Transient interband light absorption by quantum dots: Degenerate pump-probe spectroscopy

The optical pump-probe method, which makes it possible to determine the energy relaxation rate for excited electron-hole pairs and excitons in semiconductor quantum dots (QDs), is theoretically described. A scheme in which the carrier frequencies of optical pump and probe pulses are close to resonance with the same interband transition in the QD electron subsystem (degenerate case) is considered. The pump-induced probe energy absorption is analyzed as a function of the delay time between the pump and probe pulses. It is shown that under certain conditions this dependence is reduced to monoexponential, whose exponent is proportional to the energy relaxation rate for the considered state of electron-hole pairs and excitons. The size dependence of the energy relaxation rate of the electron-hole pair states is modeled by the example of PbSe-based QDs, whose electron subsystem is in the strong-confinement regime.     

Transient intraband light absorption by quantum dots: Pump-probe spectroscopy

We have developed a theory of a transient intraband light absorption by semiconductor quantum dots. This absorption plays an important role in the two-pulse pump-probe method, which enables determining the energy relaxation rates of electron-hole excited states. We have considered all possible schemes of this process wherein the carrier frequency of optical pump pulses is close to the resonance with the interband transition of the quantum-dot electronic subsystem, while the carrier frequency of probe pulses is resonant to the intraband transition. For ensembles of identical and size-distributed quantum dots, the probe pulse energy absorption induced by the pump pulse is analyzed in relation to the delay time between the pulses. We have found that, under certain conditions, this dependence can be described by a single, two, or three exponentials. The exponents of the exponentials are proportional to the energy relaxation rates of electron-hole excited states.     

Exciton optical transitions in quantum wells with spin-orbit coupling

The energy spectrum of light-hole and heavy-hole excitons and optical absorption in a quantum well have been analyzed taking into account Rashba spin-orbit coupling. Interband and intraband exciton transitions have been considered. It has been shown that, in the presence of spin-orbit coupling, the probabilities of the interband and intraband photoelectric effects diverge in the vicinity of the threshold if the electron-hole interaction is neglected. The threshold probabilities of the interband and intraband photoelectric effects become finite when Coulomb interaction is taken into account.     

Femtosecond response from two copolymers with intense two-photon absorption

Under excitation of femtosecond laser pulses at 800 nm, intense two-photon absorption induced fluorescence was observed from two copolymers, linear structure copolymer M2 and tri-branched copolymer M3. In a one-color pump–probe experiment at 800 nm, an ultrafast transient absorption was observed, which was mainly from the simultaneous absorption of the one photon from the pump beam and another photon from the probe beam. This analysis was further confirmed by a two-color pump–probe measurement with a pump at 800 nm and a probe at 556 nm, respectively. The other two decaying processes in transient absorption have a lifetime of about 14 and 126 ps, which reflects the intraband relaxation and the decay of the excited state via intersystem crossing or the solvation effect, respectively.     

飞秒时间分辨实验中相关函数和时间零点的确定

结合飞秒激光在研究分子激发态弛豫动力学中的应用,介绍了几种飞秒时间分辨实验中确定泵浦激光脉冲与探测激光脉冲的相关函数和时间零点的方法.对于波长在可见波段的泵浦和探测激光脉冲,我们可以利用非线性光学的技术手段,探测泵浦光与探测光的和频光的强度随二者间的时间延迟的变化来确定相关函数和时间零点;对于波长在紫外甚至更短的波段的泵浦和探测激光脉冲,由于单脉冲能量比较低,目前还很难利用技术手段来测定泵浦激光与探测激光的相关函数及时间零点,可以利用某些原子气体(如Xe)或某些具有短寿命态的分子作平行实验进行间接测量.     

Full configuration interaction studies of phonon and photon transition rates in semiconductor quantum dots

Quantum chemical methods originally developed for studying atomic and molecular systems can be applied successfully to the study of few-body electron-hole systems in semiconductor nanostructures. A new computational approach is presented for studying the energetics and dynamics of interacting electrons and holes in a semiconductor quantum dot. The electron-hole system is described by a two-band effective mass Hamiltonian. The Hamiltonian is diagonalized in a configuration state function basis constructed as antisymmetric products of the electron one-particle functions and antisymmetric products of the hole one-particle functions. The symmetry adapted basis set used for the expansion of the one-particle functions consists of anisotropic Gaussian basis functions. The transition probability between electron-hole states consisting of different numbers of carrier pairs is calculated at the full configuration interaction level. The results show that the electron-hole correlation affects the radiative recombination rates significantly. A method for calculating the phonon relaxation rates between excited states and the ground state of quantum dots is described. The phonon relaxation calculations show that the relaxation rate is strongly dependent on the energy level spacings between the states.     

