Study of absorption spectrum and dynamics evaluation of the indocyanine‐green first singlet excited state

Excited state absorption and excited state dynamics of indocyanine‐green (ICG) dissolved in dymethyl sulfoxide were measured using white‐light continuum Z‐scan (WLCZScan) and white‐light continuum pump–probe (WLCPP) techniques. The excited state absorption spectrum, obtained through Z‐scan measurements, revealed saturable absorption (SA) for wavelengths longer than 630 nm, while reverse saturable absorption (RSA) appeared, as indicated by a band at approximately 570 nm. Both processes were modeled by a three‐energy‐level diagram, from which the excited state cross‐section values were determined. SA and RSA were also observed in pump–probe experiments, with a recovery time in the hundreds of picoseconds time scale due to the long lifetime of the first excited state of ICG. Such results contribute to the understanding of ICG optical properties, allowing application in photonics and medicine. Copyright © 2010 John Wiley & Sons, Ltd.     

Excited state absorption of 1,3,3,1′,3′,3′-hexamethylindotricarbocyanine Iodide: A quantitative study by ultrafast absorption spectroscopy

A quantitative investigation of HITC dissolved in methanol has been made using the method of ultrafast absorption spectroscopy with a streak camera. Samples were excited by picosecond pulses of a mode-locked ruby laser. Analysis of time-resolved spectra yielded non-exponential decay kinetics consisting of a fast (τ variable) and a slow (τ=1.13±0.08 ns) component. The excited state absorption spectrum has its maximum at 493 nm and shoulders at 415 and 540 nm. The excited state absorption cross section was determined by simulataneous measurement of the bleaching of ground state absorption taking polarization of excitation and probe light and excited state absorption at the laser wavelength into account. A value of σ₁ (493 nm)=1.0·10^?16 cm² was found.     

Thermionic detection of the ionic fragments of continuum-state pair absorption systems

Using a thermionic diode we have detected the ionic fragments formed by associative ionization and dissociation after continuum-state pair absorption processes in Cs-Cs and Cs-K systems. Assuming an ionization probability of unity of the excited species and calibrating the pair absorption bands by taking into account the known photoionization cross section of the atoms we found excellent agreement with data from classical absorption measurements.     

Light absorption and excitation energy transfer calculations in primitive photosynthetic bacteria

In photosynthetic organisms, light energy is converted into chemical energy through the light absorption and excitation energy transfer (EET) processes. These processes start in light-harvesting complexes, which contain special photosynthetic pigments. The exploration of unique mechanisms in light-harvesting complexes is directly related to studies, such as artificial photosynthesis or biosignatures in astrobiology. We examined, through ab initio calculations, the light absorption and EET processes using cluster models of light-harvesting complexes in purple bacteria (LH2). We evaluated absorption spectra and energy transfer rates using the LH2 monomer and dimer models to reproduce experimental results. After the calibration tests, a LH2 aggregation model, composed of 7 or 19 LH2s aligned in triangle lattice, was examined. We found that the light absorption is red shifted and the energy transfer becomes faster as the system size increases. We also found that EET is accelerated by exchanging the central pigments to lower energy excited pigments. As an astrobiological application, we calculated light absorptions efficiencies of the LH2 in different photoenvironments.     

Intrasubband light absorption in a parabolic quantum well with consideration of scattering on the three-dimensional optical phonons

Within the frameworks of the second order perturbation theory the light absorption by free carriers in a parabolic quantum well (QW) is investigated taking into account the scattering by the three-dimensional optical phonons. An analytical expression for the absorption coefficient is obtained taking into the consideration two processes, with initial absorption of a photon and further scattering by optical phonons, and with the initial scattering by the optical phonons and the subsequent absorption of the photon. Frequency characteristics and dependences on the temperature and the width of QW are examined.     

Free-carrier absorption in a parabolic quantum well with consideration of scattering on ionized impurities

Intra-subband transitions caused by light absorption in a parabolic quantum well is considered taking into account the scattering by ionized impurity centers. To calculate the scattering matrix element, the Born approximation is used and the interaction with the impurity is described by the Coulomb potential. An analytical expression for the absorption coefficient of processes with the initial absorption of photon and further scattering by an ionized impurity center is obtained. For absorption coefficient the frequency characteristics and dependence on the width of quantum well are examined.     

