arXiv subjects

Vivek Unikandanunni

Publications and source records attributed to Vivek Unikandanunni.

9 recordsLinked to original sources

arXiv2026

Anharmonic phonon coupling enabled by local inversion symmetry breaking at domain walls in ferroelastics

In ferroelastic materials, spontaneous symmetry breaking leads to the formation of twin domains. Although the bulk crystal typically remains centrosymmetric, inversion symmetry can be locally broken at the domain walls, potentially changing phonon selection rules and enabling local anharmonic phonon coupling. Here we report direct evidence of such anharmonic coupling in ferroelastic LaAlO$_3$ using two-dimensional Raman-terahertz spectroscopy. We attribute the cross-peaks observed in the two-dimensional spectra to both mechanical and electrical anharmonicity between the $A_{1g}$ Raman-active phonon and the $E_g$ phonon, which acquires finite infrared activity through local inversion symmetry breaking at ferroelastic domain walls. These findings provide new insight into the complex lattice dynamics of ferroelastic materials and highlight the potential of two-dimensional Raman-terahertz spectroscopy to uncover subtle symmetry breaking through the detection of intrinsically weak anharmonic signals.

cond-mat.mtrl-sci↗

arXiv2026

Uniaxial strain-driven ferroelastic domain control in LaAlO3

Multiferroic domain walls in functional oxides exhibit properties distinct from the bulk and are increasingly exploited as active elements in nanoelectronic and photonic devices. Deterministic control of domain populations has typically remained limited to local control, or removal with temperature. Here we demonstrate continuous, reversible manipulation of the ferroelastic domain structure in single-crystal LaAlO$_3$ using in-situ uniaxial strain. Combining atomic force microscopy, X-ray diffraction, and Raman spectroscopy with first-principles calculations we map the complete microscopic evolution of the twin domain population through the strain-driven transition from the rhombohedral $R\bar{3}c$ ground state toward the predicted orthorhombic $Fmmm$ phase. Applied strains below $0.5\%$ produce pronounced surface flattening and large-scale domain reorganisation, establishing uniaxial strain as a technically accessible control parameter for ferroelastic domain engineering. These results open a route to active, real-time programming of domain architectures in LaAlO$_3$-based heterostructures, with implications for strain-tunable superconducting interfaces, nanoscale phonon-polariton optics, and ultrafast lattice control.

cond-mat.mtrl-sci↗

arXiv2025

Intrinsic non-Markovian magnetisation dynamics

Memory effects arise in many complex systems, from protein folding, to the spreading of epidemics and financial decisions. While so-called non-Markovian dynamics is common in larger systems with interacting components, observations in fundamental physical systems have been confined to specifically engineered cases. Here, we report the experimental observation of non-Markovian dynamics in an elemental material, crystalline cobalt. By driving this material with an intense terahertz electromagnetic field, we bring its magnetisation into a non-equilibrium state and follow its evolution. We measure the sample's low temperature magnetic response in the time domain which leads to an unexpectedly rich multi-peaked spectrum in the Fourier domain, that cannot be explained by established models. We use open quantum system theory, which predicts a non-Markovian memory kernel in the dynamical equations to capture the fundamental interaction between the spin system and the phonon bath. Simulations based on this theory produce a multi-peaked spectrum, which matches the measured one. Our non-Markovian approach is also able to reproduce the modification of the spectrum at higher temperatures. Our findings demonstrate that non-Markovian effects are observable at a much more fundamental level than previously thought, opening the door to their exploration and control in a broad range of condensed matter systems.

quant-ph↗

arXiv2024

Terahertz ionic Kerr effect: Two-phonon contribution to the nonlinear optical response in insulators

The THz Kerr effect measures the birefringence induced in an otherwise isotropic material by a strong THz pulse driving the Raman-active excitations of the systems. Here we provide experimental evidence of a sizable Kerr response in insulating SrTiO3 due to infrared-active lattice vibrations. Such a signal, named ionic Kerr effect, is associated with the simultaneous excitation of multiple phonons. Thanks to a theoretical modeling of the time, polarization and temperature dependence of the birefringence we can disentangle the ionic Kerr effect from the off-resonant electronic excitations, providing an alternative tunable mechanism to modulate the refractive index on ultrashort time-scales via infra-red active phonons.

cond-mat.mtrl-sci↗

arXiv2024

Characterizing the Nonequilibrium Response of FeRh Thin Films using Time-Domain Thermoreflectance (TDTR)

