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, KTaO_{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. 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.

Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3.

The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI3 is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI3 using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse's helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI3 and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

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

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.

Photocurrent-driven transient symmetry breaking in the Weyl semimetal TaAs.

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry changes a critical step in developing future technologies that rely on such control. Topological materials, like topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second harmonic generation spectroscopy as a sensitive probe of symmetry changes, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast timescales.

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

We investigate 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.

Temperature-tunable Fano resonance induced by strong coupling between Weyl fermions and phonons in TaAs.

Strong coupling between discrete phonon and continuous electron-hole pair excitations can induce a pronounced asymmetry in the phonon line shape, known as the Fano resonance. This effect has been observed in various systems. Here we reveal explicit evidence for strong coupling between an infrared-active phonon and electronic transitions near the Weyl points through the observation of a Fano resonance in the Weyl semimetal TaAs. The resulting asymmetry in the phonon line shape, conspicuous at low temperatures, diminishes continuously with increasing temperature. This behaviour originates from the suppression of electronic transitions near the Weyl points due to the decreasing occupation of electronic states below the Fermi level (EF) with increasing temperature, as well as Pauli blocking caused by thermally excited electrons above EF. Our findings not only elucidate the mechanism governing the tunable Fano resonance but also open a route for exploring exotic physical phenomena through phonon properties in Weyl semimetals.

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.

Probing the interplay between quantum charge fluctuations and magnetic ordering in LuFe2O4.

The mechanisms producing strong coupling between electric and magnetic order in multiferroics are not always well understood, since their microscopic origins can be quite different. Hence, gaining a deeper understanding of magnetoelectric coupling in these materials is the key to their rational design. Here, we use ultrafast optical spectroscopy to show that the influence of magnetic ordering on quantum charge fluctuations via the double-exchange mechanism can govern the interplay between electric polarization and magnetism in the charge-ordered multiferroic LuFe2O4.

Measurement of two low-temperature energy gaps in the electronic structure of antiferromagnetic USb2 using ultrafast optical spectroscopy.

Ultrafast optical spectroscopy is used to study the antiferromagnetic f-electron system USb(2). We observe the opening of two charge gaps at low temperatures (

Ultrafast optical wide field microscopy.

We have developed a new imaging method, ultrafast optical wide field microscopy, capable of rapidly acquiring wide field images of nearly any sample in a non-contact manner with high spatial and temporal resolution. Time-resolved images of the photoinduced changes in transmission for a patterned semiconductor thin film and a single silicon nanowire after optical excitation are captured using a two-dimensional smart pixel array detector. These images represent the time-dependent carrier dynamics with high sensitivity, femtosecond time resolution and sub-micrometer spatial resolution.

Mapping carrier diffusion in single silicon core-shell nanowires with ultrafast optical microscopy.

Recent success in the fabrication of axial and radial core-shell heterostructures, composed of one or more layers with different properties, on semiconductor nanowires (NWs) has enabled greater control of NW-based device operation for various applications. (1-3) However, further progress toward significant performance enhancements in a given application is hindered by the limited knowledge of carrier dynamics in these structures. In particular, the strong influence of interfaces between different layers in NWs on transport makes it especially important to understand carrier dynamics in these quasi-one-dimensional systems. Here, we use ultrafast optical microscopy (4) to directly examine carrier relaxation and diffusion in single silicon core-only and Si/SiO(2) core-shell NWs with high temporal and spatial resolution in a noncontact manner. This enables us to reveal strong coherent phonon oscillations and experimentally map electron and hole diffusion currents in individual semiconductor NWs for the first time.

Ultrafast carrier dynamics in an InAs/InGaAs quantum dots-in-a-well heterostructure.

Ultrafast differential transmission spectroscopy is used to explore temperature-dependent carrier dynamics in an InAs/InGaAs quantum dots-in-a-well heterostructure. Electron-hole pairs are optically injected into the three dimensional GaAs barriers, after which we monitor carrier relaxation into the two dimensional InGaAs quantum wells and the zero dimensional InAs quantum dots by tuning the probe photon energy. We find that carrier capture and relaxation are dominated by Auger carrier-carrier scattering at low temperatures, with thermal emission playing an increasing role with temperature. Our experiments provide essential insight into carrier relaxation across multiple spatial dimensions.

