Femtosecond Dynamics of Energy Transfer in Native B800-B850 and B800-Released LH2 Complexes of Rhodobacter Sphaeroides

Two kinds of antenna complexes LH2 of Rhodobacter sphaeroides, wild type RS601 and the removal of B800pigments (B800-released), were used in our experiment. These two LH2 complexes show quite different behaviour in absorption and femtosecond dynamics. By using the femtosecond pump-probe technique, the energy transfer processes occurring in two complexes were studied. Because of removing the B800 pigment from the LH2 in B800-released LH2 complex, the energy transfer between the B800 to B850 pigment was completely eliminated, while the pure internal energy transfer within the exciton states of B850 pigment could be carefully investigated. The results show that, at B800 absorption band, B800-released LH2 obviously shows a dominated transient absorption different from the photobleaching observed in RS601; while at the B850 band, these two complexes show similar photobleaching behaviour.     

Photoluminescence of ZnSe—ZnS Single Quantum Wells Grown by Vapour Phase Epitaxy

We study the photoluminescence (PL) of ultra thin layer ZnSe quantum Wells in ZnS barriers.Samples with different well widths are grown by vapour phase epitaxy and the PL spectra of these samples are measured by the excitation of a 500W Hg lamp.The peak positions of the bands coming from the excitonic luminescence show a larger blueschift with respect to the energy of free excitons in the ZnSe bulk material.The observed variation of the full width at half maximum and peak position of the bands in the spectra with the well width are interpreted to the formation of the ZnSxSe1-x alloy layer due to the interdiffusion in the interfaces between ZnSe and ZnS.According to the behaviour of the excitons in the smaller conduction band offset,the exciton binding energy is estimated from the dependence of the PL intensity on the temperature.from this result,excitons seem to show nearly three-dimensional characteristics.     

Lasing behaviour from the condensation of polaronic excitons in a ZnO nanowire

Atoms under optical and magnetic trapping in a limited space at a very low temperature can lead to Bose-Einstein condensation (BEC),even in a one-dimensional (1D) optical lattice. However,can the confinment of dense excitons in a 1D semiconductor microstructure easily reach the excitonic BEC A lightly Mn(Ⅱ)-doped ZnO nanowire under a femtosecond laser pulse pump at room temperature produces single-mode lasing from coherent bipolaronic excitons,which is much like a macroscopic quantum state due to the condensation of the bipoaronic excitons if not real BEC. In this process,longitudinal biphonon binding with the exciton plays an important role. We revisit this system and propose possibility of bipolaronic exciton condensation. More studies are needed for this condensation phenomenon in 1D microcavity systems.     

Theoretical study on the exciton dynamics of coherent excitation energy transfer in the phycoerythrin 545 light-harvesting complex

The experimental observation of long-lived quantum coherence in the excitation energy transfer(EET)process of the several photosynthetic light-harvesting complexes at low and room temperatures has aroused hot debate.It challenges the common perception in the field of complicated pigment molecular systems and evokes considerable theoretical efforts to seek reasonable explanations.In this work,we investigate the coherent exciton dynamics of the phycoerythrin 545(PE545)complex.We use the dissipation equation of motion to theoretically investigate the effect of the local pigment vibrations on the population transfer process.The result indicates that the realistic local pigment vibrations do assist the energy transmission.We demonstrate the coherence between different pigment molecules in the PE545 system is an essential ingredient in the EET process among various sites.The coherence makes the excitation energy delocalized,which leads to the redistribution of the excitation among all the chromophores in the steady state.Furthermore,we investigate the effects of the complex high-frequency spectral density function on the exciton dynamics and find that the high-frequency Brownian oscillator model contributes most to the exciton dynamic process.The discussions on the local pigment vibrations of the Brownian oscillator model suggest that the local heterogeneous protein environments and the effects of active vibration modes play a significant role in coherent energy transport.     

