Optical limiting and pulse reshaping of picosecond pulse trains by fullerene C60

We present a dynamical theory of nonlinear absorption and propagation of a laser pulse train that contains 20 subpulses with an individual pulse width of 100 ps. It is shown that the accumulative nonlinearity and the reverse saturation absorption play important roles in the optical limiting performance and pulse shaping. When the incident field is not too strong, the population transfer reveals a slow response process, and the periodic sequence of short light pulses can be regarded as a continuous long pulse. The general theory is applied to fullerence C₆₀, which is a popular reverse saturable absorption material and a good limiter because of its larger excited-state absorption cross-section compared with that of the ground state. The propagation of the front subpulses is mainly affected by the linear transition between the ground state and the first excited singlet state, while the latter subpulses are attenuated by the excited-state absorption. Moreover, these two different kinds of absorption mechanisms result in different radial distributions for different subpulses. The pulse propagation is studied by solving numerically the coupled rate equations and the propagation equation of the optical pulse intensity, using experimental parameters as input. We suggest a new method to measure the lifetime of the triplet state.     

一种新型非晶态分子材料的非线性光学折射率和吸收特性

用单光束扫描法测量了在532nm处一种新型非晶态分子材料5,5′Bis(dimesitylboryl)2,2′bithiophene的非线性折射率和吸收系数样品非线性透射特性的分析表明,在靠近线性吸收区的532nm处有饱和吸收存在由三能级饱和模型和Zscan法确定了饱和强度、非线性折射率的实部和虚部研究结果表明:这种新型非晶态分子材料具有非常好的光子学应用前景.     

Two-dimensional materials-decorated microfiber devices for pulse generation and shaping in fiber lasers

Two-dimensional(2D) materials have been regarded as a promising nonlinear optical medium for fabricating versatile optical and optoelectronic devices. Among the various photonic applications, the employment of 2D materials as nonlinear optical devices such as saturable absorbers for ultrashort pulse generation and shaping in ultrafast lasers is one of the most striking aspects in recent years. In this paper, we review the recent progress of 2D materials based pulse generation and soliton shaping in ultrafast fiber lasers, and particularly in the context of 2D materials-decorated microfiber photonic devices. The fabrication of 2D materials-decorated microfiber photonic devices, high performance mode-locked pulse generation, and the nonlinear soliton dynamics based on pulse shaping method are discussed. Finally, the challenges and the perspective of the 2D materials-based photonic devices as well as their applications are also discussed.     

Excited-state absorption in oxidized cytochrome c solution

Nonlinear absorption dynamics of oxidized cytochrome c in water solution was investigated at 532 nm with Z-scan and pump–probe techniques. The optical characterization of this compound is very important owing to its similarity with hematoporphyrin-based drugs commonly used in photodynamic therapy for cancer treatment. We observed a saturable absorption process related to the excited singlet population, followed by a fast decay to the ground state. The optical excitation and subsequent relaxation were interpreted with a three-energy-level diagram, allowing the first singlet excited-state absorption cross section and lifetime determination. PACS 42.65.Sf; 78.66.Qn; 42.62.Be     

萘酞菁铅化合物的光限幅特性研究

应用调Q倍频ns/ps Nd：YAG脉冲激光,在波长为532nm,脉冲宽度为8ns,重复频率为1Hz的条件下,研究了溶于二甲基亚砜(DMSO)中的萘酞菁铅溶液的反饱和吸收和光限幅特性。实验表明,萘酞菁铅具有良好的光限幅特性,它的有效激发态吸收截面与基态吸收截面的比值约为15．21,大于萘酞菁铜。研究结果表明,萘酞菁铅的光限幅特性优于C60,激发态吸收是其主要的光限幅机理。实验结果证实了重原子效应可以通过增强系际跃迁而使三重态的反饱和吸收增强,从而提高光限幅的能力。     

Nonresonant and Resonant Nonlinear Absorption of CdSe-Based Nanoplatelets

We present a comprehensive understanding of the nonlinear absorption characteristics of CdSe-based nanoplatelets(NPLs) synthesized by the solution-phase method and the colloidal atomic layer deposition approach through Z-scan techniques at 532 nm with picosecond pulses. The CdSe NPLs exhibit strong two-photon induced free carrier absorption(effective three-photon absorption) upon the nonresonant excitation, resulting in a remarkable optical limiting behavior with the limiting threshold of approximately 75 GW/cm~2. A nonlinear optical switching from saturable absorption(SA) to reverse saturable absorption(RSA) with increasing the laser intensity is observed when coating CdSe NPLs with a monolayer of CdS shell to realize the resonant absorption. The SA behavior originates from the ground state bleaching and the RSA behavior is attributed to the free carrier absorption.These findings explicitly demonstrate the potential applications of CdSe-based NPLs in nonlinear optoelectronics such as optical limiting devices, optical pulse compressors and optical switching devices.     

