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Alaska Subedi

Publications and source records attributed to Alaska Subedi.

At least 19 recordsLinked to original sources
arXiv2026

Hydrodynamics of the viscous electron fluid in cadmium

Thanks to electron-electron ($e$-$e$) collisions conserving momentum, metallic electron fluids are viscous. Yet, this viscosity is rarely detectable in bulk transport. Here, we report on the canonical realization of the Gurzhi effect in an elemental three-dimensional metal: cadmium. Using focused ion beam microstructuring to tune the effective thickness, we detected a low-temperature size-dependent resistivity upturn in a finite window sandwiched between ballistic and diffusive regimes. Within this window, the electrical conductivity displays a simultaneous quadratic dependence on both sample size and temperature -- fingerprint of a hydrodynamic flow. This leads us to quantify the amplitude and the temperature dependence of kinematic and dynamic viscosity of the electron fluid. In cadmium, in contrast with graphene and $^3$He, the rate of momentum-conserving $e$-$e$ collisions is not set by the main Fermi energy, but by Lilliputian energy scales and inter-valley bottlenecks.

cond-mat.str-el↗
arXiv2026

Interaction driven transverse thermal resistivity in a phonon gas

The amplitude of the Hall response of electrons can be understood without invoking interactions. Most theories of the phonon thermal Hall effect have likewise opted for a non-interacting picture. Here, we challenge this approach. Our study of WS$_2$, a transition metal dichalcogenide (TMD) insulator, finds that longitudinal, $\kappa_{xx}$, and transverse, $\kappa_{xy}$, thermal conductivities peak at almost the same temperature. Their ratio obeys an upper bound, as in other insulators. We then compare transverse thermal transport in a phonon gas and in a molecular gas. In the latter, the Senftleben-Beenakker effect is driven by the competition between molecular collisions and applied magnetic field in setting the distribution of molecular angular momenta. An off-diagonal transport response arises thanks to interactions between non-spherical particles, which do not need to be chiral. By analogy, we argue that in a phonon gas, magnetic field will influence phonon-phonon interactions, and generates a transverse thermal \emph{resistivity}, whose order of magnitude can be accounted for by invoking a Berry force on the drift velocity of the nuclei in the presence of a finite heat. This simple picture gives a reasonable account of the experimentally measured transverse thermal resistivity of seven different crystalline insulators.

cond-mat.mtrl-sci↗
arXiv2025

Octahedral rotation instability in Ba$_2$IrO$_4$

Ba$_2$IrO$_4$ has been refined in the tetragonal $I4/mmm$ phase without octahedral rotations, and its physical properties have been interpreted in this high-symmetry structure. However, the dynamical stability of this undistorted phase has not previously been questioned. It is important to establish whether other lower-symmetry structures are energetically more favorable because octahedral rotations control electronic bandwidths and constrain which magnetic interactions are allowed by symmetry. Here I compute first-principles phonon dispersions of $I4/mmm$ Ba$_2$IrO$_4$ including spin-orbit interaction. I find a nearly-flat nondegenerate unstable branch along the Brillouin-zone boundary segment $XP$ associated with inplane rotations of the IrO$_6$ octahedra. Using group-theoretical analysis, I enumerate the symmetry-allowed distortions associated with the $X_2^+$ and $P_4$ instabilities and fully relax the resulting structures. Only five of the twelve possible distortions can be stabilized, and the energy gain scales with the number of layers that exhibit octahedral rotations: phases with rotations in every IrO$_6$ layer are lower by $-5.8$ meV/atom and are nearly degenerate with respect to the stacking phase. Electronic structure calculations show that these rotated phases host a narrow and well-separated half-filled $J_{\textrm{eff}} = 1/2$ manifold, whereas structures with rotations only in alternate layers have broader and more entangled bands. This motivates a reinvestigation of the crystal structure of Ba$_2$IrO$_4$ and indicates that octahedral rotations should be considered in modeling its correlated electronic and magnetic properties.

