Coherent Phonon Dynamics Research Articles

Probing precise interatomic potentials by nonadiabatic nonlinear phonons

Accurately probing the interatomic potential (IP) in crystals is essential for understanding the dynamic mechanisms in phase transitions and chemical reactions. Here, by interrogating laser-induced coherent phonon dynamics, we propose a new kind of optical microscopy for determining effective interatomic potentials beyond the harmonic and adiabatic approximation. This technique is tested against available experimental and first-principles data, by which the interatomic potential of graphene and a few other materials are successfully reconstructed in a large configuration space and beyond the ground state. A significant nonadiabatic effect emerges in nonlinear phonon dynamics and the IP reconstruction, which corrects the anharmonic part of IP much stronger (up to 50%) than the harmonic part. The nonadiabaticity-modulated potentials can lead to ∼10% correction on thermal expansion coefficients and ∼0.3 eV on phase transition barriers. This work offers a new strategy for probing complex interactions in quantum materials and exemplifies the universality of nonadiabaticity, which deserves a full consideration for precisely determining physical properties of quantum many-body systems.

Effect of crystallinity and thickness on thermal transport in layered PtSe2

We present a comparative investigation of the influence of crystallinity and film thickness on the acoustic and thermal properties of layered PtSe2 films of varying thickness (1–40 layers) using frequency-domain thermo-reflectance, low-frequency Raman, and pump-probe coherent phonon spectroscopy. We find ballistic cross-plane heat transport up to ~30 layers PtSe2 and a 35% reduction in the cross-plane thermal conductivity of polycrystalline films with thickness larger than 20 layers compared to the crystalline films of the same thickness. First-principles calculations further reveal a high degree of thermal conductivity anisotropy and a remarkable large contribution of the optical phonons to the thermal conductivity in bulk (~20%) and thin PtSe2 films (~30%). Moreover, we show strong interlayer interactions in PtSe2, short acoustic phonon lifetimes in the range of picoseconds, an out-of-plane elastic constant of 31.8 GPa, and a layer-dependent group velocity ranging from 1340 ms−1 in bilayer to 1873 ms−1 in eight layers of PtSe2. The potential of tuning the lattice thermal conductivity of layered materials with the level of crystallinity and the real-time observation of coherent phonon dynamics open a new playground for research in 2D thermoelectric devices and provides guidelines for thermal management in 2D electronics.

Giant effective magnetic fields from optically driven chiral phonons in 4f paramagnets

We present a mechanism by which optically driven chiral phonon modes in rare-earth trihalides generate giant effective magnetic fields acting on the paramagnetic $4f$ spins. With cerium trichloride (CeCl$_3$) as our example system, we calculate the coherent phonon dynamics in response to the excitation by an ultrashort terahertz pulse using a combination of phenomenological modeling and first-principles calculations. We find that effective magnetic fields of over 100 tesla can possibly be generated that polarize the spins for experimentally accessible pulse energies. The direction of induced magnetization can be reversed by changing the handedness of circular polarization of the laser pulse. The underlying process is a phonon analog of the inverse Faraday effect in optics that has been described recently, and which enables novel ways of achieving control over and switching of magnetic order at terahertz frequencies.

Strong laser polarization control of coherent phonon excitation in van der Waals material Fe3GeTe2

Optical manipulation of coherent phonon frequency in two-dimensional (2D) materials could advance the development of ultrafast phononics in atomic-thin platforms. However, conventional approaches for such control are limited to doping, strain, structural or thermal engineering. Here, we report the experimental observation of strong laser-polarization control of coherent phonon frequency through time-resolved pump-probe spectroscopic study of van der Waals (vdW) materials Fe3GeTe2. When the polarization of the pumping laser with tilted incidence is swept between in-plane and out-of-plane orientations, the frequencies of excited phonons can be monotonically tuned by as large as 3% (~100 GHz). Our first-principles calculations suggest the strong planar and vertical inter-atomic interaction asymmetry in layered materials accounts for the observed polarization-dependent phonon frequencies, as in-plane/out-of-plane polarization modifies the restoring force of the lattice vibration differently. Our work provides insightful understanding of the coherent phonon dynamics in layered vdW materials and opens up new avenues to optically manipulating coherent phonons.

