Coherent Lattice Dynamics Research Articles

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).

Quantum theory of light-driven coherent lattice dynamics

The exposure to intense electromagnetic radiation can induce distortions and symmetry breaking in the crystal structure of solids, providing a route for the all-optical control of their properties. In this manuscript, we formulate a unified theoretical approach to describe the coherent lattice dynamics in presence of external driving fields, electron-phonon and phonon-phonon interactions, and quantum nuclear effects. The main mechanisms for the excitation of coherent phonons - including infrared absorption, displacive excitation, inelastic stimulated Raman scattering, and ionic Raman scattering - can be seamlessly accounted for. We apply this formalism to a model consisting of two coupled phonon modes, where we illustrate the influence of quantum nuclei on structural distortions induced by ionic Raman scattering. Besides validating the widely-employed classical models for the coherent lattice dynamics, our work provides a versatile approach to methodically explore the emergence of quantum nuclear effects in the structural response of crystal lattice to strong fields.

Ultrafast formation of quantized interlayer vibrations in Bi2Se3 by photoinduced strain waves.

This study comprehensively investigated the coherent lattice dynamics in Bi2Se3 by ultrafast optical pump-probe spectroscopy with tunable near-infrared probe pulses. Sample-thickness- and probe-wavelength-dependent experiments revealed the key role of Bi2Se3 optical property in the generation and detection of photoinduced strain waves, whose confinement initiated coherent interlayer vibrations. Furthermore, the frequency and lifetime of the interlayer vibrations could be quantitatively explained with a modified linear chain and an acoustic mismatch model considering elastic coupling at sample-substrate interfaces. The results of this work provide insights for analyzing and interpreting, through ultrafast optical spectroscopy, nanomechanical interactions in layered materials.

High-harmonic spectroscopy of coherent lattice dynamics in graphene

High-harmonic spectroscopy of solids is a powerful tool, which provides access to both electronic structure and ultrafast electronic response of solids, from their band structure and density of states to phase transitions, including the emergence of the topological edge states, to the PetaHertz electronic response. However, in spite of these successes, high-harmonic spectroscopy has hardly been applied to analyze the role of coherent femtosecond lattice vibrations in the attosecond electronic response. Here we study coherent phonon excitations in monolayer graphene to show how high-harmonic spectroscopy can be used to detect the influence of coherent lattice dynamics, particularly longitudinal and transverse optical phonon modes, on the electronic response. Coherent excitation of the in-plane phonon modes results in the appearance of sidebands in the spectrum of the emitted harmonic radiation. We show that the spectral positions and the polarization of the sideband emission offer a sensitive probe of the dynamical symmetries associated with the excited phonon modes. Our work brings the key advantage of high-harmonic spectroscopy---the combination of subfemtosecond to tens of femtoseconds temporal resolution---to the problem of probing phonon-driven electronic response and its dependence on the dynamical symmetries in solids.

Time-resolved interplay between superradiant and subradiant states in superradiance lattices of Bose-Einstein condensates

The collective spontaneous emission of many atoms is significantly different from that of a single atom, depending on the geometry and the phase correlation of atomic ensembles. However, experimental observation of arbitrary superradiant and subradiant states of atoms remains challenging due to the difficulties in both preparation and detection of those states. Here we report the time-resolved observation of superradiance from a timed Dicke state in a momentum-space superradiance lattice of Bose-Einstein condensates, which enables an in situ measurement of the coherent lattice dynamics involving both superradiant and subradiant states. The long-lasting oscillation in the superradiant emission is contributed by population transport from the subradiant states in the superradiance lattice. This work paves the way to prepare and observe subradiant states, which has promising applications in quantum information processing.

Coherent GHz lattice and magnetization excitations in thin epitaxial Ag/Fe/Cr/Fe films

We excited an epitaxial magnetic Ag/Fe/Cr/Fe multilayer nonthermally and nonoptically with very short (1 ps) electromagnetic pulses. We detected the synchronous phononic-magnetic response by time-resolved magneto-optical Kerr effect measurements. The Ag/Fe/Cr/Fe multilayer was patterned into a coplanar waveguide transmission line, and the electromagnetic pulses were generated by pulsed-laser illumination of an integrated GaAs photoconductive switch (PCS). The detected magnetic excitations comprise up to four narrow-band high-order modes with the highest frequency reaching 30 GHz. The mode frequencies are independent of both temperature in the range from 16 to 300 K and the applied external magnetic field up to 120 mT. Our analysis shows that the origin of the rigidity of these high-frequency modes is the strong coupling of the magnetic subsystem with the lattice of the Ag/Fe/Cr/Fe multilayer. The exciting electromagnetic pulse generated by the PCS induces, via magnetoelastic coupling, long-lived (ns) standing GHz acoustic waves normal to the Ag/Fe/Cr/Fe film plane. These lattice oscillations in turn couple back and drive the magnetization oscillations via the magnetoelastic coupling. The temperature and field dependence of the damping of the oscillations can be described by inelastic phonon-phonon and phonon-magnon scattering. Our study opens up a possibility of using coherent lattice and magnetization dynamics in ferromagnetic films for spintronic devices at GHz clock rates.

