Phonon coherent surface

Chang, Y. M., Xu, L. and Tom, H. W. K. (1997) Observation of coherent surface optical phonon oscillations by time-resolved surface second-harmonic generation. Phys. Rev. Lett., 78, 4649-4652. 

Fuyukui, M., Watanabe, K. and Matsumoto, Y. (2006) Coherent surface phonon dynamics at K-coverd Pt(lll) surface investigated by time-resolved second harmonic generation. Phys. Rev. B, 74, 195412. 

The SH intensity is proportional to P 2. Experimentally, the oscillatory part of the total SH is so small that one can ignore its second-order term. If coherent surface phonons are created by ISRS, the whole process including excitation and detection is the coherent time-domain analogue of stimulated hyper Raman scattering (y(4) process) [14]. The cross section of the SHG process is then proportional to the product of a Raman tensor in the pump transition and a hyper-Raman tensor dx k/dQn in the probe transition. 

Mode Selective Excitation of Coherent Surface Phonons [37, 38]... 

For the coherent control of reactions at surfaces, the manipulation of adsorbate motion is essential. Cs/Pt(lll) is a suitable system which provides us with a good opportunity to test whether or not we can excite preferentially one of the two modes whose frequencies are very close to each other by using tailored laser pulses. We have demonstrated the mode-selective excitation of coherent surface phonon modes on Cs/Pt(lll) by synthesized femtosecond pulse trains. 

Watanabe, K., Takagi, N. and Matsumoto, Y. (2005) Mode-selective excitation of coherent surface phonons on alkali-covered metal surfaces. Phys. Chem. Chem. Phys., 7, 2697-2700. 

A number of solid compounds have been examined with this time-domain method since the first report of coherent phonons in GaAs [10]. Coherent phonons were created at the metal/semiconductor interface of a GaP photodiode [29] and stacked GaInP/GaAs/GalnP layers [30]. Cesium-deposited [31-33] and potassium-deposited [34] Pt surfaces were extensively studied. Manipulation of vibrational coherence was further demonstrated on Cs/Pt using pump pulse trains [35-37]. Magnetic properties were studied on Gd films [38, 39]. 

Melnikov, A. V., Radu, I., Bovensiepen, U., Krupin, O., Starke, K., Matthias, F. and Wolf M. (2003) Coherent optical phonons and parametrically coupled magnons induced by femtosecond laser excitation of the Gd(OOOl) surface. Phys. Rev. Lett., 91, 227403. 

For surface coherent phonons of ferromagnetic metals, a spin-driven generation mechanism was proposed, as will be described in Sect. 2.6. 

Fig. 2.8. Left oscillatory part of the reflectivity change of Bi (0001) surface at 8K (open circles). Fit to the double damped harmonic function (solid curve) shows that the Aig and Eg components (broken and dotted curves) are a sine and a cosine functions of time, respectively. Right pump polarization dependence of the amplitudes of coherent Aig and Eg phonons of Bi (0001). Adapted from [25]...

Systematic TRSHG studies on alkali-atom adsorbed metal surfaces by Matsumoto and coworkers provided a deep insight on how coherent motions are created under very different electronic configurations [15, 77, 78]. The results showed that the coherent phonon generation critically depends on the surface and bulk electronic structure of the substrate. 

Gd(0001) surface, which serves as a model system for a ferromagnetic metal, presented a coherent coupled phonon-magnon mode at 3 THz in the TRSHG measurements, as presented in Sect. 2.6 in the previous chapter. 

An intense femtosecond laser spectroscopy-based research focusing on the fast relaxation processes of excited electrons in nanoparticles has started in the past decade. The electron dynamics and non-linear optical properties of nanoparticles in colloidal solutions [1], thin films [2] and glasses [3] have been studied in the femto- and picosecond time scales. Most work has been done with noble metal nanoparticles Au, Ag and Cu, providing information about the electron-electron and electron-phonon coupling [4] or coherent phenomenon [5], A large surface-to-volume ratio of the particle gives a possibility to investigate the surface/interface processes. 

This section has been devoted to the study of the surface excitons of the (001) face of the anthracene crystal, which behave as 2D perturbed excitons. They have been analyzed in reflectivity and transmission spectra, as well as in excitation spectra bf the first surface fluorescence. The theoretical study in Section III.A of a perfect isolated layer of dipoles explains one of the most important characteristics of the 2D surface excitons their abnormally strong radiative width of about 15 cm -1, corresponding to an emission power 10s to 106 times stronger than that of the isolated molecule. Also, the dominant excitonic coherence means that the intrinsic properties of the crystal can be used readily in the analysis of the spectroscopy of high-quality crystals any nonradiative phenomena of the crystal imperfections are residual or can be treated validly as perturbations. The main phenomena are accounted for by the excitons and phonons of the perfect crystal, their mutual interactions, and their coupling to the internal and external radiation induced by the crystal symmetry. No ad hoc parameters are necessary to account for the observed structures. 

This uitrasonio-opticai technique (or haif-opticai technique [89]) was aiso a hyphenated technique in terms of energy sources viz. thermai and opticai for phonon and photon production, respectiveiy). Thermai surface phonons restrict practical application of the technique owing to their iow scattering efficiency, which results in overly long data collection times (typicaiiy severai hours for a singie spectrum, even with advanced multipass interferometers). Similar to active Raman spectroscopy, coherent acoustic phonons are assumed to be excited by two narrow-line frequency tunable laser beams at different frequencies or by laser pulses of short duration compared to the acoustic period. 

Previous studies on phonon confinement in nanocrystals did not account for possible contributions from lattice defects [100-102]. However, the parameter L in (12.3) represents the coherence length and is, therefore, a measure of the distance between dislocation, vacancies, interstitials, impurities, and other defects within the crystal lattice. The assumption that L represents the crystal size is only valid for defect-free crystals, where the surface is considered to limit the propagation of the phonons. This assumption does not hold for imperfect crystals produced by... 

Cardona M, Giintherodt G (eds) (2000) Light scattering in solids VIII fullerenes, semiconductor surfaces, coherent phonons, vol 76, Topics in applied physics. Springer, Berlin... 

Sq Si absorption band, shifting of the probe wavelength affects probe transmission just as does shifting of the crystalline absorption spectrum. In Figure 15, the major contribution is that due to coherent scattering. Quantitative determination of the phonon-induced spectral shift is impossible, but an approximate upper limit can be set. Its value ( 1 cm" for a 10" -A phonon amplitude) indicates that the initial slope of the Sj potential with respect to intermolecular separation is rather gradual and that the slope must increase as displacement increases [98]. Thus, in addition to information about excimer formation dynamics, partial (and at this point, qualitative) information about the reactive potential surface has been elucidated. 

Since the development of ultrashort lasers, nudear wavepacket dynamics of various matters have attracted continuing attention [1,2]. The research targets extend from gas phase molecules [3, 4] to molecules in solution [5, 6], and solids [7]. In general, an excitation of matter by an ultrashort pulse with sufficient bandwidth leads to the creation of coherence between vibrational (or vibronic) eigenstates [1]. The induced nuclear wavepacket then starts to evolve on a certain potential energy surface and the dynamics is probed by a suitable pump-probe spectroscopy. The direct time-domain observation of the nudear motion provides us with valuable information on photochemical reaction dynamics, vibrational excitation/relaxation mechanisms, electron-vibration (phonon) coupling, and so on. 

Vibrational Coherence and Coherent Phonons at Alkali-Covered Metal Surfaces [24, 25, 32-34]... 

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