Pulsar giant pulse: Coherent instability near light cylinder

Giant pulses(GPs) are extremely bright individual pulses of radio pulsar. In microbursts of Crab pulsar, which is an active GP emitter, zebra-pattern-like spectral structures are observed, which are reminiscent of the "zebra bands" that are observed in type Ⅳ solar radio flares. However, band spacing linearly increases with the band center frequency of ～5-30 GHz. In this study, we propose that the Crab pulsar GP can originate from the coherent instability of plasma near a light cylinder. Further, the growth of coherent instability can be attributed to the resonance observed between the cyclotron-resonant-excited wave and the background plasma oscillation. The particles can be injected into the closed-field line regions owing to magnetic reconnection near a light cylinder. These particles introduce a large amount of free energy that further causes cyclotron-resonant instability, which grows and amplifies radiative waves at frequencies close to the electron cyclotron harmonics that exhibit zebra-pattern-like spectral band structures. Further, these structures can be modulated by the resonance between the cyclotron-resonant-excited wave and the background plasma oscillation. In this scenario, the band structures of the Crab pulsar can be well fitted by a coherent instability model, where the plasma density of a light cylinder should be ～10~(13-15) cm~(-3), with an estimated gradient of 5.5 × 10~5 cm~(-4). This process may be accompanied by high-energy emissions. Similar phenomena are expected to be detected in other types of GP sources that have magnetic fields of ? 106 G in a light cylinder.     

Origin and Characteristics of Blue Light Emission in Solid State Cathodoluminescence of MEH－PPV

Based on our previous study [Chin. Phys. Lett. 20 (2003) 1144] on the sofid-state cathodoluminescence from organic luminescent materials, here we study the origin and characteristics of blue light emission in solid-state cathodoluminescence of Poly [(2-methoxy-5-(2‘-ethyl-hexyloxy)phenylene vinyene] (MEH-PPV) and the dependence of each spectral peak on electric field strength. The results demonstrate that the blue spectral shift benefits from field ionization of excitons, and three regions of electric field are found, in which there are pure exciton emission, coexistence of exciton emission and radiative recombination, and pure radiative recombination.     

Radiative life time of an exciton confined in a strained GaN/Ga1-xAlxN cylindrical dot: built-in electric field effects

The binding energy of an exciton in a wurtzite GaN/GaAlN strained cylindrical quantum dot is investigated theoretically.The strong built-in electric field due to the spontaneous and piezoelectric polarizations of a GaN/GaAlN quantum dot is included.Numerical calculations are performed using a variational procedure within the single band effective mass approximation.Valence-band anisotropy is included in our theoretical model by using different hole masses in different spatial directions.The exciton oscillator strength and the exciton lifetime for radiative recombination each as a function of dot radius have been computed.The result elucidates that the strong built-in electric field influences the oscillator strength and the recombination life time of the exciton.It is observed that the ground state exciton binding energy and the interband emission energy increase when the cylindrical quantum dot height or radius is decreased,and that the exciton binding energy,the oscillator strength and the radiative lifetime each as a function of structural parameters (height and radius) sensitively depend on the strong built-in electric field.The obtained results are useful for the design of some opto-photoelectronic devices.     

Spontaneous emission from an atom in a photonic crystal with two coherent bands

The dynamic and the radiative properties of an excited three-level atom embedded in an anisotropic photonic crystal with two coherent bands are investigated.The relative position of the atom in a Wigner-Seitz cell is described with a position-dependent parameter θ(r0),which is used as the coherent parameter for the two bands.The result shows that the dynamic properties of the atomic system are not only determined by atomic transition frequencies,but also affected by the gap width and the coherence of the two bands.In addition,the spontaneous emission spectrum of the atomic transition in free space is discussed.The center and the intensity of the spectrum can be obviously manipulated via the coherent parameter.     

Modifying optical properties of ZnO nanowires via strain-gradient

We conduct systematical cathodolumiuescence study on red-shift of near-band-edge emission energy in elastic bent ZnO nanowires with diameters within the exciton diffusion length （- 200 nm） in liquid nitrogen temperature （81 K）. By charactering the emission spectra of the nanowires with different; local curvatures, we find a linear relationship between strain-gradient and the red-shift of near-band-edge emission photon energy, an elastic strain-gradient effect in semiconductor similar to the famous flexoelectric effect in liquid crystals. Our results provide a new route to understand the inhomogeneous strain effect on the energy bands and optical properties of semiconductors and should be useful for designing advanced nano-optoelectronic devices.     

