Coherent generation of acoustic phonons in an optical microcavity

Ultrafast coherent generation of acoustic phonons is studied in a semiconductor optical microcavity. The confinement of the light pulse amplifies both the generation and the detection of phonons. In addition, the standing wave character of the photon field modifies the generation and detection phonon bandwidth. Coherent generation experiments in an acoustic nanocavity embedded in an optical microcavity are reported as a function of laser energy and incidence angle to evidence the separate role of the optical and exciton resonances. Amplified signals and phonon spectra modified by the optical confinement are demonstrated.     

Probing unfolded acoustic phonons with X rays

Ultrafast laser excitation of an InGaAs/InAlAs superlattice (SL) creates coherent folded acoustic phonons that subsequently leak into the bulk (InP) substrate. Upon transmission, the phonons become "unfolded" into bulk modes and acquire a wave vector much larger than that of the light. We show that time-resolved x-ray diffraction is sensitive to this large-wave vector excitation in the substrate. Comparison with dynamical diffraction simulations of propagating strain supports our interpretation.     

Time-resolved X-Ray diffraction from coherent phonons during a laser-induced phase transition

Time-resolved x-ray diffraction with picosecond temporal resolution is used to observe scattering from impulsively generated coherent acoustic phonons in laser-excited InSb crystals. The observed frequencies and damping rates are in agreement with a model based on dynamical diffraction theory coupled to analytic solutions for the laser-induced strain profile. The results are consistent with a 12 ps thermal electron-acoustic phonon coupling time together with an instantaneous component from the deformation-potential interaction. Above a critical laser fluence, we show that the first step in the transition to a disordered state is the excitation of large amplitude, coherent atomic motion.     

Coherence properties of individual femtosecond pulses of an x-ray free-electron laser

Measurements of the spatial and temporal coherence of single, femtosecond x-ray pulses generated by the first hard x-ray free-electron laser, the Linac Coherent Light Source, are presented. Single-shot measurements were performed at 780?eV x-ray photon energy using apertures containing double pinholes in "diffract-and-destroy" mode. We determined a coherence length of 17 μm in the vertical direction, which is approximately the size of the focused Linac Coherent Light Source beam in the same direction. The analysis of the diffraction patterns produced by the pinholes with the largest separation yields an estimate of the temporal coherence time of 0.55?fs. We find that the total degree of transverse coherence is 56% and that the x-ray pulses are adequately described by two transverse coherent modes in each direction. This leads us to the conclusion that 78% of the total power is contained in the dominant mode.     

Scattering of nonequilibrium acoustic phonons in coarse-grained pure ZnSe with random microtwin structure

Propagation of nonequilibrium acoustic phonons in a coarse-grained ZnSe produced through chemical synthesis from a vapor phase was studied for phonons generated optically or by a metallic heater. The material is characterized by a microtwin structure in randomly oriented grains. Phonon transport studies, in combination with low-temperature photoluminescence, optical and electron microscopy, and x-ray diffraction analysis, made it possible to establish the decisive role played by extended defects in scattering of high-frequency acoustic phonons in this matterial.     

Picosecond X-ray diffraction studies of laser-excited acoustic phonons in InSb

We have employed time-resolved X-ray diffraction with picosecond temporal resolution to measure the time-dependent rocking curves of laser-irradiated asymmetrically cut single InSb crystals. Coherent acoustic phonons were excited in the crystals by irradiation with 800-nm, 100-fs laser pulses at irradiances between 0.25 and 12 mJ/cm². The induced time-dependent strain profiles (corresponding to the coherent phonons) were monitored by diffracting collimated, monochromatic pulses of X-rays from the irradiated crystals. Recording of the diffracted radiation with a fast low-jitter X-ray streak camera resulted in an overall temporal resolution of better than 2 ps. The strain associated with the coherent phonons modifies the rocking curve of the crystal in a time-dependent manner, and the rocking curve is recorded by keeping the angle of incidence of the X-rays upon the crystal fixed, but varying the energy of the incident X-rays around a central energy of 8.453 keV (corresponding to the peak of the rocking curve of the unperturbed crystal). The observed time-dependent diffraction from the irradiated crystals is in reasonable agreement with simulations over a wide range of energies from the unperturbed rocking-curve peak. Received: 22 March 2002 / Revised version: 25 March 2002 / Published online: 6 June 2002     

Control of coherent acoustic phonons in semiconductor quantum wells.

