Biexciton quantum coherence in a single quantum dot

Nondegenerate (two-wavelength) two-photon absorption using coherent optical fields is used to show that there are two different quantum mechanical pathways leading to formation of the biexciton in a single quantum dot. Of specific importance to quantum information applications is the resulting coherent dynamics between the ground state and the biexciton from the pathway involving only optically induced exciton/biexciton quantum coherence. The data provide a direct measure of the biexciton decoherence rate which is equivalent to the decoherence of the Bell state in this system, as well as other critical optical parameters.     

Coherent control in a single semiconductor quantum dot exhibiting excitonic and biexcitonic features

We have developed a simplified theoretical model to analyze the phenomenon of coherent control in a single semiconductor quantum dot excited by a pair of optical pulses. The first pulse populates a biexciton state by two-photon absorption while the second pulse generates population in the exciton state via deexcitation from the biexciton state. We have used density-matrix analysis for a 3-level system to calculate the time dependent biexciton and exciton state populations. The usual 9×9 matrix has been reduced to a 6×6 matrix. The time variation of the population in each state and it’s dependence on the pulse delay manifest coherent control. Numerical estimates made for In_0.5Ga_0.5As/GaAs single quantum dots qualitatively agree with the recent experimental results. PACS 78.67.Hc; 42.50.Md; 78.55.Cr     

Optical properties of semiconductors under strong pumping in the <Emphasis Type="Italic">M</Emphasis>-band region and two-photon probing of the biexciton state

The behavior of the semiconductor dielectric susceptibility under the action of a strong laser pulse in the range of the luminescent M band and two-photon probe of a biexciton level is investigated. It is shown that the pronounced Autler-Towns effect occurs at the two-photon transition. The position of the absorption peaks is essentially determined by the amplitude and frequency of the pump field.     

Direct two-photon creation of a biexciton

The nonlinear absorption coefficient for the two-photon creation of biexciton in CuCl is calculated in the approximation of one intermediate, optically active excitonic state. The two-band model with realistic band structure at the band extrema is considered. The exciton-biexciton dipole transition momentum matrix element is expressed by the functional of the exciton and biexciton envelopes. In the numerical calculations the envelope of the Hylleraas-Ore type, modified by Brinkman et al., is used. Our calculated value of the absorption coefficient is about two orders of magnitude smaller than that estimated previously by Hanamura, and agrees better with the experimental value reported by Gale and Mysyrowicz.     

Two-photon excitation of confined biexcitons in CuCl quantum dots

We have studied direct creation processes of confined biexcitons in CuCl quantum dots by polarization-dependent resonant two-photon excitation spectroscopy. The two-photon absorption band for the lowest state of the biexciton (total angular momentum J=0) which appears on the lower energy side of confined exciton band was identified from the analysis of the polarization dependence of the photoluminescence excitation spectrum of the biexciton. Furthermore, the two-photon excitation process for the excited state of the biexciton (J=2) was also found with polarization dependence different from the J=0 biexciton state.     

Efficient two-photon light amplification by a coherent biexciton wave

A reversible coupling between photon pair states and a long-lived, highly coherent biexciton wave in CuCl allows efficient phase-sensitive two-photon amplification or attenuation of ultrashort light pulses. We demonstrate a gain of 350 cm(-1) for a pump intensity of 1 MW/cm(2), nearly 2 orders of magnitude higher than that achievable with conventional parametric crystal amplifiers. We develop a theoretical model that describes this new type of parametric converter where the light pump is replaced by a coherent biexciton wave and show that it is well suited for the generation of entangled photons and the squeezing of an optical beam with ultrafast time gating.     

Stimulated emission from the biexciton in a single self-assembled II-VI quantum dot

Using two-photon excitation, stimulated emission from the biexciton state in a single CdSe/ZnSe quantum dot is observed in a two-pulse configuration. We directly time resolve the emission-absorption characteristics and verify the potential for laser action. By setting the polarization of the stimulation pulse, the recombination path of the biexciton and, by this, the state of the photons emitted in the decay cascade is controlled. We elaborate also the coherent response and address entanglement and disentanglement of the exciton-biexciton system.     

单光子和双光子电磁诱导透明谱的相干调制

采用一束相干外场作用在倒Y模型原子的基态与另外状态构成的跃迁上,实现对单光子和双光子电磁诱导透明谱的调制。经研究发现相干外场对单光子和双光子的吸收性质有类似的影响效果。由于相干外场的作用,吸收谱的共振点附近出现吸收峰将原单重透明谱分裂为双重透明谱。诱导的吸收峰的高度和透明谱的频谱宽度与相干外场的强度有密切关系。并用缀饰态理论解释了这些物理现象。这些研究对多通道光通信以及对原子光学性质的调控方面有积极意义。     

Two-photon coherent control of a single quantum dot

We report on two-photon coherent control of the biexciton state in single Stranski-Krastanov CdSe quantum dots. Clear interference patterns are observed at twice the optical frequency. The decay of the interference contrast is nonexponential and caused by a dynamical inhomogeneous broadening of the energy levels due to long-term fluctuations in the dot environment.     

