Coherent Optical Phonons Research Articles

Terahertz electromagnetic waves radiated from coherent longitudinal optical (LO) phonons and LO-phonon plasmon coupled modes in (001)-, (110)-, and (111)-oriented semi-insulating GaAs single crystals

We report on terahertz electromagnetic waves from coherent longitudinal optical (LO) phonons and coherent LO-phonon plasmon coupled (LOPC) modes in (001)-, (110)-, and (111)-oriented semi-insulating GaAs single crystals. The coherent LO phonons and coherent LOPC modes are observed in the three samples. In contrast, coherent transverse optical (TO) phonons are not observed in the (110)- and (111)-oriented samples in spite of that the TO phonon is the Raman active mode. We conclude that only the coherent longitudinal oscillating polarization such as coherent LO phonons and coherent LOPC modes radiate the terahertz wave and that the Raman selection rule does not contribute to the terahertz-wave-radiation process. The photogenerated electron-density dependence of the frequencies of the coherent LOPC mode is almost the same in the three samples. This finding indicates that the coupling of the LO phonon with the plasmon is not influenced by the surface orientations of the three samples.

Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites

AbstractHybrid organic–inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy‐relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time‐resolved optical spectroscopy is performed, with off‐resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off‐resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the Ag vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead–iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.

Detection of coherent optical phonons in a thin bismuth film by ultrafast electron diffraction

Coherent dynamics of lattice oscillations in a ∼20-nm-thick film obtained by thermal sputtering of bismuth is studied using ultrashort electron bunches synchronised with femtosecond laser pulses irradiating the sample. The Fourier analysis of ultrafast electron diffraction (UED) data shows that the observed modulation of the signal is due to the ensemble of modes corresponding to optical phonons with frequencies of approximately 3, 6 and 9 THz. A conclusion is made that these peaks correspond to the manifestation of the bismuth A1g mode (three-terahertz peak), as well as its first and second overtones, which is probably due to quantum confinement in a 20-nm Bi nanostructure. The possibility of a detailed study of the quantum-size effect in bismuth with the help of a transmission UED is analysed.

Another transfer channel for shock energy flowing into intra-molecular: the coherent transfer channel

In this paper, we have proposed that there is another transfer channel for shock energy flowing into to intra-molecular vibration mode. During this energy transfer process, these higher frequency vibrations would gradually possess a coherence at the direction of shock wave. Namely, these optical phonons could be coherent after shock wave compressed. Based on the probe light can be scattered by the coherent optical phonons, a series of light scattering experiments at varying detection angles were performed to explore the existing evidence of coherent optical phonon in shocked materials. No matter the incident angle is 6.2° or 15.7°, the Signal intensity ratio γs and the line width Γ of compressed vibration were both showed peak value around the corresponding phase matching angle which was attributed to the contribution of coherent optical phonons. Taken together, these experimental results demonstrated the existence of new proposed shock energy transfer channel, that coherent transfer channel, and open new perspectives in the molecular dissociation channel research in shocked materials.

Hot carrier dynamics and phonon anharmonicity of ZrTe5 revealed with femtosecond transient optical spectroscopy

We present a time-resolved ultrafast optical spectroscopy study on thermoelectric material ${\mathrm{ZrTe}}_{5}$, regarding its carrier decay dynamics and anharmonic decay of coherent optical phonons at 5--280 K. A reflectivity time series consists of a single exponential decay due to the relaxation of carriers via electron-phonon coupling and decaying oscillations due to coherent phonon vibration of the ${A}_{g}$ mode. The carrier decay characteristics follow the temperature-induced electronic transitions of ${\mathrm{ZrTe}}_{5}$. The coherent optical phonon vibrations can be well described with the anharmonicity model including lattice thermal expansion and phonon-phonon coupling. The phonon vibration frequency and dephasing time are obtained as a function of temperature, and decrease with increasing temperature. The effects of pump fluence are also explored.

