Time-Resolved Terahertz Spectroscopy with Free-Space Electro-Optic Sampling

We present a time-resolved ultrafast measurement in terahertz (THz) frequency region by means of the free-space electro-optic sampling. The fast delay scan technique is used to suppress the noise with low frequency and to improve the signal-to-noise ratio of the system. The transmission spectra of different materials are obtained.The optical properties of these materials in a THz region are shown. The broadening of spectrum and chirping phenomena are illustrated. We find that polystyrene is an excellent material for the THz application.     

High density gas state at water/graphite interface studied by molecular dynamics simulation

In this paper molecular dynamics simulations are performed to study the accumulation behaviour of N2 and H2 at water/graphite interface under ambient temperature and pressure. It finds that both N2 and H2 molecules can accumulate at the interface and form one of two states according to the ratio of gas molecules number to square of graphite surface from our simulation results： gas films （pancake-like） for a larger ratio and nanobubbles for a smaller ratio. In addition, we discuss the stabilities of nanobubbles at different environment temperatures. Surprisingly, it is found that the density of both kinds of gas states can be greatly increased, even comparable with that of the liquid N2 and liquid H2. The present results are expected to be helpful for the understanding of the stable existence of gas film （pancake-like） and nanobubbles.     

Two-Photon Absorption and Excited State Dynamics of Two Organic Molecules Containing Donor/Acceptor Moieties

Two new two-photon absorption （TPA） molecules, named SK-G1 and NT-G1, are synthesized and the photo- physical characteristics are investigated by using linear absorption spectra, one-photon fluorescence spectra and two-photon excited fluorescence spectra. Both the compounds exhibit TPA properties, and the TPA values determined by z-scan measurement are 10 GM and 39 GM for SK-G1 and NT-G1, respectively, at wavelength 80Ohm. Time-resolved spectroscopic techniques are employed to further explore the excited state dynamics of NT-G l with larger TPA cross section. The research results show that there is an ultrafast intraband energy transfer process （about 3ps） before the formation of charge transfer state with a relatively long lifetime.     

Modeling the interaction of nitrate anions with ozone and atmospheric moisture

The molecular dynamics method is used to investigate the interaction between one–six nitrate anions and water clusters absorbing six ozone molecules. The infrared(IR) absorption and reflection spectra are reshaped significantly, and new peaks appear at Raman spectra due to the addition of ozone and nitrate anions to the disperse water system. After ozone and nitrate anions are captured, the average(in frequency) IR reflection coefficient of the water disperse system increased drastically and the absorption coefficient fell.     

Time-Resolved Visualization of Laser-Induced Heating of Gold with MeV Ultrafast Electron Diffraction

Time-resolved electron diffraction employing MeV electron beams is demonstrated experimentally at the center for ultrafast diffraction and microscopy of Shanghai Jiao Tong University. A high-quality diffraction pattern is recorded by a single shot of electron pulse. Synchronization between the pump laser and the probe electron beam is achieved through measurement of electron deflection caused by the laser-induced plasmas in a metal tip. We study the ultrafast structural dynamics of the gold lattice excited by a femtosecond laser through tracing the change of Bragg peaks intensity at different time delays. It is expected that the combination of MeV ultrashort electron beams and femtoseeond laser pulses will open many new opportunities in the ultrafast and ultrasmall world.     

Dynamics of Coupled Quantum-Classical Oscillators

The dynamics of systems consisting of coupled quantum-classical oscillators is numerically investigated. It is shown that, under certain conditions, the quantum oscillator exhibits chaos. When the mass of the classical oscillator increases, the chaos will be suppressed; if the energy of the system and/or the coupling strength between the two oscillators increases, chaotic behaviour of the system appears. This result will be helpful to understand the probability of the emergence of quantum chaos and may be applied to explain the spectra of complex atoms qualitatively.     

氧化石墨烯功能化后含水甲基蓝中隐藏的驰豫通道

The mixture of graphene oxide (GO) and dye molecules may provide some new applications due to unique electronic, optical, and structural properties. Methylene blue (MB), a typical anionic dye, can attach on GO via π-π stacking and electrostatic interaction, and the molecule removal process on GO has been observed. However, it remains unclear about the ultrafast carrier dynamics and the internal energy transfer pathways of the system which is composed of GO and MB. We have employed ultrafast optical pump-probe spectroscopy to investigate the excited dynamics of the GO-MB system dispersed in water by exciting the samples at 400 nm pump pulse. The pristine MB and GO dynamics are also analyzed in t_andem for a direct comparison. Utilizing the global analysis to fit the measured signal via a sequential model, five lifetimes are acquired:(0.61±0.01) ps, (3.52±0.04) ps, (14.1±0.3) ps, (84±2) ps, and (3.66±0.08) ns. The ultrafast dynamics corresponding to these lifetimes was analyzed and the new relaxation processes were found in the GO-MB system, compared with the pristine MB. The results reveal that the functionalization of GO can alter the known decay pathways of MB via the energy transfer from GO to MB in system, the increased intermediate state, and the promoted energy transfer from triplet state MB to ground state oxygen molecules dissolved in aqueous sample.     

