magnetism, which non-trivially bridges the spin system and the lattice. Here, we directly prove the presence of chiral phonons in a prototypical polar crystal LiNbO3. Our demonstration adds a polar crystal in the showcase of materials hosting chiral phonons and, furthermore, creates a substantial potential in chiral phononics because of its expected in-situ switchable phonon chirality and associated control of phonon angular momentum.

cond-mat.str-el↗

arXiv2024

Phonon-induced geometric chirality

Chiral properties have seen increasing use in recent years, leading to the emerging fields of chiral quantum optics, plasmonics, and phononics. While these fields have achieved manipulation of the chirality of light and lattice vibrations, controlling the chirality of materials on demand has yet remained elusive. Here, we demonstrate that linearly polarized phonons can be used to induce geometric chirality in achiral crystals when excited with an ultrashort laser pulse. We show that nonlinear phonon coupling quasistatically displaces the crystal structure along phonon modes that reduce the symmetry of the lattice to that of a chiral point group corresponding to a chiral crystal. By reorienting the polarization of the laser pulse, the two enantiomers can be induced selectively. Therefore, geometric chiral phonons enable the light-induced creation of chiral crystal structures and offer a pathway to engineering chiral electronic states and optical properties.

cond-mat.mtrl-sci↗

arXiv2024

Electronic Structure and Transport in the Potential Luttinger Liquids CsNb$_3$Br$_7$S and RbNb$_3$Br$_7$S

The crystal structures of ANb$_3$Br$_7$S (A = Rb and Cs) have been refined by single crystal X-ray diffraction, and are found to form highly anisotropic materials based on chains of the triangular Nb$_3$ cluster core. The Nb$_3$ cluster core contains seven valence electrons, six of them being assigned to Nb-Nb bonds within the Nb$_3$ triangle and one unpaired d electron. The presence of this surplus electron gives rise to the formation of correlated electronic states. The connectivity in the structures is represented by one-dimensional [Nb$_3$Br$_7$S]$^-$ chains, containing a sulphur atom capping one face ($μ_3$) of the triangular niobium cluster, which is believed to induce an important electronic feature. Several types of studies are undertaken to obtain deeper insight into the understanding of this unusual type of material: the crystal structure, morphology and elastic properties are analysed, as well the (photo-) electrical properties and NMR relaxation. Electronic structure (DFT) calculations are performed in order to understand the electronic structure and transport in these compounds, and, based on the experimental and theoretical results, we propose that the electronic interactions along the Nb chains are sufficiently one-dimensional to give rise to Luttinger liquid (rather than Fermi liquid) behaviour of the metallic electrons.

cond-mat.str-el↗

arXiv2023

Chiral phonons as dark matter detectors

We propose a method for detecting single chiral phonons that will enable their use as dark-matter detectors. We suggest metal--organic frameworks (MOFs) as detector materials, as their flexibility yields low-energy chiral phonons with measurable magnetic moments, and their anisotropy leads to directional sensitivity, which mitigates background contamination. To demonstrate our proposal, we calculate the phononic structure of the MOF InF$_3$($4,4'$-bipyridine), and show that it has highly chiral acoustic phonons. Detection of such chiral phonons via their magnetic moments would dramatically lower the excitation energy threshold for dark matter detection to the energy of a single phonon. We show that single phonon detection in a MOF would extend detector reach ten or more orders of magnitude below current limits, enabling exploration of a multitude of as-yet-unprobed dark matter candidates.

hep-ph↗

arXiv2023

Chiral phonons probed by X rays

The concept of chirality is of great relevance in nature, from chiral molecules such as sugar to parity transformations in particle physics. In condensed matter physics, recent studies have demonstrated chiral fermions and their relevance in emergent phenomena closely related to topology. The experimental verification of chiral phonons (bosons) remains challenging, however, despite their expected strong impact on fundamental physical properties. Here we show experimental proof of chiral phonons using resonant inelastic X-ray scattering with circularly polarized X rays. Using the prototypical chiral material, quartz, we demonstrate that circularly polarized X rays, which are intrinsically chiral, couple to chiral phonons at specific positions in reciprocal space, allowing us to determine the chiral dispersion of the lattice modes. Our experimental proof of chiral phonons demonstrates a new degree of freedom in condensed matter that is both of fundamental importance and opens the door to exploration of novel emergent phenomena based on chiral bosons

cond-mat.str-el↗

arXiv2019

Anomalous thermal expansion and chiral phonons in BiB$_{3}$O$_{6}$

The origins of anomalous thermal expansion in the chiral monoclinic solid $α$-BiB$_{3}$O$_{6}$ have been studied through ab initio calculations. Positive and negative axial thermal expansion are shown to be driven by librations of borate units, elastic anisotropy, and most notably by chiral acoustic phonons involving elliptical revolutions of bismuth atoms. The chirality of the lattice gives rise to these modes by allowing the transverse acoustic branches to have opposite circular polarizations, only one of which couples strongly to the lattice strains. These results further understanding of relationships between crystallographic symmetry and physical properties.

cond-mat.mtrl-sci↗

arXiv2017

Origins of anisotropic thermal expansion in flexible materials

A definition of the Grüneisen parameters for anisotropic materials is derived based on the response of phonon frequencies to uniaxial stress perturbations. This Grüneisen model relates the thermal expansion in a given direction ($α_{ii}$) to one element of the elastic compliance tensor, which corresponds to the Young's modulus in that direction ($Y_{ii}$). The model is tested through ab initio prediction of thermal expansion in zinc, graphite, and calcite using density functional perturbation theory, indicating that it could lead to increased accuracy for structurally complex systems. The direct dependence of $α_{ii}$ on $Y_{ii}$ suggests that materials which are flexible along their principal axes but rigid in other directions will generally display both positive and negative thermal expansion.

cond-mat.mtrl-sci↗