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Prasankumar, R. P.

Publications and source records attributed to Prasankumar, R. P..

13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Ultrafast Suppression of the Ferroelectric Instability in KTaO 3

We use an x-ray free-electron laser to study the lattice dynamics following photoexcitation with ultrafast near-UV light (wavelength 266 nm, 50 fs pulse duration) of the incipient ferroelectric potassium tantalate, KT a O 3 . By probing the lattice dynamics corresponding to multiple Brillouin zones through the x-ray diffuse scattering with pulses from the Linac Coherent Light Source (LCLS) (wavelength 1.3 Å and < 10 fs pulse duration), we observe changes in the diffuse intensity associated with a hardening of the transverse acoustic phonon branches along Γ to X and Γ to M. Using force constants from density functional theory, we fit the quasiequilibrium intensity and obtain the instantaneous lattice temperature and density of photoexcited charge carriers. Additionally, the density functional theory calculations demonstrate that photoexcitation transfers charge from oxygen 2p derived π-bonding orbitals to Ta 5d derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Direct Observation of Coherent Longitudinal and Shear Acoustic Phonons in TaAs Using Ultrafast X-Ray Diffraction

Here, using femtosecond time-resolved x-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral line shape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Tracking Ultrafast Photocurrents in the Weyl Semimetal TaAs Using THz Emission Spectroscopy

We investigate here polarization-dependent ultrafast photocurrents in the Weyl semimetal TaAs using terahertz (THz) emission spectroscopy. Our results reveal that highly directional, transient photocurrents are generated along the noncentrosymmetric c axis regardless of incident light polarization, while helicity-dependent photocurrents are excited within the ab plane. This is consistent with earlier static photocurrent experiments, and demonstrates on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry of the transition metal monopnictide family of Weyl semimetals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Unraveling thickness-dependent spin relaxation in colossal magnetoresistance manganite films

In this paper, we used ultrafast optical spectroscopy to study photoinduced spin relaxation in 10–100 nm thick La 0.7 Ca 0.3 MnO 3 films. The spin-lattice relaxation time displays a strong dependence on thickness below the Curie temperature. Our simulations show that the observed thickness-dependent relaxation results from much faster thermal decay through the substrate in thinner films that leads to artificially faster demagnetization. Furthermore, we provide an analytical approach to gain insight into the spin-lattice relaxation time for highly thermal dissipative films. Finally, our study strongly suggests that careful consideration of the influence of transient thermal variations on photoinduced demagnetization is mandatory when incorporating absorbing thin magnetic films into heterostructures and devices.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Probing and controlling terahertz-driven structural dynamics with surface sensitivity

Intense, single-cycle terahertz (THz) pulses are powerful tools to understand and control material properties through low-energy resonances, such as phonons. Combining this with optical second harmonic generation (SHG) makes it possible to observe the resulting ultrafast structural changes with surface sensitivity. This makes SHG an ideal method to probe phonon dynamics in topological insulators (TI), materials with unique surface transport properties. Here, we resonantly excite a phonon mode in the TI Bi 2 Se 3 with THz pulses and use SHG to separate the resulting symmetry changes at the surface from the bulk. Furthermore, we coherently control the lattice vibrations with a pair of THz pulses. Lastly, our work demonstrates a versatile, table-top tool to probe and control phonon dynamics in a range of systems, particularly at surfaces and interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Probing ultrafast spin dynamics through a magnon resonance in the antiferromagnetic multiferroic HoMnO 3

Here, we demonstrate an approach for directly tracking antiferromagnetic (AFM) spin dynamics by measuring ultrafast changes in a magnon resonance. We also test this idea on the multiferroic HoMnO 3 by optically photoexciting electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced change in the magnon line shape that builds up over 5–12 picoseconds, which we show to be the spin-lattice thermalization time, indicating that electrons heat the spins via phonons. We compare our results to previous studies of spin-lattice thermalization in ferromagnetic manganites, giving insight into fundamental differences between the two systems. Finally, our work sheds light on the microscopic mechanism governing spin-phonon interactions in AFMs and demonstrates a powerful approach for directly monitoring ultrafast spin dynamics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Optical spectroscopy of the Weyl semimetal TaAs