Ultrafast Carrier and Lattice Dynamics in Plasmonic Nanocrystalline Copper Sulfide Films.

Excited carrier dynamics in plasmonic nanostructures determines many important optical properties such as nonlinear optical response and photocatalytic activity. Here it is shown that mesoscopic plasmonic covellite nanocrystals with low free‐carrier concentration exhibit a much faster carrier relaxation than in traditional plasmonic materials. A nonequilibrium hot‐carrier population thermalizes within first 20 fs after photoexcitation. A decreased thermalization time in nanocrystals compared to a bulk covellite is consistent with the reduced Coulomb screening in ultrathin films. The subsequent relaxation of thermalized, equilibrium electron gas is faster than in traditional plasmonic metals due to the lower carrier concentration and agrees well with that in a bulk covellite showing no evidence of quantum confinement or hot‐hole trapping at the surface states. The excitation of coherent optical phonon modes in a covellite is also demonstrated, revealing coherent lattice dynamics in plasmonic materials, which until now was mainly limited to dielectrics, semiconductors, and semimetals. These findings show advantages of this new mesoscopic plasmonic material for active control of optical processes.

Coherent lattice dynamics in opaque crystals: Testing the adequacy of two-tensor model

We report the ultrafast pump-probe study of $\mathrm{B}{\mathrm{i}}_{2}\mathrm{T}{\mathrm{e}}_{3}$, Sb, Bi, and Te aimed to check the two-tensor model predictions for the creation of lattice coherence. The dependence of coherent ultrafast response on phonon frequency was measured for topological insulator $\mathrm{B}{\mathrm{i}}_{2}\mathrm{T}{\mathrm{e}}_{3}$, the spectrum of which possesses two fully symmetric phonons. The effect of the pump pulse duration and power on the magnitude of coherent amplitude was evaluated in the model opaque crystals, such as two semimetals, bismuth and antimony, and semiconducting tellurium. In our analysis of the pump-probe data, we separated the transient total reflectivity into the sum of two contributions: one due to the photogenerated carriers and the second due to the coherent phonons. All fully symmetric phonons exhibit a cosinelike dependence and grow linearly with increasing average pump power provided the pulse duration remains unchanged. Varying the pump pulse duration, we observed a monotonic decrease of coherent amplitude for longer pulses, whereas the electronic contribution was almost unchanged. This lack of the correlation between the carriers and the coherent amplitude was further supported by coherent control experiments on Te. Based on the comparison of theoretical predictions with experimental observations, we conjecture that the lattice coherence creation in opaque crystals can be linked to a Raman-like process.

Direct characterization of photoinduced lattice dynamics in BaFe2As2.

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe2As2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands.

Ultrafast lattice response of photoexcited thin films studied by X-ray diffraction.

Using ultrafast X-ray diffraction, we study the coherent picosecond lattice dynamics of photoexcited thin films in the two limiting cases, where the photoinduced stress profile decays on a length scale larger and smaller than the film thickness. We solve a unifying analytical model of the strain propagation for acoustic impedance-matched opaque films on a semi-infinite transparent substrate, showing that the lattice dynamics essentially depend on two parameters: One for the spatial profile and one for the amplitude of the strain. We illustrate the results by comparison with high-quality ultrafast X-ray diffraction data of SrRuO3 films on SrTiO3 substrates.

Ultrafast coherent lattice and incoherent carrier dynamics in bismuth: time-domain results

The investigations of transient electronic processes and their influence on coherent lattice dynamics in Bi by different femtosecond spectroscopy methods are reviewed. The results of broadband optical, x-ray, and ultrashort electron beam probes in the study of coherent phonons and incoherent carrier dynamics are compared. Some coherent phonon peculiarities arising at high excitation are described. The difference between phonons of different symmetries and various generation mechanisms are discussed, highlighting their assignment to the decay of particular excited electronic states of bismuth. Data analysis revealed significant wavevector dependence of electron–hole and electron–phonon coupling strength along the Г–T direction of the Brillouin zone. Comparison of the coherent amplitude as a function of the pump photon wavelength from 400 to 2500 nm for two different in symmetry Eg and A1g phonon modes with respective spontaneous resonance Raman profiles revealed that their generation mechanisms are quite distinct. Displacive excitation, which is the main mechanism for the generation of coherent A1g phonons, cannot be reduced to the Raman scattering responsible for the generation of lower symmetry coherent lattice modes.

Coherent structural dynamics of a prototypical charge-density-wave-to-metal transition.

Using femtosecond time-resolved x-ray diffraction, we directly monitor the coherent lattice dynamics through an ultrafast charge-density-wave-to-metal transition in the prototypical Peierls system K(0.3)MoO(3) over a wide range of relevant excitation fluences. While in the low fluence regime we directly follow the structural dynamics associated with the collective amplitude mode; for fluences above the melting threshold of the electronic density modulation we observe a transient recovery of the periodic lattice distortion. We can describe these structural dynamics as a motion along the coordinate of the Peierls distortion triggered by the prompt collapse of electronic order after photoexcitation. The results indicate that the dynamics of a structural symmetry-breaking transition are determined by a high-symmetry excited state potential energy surface distinct from that of the initial low-temperature state.

