arXiv subjects

B. K. Mani

Publications and source records attributed to B. K. Mani.

At least 19 recordsLinked to original sources

arXiv2026

Atomistic study of finite temperature properties in ferroelectric BiAlO$_3$

The lead-free perovskite ferroelectrics captivate researchers with their unique functional properties leading to important technological applications. In the search for a new lead-free perovskite of technological importance, we develop a first-principles based atomistic model to accurately predict the properties of BiAlO$_3$ in experimentally relevant conditions. Consistent with the experimental observations, our simulations predict a rhombohedral ferroelectric ($R3c$) ground state for BiAlO$_3$ facilitated by a structural phase transition from paraelectric (cubic, $Pm\Bar{3}m$) phase. The room-temperature spontaneous polarization and Curie temperature are obtained to be 81 $μ$C/cm$^2$ (along [111] direction) and 1160 K, respectively. Our simulations reveal strong coupling between ferroelectric and antiferrodistortive modes for a broad spectrum of temperature and electric field. We find that hydrostatic pressure suppresses both spontaneous polarization and Curie temperature, while both uniaxial and biaxial stresses induce multiple phase transitions in BiAlO$_3$.

cond-mat.mtrl-sci↗

arXiv2026

Transition metal (group V) doping induced spin and valley polarization in MoS$_2$ monolayer

Doping in two-dimensional materials has emerged as an effective tool for modulating their electronic properties and thereby enabling their multifunctional applications. In this work, we present a first-principles study on induced effective magnetic moment and metallicity in MoS$_2$ monolayer by substitutional doping of group-5 transition metal (TM) elements -- V, Nb and Ta. From our study, we observe that the V doping induces half-metallicity, whereas metallic characteristics are observed in the case of Nb and Ta doping. Moreover, V and Ta-doped MoS$_2$ monolayers are observed to show total induced magnetic moments of 0.922 and 0.624 $μ_{\rm B}$, respectively. Importantly, the combined effects of strong spin-orbit coupling (SOC), broken inversion symmetry, and structural asymmetry is observed to lead to a permanent valley polarization in the V- and Ta-MoS$_2$ systems. In particular, we observed a valley polarization of 121 and 21 meVs for V and Ta-doped MoS$_2$, respectively. Furthermore, an enhanced piezoelectric coefficient for the doped systems is observed compared to pristine MoS$_2$. Notably, the simultaneous presence of half-metallicity, substantial valley polarization, and enhanced piezoelectricity in V-doped MoS$_2$ establishes this system as a promising multifunctional platform for next-generation spintronic, valleytronic, and piezoelectric nanodevices. Overall, our findings provide fundamental insights into engineering coupled spin-valley-mechanical degrees of freedom in two-dimensional materials for advanced quantum and nanoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2026

Anomalous lattice anharmonicity and spin-lattice coupling in spin orbit coupled halide K2IrBr6

The interplay between lattice distortions, magnetism, and spin-orbit coupling in 5d transition-metal halides offers a fertile platform for exploring correlated spin-lattice dynamics. Here, we investigate the impact of structural symmetry breaking on lattice vibrations and local spin environments in the antifluorite compound K2IrBr6 using temperature dependent Raman spectroscopy, electron paramagnetic resonance (EPR), and first-principles lattice dynamics calculations. K2IrBr6 undergoes successive cubic-to-tetragonal and tetragonal-to-monoclinic phase transitions at 170 K and 122 K, respectively, driven by cooperative distortions of the IrBr6 octahedra. Raman spectroscopy reveals anomalous phonon linewidth broadening and unconventional temperature dependence of phonon energies near these transitions, indicating that dynamic spin-phonon coupling is significant well above the Neel temperature (16 K). First-principles phonon calculations support the mode assignments and demonstrate that symmetry-lowering distortions significantly renormalize vibrational modes, consistent with the experimental observations. Complementary EPR measurements detect anisotropic g-factors, resonance field shifts, and linewidth narrowing across the structural transitions, reflecting the emergence of static spin-lattice correlations mediated by spin-orbit entanglement. These findings establish K2IrBr6 as a model system where halide ligand fields, octahedral distortions, and SOC collaboratively govern spin-lattice coupling, providing chemical pathways to engineer quantum materials with tunable magnetic and lattice responses.

cond-mat.str-el↗

arXiv2025

Designing new Zintl phases SrBaX (X = Si, Ge, Sn) for thermoelectric applications using \textit{ab initio} techniques

