Spectrally resolved coherent transient signal for ultracold rubidium molecules

We present spectrally resolved pump-probe experiments on the photoassociation of ultracold rubidium atoms with shaped ultrashort laser pulses. The pump pulse causes a free-bound transition leading to a coherent transient signal of rubidium molecules in the first excited state. In order to achieve a high frequency resolution the bandwidth of the pump pulse is reduced to a few wavenumbers. The frequency dependence of the transient signal close to the D1 atomic resonance is investigated for characteristic pump-probe delay times. The observed spectra, which show a pronounced dip for pump-probe coincidence, are interpreted using quantum dynamical calculations.     

Ultrafast dynamics of a charge-transfer dimer as a model for the photoinduced phase transition of charge-transfer compounds

By applying ultrafast pump-probe spectroscopy with 15 fs temporal resolution to (TMTTF(+))(2) dimers we provide a full picture of the structural relaxation following photoexcitation of their CT transition. Both population and coherent phonon dynamics allow tracking wave packet motion onto the multidimensional excited state potential energy surface, as obtained by density functional theory calculations. We show that the vibrations that are strongly coupled to the charge-transfer transition of the dimer correspond to those driving the photoinduced phase transition occurring in charge-transfer crystalline solids.     

Excited State Absorption Study in Hematoporphyrin IX

We present the study of the excited state absorption of Hematoporphyrin IX dissolved in dimethyl sulfoxide. All measurements were carried out using open aperture Z-scan and white-light continuum pump-probe with picosecond pulses to avoid triplet excited state absorption. Without the latter contribution, the results obtained with both techniques show a transition to a high singlet excited state. The vibronic progression of the Q-band is observed due to photobleaching of the ground state. In addition, we show that the excited state presents reverse saturable absorption for most of the spectral range studied. A long relaxation component of the first singlet excited state was evidenced with the pump-probe experiment. This result is in agreement with fluorescence lifetime and fluorescence quantum yield measurements. In order to elucidate the origin of the nonlinear effects, we used a three-level energy diagram to describe the principal singlet-singlet transitions.     

Electromagnetically induced transparency in a cascade-type quantum well subband system under intense picosecond excitation

The coherent light–matter interaction in a 4-level cascade-type subband system of an asymmetric GaAs/AlGaAs quantum well structure is studied in pump-probe transmission experiments with picosecond (ps) time resolution. Coupling two excited subbands by an intense mid-infrared laser pulse at low sample temperatures is found to result in a substantially increased transparency of the fundamental e₁–e₂ transition. We find a reduction of the absorption coefficient by ~80%, which is one of the most pronounced electromagnetically induced transparency in solid state systems observed so far.     

Intra-acceptor hole relaxation in Be δ-doped GaAs/AlAs multiple quantum wells

This paper studies the dynamics of intra-acceptor hole relaxation in Be δ -doped GaAs/AlAs multiple quantum wells (MQW) with doping at the centre by time-resolved pump-probe spectroscopy using a picosecond free electron laser for infrared experiments. Low temperature far-infrared absorption measurements clearly show three principal absorption lines due to transitions of the Be acceptor from the ground state to the first three odd-parity excited states respectively. The pump-probe experiments are performed at different temperatures and different pump pulse wavelengths. The hole relaxation time from 2p excited state to 1s ground state in MQW is found to be much shorter than that in bulk GaAs, and shown to be independent of temperature but strongly dependent on wavelength. The zone-folded acoustic phonon emission and slower decay of the wavefunctions of impurity states are suggested to account for the reduction of the 2p excited state lifetime in MQW. The wavelength dependence of the 2p lifetime is attributed to the diffusion of the Be atom δ -layer in quantum wells.     

Investigation of the dependence of the coherent dynamics of a bismuth lattice on the crystal excitation level

Fully symmetric coherent phonons in bismuth have been investigated in a wide range of pumppulse energies by the pump-probe method using femtosecond laser pulses. It has been shown that in the linear regime, which is implemented only for low pump intensities, the coherent amplitude is proportional to the pump intensity, whereas the relaxation rate of the coherent state and its frequency remain unchanged. In the nonlinear regime, which can be divided into superlinear and sublinear regions, the relaxation rate of a photoinduced lattice state can be approximated by a two-component response, where only one component depends strongly on the pump intensity. The nature of the coherence of the phonon subsystem, which is created by an ultrashort laser pulse, is discussed on the basis of the analysis of the data.     

