Single molecule photobleaching probes the exciton wave function in a multichromophoric system

The exciton wave function of a trichromophoric system is investigated by means of single molecule spectroscopy at room temperature. Individual trimers exhibit superradiance and loss of vibronic structure in emission spectrum, features proving exciton delocalization. We identify two distinct photodegradation pathways for single trimers upon sequential photobleaching of the chromophores. The rate of each pathway is a measure for the contribution of the separate dyes to the collective excited state of the system, in this way probing the wave function of the delocalized exciton.     

The vibrational exciton spectrum of p-nitrotoluene crystal film

The exciton absorption spectrum of p-nitrotoluene crystal film has been investigated by polarized IR radiation at low temperature. The Raman scattering in the crystalline and the solution state has been studied as an aid in the interpretation of the crystal spectrum. The observed exciton splittings are small and could be measured with certainty for only a few vibrations. The interpretation of the low temperature spectrum conforms to the crystal structure determined at room temperature by Barve and Pant.     

Collective state of interwell excitons in GaAs/AlGaAs double quantum wells under pulse resonance excitation

The time evolution and kinetics of photoluminescence (PL) spectra of interwell excitons in double GaAs/AlGaAs quantum wells (n-i-n structures) have been investigated under the pulse resonance excitation of intrawell 1sHH excitons using a pulsed tunable laser. It is found that the collective exciton phase arises with a time delay relative to the exciting pulse (several nanoseconds), which is due to density and temperature relaxation to the equilibrium values. The origination of the collective phase of interwell excitons is accompanied by a strong narrowing of the corresponding photoluminescence line (the line width is about 1.1 meV), a superlinear rise in its intensity, a long time in the change of the degree of circular polarization, a displacement of the PL spectrum toward lower energies (about 1.5 meV) in accordance with the filling of the lowest state with the exciton Bose condensate, and a significant increase in the radiative decay rate of the condensed phase. The collective exciton phase arises at temperatures T<6 K and interwell exciton densities n=3×10¹⁰ cm^?2. Coherent properties of the collective phase of interwell excitons and experimental manifestations of this coherence are discussed.     

Exciton-photon interaction in low-dimensional semiconductor microcavities

The structure of the photon states and dispersion of cavity polaritons in semiconductor microcavities with two-dimensional optical confinement (photon wires), fabricated from planar Bragg structures with a quantum well in the active layer, are investigated by measuring the angular dependence of the photoluminescence spectra. The size quantization of light due to the wavelength-commensurate lateral dimension of the cavity causes additional photon modes to appear. The dispersion of polaritons in photon wires is found to agree qualitatively with the prediction for wires having an ideal quantum well, for which the spectrum is formed by pairwise interaction between exciton and photon modes of like spatial symmetry. The weak influence of the exciton symmetry-breaking random potential in the quantum well indicates a mechanism of polariton production through light-induced collective exciton states. This phenomenon is possible because the light wavelength is large in comparison with the exciton radius and the dephasing time of the collective exciton state is long. Zh. éksp. Teor. Fiz. 114, 1329–1345 (October 1998)     

Non-radiative transformation of a singlet exciton into a triplet one in organic molecular crystals

The probability of non-radiative transformation of a singlet exciton into a triplet one in organic molecular crystals is calculated. Mechanisms caused by intermolecular interactions apparent at grouping molecules into a crystal together with spin-orbital molecular interactions are considered as mechanisms of non-radiative transformation. Dependence of the calculated probability on the temperature and the character of an energetic spectrum of a singlet and a triplet exciton is discussed. On the basis of the calculated probabilities for various specific mechanisms the influence of intermolecular interactions, when arranging molecules into a crystal, on the intensity of non-radiative transitions between singlet and triplet excited states of molecules in the crystal is analyzed.Na Slovance 2, Praha 8, Czechoslovakia.     

Bleaching in the region of exciton resonance of layered GaSe crystals

Light absorption in the region of exciton resonance of GaSe crystal is studied experimentally at high levels of optical excitation. A picosecond YAG:Nd³⁺ laser emitting 30-ps light pulses and a dye laser with a pulse width of ～3 ns tunable within the range 594–643 nm were used as light sources. It was found that, at high levels of optical excitation, the exciton absorption line of the GaSe crystal disappeared, which was attributed to increasing exciton density with arising mechanisms of their decay: exciton-exciton interactions and screening of excitons by the free charge-carrier plasma. It is shown that these mechanisms are also responsible for the arising new emission band in the long-wavelength region of the photoluminescence spectrum.     

