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.     

Optimal spectral phase control of femtosecond laser-induced up-conversion luminescence in Sm3+:NaYF4 glass

The spectral phase of the femtosecond laser field is an important parameter that affects the up-conversion(UC)luminescence efficiency of dopant lanthanide ions.In this work,we report an experi-mental study on controlling the UC lmiiinescence efficiency in Sm^3+:NaYF4 glass by 800-nm femtosec-ond laser pulse shaping using spectral phase modulation.The optimal phase control strategy efficiently enhances or suppresses the UC luminescence intensity.Based on the laser-power dependence of the UC luminescence intensity and its comparison with the luminescence spectrum under direct 266-nm fem-tosecond lciser irradiation,we propose herein an excitation model combining non-resonant two-photon absorption with resonance-media ted three-photon absorption to explain the experimental observations.     

Up-conversion luminescence tuning in Er~(3+) -doped ceramic glass by femtosecond laser pulse at different laser powers

The up-conversion luminescence tuning of rare-earth ions is an important research topic for understanding luminescence mechanisms and promoting related applications. In this paper, we experimentally study the up-conversion luminescence tuning of Er~(3+)-doped ceramic glass excited by the unshaped, V-shaped and cosine-shaped femtosecond laser field with different laser powers. The results show that green and red up-conversion luminescence can be effectively tuned by varying the power or spectral phase of the femtosecond laser field. We further analyze the up-conversion luminescence tuning mechanism by considering different excitation processes, including single-photon absorption(SPA), two-photon absorption(TPA), excited state absorption(ESA), and energy transfer up-conversion(ETU). The relative weight of TPA in the whole excitation process can increase with the increase of the laser power, thereby enhancing the intensity ratio between green and red luminescence(I_(547)/I_(656)). However, the second ETU(ETU2) process can generate red luminescence and reduce the green and red luminescence intensity ratio I_(547)/I_(656), while the third ESA(ESA3) process can produce green luminescence and enhance its control efficiency. Moreover, the up-conversion luminescence tuning mechanism is further validated by observing the up-conversion luminescence intensity, depending on the laser power and the down-conversion luminescence spectrum under the excitation of 400-nm femtosecond laser pulse. These studies can present a clear physical picture that enables us to understand the up-conversion luminescence tuning mechanism in rare-earth ions, and can also provide an opportunity to tune up-conversion luminescence to promote its related applications.     

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.     

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.     

低强度飞秒激光激发下CdTe和CdTe/CdS核壳量子点的荧光上转换研究

利用400 nm和800 nm不同波长的低强度飞秒激光,对CdTe和CdTe/CdS核壳量子点溶胶进行激发,研究其稳态和时间分辨荧光性质.800 nm飞秒激光激发下,CdTe和CdTe/CdS核壳量子点产生上转换发光现象,上转换荧光峰与400 nm激发下的荧光峰相比蓝移最多达15 nm,而且蓝移值与荧光量子产率有关.变功率激发确认激发光功率与上转换荧光强度间满足二次方关系,时间分辨荧光的研究表明荧光动力学曲线服从双e指数衰减.提出表面态辅助的双光子吸收模型是低激发强度上转换发光的主要机理.CdTe和CdT 关键词： CdTe量子点 CdTe/CdS核壳量子点 时间分辨荧光 上转换荧光     

Simulation of Intermediate State Absorption Enhancement in Rare-Earth Ions by Polarization Modulated Femtosecond Laser Field

We extend the third perturbation theory to study the polarization control behavior of the intermediate state absorption in Nd~(3+)ions. The results show that coherent interference can occur between the single-photon and three-photon excitation pathways, and depends on the central frequency of the femtosecond laser field. Moreover,single-photon and three-photon absorptions have different polarization control efficiencies, and the relative weight of three-photon absorption in the whole excitation processes can increase with increasing the laser intensity.Therefore, the enhancement or suppression of the intermediate state absorption can be realized and manipulated by properly designing the intensity and central frequency of the polarization modulated femtosecond laser field.This research can not only enrich theoretical research methods for the up-conversion luminescence manipulation of rare-earth ions, but also can provide a clear physical picture for understanding and controlling multi-photon absorption in a multiple energy level system.     

Simulating the resonance-mediated (1+2)-three-photon absorption enhancement in Pr3+ ions by a rectangle phase modulation

Enhancing the upconversion luminescence of rare earth ions is crucial for their applications in the laser sources, fiber optic communications, color displays, biolabeling, and biomedical sensors. In this paper, we theoretically study the resonance-mediated (1+2)-three-photon absorption in Pr³⁺ ions by a rectangle phase modulation. The results show that the resonance-mediated (1+2)-three-photon absorption can be effectively enhanced by properly designing the depth and width of the rectangle phase modulation, which can be attributed to the constructive interference between on-resonant and near-resonant three-photon excitation pathways. Further, the enhancement efficiency of resonance-mediated (1+2)-three-photon absorption can be affected by the pulse width (or spectral bandwidth) of femtosecond laser field, final state transition frequency, and absorption bandwidths. This research can provide a clear physical picture for understanding and controlling the multi-photon absorption in rare-earth ions, and also can provide theoretical guidance for improving the up-conversion luminescence.     

