Three-dimensional observation of internal defects in semiconductor crystals by use of two-photon excitation

We present a method of three-dimensional observation of internal defects in semiconductor crystals for blue lasers by use of two-photon excitation. We excite photoluminescence by using a two-photon process. Since semiconductor materials have intrinsically high absorption in the short-wavelength region, the excitation light of photoluminescence is largely absorbed by the crystals. It is difficult to observe defects in deep regions. Two-photon excitation can overcome this limitation because near-infrared light can be used instead of blue light for excitation of photoluminescence, and the near-infrared light is absorbed at only the focused point. The excitation light can penetrate into the deep regions of the crystal. We succeeded in observing defects in a ZnSe crystal ~200 microm below the crystal surface. This is, as far as we know, the first demonstration of the observation of three-dimensional structures of defects in semiconductor crystals by the use of two-photon excitation.     

The features of nonlinear absorption during resonance one- and two-photon excitation of the basic exciton transition in colloidal CdSe/ZnS quantum dots

The features of the nonlinear absorption of CdSe/ZnS quantum dots (colloidal solution) in the case of resonant one- and two-photon excitation of the basic exciton transition by powerful ultra-short laser pulses were determined. In one-photon excitation, with an increasing intensity of impulses, a decrease in absorption (bleaching) is relayed by an increase in absorption, which is associated with the process of the filling of the states (saturation) of a two-level system with the lifetime of the excited state depending on the light intensity. The arising Fresnel or Fraunhofer diffraction of the laser ray that pass through a colloidal solution with a high concentration of quantum dots is associated with the formation of the transparency channel and self-diffraction of laser ray on an induced diaphragm. In two-photon excitation, the features of the nonlinear absorption and luminescence tracks (the dependence of luminescence intensity on distance) were explained by the influence, in addition to the two-photon absorption, of the processes that are responsible for the slower growth of nonlinear absorption and luminescence quenching at high intensities of laser pulses.     

Polarization control of multi-photon absorption under intermediate femtosecond laser field

It has been shown that the femtosecond laser polarization modulation is a very simple and well-established method to control the multi-photon absorption process by the light–matter interaction. Previous studies mainly focused on the multiphoton absorption control in the weak field. In this paper, we further explore the polarization control behavior of multiphoton absorption process in the intermediate femtosecond laser field. In the weak femtosecond laser field, the secondorder perturbation theory can well describe the non-resonant two-photon absorption process. However, the higher order nonlinear effect(e.g., four-photon absorption) can occur in the intermediate femtosecond laser field, and thus it is necessary to establish new theoretical model to describe the multi-photon absorption process, which includes the two-photon and four-photon transitions. Here, we construct a fourth-order perturbation theory to study the polarization control behavior of this multi-photon absorption under the intermediate femtosecond laser field excitation, and our theoretical results show that the two-photon and four-photon excitation pathways can induce a coherent interference, while the coherent interference is constructive or destructive that depends on the femtosecond laser center frequency. Moreover, the two-photon and fourphoton transitions have the different polarization control efficiency, and the four-photon absorption can obtain the higher polarization control efficiency. Thus, the polarization control efficiency of the whole excitation process can be increased or decreased by properly designing the femtosecond laser field intensity and laser center frequency. These studies can provide a clear physical picture for understanding and controlling the multi-photon absorption process in the intermediate femtosecond laser field, and also can provide a theoretical guidance for the future experimental realization.     

Photobleaching and stabilization of. fluorophores used for single-molecule analysis. with one- and two-photon excitation

Fluorescence spectroscopic measurements at the single-molecule level usually require large absorption cross sections and fluorescence quantum yields for the dyes under study. In addition to these parameters, the collectable number of fluorescence photons and, thus, the signal-to-noise ratio of the measurement, is influenced by processes like triplet-state population and photobleaching, shifting the saturation threshold of the dye to lower excitation intensities. Confocal fluorescence correlation spectroscopy (FCS) is a versatile method to precisely determine photon emission rates of single molecules but also gives access to rate constants of dynamic bleaching and intersystem crossing. In recent FCS studies in solution and living cells, two-photon excitation with its inherent spatial sectioning has proven to be a very valuable alternative to minimize background and cumulative signal loss. However, there is evidence that in many dye systems, the photobleaching rates with two-photon excitation are significantly enhanced with respect to one-photon excitation at comparable photon-emission yields. The reasons have so far remained mainly speculative. In the present study, potential photobleaching pathways are investigated by adding chemical stabilizers and by working at different oxygen concentrations. The results suggest that the population of triplet states does not appear to be responsible for the limited emission rate with two-photon excitation. Rather, photobleaching pathways via the formation of radicals seem to be plausible causes for the signal limitation. Favorable conditions are discussed to maximize the overall photon-collection yield in two-photon experiments. Received: 4 July 2001 / Published online: 23 November 2001     

