Stimulated two-photon emission from excitonic molecules in ZnO

The M-band emission in ZnO at 1.7 K is investigated by tuning the excitation light through the A-B exciton region. Externally stimulated two-photon emission from excitonic molecules is observed when the pump photon energy is resonant with the upper B-polariton. The experiments suggest two excitonic molecule levels separated by 4.6 meV and with a ground state energy E_M = 6.7394 eV.     

Pico-second transient luminescence of resonantly excited excitonic molecules in CuCl

Time-resolved luminescence spectra of excitonic molecules in CuCl created by the two-photon resonance excitation are studied at 4.2 K with a time resolution of ～ 60 psec. Two sharp emission lines observed are ascribed to the radiative decay of “cold” excitonic molecules with k ～ 2K₀. Stimulated emission process gives a considerable influence on luminescence properties.     

Resonant Raman scattering of optical phonons in self-assembled quantum dots

We have investigated the carrier relaxation mechanism in InGaAs/GaAs quantum dots by photoluminescence excitation (PLE) spectroscopy. Near-field scanning optical microscope successfully shows that a PLE resonance at a relaxation energy of 36 meV can be seen in all single-dot luminescence spectra, and thus can be attributed to resonant Raman scattering by a GaAs LO phonon to the excitonic ground state. In addition, a number of sharp resonances observed in single-dot PLE spectra can be identified as resonant Raman features due to localized phonons, which are observed in the conventional Raman spectrum. The results reveal the mechanism for the efficient relaxation of carriers observed in self-assembled quantum dots: the carriers can relax within the continuum states, and make transitions to the excitonic ground state by phonon emission.     

Multi-polariton scattering via excitonic molecules

We develop the theory of multi-polariton scattering via excitonic molecules under strong excitation. New emission lines, denoted by X- and L-bands, were observed at slightly lower energy side of two-photon Raman line in CuCl under strong excitation. In terms of the present theory, these lines can be for the first time assigned to the multi-polariton scatterings associated with the coherently (virtually) and incoherently (realy) created excitonic molecules, respectively.     

Two-photon resonant Raman and luminescence of excitonic molecules in CuCl

Two-photon resonant Raman scattering via excitonic molecule in CuCl is studied with using dye laser excitation of different band widths. The yield of the Raman scattering is found to drop remarkably at resonant excitation and luminescence line of 0.3 meV half-width comes out. The predominance of the Raman or luminescence or their coexistence depends on the intensity and energy band width of excitation light.     

Observation of the Bose condensation of excitonic molecules in CdSe

It is observed that excitonic molecules in CdSe exhibit the Bose condensation when excitation is given at 1.8–4.2 K by pico-second light pulses from a mode-locked glass laser. Strong evidence is provided by the appearance of an extremely sharp luminescence line produced from the excitonic molecules condensed to the k = 0 state.     

KLL Auger resonant Raman transition in metallic Cu and Ni

High energy resolution KL₂₃L₂₃ Auger spectra of polycrystalline Cu and Ni were measured using photon energies up to about 50 eV above the K-absorption edge and down to 5 eV (Cu KLL) and 4 eV (Ni KLL) below threshold. The spectra show strong satellite structures varying considerably as a function of the photon energy. In the sub-threshold region the linear dispersion of the diagram line energy positions and a distortion of the line shape as a function of photon energy, attributable to the Auger resonant Raman process, is clearly observed, indicating the one-step nature of the Auger emission. These changes in the resonant spectra are interpreted using a simple model based on resonant scattering theory in combination with partial density of states obtained from cluster molecular orbital (DV-Xα) calculations.     

Pico-second spectroscopy of the secondary radiation from resonantly excited excitonic molecules in CuCl

Pico-second time-resolved measurements of the two-photon resonant Raman scattering via excitonic molecules in CuCl were carried out for the first time. The Raman scattering leaving transverse excitons decays as fast as the laser light. When the energy of the incident light falls in the vicinity of the two-photon resonant absorption, both Raman and luminescence lines are simultaneously observed. In case of just resonant excitation, the transient response indicates that the secondary radiation can be decomposed into the Raman and the luminescence components as regards its temporal and spectral behavior.     