Simultaneous low extinction and high local field enhancement in Ag nanocubes

We theoretically investigate surface plasmon resonance properties in Au and Ag cubic nanoparticles and find a novel plasmonic mode that exhibits simultaneous low extinction and high local field enhancement properties. We analyse this mode from different aspects by looking at the distribution patterns of local field intensity, energy flux, absorption and charge density. We find that in the mode the polarized charge is highly densified in a very limited volume around the corner of the nanocube and results in very strong local field enhancement. Perturbations of the incident energy flux and light absorption are also strongly localized in this small volume of the corner region, leading to both low absorption and low scattering cross section. As a result, the extinction is low for the mode. Metal nanoparticles involving such peculiar modes may be useful for constructing nonlinear compound materials with low linear absorption and high nonlinearity.     

Picosecond excitonic luminescence in ZnO and other wide-gap semiconductors

Radiative lifetimes of free-atom transitions, scaled by ω³ for comparison at 368 nm, are not faster than about 6.9 ns. BaF₂ core-valence luminescence, scaled in the same way from 220 to 368 nm, corresponds to 4.1 ns. In contrast, excitonic transitions in wide-gap semiconductors display subnanosecond radiative lifetimes, and in particular ZnO has radiative lifetimes measured at 50–300 ps for D^o,X and 400–900 ps for free excitons. The “giant oscillator strength” corresponding to these lifetimes can be explained by theories developed initially for defect-bound excitons, then quantum wells, and nanoparticles. An exciton is a coherent array of N dipoles, where N is the number of sites covered by coherent translational motion of the exciton. This is not essentially a phenomenon of multiple excitons, but applies as well to single-exciton decay. It differs in that regard from the more familiar Dicke giant dipole of N coherently excited atoms lacking translational periodicity. The phenomenon suggests possibilities for achieving ultrafast scintillators and high light yield.     

Ⅲ-Ⅴ族化合物中氮束缚激子发光的动力学研究

用发光动力学的分析方法,研究了Ⅲ—Ⅴ族化合物中N束缚激子的发光强度与温度的关系,得到的理论公式与实验结果符合得较好。我们的分析指出,由于无辐射能量传递的存在,束缚激子的△J=2跃迁的发光效率低于△J=1跃迁的发光效率,致使低温(T<50K)下束缚激子的发光强度可能随温度的下降而变弱。另外,N杂质对自由激子再俘获的可能性的大小直接影响束缚激子发光的热猝灭过程:束缚激子可能因热离解成自由激子或自由的电子和空穴。我们找到了区分这两类情况的条件。     

Exciton absorption of light in a smooth random field

A study is made of interband absorption of light in a smooth random field that varies slowly in space. When the exciton energy in the random field is much less than the exciton binding energy, the influence of the random field on the discrete spectrum of the exciton is expressed through the appearance of an exponential “tail” to every exciton line. But if the exciton energy in the random field is much greater than the exciton binding energy, the exciton effects are unimportant because the random field breaks up the excitons.     

The anisotropy of fluorescence in ring units III: Tangential versus radial dipole arrangement

The time dependence of the anisotropy of fluorescence can indicate the coherent exciton transfer regime in molecular rings. We are comparing time development of this quantity after an impulsive excitation obtained for the ring models of bacterial antenna complexes with tangential and radial optical transition dipole moments arrangement as in nonameric LH2 and octameric LH4 units. We use non-correlated static Gaussian disorder in the local exciton energies. We take into account simultaneously dynamic disorder using a Markovian treatment of the interaction with the bath. We show that the influence of dynamic disorder on difference of the anisotropy of fluorescence is more important then the influence of static disorder in consequence of different band width.     