Coherent Features of Resonance-Mediated Two-Photon Absorption Enhancement by Varying the Energy Level Structure,Laser Spectrum Bandwidth and Central Frequency

The femtosecond pulse shaping technique has been shown to be an effective method to control the multi-photon absorption by the light-matter interaction. Previous studies mainly focused on the quantum coherent control of the multi-photon absorption by the phase, amplitude and polarization modulation, but the coherent features of the multi-photon absorption depending on the energy level structure, the laser spectrum bandwidth and laser central frequency still lack in-depth systematic research. In this work, we further explore the coherent features of the resonance-mediated two-photon absorption in a rubidium atom by varying the energy level structure, spectrum bandwidth and central frequency of the femtosecond laser field. The theoretical results show that the change of the intermediate state detuning can effectively influence the enhancement of the near-resonant part, which further affects the transform-limited(TL)-normalized final state population maximun. Moreover, as the laser spectrum bandwidth increases, the TL-normalized final state population maximum can be effectively enhanced due to the increase of the enhancement in the near-resonant part, but the TL-normalized final state population maximum is constant by varying the laser central frequency. These studies can provide a clear physical picture for understanding the coherent features of the resonance-mediated two-photon absorption, and can also provide a theoretical guidance for the future applications.     

Two-photon-excited luminescence in a Tb3+ -doped lithium niobate crystal pumped by a near-infrared femtosecond laser

Blue (487.6 nm), green (544.1 nm), yellow (582.1 nm), and red (623.6 nm) upconversion (UC) luminescences are achieved in a Tb(3+)-doped lithium niobate crystal when an 800 nm femtosecond laser is loosely focused onto the sample at room temperature. The relationship between UC luminescence intensity and the pump energy indicates that a two-photon excitation process is dominant in this UC luminescence phenomenon. The Tb(3+) sensitive temperature dependence of the luminescence intensity is demonstrated via an obvious reduction of luminescence intensity with durative laser irradiation.     

Quantum control of two-photon photochromism in the solid phase

Phase and polarization control of photochromism in the solid phase is experimentally demonstrated. Photochromism initiated by a two-photon absorption of femtosecond laser pulses in a three-dimensional solid-phase polymer sample of spiropyran is controlled by varying the polarization state and the chirp of laser pulses.     

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。     

Luminescence and structural properties of thermally evaporated benzanthrone dyes thin films

We report optical and luminescence properties of 3-N, N-diacetylaminobenzanthrone thin films deposited on glass substrate by thermal evaporation. The structural and optical properties of organic thin films were studied by means of the confocal microscope with an input of femtosecond laser radiation, X-ray diffractometer, and scanning electron microscope (SEM). Intense luminescence with the maximum at 530 nm was observed when excited by laser radiation with the wavelengths 458, 476, 488, 496, 514 nm. In addition, the luminescence caused by two-photon absorption of femtosecond (fs) laser radiation has been investigated. Semi empirical calculations by AM1 and ZINDO/S methods and ab initio calculations using Gaussian software were carried out to estimate the electron system of structure. The calculations show planar configurations for the aromatic core and diacetylamino fragment of this compound. The study of the structure of benzanthrone derivative thin films with X-ray diffraction (XRD) methods, indicates the distance between molecular layers and ordered molecular fragments.     

Coherent control of non-resonant two-photon transition in molecular system

In this paper,we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape).The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth.Our results demonstrate that,the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field,and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.     