Absorptionsspektroskopie angeregter Cäsiumatome

Cesium atoms, enclosed in a glass vessel, are excited by a weak electrical discharge and irradiated by monochromatic light with wavelengths corresponding to the sharp, diffuse, and fundamental series. By light absorption, highly excited atoms are produced, which are ionized by electron collisions. These ions diffuse into the space charge region of a diode path, compensate partially the space charge, and increase the thermionic diode current. By this method, ionic currents of about 10 ions per sec can be detected. If the wavelength of the incident light is varied continuously, the complete absorption spectrum of excited cesium atoms can be found in the recorded diode current.     

染料分子电子激发态振动失相过程的非相干光时延四波混频研究

本文对噁嗪(Oxagine)、甲酚紫(cresyl violet)染料分子的吸收带和吸收边进行了非相干光时延四波混频(TDFWM-IL)的详细研究,得到了有关失相参量的数据,并利用非相干光时延四渡混频的多能理论解释了实验结果和失相参量的物理意义。     

Characterization of nonlinear optical parameters of polymethine dyes

We investigated nonlinear refraction, nonlinear absorption, and saturable absorption of polymethine dyes by the Z-scan technique (λ=1064 nm). The analysis of simultaneous appearance of several nonlinear optical processes in dye solutions excited by picosecond pulses was carried out. The saturable absorption was analyzed taking into account various models. Nonlinear refractive indices, nonlinear absorption coefficients, and saturation intensities of various polymethine dyes were measured. Received: 27 December 2002 / Revised version: 6 March 2003 / Published online: 5 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-471/363-366, E-mail: r_ganeev@issp.u-tokyo.ac.jp RID="**" ID="**"Present address: The Institute for Solid State Physics, The Tokyo University, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan     

Large index of refraction without absorption via decay-induced coherence in a three-level V system

We study the effects of quantum interference from spontaneous emission on the dispersion-absorption properties in a three-level V-type atomic system with two near-degenerate excited levels. We found that due to the quantum interference between two spontaneous decay channels, large index of refraction without absorption always can be obtained just by choosing proper values of the relative phase between the two applied fields.Received: 27 February 2004, Published online: 26 May 2004PACS: 42.50.Gy Effects of atomic coherence on propagation, absorption, and amplification of light; electromagnetically induced transparency and absorption - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift     

Energy spectrum and optical absorption in p-CdGeAs2

In the Kein four-band model, taking account of interaction with excited bands, the energy spectrum and effective masses of electrons and holes in CdGeAs₂ are calculated. The polarizational dependence of the optical absorption spectrum is investigated for transitions between bands of light and heavy holes. The results are compared with experimental data.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 1, pp. 68–72, January, 1982.     

Theoretical investigation of amplified spontaneous emission with picosecond light pulses in dye solutions

The amplified spontaneous emission in dye solutions excited with intense picosecond light pulses is studied theoretically. A multi-level model is applied to take into account the effects of the various dye parameters such as ground-state absorption, stimulated emission, excited-state absorption, reabsorption and relaxations from populated excited levels. The influence of the pump laser duration and intensity and of the dye concentration and sample length is investigated. Optimum situations are derived for the generation of intense picosecond light pulses at new frequencies by amplified spontaneous emission. On the other hand, conditions are found where amplification of spontaneous emission may be neglected. The analysis allows the determination of unknown dye parameters by comparing the calculations with the experiment.     

Electronic structure and energy relaxation in strained InAs/GaAs quantum pyramids

We perform experimental and theoretical studies of the electronic structure and relaxation processes in pyramid shaped InAs/GaAs quantum dots (QDs), grown by molecular beam epitaxy in the Stranski-Krastanow growth mode. Structural properties are characterized with plan view and cross section transmission electron microscopy.Finite difference calculations of the strain and the 3D Schrödinger equation, taking into account piezoelectric and excitonic effects, agree with experimental results on transition energies of ground and excited states, revealed in luminescence and absorption spectra. We find as relative standard deviation of the size fluctuation ξ=0.04; the pyramid shape fluctuates between {101} and {203} side facets.Carrier capture into the QD ground state after carrier excitation above barrier is a very efficient process. No luminescence from excited states is observed at low excitation density. Energy relaxation processes in the zero-dimensional energy states are found to be dominated by phonon energy selection rules. However, multi-phonon emission (involving GaAs barrier, InAs wetting layer, InAs QD and interface modes) allows for a large variety of relaxation channels and thus a phonon bottleneck effect does not exist here.     