Theory and ab initio calculation of radiative lifetime of excitons in semiconducting carbon nanotubes

We present a theoretical analysis and first-principles calculation of the radiative lifetime of excitons in semiconducting carbon nanotubes. An intrinsic lifetime of the order of 10 ps is computed for the lowest optically active bright excitons. The intrinsic lifetime is, however, a rapid increasing function of the exciton momentum. Moreover, the electronic structure of the nanotubes dictates the existence of dark excitons near in energy to each bright exciton. Both effects strongly influence measured lifetime. Assuming a thermal occupation of bright and dark exciton bands, we find an effective lifetime of the order of 10 ns at room temperature, in good accord with recent experiments.     

Photon Echo from Localized Excitons in Semiconductor Nanostructures

An overview on photon echo spectroscopy under resonant excitation of the exciton complexes in semiconductor nanostructures is presented. The use of four-wave-mixing technique with the pulsed excitation and heterodyne detection allowed us to measure the coherent response of the system with the picosecond time resolution. It is shown that, for resonant selective pulsed excitation of the localized exciton complexes, the coherent signal is represented by the photon echoes due to the inhomogeneous broadening of the optical transitions. In case of resonant excitation of the trions or donor-bound excitons, the Zeeman splitting of the resident electron ground state levels under the applied transverse magnetic field results in quantum beats of photon echo amplitude at the Larmor precession frequency. Application of magnetic field makes it possible to transfer coherently the optical excitation into the spin ensemble of the resident electrons and to observe a long-lived photon echo signal. The described technique can be used as a high-resolution spectroscopy of the energy splittings in the ground state of the system. Next, we consider the Rabi oscillations and their damping under excitation with intensive optical pulses for the excitons complexes with a different degree of localization. It is shown that damping of the echo signal with increase of the excitation pulse intensity is strongly manifested for excitons, while on trions and donor-bound excitons this effect is substantially weaker.     

镓铟磷三元化合物中的自由激子和杂质N发光中心的结构位形

我们研究了GaxIn1-xP:N(x=0.99,0.98,0.96)的发光光谱,用Ar+离子激光器的458nm线激发。N的浓度为5×1017cm-3。图1示出了在6K下Ga0.99In0.01P:N的发光光谱。Mariette和Chevallier[1,2]以及Nelson和Holonyak,Jr[3]。认为Nx0带起源于束缚在孤立N中心上激子的辐射复合。     

Linear and nonlinear optical properties of excitons in semiconductor quantum wells and microcavities

Linear and nonlinear light propagation in single and multiple quantum wells and in semiconductor microresonators are studied on the basis of Maxwell’s equations. The treatment includes radiative broadening of quantum-confined excitons, radiative coupling between quantum wells as well as coupling of quantum wells to the cavity field of a microresonator for steady state or ultrashort pulse excitation. The dynamical evolution of the coherent quantum-well polarization under the influence of many-body effects is studied within a microscopic model. The theory is used to investigate the influence of exciton saturation and dephasing on pulse propagation and excitonic normal-mode coupling.     

Polariton-mode lasing and Bose condensate of dipolar excitons in heterostructures

The analysis of the polariton modes in 2D traps based on heterostructures with quantum wells for Bose-Einstein condensation of dipolar excitons is presented. The characteristic equation of such modes is derived with allowance for the polarization relaxation of excitons and radiative losses from the trap. The spectrum and structure of high-quality modes are analytically and numerically studied. It is demonstrated that several modes become unstable at a high enough density of excitons and a long relaxation time of the exciton polarization. In accordance with the estimations, such an instability can be reached in the experiments on the Bose-Einstein condensation of dipolar excitons and can be used to interpret the corresponding coherent emission.     

多组分纠缠在光子晶体中的存储

研究了激子的多组分纠缠相干态保真度在各向异性光子晶体中的演化行为.结果表明,当激子的跃迁频率处于光子晶体带隙时,保真度随时间变化作周期振荡,这与激子处于真空环境时,保真度振荡衰减的演化行为不同.此外,当激子跃迁频率离光子晶体带边较远时,其多组分纠缠相干态越容易被保存.