cond-mat.mtrl-sci↗
arXiv2024

Pressure-tunable structural instabilities in single-layer-trilayer La$_3$Ni$_2$O$_7$

Layered nickelates are believed to exhibit superconductivity similar to that found in the cuprates. However, the precise crystal structure of the superconducting phase of the layered nickelates has not been fully clarified. Here, I use first principles calculations to study the pressure dependence of the structural instabilities in the single-layer-trilayer La$_3$Ni$_2$O$_7$, which is one member of the layered nickelates family that also shows signatures of superconductivity. I find a nearly dispersionless nondegenerate phonon branch in the parent $P4/mmm$ phase that is unstable along the Brillouin zone edge $M$ $(\frac{1}{2}, \frac{1}{2}, 0)$ $\rightarrow$ $A$ $(\frac{1}{2},\frac{1}{2},\frac{1}{2})$ at all investigated pressures up to 30 GPa. Calculations show additional doubly-degenerate instabilities along the edge $MA$ at lower pressures. I used group-theoretical analysis to identify the distinct low-symmetry distortions possible due to these instabilities and generated them using the eigenvectors of the unstable modes. Structural relaxations show that the lowest energy structures at 0 and 10 GPa involve condensation of both the nondegenerate and doubly-degenerate instabilities, which is in contrast to the experimental refinements that involve condensation of only the doubly-degenerate branch. I also find that structural distortions are energetically favorable at 20 GPa, contrary to the experiments that do not observe any distortions of the parent $P4/mmm$ structure at high pressures.

cond-mat.supr-con↗
arXiv2024

Deep-lying semi-Dirac fermions in hexagonal close-packed cadmium

Semi-Dirac fermions are massless in one direction and massive in the perpendicular directions. Such quasiparticles have been proposed in various contexts in condensed matter. Using first principles calculations, we identify a pair of semi-Dirac bands anti-crossing at $-3$ eV below the Fermi level in the electronic structure of hexagonal close-packed cadmium. The linear out-of-plane dispersion is kept up to the Fermi level. We demonstrate that the dichotomy between the linear and quadratic dispersions is driven by an orientation-sensitive hybridization between the $s$ and $p_z$ orbitals. The upper semi-Dirac band produces a lens-shaped nonellipsoidal Fermi sheet whose cross-section area has a $k$-dependence that is in excellent agreement with the experimentally measured period of Sondheimer oscillations.

cond-mat.mtrl-sci↗
arXiv2024

Impact of hole-doping on the thermoelectric properties of pyrite FeS2

We present a comprehensive first-principles analysis of the thermoelectric transport properties of hole-doped pyrite FeS$_2$ that includes electron-phonon interactions. This work was motivated by the observed variations in the magnitude of thermopower reported in previous experimental and theoretical studies of hole-doped FeS$_2$ systems. Our calculations reveal that hole-doped FeS$_2$ exhibits large positive room-temperature thermopower across all doping levels, with a room-temperature thermopower of 608 $\mu$V/K at a low hole-doping concentration of 10$^{19}$ cm$^{-3}$. This promising thermopower finding prompted a comprehensive investigation of other key thermoelectric parameters governing the thermoelectric figure of merit $ZT$. The calculated electrical conductivity is modest and remains below 10$^5$ S/m at room-temperature for all doping levels, limiting the achievable power factor. Furthermore, the thermal conductivity is found to be phonon driven, with a high room-temperature lattice thermal conductivity of 40.5 W/mK. Consequently, the calculated $ZT$ remains below 0.1, suggesting that hole-doped FeS$_2$ may not a viable candidate for effective thermoelectric applications despite its promising thermopower.

