Exciton and biexciton fine structure in single elongated islands grown on a vicinal surface

We report a microphotoluminescence study of the exciton and the biexciton localized in very elongated islands formed by well-width fluctuations in a thin CdTe/CdMgTe quantum well grown on a vicinal surface. The electron-hole exchange interaction in a local reduced symmetry splits the exciton states. The resulting transitions are linearly polarized along the two orthogonal principal axes of the island. The valence band mixing induced by the elongated shape of the potential leads to a strong polarization anisotropy and to the observation of dark exciton states under magnetic field. The biexciton-exciton transition reproduces all the fine structure of the exciton state including the transition of the biexciton to the dark exciton state.     

Relaxation and dephasing of multiexcitons in semiconductor quantum dots

We measure the dephasing time of ground-state excitonic transitions in InGaAs quantum dots under electrical injection in the temperature range from 10 to 70 K. Electrical injection into the barrier region results in a pure dephasing of the excitonic transitions. Once the injected carriers fill the electronic ground state, the biexciton to exciton transition is probed and a correlation of the exciton and biexciton phonon scattering mechanisms is found. Additional filling of the excited states creates multiexcitons that show a fast dephasing due to population relaxation.     

Using two-dimensional photon echo spectroscopy to probe the fine structure of the ground state biexciton of CdSe nanocrystals

The origin of the fine structure of the ground state single- and biexciton of CdSe nanocrystals is reviewed, along with the theoretical framework used to describe these states. Calculations were performed to determine the transition dipole moments of optically allowed transitions from the single- to biexciton fine structure states. Two-dimensional photon echo spectroscopy measurements for a sample of CdSe nanocrystals are reported. The two-dimensional electronic spectrum at a population time of 0 fs is analyzed using a simulation based on k.p theory predictions of the exciton and biexciton manifolds of states. The analysis suggests that a particular excited state absorption transition from the single- to biexciton fine structure dominates the 2D spectra. These excited state absorptions are clearly resolved in 2D spectra and the method therefore has promise for gaining clearer insights into quantum dot spectroscopy.     

Electronic structure and absorption spectrum of biexciton obtained by using exciton basis

We approach the biexciton Schrödinger equation not through the free-carrier basis as usually done, but through the free-exciton basis, exciton–exciton interactions being treated according to the recently developed composite boson many-body formalism which allows an exact handling of carrier exchange between excitons, as induced by the Pauli exclusion principle. We numerically solve the resulting biexciton Schrödinger equation with the exciton levels restricted to the ground state and we derive the biexciton ground state as well as the bound and unbound excited states as a function of hole-to-electron mass ratio. The biexciton ground-state energy we find, agrees reasonably well with variational results. Next, we use the obtained biexciton wave functions to calculate optical absorption in the presence of a dilute exciton gas in quantum well. We find an asymmetric peak with a characteristic low-energy tail, identified with the biexciton ground state, and a set of Lorentzian-like peaks associated with biexciton unbound states, i.e., exciton–exciton scattering states. Last, we propose a pump–probe experiment to probe the momentum distribution of the exciton condensate.     

Nonlinear optical properties of biexciton states in GaN quantum disks

The ground state energy of an exciton and biexciton states, in a GaN/Al_xGa_1-xN quantum disk are investigated by the variation method, within envelope function and effective mass approximations. Exciton and biexciton binding energy, and the dipole moments related to the transition between ground, exciton and biexciton states, are calculated as a function of quantum disk geometry. The optical nonlinearity via the exciton and biexciton states is studied on the basis of a three level model through the density matrix formalism. The behavior of different terms of third order susceptibility χ⁽³⁾, are studied around resonance frequencies and for different geometries of disk. The effect of values of the decay rates on χ⁽³⁾ are studied. It is found that these values have remarkable effect on the second term of, χ⁽³⁾.     

Surface photovoltage in exciton absorption range in CdS

The high resolution, intrinsic spectra of surface photovoltage are reported for semiconducting n-type CdS single crystals. At reduced temperatures (120–160 K) the spectra exhibit three sharp maxima due to A, B and C free exciton transitions. Energy positions of these lines and valence band parameters (spin-orbit and crystal field splittings) estimated from surface photovoltage are in good agreement with values obtained by other methods. The excitonic transitions are very sensitive to surface treatment, i.e. polishing, etching, background illumination and surface doping. The mechanism of direct interaction of free excitons with surface states is proposed to explain exciton lines in surface photovoltage.     

Theory of exciton effects in the high-field magnetoabsorption of real semiconductors

Direct exciton states of cubic semiconductors in a high magnetic field are investigated taking into full account the degeneracy and anisotropy of the valence bands. The adiabatic method is used to decouple the components of the motion parallel and perpendicular to the magnetic field. One-dimensional Hamiltonians are obtained analytically for the various exciton states and selection rules for optical transitions are discussed. Accurate numerical values of the energy levels are given for H parallel to the (110) direction. The results obtained provide the first quantitative interpretation of the fine structure observed in high resolution measurements of magnetoabsorption in Ge.     

