Shining light on complex matter

I am interested in materials that exhibit intriguing behavior originating in microscopic quantum phenomena. These ‘quantum materials‘ possess traits – electronic, spin, orbital, lattice – intertwined by interactions at the atomic scale, that give rise to fascinating emergent behavior.

I study these materials at their fundamental length- and time-scales using a variety of experimental and theoretical tools, including optical spectroscopy, electron and X-ray scattering, and first-principles calculations.

Interrogating exchange pathways in magnetic topological insulators

The emergence of magnetism in topological materials creates a platform to realize spin-based phenomena with applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the identification of enhanced coupling routes between spins and other microscopic degrees of freedom. Bringing together insights from magneto-Raman spectroscopy and optical pump-probe experiments, we discover that phonons can act as a ‘knob’ to control interlayer exchange interaction in the antiferromagnetic topological insulator MnBi2Te4.

Magnetic field-induced interlayer magnetic phase transitions in MnBi2Te4 result in the modulation of A1g Raman phonon scattering intensities, evidence of an interlayer magnetophononic coupling.

Selected publications

Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi2Te4.
H. Padmanabhan, V. A. Stoica, P. K. Kim, M. Poore, T. Yang, X. Shen, A. H. Reid, M-F. Lin, S. Park, J. Yang, H. Wang, N. Z. Koocher, D. Puggioni, L. Min, S. H. Lee, Z. Mao, J. M. Rondinelli, A. M. Lindenberg, L-Q. Chen, X. Wang, R. D. Averitt, J. W. Freeland, V. Gopalan. Advanced Materials 2022.

Interlayer magnetophononic coupling in MnBi2Te4.
H. Padmanabhan*, M. Poore*, P. K. Kim*, N. Z. Koocher, V. A. Stoica, D. Puggioni, H. Wang, X. Shen, A. H. Reid, M. Gu, M. Wetherington, S. H. Lee, R. Schaller, Z. Mao, A. M. Lindenberg, X. Wang, J. M. Rondinelli, R. D. Averitt, V. Gopalan. Nature Communications 2022.

Formation of unconventional ferroelectrics

Ferroelectric materials are characterized by long-range ordering of electric dipoles, realized by spontaneous symmetry breaking across structural phase transitions. I am interested in understanding the mechanisms that stabilize unconventional polar phases in these materials. Nonlinear optics, as a sensitive probe of symmetry breaking, is well suited to the study of such materials and their phase transitions. For example, using nonlinear optical anisotropy and Raman spectroscopy, we find that the seemingly incompatible properties of polar order and metallic conduction are stabilized in LiOsO3 through a decoupling of charge carriers from the polar distortion. In another collaborative study, our nonlinear optical measurements helped design a lead-free ferroelectric material stabilized by rotational distortions.

An image of polar, ferroelastic domains in LiOsO3, measured using a home-built scanning second harmonic generation microscope. The domains are a result of breaking of three-fold rotational symmetry and inversion symmetry across structural transitions.

Selected publications

Linear and nonlinear optical probe of the ferroelectric-like phase transition in a polar metal, LiOsO3.
H. Padmanabhan, Y. Park, D. Puggioni, Y. Yuan, Y. Cao, L. Gasparov, Y. Shi, J. Chakhalian, J. M. Rondinelli, V. Gopalan. Applied Physics Letters 2018.

Hybrid Improper Ferroelectricity in (Sr,Ca)3Sn2O7 and Beyond: Universal Relationship between Ferroelectric Transition Temperature and Tolerance Factor in n = 2 Ruddlesden–Popper Phases.
S. Yoshida, H. Akamatsu, R. Tsuji, O. Hernandez, H. Padmanabhan, A. S. Gupta, A. S. Gibbs, K. Mibu, S. Murai, J. M. Rondinelli, V. Gopalan, K. Tanaka, K. Fujita. Journal of the American Chemical Society 2018.

Symmetry and materials theory

Symmetry is a singularly powerful concept in physics, and lays the foundation for the study of everything from fundamental particles to atomic wavefunctions and crystals. In materials science, point group and space group symmetries are ubiquitous in the description of physical properties. To help extend these ideas to dynamical processes, we formulate the concept of ‘distortion symmetry’. By incorporating distortion symmetry into transition state tools in density functional theory codes, we systematically explore the energy landscape of various processes in materials, revealing new and unexpected dynamical pathways. For example, we apply this to the multiferroic BiFeO3, to help address a physical problem of great interest – switching magnetic moments using an electric field. Using our calculations, we predict competing transient switching pathways that prohibit the deterministic switching of magnetism through an electric field, in agreement with experimental results.

Possible ferroelectric switching pathways in BiFeO3 – one that simultaneously switches the magnetization (right), and one that does not (left). Our calculations show that the two pathways have comparable energy barriers, inhibiting deterministic electric switching of magnetization.

Selected publications

Antisymmetry: Fundamentals and Applications.
H. Padmanabhan*, J. M. Munro*, I. Dabo, V. Gopalan. Annual Review of Materials Research 2020.

Discovering minimum energy pathways via distortion symmetry groups.
J. M. Munro, H. Akamatsu, H. Padmanabhan, V. S. Liu, Y. Shi, L. Q. Chen, B. VanLeeuwen, I. Dabo, V. Gopalan. Physical Review B 2018.

Spatio-Temporal Symmetry—Point Groups with Time Translations.
H. Padmanabhan, M. L. Kingsland, J. M. Munro, D. B. Litvin, V. Gopalan. Symmetry 2017.

Intertwined lattice deformation and magnetism in monovacancy graphene.
H. Padmanabhan, B. R. K. Nanda. Physical Review B 2016.