cond-mat.mtrl-sci↗
arXiv2024

Phonon hydrodynamic regimes in sapphire

When an ideal insulator is cooled, four regimes of thermal conductivity are expected to emerge one after another. Two of these, the Ziman and the Poiseuille, are hydrodynamic regimes in which collision among phonons are mostly Normal. It has been difficult to observe them, save for a few insulators with high levels of isotopic and chemical purity. Our thermal transport measurements, covering four decades of temperatures between 0.1 K and 900 K, reveal that sapphire displays all four regimes, despite its isotopic impurity. In the Ziman regime, the thermal conductivity exponentially increases attaining an amplitude as large as 35,000 W/Km. We show that the peak thermal conductivity of ultra-pure, simple insulators, including diamond, silicon and solid helium, is set by a universal scaling depending on isotropic purity. The thermal conductivity of sapphire is an order of magnitude higher than what is expected by this scaling. We argue that this may be caused by the proximity of optical and acoustic phonon modes, as a consequence of the large number of atoms in the primitive cell.

cond-mat.mtrl-sci↗
arXiv2024

Near-critical dark opalescence in out-of-equilibrium SF$_6$

The first-order phase transition between the liquid and gaseous phases ends at a critical point. Critical opalescence occurs at this singularity. Discovered in 1822, it is known to be driven by diverging fluctuations in the density. During the past two decades, boundaries between the gas-like and liquid-like regimes have been theoretically proposed and experimentally explored. Here, we show that fast cooling of near-critical sulfur hexafluoride (SF$_6$), in presence of Earth's gravity, favors dark opalescence, where visible photons are not merely scattered, but also absorbed. When the isochore fluid is quenched across the critical point, its optical transmittance drops by more than three orders of magnitude in the whole visible range, a feature which does not occur during slow cooling. We show that transmittance shows a dip at 2eV near the critical point, and the system can host excitons with binding energies ranging from 0.5 to 4 eV. The spinodal decomposition of the liquid-gas mixture, by inducing a periodical modulation of the fluid density, can provide a scenario to explain the emergence of this platform for coupling between light and matter. The possible formation of excitons and polaritons points to the irruption of quantum effects in a quintessentially classical context.

cond-mat.mtrl-sci↗
arXiv2023

Thermoelectric transport properties of electron doped pyrite FeS2

Pyrite FeS$_2$ has been investigated for a wide range of applications, including thermoelectrics due to previous observation of large thermopower at room-temperature. However, the values of thermopower reported in the literature is extremely sensitive to the nature of sample -- whether they are natural or lab grown, bulk crystals or thin films -- and an ambiguity in the magnitude and sign of thermopower of pure FeS$_2$ exists. Variation in the magnitude of room-temperature thermopower has also been observed in Co-doped samples. Therefore, it is of interest to clarify the intrinsic thermopower of this system that could be measured in more pure samples. In this paper, we investigate the thermoelectric properties of Co-doped FeS$_2$ using first principles calculations. We apply three different doping schemes to understand the effect of electron doping in FeS$_2$, namely explicit Co-substitution, jellium doping and electron addition within rigid band approximation (RBA) picture. The calculated thermopower is less than $-50$ $\mu$V/K for all values of Co doping that we studied, suggesting that this system may not be useful in thermoelectric applications. Interestingly, we find that RBA substantially overestimates the magnitude of calculated thermopower compared to the explicit Co-substitution and jellium doping schemes. The overestimation occurs because the changes in the electronic structure due to doping-induced structural modification and charge screening is not taken into account by the rigid shift of the Fermi level within RBA. RBA is frequently used in first principles investigations of the thermopower of doped semiconductors, and Co-substituted FeS$_2$ illustrates a case where it fails.

cond-mat.mtrl-sci↗
arXiv2023

Order-by-disorder charge density wave condensation at $\mathbf{\textit{q} =(\frac{1}{3},\frac{1}{3},\frac{1}{3})}$ in kagome metal ScV$_6$Sn$_6$