Ultrafast Imaging of Electronic Relaxation in Ortho-xylene： New Features from Fragmentation-Ion Spectroscopy

After light absorption, a molecule can undergo ra- diationless processes, and photophysics is one of the important general types. The photophysical pro- cesses involve internal conversion （IC） due to elec- tronic nonadiabaticity and intersystem crossing （ISC） induced by spin-orbit coupling. In polyatomic molecules that are excited IC and ISC to vibronic to higher electronic states, levels of lower electronic states are two dominant mechanisms. With the ad- vent of femtosecond ultrashort pulse, tracking and controlling the ultrafast photophysical processes be- come realizable. Due to the fact that ISC requires a change in the spin of an electron, it is usually a slower process than IC. However, extensive reports show that ultrafast competing ISC exists in a number of systems. Re- cently, Richter et al. reported femtosecond ISC in cytosine. Martinez-Fernandez et al. simulated the deactivation dynamics of photo-excited 6-thioguanine using a direct surface hopping dynamics approach Their simulations show that 6-thioguanine is another example of a system showing ultrafast ISC that can compete with IC in the same time scale. Both the spin-orbit and the dynamic couplings are important to describe realistically the excited state dynamics of 6-thioguanine. A similar phenomenon has also been evidenced in the S1 state of benzene. The exper- imental results show that the ultrafast decay of the S1 state is due to competing IC and ISC processes and both processes occur on a femtosecond timescale. Spin-orbit coupling is highly effective when the in- volved states are nearly isoenergetic.     

Real-space visualization of intercalated water phases at the hydrophobic graphene interface with atomic force microscopy

The phase behavior of water is a topic of perpetual interest due to its reinai kable anomalous properties and importance to biology,material science,geoscience,nanoscience,etc.It is predicted confined water at interface can exist in large amounts of crystalline or amorphous states.However,the experimental evidence of coexistence of liquid water phases at interface is still insufficient.Here,a special folding few-layers graphene film was elaborate prepared to form a hydrophobic/hydrophobic interface,which can provide a suited platform to study the structure and properties of confined liquid water.The real-space visualization of intercalated water layers phases at the folding interface is obtained using advanced atomic force microscopy(AFM).The folding graphene interface displays complicated internal interfacial characteristics.The intercalated water molecules present themselves as two phases,low-density liquid(LDL,solid-like)and high-density liquid(HDL,liquid-like),according to their specific mechanical properties taken in two multifrequency-AFM(MF-AFM)modes.Furthermore,the water molecules structural evolution is demonstrated in a series of continuous MF-AFM measurements.The work preliminary confirms the existence of two liquid phases of water in real space and will inspire further experimental work to deeply understanding their liquid dynamics behavior.     

Structure and dynamics of ordered water in a thick nanofilm on ionic surfaces

The structure and dynamics of water in a thick film on an ionic surface are studied by molecular dynamic simulations. We find that there is a dense monolayer of water molecules in the vicinity of the surface. Water molecules within this layer not only show an upright hydrogen-down orientation, but also an upright hydrogen-up orientation. Thus, water molecules in this layer can form hydrogen bonds with water molecules in the next layer. Therefore, the two-dimensional hydrogen bond network of the first layer is disrupted, mainly due to the O atoms in this layer, which are affected by the next layer and are unstable. Moreover, these water molecules exhibit delayed dynamic behavior with relatively long residence time compared with those bulk-like molecules in the other layers. Our study should be helpful to further understand the influence of water film thickness on the interfacial water at the solid-liquid interface.     

二维格子神经元网络的振动共振和非线性振动共振

本文采用数值模拟的方法, 在通过电突触耦合或化学突触耦合的二维格子神经元网络中, 研究了FitzHugh-Nagumo神经元受到双频信号输入时神经元网络对低频信号的响应特性. 结果表明:当固定受到双频输入信号的神经元在体系中所占的比例且FitzHugh-Nagumo神经元参数处于可激发区域时双频信号中的高频部分可诱导出动作电位产生, 而且随着高频输入信号强度的增加, 神经元网络对低频输入信号响应先增大后减小, 出现了极大值, 即发生了振动共振现象. 另外本文还研究了神经元网络对低频输入信号的二次谐波的响应, 同样发现了非线性振动共振现象, 并且体系对低频信号的响应随着其频率ω 的增加也产生共振现象, 即发生了双共振现象. 上述共振现象在以电突触耦合的二维格子神经元网络中和以化学突触耦合的二维格子神经元网络中都可以观察到. 当固定双频输入信号中高频输入信号强度时, 随着受到双频输入信号的神经元在体系中所占比例的变化, 电突触耦合的二维格子神经元网络对低频输入信号的响应与化学突触耦合的二维格子神经元网络对低频输入信号的响应相比有很大的不同.     

