Emergence of spectral line jumps and spectral diffusion in the two-photon correlator of a single impurity center

A dynamic theory of two-photon correlators for a single impurity center developed recently by the author [I. S. Osad’ko, Zh. éksp. Teor. Fiz. 113, 1606 (1998) [JETP 86, 875 (1998)] has been generalized to the case in which the center interacts with nonequilibrium two-level systems (TLSs) in polymers and glasses. Quantum tunneling transitions in TLS manifest themselves as random jumps of a spectral line of an impurity center. These jumps can be either spontaneous or light-induced. Interaction between the impurity center and many nonequilibrium TLSs, which exist in polymers, results in a time dependence of the optical dephasing rate 1/T ₂ of an impurity molecule, i.e., in spectral diffusion. This paper describes how the jumps of the spectral line manifest themselves in the two-photon correlator, which can be measured in experiments. Zh. éksp. Teor. Fiz. 116, 962–985 (September 1999)     

Peculiarities of two-photon impurity absorption spectra in a quantum molecule with a tunnel-transparent potential barrier

The effect of dissipative tunneling parameters on the spectral dependence of the probability of two-photon impurity absorption in a quantum molecule is theoretically investigated. The effect of the tunnel barrier transparency on two-photon impurity absorption in a quantum molecule is shown to manifest itself as a change in the width of energy levels of the virtual and final states due to variations in such parameters of dissipative tunneling as temperature, photon-mode frequency, and the constant of interaction with a heat bath.     

Resonant two-photon absorption in ZnSiP2

The complex of optical investigations into the intrinsic (I) and resonant (R) two-photon absorption (TPA) inZnSiP ₂ crystals of tetragonal modifications is performed by methods of amplitude laser-modulation spectroscopy. The ITPA of allowed-forbidden type and the two Lorentz spectral lines associated with coherent resonant two-photon transitions through impurity states of allowed-allowed type are found. The electron transverse relaxation time at the RTPA is determined, and the total absorption cross section of laser-radiation photons emitted at electron transitions between the valence band v, the conduction band c, and local centers that produce real states intermediate for the RTPA in the forbidden band is estimated. M. P. Dragomanov National Pedagogical University. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 2, pp. 36–43, February, 2000.     

Nonresonant two-photon generation of excitonic matter in a CuCl pellet

A pressed CuCl pellet is optically excited at 2 K using an excitation energy in the range from 1892 to 2843 meV, which is far below the bandgap. The steady-state population dynamics unambiguously indicates an unusual two-photon generation of ground-state excitons. At high-excitation levels, the observed spectra exhibit rich spectral features arising from electron-hole plasma and electron-hole droplets formation. This nonresonant two-photon excitation is presumably assisted by impurity bands due to grain boundaries and surfaces in this random semiconductor.     

Two-Photon Absorption in Nanoheterostructures with <Emphasis Type="Italic">D</Emphasis><Superscript>(−)</Superscript>-Centers

A two-photon impurity absorption coefficient of the “quantum dot — D⁽⁻⁾-center” complexes synthesized in a transparent dielectric matrix is calculated within the model of zero-radius potential. The evolution of spectral dependence of the absorption coefficient of the nanoheterostructure based on semiconductor CdS _x Se _1−x glasses is studied versus the average quantum-dot radius. It is shown that the contribution of the two-photon impurity absorption to the exited two-photon luminescence is fairly significant at a reasonable quantum-dot concentration. __________ Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 7, pp. 46–50, July, 2005.     

Some simple mechanisms of multiphoton excitation in many-level systems

Results are reported on coherent monochromatic multiphoton excitation in many-level systems, which are representative for some of the basic mechanisms for atomic and molecular multiphoton processes. Numerical solutions are discussed that use the Floquet and quasi-resonant approximations in the framework of the URIMIR program package. The excitation schemes include direct three-photon excitation, two-photon excitation with diagonal coupling, Göppert-Mayer-type two-photon processes, multiphoton excitation with off-resonant inter-mediates, and practically irreversible coherent excitation into dense spectral structures. Several interesting phenomena are observed, such as nonlinear line shifts and broadenings of multi-photon resonances of relevance for multiphoton spectroscopy and almost constant intermediate population inversions, potentially useful for laser design. The accurate numerical results are compared with approximate solutions from perturbation theory, and with simple analytical solutions from Rabi-type formulae.     