The recent discovery of a charge density wave order at the wave vector $P$ $(\frac{1}{3},\frac{1}{3},\frac{1}{3})$ in the kagome metal ScV$_6$Sn$_6$ has created a mystery because subsequent theoretical and experimental studies show a dominant phonon instability instead at another wave vector $H$ $(\frac{1}{3},\frac{1}{3},\frac{1}{2})$. In this paper, I use first principles total energy calculations to map out the landscape of the structural distortions due to the unstable phonon modes at $H$, $L$ $(\frac{1}{2},0,\frac{1}{2})$, and $P$ present in this material. In agreement with previous results, I find that the distortions due to the $H$ instability cause the largest gain in energy relative to the parent structure, followed in order by the $L$ and $P$ instabilities. However, only two distinct structure occur due to this instability, which are separated by 6 meV/f.u. The instability at $L$ results in three distinct structures separated in energy by 5 meV/f.u. In contrast, six different distorted structures are stabilized due to the instability at $P$, and they all lie within 2 meV/f.u.\ of each other. Hence, despite a lower energy gain, the condensation at $P$ could be favorable due to a larger entropy gain associated with the fluctuations within a manifold with larger multiplicity via the order-by-disorder mechanism.

cond-mat.str-el↗
arXiv2023

Emergent electronic landscapes in a novel valence-ordered nickelate with tri-component nickel coordination

The metal-hydride-based topochemical reduction process has produced novel thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and non-trivial ground states. Here, by such an oxygen (de-) intercalation method we synthesis a novel samarium nickelate with ordered nickel valences associated with tri-component coordination configurations. This structure, with a formula of Sm$_{9}$Ni$_{9}$O$_{22}$ as revealed by four-dimensional scanning transmission electron microscopy, emerges from the intricate planes of {303}$_{\text{pc}}$ ordered apical oxygen vacancies. X-ray spectroscopy measurements and ab-initio calculations show the coexistence of square-planar, pyramidal and octahedral Ni sites with mono-, bi- and tri-valences. It leads to an intense orbital polarization, charge-ordering, and a ground state with a strong electron localization marked by the disappearance of ligand-hole configuration at low-temperature. This new nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents a unique platform where mixed Ni valence can give rise to exotic phenomena.

cond-mat.mtrl-sci↗
arXiv2023

Minority-spin conducting states in Fe substituted pyrite CoS$_2$

There has been a longstanding debate whether the pyrite CoS$_2$ or its alloys with FeS$_2$ are half metallic. We argue using first principles calculations that there is a finite occupation of minority-spin states at the Fermi level throughout the series Co$_{1-x}$Fe$_x$S$_2$. Although the exchange-correlation functional influences the specifics of the electronic structure, we observe a similar trend with increasing Fe concentration in both LDA and GGA calculations. Specifically, even as band filling is decreased through Fe substitution, the lowest-lying conduction band in the minority-spin channel broadens such that these states keep getting lowered relative to the Fermi level, which is contrary to the expectations from a rigid band picture. Furthermore, the exchange splitting decreases as more Co atoms are replaced by Fe, and this again brings the minority-spin states closer to the Fermi level. These two mechanisms, in conjunction with the experimental observation that minority-spin bands cross the Fermi level in stoichiometric CoS$_2$, indicate that minority-spin charge carriers will always be present in Co$_{1-x}$Fe$_x$S$_2$.

cond-mat.mtrl-sci↗
arXiv2023

Transient translation symmetry breaking via quartic-order negative light-phonon coupling at the Brillouin zone boundary in KTaO${}_{3}$