Using subpicosecond optical pump-probe techniques, coherent zone-folded longitudinal acoustic phonons (ZFLAPs) were investigated in an InGaN multiple quantum well structure. A two-pump differential transmission technique was used to generate and control coherent ZFLAP oscillations through the relative timing and amplitude of the two pump pulses. Enhancement and suppression of ZFLAP oscillations were demonstrated, including complete cancellation of generated acoustic phonons for the first time in any material system. Coherent control was used to demonstrate that ZFLAPs are generated differently in InGaN multiple quantum wells than in GaAs/AlAs superlattices.     

Spatiotemporal stability of a femtosecond hard-x-ray undulator source studied by control of coherent optical phonons

We report on the temporal and spatial stability of the first tunable femtosecond undulator hard-x-ray source for ultrafast diffraction and absorption experiments. The 2.5-1 Angstrom output radiation is driven by an initial 50 fs laser pulse employing the laser-electron slicing technique. By using x-ray diffraction to probe laser-induced coherent optical phonons in bulk bismuth, we estimate an x-ray pulse duration of 140+/-30 fs FWHM with timing drifts below 30 fs rms measured over 5 days. Optical control of coherent lattice motion is demonstrated.     

Anharmonic lattice dynamics in germanium measured with ultrafast x-ray diffraction

Damping of impulsively generated coherent acoustic oscillations in a femtosecond laser-heated thin germanium film is measured as a function of fluence by means of ultrafast x-ray diffraction. By simultaneously measuring picosecond strain dynamics in the film and in the unexcited silicon substrate, we separate anharmonic damping from acoustic transmission through the buried interface. The measured damping rate and its dependence on the calculated temperature of the thermal bath is consistent with estimated four-body, elastic dephasing times (T2) for 7-GHz longitudinal acoustic phonons in germanium.     

Probing impulsive strain propagation with X-ray pulses

Pump-probe time-resolved x-ray diffraction of allowed and nearly forbidden reflections in InSb is used to follow the propagation of a coherent acoustic pulse generated by ultrafast laser excitation. The surface and bulk components of the strain could be simultaneously measured due to the large x-ray penetration depth. Comparison of the experimental data with dynamical diffraction simulations suggests that the conventional model for impulsively generated strain underestimates the partitioning of energy into coherent modes.     

Nonequilibrium phase transition in v-group semimetals,induced by ultrashort laser pulses

Coherent, totally symmetric large-amplitude phonons in bismuth and antimony were investigated by the pump—probe method using femtosecond laser pulses. The obtained results are compared to time-resolved Raman data. It is shown that intense photoexcitation by laser pulses with a duration shorter than the lifetime and reverse phonon frequency in Bi and Sb can lead to a nonequilibrium semimetal—metal phase transition, most likely caused by the instability of the crystal’s electron subsystem.     

Transient strain driven by a dense electron-hole plasma

We measure transient strain in ultrafast laser-excited Ge by time-resolved x-ray anomalous transmission. The development of the coherent strain pulse is dominated by rapid ambipolar diffusion. This pulse extends considerably longer than the laser penetration depth because the plasma initially propagates faster than the acoustic modes. X-ray diffraction simulations are in agreement with the observed dynamics.     

A two-temperature model of optical excitation of acoustic waves in conductors

A two-temperature model of optical excitation of acoustic pulses in conductors has been developed. According to this model, the energy of light at first is absorbed by free carriers and only then is the optical pulse energy transferred to long-wavelength phonons of the conductor lattice. It is shown that the shape of the acoustic pulse excited by a laser in conductors can be presented as a convolution of the laser pulse envelope and the transfer function. An analytical dependence of the transfer function on time is derived.     