The impact of vibrational wave function on low energy electron vibrational scattering from nitrogen molecule

The vibrational wave function of the target theoretically plays an important role in the calculation of vibrational excitation cross sections. By a careful study of the differential cross sections resulting from different vibrational wave functions we find that cross sections are susceptible to vibrational wave functions. Minor changes in the vibration wave function may cause a significant change in the cross section. Even more surprising is that by selecting a few numbers of potential models(which determine the vibrational wave functions) we can often calculate the differential scattering cross section in much closer agreement with experiment in the framework of body-frame vibrational close-coupling theory, which suggest that an accurate potential energy may play a more important role in scattering than we thought before.     

Vibrational spectra and intramolecular vibrational redistribution in methane and its isotopomers

An improved U(2) algebraic model is introduced to study the stretching and bending vibrational spectra of methane and its isotopomers.The algebraic model with fewer parameters reproduces the experimental spectra with good precision.Moreover,the obtained parameters describe well the correct behavior of isotopic substitution.It is shown that the Fermi resonance leads to a very fast intramolecular vibrational redistribution among stretches and bends.     

Vibrational dynamics of nitromethane mixed with IR780 dye studied by coherent anti‐stokes Raman spectroscopy

Vibrational coupling between different kinds of molecules in liquid mixture is studied by multiplex coherent anti‐Stokes Raman spectroscopy (CARS). To identify vibrational coherence, fs‐probe with high time resolution and narrowband‐probe with high spectral resolution are adopted in CARS experiments. Using liquid nitromethane (NM) mixed with organic dye IR780 perchlorate as the sample, we can clearly observe the interference between different vibrational modes. The intermolecular vibrational interaction between NM and IR780 molecules results in the vibrational coherence transfer (VCT) in the form of a change of phase correlation. Compared with symmetric bending vibration of NO₂, coherence transfer is found to be easier to take place between C―N bond of NM and vibrations of IR780, which indicates the selectivity of intermolecular vibrational interaction. The selectivity is deduced to be related to the coordination between intramolecular and collective motion of molecules. Copyright © 2016 John Wiley & Sons, Ltd.     

Analysis of vibrational spectra of nano-bio molecules： Application to metalloporphrins

In this paper, we have applied the Lie algebraic model to nano-bio molecules to determine the vibrational spectra of different stretching and bending vibrational modes. The determined vibrational energy levels by the Lie algebraic model are compared with the experimental data. The results from the theoretical mode[ are consistent with the experimental data. The vibrational energy levels are clustering in the excited states.     

振动图像获得的普遍方法

利用自制电位传感器将振动的信息传递给示波器,即可在示波器屏幕上显示出振动图像,可进一步得到振动周期,从而达到对诸多物理量的间接测量.     

Rovibrational and energetic analysis of the hydroxyethynyl anion (CCOH−)

For the first time, high-level structural and rovibrational data are provided for the hyroxyethynyl anion, CCOH^?. CCOH^? is a promising molecule for interstellar detection even though no new anions have been observed in the interstellar medium for the past half-decade. The large dipole moment of the corresponding neutral radical may be key for its creation as has been hypothesised and supported for other anions known to exist in various astronomical environments. Highly accurate quartic force fields are employed where previous benchmarks have produced spectroscopic constants and anharmonic vibrational frequencies within 20 MHz and 1 cm^?1, respectively, of experiment. This same approach is applied here for CCOH^? and its deuterated isotopologue with the goal of assisting laboratory experiments and/or astronomical observers in the potential detection of this anion.     

Density functional theory calculations and vibrational spectra of p‐bromonitrobenzene

FT‐IR and FT‐Raman spectra of p‐bromonitrobenzene (p‐BNB) have been recorded in the region 4000–400 cm⁻¹ and 4000–50 cm⁻¹, respectively. The molecular structure, geometry optimization, vibrational wavenumbers have been investigated. The spectra were interpreted with the aid of normal coordinate analysis based on the density functional theory (DFT) using the standard B3LYP/6‐31G method and basis set combination and was scaled using multiple scale factors yielding good agreement between observed and calculated wavenumbers. The results of the calculations are applied to simulate infrared and Raman spectra of the title compound which showed reasonable agreement with the observed spectra. Copyright © 2009 John Wiley & Sons, Ltd.     

Generation of Arbitrary Pure States for Three-Dimensional Motion of a Trapped Ion

In this paper, we propose a scheme for generating an arbitrary three-dimensional pure state of vibrational motion of a trapped ion. Our scheme is based on a sequence of laser pulses, which are tuned to the appropriate vibrational sidebands with respect to the appropriate electronic transition.     

相干喇曼诱导甲烷V-T弛豫过程

本文首次报道了用相干喇曼激光诱导红外荧光的方法,研究多原子分于-OH_4的振动能转移过程,并测出v_4振动能级到平动能转移速率常数为:K_(VL)=(8±)×10_(-5).