Motional-narrowing-type dephasing of electron and hole spins of itinerant excitons in magnetically doped II-VI bulk semiconductors

Time-resolved optical spin-quantum-beat measurements performed on magnetically doped II-VI bulk semiconductors reveal an increase of the electron spin dephasing time with rising temperature typical for motional narrowing. With the dephasing being notably faster than in undoped II-VI semiconductors, the magnetic dopants must play a key role, modifying the known dephasing mechanisms and introducing new ones. Focusing on the latter, we theoretically explore the spin dephasing channel arising from magnetization fluctuations sampled by the itinerant excitons. This mechanism suffices to explain quantitatively the results of our time-resolved Faraday-rotation experiments on optically excited Cd(1-x)Mn(x)Te which we present here as a function of magnetic field, temperature and manganese dopant density. In addition to electron spin-quantum beats, some of our experiments reveal hole spin beats as well.     

Optical investigation of bloch oscillations in semiconductor superlattices

We investigate the dephasing dynamics in semiconductor superlattices using time-resolved four-wave mixing. The signals show a periodic modulation which can be related to Bloch oscillations in the superlattice miniband. The oscillation frequency is strongly dependent on the applied field, in agreement with theoretical expectation. At high fields, the dephasing times become very short due to field-induced scattering.     

Coherent spin dynamics of different density high mobility two-dimensional electron gas in a GaAs quantum well

We have addressed the dependence of quasi-two-dimensional electron spin dephasing time on the electron gas density in a 17-nm GaAs quantum well using the time-resolved magneto-optical Kerr effect. A superlinear increase in the electron dephasing time with decreasing electron density has been found. The degree of electron spin relaxation anisotropy has been measured and the dependence of spin-orbit splitting on electron gas density has been determined.     

Identification of single fluorescently labelled mononucleotide molecules in solution by spectrally resolved time-correlated single-photon counting

We describe a method to identify single dye-labelled mononucleotide molecules in solution with high classification probability based on confocal microscopy in combination with spectrally and time-resolved fluorescence detection with two detectors. For efficient excitation of the labelled mononucleotide molecules JA133-dUTP, JA169-dUTP, Cy5-dCTP, and JA242-dUTP a short-pulse diode laser emitting at 634 nm with a repetition rate of 64 MHz was applied. The time-resolved fluorescence signals of individual molecules were analyzed and identified by a maximum likelihood estimator (MLE). Scatter plots of spectrally and time-resolved fluorescence data demonstrated the existence of four distinct populations with symmetrical shape. The distributions of each of the mononucleotide conjugates were determined by fitting a superposition of two independent Gaussians. Taking only those single-molecule bursts which contain more than 50 photon counts, three labelled mononucleotide molecules were identified in solution by spectrally and time-resolved fluorescence spectroscopy with a probability of correct classification of ≈99%. Received: 31 March 2000 / Revised version: 31 May 2000 / Published online: 13 September 2000     

Connections of Coherent Information,Quantum Discord,and Entanglement

For a pure non-markovian dephasing model we derive analytic expressions of coherent information,quantum discord,and entanglement.We find that for the cases of the initial Werner states,the dynamical behavior of coherent information is similar to that of quantum discord but different from that of entanglement.Coherent information,as well as quantum discord,can reveal the quantum correlations in some mixed-states,in which the entanglement is zero.     

Detection of spectrally narrow light emission by laser intra-cavity spectroscopy

The spectral distribution of the output of a multimode laser is extremely sensitive to narrow-band absorption, gain, or light injection. We demonstrate dramatic redistribution in such output spectra to depend on the time delay of the injection. This effect seems to be useful for spectrally resolved detection of weak light signals.     

Combined soot optical characterization using 2-D multi-angle light scattering and spectrally resolved line-of-sight attenuation and its implication on soot color-ratio pyrometry

Soot characterization using multiple techniques has been performed in a series of nitrogen-diluted ethylene coflow laminar diffusion flames. Soot aggregate sizes have been measured in two dimensions, as opposed to traditional point measurements, by a newly developed two-dimensional multi-angle light scattering technique where image processing was applied to align images for Guinier analysis. Extinction measurements have also been performed using spectrally resolved line-of-sight attenuation with an imaging spectrometer. Spectrally and spatially resolved extinction measurements have been obtained as well. Combined with previously obtained time-resolved laser-induced incandescence measurements of primary particle diameters, the scattering and absorption components of extinction can be estimated. The so-called dispersion exponent that describes the wavelength dependence of spectral emissivity was determined in two dimensions and found to improve the accuracy of soot color-ratio pyrometry measurements.     

Femtosecond spectrotemporal magneto-optics

A new method to measure and analyze the time and spectrally resolved polarimetric response of magnetic materials is presented. It allows us to study the ultrafast magnetization dynamics of a CoPt3 ferromagnetic film. The analysis of the pump-induced rotation and ellipticity detected by a broad spectrum probe beam shows that magneto-optical signals predominantly reflect the spin dynamics in ferromagnets.     

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.     