Quasiparticle dynamics and phonon softening in FeSe0.9S0.1 superconductors

The quasiparticle and longitudinal acoustic (LA) coherent phonon dynamics of the FeSe0.9S0.1 single crystal were investigated by femtosecond transient optical spectroscopy. The FeSe0.9S0.1 single crystal undergoes metal-superconductor transition at Tc = 9.5 K and structural phase transition at Ts = 72 K. To investigate the correlation between the quasiparticle/LA coherent phonon dynamics and the antiferromagnetic spin/nematic fluctuation, we measured the transient differential reflectivity ΔR(t)/R0 in time series (R is the reflectivity) between 4-130 K. The ΔR(t)/R0 time series showed a negative sign below Ts = 72 K, while its sign reversed from negative to positive above Ts. The ΔR(t)/R0 time series was contributed by a combination of two exponential decays and an oscillation term. The slow decay attributed to electron-phonon and phonon-phonon coupling showed a negative amplitude below Ts and a positive amplitude above Ts. A fast decay with positive amplitude appeared at T ≥ 55 K was induced by the electron-phonon coupling of the high-temperature orthorhombic phase FeSe0.9S0.1. The oscillation contributed by the LA coherent phonon emerged below Ts but was not observed above Ts, indicating that it was impacted by the nematic fluctuation of FeSe0.9S0.1.

Absence of Kondo effect in CeNiGe3 revealed by coherent phonon dynamics

Cerium-based intermetallic ${\mathrm{CeNiGe}}_{3}$ has been generally believed to be a heavy-fermion material with Kondo behavior at low temperatures. Using femtosecond-resolved coherent phonon spectroscopy, we present a temperature-dependent dynamic investigation of the bosonic quasiparticles in ${\mathrm{CeNiGe}}_{3}$. Our data do not agree with the heavy-fermion expectation and instead show that the phonon stiffening from room temperature down to 5 K can be well explained by the anharmonic effect in the absence of a Kondo mechanism. Furthermore, the coherent lattice vibration located at \ensuremath{\sim}7.9 THz exhibits a mode splitting at ${T}^{+}\ensuremath{\approx}105\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, which is close to the energy scale of the first excited crystal field splitting of the Ce $4f$ level. We argue that an orbital crossover may account for this intriguing observation.

Ultrafast dynamics of photoexcited carriers and coherent phonons in ultrathin Bi2Te3 thermoelectric films

Ultrafast dynamics of photoexcited carriers and coherent phonons in ultrathin Bi2Te3 thermoelectric films

Dichroic Photoelasticity in Black Phosphorus Revealed by Ultrafast Coherent Phonon Dynamics.

Coherent longitudinal lattice vibrations of black phosphorus provide unique access to the out-of-plane strain coupled in-plane optical properties. In this work, polarization-resolved femtosecond transient absorption microscopy is applied to study the anisotropic coherent phonon responses. Multiorder phonon harmonics were observed with thickness dependence well explained by the linear chain model, allowing rapid optical mapping of phonon frequency distributions. More interestingly, exotic coherent phonon oscillations occourred with a π-phase jump between the armchair and zigzag polarizations, which reveals opposite signs of photoelasticity under the longitudinal strain. Specifically, compressive strain reduces the imaginary refractive index in the armchair polarization but increases the real refractive index in the zigzag polarization, as confirmed by the ab initio calculations and thin film model. These fundamental properties of black phosphorus hold potential for applications in ultrafast and polarization-sensitive photoacoustic/photoelastic modulators.

Interlayer Coupling and Ultrafast Hot Electron Transfer Dynamics in Metallic VSe2/Graphene van der Waals Heterostructures.

Atomically thin vanadium diselenide (VSe2) is a two-dimensional transition metal dichalcogenide exhibiting attractive properties due to its metallic 1T phase. With the recent development of methods to manufacture high-quality monolayer VSe2 on van der Waals materials, the outstanding properties of VSe2-based heterostructures have been widely studied for diverse applications. Dimensional reduction and interlayer coupling with a van der Waals substrate lead to its distinguishable characteristics from its bulk counterparts. However, only a few fundamental studies have investigated the interlayer coupling effects and hot electron transfer dynamics in VSe2 heterostructures. In this work, we reveal ultrafast and efficient interlayer hot electron transfer and interlayer coupling effects in VSe2/graphene heterostructures. Femtosecond time-resolved reflectivity measurements showed that hot electrons in VSe2 were transferred to graphene within a 100 fs time scale with high efficiency. Besides, coherent acoustic phonon dynamics indicated interlayer coupling in VSe2/graphene heterostructures and efficient thermal energy transfer to three-dimensional substrates. Our results provide valuable insights into the intriguing properties of metallic transition metal dichalcogenide heterostructures and motivate designing optoelectronic and photonic devices with tailored properties.

Effect of alloying on the dynamics of coherent acoustic phonons in bismuth double perovskite single crystals.