Acoustic and optical phonons and their dispersion in model ferroelastics Hg<Subscript>2</Subscript>Cl<Subscript>2</Subscript>

Thefrequency dispersion curve of acoustic and optical phonons are calculated and constructed, and the density of states of the phonon spectrum is obtained for Hg₂Cl₂ crystals. The influence of the hydrostatic pressure on the frequencies of acoustic and optical phonons and their dispersion is analyzed theoretically. It is revealed that an increase in the pressure leads to a considerable softening of the slowest acoustic TA branch (soft mode) at the X point of the Brillouin zone boundary. This behavior is consistent with the phenomenological Landau theory and correlate with experiments.     

Ultrafast acoustics in the middle UV range: coherent phonons at higher frequencies and in smaller objects

We show that the propagation of coherent acoustic phonons generated by femtosecond optical excitation can be clearly resolved using a probe laser in the middle UV (MUV) range. The MUV probe is easily produced from a high-repetition-rate femtosecond laser and a homemade frequency tripler. We present various experimental results that demonstrate efficient and high frequency detection of acoustic phonons. Thus, we show that the MUV range offers a unique way to reach higher frequencies and probe smaller objects in ultrafast acoustics.     

AMO instrumentation for the LCLS X-ray FEL

Instrumentation is being developed to conduct atomic, molecular and optical science experiments at the Linac Coherent Light Source x-ray free electron laser at the Stanford Linear Accelerator Center. This suite of instruments will be used to study the interaction of the very intense x-ray beam with the simplest forms of matter, namely atoms, molecules and clusters. The instrumentation will be ready for the start of operations of the facility in August 2009.     

Acoustic phonon emission from a weakly coupled superlattice under vertical electron transport: observation of phonon resonance

We report measurements of acoustic phonon emission from a weakly coupled AlAs/GaAs superlattice (SL) under vertical electron transport. The phonons were detected using superconducting bolometers. A peak (resonance) was observed in emission parallel to the SL growth axis when the electrical energy drop per SL period matched the energy of the first SL mini-Brillouin zone-center phonon mode. This peak was mirrored by an increase of the differential conductance of the SL. These results are evidence for stimulated emission of terahertz phonons as previously predicted theoretically and suggest that such a SL may form the basis of a SASER (sound amplification by stimulated emission of radiation) device.     

Bulk dislocation core dissociation probed by coherent x rays in silicon

We report on a new approach to probe bulk dislocations by using coherent x-ray diffraction. Coherent x rays are particularly suited for bulk dislocation studies because lattice phase shifts in condensed matter induce typical diffraction patterns which strongly depend on the fine structure of the dislocation cores. The strength of the method is demonstrated by performing coherent diffraction of a single dislocation loop in silicon. A dissociation of a bulk dislocation is measured and proves to be unusually large compared to surface dislocation dissociations. This work opens a route for the study of dislocation cores in the bulk in a static or dynamical regime, and under various external constraints.     

Response of acoustic phonons to charge and orbital order in the 50% doped bilayer manganite LaSr2Mn2O7

We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr(2)Mn(2)O(7). For excitation energies less than 15 meV, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at q = (h, h, 0), h ≤ 0.3, upon entering the low temperature charge and orbital ordered state (T(COO) = 225 K). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface below T(COO) and provides direct experimental evidence for a link between electron-phonon coupling and charge order in manganites.     

Coherent x-ray diffraction imaging with nanofocused illumination

Coherent x-ray diffraction imaging is an x-ray microscopy technique with the potential of reaching spatial resolutions well beyond the diffraction limits of x-ray microscopes based on optics. However, the available coherent dose at modern x-ray sources is limited, setting practical bounds on the spatial resolution of the technique. By focusing the available coherent flux onto the sample, the spatial resolution can be improved for radiation-hard specimens. A small gold particle (size <100 nm) was illuminated with a hard x-ray nanobeam (E=15.25 keV, beam dimensions approximately 100 x 100 nm2) and is reconstructed from its coherent diffraction pattern. A resolution of about 5 nm is achieved in 600 s exposure time.