1 520 nm激光激发的Er(0.5):FOG材料的上转换发光与立体显示研究

立体显示为现代重要的科学前沿。上转换三维立体显示为一种新颖的自体视三维立体显示,在1996年被评为十大科技创新成就之一,现正向应用快速发展。研究了1 520 nm半导体激光激发的Er(0.5):FOG材料的上转换发光,发现了(407.43, 411.20 nm), (522.51m, 528.57 nm), (540.53m, 543.70,549.00 nm), (654.75m, 665.50 nm), 和802.10m nm的上转换发光(m代表主峰),依次为(2G4F2H)_9/2→4I_15/2, 4H_11/2→4I_15/2, 4S_3/2→4I_15/2, 4F_9/2→4I_15/2和4I_9/2→4I_15/2的跃迁。值得注意的是上转换发光强度随激光功率变化的双对数曲线的斜率有各种各样的值。通过详细研究发现(407.43, 411.20 nm)的(2G4F2H)_9/2→4I_15/2上转换发光是四光子荧光;(522.51m, 528.57 nm)的2H_11/2→4I_15/2,(540.53m, 543.70,549.00 nm)的4S_3/2→4I_15/2和(654.75m, 665.50 nm)的4F_9/2→4I_15/2的上转换发光为三光子荧光;而802.10m nm的4I_9/2→4I_15/2上转换发光为双光子荧光。很明显从基态4I_15/2到第一激发态的吸收很大,因为它的振子强度f和与1 520 nm激光的匹配都很好,随后的起源于第一激发态的能量传递和相继吸收都很易于发生,这导致了1 520 nm激光激发下的Er(0.5): FOG材料的丰富和有意义的上转换发光现象。     

水溶性CdTe量子点的稳态和纳秒时间分辨光致发光光谱

报道了以飞秒脉冲激光为激发光源的水溶性CdTe量子点(QDs)的稳态荧光光谱和纳秒时间分辨荧光光谱.实验发现CdTe量子点的荧光光谱峰值位置随激发波长变化发生明显移动，激发脉冲波长越长，荧光峰位红移越大.荧光动力学实验数据显示，在400nm和800nm脉冲激光激发下，水溶性CdTe量子点的荧光光谱中均含有激子态和诱捕态两个衰减成分，两者的发射峰相距很近，诱捕态的发射峰波长较长.在800nm脉冲激光激发下的诱捕态成分占总荧光强度的比重比400nm激发下的约高3倍，其相对强度的这种变化导致了稳态荧光发射峰位的红移. 关键词： CdTe 量子点 时间分辨 荧光光谱 上转换荧光     

The Dynamic Behaviour Analysis of Up－Conversion Luminescence in ErP_5O_（14） Glass

ＴｈｅＤｙｎａｍｉｃＢｅｈａｖｉｏｕｒＡｎａｌｙｓｉｓｏｆＵｐ－ＣｏｎｖｅｒｓｉｏｎＬｕｍｉｎｅｓｃｅｎｃｅｉｎＥｒＰ_５Ｏ_（１４）ＧｌａｓｓＴｈｅＤｙｎａｍｉｃＢｅｈａｖｉｏｕｒＡｎａｌｙｓｉｓｏｆＵｐ－ＣｏｎｖｅｒｓｉｏｎＬｕｍｉｎｅｓｃｅｎｃｅ...     

稀土掺杂材料的上转换发光

稀土掺杂材料的上转换发光是实现光波频率转换的重要途径,也是稀土掺杂发光材料研究的重要内容。本文从介绍与上转换相关的基本概念出发,阐述了稀土离子上转换发光的发展历史;对稀土离子掺杂材料的能量传递、激发态吸收、合作敏化、合作发光、双光子吸收激发及光子吸收雪崩等上转换发光机制进行了概述,并对各机制进行了比较;对不同稀土离子掺杂体系中上转换发光的机制进行了总结;对以往研究的稀土掺杂上转换发光材料的基质,包括粉体材料、晶体材料、非晶材料进行了概括;最后对影响稀土离子上转换发光效率的因素进行了分析,提出了在上转换发光材料的设计中应重点考虑基质对泵浦光及上转换发射光的吸收、基质材料的声子能量、稀土离子的掺杂方案及泵浦途径等因素。     

Multicontrast nonlinear optical microscopy with a compact and rapid pulse shaper

Homodyne detection can dramatically enhance measurement sensitivity for weak signals. In nonlinear optical microscopy it can make accessible a range of novel, intrinsic, contrast like nonlinear absorption and nonlinear phase contrast. Here a compact and rapid pulse shaper is developed, implemented, and demonstrated for homodyne detection in nonlinear microscopy with high-repetition rate mode-locked femtosecond lasers. With this method we generate two-photon absorption (TPA) and self-phase modulation images of gold nanostars in biological samples. Simultaneous imaging of two-photon luminescence and TPA also enables us to produce two-photon quantum yield images.     

Enhanced luminescence of silver nanoclusters in mesoporous film

Luminescence of silver nanoparticles photodeposited on titan dioxide nanoparticles of mesoporous film is studied. Luminescence was registered under the two-photon excitation by femtosecond laser pulses of Ti:sapphire laser. It occurs that Ag/TiO₂ mesoporous films have high concentration of bright luminescence spots which reveal stability to degradation under long illumination. Various configurations of silver nanoparticles are analyzed to explain the physics of bright luminescence spots (“hot spots”). Luminescence intensity reveals “hot spots” dependence on excitation laser pulse polarization. Properties of Ag/TiO₂ system show its promising usage for single molecule spectroscopy and biological objects visualization.