Ultrafast electron and hole dynamics in germanium nanowires.

We present the first ultrafast time-resolved optical measurements, to the best of our knowledge, on ensembles of germanium nanowires. Vertically aligned germanium nanowires with mean diameters of 18 and 30 nm are grown on (111) silicon substrates through chemical vapor deposition. We optically inject electron-hole pairs into the nanowires and exploit the indirect band structure of germanium to separately probe electron and hole dynamics with femtosecond time resolution. We find that the lifetime of both electrons and holes decreases with decreasing nanowire diameter, demonstrating that surface effects dominate carrier relaxation in semiconductor nanowires.

Enhanced photosusceptibility near Tc for the light-induced insulator-to-metal phase transition in vanadium dioxide.

We use optical-pump terahertz-probe spectroscopy to investigate the near-threshold behavior of the photoinduced insulator-to-metal (IM) transition in vanadium dioxide thin films. Upon approaching Tc a reduction in the fluence required to drive the IM transition is observed, consistent with a softening of the insulating state due to an increasing metallic volume fraction (below the percolation limit). This phase coexistence facilitates the growth of a homogeneous metallic conducting phase following superheating via photoexcitation. A simple dynamic model using Bruggeman effective medium theory describes the observed initial condition sensitivity.

Coupled charge-spin dynamics of the magnetoresistive pyrochlore TI2Mn2O7 probed using ultrafast midinfrared spectroscopy.

Optical-pump midinfrared probe spectroscopy is used to investigate coupled charge-spin dynamics in the magnetoresistive pyrochlore TI(2)Mn(2)O(7). We find that the temporal persistence of the photoexcited carrier density is strongly influenced by spin disorder above and below the ferromagnetic Curie temperature. Our results are consistent with a picture whereby spin disorder leads to spatial segregation of the initially excited Tl 6s-O 2p electron-hole pairs, effectively reducing the probability for recombination. This further implies that colossal magnetoresistance in these materials may be driven primarily by Mn t(2g) spin disorder.

High-speed femtosecond pump-probe spectroscopy with a smart pixel detector array.

A new femtosecond pump-probe spectroscopy technique is demonstrated that permits the high-speed, parallel acquisition of pump-probe measurements at multiple wavelengths. This is made possible by use of a novel, two-dimensional smart pixel detector array that performs amplitude demodulation in real time on each pixel. This detector array can not only achieve sensitivities comparable with lock-in amplification but also simultaneously performs demodulation of probe transmission signals at multiple wavelengths, thus permitting rapid time- and wavelength-resolved femtosecond pump-probe spectroscopy. Measurements on a thin sample of bulk GaAs are performed across 58 simultaneous wavelengths. Differential probe transmission changes as small as approximately 2 x 10(-4) can be measured over a 5-ps delay scan in only approximately 3 min. This technology can be applied to a wide range of pump-probe measurements in condensed matter, chemistry, and biology.

Self-starting mode locking in a Cr:forsterite laser by use of non-epitaxially-grown semiconductor-doped silica films.

We demonstrate RF sputtered, non-epitaxially-grown semiconductor nanocrystallite-doped silica films for mode locking a Cr:forsterite laser. We controlled the size and the optical properties of the nanocrystallites by varying the ratio of InAs to SiO(2) during fabrication. Femtosecond pump-probe measurements were performed to characterize the nonlinear optical properties of these films, revealing their lower saturation fluences. Using the InAs-doped silica films as saturable absorbers permitted self-starting Kerr-lens mode locking (KLM), generating pulses of 25-fs duration with 91-nm spectral bandwidth at 1.3 microm . We also describe saturable-absorber mode-locked operation without KLM and investigate its dependence on intracavity dispersion.