Diffusion-Dominated Luminescence Dynamics of CsPbBr3 Studied Using Cathodoluminescence and Microphotoluminescence Spectroscopy.

Time-resolved or time-correlation measurements using cathodoluminescence (CL) reveal the electronic and optical properties of semiconductors, such as their carrier lifetimes, at the nanoscale. However, halide perovskites, which are promising optoelectronic materials, exhibit significantly different decay dynamics in their CL and photoluminescence (PL). We conducted time-correlation CL measurements of CsPbBr3 using Hanbury Brown-Twiss interferometry and compared them with time-resolved PL. The measured CL decay time was on the order of subnanoseconds and was faster than PL decay at an excited carrier density of 2.1 × 1018 cm-3. Our experiment and analytical model revealed the CL dynamics induced by individual electron incidences, which are characterized by highly localized carrier generation followed by a rapid decrease in carrier density due to diffusion. This carrier diffusion can play a dominant role in the CL decay time for undoped semiconductors, in general, when the diffusion dynamics are faster than the carrier recombination.

Attosecond-Resolved Coherent Control of Lattice Vibrations in Thermoelectric SnSe.

Manipulating lattice vibrations is the cornerstone to achieving ultralow thermal conductivity in thermoelectrics. Although spatial control by novel material designs has been recently reported, temporal manipulation, which can shape thermoelectric properties under nonequilibrium conditions, remains largely unexplored. Here, taking SnSe as a representative, we have demonstrated that in the ultrafast pump-pump-probe spectroscopy, electronic and lattice coherences inherited from optical excitations can be exploited independently to manipulate phonon oscillations in a highly selective manner. Specifically, when the pump-pump delay time (tmod) is in the electronic coherence time range, the amplitude, frequency, and lifetime of all phonon modes are simultaneously following the optical cycle. While extending tmod into the lattice coherence time range, the amplitude of each coherent phonon mode can be selectively manipulated according to its intrinsic period without changing the frequency and lifetime. This work opens up exciting avenues to temporally and discriminatorily manipulate phononic processes in thermoelectric materials.

Photoinduced Ultrafast Symmetry Switch in SnSe.

Layered tin selenide (SnSe) has recently emerged as a high-performance thermoelectric material with the current record for the figure of merit (ZT) observed in the high-temperature Cmcm phase. So far, access to the Cmcm phase has been mainly obtained via thermal equilibrium methods based on sample heating or application of external pressure, thus restricting the current understanding only to ground-state conditions. Here, we investigate the ultrafast carrier and phononic dynamics in SnSe. Our results demonstrate that optical excitations can transiently switch the point-group symmetry of the crystal from Pnma to Cmcm at room temperature in a few hundreds of femtoseconds with an ultralow threshold for the excitation carrier density. This nonequilibrium Cmcm phase is found to be driven by the displacive excitation of coherent Ag phonons and, given the absence of low-energy thermal phonons, exists in SnSe with the status of 'cold lattice with hot carriers'. Our findings provide an important insight for understanding the nonequilibrium thermoelectric properties of SnSe.

Microstructural deformation process of shock-compressed polycrystalline aluminum.

Plastic deformation of polycrystalline materials under shock wave loading is a critical characteristic in material science and engineering. However, owing to the nanosecond time scale of the shock-induced deformation process, we currently have a poor mechanistic understanding of the structural changes from atomic scale to mesoscale. Here, we observed the dynamic grain refinement of polycrystalline aluminum foil under laser-driven shock wave loading using time-resolved X-ray diffraction. Diffraction spots on the Debye-Scherrer ring from micrometer-sized aluminum grains appeared and disappeared irregularly, and were shifted and broadened as a result of laser-induced shock wave loading. Behind the front of shock wave, large grains in aluminum foil were deformed, and subsequently exhibited grain rotation and a reduction in size. The width distribution of the diffraction spots broadened because of shock-induced grain refinement and microstrain in each grain. We performed quantitative analysis of the inhomogeneous lattice strain and grain size in the shocked polycrysalline aluminum using the Williamson-Hall method and determined the dislocation density under shock wave loading.

Coherent control theory and experiment of optical phonons in diamond.

The coherent control of optical phonons has been experimentally demonstrated in various physical systems. While the transient dynamics for optical phonons can be explained by phenomenological models, the coherent control experiment cannot be explained due to the quantum interference. Here, we theoretically propose the generation and detection processes of the optical phonons and experimentally confirm our theoretical model using the diamond optical phonon by the doublepump-probe type experiment.

