arXiv subjects

Alaska Subedi

Publications and source records attributed to Alaska Subedi.

At least 37 records · Page 2Linked to original sources

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↗

arXiv2021

Hexagonal-to-base-centered-orthorhombic $4Q$ charge density wave order in kagome metals KV$_3$Sb$_5$, RbV$_3$Sb$_5$, and CsV$_3$Sb$_5$

I search for the ground state structures of the kagome metals KV$_3$Sb$_5$, RbV$_3$Sb$_5$, and CsV$_3$Sb$_5$ using first principles calculations. Group-theoretical analysis shows that there are seventeen different distortions that are possible due to the phonon instabilities at the $M$ $(\frac{1}{2},0,0)$ and $L$ $(\frac{1}{2},0,\frac{1}{2})$ points in the Brilouin zone of the parent $P6/mmm$ phase of these materials. I generated these structures for the three compounds and performed full structural relaxations that minimize the atomic forces and lattice stresses. I find that the $Fmmm$ phase with the order parameter $M_1^+$ $(a,0,0)$ $+$ $L_2^-$ $(0,b,b)$ has the lowest energy among these possibilities in all three compounds. However, the $Fmmm$ exhibits a dynamical instability at its $Z$ $(0,0,1)$ point, which corresponds to the $A$ $(0,0,\frac{1}{2})$ point in the parent $P6/mmm$ phase. Condensation of this instability leads to a base-centered orthorhombic structure with the space group $Cmcm$ and $4Q$ order parameter $M_1^+$ $(a,0,0)$ $+$ $L_2^-$ $(0,b,b)$ $+$ $A_6^+$ $(\frac{1}{2}c,\frac{-\sqrt{3}}{2}c)$.

cond-mat.mtrl-sci↗

arXiv2021

Trigonal-to-monoclinic structural transition in TiSe$_2$ due to a combined condensation of $\mathbf{ \textit{q} = (\frac{1}{2},0,0)}$ and $\mathbf{(\frac{1}{2},0,\frac{1}{2})}$ phonon instabilities

I present first principles calculations of the phonon dispersions of TiSe$_2$ in the $P\overline{3}c1$ phase, which is the currently accepted low-temperature structure of this material. They show weak instabilities in the acoustic branches in the out-of-plane direction, suggesting that this phase may not be the true ground state. To find the lowest energy structure, I study the energetics of all possible distorted structures corresponding to the isotropy subgroups of $P\overline{3}m1$ for the $M_1^-$ and $L_1^-$ phonon instabilities present in this high-temperature phase at $q = (\frac{1}{2},0,0)$ and $(\frac{1}{2},0,\frac{1}{2})$, respectively. I was able to stabilize 10 different structures that are lower in energy relative to the parent $P\overline{3}m1$ phase, including two monoclinic structures more energetically stable than the $P\overline{3}c1$ phase. The lowest energy structure has the space group $C2$ with the order parameter $M_1^- (a,0,0) + L_1^- (0,b,b)$. This structure lacks inversion symmetry, and its primitive unit cell has 12 atoms.

cond-mat.mtrl-sci↗

arXiv2021

First principles study of thermal conductivity of In$_2$O$_3$ in relation to Al$_2$O$_3$, Ga$_2$O$_3$, and KTaO$_3$