Ultrafast nonlinear optical response and high density excitation effects of the stacking fault exciton in BiI3

On the exciton states localized at a two-dimensional stacking fault interface in a layered crystal BiI₃, some nonlinear optical phenomena clearly appear reflecting large transition probability. The optical Stark shift and other high density exciton effect on the energy-shift and the spectral broadening are observed with clear separation under intense laser pumping by time-resolved measurements. The optical Stark shift is analyzed based on the dressed exciton model. The ultrafast optical response faster than 3 ps for the pump-laser field is confirmed on the Stark shift. Degenerate four-wave-mixing signals show fairly long dephasing time of 40 ps in this system. The dephasing probability depends linearly on the pump-laser intensity in the same manner as that of the spectral line-broadening reflecting the relaxation process. The dephasing mechanisms are understood by the exciton scattering at high density in parallel with the spectral changes. The blue-shift due to the high density excitons are discussed on the basis of exciton-exciton interaction in connection with a phase-space filling theory in two-dimensional systems.     

Simultaneous measurements of global vibrational spectra and dephasing times of molecular vibrational modes by broadband time-resolved coherent anti-Stokes Raman scattering spectrography

In broadband coherent anti-Stokes Raman scattering (CARS) spectroscopy with supercontinuum (SC), the simultaneously detectable spectral coverage is limited by the spectral continuity and the simultaneity of various spectral components of SC in an enough bandwidth. By numerical simulations, the optimal experimental conditions for improving the SC are obtained. The broadband time-resolved CARS spectrography based on the SC with required temporal and spectral distributions is realised. The global molecular vibrational spectrum with well suppressed nonresonant background noise can be obtained in a single measurement. At the same time, the measurements of dephasing times of various molecular vibrational modes can be conveniently achieved from intensities of a sequence of time-resolved CARS signals. It will be more helpful to provide a complete picture of molecular vibrations, and to exhibit a potential to understand not only both the solvent dynamics and the solute-solvent interactions, but also the mechanisms of chemical reactions in the fields of biology, chemistry and material science.     

分子环境变化对振动退相时间影响的实验研究

物质分子振动退相时间测量是一种非标记无损分子检测方法, 用超连续谱时间分辨相干反斯托克斯拉曼散射方法可同时获得分子振动谱和退相时间. 实验以苯甲腈和甲醇为样品, 研究当分子环境变化时, 其主要振动谱的振动退相时间变化情况. 将苯甲腈与无水乙醇混合, 测量了苯甲腈分子1017, 2247和3085 cm^-1三个典型分子振动的退相时间随环境变化的规律, 并得到了变化后的振动退相时间. 测量了甲醇分子2851, 2960 cm^-1两个相邻分子振动的退相时间随环境的变化情况, 给出实验变化规律. 这种方法具有检测分子所处环境变化和分子相互作用的能力, 在生命科学、分子生物学和材料科学等研究领域中具有重要的应用前景.     

New results on ultrafast coherent excitation of molecular vibrations in liquids

Coherent Raman probe scattering experiments are performed to study dynamical processes of polyatomic liquids at 300 K. For single homogeneous transitions the dephasing timeT ₂ is readily obtained from time resolved investigations. Spectral studies show an interesting time dependent shift in scattered frequency. After the excitaiton the vibrating molecules are shown to relax freely with their resonance frequency. Multiple, equally spaced transitions exhibit a beating phenomenon which provides the dephasing time and the frequency interval between neighboring vibrational states. Inhomogeneously broadened systems do not allow a ready determination of the dephasing time by the present probing technique. Previous experiments on the subject have to be reconsidered.     

Phase coherence and line broadening of free excitons in GaAs quantum wells

The optical dephasing of 2D excitons in GaAs single quantum wells is studied by means of time-resolved Degenerate Four-Wave Mixing and transmission spectroscopy. The measured phase coherence time directly corresponds to the absorption line-width confirming the homogeneous nature of the line broadening. The observed linear temperature dependence of the homogeneous linewidth below 80K reveals acoustic-phonon scattering as the dominant optical dephasing process.     

Direct time-domain observation of ultrafast dephasing in adsorbate-substrate vibration under the influence of a hot electron bath: Cs adatoms on Pt(111)

The stretching vibration of Cs adsorbed on Pt(111) is excited coherently by resonant stimulated Raman excitation and its time evolution is probed by fs time-resolved second harmonic generation as a function of pump laser fluence I. As I increases, a fast dephasing component with the lifetime of tau=0.7 ps grows, being superimposed on a slow one with tau=1.9 ps. The fast component is a manifestation of pure dephasing caused by elastic and inelastic scattering of hot electrons at adsorbate.     

Non-radiative exciton recombination through excitation energy transfer in quantum dot clusters

Excitation energy transfer (EET) processes in CdSe/CdZnS quantum dot (QD) clusters have been investigated in this study by measuring their time-resolved and spectrally resolved fluorescence intensities. The contributions of radiative and non-radiative exciton recombination through EET are evaluated, where the latter is expected to occur in a large class of QD ensembles because of the presence of nonluminescent QDs. It appears that the fluorescence decay in larger QDs serving as acceptor does not show an initial rise, in addition the lifetime of the acceptor QD is independent of the excitation wavelength, suggesting that an EET is followed mostly by non-radiative recombination.     

分子多振动模式的振动退相时间同时测量方法

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...     

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.     

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.     

Optical phonon dynamics of GaAs studied with time-resolved terahertz spectroscopy

We investigate the reflection near the reststrahlen band of the optical phonon in bulk GaAs in the time domain, using time-resolved terahertz spectroscopy. We find that the dynamics of the reflection measured for GaAs differs strongly from the reflection dynamics that would be expected for a TO phonon with a frequency-independent dephasing time.