Slack's phonon-glass and electron-crystal concept has been the guiding paradigm for designing new thermoelectric materials. Zintl phases, in principle, have been shown as great contenders of the concept and thereby good thermoelectric candidates. With this as motivation, we design new Zintl phases SrBaX (X = Si, Ge, Sn) using state-of-the-art computational methods. Herein, we use first-principles simulations to provide key theoretical insights to thermal and electrical transport properties. Some of the key findings of our work feature remarkably low lattice thermal conductivities ($<$~1~W~m$^{-1}$~K$^{-1}$), putting proposed materials among the well-known thermoelectric materials such as SnSe and other contemporary Zintl phases. We ascribe such low values to antibonding states induced weak bonding in the lattice and intrinsically weak phonon transport, resulting in low phonon velocities, short lifetimes, and considerable anharmonic scattering phase spaces. Besides, our results on electronic structure and transport properties reveal tremendous performance of SrBaGe ($ZT\sim$ 2.0 at 700~K), highlighting the relevance among state-of-the-art materials such as SnSe. Further, the similar performances for both $p$- and $n$-type dopings render these materials attractive from device fabrication perspective. We believe that our study would invite experimental investigations for realizing the true thermoelectric potential of SrBaX series.

cond-mat.mtrl-sci↗

arXiv2025

Probing transition rates, nuclear moments and electric dipole polarizability in nobelium using multireference FSRCC and PRCC theories

We employ an all-particle multireference Fock-space relativistic coupled-cluster (FSRCC) theory to compute the ionization potential, excitation energy, transition rate and hyperfine structure constants associated with $7s^2\;^{1}S_{0}\rightarrow 7s7p\;^{3}P_{1}$ and $7s^2\;^{1}S_{0}\rightarrow 7s7p\;^1P_{1}$ transitions in nobelium (No). Using our state-of-the-art calculations in conjunction with available experimental data \cite{raeder-18}, we extract the values of nuclear magnetic dipole ($μ$) and electric quadrupole ($Q$) moments for $^{253}$No. Further, information on nuclear deformation in even-mass isotopes is extracted from the isotope shift calculations. Moreover, we employ a perturbed relativistic coupled-cluster (PRCC) theory to compute the ground state electric dipole polarizability of No. In addition, to assess the accuracy of our calculations, we compute the ionization potential and dipole polarizability of lighter homolog ytterbium (Yb). To account for strong relativistic and quantum electrodynamical (QED) effects in No, we incorporate the corrections from Breit interaction, vacuum polarization and self-energy in our calculations. The contributions from triple excitations in coupled-cluster is accounted perturbatively. Our calculations reveal a significant contribution of $\approx$10\% from the perturbative triples to the transition rate of $7s^2\;^1S_{0}\rightarrow 7s7p\;^3P_{1}$ transition. The largest cumulative contribution from Breit+QED is observed to be $\approx$4\%, to the magnetic dipole hyperfine structure constant of $7s7p\;^1P_{1}$ state. Our study provides a comprehensive understanding of atomic and nuclear properties of nobelium with valuable insights into the electron correlation and relativistic effects in superheavy elements.

physics.atom-ph↗

arXiv2024

Fock-space perturbed relativistic coupled-cluster calculations of electric dipole polarizability and nuclear spin-dependent parity non-conservation in Cs

We implement the Fock-space perturbed relativistic coupled-cluster theory to compute the electric dipole polarizability of ground and low lying excited states, and nuclear spin-dependent parity violating (NSD-PNC) transition amplitudes in Cs. Moreover, to check the accuracy of the wavefunctions used in the calculations, we compute the excitation energies, E1 transition amplitudes and magnetic dipole hyperfine constants for ground and low lying excited states. To improve the accuracy of the computed properties, we have incorporated the corrections from the relativistic and QED effects in our calculations. The contributions from triple excitations are accounted perturbatively. Our results on excitation energies, E1 transition amplitudes and hyperfine constants are in good agreement with the available experimental results. Our polarizability results using FS-PRCC theory match well with the experimental values. The values of parity-violating transition amplitudes from our calculations are, in general, on the lower side of the previous values. From the detail analysis of electron correlations, we find that the corrections from the Breit interaction and QED effects are important to get accurate results of NSD-PNC amplitudes in Cs. The largest cumulative contribution from the Breit and QED corrections is found to be $\approx$ 3.2\% of the total value. The upper bound on the theoretical uncertainty in our calculated NSD-PNC amplitudes is estimated to be about 1\%.