CdSe/ZnS核-壳结构量子点的非线性光学吸收

利用开孔Z扫描技术研究了吸收峰分别为553 nm和503 nm的两种尺寸CdSe/ZnS核-壳结构量子点溶液的非线性吸收性质.对于532 nm,6 ns激光脉冲,两种材料均表现出饱和吸收向反饱和吸收转化的现象.数值模拟结果表明：当吸收峰波长大于激光波长时,饱和吸收过程由快、慢两种机制组成,分别对应基态载流子被激发至不同的激发态,而强光下的反饱和吸收与快过程相关;当吸收峰波长小于激光波长时,饱和吸收主要由快过程机制引起,强光下的反饱和吸收源自激发态吸收和双光子吸收.我们的研究结果表明半导体量子点是研制光开关和光限制器件的理想候选材料.     

Tracking the relaxation pathway of photo-excited electrons in 1T-TiSe2

The ultrafast dynamics of excited electrons in 1T-TiSe₂ after absorption of a 390 nm light pulse is probed by time- and angle-resolved photoemission spectroscopy using femtosecond XUV pulses. It is demonstrated that the experimental approach can provide a comprehensive view of hot carrier motion in momentum space during relaxation back to equilibrium. This capability opens a new avenue in the investigation of energy dissipation processes in solids after intense optical excitation.     

Resonance-Raman-induced Kerr effect in molecules in the ground and electronically excited states

A theoretical investigation of the resonantly enhanced, Raman-induced Kerr effect (resonance-RIKE) is given, taking into account the resonance absorption of the laser wave and the population of excited electronic states. Line shape, maximum amplification and optimum conditions for the resonance-RIKE from the ground state as well as for the resonance-RIKE from an initial excited electronic state are discussed in detail. The possibility is studied of applying this method to the investigation of the vibrational structure of excited electronic states in molecules.     

利用原子的塞曼光谱对半导体激光器进行稳频

中性原子的超精细能级在磁场中产生塞曼分裂 ,另外 ,左旋和右旋圆偏振光激发下原子的跃迁选择定则不同 ,因此 ,原子在超精细塞曼能级间的吸收谱峰相对无磁场条件下的吸收谱峰有一定的移动。利用这一点 ,验证了一种简单、灵活的方法对半导体激光器进行稳频 ,使激光器的线宽稳到小于 1MHz。通过对实验结果的分析 ,发现由左旋和右旋圆偏振光激发引起的原子吸收谱峰移动之和与饱和吸收峰半高宽相等时 ,稳频效果最好     

Luminescence of lithium hydride crystal induced by UV-light

Emission and excitation spectra of a lithium hydride crystal were measured at 8 K. The emission bands at 3.65 and 2.7 eV were excited by the light above the absorption edge at 4.8 eV. The high energy emission at 4.6 eV was excited by the light above 6.0 eV. The emissions correspond to those from the relaxed exciton in alkali halides.     

Optical properties in photoelectron diffraction theory

Photoelectron diffraction effects may be strongly influenced by optical properties of the solid. Due to refraction and absorption of light at a surface, the state of polarization of light may be changed and, therefore, the corresponding photoelectron diffraction intensity. In order to include optical properties of solids in photoelectron diffraction theory, a general polarization vector of light is defined taking into account both refraction and absorption of light at the vacuum–solid boundary. In a first step, the radiation field of light inside the solid is approximated macroscopically according to classical electrodynamics. Analytical expressions are derived within a real-angle representation of Fresnel equations to reveal the influence of refraction and absorption of light on the state of polarization of light. A general refractive index in dependence on the incident angle of light is introduced which determines the refractive angle inside the solid (refraction law with real angles) and the order of influence of absorption of light. The general polarization vector is applied in the calculation of dipole transition matrix elements in a multiple-scattering cluster model of photoelectron diffraction, where the process of photoabsorption (dipole transition matrix element) and multiple scattering processes of photoelectrons (scattering path operator) are considered separately. Different analytical and numerical results of photoelectron diffraction effects are presented for light of general polarization incident at general angles taking into account the optical properties of the solid. Examples are shown and discussed in detail for Cu(001) and GaAs(110) surfaces.