Generation Of Coherent Phonons Research Articles

Strong Surface-Enhanced Coherent Phonon Generation in van der Waals Materials.

Terahertz (THz) coherent phonons have emerged as promising candidates for the next generation of high-speed, low-energy information carriers in atomically thin phononic or phonon-integrated on-chip devices. However, effectively manipulating THz coherent phonons remains a significant challenge. In this study, we investigated THz coherent phonon generation in exfoliated van der Waals (vdW) flakes of Fe3GeTe2, Fe5GeTe2, and FePS3. We successfully generated the THz A1g coherent phonon mode in these vdW flakes. An innovative approach involved partially exfoliating vdW flakes on a gold substrate and partially on a silicon (Si) substrate to compare the THz coherent phonon generation between both sides. Interestingly, we observed a significantly enhanced THz coherent phonon in the vdW/gold area compared with that in the vdW/Si area. Frequency-domain Raman mapping across the vdW flakes corroborated these findings. Numerical simulations further indicated a stronger enhanced surface field in vdW/gold structures than in vdW/Si structures. Consequently, we attribute the observed enhancement in THz coherent phonon generation to the increased surface field on the gold substrate. This enhancement was consistent across the three different vdW materials studied, suggesting the universality of this strategy. Our results hold promise for advancing the design of THz phononic and phonon-integrated devices.

Real‐Time Detection of Coherent Vibrational Dynamics in TiN Films

AbstractTitanium nitride (TiN) has recently gained considerable interest because of its remarkable plasmonic properties and for its strong electron–phonon (e–ph) coupling, leading to extremely fast (<100 fs) electron‐lattice cooling. Here, the generation of coherent phonons in TiN films is reported, along with their real‐time detection by means of broadband transient reflection spectroscopy with sub‐15‐fs temporal resolution. The measurements show damped oscillations, superimposed to excited state electronic decay. A coherent vibrational mode is revealed, with ≈10 THz frequency ascribed to defect‐activated normal modes, consistent with spontaneous Raman scattering data, and a dephasing time of ≈250 fs. Two π‐phase flips are also observed located at photon energies corresponding to interband optical transitions (at 3.2 and 2.5 eV), ascribed to selective coupling of the vibrational mode to these transitions; the energy modulation induced by the vibrational coherence is evaluated. It is shown that the displacive excitation of coherent phonons model describes the coherent response in terms of temporal behavior and of spectral amplitude profile. Overall, a comprehensive and detailed analysis of coherent phonons in TiN films, so far undected, is provided and relevant information on TiN photo‐physical properties, potentially useful for its applications, is given.

AbInitio Self-Trapped Excitons.

We propose a new formalism and an effective computational framework to study self-trapped excitons (STEs) in insulators and semiconductors from first principles. Using the many-body Bethe-Salpeter equation in combination with perturbation theory, we are able to obtain the mode- and momentum-resolved exciton-phonon coupling matrix element in a perturbative scheme and explicitly solve the real space localization of the electron (hole), as well as the lattice distortion. Further, this method allows us to compute the STE potential energy surface and evaluate the STE formation energy and Stokes shift. We demonstrate our approach using two-dimensional magnetic semiconductor chromium trihalides and a wide-gap insulator BeO, the latter of which features dark excitons, and make predictions of their Stokes shift and coherent phonon generation which we hope will spark future experiments such as photoluminescence and transient absorption studies.

Uncovering White Light Emission in Pressure‐Treated Sb‐Doped Double Perovskite by Coherent Optical Phonon