Excitation of coherent optical phonons in iron garnet by femtosecond laser pulses

We employed femtosecond pump-probe technique to investigate the dynamics of coherent optical phonons in iron garnet. A phenomenological symmetry-based consideration reveals that oscillations of the terahertz T2g mode are excited. Selective excitation by a linearly polarized pump and detection by a circularly polarized probe confirm that impulsive stimulated Raman scattering (ISRS) is the driving force for the coherent phonons. Experimental results obtained from ISRS measurements reveal excellent agreement with spontaneous Raman spectroscopy data, analyzed by considering the symmetry of the phonon modes and corresponding excitation and detection selection rules.

Terahertz Driven Amplification of Coherent Optical Phonons in GaAs Coupled to a Metasurface.

We demonstrate amplification of longitudinal optical (LO) phonons by polar-optical interaction with an electron plasma in a GaAs structure coupled to a metallic metasurface using two-color two-dimensional spectroscopy. In a novel scheme, the metamaterial resonator enhances broadband terahertz fields, which generate coherent LO phonons and drive free electrons in the conduction band of GaAs. The time evolution of the LO phonon amplitude is monitored with midinfrared pulses via the LO-phonon-induced Kerr nonlinearity of the sample, showing an amplification of the LO phonon amplitude by up to a factor of 10, in agreement with a theoretical estimate.

Characteristics of Coherent Optical Phonons in a Hexagonal YMnO3 Thin Film

This paper reviews our recent study on a coherent optical phonon in a hexagonal YMnO3 thin film together with related optical studies in hexagonal RMnO3 (R = Y, Lu, Ho) compounds. Coherent phonons have been observed in RMnO3 compounds by pump-probe spectroscopy with subpicosecond laser pulses, whereas the observation of coherent optical phonons was reported only in LuMnO3. Recently, we succeeded in the observation of the coherent optical phonon in a YMnO3 thin film. The generation process of the coherent optical phonon is assigned to a displacive mechanism, which is identical to that in LuMnO3. The coherent optical phonon is observed in the temperature range from 10 K to room temperature, while the oscillation intensity strongly decreases as the temperature increases to the Néel temperature of ~70 K from a lower temperature range. It is interesting that the temperature dependence is largely different from that in LuMnO3. We describe that the result can be qualitatively explained by the property of an isostructural transition around the Néel temperature in RMnO3 compounds. In addition, we briefly discuss ultrafast incoherent responses of excited electronic states from the viewpoint of the excitation photon energy of laser pulses.

Coherent optical and acoustic phonons generated at lattice-matched GaP/Si(0 0 1) heterointerfaces

Thin GaP films can be grown on an exact Si(0 0 1) substrate with nearly perfect lattice match. We perform all-optical pump–probe measurements to investigate the ultrafast electron–phonon coupling at the buried interface of GaP/Si. Above-bandgap excitation with a femtosecond laser pulse can induce coherent longitudinal optical (LO) phonons both in the GaP overlayer and in the Si substrate. The coupling of the GaP LO phonons with photoexcited plasma is reduced significantly with decreasing GaP layer thickness from 56 to 16 nm due to the quasi-two-dimensional confinement of the plasma. The same laser pulse can also generate coherent longitudinal acoustic phonons in the form of a strain pulse. The strain pulse induces not only a periodic modulation in the optical reflectivity as it propagates in the semiconductor, but also a sharp spike when it arrives at the GaP layer boundary. The acoustic pulse induced at the GaP/Si interface is remarkably stronger than that at the Si surface, suggesting a possible application of the GaP/Si heterostructure as an opto-acoustic transducer. The amplitude and the phase of the reflectivity modulation varies with the GaP layer thickness, which can be understood in terms of the interference caused by the multiple acoustic pulses generated at the top surface and at the buried interface.

Terahertz driven amplification of coherent optical phonons in GaAs coupled to metallic dog-bone resonators

Two-dimensional terahertz spectroscopy on an AlAs/GaAs nanostructure covered by field-enhancing dog-bone resonators shows signatures of coherent optical phonon amplification. Amplification is due to stimulated phonon emission by a terahertz-driven electron current.