Properties of collective Rabi oscillations with two Rydberg atoms

Motivated by experimental advances that the collective excitation of two Rydberg atoms was observed, we provide an elaborate theoretical study for the dynamical behavior of two-atom Rabi oscillations. In the large-intermediate-detuning case, the two-photon Rabi oscillation is found to be significantly affected by the strength of the interatomic van der Waals interaction. With a careful comparison of the exact numbers and values of the oscillation frequency, we propose a new way to determine the strength of excitation blockade, agreeing well with the previous universal criterion for full, partial, and no blockade regions. In the small-intermediate-detuning case, we find a blockade-like effect, but the collective enhancement factor is smaller than ~(1/2) due to the quantum interference of double optical transitions involving the intermediate state.Moreover, a fast two-photon Rabi oscillation in ns timescale is manifested by employing intense lasers with an intensity of ~MW/cm~2, offering a possibility of ultrafast control of quantum dynamics with Rydberg atoms.     

Two-photon optical-beam-induced current solid-immersion imaging of a silicon flip chip with a resolution of 325 nm

We report high-resolution subsurface imaging of a silicon flip chip by detection of the photocurrent generated by the two-photon absorption of 1530-nm light from a femtosecond Er:fiber laser. The technique combines the focal sensitivity of two-photon excitation with the enhanced optical resolution of high-numerical-aperture solid-immersion imaging. Features on a sub-1-microm scale are clearly resolvable with high contrast, showing a resolution of 325 nm.     

Intrinsic photorefractive effect of LiNbO3

The photorefractive effect of undoped LiNbO₃ crystals of high purity is studied by means of two-photon excitation of picosecond light pulses. We show that two-photon photorefractive recording is accompanied by characteristic changes of the optical absorption and electron spin resonance spectra due to the formation of color centers. The role of these centers for the photorefractive process in discussed.     

Light quenching of tetraphenylbutadiene fluorescence observed during two-photon excitation

We observed the steady-state and time-resolved emission of tetraphenylbutadiene (TPB) whea excited by simultaneous absorption of two photons (514 to 610 nm). The intensity initially increased quadratically with laser power, as expected for a two-photon process. At higher laser powers the intensity increases in TPB were subquadratic. The intensity and anisotropy decay times of TPB were unchanged under the locally intense illumination. Importantly, the time zero anisotropy of TPB was decreased under conditions where the intensity was subquadratic. Furthermore, the subquadratic dependence on incident power was not observed for two-photon excitation of 2,5-diphenyloxazole (PPO), for which the incident wavelength does not overlap with the emission spectrum. These results are consistent with stimulated emission (light quenching) of TPB at high laser intensities. The phenomenon of light quenching may be important for other fluorophores used in biochemical research, particularly for the high local intensities used for two-photon excitation.     

Ultrafast carrier dynamics of Cu2O thin film induced by two-photon excitation

Cuprous oxide (Cu₂O) has attracted plenty of attention for potential nonlinear photonic applications due to its superior third-order nonlinear optical property such as two-photon absorption. In this paper, we investigated the two-photon excitation induced carrier dynamics of a Cu₂O thin film prepared by radio-frequency magnetron sputtering, using the femtosecond transient absorption experiments. Biexponential dynamics including an ultrafast carrier scattering (< 1 ps) followed by a carrier recombination (> 50 ps) were observed. The time constant of carrier scattering under two-photon excitation is larger than that under one-photon excitation, due to the different transition selection rules and smaller absorption coefficient of the two-photon excitation.     