Stimulated photoluminescence of ZnSe

The stimulated emission from ZnSe under one photon or two photon excitation has been investigated in the temperature range between 20 and 100 K. The spectra obtained under quasi-resonant one photon pumping show a dominant P line, ascribed to exciton-exciton scattering on the basis of its intensity dependence and its optical gain spectrum. The role of many-body processes under non-resonant one photon excitation is discussed. Under two photon pumping the LO-phonon assisted free exciton recombination is shown to be the dominant lasing mechanism.     

Near infrared to UV dielectric functions of Al doped ZnO films deposited on c-plane sapphire substrate using pulsed laser deposition

Transparent conducting polycrystalline Al-doped ZnO (AZO) films were deposited on sapphire substrates at substrate temperatures ranging from 200 to 300 °C by pulsed laser deposition (PLD). X-ray diffraction measurement shows that the crystalline quality of AZO films was improved with increased substrate temperature. The electrical and optical properties of the AZO films have been systematically studied via various experimental tools. The room-temperature micro-photoluminescence (µ-PL) spectra show a strong ultraviolet (UV) excitonic emission and weak deep-level emission, which indicate low structural defects in the films. A Raman shift of about 11 cm⁻¹ is observed for the first-order longitudinal-optical (LO) phonon peak for AZO films when compared to the LO phonon peak of bulk ZnO. The Raman spectra obtained with UV resonant excitation at room temperature show multi-phonon LO modes up to third order. Optical response due to free electrons of the AZO films was characterized in the photon energy range from 0.6 to 6.5 eV by spectroscopic ellipsometry (SE). The free electron response was expressed by a simple Drude model combined with the Cauchy model are reported.     

利用拉曼散射、共振拉曼散射及瑞利散射对ZnSe-ZnS多量子阱材料光谱的判定

利用拉曼散射、共振拉曼散射及瑞利散射对ＺｎＳｅ┐ＺｎＳ多量子阱材料光谱的判定赵福潭王淑梅苏锡安刘行仁（中国科学院激发态物理开放研究实验室长春１３００２１）ＤｉｓｔｉｎｇｕｉｓｈｉｎｇｏｆＬｕｍｉｎｅｓｃｅｎｃｅＳｐｅｃｔｒａｉｎＺｎＳｅ┐ＺｎＳＭＱＷ...     

Intra-center energy transfer dynamics in Cd1−xMnxTe semi magnetic semiconductors

Intra-center luminescence of Cd_1?xMn_xTe semi magnetic semiconductors under low excitation density was investigated both experimentally and by Monte-Carlo simulation. Experimental time-resolved spectra of 2 eV-band under different photon energy for excitation were used. The approach revealed that Mn²⁺–Mn²⁺excitation energy transfers take place by means of resonant dipole–dipole interaction. Besides energy transfer dynamics is strongly influenced by hopping-assisted quenching. Having been intra-center excitation selective-, mixed- and non-selective types of excitation are proved to occur if photon energy for excitation is increased. This is originated from overlapping of ⁴T₁- and ⁴T₂-states. Under inter-band excitation it was established that Mn²⁺-ion excitation takes place with the aid of excitonic energy transfer, with excitation energy being centered at exciton energy. Under temperature rise the transfer rate vigorously enhances due to great increase of overlap integral of Mn²⁺- ions' side-bands. The quenching is proved to be limited in accordance with existing theory. Inhomogeneous broadening diminishes as a result of fast fluctuation rate of excited ions' energy.     

Deep-ultraviolet near band-edge emissions from nano-polycrystalline diamond

ABSTRACT

Deep-ultraviolet continuous-wave photoluminescence spectroscopy is performed for nano-polycrystalline diamond (NPD) synthesized by a high pressure high-temperature technique. NPD exhibits clear deep-ultraviolet emissions, which originate from intrinsic excitonic transitions assisted by a momentum-conserving phonon with a photon. Surprisingly, the peak emission energy is about 30?meV higher than that of the single-crystalline diamond. Raman scattering spectroscopy indicates that the energy difference should originate from the excitonic properties of the NPD and not the phonon. Hence, NPD has a large bandgap compared to single-crystalline diamond.     