AbstractSingle‐component white‐light emitters are ideal for solid‐state lighting applications. Here, the dual‐emission white light in the 3D Cs2NaInCl6:0.1 Sb3+ crystal is successfully achieved by the high‐pressure treatment strategy. Upon compression, the remarkable self‐trapped exciton (STE) emission enhancement is observed at 20.6 GPa due to the tilting and twisting of inorganic octahedron caused by the phase transition of Cs2NaInCl6:0.1 Sb3+ crystal. Intriguingly, after undergoing the high‐pressure treatment, in addition to the blue high‐energy emission from the STEs, [SbCl6]3− exhibits the orange low‐energy emission from STEs, which is ascribed to the remaining local distortion of inorganic octahedron resulting from the presence of residual amorphous phase in the local region upon decompression. Furthermore, coherent phonon generation and density functional theory calculations indicate that the electrons exhibit a strong coupling to A1g stretch mode and T2gIn bending mode in Cs2NaInCl6:0.1 Sb3+. After high‐pressure treatment, the coupling between the electrons and the T2gIn bending mode disappears, suggesting local octahedral symmetry disruption due to residual amorphous structures induced by high‐pressure treatment. This work unveils the relationship between the electron‐phonon coupling and the STE emission and offers a new strategy to design and synthesize the new single‐component white‐light metal halide perovskites.

Capturing the non-equilibrium state in light–matter–free-electron interactions through ultrafast transmission electron microscopy

Ultrafast transmission electron microscope (UTEM) with the multimodality of time-resolved diffraction, imaging, and spectroscopy provides a unique platform to reveal the fundamental features associated with the interaction between free electrons and matter. In this review, we summarize the principles, instrumentation, and recent developments of the UTEM and its applications in capturing dynamic processes and non-equilibrium transient states. The combination of the transmission electron microscope with a femtosecond laser via the pump–probe method guarantees the high spatiotemporal resolution, allowing the investigation of the transient process in real, reciprocal and energy spaces. Ultrafast structural dynamics can be studied by diffraction and imaging methods, revealing the coherent acoustic phonon generation and photo-induced phase transition process. In the energy dimension, time-resolved electron energy-loss spectroscopy enables the examination of the intrinsic electronic dynamics of materials, while the photon-induced near-field electron microscopy extends the application of the UTEM to the imaging of optical near fields with high real-space resolution. It is noted that light–free-electron interactions have the ability to shape electron wave packets in both longitudinal and transverse directions, showing the potential application in the generation of attosecond electron pulses and vortex electron beams.

Trapping-induced quantum beats in a van-der-Waals heterostructure microcavity observed by two-dimensional micro-spectroscopy

Spatial confinement has been frequently engineered to control the flow and relaxation dynamics of exciton polaritons. While widely investigated in GaAs microcavities, exciton-polariton coupling between discretized polariton modes arising from spatially confined 2D crystals been has been less exhaustively studied. Here, we use coherent 2D photoluminescence-detected micro-spectroscopy to detect oscillating 2D peaks exclusively from a spatial trap in a microcavity with an embedded van-der-Waals heterostructure at room temperature. We observe a wide variation of oscillatory phases as a function of spectral position within the 2D spectrum, which suggests the existence of a coupling between the discretized polariton modes. The latter is accompanied by the generation of coherent phonons.

Stimulated Raman blockade in coherent phonon generation

We theoretically investigate the behavior of coherent optical phonons in an electron–phonon coupled system at moderate laser intensity: below GW/cm2. We calculate the coherent phonons from impulsive stimulated Raman scattering (ISRS) and impulsive absorption (IA) mechanisms with a nonperturbative model. The generation efficiency of coherent phonons in single-pulse excitation exhibits gradual nonlinear saturation with increasing optical intensity in a nonperturbative regime. The ISRS mechanism exhibits substantial saturation at relatively low pulse intensity, whereas the IA mechanism remains roughly linear. We further examine the influence of double-pulse excitation on quantum path interference. The ISRS mechanism exhibits a pronounced saturation effect near 0 fs of pump–pump delay, whereas the IA process exhibits negligible saturation behavior. These results reproduce well experimental data obtained by double-pulse excitation and support our proposal that ISRS is the primary quantum path for the observed coherent phonons in gallium arsenide.

Ion trap long-range XY model for quantum state transfer and optimal spatial search

Linear ion trap chains are a promising platform for quantum computation and simulation. The XY model with long-range interactions can be implemented with a single side-band Mølmer–Sørensen scheme, giving interactions that decay as , where parameterises the interaction range. Lower leads to longer range interactions, allowing faster long-range gate operations for quantum computing. However, decreasing causes an increased generation of coherent phonons and appears to dephase the effective XY interaction model. We characterise and show how to correct for this effect completely, allowing lower interactions to be coherently implemented. Ion trap chains are thus shown to be a viable platform for spatial quantum search in optimal time, for N ions. Finally, we introduce a quantum state transfer protocol, with a qubit encoding that maintains a high fidelity.