Time-Domain Thermoreflectance (TDTR) characterization of FeRh throughout its first-order antiferromagnetic (AF) to ferromagnetic (FM) transition shows that the transient reflectance, $Δ$R(t)/R, strongly depends on the magnetic order of the sample. Using TDTR, which uses optical pulses to induce small temperature excursions, we have found that the $Δ$R(t)/R of the AF phase exhibits a large negative response, while the response of the FM phase is positive. This magnetic phase sensitivity has allowed us to study the transient response of both the AF and FM phase to the pump pulse excitation and the mixed phase of the material. These results are significant since the ultrafast properties of antiferromagnetic materials and mixed antiferromagnetic and ferromagnetic materials are difficult to detect using other conventional techniques.We have found that the AF phase exhibits a strong subpicosecond signal not observed in the FM phase. The magnetic phase dependence of the sign of $Δ$R(t)/R is qualitatively explained using the results of ab-initio density functional theory (DFT) calculations. Using the two-temperature model, we found that the change in the thermalization time across the transition is caused by differences in both the electronic heat capacity and the electron-phonon coupling factor of the AF and FM phases. The electron-phonon coupling constant in the AF phase is also determined using the two-temperature model conducted using the NTMpy code package. For the FM phase, we provide boundaries for the magnitude of the electron-phonon coupling factor for the FM phase. These results indicate that TDTR can be used to study the transient properties of magnetic materials that are otherwise challenging to probe.

cond-mat.mtrl-sci↗

arXiv2021

Inertial spin dynamics in epitaxial cobalt films

We investigate the spin dynamics driven by terahertz magnetic fields in epitaxial thin films of cobalt in its three crystalline phases. The terahertz magnetic field generates a torque on the magnetization which causes it to precess for about 1 ps, with a sub-picosecond temporal lag from the driving force. Then, the magnetization undergoes natural damped THz oscillations at a frequency characteristic of the crystalline phase. We describe the experimental observations solving the inertial Landau-Lifshitz-Gilbert equation. Using the results from the relativistic theory of magnetic inertia, we find that the angular momentum relaxation time $η$ is the only material parameter needed to describe all the experimental evidence. Our experiments suggest a proportionality between $η$ and the strength of the magneto-crystalline anisotropy.

cond-mat.mes-hall↗

arXiv2021

Ultrafast electron dynamics in platinum and gold thin films driven by optical and terahertz fields

We investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically-induced dynamics of both films and can be described by a two-temperature model. Surprisingly, gold can exhibit a much smaller terahertz pulse-induced reflectivity change and with opposite sign. For platinum, we estimate a 20% larger electron-phonon coupling for the terahertz-driven dynamics compared to the optically-induced one, which we ascribe to an additional nonthermal electron-phonon coupling contribution. We explain the remarkable response of gold to terahertz radiation with the field emission of electrons due the Fowler-Nordheim tunneling process, in samples with thickness below the structural percolation threshold where near-field enhancement is possible. Our results provide a fundamental insight into the ultrafast processes relevant to modern electro- and magneto-optical applications.

cond-mat.mtrl-sci↗

arXiv2020

Anisotropic Ultrafast Spin Dynamics in Epitaxial Cobalt

We investigate the ultrafast spin dynamics in an epitaxial hcp(1100) cobalt thin film. By performing pump-probe magneto-optical measurements with the magnetization along either the easy or hard magnetic axis, we determine the demagnetization and recovery times for the two axes. We observe a 35% slower dynamics along the easy magnetization axis, which we attribute to magneto-crystalline anisotropy of the electron-phonon coupling, supported by our ab initio calculations. This points towards an unambiguous and previously undisclosed role of anisotropic electron-lattice coupling in ultrafast magnetism.

cond-mat.mes-hall↗

arXiv2020

NTMpy: An open source package for solving coupled parabolic differential equations in the framework of the three-temperature model

The NTMpy code package allows for simulating the one-dimensional thermal response of multilayer samples after optical excitation, as in a typical pump-probe experiment. Several Python routines are combined and optimized to solve coupled heat diffusion equations in one dimension, on arbitrary piecewise homogeneous material stacks, in the framework of the so-called three-temperature model. The energy source deposited in the material is modelled as a light pulse of arbitrary cross-section and temporal profile. A transfer matrix method enables the calculation of realistic light absorption in presence of scattering interfaces as in multilayer samples. The open source code is fully object-oriented to enable a user-friendly and intuitive interface for adjusting the physically relevant input parameters. Here, we describe the mathematical background of the code, we lay out the workflow, and we validate the functionality of our package by comparing it to commercial software, as well as to experimental transient reflectivity data recorded in a pump-probe experiment with femtosecond light pulses.

cond-mat.other↗