Ultrafast S1 and ICT state dynamics of a marine carotenoid probed by femtosecond one- and two-photon pump-probe spectroscopy

Ultrafast relaxation kinetics of fucoxanthin in polar and non-polar solvents have been studied by femtosecond pump-probe spectroscopy. Transient absorption associated with S₁ or intramolecular charge transfer (ICT) excited state has been observed following either one-photon excitation to the optically allowed S₂ state or two-photon excitation to the symmetry-forbidden S₁ state. The results suggest that the ICT state formed after excitation of fucoxanthin in a polar solvent is a distinct excited state from S₁.     

叠加激发对相干态的非经典特性

从激发对相干态出发,构造了叠加激发对相干态,研究了该叠加态的非经典特性.结果表明:在一定条件下,随着相位的变化,叠加态场模的平均光子数呈现类似于拉比振荡的坍塌与复原现象,与激发对相干态相比,在叠加激发对相干态中亚泊松光子统计特性和CauchySchwatz不等式的破坏都得到了增强,但正交相位分量的压缩减弱.     

Role of excited states in the splitting of a trapped interacting Bose-Einstein condensate by a time-dependent barrier

An essentially exact approach to compute the wave function in the time-dependent many-boson Schr?dinger equation is derived and employed to study accurately the process of splitting a trapped condensate. As the trap transforms from a single to double well the ground state changes from a coherent to a fragmented state. We follow the role played by many-body excited states during the splitting process. Among others, a "counterintuitive" regime is found in which the evolution of the condensate when the splitting is sufficiently slow is not to the fragmented ground state, but to a low-lying excited state which is a coherent state. Experimental implications are discussed.     

Stark spectroscopy of excited-state transitions in a conjugated polymer

Stark spectroscopy, which is well established for probing transitions between the ground and excited states of many material classes, is extended to transitions between transient excited states. To this end, it is combined with femtosecond pump-probe spectroscopy on a conjugated polymer with appropriately introduced traps which harvest excitation energy and build up a sufficient excited state population. The results indicate a significant difference in the effective dipole moments between two short lived excited states.     

[Au25(SR)18]-团簇的相干振动动力学研究

利用飞秒时间分辨光谱,可观测叠加在电子态动力学上的相干振动动力学. 从金团簇的相干振动中,不仅能提取电子与振动的耦合信息,也能得到力学性质和电子结构,进而有望实现微小质量探测等应用. 本文利用飞秒时间分辨的瞬态吸收探测了[Au₂₅(SR)₁₈]^-团簇的相干振动动力学,通过对相干振动的频率、相位、波长分布的详细分析进一步揭示了其来源. 在[Au₂₅(SR)₁₈]^-团簇的飞秒瞬态吸收动力学中可以观测到频率为40 cm^-1和80 cm^-1的两种振动,均来源于团簇中心Au₁₃核的振动. 通过对相干振动的相位分析发现频率为80 cm^-1的振动来自于对电子态之间吸收频率的调制,而频率为40 cm^-1的振动来源于对电子态之间吸收强度的调制. 同时,研究发现[Au₂₅(SR)₁₈]^-团簇相干振动的频率对其表面配体不敏感,该振动是来源于Au₁₃核的本征性质.     

三能级原子与奇偶纠缠相干光作用的光场压缩

采用求解薛定谔方程和数值计算方法,研究了V型三能级原子与双模奇偶纠缠相干光场相互作用过程中的光场压缩效应,讨论了压缩效应与双模奇偶纠缠相干光场的纠缠程度、系统失谐量、双模光场的平均光子数和原子基态概率幅的依赖关系。结果表明：光场压缩效应与双模奇偶纠缠相干光场的纠缠程度、失谐量、平均光子数和原子初态相关联：双模纠缠相干光场处于非纠缠状态时的光场压缩量比光场处于纠缠状态时要大;原子处在单纯的基态或激发态时光场都有明显的压缩现象出现;而原子初态中基态和激发态的概率幅较接近时无光场压缩现象;无论光场是否处于纠缠态,只有两模平均光子数接近时,光场才会出现压缩效应。     

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.     