强光场下非共振双光子跃迁相干控制

利用飞秒激光脉冲相位整形技术,从理论和实验两方面,对强激光场下分子体系苝溶液中非共振双光子跃迁的相干控制进行了研究。通过对飞秒激光脉冲进行相位扫描和余弦相位调制,发现分子体系中非共振双光子的跃迁几率能够被削弱,但不能完全消除。分子体系中非共振双光子跃迁的相干控制受到激光光场的形状和分子吸收谱谱宽的影响;与原子体系相比,分子体系中非共振双光子跃迁相干控制的调制效率降低。     

Extremely large binding energy of biexcitons in an organic-inorganic quantum-well material (C4H9NH3)2PbBr4

We have confirmed biexciton formation in an organic-inorganic hybrid quantum-well material (C₄H₉NH₃)₂PbBr₄ by photoluminescence and two-photon absorption measurements. The biexciton has extremely large binding energy, 60 meV, which to our knowledge is the largest value ever reported for a semiconductor. By analyzing the spectrum of biexciton luminescence, the biexciton gas temperature was found to be much higher than the bath temperature due to a higher local temperature arising from the large biexciton binding energy.     

Coherent control of non-resonant two-photon transition in molecular system

In this paper,we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape).The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth.Our results demonstrate that,the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field,and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.     

Local Control of Two-Photon Absorption in a Six-Level Atomic System by Using a Coherent Perturbation Field

If a coherent perturbation field is used to couple the excited level of thecoupling transition in the five-level K-type atom with another higher excitedlevel, the two-photon electromagnetically induced transparency can belocally modulated by altering the parameters of the additional perturbationfield. With different detunings of the coherent perturbation field, theabsorption peak or transparency window with sharp and high-contrast spectral feature can be generated in the two-photon absorption spectrum. The physical interpretation of these phenomena is given in terms of the dressed states.     

Spontaneous two-photon emission from a single quantum dot

Spontaneous two-photon emission from a solid-state single quantum emitter is observed. We investigated photoluminescence from the neutral biexciton in a single semiconductor quantum dot coupled with a high Q photonic crystal nanocavity. When the cavity is resonant to the half energy of the biexciton, the strong vacuum field in the cavity inspires the biexciton to simultaneously emit two photons into the mode, resulting in clear emission enhancement of the mode. Meanwhile, the suppression of other single photon emission from the biexciton was observed, as the two-photon emission process becomes faster than the others at the resonance.     

Nonlinear spectrum effect on the coherent control of molecular systems

This work demonstrates that the detuning of the fs-laser spectrum from the two-photon absorption band of organic materials can be used to reach further control of the two-photon absorption by pulse spectral phase manipulation. We investigate the coherent control of the two-photon absorption in imidazole-thiophene core compounds presenting distinct two-photon absorption spectra. The coherent control, performed using pulse phase shaping and genetic algorithm, exhibited different growth rates for each sample. Such distinct trends were explained by calculating the two-photon absorption probability considering the intrapulse interference mechanism, taking into account the two-photon absorption spectrum of the samples. Our results indicate that tuning the relative position between the nonlinear absorption and the pulse spectrum can be used as a novel strategy to optimize the two-photon absorption in broadband molecular systems.     

Coherent Phase Control of Ultrafast Polarization Beats in Reverse V-Type Three-Level System

We investigate the third-order nonlinear absorption and dispersion of femto- and atto-second polarization beats between the one-photon degenerate four-wave mixing process and the two-photon nondegenerate four-wave mixing process in the pure homogeneously-broadened reverse V-three-level using twin noisy fields. The third-order nonlinear response can be controlled and modified by the colour-locked correlation of twin noisy fields. Most importantly, the coherent phase control in optical heterodyne detection for studying the phase dispersion of the third-order susceptibility is demonstrated. The radiation-matter detuning oscillation is also considered in the freauencv domain.     

Multichannel selective femtosecond coherent control based on symmetry properties

We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of "two-photon dark pulses" inducing widely tunable three-photon absorption.     

Strongly confined semiconductor quantum dots: Pair excitations and optical properties

This paper reviews a microscopic model of basic electron-hole pair excitation processes in strongly confined semiconductor quantum dots (QD) and their influence on the optical QD properties. The effects of valence band mixing, Coulomb interaction, and surface polarization are taken into account. The exciton and biexciton wave functions and energies are obtained using a numerical diagonalization method. The computed optical spectra, such as absorption, gain, pump-probe, and two-photon absorption, agree well with experiments.     

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.     

Coherent longitudinal-optical ground-state phonon in CdSe quantum dots triggered by ultrafast charge migration

We observe the CdSe longitudinal-optical ground-state phonon in the electron transfer system composed of CdSe quantum dots and methylviologen directly by femtosecond absorption spectroscopy. A significant phase shift indicates that the coherent oscillations are triggered by an ultrafast charge migration, which is the consequence of an electron transfer from the photoexcited quantum dot to the molecular acceptor methylviologen. In contrast, the observed coherent phonons in isolated quantum dots stem from the frequency modulation of the quantum dot excited-state spectrum. From the probe wavelength dependence of the longitudinal-optical phonons in the electronic ground state and excited state it is possible to determine a biexciton binding energy of 35?meV.