A comparative study of the spectral and kinetic properties of photochromic derivatives of perfluorocyclopentene diarylethenes

A comparative spectral-kinetic study of the photochromism of a series of synthesized thienyl derivatives of perfluorocyclopentene dihetarylethenes is performed. A relation between the photochromic properties of these compounds (the absorption spectra of the initial and photoinduced forms, the photosensitivity, the interconversion constants of both forms, and the photodegradation) and their structure is established. For some compounds experiencing reversible and irreversible phototransformations, photoinduced fluorescence was observed. The data obtained give grounds to suggest that the compounds synthesized can be used in developing recording media for two-photon 3D main and archival storage.     

Ultrafast optical nonlinearity in the quasi-one-dimensional mott insulator Sr2CuO3

We report strong instantaneous photoinduced absorption in the quasi-one-dimensional Mott insulator Sr2CuO3 in the IR spectral region. The observed photoinduced absorption is to an even-parity two-photon state that occurs immediately above the absorption edge. Theoretical calculation based on a two-band extended Hubbard model explains the experimental features and indicates that the strong two-photon absorption is due to a very large dipole coupling between nearly degenerate one- and two-photon states. Room temperature picosecond recovery of the optical transparency suggests the strong potential of Sr2CuO3 for all-optical switching.     

Two-photon lasers based on intersubband transitions in semiconductor quantum wells

We propose to make a two-photon laser based on intersubband (sublevel) transitions in semiconductor nanostructures. The advantages and feasibility of such a two-photon laser are analyzed in detail using the density matrix approach. Both one-photon and two-photon gains in a three subband quantum well structure are studied on the same footing to show how the two-photon gain can be maximized, while the competing one-photon gain is minimized. The results show that a sufficient two-photon gain can be achieved to overcome one-photon competition and the loss of a conventional semiconductor cavity, making intersubband transitions one of the very few feasible approaches to two-photon lasing.     

Enhanced narrow spectral line and double electromagnetically induced two-photon transparency induced by double dark resonances

We theoretically investigate the features of two-photon absorption in a five-level atomic system with interacting dark resonances. It is found that two-photon absorption can be completely suppressed at two different frequencies due to the application of two coherent coupling fields and the atomic system exhibits double electromagnetically induced transparency windows against two-photon absorption. The position and width of the double two-photon transparency windows can be controlled via properly adjusting the frequency detuning and the intensities of the two coupling fields. In addition, one enhanced narrow central line can be observed in the two-photon absorption spectra, which may find applications in high-precision spectroscopy. Form a physical point of view, we explicitly explain these results in terms of quantum interference induced by three different two-photon excitation channels in the dressed-state picture.     

Two-photon absorption spectrum of the photoinitiator Lucirin TPO-L

Two-photon absorption induced polymerization provides a powerful method for the fabrication of intricate three-dimensional microstructures. Recently, Lucirin TPO-L was shown to be a photoinitiator with several advantageous properties for two-photon induced polymerization. Here we measure the two-photon absorption cross-section spectrum of Lucirin TPO-L, which presents a maximum of 1.2 GM at 610 nm. Despite its small two-photon absorption cross-section, it is possible to fabricate excellent microstructures by two-photon polymerization due to the high polymerization quantum yield of Lucirin TPO-L. These results indicate that optimization of the two-photon absorption cross-section is not the only material parameter to be considered when searching for new photoinitiators for microfabrication via two-photon absorption. PACS 42.65.-k; 78.40.Me; 42.70.Jk; 81.05.Lg     

强光场下非共振双光子跃迁相干控制

利用飞秒激光脉冲相位整形技术,从理论和实验两方面,对强激光场下分子体系苝溶液中非共振双光子跃迁的相干控制进行了研究。通过对飞秒激光脉冲进行相位扫描和余弦相位调制,发现分子体系中非共振双光子的跃迁几率能够被削弱,但不能完全消除。分子体系中非共振双光子跃迁的相干控制受到激光光场的形状和分子吸收谱谱宽的影响;与原子体系相比,分子体系中非共振双光子跃迁相干控制的调制效率降低。     

双光子失谐对慢光和光存储影响的实验研究

利用电磁感应透明(EIT)效应在87Rb热原子气室中进行了慢光和光存储的实验研究,在单光子红失谐650 MHz处测量了双光子失谐对光脉冲延迟和光存储的影响.结果表明:在双光子失谐0—0.5 MHz范围内存在显著的光脉冲延迟和光存储恢复信号,其慢光波形与理论计算结果基本相符;而恢复光脉冲信号随着双光子失谐的变化出现形变,这是由于多个EIT子系统之间的干涉引起的.这一研究结果为连续变量光场在热原子系综中的存储提供了实验参考.     