Photon Excitations Excitated the Sqeezing Properties of the Excited Entangled Coherent States

In our previous paper, we have introduced a new kind of continuous-variable-type entangled states, called double-mode excited entangled coherent states. In this paper, we study sum squeezing properties of such excited entangled coherent states. We focus on discussing the influence of photon excitations on sum squeezing properties. It is found that the photon excitations seriously affected sqeezing properties of the excited entangled coherent states. With increasing the number of the photon excitations m, the higher-order terms move away from its initial state |ψ ₀〉 and the degrees of sum squeezing are increasing. In this sense, it implies that the photon excitations excitated the sum sqeezing properties of the double-mode excited entangled coherent states.     

Picosecond ground state recovery of the F-center in RbCl,KCl and KBr

Abstract

Optical pump-probe measurements on the F-center in RbCl, KCl and KBr show a ps ground state recovery, when a substantial number of F-aggregates is present. The observed de-excitation process becomes faster for a larger concentration of aggregate centers and is related to energy transfer from the excited state of the F-center to aggregate centers. This energy transfer occurs towards F₂- and N-centers in KCl. Our results are in accordance with measurements of the quantum efficiency of the F-center luminescence and with transient absorption measurements.     

Coherent control of the lattice dynamics of bismuth near the lindemann stability limit

The relative contributions of the anharmonicity of the lattice potential and the nonequilibrium concentration of charge carriers to the time dependence of the coherent A _1g phonon frequency in bismuth excited by high-energy ultrashort laser pulses are studied by the coherent control method. The contributions are separated by the pump-probe method in which excitation is performed by two pulses with a controlled time delay. It is shown that, depending on the relative delay between the pump pulses, both correlation and anticorrelation between the amplitude and the initial frequency of oscillations are observed while the chirp and the initial frequency of the coherent phonon are anticorrelated. In addition, it has been found that the contributions of the lattice and the electronic subsystem are always anticorrelated. Therefore, a certain phase can be assigned to an electronic excitation and it may be suggested that the time dependence of the phonon frequency is determined not only by instantaneous values of the lattice and electronic response but also by the phase relations between them.     

Nonlinear absorption of CS2 at the wavelength of 400 nm with femtosecond pulses

Nonlinear absorption of carbon disulfide (CS₂) was investigated by Z-scan technique and time-resolved pump-probe technique with femtosecond pulses at 400 nm wavelength. By the two techniques, we confirmed that the nonlinear absorption of CS₂ arise from a combination of two-photon absorption (TPA) and the excited state absorption induced by TPA under the incident laser pulses with 400 nm wavelength. The coefficient of TPA, the absorption cross-section of low excited state and lifetime of low excited state were obtained by theoretical fitting the experimental results. The results indicated that the CS₂ has good optical limiting capability at 400 nm wavelength.     

Two-photon revival-collapse phenomenon in the evolution of the quadrature squeezing of the four-photon Jaynes-Cummings model

We prove that the revival-collapse phenomenon occurring in the atomic inversion of the two-photon Jaynes-Cummings model, when the mode is initially prepared in the coherent state and the atom is in the excited state, can be obtained from the evolution of the quadrature squeezing of the four-photon Jaynes-Cummings model.     

Coherent transients in the femtosecond photoassociation of ultracold molecules

We demonstrate the photoassociation of ultracold rubidium dimers using coherent femtosecond pulses. Starting from a cloud of ultracold rubidium atoms, electronically excited rubidium molecules are formed with shaped photoassociation pump pulses. The excited state molecules are projected with a time-delayed probe pulse onto molecular ion states which are detected in a mass spectrometer. Coherent transient oscillations of the excited state population are observed in the wings of the pump pulse, in agreement with the time-dependent solution of the Schr?dinger equation of the excitation process.     

Strengthened Hyper-Raman Lines with the Coherent Superposition State

High-order harmonic generations from a one-dimensional Coulomb potential atom are calculated with the initial state prepared as a coherent superposition between its ground and first excited states. When the energy difference of the two states is small, we can choose proper laser pulse such that the first excited state can be excited only to other bound states instead of being ionized. We show that only the hyper-Raman lines are observable instead of the harmonics. The energy difference of the ground and the first excited state can be deduced from the highest peak of the hyper-Raman lines. We further show that the similar results can be obtained by using a combination of two laser pulses with different frequencies interacting with the atom initially at the ground state.