KTaO${}_{3}$ presents a rich hyper-Raman spectrum originating from two-phonon processes at the Brillouin zone boundary, indicating the possibility of driving these phonon modes using intense midinfrared laser sources. We obtained the coupling of light to the highest-frequency longitudinal optic phonon mode $Q_{\rm{HY}}$ at the $X$ $(0,0, \frac{1}{2})$ point by first principles calculations of the total energy as a function of the phonon coordinate $Q_{\rm{HY}}$ and electric field $E$. We find that the energy curve as a function of $Q_{\rm{HY}}$ softens for finite values of electric field, indicating the presence of $Q_{\rm{HY}}^2 E^2$ nonlinearity with negative coupling coefficient. We studied the feasibility of utilizing this nonlinearity to transiently break the translation symmetry of the material by making the $Q_{\rm{HY}}$ mode unstable with an intense midinfrared pump pulse. We also considered the possibility that nonlinear phonon-phonon couplings can excite the lowest-frequency phonon coordinates $Q_{\rm{LZ}}$ and $Q_{\rm{LX}}$ at $X$ when the $Q_{\rm{HY}}$ mode is externally driven. The nonlinear phonon-phonon couplings were also obtained from first principles via total-energy calculations as a function of the phonon coordinates, and these were used to construct the coupled classical equations of motion for the phonon coordinates in the presence of an external pump term on $Q_{\rm{HY}}$. We numerically solved them for a range of pump frequencies and amplitudes and found three regimes where the translation symmetry is broken: i) rectification of the lowest-frequency coordinates due to large amplitude oscillation of the $Q_{\rm{HY}}$ coordinate about its equilibrium position, ii) rectification of only the $Q_{\rm{HY}}$ coordinate without displaced oscillations of the lowest-frequency coordinates, and iii) rectification of all three coordinates.

cond-mat.mtrl-sci↗
arXiv2023

The phonon thermal Hall angle in black phosphorus

The origin of phonon thermal Hall Effect (THE) observed in a variety of insulators is yet to be identified. Here, we report on the observation of a thermal Hall conductivity in a non-magnetic elemental insulator, with an amplitude exceeding what has been previously observed. In black phosphorus (BP), the longitudinal ($\kappa_{ii}$), and the transverse, $\kappa_{ij}$, thermal conductivities peak at the same temperature and at this peak temperature, the $\kappa_{ij}/\kappa_{jj}/B $ is $\approx 10^{-4}$-$10^{-3}$ T$^{-1}$. Both these features are shared by other insulators displaying THE, despite an absolute amplitude spreading over three orders of magnitude. The absence of correlation between the thermal Hall angle and the phonon mean-free-path imposes a severe constraint for theoretical scenarios of THE. We show that in BP a longitudinal and a transverse acoustic phonon mode anti-cross, facilitating wave-like transport across modes and the anisotropic charge distribution surrounding atomic bonds, paving the way for coupling with magnetic field.

cond-mat.str-el↗
arXiv2022

Light-induced translation symmetry breaking via nonlinear phononics

Light has a wavelength that is usually longer than the size of the unit cell of crystals. Hence, even intense light pulses are not expected to break the translation symmetry of materials. However, certain materials, including KTaO$_3$, exhibit peaks in their Raman spectra corresponding to their Brillouin zone boundary phonons due to second-order Raman processes, which provide a mechanism to drive these phonons using intense midinfrared lasers. We investigated the possibility of breaking the translation symmetry of KTaO$_3$ by driving its highest-frequency transverse optic mode $Q_{\textrm{HX}}$ at the $X$ $(0,\frac{1}{2},0)$ point. Our first principles calculations show that the energy curve of the transverse acoustic mode $Q_{\textrm{LZ}}$ at $X$ softens and develops a double-well shape as the value of the $Q_{\textrm{HX}}$ coordinate is increased, while that of the other transverse acoustic component $Q_{\textrm{LX}}$ hardens when the value of the $Q_{\textrm{HX}}$ coordinate is similarly varied. We performed similar total energy calculations as a function of the $Q_{\textrm{HX}}$ coordinate and electric field to extract the nonlinear coupling between them. These were then used to construct the coupled equations of motion for the three phonon coordinates in the presence of an external pump term on the $Q_{\textrm{HX}}$ mode, which we numerically solved for a range of pump frequencies and amplitudes. We find that 465 MV/cm is the smallest pump amplitude that leads to an oscillation of the $Q_{\textrm{LZ}}$ mode at a displaced position, hence, breaking the translation symmetry of the material. Such highly intense light pulses cannot be generate by currently available laser sources, and they have the possibility to damage the material. Nevertheless, our work shows that light can in principle be used to break the translation symmetry of a material via nonlinear phononics.

