Coherent coupling between vibrational modes of Cben H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering

We performed femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) measurements on liquid toluene and PVK film. For both samples, we selectively excited the CH stretching vibrational modes and observed the expected quantum beat signals. The frequency of the well-defined beats is in good agreement with the energy difference between the two simultaneously excited modes, which demonstrates that a coherent coupling between the vibrational modes of the C-H chemical bonds exists at the different positions of the molecules. The dephasing times of the excited modes are obtained simultaneously.     

Coherent coupling between vibrational modes of C-H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering

We performed femtosecond time-resolved coherent anti-Stokes Raman scattering(fs-CARS) measurements on liquid toluene and PVK film.For both samples,we selectively excited the CH stretching vibrational modes and observed the expected quantum beat signals.The frequency of the well-defined beats is in good agreement with the energy difference between the two simultaneously excited modes,which demonstrates that a coherent coupling between the vibrational modes of the C-H chemical bonds exists at the different positions of the molecules.The dephasing times of the excited modes are obtained simultaneously.     

Fe/Si薄膜中相干声学声子的光激发研究

本文通过抽运-探测技术, 利用飞秒激光脉冲激发并探测了Fe/Si薄膜中的高频相干声学声子. 通过经典的阻尼谐振函数, 对声学声子的动力学行为进行了拟合. 实验及拟合结果表明, 该声学声子的共振频率约为0.25 THz, 其退相时间约为12 ps, 且都与激发光的波长和能量密度无关. 声学声子的振幅随着激发光能量密度的增加而线性地增强. 临界参数12_τe-ph/T约为0.6, 表明相干声学声子的驱动力主要来源于电子热应力的贡献. 最后, 结合薄膜的厚度和质量密度, 可以得到室温下垂直于该Fe/Si薄膜表面(out of plane) 的弹性常数C_⊥约为283 GPa.     

The influence of surfaces and interfaces on coherent phonons in semiconductors

Experiments have shown that ultrafast optical excitation of semiconductors can produce oscillating changes in the optical properties of the material. The frequency of the oscillations in transmission or reflection usually matches one of the phonon modes, typically theq = 0 optical mode. These oscillations are known as coherent phonons. We discuss the role of surfaces and interfaces on the coherent phonon signal. We show that: (1) the coherent phonon signal can be used as a probe of the surface depletion field and (2) multiple interfaces as in a superlattice, can drastically alter the coherent phonon spectrum: screening of the modes in the superlattices is reduced and acoustic modes can now be excited.     

Observation of coherent phonon states in porous silicon films

The dynamics of differential transmission and reflectance spectra of porous silicon films was studied using the femtosecond excitation technique (τ≈50 fs, ?ω_pump=2.34 eV) with supercontinuum probing (?ω_probe=1.6–3.2 eV) and controlled time delay with a step of Δt=7 fs between the pump and probe pulses. A short-lived region of photoinduced bleaching was observed in the differential transmission spectra at wavelengths shorter than the pump wavelength. The excitation of coherent phonon states with a spectrum corresponding to nanocrystalline silicon with an admixture of a disordered phase was observed. The relaxation of electronic excitation was found to slow down in the spectral region where the amplitude of excited coherent vibrations was maximal.     

Selective cap opening in carbon nanotubes driven by laser-induced coherent phonons

We demonstrate the possibility of a selective nonequilibrium cap opening of carbon nanotubes as a response to femtosecond laser excitation. By performing molecular dynamics simulations based on a microscopic electronic model we show that the laser-induced ultrafast structural changes differ dramatically from the thermally induced dimer emission. Ultrafast bond weakening and simultaneous excitation of two coherent phonon modes of different frequencies, localized in the spherical caps and cylindrical nanotube body, are responsible for the selective cap opening.     

用超快电子衍射技术研究Al薄膜的超快动力学行为

超快电子衍射（UED）技术因其同时具有亚皮秒的时间分辨和亚毫埃的空间分辨能力,成为研究物质瞬态结构变化,特别是研究晶格材料超快动力学的有力工具.应用国内首台自行研制的UED系统,我们实时测量了超快激光脉冲激发下,20 nm金属Al多晶薄膜产生的相干声子和晶格热运动.实验结果显示,在晶格热运动加剧的同时,热应力的作用使晶格产生了相干振荡,并最终膨胀达到新的平衡位置.实验中测得的振荡周期以及晶格上升的温度与理论计算的结果符合较好,展示了UED技术在超快晶格动力学研究方面的广阔应用前景 关键词： 超快电子衍射 相干声子 晶格热运动     