I use first principles calculations to investigate the thermal conductivity of $β$-In$_2$O$_3$ and compare the results with that of $α$-Al$_2$O$_3$, $β$-Ga$_2$O$_3$, and KTaO$_3$. The calculated thermal conductivity of $β$-In$_2$O$_3$ agrees well with the experimental data obtain recently, which found that the low-temperature thermal conductivity in this material can reach values above 1000 W/mK. I find that the calculated thermal conductivity of $β$-Ga$_2$O$_3$ is larger than that of $β$-In$_2$O$_3$ at all temperatures, which implies that $β$-Ga$_2$O$_3$ should also exhibit high values of thermal conductivity at low temperatures. The thermal conductivity of KTaO$_3$ calculated ignoring the temperature-dependent phonon softening of low-frequency modes give high-temperature values similar that of $β$-Ga$_2$O$_3$. However, the calculated thermal conductivity of KTaO$_3$ does not increase as steeply as that of the binary compounds at low temperatures, which results in KTaO$_3$ having the lowest low-temperature thermal conductivity despite having acoustic phonon velocities larger than that of $β$-Ga$_2$O$_3$ and $β$-In$_2$O$_3$. I attribute this to the fact that the acoustic phonon velocities at low frequencies in KTaO$_3$ is less uniformly distributed because its acoustic phonon branches are more dispersive compared to the binary oxides, which causes enhanced momentum loss even during the normal phonon-phonon scattering processes. I also calculate thermal diffusivity using the theoretically obtained thermal conductivity and heat capacity and find that all four materials exhibit the expected $T^{-1}$ behavior at high temperatures. Additionally, the calculated ratio of the average phonon scattering time to Planckian time is larger than the lower bound of 1 that has been observed empirically in numerous other materials.

cond-mat.mtrl-sci↗

arXiv2020

Orthorhombic-to-monoclinic transition in Ta$_2$NiSe$_5$ due to a zone-center optical phonon instability

I study dynamical instabilities in Ta$_2$NiSe$_5$ using density functional theory based calculations. The calculated phonon dispersions show two unstable optical branches. All the acoustic branches are stable, which shows that an elastic instability is not the primary cause of the experimentally observed orthorhombic-to-monoclinic structural transition in this material. The largest instability of the optical branches occurs at the zone center, consistent with the experimental observation that the size of the unit cell does not multiply across the phase transition. The unstable modes have the irreps $B_{1g}$ and $B_{2g}$. Full structural relaxations minimizing both the forces and stresses find that the monoclinic $C2/c$ structure corresponding to the $B_{2g}$ instability has the lowest energy. Electronic structure calculations show that this low-symmetry structure has a sizable band gap. This suggest that a $B_{2g}$ zone-center optical phonon instability is the primary cause of the phase transition. An observation of a softening of a $B_{2g}$ zone-center phonon mode as the transition is approached from above would confirm the mechanism proposed here. If none of the $B_{2g}$ modes present in the material soften, this would imply that the transition is caused by electronic or elastic instability.

cond-mat.str-el↗

arXiv2019

Anisotropic thermal transport in magnetic intercalates Fe$_{x}$TiS$_2$

We present a study of the of thermal transport in thin single crystals of iron-intercalated titanium disulphide, Fe$_{x}$TiS$_2$ for $0\leq x \leq 0.20$. We determine the distribution of intercalants using high-resolution crystallographic and magnetic measurements, confirming the insertion of Fe without long-range ordering. We find that iron intercalation perturbs the lattice very little, and suppresses the tendency of TiS$_2$ to self-intercalate with excess Ti. We observe trends in the thermal conductivity that are compatible with our ab initio calculations of thermal transport in perfectly stoichiometric TiS$_2$.

cond-mat.mtrl-sci↗

arXiv2018

Momentum-space and real-space Berry curvatures in Mn$_{3}$Sn

Mn$_{3}$X (X= Sn, Ge) are noncollinear antiferromagnets hosting a large anomalous Hall effect (AHE). Weyl nodes in the electronic dispersions are believed to cause this AHE, but their locus in the momentum space is yet to be pinned down. We present a detailed study of the Hall conductivity tensor and magnetization in Mn$_{3}$Sn crystals and find that in the presence of a moderate magnetic field, spin texture sets the orientation of the $k$-space Berry curvature with no detectable in-plane anisotropy due to the $Z_6$ symmetry of the underlying lattice. We quantify the energy cost of domain nucleation and show that the multidomain regime is restricted to a narrow field window. Comparing the field dependence of AHE and magnetization, we find that there is a distinct component in the AHE which does not scale with magnetization when the domain walls are erected. This so-called `topological' Hall effect provides indirect evidence for a non-coplanar spin components and real-space Berry curvature in domain walls.