Selective coupling of coherent optical phonons in YBa2Cu3O7−δ with electronic transitions

We investigate coherent lattice dynamics in optimally doped ${\mathrm{YBa}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{7\ensuremath{-}\ensuremath{\delta}}$ driven by ultrashort ($\ensuremath{\sim}12$ fs) near-infrared and near-ultraviolet pulses. Transient reflectivity experiments, performed at room temperature and under moderate ($<0.1$ mJ/${\mathrm{cm}}^{2}$) excitation fluence, reveal ${A}_{g}$-symmetry phonon modes related to the O(2,3) bending in the ${\mathrm{CuO}}_{2}$ planes and to the apical O(4) stretching at frequencies between 10 and 15 THz, in addition to the previously reported Ba and Cu(2) vibrations at 3.5 and 4.5 THz. The relative coherent phonon amplitudes are in stark contrast to the relative phonon intensities in the spontaneous Raman scattering spectrum excited at the same wavelength. This contrast indicates mode-dependent contributions of the Raman and non-Raman mechanisms to the coherent phonon generation. We show that the particularly intense coherent Cu(2) phonon, together with its initial phase, supports its generation predominately via a displacive mechanism, possibly involving the charge transfer within the ${\mathrm{CuO}}_{2}$ planes. The small amplitude of the coherent out-of-phase O(2,3) bending mode at 10 THz also suggests the involvement of non-Raman generation mechanism. The generation of the other coherent phonons can in principle be explained within the framework of Raman mechanism. When the pump light has the polarization component perpendicular to the ${\mathrm{CuO}}_{2}$ plane, the coherent O(4) mode at 15 THz is strongly enhanced compared to the in-plane excitation, corresponding to the large polarizability component associated with the hopping between the apical and the chain oxygens, O(4) and O(1).

Towards chiral acoustoplasmonics.

The possibility of creating and manipulating nanostructured materials encouraged the exploration of new strategies to control electromagnetic properties. Among the most intriguing nanostructures are those that respond differently to helical polarization, i.e., exhibit chirality. Here, we present a simple structure based on crossed elongated bars where light-handedness defines the dominating cross-section absorption or scattering, with a 200 % difference from its counterpart (scattering or absorption). The proposed chiral system opens the way to enhanced coherent phonon excitation and detection. We theoretically propose a simple coherent phonon generation (time-resolved Brillouin scattering) experiment using circularly polarized light. In the reported structures, the generation of acoustic phonons is optimized by maximizing the absorption, while the detection is enhanced at the same wavelength and different helicity by engineering the scattering properties. The presented results constitute one of the first steps towards harvesting chirality effects in the design and optimization of efficient and versatile acoustoplasmonic transducers.

Optomechanical Generation of Coherent GHz Vibrations in a Phononic Waveguide.

Nanophononics has the potential for information transfer, in an analogous manner to its photonic and electronic counterparts. The adoption of phononic systems has been limited, due to difficulties associated with the generation, manipulation, and detection of phonons, especially at GHz frequencies. Existing techniques often require piezoelectric materials with an external radiofrequency excitation that are not readily integrated into existing CMOS infrastructures, while nonpiezoelectric demonstrations have been inefficient. In this Letter, we explore the optomechanical generation of coherent phonons in a suspended 2D silicon phononic crystal cavity with a guided mode around 6.8GHz. By incorporating an air-slot into this cavity, we turn the phononic waveguide into an optomechanical platform that exploits localized photonic modes resulting from inherent fabrication imperfections for the transduction of mechanics. Such a platform exhibits very fine control of phonons using light, and is capable of coherent self-sustained phonon generation around 6.8GHz, operating at room temperature. The ability to generate high frequency coherent mechanical vibrations within such a simple 2D CMOS-compatible system could be a first step towards the development of sources in phononic circuitry and the coherent manipulation of other solid-state properties.