Two-photon confocal microscopy in the study of the volume characteristics of semiconductors

Zn–Se crystals are used to analyze prospects for application of two-photon confocal microscopy in the study of plane and volume interband and impurity luminescence in semiconductors. Such maps can be formed with a depth step and planar spatial resolution of several micrometers at distances of up to 1 mm from the surface. The method is used to detect luminescence-active inhomogeneities in crystals and study their structure and luminescence characteristics. Prospects for the application of the two-photon confocal microscopy in the study of direct-band-semiconductors and materials of the fourth group are discussed.     

76500～81120cm~(-1)范围内碘甲烷分子的双光子电离光谱

在离子速度成像的实验装置中,将波长为492~523 nm范围内的激光倍频,以经过倍频的激光作光源,将碘甲烷分子(CH3I)电离,获得了碘甲烷母体分子离子(CH3I+)在76 500~81 120 cm-1范围内的高分辨双光子电离光谱;介绍了CH3I的双光子电离机制,根据Rydberg公式和量子数亏损成功对实验所得到的CH3I+谱中的46个谱峰做了标识,并观察到了CH3I+谱中p,d,f系列的能级分裂。标识结果表明,在CH3I的双光子电离谱中除了可以观察到单光子电离谱的特征,还可以观察到在单光子电离中禁阻的f系列跃迁。     

Statistical analysis of spectra of single impurity molecules and dynamics of disordered solids: I. Distributions of linewidths,moments, and cumulants

A review of recent results of studying the low-temperature dynamics of a disordered solid-state medium that were obtained by the method of single molecule spectroscopy (SMS) is presented. The studies were carried out with the use of the new approach of the statistical analysis of a large number of spectra of single molecules embedded into a medium under study as a microscopic spectral probe. The measurements were performed in the range 2–7 K. The use of SMS allowed us to avoid the information losses connected with the averaging over an ensemble of impurity molecules that is inherent in conventional spectral methods. For the example of the system studied (amorphous polyisobutylene doped with molecules of tetra-tert-butylterrylene), it was shown experimentally that, at low temperatures, the spectra of single impurity molecules in disordered media obey the Levy statistics. New microscopic information on the interaction of two-level systems and quasi-local low-frequency vibrational modes of the matrix with impurity molecules in a disordered medium was obtained.     

Two- and three-photon excitation of Gd in CaAl12O19

We have employed two-photon excitation to study the higher energy levels of Gd³⁺ ions in CaAl₁₂O₁₉ and we compare the results with those obtained using conventional UV excitation techniques. Under two-photon excitation, the luminescence intensity exhibits an unusual temporal behavior, a very long build-up followed by a decrease by orders of magnitude, ascribed to a recombination-assisted luminescence excitation mechanism assuming photo-ionization of Gd³⁺ ions and trapping of free electrons on deep traps.

We also find that the two-photon excitation spectra contain an additional broadening contribution which can be attributed to homogeneous broadening of excitation levels caused by excited state absorption into the conduction band. We believe that this may be a general phenomenon whenever participating photons produce ionization of impurity ions from metastable excited states. The phenomenon can manifest itself also in two-photon ionization spectral hole burning and in up-conversion processes (in the latter case, the homogeneous broadening can be caused by an intra-ion excited-state absorption).     

Two photon absorption and coherent control with broadband down-converted light

We experimentally demonstrate two-photon absorption with broadband down-converted light (squeezed vacuum). Although incoherent and exhibiting the statistics of a thermal noise, broadband down-converted light can induce two-photon absorption with the same sharp temporal behavior as femtosecond pulses, while exhibiting the high spectral resolution of the narrow band pump laser. Using pulse-shaping methods, we coherently control two-photon absorption in rubidium, demonstrating spectral and temporal resolutions that are 3-5 orders of magnitude below the actual bandwidth and temporal duration of the light itself. Such properties can be exploited in various applications such as spread-spectrum optical communications, tomography, and nonlinear microscopy.     

天然FeS2(黄铁矿)的红外光谱研究

主要报道天然FeS₂黄铁矿,(以下称FeS₂(P))的室温、低温的远红外反射光谱和透射光谱,并对其光谱结构及物理起源作了较详细的讨论。通过我们的研究发现:室温反射光谱低频端等离子体反射边和样品中所含的PbS(方铅矿)杂技存在密切的联系。我们以FeS₂(P)矿物单晶和PbS矿物单晶的反射光谱作为基谱对不同样品的实验结果进行了复合,所得出的x值不仅可以反映PbS杂质的含量,而且间接地与贵金属元素Au等存在较好的正相关性。这对于研究矿物的成因等有 关键词：     

Dynamic theory of two-photon correlators in the spectroscopy of single impurity centers