physics.atom-ph↗

arXiv2024

Emergence of half-metallic ferromagnetism and valley polarization in transition metal substituted WSTe monolayer

Two-dimensional (2D) Janus materials hold a great importance in spintronic and valleytronic applications due to their unique lattice structures and emergent properties. They intrinsically exhibit both an in-plane inversion and out-of-plane mirror symmetry breakings, which offer a new degree of freedom to electrons in the material. One of the main limitations in the multifunctional applications of these materials is, however, that, they are usually non-magnetic in nature. Here, using first-principles calculations, we propose to induce magnetic degree of freedom in non-magnetic WSTe via doping with transition metal (TM) elements -- Fe, Mn and Co. Further, we comprehensively probe the electronic, spintronic and valleytronic properties in these systems. Our simulations predict intrinsic Rashba and Zeeman-type spin splitting in pristine WSTe. The obtained Rashba parameter is $\sim$ 422 meVÅ\; along the $Γ- K$ direction. Our study shows a strong dependence on uniaxial and biaxial strains where we observe an enhancement of $\sim$ 2.1\% with 3\% biaxial compressive strain. The electronic structure of TM-substituted WSTe reveals half-metallic nature for 6.25 and 18.75\% of Fe, 25\% of Mn, and 18.75 and 25\% of Co structures, which leads to 100\% spin polarization. The obtained values of valley polarization 65, 54.4 and 46.3 meV for 6.25\% of Fe, Mn and Co, respectively, are consistent with the literature data for other Janus materials. Further, our calculations show a strain dependent tunability of valley polarization, where we find an increasing (decreasing) trend with uniaxial and biaxial tensile (compressive) strains. We observed a maximum enhancement of $\sim$ 1.72\% for 6.25\% of Fe on application of 3\% biaxial tensile strain.

cond-mat.mtrl-sci↗

arXiv2024

Fock-space relativistic coupled-cluster calculations of clock transition properties in Pb$^{2+}$

We have implemented an all-particle multireference Fock-space relativistic coupled-cluster theory to probe $6s^2{\;^1}S_{0} - 6s6p{\;^3P^o_{0}}$ clock transition in an even isotope of Pb$^{2+}$. We have computed, excitation energy for several low lying states, E1 and M1 transition amplitudes, and the lifetime of the clock state. Moreover, we have also calculated the ground state dipole polarizability using perturbed relativistic coupled-cluster theory. To improve the accuracy of results, we incorporated the corrections from the relativistic and QED effects in all our calculations. The contributions from triple excitations are accounted perturbatively. Our computed excitation energies are in excellent agreement with the experimental values for all the states. Our result for lifetime, $9.76\times10^{6}$ s, of clock state is $\approx$ 8.5\% larger than the previous value using CI+MBPT [Phys. Rev. Lett. {\bf 127}, 013201 (2021)]. Based on our analysis, we find that the contributions from the {\em valence-valence} correlations arising from higher energy configurations and the corrections from the perturbative triples and QED effects are essential to get accurate clock transition properties in Pb$^{2+}$. Our computed value of dipole polarizability is in good agreement with the available theoretical and experimental data.

physics.atom-ph↗

arXiv2023

Emergence of half-metallic ferromagnetism in transition metal substituted Na$_{0.5}$Bi$_{0.5}$TiO$_3$

The multifunctional materials with prominent properties such as electrical, ferroelectric, magnetic, optical and magneto-optical are of keen interest to several practical implications. In the roadmap of designing such materials, in the present work, using density functional theory based first-principles calculations, we have investigated the functional properties of transition metal substituted-NBT. Our calculations predict the emergence of half-metallic ferromagnetism in the system. A nonzero magnetic moment of 1.49 $μ_{\rm B}/{\rm f.u.}$ is obtained for 25\% concentration of Ni. Our data on optical properties for pure NBT is in excellent agreement with available theory and experiments. For Ni-NBT, we observed a diverging nature of static dielectric constant, which could be attributed to the induced metallic character in the material. Our simulations on MOKE predict a significant Kerr signal of 0.7$^\circ$ for 6.25\% Ni-concentration.

cond-mat.mtrl-sci↗

arXiv2023

First-principles study of disordered half-Heusler alloys \textit{X}Fe$_{0.5}$Ni$_{0.5}$Sn (\textit{X} = Nb, Ta) as thermoelectric prospects