Ultrafast generation and detection of coherent acoustic phonons in SnS0.91Se0.09

The rapid growth of attention to tin sulfide (SnS) is due to its efficient application in the field of thermoelectricity, and its doping product SnS0.91Se0.09 can obtain a high average thermoelectric figure of merit (ZTave≈ 1.25). Although many efforts have been made to reveal the mechanisms associated with electron transport and heat conduction, the role of lattice vibration remains poorly understood. Here, we studied the coherent vibration dynamics in SnS0.91Se0.09 bulk single crystal by using the femtosecond two-color pump-probe optical reflectivity technique. The oscillation signal in the time domain of SnS0.91Se0.09 is considered to be an electron–phonon interaction. The coherent dynamics of longitudinal acoustic phonons in this coupling behavior is closely related to probe polarization and excitation power. The stability of oscillation frequency reveals the microscopic mechanism of phonon conduction, and further understands the lattice nonharmonic caused by electron–phonon interaction in light-induced.

Localized coherent phonon generation in monolayer MoSe2 from ultrafast exciton trapping at shallow traps.

We report spectroscopic evidence for the ultrafast trapping of band edge excitons at defects and the subsequent generation of defect-localized coherent phonons (CPs) in monolayer MoSe2. While the photoluminescence measurement provides signals of exciton recombination at both shallow and deep traps, our time-resolved pump-probe spectroscopy on the sub-picosecond time scale detects localized CPs only from the ultrafast exciton trapping at shallow traps. Based on occupation-constrained density functional calculations, we identify the Se vacancy and the oxygen molecule adsorbed on a Se vacancy as the atomistic origins of deep and shallow traps, respectively. Establishing the correlations between the defect-induced ultrafast exciton trapping and the generation of defect-localized CPs, our work could open up new avenues to engineer photoexcited carriers through lattice defects in two-dimensional materials.

Resonance-enhanced excitation and relaxation dynamics of coherent phonons in Fe1.14Te.

Lattice dynamics plays a significant role in manipulating the unique physical properties of materials. In this work, femtosecond transient optical spectroscopy is used to investigate the generation mechanism and relaxation dynamics of coherent phonons in Fe1.14Te-a parent compound of chalcogenide superconductors. The reflectivity time series consist of the exponential decay component due to hot carriers and damped oscillations caused by the A1g phonon vibration. The vibrational frequency and dephasing time of the A1g phonons are obtained as a function of temperature. With increasing temperature, the phonon frequency decreases and can be well described with the anharmonicity model. Dephasing time is independent of temperature, indicating that the phonon dephasing is dominated by phonon-defect scattering. The impulsive stimulated Raman scattering mechanism is responsible for the coherent phonon generation. Owing to the resonance Raman effect, the maximum photosusceptibility of the A1g phonons occurs at 1.590 eV, corresponding to an electronic transition in Fe1.14Te.

The influence of initial phonon states on the generation of coherent optical phonons

The generation of coherent phonons is theoretically studied using a thermal equilibrium phonon distribution as the initial condition. The time evolution of the coherent phonon amplitude and phonon population is calculated for 4.5-THz phonons with initial phonon distributions at 10 and 300 K. It is determined that the coherent-phonon amplitudes of state-selected phonons are dependent on the initial phonon distribution. The coherent-phonon amplitudes, when considering all phonon states instead of selecting certain phonon levels, are almost the same for both initial distributions. The variance of the coherent-phonon amplitudes is found to oscillate with twice the phonon frequency, and its oscillation amplitude depends on the initial phonon distribution.

TRANSDUCCIÓN OPTOMECÁNICA Y BIESTABILIDADES ÓPTICAS ENMICRORRESONADORES BASADOS EN REFLECTORES DE BRAGG

In cavity optomechanics experiments with ultrashort laser pulses, the temporal dynamics of the optical modes of the system play a fundamental role in the generation and detection of coherent phonons. In this work, we analyze the feasibility of using a second continuous emission laser to optimize the detection efficiency, by setting the fundamentalótical mode to a specific spectral position. Under certain conditions, and through this continuum excitation, it is possible to modify the recovery dynamics of the optical modes after an ultrafast pulsed excitation, to the point of stopping it on a quasiequilibrium. This phenomenon is directly related to the optical bistability of the resonator.

