共查询到20条相似文献,搜索用时 31 毫秒
1.
Coherent coupling between vibrational modes of C-H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering 下载免费PDF全文
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. 相似文献
2.
Takanori Kozai Yuya Kayano Takahito Aoi Noriaki Tsurumachi Shunsuke Nakanishi 《Journal of Raman spectroscopy : JRS》2015,46(4):384-387
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. 相似文献
3.
Theoretical and experimental investigations of coherent phonon dynamics in sapphire crystal using femto- second time-resolved coherent anti-Stokes Raman scattering 下载免费PDF全文
We report on the theoretical and the experimental investigations of the coherent phonon dynamics in sapphire crystal using the femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) technique. The temporal chirped white-light continuum (WLC) is used for the Stokes pulse, therefore we can perform the selective excitation of the phonon modes without using a complicated laser system. The expected quantum beat phenomenon is clearly observed. The theoretical formulas consist very well with the experimental results. The dephasing times of the excited phonon modes, the wavenumber difference, and the phase shift between the simultaneously excited modes are obtained and discussed. This work opens up a way to study directly high-frequency coherent phonon dynamics in bulk crystals on a femtosecond time scale and is especially helpful for understanding the nature of coherent phonons. 相似文献
4.
ZHENG Shi-Biao 《理论物理通讯》2005,43(3):523-525
We propose a scheme to generate entangled coherent states for the
vibrational modes of N trapped ions. In the scheme the first ion is
sequentially excited by two travelling wave laser fields tuned to the ion
transition. The scheme works in the strong-excitation regime, which is of
experimental importance in view of decoherence. 相似文献
5.
We propose a scheme for the generation of entangled coherent states for the center-of-mass and relative vibrational modes of two trapped ions. In the scheme the ions are simultaneously illuminated by a single standing-wave laser tuned to the carrier. The scheme allows the production of an entangled coherent states with a considerably high speed as long as a laser field of sufficiently high intensity is available. 相似文献
6.
LIN Li-Hua JIANG Yun-Kun YANG Zhen-Biao YE Sai-Yun 《理论物理通讯》2005,44(4):712-714
We propose a scheme for the generation of entangled coherent states for the center-of-mass and relative vibrational modes of two trapped ions. In the scheme the ions are simultaneously illuminated by a single standing-wave laser tuned to the carrier. The scheme allows the production of an entangled coherent states with a considerably high speed as long as a laser field of sufficiently high intensity is available. 相似文献
7.
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. 相似文献
8.
LINLi-Hua WANGLing-Zhi JIANGYun-Kun 《理论物理通讯》2003,40(2):207-210
We proposed a scheme for the reconstruction of the quantum states for the center-of-mass vibrational mode of two trapped ions. In the scheme the ions are multichromatically excited by three lasers. Then measurement of the difference between probabilities of the ions being both in electronic ground and excited states directly yields the Wigner characteristic function for the center-of-mass vibrational state. The scheme can also be used to prepare entangled coherent states for the center-of-mass and relative vibrational modes. 相似文献
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10.
ZHENG Shi-Biao 《理论物理通讯》2005,44(12)
We propose a method for the generation of superpositions of two-mode coherent states for the center-of-mass and relative vibrational modes of two trapped ions. In the scheme the ions are driven by a single travelling-wave laser field tuned to the carrier. Then a measurement of the internal states collapses the vibrational modes to the entangled coherent state. 相似文献
11.
ZHENG Shi-Biao 《理论物理通讯》2005,44(6):1071-1072
We propose a method for the generation of superpositions of two-mode coherent states for the center-of-mass and relative vibrational modes of two trapped ions. In the scheme the ions are driven by a single travelling-wave laser field tuned to the carrier. Then a measurement of the internal states collapses the vibrational modes to the entangled coherent state. 相似文献
12.
I. V. Shelaev M. N. Mozgovaya O. A. Smitienko F. E. Gostev T. B. Fel’dman V. A. Nadtochenko O. M. Sarkisov M. A. Ostrovskii 《Russian Journal of Physical Chemistry B, Focus on Physics》2014,8(4):510-517
The dynamics of the coherent photoisomerization of the 11-cis-retinal in bovine rhodopsin is studied by femtosecond time-resolved laser absorption spectroscopy with a resolution of 30 fs. Rhodopsin is excited with 500-, 535-, and 560-nm femtosecond pulses to produce different initial Franck-Condon states with different vibrational energies of the molecule in its electronically excited state. The time evolution of the photoinduced differential absorption spectra of rhodopsin is measured upon excitation with a femtosecond pulse in a spectral range from 400 to 720 nm. Oscillations in the time-resolved absorption of the rhodopsin photoproducts, such as photorhodopsin with a vibrationally excited all-trans-retinal and in its initial-state rhodopsin with a vibrationally excited 11-cis-retinal, are examined. It is demonstrated that these oscillations reflect the dynamics of coherent vibrational wavepackets. The Fourier transform of these oscillatory components yields frequencies, amplitudes, and initial phases of various vibrational modes involved in the motion the wavepackets in both photoproducts. The main vibrational modes manifest themselves at frequencies of 62 and 160 cm?1 for photorhodopsin and 44 and 142 cm?1 for initial-state rhodopsin. It is shown that these vibrational modes are directly involved in the coherent reaction under the study, with their amplitudes in the power spectrum produced by the Fourier transform of the kinetic curves being dependent on the wavelength of rhodopsin excitation. 相似文献
13.
