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We present a novel and simple picture of the generation dynamics of coherent longitudinal optical (LO) phonons and LO-phonon-plasmon-coupled (LOPC) modes by the ultrafast infrared pump-pulses in gallium arsenide (GaAs) employing the low-temperature approximation. LO phonons exhibit a pronounced coupling with plasmons formed by the optically excited electrons in the excited states of GaAs. This coupling results in the coherent oscillation of the LOPC modes in the excited states. The pump pulse also induces stimulated Raman scattering, which generates the coherent LO-phonon oscillation in the ground state. This picture is incorporated into a simplified model, and the time evolution of the density operator is calculated using the Lindblad-type quantum master equation. The theoretical results explain well the reported experimental results on the coherent oscillation of LO phonons and LOPC modes observed through transient reflection measurements. Above all, our model provides a natural reason for the simultaneous manifestation of the LO phonons and the LOPC modes., Comment: 6+2 pages, 3 figures

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 of 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 non-equilibrium 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 important insight for understanding non-equilibrium thermoelectric properties of SnSe., Comment: 4 figures

Coherent control is an optical technique to manipulate quantum states of matter. The coherent control of 40-THz optical phonons in diamond was demonstrated by using a pair of sub-10-fs optical pulses. The optical phonons were detected via transient transmittance using a pump and probe protocol. The optical and phonon interferences were observed in the transient transmittance change and its behavior was well reproduced by quantum mechanical calculations with a simple model which consists of two electronic levels and shifted harmonic oscillators., Comment: 5 pages, 6 figures

Optical dual-pulse pumping actively creates quantum-mechanical superposition of the electronic and phononic states in a bulk solid. We here made transient reflectivity measurements in an n-GaAs using a pair of relative-phase-locked femtosecond pulses and found characteristic interference fringes. This is a result of quantum-path interference peculiar to the dual-pulse excitation as indicated by theoretical calculation. Our observation reveals that the pathway of coherent phonon generation in the n-GaAs is impulsive stimulated Raman scattering at the displaced potential due to the surface-charge field, even though the photon energy lies in the opaque region., Comment: 6 + 4 pages, 5 + 3 figures

The coupling between longitudinal optical (LO) phonons and plasmons plays a fundamental role in determining the performance of doped semiconductor devices. In this work, we report a comparative investigation into the dependence of the coupling on temperature and doping in n- and p-type GaAs by using ultrafast optical phonon spectroscopy. A suppression of coherent oscillations has been observed in p-type GaAs at lower temperature, strikingly different from n-type GaAs and other materials in which coherent oscillations are strongly enhanced by cooling. We attribute this unexpected observation to a cooling-induced elongation of the depth of the depletion layer which effectively increases the screening time of surface field due to a slow diffusion of photoexcited carriers in p-type GaAs. Such an increase breaks the requirement for the generation of coherent LO phonons and, in turn, LO phonon-plasmon coupled modes because of their delayed formation in time., Comment: 18 pages, 4 figures

Fully symmetric A1g phonons are expected to play a dominant role in electron scattering in strong topological insulators (TIs), thus limiting the ballistic transport of future electronic devices. Here, we report on femtosecond time-resolved observation of a pair of A1g coherent phonons and their optical control in two strong 3D TIs, Bi2Te3 and Bi2Se3, by using a second pump pulse in ultrafast spectroscopy measurements. Along with well-defined phonon properties such as frequency and lifetime, an obvious phonon chirp has been observed, implying a strong coupling between photo-carriers and lattices. The coherent phonon manipulation, on the other hand, allows us to change the phonon amplitude selectively but does not affect either the frequency or coherence lifetime of the chosen mode., Comment: 18 pages, 4 figures

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 double-pump-probe type experiment., Comment: 11 pages, 5 figures

Coherent optical phonons in bulk solid system play a crucial role in understanding and designing light-matter interactions and can be detected by the transient-reflectivity measurement. In this paper, we demonstrate spectrally resolved detection of coherent optical phonons in diamond from ultrashort infrared pump-probe measurements using optical band-pass filters. We show that this enhances the sensitivity approximately 35 times in measuring the coherent oscillations in the transient reflectivity compared with the commonly used spectrally integrated measurement. To explain this observation, we discuss its mechanism., Comment: 8 pages, 4 figures