Investigation of non-equilibrium electron-hole plasma in nanowires by THz spectroscopy

Efficient emission of THz radiation by AlGaAs nanowires via excitation of photocurrent by femtosecond optical pulses in nanowires was observed. Dynamics of photoinduced charge carrier was studied via influence of electron-hole plasma on THz radiation by optical pump THz probe method. It was found that characteristic time of screening of contact field is about 15 ps. Recombination of non-equilibrium occurs in two stages: fast recombination of free electron and holes (with relaxation time about 700 ps), and slow recombination (with relaxation time about 15 ns), which involves a capture of electrons and holes on the defects of crystalline structure of nanowires.     

飞秒时间分辨实验中泵浦-探测交叉相关函数的测量和时间零点的确定

飞秒激光技术的出现使得实时探测与跟踪激发态超快弛豫动力学过程成为可能,并能够给出激发态动力学过程清晰的物理图像。而在飞秒时间分辨实验中,泵浦-探测相关函数和时间零点直接影响实验结果的可靠性和准确性。本文结合飞秒激光在分子激发态超快动力学过程中的应用进展,介绍了根据实验条件和要求,在具体实验过程中泵浦-探测相关函数测量和时间零点确定的几种方法。实验中选择可见光作为泵浦光和探测光时,可以通过测定随泵浦-探测时间延迟变化的泵浦激光与探测激光的和频/差频光强来确定泵浦探测交叉相关函数和时间零点;而选择中心波长在紫外甚至真空紫外的激光脉冲作为泵浦光或探测光时,泵浦-探测交叉相关函数通常采用校正的方法测量。     

Detection of directed electron-hole recombination energy transfer from an ionic crystal matrix to self-assembled nanocrystals

It is found that the energy released in the spin-dependent tunneling recombination of electron-hole pairs and self-trapped excitons in an ionic crystal matrix is directionally transferred to low-dimensional semiconductor structures embedded in the matrix as a result of self-assembled growth. The EPR spectra of electron and hole centers in the matrix crystal are detected by tunneling afterglow and photostimulated luminescence that are excited in the low-dimensional structure.     

Observation of excitons in one-dimensional metallic single-walled carbon nanotubes

Excitons are generally believed not to exist in metals because of strong screening by free carriers. Here we demonstrate that excitonic states can in fact be produced in metallic systems of a one-dimensional character. Using metallic single-walled carbon nanotubes as a model system, we show both experimentally and theoretically that electron-hole pairs form tightly bound excitons. The exciton binding energy of 50 meV, deduced from optical absorption spectra of individual metallic nanotubes, significantly exceeds that of excitons in most bulk semiconductors and agrees well with ab initio theoretical predictions.     

Spin relaxation of Mn ions in (CdMn)Te/(CdMg)Te quantum wells under picosecond optical pumping

Spin relaxation of Mn ions in a Cd_0.97Mn_0.03Te/Cd_0.75Mg_0.25Te quantum well with photogenerated quasi-two-dimensional electron-hole plasma at liquid helium temperatures in an external magnetic field has been investigated. Heating of Mn ions by photogenerated carriers due to spin and energy exchange between the hot electron-hole plasma and Mn ions through direct sd-interaction between electron and Mn spins has been detected. This process has a short characteristic time of about 4 ns, which leads to appreciable heating of the Mn spin subsystem in about 0.5 ns. Even under uniform excitation of a dense electron-hole plasma, the Mn heating is spatially nonuniform, and leads to formation of spin domains in the quantum well magnetic subsystem. The relaxation time of spin domains after pulsed excitation is measured to be about 70 ns. Energy relaxation of excitons in the random exchange potential due to spin domains results from exciton diffusion in magnetic field B=14 T with a characteristic time of 1 to 4 ns. The relaxation time decreases with decreasing optical pump power, which indicates smaller dimensions of spin domains. In weak magnetic fields (_B=2 T) a slow down in the exciton diffusion to 15 ns has been detected. This slow down is due to exciton binding to neutral donors (formation of bound excitons) and smaller spin domain amplitudes in low magnetic fields. The optically determined spin-lattice relaxation time of Mn ions in a magnetic field of 14 T is 270±10 and 16±7 ns for Mn concentrations of 3% and 12%, respectively. Zh. éksp. Teor. Fiz. 112, 1440–1463 (October 1997)     