Properties of pulsed entangled two-photon fields

The dependence of one- and two-photon characteristics of pulsed entangled two-photon fields generated in spontaneous parametric down-conversion on the pump-pulse properties (shape of the pump-pulse spectrum and its internal structure) is examined. It is shown that entangled two-photon fields with defined properties can be generated. A general relation between the spectra of the down-converted fields is established. As a special case the interference of two partially overlapping pulsed two-photon fields is studied. The fourth-order interference pattern of entangled two-photon fields is investigated in the polarization analog of the Hong-Ou-Mandel interferometer. Received: 23 December 1998 / Received in final form: 14 April 1999     

On nonclassical effects in two-photon optical bistability and two-photon laser

We analyse the fluctuations at steady state in the good quality cavity case in two-photon lasers with running wave and two-photon absorptive optical bistability in a ring cavity. In the case of two-photon laser we do not find any nonclassical effect, contrary to expectations. On the other hand, in two-photon optical bistability we find squeezing and antibunching in the low transmission branch. The maximum reduction of fluctuations that can be obtained is slightly larger than by a factor of two.     

Two photon-induced fluorescence intensity and anisotropy decays of diphenylhexatriene in solvents and lipid bilayers

We measured the fluorescence intensity and anisotropy decays of 1,6-diphenyl-1,3,5-hexatriene (DPH)-labeled membranes resulting from simultaneous two-photon excitation of fluorescence. Comparison of these two-photon data with the more usual one-photon measurements revealed that DPH displayed identical intensity decays, anisotropy decays, and order parameters for one- and two-photon excitation. While the anisotropy data are numerically distinct, they can be compared by use of the factor 10/7, which accounts for the two-photon versus one-photon photoselection. The increased time 0 anisotropy of DPH can result in increased resolution of complex anisotropy decays. Global analysis of the one- and two-photon data reveals consistency with a single apparent angle between the absorption and the emission oscillators. The global anisotropy analysis also suggests that, except for the photoselection factor, the anisotropy decays are the same for one-and two-photon excitation. This ideal behavior of DPH as a two-photon absorber, and its high two-photon cross section, makes DPH a potential probe for confocal two-photon microscopy and other systems where it is advantageous to use long-wavelength (680- to 760-nm) excitation.     

Enhancing Parameter Estimation Precision in a Dissipative Environment with Two-Photon Driving

The frequency estimation of an optical cavity field suffering from an unavoidable dissipative environment is investigated. Generally, dissipative noise significantly reduces the precision. Here, it is found that two-photon driving can improve measurement precision by resisting the noise. Moreover, over a long duration, the frequency uncertainty can be minimized with the right magnitude of the parametric two-photon drive, which is in sharp contrast to the uncertainty tending to infinity without two-photon driving. The results show that two-photon driving can achieve ultrasensitive measurement in a dissipative environment under the long-encoding-time condition.     

Nonlinear spectrum effect on the coherent control of molecular systems

This work demonstrates that the detuning of the fs-laser spectrum from the two-photon absorption band of organic materials can be used to reach further control of the two-photon absorption by pulse spectral phase manipulation. We investigate the coherent control of the two-photon absorption in imidazole-thiophene core compounds presenting distinct two-photon absorption spectra. The coherent control, performed using pulse phase shaping and genetic algorithm, exhibited different growth rates for each sample. Such distinct trends were explained by calculating the two-photon absorption probability considering the intrapulse interference mechanism, taking into account the two-photon absorption spectrum of the samples. Our results indicate that tuning the relative position between the nonlinear absorption and the pulse spectrum can be used as a novel strategy to optimize the two-photon absorption in broadband molecular systems.     