Optical properties of ultrathin PbI2 microcrystallite in polymer

We have prepared PbI₂ microcrystallites embedded in polymer, which have a layer structure and are ultrathin crystals consisting of two to nine monolayers.

A very large energy shift of the exciton absorption band has been observed in these microcrystallites and interpreted in terms of size confinement of the translational motion of excitons in the c-direction perpendicular to the crystal surface. The simple effective mass approximation is broken down in 2, 3, 4 layer crystallites, because the crystal thickness is smaller compared to the exciton Bohr radius.

Secondly, in the Raman spectrum where the excitation energy is resonant to the exciton energy, there appears a new line in the energy region below 20cm⁻¹ which is characteristic of a ultrathin crystal. The Raman shift increases with decreasing the crystal thickness. This line is assigned as due to a longitudinal mode of a rigid-layer phonon.

Thirdly, the confinement of the internal motion is studied by measuring a diamagnetic shift of the exciton energy in the magnetic field up to 150 T and a bound exciton luminescence in the ultrathin microcrystallites. Much larger binding energy of the exciton compared to the bulk value is estimated. This fact suggests that the envelope function of the exciton shrinks not only by a strong spacial restriction in the c-direction but also by the dielectric screening from the surrounding polymer.

Fourthly, the exciton-phonon interaction is studied by the hole-burning measurement. From the temperature dependence of the hole width, it is suggested that the exciton is scattered by impurities or defects below 40 K and by a LO phonon above 40 K.

Finally, the hydrostatic pressure dependence of the exciton energy and the resonant Raman scattering in the energy region of the optical phonons have been measured and the size effect on the atomic bonding between I and Pb is discussed. It is concluded that covalent bonding between Pb and I atoms changes to ionic bonding in the ultrathin crystallites.     

GaAs/AlGaAs异质结的界面束缚二维激子效应

本文讨论了GaAs/AlGaAs异质结界面的H线发光及其性能。用双晶X射线衍射及皮秒光致发光证明了H线与界面质量密切相关,并且有相似于激子跃迁的寿命行为。用限制于异质结界面势阱的二维电子(或空穴)与分布于GaAs边的三维空穴(或电子)组成的二维激子效应,解释了H线的实验结果。并讨论了不同外延生长的异质结与界面有关的发光行为。     

CdS单晶中的绿色电致发光和光致发光

在50-290K温度范围内,研究了在正向电压激发下,用高纯CdS单晶制备的MIS发光二极管的电致发光光谱。在室温时,发射光谱分别由峰值为5135±25Å和5300±15Å的二个绿色谱带所组成,而在低温下,观测到有很多结构的光谱。在50K时,自由和束缚激子的发射实际上占有统治地位。文中提出,在室温时,谱峰为5135±25Å的谱带是与受导带自由电子散射的自由激子的发射有关;而谱峰为5300±15Å的谱带归结为与同时发射二个纵光学声子的自由激子的发射有关。比较了刚生长的高阻CdS单晶以及在熔融镉中热处理的低阻CdS单晶的光致发光光谱。在熔融镉中的热处理抑制了自由到束缚(HES)和束缚到束缚(LES)的边缘发射,也抑制了I2束缚激子谱线,但是增强了自由激子的发射,在电场激发下,也使自由激子的发射增强。     

Charged many-particle complexes: Properties of an indirect trion

A system of spatially separated interacting excitons and electrons is considered. The formation of a spatially indirect trion in this system is investigated. The asymptotic behavior of the binding energy of this charged many-particle complex is determined in the limits of large and small layer separations. The variation of the binding energy due to screening by the 2D electron gas is calculated. The bound state of the spatially separated exciton and electron is shown to disappear from the collective excitation spectrum at a certain threshold concentration of 2D electrons.     

Das Energiespektrum und die mittlere freie Bahn der deformierenden Excitonen in Molekularkristallen

A study is made of the energy spectrum of a deforming exciton and its temperature dependence in molecular crystals. The mean free path and diffusion coefficient of the deforming exciton with respect to multi-phonon collisions with crystal lattice vibrations are theoretically determined. The possibility of distinguishing the propagation of excitation in molecular crystals in the form of deforming excitons from that in the form of non-deforming excitons and from the propagation of excitation by random jumps from one molecule to another is discussed on the basis of the theoretically derived temperature dependence of the diffusion coefficient of the deforming exciton.     