A dynamic theory of two-photon correlators measured in experiments with single molecular impurity centers has been developed. The theory takes into account the interaction between optically active electrons of an impurity center and phonons, excitations in tunneling systems of polymers and glasses, and transverse electromagnetic field. Both the correlator measured in the start-stop regime and the “full” correlator have been analyzed, and equations for these correlators have been derived. An equation relating these two correlators has been also obtained. The effect of the triplet level of an impurity molecule on the correlators leading to bunching of spontaneously emitted photons has been studied. The two-photon correlators have been calculated numerically, and their dependence on the incident light frequency and time between the pairs of detected photons in various realistic situations has been derived. Zh. éksp. Teor. Fiz. 113, 1606–1631 (May 1998)     

A polarization method for measuring absorption spectra of single molecules

A new method for measuring low-temperature absorption spectra of single impurity molecules using a laser confocal polarized-light transmission microscope is proposed. The sensitivity of this method is of the same order of magnitude as that of fluorescence excitation spectroscopy. Combined use of both methods makes it possible to study distributions of impurity molecules by the magnitude of fluorescence quantum yield and their correlations with the linewidth distributions, as well as to determine if spectral jumps lead to changes in the fluorescence quantum yield.     

Interferometric Hetero-Detector Phase Measurement

We present a new method for the measurement of the phase of ultrashort optical pulses with high spectral resolution. This employs an interferometer with a monochromator in one arm. Two detectors operating in single photon and two-photon absorption regimes monitor the output from the interferometer. Comparison of the signals from the two detectors gives a measurement of the phase of the light pulse. The principles underpinning this technique are discussed and the experimental application to picosecond pulses is demonstrated.     

飞秒激光双光子微细加工技术及研究现状

飞秒激光双光子微细加工技术以其特有的高精度三维微加工优势,成为微型机械加工领域新的发展方向之一。介绍了飞秒激光双光子微细加工技术的原理和应用的现状。结合目前已有的微细加工技术,对双光子微细加工技术的特点加以评述。简要报道了利用飞秒激光双光子微细加工技术的一些研究进展。探讨了飞秒激光双光子微细加工技术今后的发展方向及其存在的基本问题。     

靶材料杂质影响新谱线产生的实验验证

 为了验证氢气放电源打靶产生的新谱线不是靶杂质的特征谱线,完成了5项检验实验。其中屏蔽实验和强电子辐照靶的实验证实了新谱线不是来自放电室中的杂质形成的;靶的打磨实验表明靶表面的污染杂质也不能产生新谱线,形成共振峰的实验和新谱线强度随放电电压变化规律的实验结果都证明靶的总杂质不影响新谱线的测量。     

Polarization and phase control of two-photon absorption in an isotropic molecular system

<正>We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system.We theoretically show that the two-photon transition probability decreases when the laser polarization changes from linear through elliptical to circular,and the laser polarization does not affect the control efficiency of two-photon transition probability by shaping the spectral phase.These theoretical results are experimentally confirmed in coumarin 480.Furthermore,we propose that the combination of the laser polarization with the spectral phase modulation can further increase the control efficiency of the two-photon absorption.     

Optical Two-Photon Surface Nonlinear Waves

A theory of the optical surface two-photon small-amplitude breather in a multilayer system of the isotropic and anisotropic left-hand metamaterials, when there are a graphene monolayer (graphene-like twodimensional material) and a transition layer with impurity optical atoms (semiconductor quantum dots), is constructed. It is shown that the system of constitutive equations for two-photon transitions and wave equation for a surface plasmon–polariton TM mode are reduced to the nonlinear Schrödinger equation with damping. Explicit analytical expressions for a surface two-photon small-amplitude self-induced transparency breather (0π-pulse) are obtained. It is shown that the optical conductivity of graphene leads to the exponential damping of intensity of a surface two-photon nonlinear wave during the propagation. One- and two-photon small-amplitude breathers in graphene are compared, and it is shown that differences between their parameters are substantial.     

Effects of phosphorus-doping upon the electronic structures of single wall carbon nanotubes

The phosphorus-doped single wall carbon nanotube (PSWCNT) is studied by using First-Principle methods based on Density Function Theory (DFT). The formation energy, total energy, band structure, geometry structure and density of states are calculated. It is found that the formation energy of the P-doped single carbon nanotubes increases with diameters; the total energy of carbon nanotubes with the same diameter decreases as the doping rate increases. The effects of impurity position on the impurity level are discussed. It illustrates that the position of the impurity level may depend on the C-P-C bond angle. According to the above results, it is feasible to substitute a carbon atom with a phosphorus atom in SWCNT. It is also found that P-doped carbon nanotubes are N type semiconductor. Supported by the Natural Science Foundation of Fujian Province of China (Grant No. A0220001)