arXiv subjects

Assa Aravindh Sasikala Devi

Publications and source records attributed to Assa Aravindh Sasikala Devi.

5 recordsLinked to original sources

arXiv2026

Data-Efficient Machine learning for Predicting Dopant Formation Energies in TiO$_2$ Monolayer

Machine learning models are increasingly applied in materials science, yet their predictive power is often constrained by data scarcity. Here, we show that accurate predictions can be achieved, even with a limited number of training examples, provided the dataset is compact and and grounded in physically relevant quantities. By combining density functional theory calculations with a machine-learning framework, we construct accurate descriptor-based models to predict the formation energies of doped lepidocrocite TiO$_2$ monolayers. The predictive accuracy of machine-learning models was first evaluated for single-dopant Pt configurations, demonstrating that the selected structural and chemical descriptors reliably capture the key factors governing dopant stability. Chemical transferability is then examined by extending the dataset to include Ag-doped configurations. Predictive accuracy improved systematically as additional Ag-doped data points were included in the training, while the performance of Pt remains robust. These results highlight the potential of small and well-curated datasets combined with physically informed descriptors to enable not only accurate but also chemically transferable machine-learning-driven screening in doped TiO$_2$ monolayer.

cond-mat.mtrl-sci↗

arXiv2026

Investigating the Electronic and Magnetic Properties of Na$_x$Fe$_{1/2}$Mn$_{1/2}$O$_2$ Cathode Materials with X-ray Compton Scattering

We discuss electronic and magnetic properties of Na$_x$Fe$_{1/2}$Mn$_{1/2}$O$_2$, a promising Na-ion battery cathode material. Using x-ray Compton scattering, SQUID magnetometry, and density-functional-theory based modeling, we probe how electrons and spins evolve during sodiation. By comparing Compton profiles of sodiated and desodiated samples, we show that oxygen 2$p$ orbitals drive the redox process, while transition-metal 3$d$ electrons become more delocalized, explaining the metallic phase at $x=2/3$. These profile differences define a quantitative descriptor for the sodiation range associated with improved conductivity. Electron holes on oxygen, reflected in oxygen magnetization, confirm the important role of oxygen in the electrochemical activity of the cathode.

cond-mat.mtrl-sci↗

arXiv2024

Compton scattering study of strong orbital delocalization in a LiNiO$_2$ cathode

Cobalt is used in Li-ion batteries, but it is expensive and could be replaced by nickel to deliver better performance at a lower cost. With this motivation, we discuss how the character of redox orbitals of LiNiO$_2$ can be ascertained through x-ray Compton scattering measurements combined with parallel first-principles simulations. Our analysis reveals the nature of hole states in Li-doped NiO resulting from the hybridization of O 2$p$ and Ni 3$d$ orbitals. Our study also gives insight into the ferromagnetic ground state and provides a pathway toward the rational design of next-generation battery materials.

cond-mat.mtrl-sci↗

arXiv2023

Ab initio insights on the ultrafast strong-field dynamics of anatase TiO$_2$

Electron dynamics of anatase TiO$_2$ under the influence of ultrashort and intense laser field is studied using the real-time time-dependent density functional theory (TDDFT). Our findings demonstrate the effectiveness of TDDFT calculations in modeling the electron dynamics of solids during ultrashort laser excitation, providing valuable insights for designing and optimizing nonlinear photonic devices. We analyze the perturbative and non-perturbative responses of TiO$_2$ to 30 fs laser pulses at 400 and 800 nm wavelengths, elucidating the underlying mechanisms. At 400 nm, ionization via single photon absorption dominates, even at very low intensities. At 800 nm, we observe ionization through two-photon absorption within the intensity range of $1\times10^{10}$ to $9\times10^{12}$ W/cm$^2$, with a transition from multiphoton to tunneling ionization occurring at $9\times10^{12}$ W/cm$^2$. We observe a sudden increase in energy and the number of excited electrons beyond $1\times10^{13}$ W/cm$^2$, leading to their saturation and subsequent laser-induced damage. We estimate the damage threshold of TiO$_2$ for 800 nm to be 0.1 J/cm$^2$. In the perturbative regime, induced currents exhibit a phase shift proportional to the peak intensity of the laser pulse. This phase shift is attributed to the intensity-dependent changes in the number of free carriers, indicative of the optical Kerr effect. Leveraging the linear dependence of phase shift on peak intensities, we estimate the nonlinear refractive index ($n_2$) of TiO$_2$ to be $3.54\times10^{-11}$ cm$^2$/W.

physics.optics↗

arXiv2021

Quasiparticle electronic structure and optical response ($G_0W_0$+BSE) of anatase TiO$_2$ starting from modified HSE06 functionals

The quasiparticle electronic structure and optical excitation of anatase TiO$_2$ is determined within the framework of many-body perturbation theory (MBPT) by combining the $G_0W_0$ method and the Bethe-Salpeter Equation (BSE). A modified version of the HSE06 screened hybrid functional, that includes 20\% exact Fock exchange (HSE06(20)) as opposed to 25\% in the standard HSE06 functional, is used to set up the starting Hamiltonian for $G_0W_0$+BSE calculations. The HSE06(20) functional accurately predicts the ground state electronic band structure. BSE calculations based on data from $G_0W_0$+HSE06(20) yield direct optical excitation energies and oscillator strengths in excellent agreement with existing experiments and theoretical calculations characterizing direct excitation. In particular, an exciton binding energy of 229 $\pm$ 10 meV is obtained, in close agreement with experiments. The projections of excitonic states onto the quasiparticle band structure in a fatband representation shows that the lowest optical transition of anatase TiO$_2$ consists of excitons originating from the mixing of direct transitions within band pairs running parallel to the $Γ-Z $ direction in the tetragonal Brillouin zone. This implies a strong spatial localization of excitons in the $xy$ plane of the lattice. This investigation highlights the importance of a suitable non-interacting Hamiltonian for the MBPT based quasiparticle $G_0W_0$ and subsequent BSE calculations and suggests HSE06(20) as an optimal choice in the case of anatase TiO$_2$.

cond-mat.mtrl-sci↗