The bismuth double perovskite Cs2AgBiBr6 has been regarded as a potential candidate for lead-free perovskite photovoltaics. A detailed study on the coherent acoustic phonon dynamics in the pure, Sb- and Tl-alloyed Cs2AgBiBr6 single crystals is performed to understand the effects of alloying on the phonon dynamics and band edge characteristics. The coherent acoustic phonon frequencies are found to be independent of the alloying, while the damping rates are highly dependent on the alloying. Based on the mechanism of coherent acoustic phonon damping, a technique has been successfully developed that can accurately extract the absorption spectra near the indirect band gap for these single crystals with coefficients on the order of 102 cm-1.

Ultrafast scattering dynamics of coherent phonons in Bi1−x Sb x in the Weyl semimetal phase

We investigate ultrafast phonon dynamics in the Bi1−x Sb x alloy system for various compositions x using a reflective femtosecond pump-probe technique. The coherent optical phonons corresponding to the A1g local vibrational modes of Bi–Bi, Bi–Sb, and Sb–Sb are generated and observed in the time domain with a few picoseconds dephasing time. The frequencies of the coherent optical phonons were found to change as the Sb composition x was varied, and more importantly, the relaxation time of those phonon modes was dramatically reduced for x values in the range 0.5–0.8. We argue that the phonon relaxation dynamics are not simply governed by alloy scattering, but are significantly modified by anharmonic phonon–phonon scattering with implied minor contributions from electron–phonon scattering in a Weyl-semimetal phase.

Quantum confinement of coherent acoustic phonons in transferred single-crystalline bismuth nanofilms

Coherent acoustic phonon dynamics in single-crystalline bismuth nanofilms transferred to a glass substrate were investigated with ultrafast pump–probe spectroscopy. Coherent phonon signals were substantially enhanced by more than four times when compared with as-grown films on Si (111) substrates. Furthermore, more than 10% reduction of the acoustic phonon velocity was observed when the film thickness decreases to 22 nm, which is attributed to the modified phonon dispersion in extremely thin films from quantum confinement effects.

Coherent phonon dynamics in a c-plane sapphire crystal before and after intense femtosecond laser irradiation.

Femtosecond pump-probe experiments with a ∼6.4 fs time-resolution were performed to investigate the coherent phonon dynamics in a c-plane sapphire crystal before and after intense 800 nm femtosecond laser irradiation. The intense femtosecond laser induced defect/distortion and even re-crystallization of crystalline structures, which result in the appearance of new peaks and relative intensity change in coherent phonon and Raman spectra. The combination of these two spectra was found to be beneficial to evidence the variation of crystalline structure and further to differentiate the origins of new Raman peaks after irradiation. Further analysis of time-dependent differential absorbance with damped cosine function fitting and Fourier transfer calculation yields the vibrational parameters, including periods, damping times and initial phases, before and after irradiation. With these parameters, the defect-effects on damping time and the mechanism of coherent phonon generation were addressed.

Ultrafast dynamics of the low frequency shear phonon in 1T′-MoTe2

We report on the dynamics of coherent phonons in semimetal 1T′-MoTe2 using femtosecond pump-probe spectroscopy. On an ultrafast sub-picosecond timescale at room temperature, a low frequency and long-lifetime shear phonon mode was observed at 0.39 THz, which was previously reported in the form of a characteristic phonon only in the low temperature Td−MoTe2 phase. Unlike the other optical phonon modes, the shear phonon mode was found to strongly couple with photoexcited carriers. Moreover, the amplitude of the shear mode surprisingly decreased with increasing excitation density, a phenomenon that can be attributed to be a consequence of the lattice temperature increasing after excitation. These results provide useful physical information on ultrafast lattice symmetry switching between the normal semimetal 1T′ and the lattice inversion symmetry breaking Type-II Weyl semimetal Td phases.

Coherent phonon dynamics in spatially separated graphene mechanical resonators

Vibrational modes in mechanical resonators provide a promising candidate to interface and manipulate classical and quantum information. The observation of coherent dynamics between distant mechanical resonators can be a key step toward scalable phonon-based applications. Here we report tunable coherent phonon dynamics with an architecture comprising three graphene mechanical resonators coupled in series, where all resonators can be manipulated by electrical signals on control gates. We demonstrate coherent Rabi oscillations between spatially separated resonators indirectly coupled via an intermediate resonator serving as a phonon cavity. The Rabi frequency fits well with the microwave burst power on the control gate. We also observe Ramsey interference, where the oscillation frequency corresponds to the indirect coupling strength between these resonators. Such coherent processes indicate that information encoded in vibrational modes can be transferred and stored between spatially separated resonators, which can open the venue of on-demand phonon-based information processing.

Highly sensitive transient reflection measurement in extreme ultraviolet region for tracking carrier and coherent phonon dynamics.