Nonlinear optical studies of the transient coherence in the Quantum Hall system

We review recent investigations of the femtosecond nonlinear optical response of the two-dimensional electron gas (2DEG) in a strong magnetic field. We probe the Quantum Hall (QH) regime for filling factors ν∼1. Our focus is on the transient coherence induced via optical excitation and on its time evolution during early femtosecond timescales. We simultaneously study the interband and intraband coherence in this system by using a nonlinear spectroscopic technique, transient three-pulse four wave mixing optical spectroscopy, and a many-body theory. We observe striking differences in the temporal and spectral profile of the nonlinear optical signal between a modulation doped quantum well system (with the 2DEG) and a similar undoped quantum well (without a 2DEG). We attribute these qualitative differences to Coulomb correlations between the photoexcited electron-hole pairs and the 2DEG. We show, in particular, that intraband many-particle coherences assisted by the inter-Landau-level magnetoplasmon excitations of the 2DEG dominate the femtosecond nonlinear optical response. The most striking effect of these exciton-magnetoplasmon coherences is a large off-resonant four-wave-mixing signal in the case of very low photoexcited carrier densities, not observed in the undoped system, with strong temporal oscillations and unusually symmetric temporal profile.     

Ultrafast changes in the optical properties of a titanium surface and femtosecond laser writing of one-dimensional quasi-periodic nanogratings of its relief

One-dimensional quasi-periodic nanogratings with spacings in the range from 160 to 600 nm are written on a dry or wet titanium surface exposed to linearly polarized femtosecond IR and UV laser pulses with different surface energy densities. The topological properties of the obtained surface nanostructures are studied by scanning electron microscopy. Despite the observation of many harmonics of the one-dimensional surface relief in its Fourier spectra, a weak decreasing dependence of the first-harmonic wavenumber (nanograting spacing) on the laser fluence is found. Studies of the instantaneous optical characteristics of the material during laser irradiation by measuring the reflection of laser pump pulses and their simulation based on the Drude model taking into account the dominant interband absorption allowed us to estimate the length of the excited surface electromagnetic (plasmon-polariton) wave for different excitation conditions. This wavelength is quantitatively consistent with the corresponding nanograting spacings of the first harmonic of the relief of the dry and wet titanium surfaces. It is shown that the dependence of the first-harmonic nanograting spacing on the laser fluence is determined by a change in the instantaneous optical characteristics of the material and the saturation of the interband absorption along with the increasing role of intraband transitions. Three new methods are proposed for writing separate subwave surface nanogratings or their sets by femtosecond laser pulses using the near-threshold nanostructuring, the forced adjustment of the optical characteristics of the material or selecting the spectral range of laser radiation, and also by selecting an adjacent dielectric.     

Interband phototransitions in AgBr nanocrystals assisted by free carriers

The photolysis of AgBr nanocrystals irradiated by picosecond light pulses with quantum energies of 3.51 and 1.17 eV is theoretically analyzed. The observed dependences of the photometric density on the long-wavelength radiation intensity are shown to be determined by the photogeneration of nonequilibrium electron-hole pairs as a result of indirect interband phototransitions involving free electrons. For such electrons to be involved in this process, they should possess a high kinetic energy, which is acquired due to intraband non-linear absorption of the intense long-wavelength radiation.     

Two-temperature relaxation and melting after absorption of femtosecond laser pulse

The theory and experiments concerned with the electron-ion thermal relaxation and melting of overheated crystal lattice constitute the subject of this paper. The physical model includes two-temperature (2T) equation of state, many-body interatomic potential, the electron-ion energy exchange, electron thermal conductivity, and optical properties of solid, liquid, and two phase solid-liquid mixture. Two-temperature hydrodynamics and molecular dynamics codes are used. An experimental setup with pump-probe technique is used to follow evolution of an irradiated target with a short time step 100 fs between the probe femtosecond laser pulses. Accuracy of measurements of reflection coefficient and phase of reflected probe light are 1% and ∼1 nm, respectively. It is found that, firstly, the electron-electron collisions make a minor contribution to a light absorption in solid Al at moderate intensities; secondly, the phase shift of a reflected probe results from heating of ion subsystem and kinetics of melting of Al crystal during  ps, where t is time delay between the pump and probe pulses measured from the maximum of the pump; thirdly, the optical response of Au to a pump shows a marked contrast to that of Al on account of excitation of d-electrons.     