Generation of coherent phonons by coherent extreme ultraviolet radiation in a transient grating experiment

We investigate the excitation of coherent acoustic and optical phonons by ultrashort extreme ultraviolet (EUV) pulses produced by a free electron laser. Two crossed femtosecond EUV (wavelength 12.7 nm) pulses are used to excite coherent phonons at a wavelength of 280 nm, which are detected via diffraction of an optical probe beam. Longitudinal and surface acoustic waves are measured in BK-7 glass, diamond, and Bi4Ge3O12; in the latter material, the excitation of a coherent optical phonon mode is also observed. We discuss probing different acoustic modes in reflection and transmission geometries and frequency mixing of surface and bulk acoustic waves in the signal. The use of extreme ultraviolet radiation will allow the creation of tunable GHz to THz acoustic sources in any material without the need to fabricate transducer structures.

Experimental observation of anharmonic effects in coherent phonon dynamics in diamond

We present a study of coherent optical phonon dynamics in monocrystalline and polycrystalline diamond using transient transmission spectroscopy with few-cycle laser pulses. Besides the oscillations at the fundamental phonon frequency of 40 THz we observe a signal at second harmonic frequency and four weak frequency sidebands (25.0 THz, 32.5 THz, 47.5 THz and 55.0 THz). Potential origin of these sidebands is discussed along with the dependence of the observed signal on experimental conditions (pump power, sample thickness, etc.). Phonon dephasing time in polycrystalline diamond T2,poly = 6.0 ± 0.4 ps is found to be shorter than in monocrystalline diamond T2,mono = 7.0 ± 0.4 ps.

Femtosecond reflectivity study of coherent phonons in doubly photoexcited bismuth

Ultrafast optical excitation generates coherent A1g optical phonons in bismuth via the mechanism of displacive excitation of coherent phonons (DECP). Here, femtosecond pump-probe reflectivity spectroscopy examines the dynamics of coherent phonons in doubly photoexcited bismuth. Two successive pump pulses are employed to generate optic phonons and thus to investigate the phonon dynamics including bond softening and dephasing with variable pump fluence and inter-pump separation times. Combined with thermal analysis, it distinguishes thermal and nonthermal effects of photoexcitation on the phonon dynamics. It also reveals that photocarriers relax via electron-hole recombination and diffusion out of the optical penetration depth on ultrafast timescales of 10–20 ps.

Lattice-mediated magnetic order melting in TbMnO3

Recent ultrafast magnetic-sensitive measurements [Phys. Rev. B 92, 184429 (2015) and Phys. Rev. B 96, 184414 (2017)] have revealed a delayed melting of the long-range cycloid spin-order in TbMnO$_3$ following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting and is interpreted as the fingerprint of the formation of anti-Jahn Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. Furthermore, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.

Controlling competing orders via nonequilibrium acoustic phonons: Emergence of anisotropic effective electronic temperature

Ultrafast perturbations offer a unique tool to manipulate correlated systems due to their ability to promote transient behaviors with no equilibrium counterpart. A widely employed strategy is the excitation of coherent optical phonons, as they can cause significant changes in the electronic structure and interactions on short time scales. Here, we explore a promising alternative route: the non-equilibrium excitation of acoustic phonons. We demonstrate that it leads to the remarkable phenomenon of a momentum-dependent temperature, by which electronic states at different regions of the Fermi surface are subject to distinct local temperatures. Such an anisotropic electronic temperature can have a profound effect on the delicate balance between competing ordered states in unconventional superconductors, opening a novel avenue to control correlated phases.

Mott transition in chain structure of strained VO2 films revealed by coherent phonons

The characteristic of strongly correlated materials is the Mott transition between metal and insulator (MIT or IMT) in the same crystalline structure, indicating the presence of a gap formed by the Coulomb interaction between carriers. The physics of the transition needs to be revealed. Using VO2, as a model material, we observe the emergence of a metallic chain in the intermediate insulating monoclinic structure (M2 phase) of epitaxial strained films, proving the Mott transition involving the breakdown of the critical Coulomb interaction. It is revealed by measuring the temperature dynamics of coherent optical phonons with separated vibrational modes originated from two substructures in M2: one is the charge-density-wave, formed by electron-phonon (e-ph) interaction, and the other is the equally spaced insulator-chain with electron-electron (e-e) correlations.