Master equation of a relevant electronic and vibrational system is derived for a special diabatic basis corresponding to vertical processes. It is shown that bath modes contribute dynamically to the inter-state coupling only at short times. For long times the bath-induced inter-state coupling is static and increases with the contribution of bath modes to the Stokes shift and to the Herzberg-Teller correction of the excited state. Simultaneously, the time evolution of excited state population is studied numerically for the system consisting of two electronic levels interacting with two vibrational modes, coupled to a heat bath. A mutual coupling of the vibrational modes in the excited state is taken into account (Duschinsky effect). Excited state population relaxes faster if interacting vibrational mode dissipates its energy via vibrational mode of a smaller eigenfrequency. Fast component of excited state depopulation cannot be achieved via coherent mode-mode coupling, if the second mode is not directly coupled to the electronic inter-state transition. 相似文献
14.
利用作者自制的超连续谱激发时间分辨相干反斯托克斯拉曼散射(coherent anti-stokes Ranman scat-tering,CARS)谱仪同时测得反映分子组成的各种振动谱以及这些振动模式各自的退相时间.实验对苯甲腈样品分子振动谱中5个典型分子振动模式的振动弛豫过程进行了测量,一次获得了这种分子各振动模式对... 相似文献
15.
Within the Franck–Condon approximation, the single ionisation of H2 leaves H+2 in a coherent superposition of 19 nuclear vibrational states. We numerically design an optimal laser pulse train to transfer such a coherent nuclear wave packet to the ground vibrational state of H+2. Frequency analysis of the designed optimal pulse reveals that the transfer principle is mainly an anti-Stokes transition, i.e. the H+2 in 1sσg with excited nuclear vibrational states is first pumped to 2pσg state by the pulse at an appropriate time, and then dumped back to 1sσg with lower excited or ground vibrational states. The simulation results show that the population of the ground state after the transfer is more than 91%. To the best of our knowledge, this is the highest transition probability when the driving laser field is dozens of femtoseconds. 相似文献
16.
Scanning the energy dissipation process of energetic materials based on excited state relaxation and vibration–vibration coupling 下载免费PDF全文
The energy dissipation mechanism of energetic materials(EMs) is very important for keeping safety. We choose nitrobenzene as a model of EM and employ transient absorption(TA) spectroscopy and time-resolved coherent anti-stokes Raman scattering(CARS) to clarify its energy dissipation mechanism. The TA data confirms that the excited nitrobenzene spends about 16 ps finishing the twist intramolecular charge transfer from benzene to nitro group, and dissipates its energy through the rapid vibration relaxation in the initial excited state. And then the dynamics of vibrational modes(VMs) in the ground state of nitrobenzene, which are located at 682 cm~(-1)(v_1), 854 cm~(-1)(v_2), 1006 cm~(-1)(v_3), and 1023 cm~(-1)(v_4),is scanned by CARS. It exhibits that the excess energy of nitrobenzene on the ground state would further dissipate through intramolecular vibrational redistribution based on the vibrational cooling of vi and v_2 modes, v_1 and v_4 modes, and v_3 and v_4 modes. Moreover, the vibration-vibration coupling depends not only on the energy levels of VMs, but also on the spatial position of chemical bonds relative to the VM. 相似文献
17.
The phonon-assisted process of energy transfer aiming at exploring the newly emerging frontier between biology and physics is an issue of central interest.This article shows the important role of the intramolecular vibrational modes for excitation energy transfer in the photosynthetic systems.Based on a dimer system consisting of a donor and an acceptor modeled by two two-level systems,in which one of them is coupled to a high-energy vibrational mode,we derive an effective Hamiltonian describing the vibration-assisted coherent energy transfer process in the polaron frame.The effective Hamiltonian reveals in the case that the vibrational mode dynamically matches the energy detuning between the donor and the acceptor,the original detuned energy transfer becomes resonant energy transfer.In addition,the population dynamics and coherence dynamics of the dimer system with and without vibration-assistance are investigated numerically.It is found that,the energy transfer efficiency and the transfer time depend heavily on the interaction strength of the donor and the high-energy vibrational mode,as well as the vibrational frequency.The numerical results also indicate that the initial state and dissipation rate of the vibrational mode have little influence on the dynamics of the dimer system.Results obtained in this article are not only helpful to understand the natural photosynthesis,but also offer an optimal design principle for artificial photosynthesis. 相似文献
18.
In this work we study the spectrum of vibrational modes in metal nanoparticles with a dielectric core. Vibrational modes are
excited by the rapid heating of the particle lattice that takes place after laser excitation, and can be monitored by means
of pump-probe spectroscopy as coherent oscillations of transient optical spectra. In nanoshells, the presence of two metal
surfaces results in a substantially different energy spectrum of acoustic vibrations than for solid particles. We calculated
the energy spectrum as well as the damping of nanoshell vibrational modes. The oscillator strength of the fundamental breathing
mode is larger than that in solid nanoparticles. At the same time, in very thin nanoshells, the fundamental mode is overdamped
due to instantaneous energy transfer to the surrounding medium.
PACS 78.67.-n; 78.67.Bf; 63.22.+m 相似文献
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20.
Preparation of multicomponent motional coherent and squeezed coherent states of a trapped ion 总被引:1,自引:0,他引:1 下载免费PDF全文
In this paper, we present a scheme for preparation of multicomponent motional coherent and squeezed coherent states of the quantized centre of mass of an ion trapped in a one-dimensional harmonic potential and driven by two travelling-wave laser beams tuned to the nth red and blue vibrational sidebands, respectively. In addition, our scheme also provides experimental possibility for quantum state engineering. 相似文献