Optical and luminescent VUV spectroscopy of La2Be2O5 crystals

Electronic excitations and the processes of their radiative relaxation are studied in pure and Ce³⁺ ion-doped crystals of lanthanum beryllate excited by synchrotron radiation in the x-ray and VUV ranges by methods of optical and luminescent vacuum ultraviolet time-resolved spectroscopy. Manifestations of excitons of the valence band are absent in the reflection spectra. However, a fast (τ=1.7 ns) and a slow (microsecond range) channel corresponding to two possible types of self-trapped excitons (STE) are found in radiative relaxation of intrinsic electronic excitations at T=10 K. The slow channel corresponds to emission of STE formed through recombination, the fast channel corresponds to emission of relaxed metastable excitons from the STE state. In the energy region higher than 14 eV (E>2E _g), the effect of multiplication of electronic excitations due to generation of secondary electron-hole pairs resulting from inelastic scattering of both hot photoelectrons and hot photoholes is exhibited.     

The model of ultrafast light-induced insulator-metal phase transition in VO2

Ultrafast light-induced insulator-metal phase transitions (PT) in VO₂ thin films was studied with use of a pump-probe technique. The theoretical and experimental study of PT kinetics shows that the PT could be realized via an intermediate state. The relaxation processes after optical pumping are dependent on pump energy. The excitonic controlled model for such type of PT is proposed. The main channel for the ultrafast light-induced PT is the resonant transition between excited states of correlated vibronic Wannier-Mott excitons (WME) in insulator phase and the unoccupied excited states in metallic phase. During this process an equilibrium local distortion occurred. According to the proposed model the experimental observation of the drastic temperature- and pump power- dependent relaxation processes could be interpreted.     

Elementary relaxation processes investigated by femtosecond photoelectron spectroscopy of two‐dimensional materials

Elementary scattering processes in solid matter occur on ultrafast timescales and photoelectron spectroscopy in the time domain represents an excellent tool for their analysis. Conventional photoemission accesses binding energies of electronic states and their momentum dispersion. The use of femtosecond laser pulses in pump‐probe experiments allows obtaining direct insights to the energy and momentum dependence of ultrafast dynamics. This article introduces the elementary interaction processes and emphasizes recent work performed in this rapidly developing field. Decay processes in the low excitation limit are addressed, where electrons decay according to their interaction with carriers in equilibrium. Here, hot electron relaxation in epitaxial metallic film is reviewed. In the limit of an intense optical excitation, scattering of the excited electrons among each other establishes a non‐equilibrium state. Results on charge‐density wave materials and the effect of coherent nuclear motion on the electronic structure, which can break low symmetry ground states, are discussed. Figure reprinted with permission from [71].     

Kinetics of thermalized luminescence of a single quantum dot at room temperature

We have developed a theory of transient secondary emission of a single quantum dot from the lowest energy states of electron-hole pairs. We consider a process in which laser pulses excite a certain highenergy state of electron-hole pairs of a quantum dot at room temperature, with the electronic subsystem then relaxing to low-energy states and photons being emitted. Therefore, the investigated secondary emission process is thermalized luminescence. For definiteness, the developed model takes into account two states of electron-hole pairs that contribute to the luminescence. We have analyzed the dependence of the secondary emission signal on the energy gap between these states, the value of which is determined by the quantum dot size. In terms of the Pauli master kinetic equation, an analytical expression for the time dependent signal of the thermalized luminescence has been obtained. We show that, as the spectral width of the exciting laser pulse tends to zero, this expression yields the signal of stationary luminescence.     

Indirect excitons and double electron-hole layers in a wide single GaAs/AlGaAs quantum well in a strong electric field

The recombination spectra of indirect excitons and double electron-hole layers in a wide single quantum well in an electric field are studied. It is found that electrons and holes in the wide well become spatially separated in a sufficiently strong electric field. This leads to a substantial reorganization of the radiative recombination spectrum and to a significant increase in the carrier lifetime. It is shown that the total charge of the electron-hole system can be changed by varying the photoexcitation frequency and the applied electric field, thus passing from the neutral case of indirect excitons to the case of charged double electron-hole layers. The concentration of excess carriers in the well is measured as a function of the electric field strength. The behavior of the excited states of indirect heavy-hole and light-hole excitions is studied for a neutral excitonic system in a strong electric field. It is shown that the electric-field dependences allow the excited states of indirect excitons with a light hole to be distinguished from the excited states with a heavy hole.