Ultrafast Optical Probe of Coherent Acoustic Phonons in Dirac Semimetal Cd3As2 Film Epitaxied on GaAs(111)B Substrate.

Coherent longitudinal acoustic phonon (CAP) generation in epitaxial Dirac semimetal Cd3As2 films with different thicknesses was investigated by a time-resolved reflectance technique. The short-lived weak CAP oscillations can be observed only in the thicker Cd3As2 films, and their central frequency of 0.039 THz has no dependence on sample thickness, but is nearly inversely proportional to the probe wavelength. For the 20 nm thin film, the observed long-lived CAP with a central frequency of 0.049 THz is generated in the GaAs(111)B substrate underneath. A sound velocity of 3800 m/s for the Cd3As2 film and 5360 m/s for the GaAs(111)B substrate is thus deduced. In addition, the opposite CAP amplitude and lifetime dependence on temperature further confirms the electronic and thermal stress origination of CAP generated in GaAs(111)B and Cd3As2 film, respectively, based on the propagating strain pulse model. The central frequency of CAP is found to be stable with increasing pumping fluence and temperature, which makes Cd3As2 a potential material for thermoelectric device applications.

Launching Coherent Acoustic Phonon Wave Packets with Local Femtosecond Coulomb Forces.

Generation and manipulation of coherent acoustic phonons enables ultrafast control of solids and has been exploited for applications in various acoustic devices. We show that localized coherent acoustic phonon wave packets can be launched by ultrafast Coulomb forces in a scanning tunneling microscope (STM) using tip-enhanced terahertz electric fields. The wave packets propagate at the speed of the longitudinal acoustic phonon, creating standing waves up to 0.26THz for a 6.4nm thin Au film on mica. The ultrafast lattice displacement can be as large as 5pm and is precisely controlled by varying the tip-sample distance. This nonthermal femtosecond Coulomb-force-based excitation mechanism is applicable in nano-optomechanics for advanced terahertz engineering and opens new perspectives in exploiting coherent phonons at the atomic scale.

Calibrating Out-of-Equilibrium Electron–Phonon Couplings in Photoexcited MoS2

Nonequilibrium electron-phonon coupling (EPC) serves as a dominant interaction in a multitude of transient processes, including photoinduced phase transitions, coherent phonon generation, and possible light-induced superconductivity. Here we use monolayer MoS2 as a prototype to investigate the variation in electron-phonon couplings under laser excitation, on the basis of real-time time-dependent density functional theory simulations. Phonon softening, anisotropic modification of the deformation potential, and enhancement of EPC are observed, which are attributed to the reduced electronic screening and modulated potential energy surfaces by photoexcitation. Furthermore, by tracking the transient deformation potential and nonthermal electronic population, we can monitor the ultrafast time evolution of the energy exchange rate between electrons and phonons upon laser excitation. This work provides an effective strategy to investigate the nonequilibrium EPC and constructs a scaffold for understanding nonequilibrium states beyond the multitemperature models.

Anisotropic electron and lattice dynamics in excitonic insulator Ta2NiSe5

We employ polarization-resolved femtosecond optical pump–probe spectroscopy to investigate the nonequilibrium photocarrier dynamics in excitonic insulator Ta2NiSe5. The electronic dynamics, including hot carrier cooling, exciton formation, and recombination in the timescale ranging from subpicoseconds to a few tens of picoseconds, have been established from the transient reflectivity spectra, showing strong in-plane anisotropy with respect to the probe polarization. Such anisotropic photocarrier dynamics possibly arise from the crystalline orientation dependence of the excitonic polarizability. Furthermore, we find that the amplitude of coherent phonons with a frequency of 1 THz is subject to the probe polarization, whereas it is not sensitive to the pump polarization. This substantiates that the displacive excitation of coherent phonons plays a decisive role in lattice dynamics. In addition, we find that the photo-induced dielectric screening tends to suppress the amplitude of coherent phonons with increasing pump fluence, manifesting a remarkable polarization dependence. Our work provides valuable insights into the excitonic dynamics and the origin of coherent phonon generation and also may contribute to the development of polarization-sensitive photoelectric devices based on Ta2NiSe5.