cond-mat.mtrl-sci↗
arXiv2022

Mesoscopic tunneling in strontium titanate

Spatial correlation between atoms can generate a depletion in the energy dispersion of acoustic phonons. Two well known examples are rotons in superfluid helium and the Kohn anomaly in metals. Here we report on the observation of a large softening of the transverse acoustic mode in quantum paraelectric SrTiO$_3$ by means of inelastic neutron scattering. In contrast to other known cases, this softening occurs at a tiny wave vector implying spatial correlation extending over a distance as long as 40 lattice parameters. We attribute this to the formation of mesoscopic fluctuating domains due to the coupling between local strain and quantum ferroelectric fluctuations. Thus, a hallmark of the ground state of insulating SrTiO$_3$ is the emergence of hybridized optical-acoustic phonons. Mesoscopic fluctuating domains play a role in quantum tunneling, which impedes the emergence of a finite macroscopic polarisation.

cond-mat.mtrl-sci↗
arXiv2022

Possible structural quantum criticality tuned by rare-earth ion substitution in infinite-layer nickelates

I show the infinite-layer rare-earth nickelates are near a structural quantum critical point by mapping the energetics of their structural instabilities using first priniciples calculations. I first confirm previous results that show a phonon instability in the $P4/mmm$ phase leading to the $I4/mcm$ structure for $R$NiO$_2$ with $R$ = Sm--Lu. I then study the non-spin-polarized phonon dispersions of the $I4/mcm$ phase and find that they exhibit rare-earth size dependent instabilities at the $X$ and $M$ points for materials with $R$ = Eu--Lu. Group-theoretical analysis was used to enumerate all the isotropy subroups due to these instablities, and the distorted structures corresponding to their order parameters were generated using the eigenvectors of the unstable phonons. These structures were then fully relaxed by minimizing both the atomic forces and lattice stresses. I was able to stabilize only five out of the twelve possible distortions. The $Pbcn$ isotropy subgroup with the $M_5^+(a,a)$ order parameter shows noticeable energy gain relative to other distortions for the compounds with late rare-earth ions. However, the order parameter of the lowest-energy phase switches first to $X_2^- (0,a) + M_5^+ (b,0)$ and then to $X_2^- (0,a)$ as the size of the rare-earth ion is progressively increased. Additionally, several distorted structures lie close in energy for the early members of this series. These features of the structural energetics persist even when antiferromagnetism is allowed. Such a competition between different order parameters that can be tuned by rare-earth ion substitution suggests that any structural transition that could arise from the phonon instabilities present in these materials can be suppressed to 0 K.

cond-mat.mtrl-sci↗
arXiv2021

Light-control of materials via nonlinear phononics

Nonlinear phononics is the phenomenon in which a coherent dynamics in a material along a set of phonons is launched after its infrared-active phonons are selectively excited using external light pulses. The microscopic mechanism underlying this phenomenon is the nonlinear coupling of the pumped infrared-active mode to other phonon modes present in a material. Nonlinear phonon couplings can cause finite time-averaged atomic displacements with or without broken crystal symmetries depending on the order, magnitude and sign of the nonlinearities. Such coherent lattice displacements along phonon coordinates can be used to control the physical properties of materials and even induce transient phases with lower symmetries. Light-control of materials via nonlinear phononics has become a practical reality due to the availability of intense mid-infrared lasers that can drive large-amplitude oscillations of the infrared-active phonons of materials. Mid-infrared pump induced insulator-metal transitions and spin and orbital order melting have been observed in pump-probe experiments. First principles based microscopic theory of nonlinear phononics has been developed, and it has been used to better understand how the lattice evolves after a mid-infrared pump excitation of infrared-active phonons. This theory has been used to predict light-induced switching of ferroelectric polarization as well as ferroelectricity in paraelectrics and ferromagnetism in antiferromagnets, which have been partially confirmed in recent experiments. This review summarizes the experimental and theoretical developments within this emerging field.

cond-mat.mtrl-sci↗