Nonlinear optics and plasma-induced bistability in CdS

The investigation of highly excited semiconductors and of nonlinear optical properties recently tends to merge into one field of semiconductor physics. This is demonstrated here for the case of CdS. Two experimental methods are presented, which allow us both to detect optical nonlinearities and to understand their physical origins. These are the creation of laser-induced gratings and the excite- and- probe technique. The reasons for the nonlinearities are a broadening of the exciton resonances, transitions to the biexciton and the formation of an electron-hole plasma. The latter point is discussed in some detail and it is demonstrated, how the nonlinearities connected with this phase transition may be exploited to produce a dispersive and an intrinsic, absorptive bistability.     

Biexcitons in II–VI crystals: New interpretation of emission spectra

We report detailed magnetooptic studies of the so-called P line in CdS and CdSe crystals at high excitations (10³-10⁴ W cm^-2). The whole complex of experimental data allows to conclude unambiguously that the P line is connected with transitions from the Γ₁ ground state of excitonic molecule to 2P excited state of free exciton. Experimental values of binding energies of biexciton, that is 2.5 meV in CdS and 1.2 meV in CdSe, have been found.     

Four-wave mixing signals from extended exciton states above the mobility edge in GaAs/(Ga,Al)As multiple quantum wells

We investigate the dependence of four-wave mixing response on the photon energy close to the fundamental exciton (X) resonance in GaAs quantum wells. We find that cross-polarised incident fields give rise to a non-linear signal which decays faster at energies below the X line centre than above. We show that this behaviour cannot be assigned to biexciton transitions alone but rather suggests that the delocalised X states above the mobility edge are excited off-resonantly by the laser light having slightly lower energies.     

Electromagnetically induced transparency in bulk and microcavity semiconductors

We discuss our recent results on electromagnetically induced transparency (EIT) effects based on intrinsic free exciton and biexciton states in semiconductors. The Λ configuration obtained from the 1S and 2P yellow exciton levels of Cu₂O leads to a well-developed EIT regime, akin to the atomic case. The coherent driving of the exciton–biexciton transition in CuCl induces a tunable transparency window within the polaritonic stop-band, due to the presence of a third polariton branch in the dressed system. In a microcavity configuration, this gives rise to three reflectivity dips in the strong coupling regime.     

Exciton-Boson Formalism in the Theory of Laser-Excited Semiconductors and Its Application in Coherent Four-Wave-Mixing Spectroscopy

By the use of a bosonization transformation and group-theoretical arguments, the Hamiltonian of an electron–hole–photon system in a laser-excited direct two-band semiconductor is transcribed into that of an exciton–photon system with the particle spins rigorously taken into consideration. It is shown that the third-order optical nonlinearities in the spectral region below the band edge have their microscopic origin in two-exciton correlations, which are expressed in terms of the effective exciton–exciton and anharmonic exciton–photon interactions. The dependence of the interparticle interactions on the spin states of quasiparticles is behind the polarization dependence of the semiconductor nonlinear optical response. On the example of the system of heavy hole excitons in quantum wells, grown from compounds with the zinc blende type of symmetry, it is demonstrated that the effective exciton–exciton interaction in two-exciton states with nonzero total spin is repulsive, while in zero-spin states it is attractive, which may result in the biexciton formation. The derived Heisenberg equations of motion for the exciton and biexciton operators form the basis for a theoretical study of the coherent four-wave-mixing in GaAs and ZnSe quantum wells. It is readily apparent from the equations that in different polarization configurations the coherent four-wave-mixing is generated by different ingredients of two-exciton Coulomb correlations: in the co-circular configuration, it is the interexciton repulsion, in the cross-linear configuration, the formation of the biexciton and its coupling to excitons, and in the collinear configuration, both of them jointly. The obtained expressions for the time-resolved and frequency-resolved four-wave-mixing signals adequately describe the main characteristics and various details of wave mixing phenomena, including a biexciton signature in the appropriate polarization configurations. Results of the work clarify the microscopic mechanism of the polarization dependence in coherent four-wave-mixing spectroscopy in semiconductor quantum wells.     

Biexcitonic absorption in a disk-shaped GaN quantum dot

The present work investigates the nonlinear optical properties of a GaN quantum dot in the disk limit via the exciton and biexciton states using the compact density matrix formalism. Based on this model, we calculate the ground state energy of the exciton and biexciton states by the variation method, within envelope function and effective mass approximations. Linear and nonlinear optical absorption (α ⁽¹⁾, α ⁽³⁾) and oscillator strengths attributed to the optical transitions are obtained. The details of the behaviour of α ⁽¹⁾ and α ⁽³⁾ around the resonance frequencies and for different quantum dot geometries are presented. It is found that the size of quantum dot and the optical intensity have a remarkable effect on the optical absorption, and the biexcitonic two-photon absorption coefficient(K ₂) has also been calculated in this system. The results show that this parameter is strongly affected by the size of the quantum dot.     