双光子吸收的Franz-Keldysh效应

从实验上证实Hg_0.695Cd_0.305Te 光电二极管空间电荷区中存在双光子吸收的Franz-Keldysh效应.利用一个皮秒Nd:YAG激光器抽运的光学参量产生器和差频产生器作为激发光源,测量了入射波长为λ₀=7.92μm的脉冲激光所激发的光响应随入射光强的变化关系.脉冲光响应峰值强度随入射光强的增大呈现二次幂函数增强趋势.采用等效RC电路模型将脉冲光伏信号峰值与入射光强相关联,得到空间电荷区中强电场下单光束 关键词： Franz-Keldysh效应 碲镉汞 双光子吸收 脉冲光伏信号     

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.     

单光子和双光子激发的超歧化聚合物的光谱学特性研究

研究了二种新型超歧化聚合物在氯仿和二甲基甲酰胺溶剂中的飞秒激光单光子和双光子激发的光谱学特性．这二种聚合物是以苯为核、以对二甲氧基苯为连接单元，分别以二甲基苯胺为端基或以特丁基苯为端基的超歧化共轭聚合物．结果表明这种超歧化聚合物具有较大的溶剂极性相关的飞秒双光子吸收截面，不同的端基不仅影响分子内的电荷转移，而且导致超歧化分子共轭程度的变化．作为一种潜在的光学非线性材料，利用这种大的双光子吸收截面的超歧化聚合物可实现了飞秒双光子直写的三维高密度数据存储．     

ʌ-type doubling and spin-rotation splitting of NO,measured in simultaneous one- and two-photon laser spectroscopy

Doppler-free two-photon excitation of NO A²Σ⁺ by visible dye laser radiation is recorded simultaneously with single-photon absorption of frequency-doubled UV laser light. The measurement of the frequency difference between corresponding lines in the one- and two-photon spectrum provides a new method for a direct optical determination of Λ-type doubling in the X²Π ground state. In addition, the spin-rotation splitting of the A²Σ⁺ excited state is resolved in the Doppler-free two-photon spectrum.     

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).     

Ultrafast dynamics of all-trans--carotene explored by resonant and nonresonant photoexcitations

Excitation energy dependence of transmittance change has been investigated in -carotene. The signal induced by nonresonant excitation is ascribed to the ac Stark effect and the two-photon absorption of the excitation and probe pulses in three-level systems. The ultrafast response following resonant excitation is assigned to the two-photon absorption and the transient absorption of the photogenerated S(2) state with a lifetime of 150 fs. The long-debated S(2)-S(1) relaxation in beta-carotene can be explained by a two-state model (S(2), S(1)) without involving any intermediate states.     

Multichannel selective femtosecond coherent control based on symmetry properties

We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of "two-photon dark pulses" inducing widely tunable three-photon absorption.     

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.     

Inhibition of Two-Photon Absorption in a Four-Level Atomic System with Closed-Loop Configuration

We theoretically investigate the features of two-photon absorption in a coherently driven four-level atomic system with closed-loop configuration. It is found that two-photon absorption can be completely suppressed just by properly adjusting the relative phase of four coherent low-intensity driving fields and the atomic system becomes trans- parent against two-photon absorption. From a physical point of view, we explicitly explain these results in terms of quantum interference induced by two different two-photon excitation channels.     

Simulating resonance-mediated two-photon absorption enhancement in rare-earth ions by a rectangle phase modulation

Improving the up-conversion luminescence efficiency of rare-earth ions via the multi-photon absorption process is crucial in several related application areas. In this work, we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er~(3+) ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components.So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. Moreover, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width(or laser spectral bandwidth), final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earthions.     

双光子吸收材料二苯乙烯衍生物的合成及光谱性质

设计、合成并用红外光谱、1H NMR、元素分析表征了三种用于双光子吸收材料的二苯乙烯衍生物,4,4′-双(二苯氨基-反式-苯乙烯基)联苯(BPSBP),4,4′-双(二乙氨基-反式-苯乙烯基)联苯(BESBP)和4,4′-双(9-咔唑基-反式-苯乙烯基)联苯(BCSBP)。实验结果表明三者最强的单光子吸收出现在350～400 nm之间,且单光子吸收和荧光光谱中表现出明显的溶剂化显色效应,揭示了分子内对称电荷转移的本质,双光子荧光光谱则揭示了单光子和双光子吸收具有相同的发射机理。利用双光子上转换荧光法测试发现,三种双光子吸收材料在800 nm飞秒激光的激发下具有较大的吸收截面,分别为892,617和483 GM,这表明在双光子领域有潜在的应用价值。