Bandgap modulation in photoexcited topological insulator Bi2Te3 via atomic displacements.

The atomic and electronic dynamics in the topological insulator (TI) Bi2Te3 under strong photoexcitation were characterized with time-resolved electron diffraction and time-resolved mid-infrared spectroscopy. Three-dimensional TIs characterized as bulk insulators with an electronic conduction surface band have shown a variety of exotic responses in terms of electronic transport when observed under conditions of applied pressure, magnetic field, or circularly polarized light. However, the atomic motions and their correlation between electronic systems in TIs under strong photoexcitation have not been explored. The artificial and transient modification of the electronic structures in TIs via photoinduced atomic motions represents a novel mechanism for providing a comparable level of bandgap control. The results of time-domain crystallography indicate that photoexcitation induces two-step atomic motions: first bismuth and then tellurium center-symmetric displacements. These atomic motions in Bi2Te3 trigger 10% bulk bandgap narrowing, which is consistent with the time-resolved mid-infrared spectroscopy results.

Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5.

Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization.

Measuring quantum coherence in bulk solids using dual phase-locked optical pulses.

Electronic and phonon coherence are usually measured in different ways because their time-scales are very different. In this paper we simultaneously measure the electronic and phonon coherence using the interference of the electron-phonon correlated states induced by two phase-locked optical pulses. Interferometric visibility showed that electronic coherence remained in a semiconducting GaAs crystal until ~40 fs; in contrast, electronic coherence disappeared within 10 fs in a semimetallic Bi crystal at room temperature, differing substantially from the long damping time of its phonon coherence, in the picosecond range.

Optical manipulation of coherent phonons in superconducting YBa2Cu3O7-delta thin films.

The coherent phonons of YBa2Cu3O7-delta are believed to be strongly coupled to its superconductivity. Controlling the phonons below its transition temperature, therefore, may serve as a promising scheme of the control of superconductivity. Here we demonstrate optical manipulation of the Ba-O and Cu-O vibrations in a thin-film YBa2Cu3O7-delta below its transition temperature using a pair of femtosecond laser pulses. The interpulse delay is tuned to integral and half-integral multiples of the oscillation period of a specific phonon mode (Ba-O or Cu-O vibration) to enhance and suppress its amplitude, respectively.

Ultrafast zone-center coherent lattice dynamics in ferroelectric lithium tantalate.

Femtosecond time-resolved pump-probe experiments were carried out to study ultrafast lattice dynamics of ferroelectric lithium tantalate. Both the fully symmetric (A1 mode) and doubly degenerate (E mode) coherent phonons at the center of the Brillouin zone were excited via impulsive stimulated Raman scattering, as confirmed by the excitation intensity dependence.

Pathway for the transformation from highly oriented pyrolytic graphite into amorphous diamond.

We report the discovery of a novel pathway for the transformation from highly oriented pyrolytic graphite foils into amorphous diamond platelets. This pathway consists of three stages of neutron irradiation, shock compression, and rapid quenching. We obtained transparent platelets which show photoluminescence but no diamond Raman peak, similar to the case of amorphous diamond synthesized from C60 fullerene. Wigner defects formed by irradiation are considered to make a high density of diamond nucleation sites under shock compression, of which growth is suppressed by rapid quenching.

Diagnostic system to measure spatial and temporal profiles of shock front using compact two-stage light-gas gun and line reflection method.

A diagnostic system has been developed to obtain spatial and temporal profiles of shock front. A two-stage light-gas gun is used to accelerate impactors in velocity range with 4-9 km/s. The system consists of the Faraday-type electromagnetic sensors to measure impactor velocity, optical system with high-speed streak camera to measure shock-wave velocities, and the delay trigger system with self-adjustable pre-event pulse generator. We describe the specifications and performance of this system and data-analysis technique on the tilt and distortion of the shock front. Finally, we obtained the Hugoniot data of copper for system demonstration.

Nanosecond rapid freezing of liquid benzene under shock compression studied by time-resolved coherent anti-Stokes Raman spectroscopy.

Nanosecond time-resolved coherent anti-Stokes Raman spectroscopy is used to investigate the shock-induced liquid-solid phase transition and crystallization of liquid benzene. Temporal evolution of the Raman shift of the ring-breathing and C-H stretching modes is investigated. A metastable supercompressed state and a liquid-solid phase transition are observed under shock compression. Time-resolved Raman spectra reveal that the liquid state is initially a metastable state and rapidly transforms to the solid state within 25 ns under shock compression at 4.2 GPa.