Theory of multi-exciton states in semiconductor nanocrystals

In this article, the fundamental physics of multi-exciton states in semiconductor nano-crystals is reviewed focusing on the mesoscopic enhancement of the excitonic radiative decay rate and the excitonic optical nonlinearity and the mechanism of their saturation with increase of the nanocrystal size. In the case of the radiative decay rate the thermal excitation of excited exciton states having small oscillator strength within the homogeneous linewidth of the exciton ground state is essential in determining the saturation behavior. The weakly correlated exciton pair states are found to cause a cancellation effect in the third-order nonlinear optical susceptibility at the exciton resonance, providing the first consistent understanding of the experimentally observed saturation of the mesoscopic enhancement of the excitonic optical nonlinearity. The presence of the weakly correlated exciton pair states is confirmed convincingly from the good correspondence between theory and experiments on the induced absorption spectra from the exciton state in CuCl nanocrystals. Furthermore, ultrafast relaxation processes of biexcitons are discussed in conjunction with the observed very fast rise of the biexciton gain in nanocrystals. In prospect of future progress in research, the theoretical formulation to calculate the triexciton states as one of the multi-exciton states beyond the biexciton is presented for the first time including the electron-hole exchange interaction.     

One-directional gain and frequency selection of electromagnetic waves in a medium with a running grating of inverse population

The effects of one-directional amplification, frequency selection and transformation of time structure of electromagnetic waves (the generation of ultra-short pulses) are considered theoretically for a medium, where the creation of a running wave of atomic states inverse population is possible under excitation by coherent light beams with different frequencies and directions. These effects are due to the possibility of synchronism of a group velocity of an amplified electromagnetic wave with the phase velocity of a wave of inverse population. The general theory is applied for describing two specific cases which are observed in CdS crystals where the gain effects are caused by: 1) radiative transitions on lines generating the P-band of recombination radiation (the visible range) and 2) radiative transitions between different exciton subbands (the far IR range).     

共轭聚合物中受激吸收与受激辐射的量子动力学研究

基于扩展的一维SSH紧束缚模型结合非绝热的分子动力学方法,理论研究了共轭聚合物分子(PPV)在光脉冲作用下受激吸收和受激辐射的量子动力学过程.首先,设定分子初始处于基态,讨论了受激吸收过程中不同的电子受激跃迁模式与光激发脉冲的关系.通过对终态的分析,发现分子受激后只能产生电子-空穴的束缚态,包括:激子、双激子和高能激子.计算了各种激发态的产率,特别是,给出了各种激发态产率与光激发能量的定量关系.此外,基于实验,分别讨论了光激发强度对高能激子和双激子产率的影响,并与实验结果进行了比较.最后,设定分子初始分别处于激子和双激子态,研究了分子内定域能级之间的受激辐射过程,并简单讨论了激子和双激子受激辐射与光激发能量及强度的关系.     

Correlated photons from multi-carrier complexes in GaAs quantum dots

We have studied micro-photoluminescence spectra of a self-assembled single GaAs quantum dot under 8 K. With strong pulsed excitation, the micro-photoluminescence spectrum shows bright emission lines originated from an exciton, a positively charged exciton, and a biexciton, together with weak lower energy emissions reflecting multi-excitonic structures with more carriers. We have identified the origins of these weak emission lines, and showed the existence of charged biexciton states, through single photon correlation measurements and excitation power dependence of the photoluminescence intensity. In addition, investigating the radiative recombination process of the charged biexciton, we have determined the electron–hole exchange energy in the GaAs quantum dot.     

Site-selective four-wave-mixing experiments in GaAs/(GaAl) As multiple quantum wells

Il Nuovo Cimento D - The influence of biexciton formation on the four-wave-mixing response of multiple quantum wells having a strong inhomogeneous broadening of the exciton transitions has been...     

Photoluminescence of tetrahedral quantum-dot quantum wells

Taking into account the tetrahedral shape of a quantum-dot quantum well (QDQW) when describing excitonic states, phonon modes, and the exciton-phonon interaction in the structure, we obtain within a nonadiabatic approach a quantitative interpretation of the photoluminescence spectrum of a single CdS/HgS/CdS QDQW. We find that the exciton ground state in a tetrahedral QDQW is bright, in contrast to the dark ground state for a spherical QDQW. The position of the phonon peaks in the photoluminescence spectrum is attributed to interface optical phonons. We also show that the experimental value of the Huang-Rhys parameter can be obtained only within the nonadiabatic theory of phonon-assisted transitions.