High lattice thermal conductivity in half-Heusler alloys has been the major bottleneck in thermoelectric applications. Disordered half-Heusler alloys could be a plausible alternative to this predicament. In this paper, utilizing first-principles simulations, we have demonstrated the low lattice thermal conductivity in two such phases, NbFe$_{0.5}$Ni$_{0.5}$Sn and TaFe$_{0.5}$Ni$_{0.5}$Sn, in comparison to well-known half-Heusler alloy TiCoSb. We trace the low thermal conductivity to their short phonon lifetime, originating from the interaction among acoustic and low-lying optical phonons. We recommend nanostructuring as an effective route in further diminishing the lattice thermal conductivity. We further predict that these alloys can be best used in the temperature range 400-600~K and carrier concentration of less than 10$^{21}$ carriers cm$^{-3}$. We found $\sim$35\% and $\sim$17\% enhancement in $ZT$ for NbFe$_{0.5}$Ni$_{0.5}$Sn and TaFe$_{0.5}$Ni$_{0.5}$Sn, respectively, as compared to TiCoSb. We are optimistic of the findings and believe these materials would attract experimental investigations.

cond-mat.mtrl-sci↗

arXiv2023

Ab initio study of NaSrSb and NaBaSb as potential thermoelectric prospects

Zintl phases are excellent thermoelectric prospects to put the waste heat to good use. In the quest of the same, using first-principles methods combined with Boltzmann transport theory, we explored two recent phases NaSrSb and NaBaSb. We found low lattice thermal conductivity of 1.9 and 1.3 W m$^{-1}$ K$^{-1}$ at 300~K for NaSrSb and NaBaSb, respectively, which are of the same order as other potential Zintl phases such as Sr$_3$AlSb$_3$ and BaCuSb. We account for such low values to short phonon lifetimes, small phonon group velocities, and lattice anharmonicity in the crystal structure. The calculated electrical transport parameters based on acoustic deformation potential, ionized impurity, and polar optical phonon scattering mechanisms reveal large Seebeck coefficients for both materials. Further, we obtain a high figure of merit of ZT$\sim$2.0 at 900~K for \textit{n}-type NaSrSb. On the other hand, the figure of merit of \textit{n}-type NaBaSb surpasses the unity. We are optimistic about our findings and believe our work would set a basis for future experimental investigations.

cond-mat.mtrl-sci↗

arXiv2021

Fock-space perturbed relativistic coupled-cluster theory for electric dipole polarizability of one-valence atomic systems: Application to Al and In

We have developed a Fock-space relativistic coupled-cluster theory based method for the calculation of electric dipole polarizability of one-valence atoms and ions. We employ this method to compute the ground-state and spin-orbit coupled excited state electric dipole polarizability of Al and In. To check the quality of many-electron wavefunctions, we also compute the excitation energies of some low-lying states of Al and In. The effects of Breit interaction and QED corrections from the Uehling potential and the self-energy are included to improve the accuracy of $α$ further. Our recommended value of ground-state $α$ for both atoms are in good agreement with the previous theoretical results. From our computations, we find that more than 65\% of contributions come from the dipolar mixing of $3p$($5p$) with $3d$($5d$) and $4s$($6s$)-electrons for Al(In). The largest Breit and QED contributions are found to be 1.3\% and 0.6\%, respectively.

physics.atom-ph↗

arXiv2021

Fock-space relativistic coupled-cluster calculation of hyperfine induced $\bf {^1S_0 \rightarrow {^3P^o_0}}$ clock transition in Al$^+$

We have developed an all-particle Fock-space relativistic coupled-cluster method to calculate the properties of two-valence atoms and ions. Using the method we compute the properties associated with hyperfine induced $^1S_0 - ^3P^o_0$ clock transition in Al$^+$. Our result of the $^3P^o_0$ metastable state life time, $20.20 \pm 0.91$ s, is in excellent agreement with the experimental value, $20.60 \pm 1.4$ s [Phys. Rev. Lett. {\bf 98}, 220801 (2007)]. Our studies show that the contributions from the triple excitations, and the corrections from the Breit interaction and QED effects are essential to obtain accurate clock properties in Al$^+$.

physics.atom-ph↗

arXiv2021

RCC calculation of electric dipole polarizability and correlation energy of Cn, Nh$^+$ and Og: Correlation effects from lighter to superheavy elements