cond-mat.mtrl-sci↗

arXiv2018

Departure from the Wiedemann-Franz Law in WP$_2$ Driven by Mismatch in $T$-square Resistivity Prefactors

The Wiedemann-Franz (WF) law establishes a link between heat and charge transport due to electrons in solids. The extent of its validity in presence of inelastic scattering is a question raised in different contexts. We report on a study of the electrical, $σ$, and thermal, $κ$, conductivities in WP$_2$ single crystals. The WF holds at 2 K, but a downward deviation rapidly emerges upon warming. At 13 K, there is an exceptionally large mismatch between Lorenz number and the Sommerfeld value. We show that this is driven by a fivefold discrepancy between the $T$-square prefactors of electrical and thermal resistivities, both caused by electron-electron scattering. This implies the existence of abundant small-scattering-angle collisions between electrons, due to strong screening. By quantifying the relative frequency of collisions conserving momentum flux, but degrading heat flux, we identify a narrow temperature window where the hierarchy of scattering times may correspond to the hydrodynamic regime.

cond-mat.str-el↗

arXiv2018

Breathing distortions in the metallic, antiferromagnetic phase of LaNiO$_3$

I study the structural and magnetic instabilities in LaNiO$_3$ using density functional theory calculations. From the non-spin-polarized structural relaxations, I find that several structures with different Glazer tilts lie close in energy. The $Pnma$ structure is marginally favored compared to the $R\overline{3}c$ structure in my calculations, suggesting the presence of finite-temperature structural fluctuations and a possible proximity to a structural quantum critical point. In the spin-polarized relaxations, both structures exhibit the $\uparrow\!\!0\!\!\downarrow\!\!0$ antiferromagnetic ordering with a rock-salt arrangement of the octahedral breathing distortions. The energy gain due to the breathing distortions is larger than that due to the antiferromagnetic ordering. These phases are semimetallic with small three-dimensional Fermi pockets, which is largely consistent with the recent observation of the coexistence of antiferromagnetism and metallicity in LaNiO$_3$ single crystals by Li \textit{et al.} [arXiv:1705.02589].

cond-mat.str-el↗

arXiv2018

Observation of Poiseuille Flow of Phonons in Black Phosphorus

The travel of heat in insulators is commonly pictured as a flow of phonons scattered along their individual trajectory. In rare circumstances, momentum-conserving collision events dominate, and thermal transport becomes hydrodynamic. One of these cases, dubbed the Poiseuille flow of phonons, can occur in a temperature window just below the peak temperature of thermal conductivity. We report on a study of heat flow in bulk black phosphorus between 0.1 and 80 K. We find a thermal conductivity showing a faster than cubic temperature dependence between 5 and 12 K. Consequently, the effective phonon mean free path shows a nonmonotonic temperature dependence at the onset of the ballistic regime, with a size-dependent Knudsen minimum. These are hallmarks of Poiseuille flow previously observed in a handful of solids. Comparing the phonon dispersion in black phosphorus and silicon, we showthat the phase space for normal scattering events in black phosphorus is much larger. Our results imply that the most important requirement for the emergence of Poiseuille flowis the facility ofmomentum exchange between acoustic phonon branches. Proximity to a structural transition can be beneficial for the emergence of this behavior in clean systems, even when they do not exceed silicon in purity.