High intensity effect on two-photon resonant,coherent Raman scattering via excitonic molecules in CuCl and CuBr

Two-phonon resonant, coherent Raman scattering (four-photon degenerate coherent scattering) via excitonic molecules has been studied as a function of intensity of incident light in CuCl and CuBr. Observed line-shaped of coherent scattering spectra broadens as excitation intensity is raised. This broadening is found to be closely correlated with that of the two-photon absorption. These results are qualitatively explained by taking account of the excitation intensity-dependence of χ⁽³⁾, but cannot be explained by the autoinization model.     

Wavelength and concentration dependence of Raman scattering from CdS1−xSex

We present measurement of the resonant Raman effect in the alloy system CdS_1?xSe_x for laser photon energies both above and below the concentration-dependent energy gap. Our data show that the Raman intensities are not simply functions of the difference between the photon energy and the gap energy. These results may be partially understood in terms of a simple theoretical model which elucidates the role of local electric fields in determining Raman intensities in alloys.     

Exciton-phonon interaction in mixed silver halides: Resonant Raman scattering vs photoluminescence

An investigation of resonant Raman scattering in mixed crystals of AgBr:Cl at 1.8 K shows that the zero-phonon and LO phonon-assisted exciton luminescence excited in the free indirect exciton absorption, exhibits an anomalous dependence on the exciton photon energy E_L. Close to the exciton gap, the bands show a Raman-like behaviour with their peaks at constant energetic distance from E_L. As E_L is tuned further into the absorption, the bands gradually develop into normal photoluminescence. The effect is explained by taking into account exciton relaxation via scattering by long-wavelength acoustic phonons, a process which is strongly energy dependent. In addition, resonant Raman scattering observed for excitation in the zero-phonon absorption suggests study for the first time of the mode behaviour of certain off-zone center phonons in this system.     

Stimulated emission effects in excitonic molecule luminescence of CuCl under resonant two-photon excitation

Luminescence spectra of excitonic molecules in CuCl resonantly created by nano-second dye laser excitation are measured at 4.2 K changing the lenghts of the excited region. The spectra are dominated by stimulated emission. The gain coefficient for the M_T line is saturated more easily than that for M_L, though the former is larger under unsaturated conditions. These gain characteristics explain well various stimulated emission effects observed.     

Secondary emissions under two-photon resonance excitation of excitonic molecules in CuCl

The origin of the narrow secondary emission lines under two-photon just- resonance excitation of the excitonic molecule in CuCl is discussed. Luminescence due to cold, but not Bose-condensed excitonic molecules is concluded to be dominant. Recent experiments to discriminate between Raman scattering and luminescence by picosecond spectroscopy on these emissions are criticized.     

Excitation spectroscopy,Raman scattering and the temperature dependence of the luminescence in highly excited red HgI2

The luminescence of red HgI₂ is investigated as a function of temperature, excitation intensity and wavelength. At high excitation intensity and low temperature an “M-band” emission dominates. This M-band is assigned to biexciton decay and bound exciton scattering with acoustic phonons (“acoustic wing”), this assumption being supported by the results of excitation spectroscopy. The energy of the biexciton is determined to be (4661 ± 1) meV. From the evaluation of Raman spectra, the phonon energies (1.9, 3.1 and 14.0 ± 0.2) meV are found. At higher temperatures two lines are observed, one of which is ascribed to exciton-free carrier scattering. Position and line shape are in good agreement with theoretical results. The other emission line is found to be due to scattering involving excitons or carriers bound to lattice defects.     

Non-linear photo-induced desorption of GaP

Laser-induced desorption of P from GaP at various photon energies near the absorption edge has been measured. The desorption yield is found to start increasing above a certain threshold laser fluence, of which the dependence on the photon energy exhibits a sharp dip near the indirect band gap besides a gradually decreasing component from the indirect band gap to the direct band gap energy. The sharp dip is ascribed to desorption induced by dense excitation of the surface states.