Femtosecond reflectivity study of coherent phonons in doubly photoexcited bismuth

Ultrafast optical excitation generates coherent A_1g optical phonons in bismuth via the mechanism of displacive excitation of coherent phonons (DECP). Here, femtosecond pump-probe reflectivity spectroscopy examines the dynamics of coherent phonons in doubly photoexcited bismuth. Two successive pump pulses are employed to generate optic phonons and thus to investigate the phonon dynamics including bond softening and dephasing with variable pump fluence and inter-pump separation times. Combined with thermal analysis, it distinguishes thermal and nonthermal effects of photoexcitation on the phonon dynamics. It also reveals that photocarriers relax via electron-hole recombination and diffusion out of the optical penetration depth on ultrafast timescales of 10–20?ps.     

Coherent optical phonons in alexandrite crystal studied by Optical Kerr Effect spectroscopy

Herewith, we report on the first observation of coherent phonons in alexandrite crystal obtained by means of the femtosecond Optical Kerr Effect spectroscopy. We have managed to observe dynamics of the Raman‐active modes with high resolution and to find their lifetimes in the temperature range between 263 K and 373 K. We have used the obtained temperature dependence of phonon lifetimes and frequencies for calculation of the anharmonic coupling constants. On the basis of our results, we have also calculated the widths of homogeneously broadened Raman lines. Our results prove that, in case of transparent samples, this experimental technique is a very good alternative to the commonly used transient reflection method. Copyright © 2013 John Wiley & Sons, Ltd.     

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 Eg and A1g 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 A1g phonons, cannot be reduced to the Raman scattering responsible for the generation of lower symmetry coherent lattice modes.     

Investigation of coherent phonons in bismuth by femtosecond laser and X-ray pulse probing

Using femtosecond laser pulses, coordinated oscillations (coherent phonons) of Bi single-crystal atoms have been excited and recorded. The comparison with experimental results on the X-ray probing of coherent phonons at the same excitation energy density demonstrates that the observed lifetime and frequency shift of the oscillations are similar in both cases. Moreover, it has been revealed that the relaxation (incoherent) contributions are identical. This coincidence of the photoinduced response parameters indicates that probing in the visible spectrum correctly reflects the coherent dynamics of the Bi crystal lattice.     

Vibration-assisted coherent excitation energy transfer in a detuned dimer

The important role of high-energy intramolecular vibrational modes for excitation energy transfer in the detuned photosynthetic systems is studied. Based on a basic dimer model which consists of two two-level systems(pigments)coupled to high-energy vibrational modes, we find that the high-energy intramolecular vibrational modes can enhance the energy transfer with new coherent transfer channels being opened when the phonon energy matches the detuning between the two pigments. As a result, the energy can be effectively transferred into the acceptor. The effective Hamiltonian is obtained to reveal the strong coherent energy exchange among the donor, the acceptor, and the high-energy intramolecular.A semi-classical explanation of the phonon-assisted mechanism is also shown.     

High contrast atomic magnetometer based on coherent population trapping

We present an experimental and theoretical investigation of the coherent population trapping （CPT） resonance excited on the D1 line of 87Rb atoms by bichromatic linearly polarized laser light. The experimental results show that a lin｜｜lin tran- sition scheme is a promising alternative to the conventional circular-circular transition scheme for an atomic magnetometer. Compared with the circular light transition scheme, linear light accounts for high-contrast transmission resonances, which makes this excitation scheme promising for high-sensitivity magnetometers. We also use linear light and circular light to detect changes of a standard magnetic field, separately.     

Ultra-fast dynamics of coherent lattice and spin excitations at the Gd(0001) surface

The Gd(0001) surface is investigated by pump–probe experiments using femtosecond laser pulses at 740–860 nm wavelength. Employing optical second-harmonic generation, spin and lattice dynamics are separated through the symmetry of optical field contributions that are even and odd with respect to magnetization reversal. A coherent phonon–magnon mode at a frequency of 3 THz that is excited through the exchange-split surface state is observed in the time domain. A magneto-elastic phonon–magnon interaction based on spin–orbit coupling is weak for Gd and a modulation of the exchange interaction mediated by the lattice vibration is proposed as a microscopic interaction mechanism of this coupled mode. In parallel, electron–electron and electron–phonon interactions and their magnetic counterparts lead to incoherent dynamics of the electron, lattice, and spin subsystems. Variation of the optical wavelength shows that for longer wavelengths up to 860 nm the coherent mode dominates, while for shorter ones (≥740 nm) incoherent contributions prevail. This dependence indicates that selective depopulation of the occupied surface state component drives the coherent excitation. However, temperature-dependent studies show that the oscillation amplitude of even and odd contributions scales with the spin polarization of the surface state, suggesting that the spin dependence of the ion potentials contributes as well. Furthermore, the frequency of the coherent mode presents a blue shift with a delay of 0.17 THz/ps that saturates at the static frequency of the respective bulk phonon. This behavior is a consequence of equilibration of the screened ion potential at the surface subsequent to the intense laser excitation. PACS 78.47.+p; 63.22.+m; 63.20.Ls; 75.30.Ds     