cond-mat.mtrl-sci↗

arXiv2017

Mott-to-Goodenough insulator-insulator transition in LiVO$_2$

I critically examine Goodenough's explanation for the experimentally observed phase transition in LiVO$_2$ using microscopic calculations based on density functional and dynamical mean field theories. The high-temperature rhombohedral phase exhibits both magnetic and dynamical instabilities. Allowing a magnetic solution for the rhombohedral structure does not open an insulating gap, and an explicit treatment of the on-site Coulomb $U$ interaction is needed to stabilize an insulating rhombohedral phase. The non-spin-polarized phonon dispersions of the rhombohedral phase show two unstable phonon modes at the wave vector $(\frac{1}{3},-\frac{1}{3},0)$ that corresponds to the experimentally observed trimer forming instability. A full relaxation of the supercell corresponding to this instability yields a nonmagnetic state containing V$_3$ trimers. These results are consistent with Goodenough's suggestion that the high-temperature phase is in the localized-electron regime and the transition to the low-temperature phase in the itinerant-electron regime is driven by V-V covalency.

cond-mat.str-el↗

arXiv2017

Modulated, three-directional, and polar structural instability in layered $d^1$ NaTiO$_2$

I study the experimentally observed metal-to-metal structural phase transition in NaTiO$_2$ using density functional calculations. I do not find the previously proposed low-temperature structure energetically favorable with respect to the high-temperature rhombohedral structure. The calculated phonon dispersions of the rhombohedral phase show dynamical instabilities at several inequivalent parts of the Brillouin zone, including at the wavevector $(\frac{1}{2},\frac{1}{5},\frac{1}{5})$. These instabilities lead to monoclinic structures without inversion symmetry that are modulated along all three directions. The calculated electronic structures show that a local bonding instability of the Ti $3d$ states is associated with the structural transition.

cond-mat.str-el↗

arXiv2016

Proposal for midinfrared light--induced ferroelectricity in oxide paraelectrics

I show that a nonequilibrium paraelectric to ferroelectric transition can be induced using midinfrared pulses. This relies on a quartic $lQ_{\textrm{l$_z$}}^2Q_{\textrm{h$_x$}}^2$ coupling between the lowest ($Q_{\textrm{l$_z$}}$) and highest ($Q_{\textrm{h$_x$}}$) frequency infrared-active phonon modes of a paraelectric material. Density functional calculations show that the coupling constant $l$ is negative, which causes a softening of the $Q_{\textrm{l$_z$}}$ mode when the $Q_{\textrm{h$_x$}}$ mode is externally pumped. A rectification along the $Q_{\textrm{l$_z$}}$ coordinate that stabilizes the nonequilibrium ferroelectric state occurs only above a critical threshold for the electric field of the pump pulse, demonstrating that this is a nonperturbative phenomenon. A first principles calculation of the coupling between light and the $Q_{\textrm{h$_x$}}$ mode shows that ferroelectricity can be induced in the representative case of strained KTaO$_3$ by a midinfrared pulse with a peak electric field of 17 MV cm$^{-1}$ and duration of 2 ps. Furthermore, other odd-order nonlinear couplings make it possible to arbitrarily switch off the light-induced ferroelectric state, making this technique feasible for all-optic devices.

cond-mat.str-el↗

arXiv2016

Competing covalent and ionic bonding in Ge-Sb-Te phase change materials

Ge2Sb2Te5 and related phase change materials are highly unusual in that they can be readily transformed between amorphous and crystalline states using very fast melt, quench, anneal cycles, although the resulting states are extremely long lived at ambient temperature. These states have remarkably different physical properties including very different optical constants in the visible in strong contrast to common glass formers such as silicates or phosphates. This behavior has been described in terms of resonant bonding, but puzzles remain, particularly regarding different physical properties of crystalline and amorphous phases. Here we show that there is a strong competition between ionic and covalent bonding in cubic phase providing a link between the chemical basis of phase change memory property and origins of giant responses of piezoelectric materials (PbTiO3, BiFeO3). This has important consequences for dynamical behavior in particular leading to a simultaneous hardening of acoustic modes and softening of high frequency optic modes in crystalline phase relative to amorphous. This different bonding in amorphous and crystalline phases provides a direct explanation for different physical properties and understanding of the combination of long time stability and rapid switching and may be useful in finding new phase change compositions with superior properties.