A highly sensitive method for detecting transient reflection in the extreme ultraviolet (XUV) region was developed on the basis of high-order harmonics for tracking carrier and coherent phonon dynamics. The use of lock-in detection and boxcar integration enables us to observe optical modulation (ΔR/R) as high as 1 × 10-4, and the data acquisition takes only four minutes. XUV transient reflections of bismuth exhibited exponential decay originating from excited carriers and periodic oscillation originating from A1g optical phonons. The linear power dependence of the electronic and phonon amplitudes indicated that one-photon excitation occurred under the experimental conditions. The cosine of the initial phase of the phonon oscillation revealed that a displacive excitation mechanism contributed to phonon generation. The phonon parameters obtained by the XUV and NIR probes were consistent even though their penetration depths were different. The result indicated that the XUV and NIR pulses probe the same excited region, which should be near the surface due to the short penetration depth of the NIR pump pulses. The present highly sensitive means of detecting XUV transient reflections in solid-state materials could be utilized for detecting attosecond dynamics in the future.

Gigahertz coherent longitudinal acoustic phonons in GaAs Single crystals with different orientations

We report an experimental study on the ultrafast dynamics of coherent longitudinal acoustic phonons (CLAPs) in GaAs single crystals with different orientations by using femtosecond pump–probe technique. Under an above-bandgap pumping at 400 nm, the CLAP wave is generated on the surface of a GaAs crystal with [100] orientation, and then it propagates into the crystal and is detected by the transient reflection of the probe beam at 800 nm. As the pumping intensity is increased, the amplitude and lifetime of generated CLAPs in GaAs crystals are increased and decreased respectively, while the phonons oscillation frequency remains a constant of 44.3±0.2 GHz. Furthermore, the CLAPs frequency is varied in GaAs crystals with different orientations which is determined by the elastic anisotropy. In addition, from the initially opposite oscillation phase of [100] and [111] oriented GaAs, tensile or compressive lattice stresses can be easily determined. Our results can facilitate the understanding of ultrafast phonon dynamics in GaAs single crystals.

Helicity-dependent terahertz photocurrent and phonon dynamics in hybrid metal halide perovskites.

We report the discovery of helicity-dependent ultrafast photocurrent generation in organic-inorganic perovskite by measuring terahertz (THz) electric field emissions in the time-domain. We find signatures of the circular photogalvanic effect (CPGE) where right circularly polarized light and left circularly polarized light lead to different photocurrent generation. The direction of photocurrent is also resolved by measuring the polarization of the emitted THz pulses. Furthermore, we observe distinct wavelength-dependent, coherent phonon dynamics using THz pump-induced differential reflectivity, indicative of multiple exciton resonances. Both the CPGE and exciton fine structure, together with theoretical simulations, provide compelling and complementary evidence for the existence of Rashba-type bands in perovskite.

Direct observation of interlayer coherent acoustic phonon dynamics in bilayer and few-layer PtSe2

This work reports the real-time observation of the interlayer lattice vibrations in bilayer and few-layer PtSe2 by means of the coherent phonon method. The layer-breathing mode and standing wave mode of the interlayer vibrations are found to coexist in such a kind of group-10 transition metal dichalcogenides (TMDCs). The interlayer breathing force constant standing for perpendicular coupling (per effective atom) is derived as 7.5 N/m, 2.5 times larger than that of graphene. The interlayer shearing force constant is comparable to the interlayer breathing force constant, which indicates that PtSe2 has nearly isotropic interlayer coupling. The low-frequency Raman spectroscopy elucidates the polarization behavior of the layer-breathing mode that is assigned to have A1g symmetry. The standing wave mode shows redshift with the increasing number of layers, which successfully determines the out-of-plane sound velocity of PtSe2 experimentally. Our results manifest that the coherent phonon method is a good tool to uncover the interlayer lattice vibrations, beyond the conventional Raman spectroscopy limit. The strong interlayer interaction in group-10 TMDCs reveals their promising potential in high-frequency (∼terahertz) micro-mechanical resonators.

Coherent phonon dynamics in diamond detected via multiphoton absorption

Coupling between ultrafast lattice dynamics and electronic polarization becomes increasingly important for generating terahertz frequency combs, monitor atomic potential landscapes, or high-speed information processing. Here, we show that the carrier population excited by multiphoton (5-photon) absorption in diamond crystal can be controlled at terahertz frequencies by coherent lattice vibrations-phonons. We introduce and compare two independent methods for direct monitoring of coherent phonon dynamics in diamond by using photoluminescence or photocurrent measurements on femtosecond time scale. We observe a strong signal enhancement compared to standard techniques due to transmission geometry and high-order nonlinearity of optical carrier generation.