Ultrafast dynamics of coherent optical phonon correlated with the antiferromagnetic transition in a hexagonal YMnO3 epitaxial film

We report on the observation of the coherent optical phonon in a hexagonal YMnO3 epitaxial film using a reflection-type pump-probe technique at various temperatures, excitation powers, and energies. We detected an oscillatory structure with a frequency of ∼5.1 THz, which is assigned to the coherent optical phonon with A1 symmetry, in a time-domain signal. It was found that the coherent optical phonon can be observed at temperatures from 10 K to room temperature, while the oscillation amplitude markedly decreases with an increase in temperature around ∼70 K corresponding to the Néel temperature. The temperature dependence of the oscillation amplitude indicates that the coherent optical phonon is sensitive to the spin-lattice coupling connected with the antiferromagnetic transition.

Screening effects of photogenerated carriers on terahertz radiation from coherent GaAs-like longitudinal optical phonons in (11n)-oriented GaAs/In0.1Al0.9As strained multiple quantum wells

We investigated terahertz radiation from coherent GaAs-like longitudinal optical (LO) phonons in (11n)-oriented GaAs/In0.1Al0.9As strained multiple quantum wells for clarifying the screening effects of photogenerated carriers. We observed the intense quasi-monochromatic terahertz wave from the coherent GaAs-like LO phonon, which originates from the initial polarization enhanced by the strong piezoelectric field. The intensity of the coherent GaAs-like LO-phonon band exhibited a saturation behavior as the pump power was increased. We evaluated the saturation behavior in terms of excitation efficiency of the terahertz wave from the coherent GaAs-like LO phonon using the parameter of unit-power intensity. From the pump-power dependence of the unit-power intensity, we conclude that the screening effect of high density photogenerated carriers on the piezoelectric field causes saturation of the terahertz-wave intensity from the coherent GaAs-like LO phonon.

Enhancement of coherent phonon amplitude in phase-change materials by near-infrared laser irradiation

We have examined the effect of pump-probe photon energy on the amplitude of coherent optical phonons in a prototypical phase change material using a femtosecond time-resolved transmission technique. The photon energy was varied between 0.8 and 1.0 eV (corresponding to the wavelengths of 1550 and 1200 nm), a range over which there is significant optical contrast between the crystalline and amorphous phases of Ge2Sb2Te5 (GST225). It was found that in crystalline GST225, the coherent phonon amplitude monotonically increases as the photon energy increases, indicating that the phonon amplitude is enhanced by interband optical absorption, which is associated with the imaginary part of the dielectric function. In amorphous GST225, in contrast, the coherent phonon amplitude does not depend on the photon energy, remaining almost constant over the tuning range. A possible contribution from the polarizability associated with the resonant bonding nature of GST225 is discussed.

Origin of the thermal expansion anomaly in layered Bi2X3 topological insulators: Ultrafast time-resolved pump-probe experiments and theory

Recent experiments on the thermal expansion of Sb2Te3, a prototypical example of strong three-dimensional topological insulators, have shown an intriguing anomaly in the thermal expansion coefficient along the hexagonal axis (alpha(parallel to)), which drops sharply to almost zero in a narrow range of temperature around similar to 225 K. With no accompanying signatures in other properties, the origin of this anomaly is not understood. We present here femtosecond pump-probe differential reflectivity measurements on single crystals of Sb2Te3 as a function of temperature from 3 to 300 K to determine the temperature dependence of coherent optical and acoustic phonons along with the dynamics of the photoexcited carriers. We find clearly anomalous temperature dependence of the parameters associated with vibrational and electronic relaxation in the narrow temperature range of 200-250 K. Within first-principles density functional theoretical analysis, we show that the observed anomalies can be explained with a mechanism of formation of stacking faults stabilized by vibrational entropy above 200 K. As a similar anomaly in the thermal expansion is also observed in other chalcogenides in the same family, the proposed mechanism may also be applicable to these layered strong topological insulators.