We investigated the coherent phonon generation mechanism by irradiation of an ultrashort pulse with a simple two-level model. Our derived formulation shows that both impulsive stimulated Raman scattering (ISRS) and impulsive absorption (IA) simultaneously occur, and phonon wave packets are generated in the electronic ground and excited states by ISRS and IA, respectively. We identify the dominant process from the amplitude of the phonon oscillation. For short pulse widths, ISRS is very small and becomes larger as the pulse width increases. We also show that the initial phase is dependent on the pulse width and the detuning., Comment: 8 pages, 6 figures

With the aid of nanosecond time-resolved X-ray diffraction techniques, we have explored the complex structural dynamics of bismuth under laser-driven compression. The results demonstrate that shocked bismuth undergoes a series of structural transformations involving four solid structures: the Bi-I, Bi-II, Bi-III and Bi-V phases. The transformation from the Bi-I phase to the Bi-V phase occurs within 4 ns under shock compression at ~11 GPa, showing no transient phases with the available experimental conditions. Successive phase transitions (Bi-V->Bi-III->Bi-II->Bi-I) during the shock release within 30 ns have also been resolved, which were inaccessible using other dynamic techniques., Comment: 17 pages, 4 figures, Appl. Phys. Lett. accepted

The high-pressure phase stability of the metastable tetragonal zirconia is still under debate. The transition dynamics of shocked Y2O3 (3 mol%) stabilized tetragonal zirconia ceramics under laser-shock compression has been directly studied using nanosecond time-resolved X-ray diffraction. The martensitic phase transformation to the monoclinic phase, which is the stable phase for pure zirconia at ambient pressure and room temperature, has been observed during compression at 5 GPa within 20 ns without any intermediates. This monoclinic phase reverts back to the tetragonal phase during pressure release. The results imply that the stabilization effect due to addition of Y2O3 is negated by the shear stress under compression., Comment: 11 pages, 4 figures, draft

Coherent control experiments using a pair of collinear femtosecond laser pulses have been carried out to manipulate longitudinal optical (LO) phonon-plasmon coupled (LOPC) modes in both p- and n-type GaAs. By tuning the interpulse separation, remarkably distinct responses have been observed in the two samples. To understand the results obtained a phenomenological model taking the delayed formation of coherent LOPC modes into account is proposed. The model suggests that the lifetime of coherent LOPC modes plays a key role and the interference of the coherent LO phonons excited successively by two pump pulses strongly affects the manipulation of coherent LOPC modes., Comment: 19 pages, 6 figures, accepted for publication in Phys. Rev. B

A coherent two-phonon bound state has been impulsively generated in ZnTe(110) via second-order Raman scattering in the time domain for the first time. The two-phonon bound state, composed of two anticorrelated in wave vector acoustic phonons, exhibits full {\Gamma}1 symmetry and has energy higher than the corresponding 2TA(X) overtone. By suppressing two-phonon fluctuations with a double-pulse excitation, the coexistence of coherently excited bound and unbound two-phonon states has been demonstrated., Comment: 14 pages, 4 figures, This paper is accepted for publication in Phys. Rev. B

When ultrafast laser pulse strikes the crystal with a van Hove singularity in the phonon density of states, it can create a pair of anti-correlated in wave-vector acoustic phonons. As a result, the atomic fluctuations in either position or momentum become squeezed in such a way that their size might fall below the vacuum level. The ultrafast pulses can also generate a two-phonon bound (biphonon) state in which the constituent phonons are correlated and/or entangled. Here we show that via the interplay between one- and two-phonon interference the bound and squeezed two-phonon state in (110) oriented ZnTe single crystal can be manipulated. We demonstrate experimentally that when two biphonon ensembles are temporally and spatially overlapped, the strength of phonon squeezing and correlation can be controlled. However, due to the complementarity of one- and two-phonon interference a larger correlation comes at the expense of a reduced squeezing.