We employ a fully relativistic coupled-cluster theory to calculate the ground-state electric dipole polarizability and electron correlation energy of superheavy elements Cn, Nh$^+$ and Og. To assess the trend of electron correlation as function of $Z$, we also calculate the correlation energies for three lighter homologs--Zn, Cd and Hg; Ga$^+$, In$^+$ and Tl$^+$; Kr, Xe and Rn--for each superheavy elements. The relativistic effects and quantum electrodynamical corrections are included using the Dirac-Coulomb-Breit Hamiltonian with the corrections from the Uehling potential and the self-energy. The effects of triple excitations are considered perturbatively in the theory. Furthermore, large bases are used to test the convergence of results. Our recommended values of polarizability are in good agreement with previous theoretical results for all SHEs. From our calculations we find that the dominant contribution to polarizability is from the valence electrons in all superheavy elements. Except for Cn and Og, we observe a decreasing contribution from lighter to superheavy elements from the Breit interaction. For the corrections from the vacuum polarization and self-energy, we observe a trend of increasing contributions with $Z$. From energy calculations, we find that the second-order many-body perturbation theory overestimates the electron correlation energy for all the elements considered in this work.

physics.atom-ph↗

arXiv2019

Electric dipole polarizability of group-IIIA ions using PRCC: Large correlation effects from nonlinear terms

We compute the ground-state electric dipole polarizability of group-IIIA ions using the perturbed relativistic coupled-cluster (PRCC) theory. To account for the relativistic effects and QED corrections, we use the Dirac-Coulomb-Breit Hamiltonian with the corrections from the Uehling potential and the self-energy. The effects of triple excitations are considered perturbatively in the PRCC. Our PRCC results for $α$ are good in agreement with the previous theoretical results for all the ions. From our computations we find that the nonlinear terms in PRCC have significant contributions and must be included to obtain the accurate value of $α$ for group-IIIA ions. For the correction from the Breit interaction, we find that it is largest for Al$^+$ and decreases as we go towards the heavier ions. The corrections from the vacuum polarization and the self-energy increase from lighter to heavier ions.

physics.atom-ph↗

arXiv2016

RCCPAC: A parallel relativistic coupled-cluster program for closed-shell and one-valence atoms and ions in FORTRAN

We report the development of a parallel FORTRAN code, RCCPAC, to solve the relativistic coupled-cluster equations for closed-shell and one-valence atoms and ions. The parallelization is implemented through the use of message passing interface, which is suitable for distributed memory computers. The coupled-cluster equations are defined in terms of the reduced matrix elements, and solved iteratively using Jacobi method. The ground and excited states coupled-cluster wave functions obtained from the code could be used to compute different properties of closed-shell and one-valence atom or ion. As an example we compute the ground state correlation energy, attachment energies, $E$1 reduced matrix elements and hyperfine structure constants.

physics.atom-ph↗

arXiv2014

Triple excitations in perturbed relativistic coupled-cluster theory and Electric dipole polarizability of groupIIB elements

We use perturbed relativistic coupled-cluster (PRCC) theory to compute the electric dipole polarizabilities $α$ of Zn, Cd and Hg. The computations are done using the Dirac-Coulomb-Breit Hamiltonian with Uehling potential to incorporate vacuum polarization corrections. The triple excitations are included perturbatively in the PRCC theory, and in the unperturbed sector, it is included non-perturbatively. Our results of $α$, for all the three elements, are in excellent agreement with the experimental data. The other highlight of the results is the orbital energy corrections from Breit interactions. In the literature we could only get the data of Hg {E. Lindroth et al., J. Phys. B 22, 2447 (1989)} and are near perfect match with our results. We also present the linearized equations of the cluster amplitudes, including the triple excitations, with the angular factors.

physics.atom-ph↗

arXiv2014

Electric dipole polarizability of alkaline-Earth-metal atoms from perturbed relativistic coupled-cluster theory with triples

The perturbed relativistic coupled-cluster (PRCC) theory is applied to calculate the electric dipole polarizabilities of alkaline Earth metal atoms. The Dirac-Coulomb-Breit atomic Hamiltonian is used and we include the triple excitations in the relativistic coupled-cluster (RCC) theory. The theoretical issues related to the triple excitation cluster operators are described in detail and we also provide details on the computational implementation. The PRCC theory results are in good agreement with the experimental and previous theoretical results. We, then, highlight the importance of considering the Breit interaction for alkaline Earth metal atoms.

physics.atom-ph↗