cond-mat.mtrl-sci↗

arXiv2016

Proposal for ultrafast switching of ferroelectrics using mid-infrared pulses

I propose a method for ultrafast switching of ferroelectric polarization using mid-infrared pulses. This involves selectively exciting the highest frequency $A_1$ phonon mode of a ferroelectric material with an intense mid-infrared pulse. Large amplitude oscillations of this mode provides a unidirectional force to the lattice such that it displaces along the lowest frequency $A_1$ phonon mode coordinate because of a nonlinear coupling of the type $g Q_{\textrm{P}} Q_{\textrm{IR}}^2$ between the two modes. First principles calculations show that this coupling is large in transition-metal oxide ferroelectrics, and the sign of the coupling is such that the lattice displaces in the switching direction. Furthermore, I find that the lowest frequency $A_1$ mode has a large $Q_{\textrm{P}}^3$ order anharmonicity, which causes a discontinuous switch of electric polarization as the pump amplitude is continuously increased.

cond-mat.str-el↗

arXiv2015

Strong-coupling electron-phonon superconductivity in noncentrosymmetric quasi-one-dimensional K$_2$Cr$_3$As$_3$

I study the lattice dynamics and electron-phonon coupling in non-centrosymmetric quasi-one-dimensional K$_2$Cr$_3$As$_3$ using density functional theory based first principles calculations. The phonon dispersions show stable phonons without any soft-mode behavior. They also exhibit features that point to a strong interaction of K atoms with the lattice. I find that the calculated Eliashberg spectral function shows a large enhancement around 50 cm$^{-1}$. The phonon modes that show large coupling involve in-plane motions of all three species of atoms. The $\mathbf{q}$ dependent electron-phonon coupling decreases strongly away from the $q_z = 0$ plane. The total electron-phonon coupling is large with a value of $λ_{\textrm{ep}} = 3.0$, which readily explains the experimentally observed large mass enhancement.

cond-mat.supr-con↗

arXiv2015

Low-energy description of the metal-insulator transition in the rare-earth nickelates

We propose a simple theoretical description of the metal-insulator transition of rare-earth nickelates. The theory involves only two orbitals per nickel site, corresponding to the low-energy anti-bonding $e_g$ states. In the monoclinic insulating state, bond-length disproportionation splits the manifold of $e_g$ bands, corresponding to a modulation of the effective on-site energy. We show that, when subject to a local Coulomb repulsion $U$ and Hund's coupling $J$, the resulting bond-disproportionated state is a paramagnetic insulator for a wide range of interaction parameters. Furthermore, we find that when $U-3J$ is small or negative, a spontaneous instability to bond disproportionation takes place for large enough $J$. This minimal theory emphasizes that a small or negative charge-transfer energy, a large Hund's coupling, and a strong coupling to bond-disproportionation are the key factors underlying the transition. Experimental consequences of this theoretical picture are discussed.

cond-mat.str-el↗

arXiv2015

Transport Properties of Cubic Crystalline Ge$_{2}$Sb$_{2}$Te$_{5}$: A Potential Low-temperature Thermoelectric Material

Ge$_{2}$Sb$_{2}$Te$_{5}$ (GST) has been widely used as a popular phase change material. In this study, we show that it exhibits high Seebeck coefficients 200 - 300 $μ$V/K in its cubic crystalline phase ($\it{c}$-GST) at remarkably high $\it{p}$-type doping levels of $\sim$ 1$\times$10$^{19}$ - 6$\times$10$^{19}$ cm$^{-3}$ at room temperature. More importantly, at low temperature (T = 200 K), the Seebeck coefficient was found to exceed 200 $μ$V/K for a doping range 1$\times$10$^{19}$ - 3.5$\times$10$^{19}$ cm$^{-3}$. Given that the lattice thermal conductivity in this phase has already been measured to be extremely low ($\sim$ 0.7 W/m-K at 300 K),\citep{r51} our results suggest the possibility of using $\it{c}$-GST as a low-temperature thermoelectric material.

cond-mat.mtrl-sci↗