Excitonic excitation spectra in ZnS: Cl crystal under pressure

The 3363 Å peak in the excitation spectrum of the S-A luminescence in the ZnS:Mn Cl cubic crystal at R.T. is ascribed to the A exciton. Its pressure coefficient is found as 6.4±0.2 meV/kbar, close to ρ = 6.3±0.2 meV/kbar reported for the gap in ZnS cubic crystal from the reflectivity measurements. This peak decreases by cooling and has not been observed at 85 K. The uv-excitation of the Mn-luminescence at R.T. is due to the energy transfer from the S-A to the Mn²⁺ centers, whereas the excitation peak at the exciton energy at 85 K comes from the excitation of the Mn²⁺ centers by the recombination energy of the Mn²⁺ bound excitons.     

Excitons in monoclinic zinc diphosphide: Orthoexciton and polariton effects at n=1 resonance

Quantitative investigations of the hydrogen-like exciton B series in the absorption spectra of the β-ZnP₂ crystal for various wave vector directions and polarization states of radiation are conducted. It is shown that the B spectrum constitutes a single orthoexciton series with S-type envelope functions, and low-energy components in doublet lines belong to the S-type for lines in the series with n≥3. Polariton effects are clearly manifested at the B _n=1 exciton resonance, and Bouguer’s law is violated. The oscillator strength tensor components are determined for transitions to the exciton states of the B series, and the polariton parameters at the B _n=1 exciton resonance are calculated.     

Collective excitations in molecular complexes

Green's functions are used to derive an equation for the energies of collective excitations in molecular complexes. It is found that the collective branch contains a solution of exciton type. An expression is derived for the energies of the exciton excitations.     

Free exciton luminescence lineshape of Hg0.3Cd0.7Te

The photoluminescence spectrum of Hg_0.3Cd_0.7Te at 77K includes a narrow, high energy free exciton line. This experimental spectrum is in good agreement with the theoretical free exciton lineshape, the Gaussian broadening of this line is due to alloy inhomogeneity, and the binding energy of the bound exciton with respect to the free exciton at 77K is 13 ± 4 meV.     

Optical bistability of a layered semiconductor in the exciton absorption region

The effect of specific features of the exciton and phonon spectra of layered semiconductors on the conditions of realization of optical bistability in the exciton absorption region has been theoretically investigated by the Green’s function method. By the example of the 2H polytype of PbI₂, it is shown that effective exciton scattering from low-energy bending-wave vibrations leads to a blue shift of the frequency range of bistability realization and its narrowing; expansion of the temperature range of bistability observation; and a shift of the hysteresis loop to higher intensities, accompanied by a decrease in its height and width. The possibility of observing polarization optical bistability, which is related to the dependence of the exciton energy spectrum on the propagation direction of a light wave in a crystal, is also substantiated.     

两种谐振腔长度的微腔有机电致发光器件模拟

微腔的谐振腔长度直接影响微腔有机电致发光器件(MOLED)的发光特性,根据微腔器件的相关计算公式运用传输矩阵法,分别对微腔长度L=λ/2和L=λ(λ:中心波长)时,在微腔内不同位置激子复合发光的电致发光谱(EL)进行模拟计算和比较。发现:微腔长度为L=λ/2时,峰值均为520nm,半峰全宽均为17nm,激子处在微腔的中心位置时,峰值强度和积分强度均为最大。L=λ时,激子在腔内不同位置时,峰值均为520nm,半峰全宽均12nm,在腔的中心区域时,与L=λ/2时正好相反,峰值强度和积分强度最小。分析后判断是因为两种长度的微腔内电场强度分布不同,激子位于腔内电场的最大值处发光性能最好。说明要制作出高效率的MOLED,要区别不同谐振腔长度,并使激子处于腔内电场最大处。     

Reflection spectra of orthorhombic indium iodide

The reflection spectra of InI single crystal have been measured using linearly polarized light. Pronounced anisotropy is observed between two directions of polarization E ∥ c and E ∥ a. The first peak at 2.018 eV for E ∥ c is direct allowed exciton transition with binding energy 4.3 meV. The E ∥ a spectrum suggests that the transition is forbidden.     

Photocurrent-action spectrum of anthracene: Tetracene mixed crystal

The photocurrent-action spectrum of an anthracene crystal doped with tetracene (in a concentration of 10^?5) exhibits the tetracene singlet exciton absorption spectrum. The two Davydov components of the first excited state are found at 2.39 and 2.47 eV. The charge carrier generation process involves intersystem crossing from guest to host resulting in anthracene triplet excitons and hole detrapping in the host lattice. A lower limit of the intersystem crossing rate k_isc = 3 × 10⁴sec^?1 is determined from the ratio of photocurrents in the guest and host absorption regions.