Generation of coherent phonons in bismuth by ultrashort laser pulses in the visible and NIR: Displacive versus impulsive excitation mechanism

We have applied femtosecond pump-probe technique with variable pump wavelength to study coherent lattice dynamics in Bi single crystal. Comparison of the coherent amplitude as a function of pump photon energy for two different in symmetry E g and A 1 g phonon modes with respective spontaneous resonance Raman profiles reveals that their generation mechanisms are quite distinct. We show that displacive excitation, which is the main mechanism for the generation of coherent A 1 g phonons, cannot be reduced to the Raman scattering responsible for the generation of lower symmetry coherent lattice modes.

Time-resolved X-ray Diffraction Studies of Coherent Lattice Dynamics Using Synchrotron Radiation

Significant progress in recent development of synchrotron radiation (SR) sources has offered the opportunity for time-resolved X-ray diffraction studies of fast lattice dynamics in the atomic scale. The coherent atomic motion, as seen in coherent optical and acoustic phonons which are induced by femtosecond pulsed laser irradiation of semiconductor surface has directly been observed with the time-resolved X-ray diffraction technique. In this article, the time-resolved diffraction methods using an SR beam are summarized, and the demonstrations for acoustic pulse echo, coherent acoustic phonon, and optical phonon are reviewed as examples of the investigation on coherent lattice dynamics. The future prospective on the investigation of lattice dynamics using time-resolved X-ray diffraction experiments is also discussed.

Generation of coherent phonons in opaque crystals: A radio engineering analogy

A model is proposed for generating coherent phonons by ultrashort laser pulses in opaque crystals. The model is based on the radio engineering analogy with two coupled RLC circuits, of which the first circuit corresponds to the electronic subsystem of the crystal and the second circuit corresponds to the lattice sub-system. It is demonstrated that this analogy makes it possible to describe a number of characteristic properties of coherent phonons and facilitates the separation of the contributions from the nonequilibrium charge carriers and the coherent lattice dynamics to the time-resolved reflection signal in opaque crystals.

Excitation of Coherent Phonons in Crystalline Bi: Theory for Driving Atomic Vibrations by Femtosecond Pulses

AbstractIn this paper we show time-resolved experiment with 35 fs resolution on bismuth single crystal, for which very high sensitivity detection system has been used. Coherent and incoherent lattice dynamics as well as electrons dynamics can be clearly seen into the reflectivity changes. The complex behaviour of the reflectivity could not be explained in the light of the existing theories. Therefore, we developed a new theory, starting from the very basic principle of laser-matter interaction, which is in good agreement with experimental results. Two main results will be shown: the coherent phonon is excited by the temperature gradient; the changes in reflectivity are related directly to the changes in electron-phonon collision frequency.

Coherent optical phonons in diamond

The authors report femtosecond dynamics of the coherent optical phonon of single crystal diamond. Sub-10fs, 395nm laser pulses excite 40THz coherent phonons with an extremely small damping rate (0.15ps−1). Linear power dependence of the phonon amplitude under off-resonant excitation condition gives a direct evidence for an eletric-field-driven generation mechanism. The coherent phonon generation is noticeably suppressed by doping with nitrogen impurities, in spite of their absorption in the near ultraviolet. The present study demonstrates that a simple pump-probe technique can be a powerful tool for evaluating the ultrafast coherent electronic and lattice dynamics of diamond materials.

Picosecond time-resolved x-ray diffraction probe of coherent lattice dynamics (abstract) (invited)

The short pulses of hard x rays from synchrotron and laser based sources are sensitive probes of lattice dynamics on an ultrafast time scale. Using pump–probe time-resolved x-ray diffraction, we are able to follow the propagation of a picosecond coherent acoustic pulse in an ultrafast laser-strained single crystal. Comparison of the data with dynamical diffraction simulations allows for the quantitative determination of both the surface and bulk components of the associated strain. This technique is scalable to femtosecond and shorter time scales as x-ray pulses become shorter in duration, such as in fourth generation light sources. In addition, the diffraction of x rays off of coherent optical phonons may lead to the production of a femtosecond x-ray switch.

Coherent lattice dynamics of highly photo-excited tellurium

We use time-resolved reflectivity measurements to investigate the ultrafast lattice dynamics of tellurium after excitation with intense femtosecond laser pulses. The frequency of impulsively generated coherent optical phonons is continuously red-shifted with increasing excitation fluence. We show experimentally that this softening of the semiconductor lattice is essentially nonthermal and directly related to the high-density electronic excitation of the crystal. Numerical simulations account for the main features of the experimental data. They indicate a dominant influence of the inhomogeneous excitation conditions on the apparent damping of the coherent phonons. From a comparison between experimental and numerical results we obtain a first estimate of the critical excitation density that leads to an optically induced, nonthermal phase transition of the crystal.