Here, we present a systematic study of both the temperature and frequency dependence of the optical response in TaAs, a material that has recently been realized to host the Weyl semimetal state. Our study reveals that the optical conductivity of TaAs features a narrow Drude response alongside a conspicuous linear dependence on frequency. The weight of the Drude peak decreases upon cooling, following a T 2 temperature dependence, in good agreement with theoretical predictions. Two linear components with distinct slopes dominate the low-temperature optical conductivity. A comparison between our experimental results and theoretical calculations suggests that the linear conductivity below ~230 cm –1 arises purely from interband transitions near the Weyl points, providing rich information about the Weyl semimetal state in TaAs.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Hall effect in the extremely large magnetoresistance semimetal WTe{sub 2}

We systematically measured the Hall effect in the extremely large magnetoresistance semimetal WTe{sub 2}. By carefully fitting the Hall resistivity to a two-band model, the temperature dependencies of the carrier density and mobility for both electron- and hole-type carriers were determined. We observed a sudden increase in the hole density below ∼160 K, which is likely associated with the temperature-induced Lifshitz transition reported by a previous photoemission study. In addition, a more pronounced reduction in electron density occurs below 50 K, giving rise to comparable electron and hole densities at low temperature. Our observations indicate a possible electronic structure change below 50 K, which might be the direct driving force of the electron-hole “compensation” and the extremely large magnetoresistance as well. Numerical simulations imply that this material is unlikely to be a perfectly compensated system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Ultrafast carrier dynamics in the large-magnetoresistance material WTe 2

In this study, ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large-magnetoresistance material WTe 2 . Our experiments reveal a fast relaxation process occurring on a subpicosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of ~5–15 ps, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the time scale governing this process increases due to the reduction of the phonon population. However, below ~50 K, an unusual decrease of the recombination time sets in, most likely due to a change in the electronic structure that has been linked to the large magnetoresistance observed in this material.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Terahertz magneto-optical spectroscopy of a two-dimensional hole gas

Two-dimensional hole gases (2DHGs) have attracted recent attention for their unique quantum physics and potential applications in areas including spintronics and quantum computing. However, their properties remain relatively unexplored, motivating the use of different techniques to study them. We then used terahertz magneto-optical spectroscopy to investigate the cyclotron resonance frequency in a high mobility 2DHG, revealing a nonlinear dependence on the applied magnetic field. This is shown to be due to the complex non-parabolic valence band structure of the 2DHG, as verified by multiband Landau level calculations. We also found that impurity scattering dominates cyclotron resonance decay in the 2DHG, in contrast with the dominance of superradiant damping in two-dimensional electron gases. Our results shed light on the properties of 2DHGs, motivating further studies of these unique 2D nanosystems.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Time-resolved terahertz dynamics in thin films of the topological insulator Bi 2 Se 3

We use optical pump–THz probe spectroscopy at low temperatures to study the hot carrier response in thin Bi 2 Se 3 films of several thicknesses, allowing us to separate the bulk from the surface transient response. We find that for thinner films the photoexcitation changes the transport scattering rate and reduces the THz conductivity, which relaxes within 10 picoseconds (ps). For thicker films, the conductivity increases upon photoexcitation and scales with increasing both the film thickness and the optical fluence, with a decay time of approximately 5 ps as well as a much higher scattering rate. Furthermore, these different dynamics are attributed to the surface and bulk electrons, respectively, and demonstrate that long-lived mobile surface photo-carriers can be accessed independently below certain film thicknesses for possible optoelectronic applications.

36 MATERIALS SCIENCE↗