Two-photon and two-photon-assisted slow light

We show that light pulses propagating in two-photon absorbing systems may present time delays like slow light produced via coherent population oscillations in one-photon interactions. Two regimes are numerically studied for a simplified two-level system: (a) a light pulse at frequency ω/2 undergoes two-photon absorption (TPA) and is delayed by the absorbing system (two-photon slow light) and (b) a light pulse at frequency ω is delayed in a system prepared by TPA of a light pulse at frequency ω/2 (two-photon-assisted slow light). The study carried out in solutions of dyes and dendrites shows significant delays, low distortion, and good transmission for easily reachable experimental conditions. The working principle can be applied to other media and can be used in telecommunications technology.     

Two-photon cooperative decay in a cavity in the presence of a thermalized electromagnetic field

We study the cooperative two-photon spontaneous decay of an excited atomic system in a microcavity whose size is of the order of several wavelengths of atomic radiation. We show that a thermalized electromagnetic field in the microcavity strongly affects the two-photon cooperative spontaneous emission of radiation. The increase in the rate of spontaneous cooperative decay is due to the presence of a small number of thermalized photons in a microcavity mode. At low temperatures, the two-photon absorption probability is found to be a linear function of the two-photon flux, and photon superbunching is observed. Zh. éksp. Teor. Fiz. 115, 1153–1167 (April 1999)     

“Spreading” of a biphoton in a group-velocity-dispersion medium and two-photon interference

It is shown that two-photon Bell states can be prepared by “spreading” of a two-photon wave packet (biphoton) in a dispersive medium without compensating for group delays between photons with orthogonal polarizations or using narrow-band filters but by selecting the time correlation function. This is possible because two-photon interference effects are manifested in the shape of the time correlation function of intensity due to its spreading.     

Theoretical analysis on two-photon absorption spectroscopy in a confined four-level atomic system

We investigate theoretically two-photon absorption spectroscopy modified by a control field in a confined Y-type four-level system. Dicke-narrowing effect occurs both in two-photon absorption lines and the dips of transparency against two-photon absorption due to enhanced contribution of slow atoms. We also find that the suppression and the enhancement of two-photon absorption can be modified by changing the strength of the control field and the detuning of three laser fields. This control of two-photon absorption may have some applications in information processing and optical devices.     

Isomeric orientation by two-photon excitation: a theoretical study

I develop the theory of molecular orientation induced by two-photon isomerization. Phenomenologically, two-photon isomeric orientational hole burning and reorientation induce molecular orientation while rotational diffusion tends to randomize it. Using the formalism of Legendre polynomials solves the general equations of the theory, and analytical solutions are derived for actual physical cases at the early time evolution and the steady state of two-photon excitation. The theory explains the observed results of two-photon molecular orientation, and predicts additional experiments in this direction. The isomerization parameters and the movement of the isomers during polarized two-photon excitation can be quantified by the analytical theory. A theoretical study on the creation of molecular orientation by competing orientational Kerr effect and two-photon orientation is also presented.     

Strong two-photon-induced fluorescence from a highly soluble polythiophene

Two-photon-induced fluorescence from a soluble polythiophene containing urethane side groups has been investigated using femto-second laser pulses at 800 nm. Strong two-photon fluorescence was measured in polymer solution. The quadratic dependence of the fluorescence on the excitation laser intensity confirmed the two-photon process. The measured two-photon absorption cross-section is larger as compared to those of other reported polythiophenes. This polymer can be readily hydrolyzed to yield a water soluble polythiophene which could be useful in biological imaging.     

以二乙烯硫/砜基为中心的新型电荷转移分子双光子吸收特性

理论研究分子结构与双光子吸收性质之间的关系对于指导实验者设计与合成功能分子材料具有重要意义. 在杂化密度泛函水平上, 利用响应函数方法, 计算了一类以二乙烯硫/砜基为中心的新型电荷转移分子的双光子吸收截面, 并在相同计算水平上, 与联苯乙烯类强双光子吸收分子做了比较; 以新型电荷转移分子为基础, 利用异构效应, 设计出了可以增强双光子吸收强度的分子结构. 研究表明, 在可应用波长范围内, 该系列分子表现出较强的双光子吸收响应, 与相似共轭长度的强双光子吸收分子具有相同量级的双光子吸收截面; 二乙烯硫/砜基在分子中心作为吸电子基团可以形成有效的电荷转移分子; 改变咔唑基的连接方式可以有效提高双光子吸收截面. 该研究为实验合成新型双光子吸收分子材料提供了理论依据.