Y. M. Sheu

Ultrafast carrier dynamics and radiative recombination in multiferroic BiFeO3

We report a comprehensive study of ultrafast carrier dynamics in single crystals of multiferroic BiFeO3. Using degenerate femtosecond optical pump-probe spectroscopy, we find that the photoexcited electrons relax to the conduction band minimum through electron-phonon coupling with a ∼1 ps time constant that does not significantly change across the antiferromagnetic transition. Electrons subsequently leave the conduction band and primarily decay via radiative recombination on a nanosecond timescale, as supported by photoluminescence measurements. We find that despite the coexisting ferroelectric and antiferromagnetic orders in BiFeO3, its intrinsic nature results in carrier relaxation similar to that observed in bulk semiconductors.

Imaging nonequilibrium atomic vibrations with x-ray diffuse scattering.

We use picosecond x-ray diffuse scattering to image the nonequilibrium vibrations in the lattice following ultrafast laser excitation. We present images of nonequilibrium phonons in InP and InSb throughout the Brillouin zone which remain out of equilibrium up to nanoseconds. The results are analyzed using a Born model that helps identify the phonon branches contributing to the observed features in the time-resolved diffuse scattering. In InP this analysis shows a delayed increase in the transverse-acoustic (TA) phonon population along high-symmetry directions accompanied by a decrease in the longitudinal-acoustic phonons. In InSb the increase in TA phonon population is less directional.

Wideband detection of transient solid-state dynamics using ultrafast fiber lasers and asynchronous optical sampling

We demonstrate optical time-domain spectroscopy from femtoseconds to nanoseconds using an ultrafast dual-fiber-laser system with kilohertz continuous scanning rates. Utilizing different wavelengths for the pump and probe beams, we exploit this systems broad range of timescales for quantitative studies of thermal transport and the detection of coherent spin and lattice excitations in epitaxial magnetic thin films. The extraordinary temporal dynamic range provides a way to connect the fast and slow timescales in the observation of dissipation and decoherence processes.

Using ultrashort optical pulses to couple ferroelectric and ferromagnetic order in an oxide heterostructure

A new approach to all-optical detection and control of the coupling between electric and magnetic order on ultrafast timescales is achieved using time-resolved second-harmonic generation (SHG) to study a ferroelectric (FE)/ferromagnet (FM) oxide heterostructure. We use femtosecond optical pulses to modify the spin alignment in a Ba(0.1)Sr(0.9)TiO3 (BSTO)/La(0.7)Ca(0.3)MnO3 (LCMO) heterostructure and selectively probe the ferroelectric response using SHG. In this heterostructure, the pump pulses photoexcite non-equilibrium quasiparticles in LCMO, which rapidly interact with phonons before undergoing spin-lattice relaxation on a timescale of tens of picoseconds. This reduces the spin-spin correlations in LCMO, applying stress on BSTO through magnetostriction. This then modifies the FE polarization through the piezoelectric effect, on a timescale much faster than laser-induced heat diffusion from LCMO to BSTO. We have thus demonstrated an ultrafast indirect magnetoelectric effect in a FE/FM heterostructure mediated through elastic coupling, with a timescale primarily governed by spin-lattice relaxation in the FM layer.

Free-carrier relaxation and lattice heating in photoexcited bismuth

We report ultrafast surface pump and interface probe experiments on photoexcited carrier transport across single crystal bismuth films on sapphire. The film thickness is sufficient to separate carrier dynamics from lattice heating and strain, allowing us to investigate the time scales of momentum relaxation, heat transfer to the lattice, and electron-hole recombination. The measured electron-hole (

Asynchronous optical probing of coherent magnetic excitations from picoseconds to nanoseconds

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Picosecond Time Resolved X-ray Diffraction Measurements of Coherent Phonons and Carrier Dynamics at a Buried Interface

) recombination time is 12--26 ps and ambipolar diffusivity is 18--40 cm

Probing unfolded acoustic phonons with X rays.

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Thermal transport in a semiconductor heterostructure measured by time-resolved x-ray diffraction

/s for carrier excitation up to

Kapitza conductance of Bi/sapphire interface studied by depth- and time-resolved X-ray diffraction

\ensuremath{\sim}{10}^{19}{\text{cm}}^{\ensuremath{-}3}