Selective excitation of molecular mode in a mixture by femtosecond resonance-enhanced coherent anti-Stokes Raman scattering spectroscopy

Femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy is used to investigate gaseous molecular dynamics. Due to the spectrally broad laser pulses, usually poorly resolved spectra result from this broad spectroscopy. However, it can be demonstrated that by the electronic resonance enhancement optimization control a selective excitation of specific vibrational mode is possible. Using an electronically resonance-enhanced effect, iodine molecule specific CARS spectroscopy can be obtained from a mixture of iodine-air at room temperature and a pressure of 1 atm (corresponding to a saturation iodine vapour as low as about 35 Pa). The dynamics on either the electronically excited state or the ground state of iodine molecules obtained is consistent with previous studies (vacuum, heated and pure iodine) in the femtosecond time resolved CARS spectroscopy, showing that an effective method of suppressing the non-resonant CARS background and other interferences is demonstrated.     

Coherent molecular vibrational dynamics of CH2 stretching modes in polyethylene studied by femtosecond‐CARS

We have studied the coherent molecular vibrational dynamics of CH₂ stretching modes in polyethylene by time‐resolved femtosecond coherent anti‐Stokes Raman spectroscopy. We observed that the coherent vibrational relaxation of symmetric CH₂ stretching modes in polyethylene at room temperature is much faster than that previously measured in polyvinyl alcohol. In addition, it was detected that, at low temperature, the coherent vibrational relaxation of the symmetric stretching modes evidently becomes slower compared with that at room temperature. These temperature‐dependent measurements enable us to discriminate the contribution of pure dephasing mechanism, due to phonons and two‐level systems in polymer, from the contribution of lifetime of the vibrational excited state to the coherent vibrational relaxation of CH₂ stretching modes. We conclude that the coherent vibrational relaxation of symmetric CH₂ stretching modes at room temperature consists of the contribution of lifetime and approximately 1.5 times larger contribution of pure dephasing. Copyright © 2015 John Wiley & Sons, Ltd.     

Observation of coherent optical phonons excited by femtosecond laser radiation in Sb films by ultrafast electron diffraction method

The generation of coherent optical phonons in a polycrystalline antimony film sample has been investigated using femtosecond electron diffraction method. Phonon vibrations have been induced in the Sb sample by the main harmonic of a femtosecond Ti:Sa laser (λ = 800 nm) and probed by a pulsed ultrashort photoelectron beam synchronized with the pump laser. The diffraction patterns recorded at different times relative to the pump laser pulse display oscillations of electron diffraction intensity corresponding to the frequencies of vibrations of optical phonons: totally symmetric (A _1g ) and twofold degenerate (E _g ) phonon modes. The frequencies that correspond to combinations of these phonon modes in the Sb sample have also been experimentally observed.     

Entropy driven atomic motion in laser-excited bismuth

We introduce a thermodynamical model based on the two-temperature approach in order to fully understand the dynamics of the coherent A(1g) phonon in laser-excited bismuth. Using this model, we simulate the time evolution of (111) Bragg peak intensities measured by Fritz et al. [Science 315, 633 (2007)] in femtosecond x-ray diffraction experiments performed on a bismuth film for different laser fluences. The agreement between theoretical and experimental results is striking not only because we use fluences very close to the experimental ones but also because most of the model parameters are obtained from ab initio calculations performed for different electron temperatures.     

Enhancement of waves at rotational oscillations of a liquid

The generation of coherent optical phonons in an antimony film has been directly observed by the femtosecond electron diffraction method. The sample has been excited by a femtosecond laser pulse (λ = 800 nm) and probed with a pulsed photoelectron beam. Oscillations of the intensity corresponding to vibration frequencies of optical phonons excited by the laser have been observed in the obtained diffraction patterns: totally symmetric (A_1g) and twofold degenerate (E_2g) phonon modes of antimony and their combinations.