Coherent Exciton-Phonon Coupling in CdSe/ZnS Nanocrystals Studied by Two-Dimensional Electronic Spectroscopy

Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy (2DES) measurements. Benefiting from the ability of 2DES to dissect assembles in nanocrystal films, we have clearly identified experimental evidences of coherent coupling between exciton and phonon in CdSe/ZnS nanocrystals. In time domain, 2DES signals of excitonic transitions beat at a frequency resonant to a longitudinal optical phonon mode; in energy domain, phonon side bands are distinct at both Stokes and anti-Stokes sides. When temperature increases, phonon-induced exciton dephasing is observed with dramatic broadening of homogeneous linewidth. The results suggest exciton-phonon coupling is essential in elucidating the quantum dynamics of excitonic transitions in semiconductor nanocrystals.     

Correlations between quantum and stochastic systems with a dephasing coupling

Correlations between single qubit and classical environment are studied by means of the stochastic Liouville equation, where a dephasing coupling between them is assumed. When the dephasing of the qubit is characterized by the two-state-jump Markov process, the properties of the total, classical and quantum correlations are examined.     

溶液和熔化状态下分子间的能量传递

通过二维红外光谱研究了GdmSCN/KSCN=1/1,GdmSCN/KS¹³CN=1/1和GdmSCN/KS¹³C¹⁵N=1/1三种混合晶体在熔融和溶液状态下的共振和非共振的分子间振动能量传递的性质. 在这些样品中,给体/受体的能量差越大,能量传递越慢. 而能量传递的快慢与拉曼光谱无关. 非共振能量传递与给体/受体的能量差的关系不能用声子补偿的机理来描述. 相反,它们的关系却可以用退相位机理来定量描述. 在熔融状态下,共振和非共振能量速率与温度的依赖关系也与退相位机理的预测相符合. 这一系列的结果表明只要分子的运动(平动和转动)远远快于非共振能量传递速率,那么退相位机理不仅在溶液中占主导,而且在熔融状态下(纯液体,不含溶剂)也占主导.     

Intermolecular Vibrational Energy Transfers in Melts and Solutions

Resonant and nonresonant intermolecular vibrational energy transfers in Gdm-SCN/KSCN=1/1, GdmSCN/KS¹³CN=1/1 and GdmSCN/KS1¹³C¹⁵N=1/1 mixed crystals in melts and in aqueous solutions are studied with the two dimensional infrared spectroscopy. The energy transfers in the samples are slower with a larger energy donor/acceptor gap, independent of the Raman spectra. The energy gap dependences of the nonresonant energy transfers cannot be described by the phonon compensation mechanism. Instead, the experimental energy gap dependences can be quantitatively described by the dephasing mechanism. Temperature dependences of resonant and nonresonant energy transfer rates in the melts are also consistent with the prediction of the dephasing mechanism. The series of results suggest that the dephasing mechanism can be dominant not only in solutions, but also in melts (pure liquids without solvents), only if the molecular motions (translations and rotations) are much faster than the nonresonant energy transfer processes.     

《光谱学与光谱分析》2007年征订启事

The authors achieved the temporal coherent control in an Er^3＋ doped telluride glass, one kind of disordered solids. The upconversion at 670 nm was modulated and the dephasing time was simulated as 300 fs. Moreover, the photon echo signal gave the dephasing time due to the phonon interaction. The agreement between the two data indicates that the interaction between the wavepacket and the phonon leads to the fast disappearance of wavepackets interference, which is helpful for the tech- nique to be applied to the disordered solids.     

On the effects of dephasing due to local gradients in diffusion tensor imaging experiments: relevance for diffusion tensor imaging fiber phantoms

The effect of susceptibility differences between fluid and fibers on the properties of DTI fiber phantoms was investigated. Thereto, machine-made, easily producible and inexpensive DTI fiber phantoms were constructed by winding polyamide fibers of 15 microm diameter around a circular acrylic glass spindle. The achieved fractional anisotropy was 0.78+/-0.02. It is shown by phantom measurements and Monte Carlo simulations that the transversal relaxation time T(2) strongly depends on the angle between the fibers and the B(0) field if the susceptibilities of the fibers and fluid are not identical. In the phantoms, the measured T(2) time at 3 T decreased by 60% for fibers running perpendicular to B(0). Monte Carlo simulations confirmed this result and revealed that the exact relaxation time depends strongly on the exact packing of the fibers. In the phantoms, the measured diffusion was independent of fiber orientation. Monte Carlo simulations revealed that the measured diffusion strongly depends on the exact fiber packing and that field strength and -orientation dependencies of measured diffusion may be minimal for hexagonal packing while the diffusion can be underestimated by more than 50% for cubic packing at 3 T. To overcome these effects, the susceptibilities of fibers and fluid were matched using an aqueous sodium chloride solution (83 g NaCl per kilogram of water). This enables an orientation independent and reliable use of DTI phantoms for evaluation purposes.     

On the relationship betweenT 1 andT 2 for stochastic relaxation models

We consider the relaxation dynamics of two quantum levels coupled to a stochastic bath. We emphasize that even if the matrix elements of the fluctuating Hamiltonian are Gaussian, a second-order cumulant truncation is not exact. For various stochastic models, including the case of a spin-1/2 particle in a fluctuating magnetic field, we calculate 1/T ₁, the population relaxation rate, and 1/T ₂, the phase relaxation rate, up to fourth order in perturbation theory. We show that unlike the commonly accepted second-order result that 1/T ₂1/2T ₁, when fourth-order terms are included, in some instances 1/T ₂<1/2T ₁.     

Acoustic phonon dephasing in shallow GaAs/Ga Al As single quantum wells

The intermediate dimensionality regime is studied on a set of shallow GaAs/Ga Al As single quantum wells. Such heterostructures exhibit 2D strong excitonic electroabsorption together with near 3D fast transport properties. We report dephasing time measurements of the heavy-hole exciton and we show that the acoustic phonon contribution decreases with to a value in good agreement with theoretical predictions for GaAs bulk.     

Dynamical suppression of dephasing for Markov processes

It is shown that the dephasing of a qubit caused by a Markov process can be suppressed by a successive application of π-pulses if two-time conditional probability of the stochastic variable depends only on the time-difference. The several types of the π-pulse sequence are compared in the case of the two-state jump Markov process.     

Coherent dynamics in InGaAs quantum dots and quantum dot molecules

We measure the dephasing time of the exciton ground state transition in InGaAs quantum dots (QD) and quantum dot molecules (QDM) using a sensitive four-wave mixing technique. In the QDs we find experimental evidence that the dephasing time is given only by the radiative lifetime at low temperatures. We demonstrate the tunability of the radiatively limited dephasing time from 400 ps up to 2 ns in a series of annealed QDs with increasing energy separation of 69–330 meV from the wetting layer continuum. Furthermore, the distribution of the fine-structure splitting δ₁ and of the biexciton binding energy δ_B is measured. δ₁ decreases from 96 to with increasing annealing temperature, indicating an improving circular symmetry of the in-plane confinement potential. The biexciton binding energy shows only a weak dependence on the confinement energy, which we attribute to a compensation between decreasing confinement and decreasing separation of electron and hole. In the QDM we measured the exciton dephasing as function of interdot barrier thickness in the temperature range from 5 to 60 K. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed, showing how the quantum mechanical coupling in the molecules affects the exciton lifetime and acoustic-phonon interaction.