Third-order optical nonlinearities of α,ω-dithienylpolyenes and oligo(thienylvinylene)

α,ω-Dithienylpolyenes and oligo(thienylvinylene) are interesting third-order nonlinear optical materials for a variety of device applications. To better understand the third-order nonlinear response of these materials, the third-order susceptibilities (χ⁽³⁾) and nonlinear absorption behaviors of two α,ω-dithienylpolyenes with different conjugation length and two oligo(thienylvinylene) with different substituents on the thiophene rings have been studied using degenerate four wave mixing (DFWM) and nonlinear transmission techniques at 532 nm. The χ⁽³⁾ values of 1×10⁻³ mol/l solutions are all of the order of 10⁻¹³ esu. The χ⁽³⁾ values increase with the increase of the linear absorption coefficient. In addition, these compounds exhibit reverse saturable absorption for nanosecond laser pulses. The strength of reverse saturable absorption varies when the conjugation length and substituents change. Moreover, the nonlinear absorption characteristics of these compounds in the picosecond regime differ from those in the nanosecond regime. The different nonlinear absorption behavior is due to the relative contributions from excited singlet–singlet and triplet–triplet absorption. The strong reverse saturable absorption characteristics of two of the compounds suggest that they could be potential candidates for optical limiting applications in the nanosecond regime.     

Ultrafast Saturable Absorption of Core/Shell Colloidal Quantum Dots

Ultrafast saturable absorption (SA) materials that are capable of blocking the optical absorption under strong excitation have extensive applications in photonic devices. This work presents core/shell colloidal quantum dots (CQDs) which have the quantized energy levels, excellent band gap tunability, and possess significant SA performance. When the band gap is close to the pump pulse energy, the CQDs show significant resonant SA response. At the same excitation conditions, the core/shell CQDs dispersions show better SA response than graphene dispersions, and comparable to the recently reported molybdenum disulfide. The carrier dynamics of the SA of the CQDs is analyzed systematically. The research has also found that the two‐photon absorption of the CQDs show nearly cubic power law of the band gap, while the SA performance keeps almost the same in the nonresonant regime. Further, superior passive Q‐switched laser behavior is observed using the CQDs as a saturable absorber. The results directly reveal the physical processes of this basic problem and broaden the applications of CQDs in photonic devices.     

S1 singlet excited-state absorption of DODCI

1 excited-state absorption cross-section spectrum of DODCI in ethylene glycol is determined in the wavelength range from 500 nm to 750 nm. The S₁ state is populated by amplified femtosecond dye laser pulses (wavelength 592 nm) and the S₁-state absorption and emission behaviour is probed with a femtosecond light continuum. A general analysis procedure is developed to extract absolute excited-state absorption cross-sections from the measured transmissions. For DODCI in ethylene glycol the wavelength regions of saturable absorption (mode-locking application), reverse saturable absorption (optical limiter application), and effective stimulated emission (laser application) are determined. Received: 25 July 1996     

Temporal response of nonlinear transmission in optically thick saturable absorbers and determination of saturable absorption parameters

The temporal response of nonlinear transmission in saturable absorbers is theoretically investigated on the basis of a four-energy-level model including an excited-state absorption, and is experimentally employed for determining saturable absorption parameters in saturable-dye-doped films. The approximation of optically thin absorbers is shown to be inadequate to this end. In theoretical calculations, optically thick saturable absorbers are treated by a set of simultaneous partial differential equations: a rate equation governing the dynamics of population densities of energy levels and a propagation equation governing the propagation of optical fields in the optically thick absorbers. By comparing experimental results with numerical ones, the saturable absorption parameters can be determined on the basis of the intensity dependence of response time. In numerical calculations, the effect of random orientation is also considered for optically anisotropic molecules rigidly fixed in saturable absorbing media. The characterization of the saturable absorption parameters is conducted by using uranine-doped poly(vinyl alcohol) films.     

被动光学限幅器的机制与研究进展

被动光学限幅器是利用介质的非线性光学性质实现对光的强度进行控制的器件，它在科研，军事和民用方面都具有广泛的应用，文章讨论了被动光学限幅器的反饱和吸收，双光子吸收，自由载流子吸收，非线性折射，光致散射和光折变机制，每种机制在光限幅器应用中的有效性及局限性，介绍了国内外研究状况及自己的工作；指出了今后被动光学限幅器研究的发展方向。     

Optical and nonlinear optical properties of copper nanocomposite glasses annealed near the glass softening temperature

Copper nanocomposite glasses have been prepared by the ion-exchange method, and annealed at different temperatures up to and above the glass softening temperature. The absorption spectra, fluorescence spectra, and nonlinear optical transmission of the samples at 532 nm for nanosecond laser pulses, have been investigated. The optical and nonlinear optical properties of the glasses are found to be distinctly different below and above the glass softening temperature. For instance, thermal annealing up to the glass softening temperature makes the samples behave like saturable absorbers, while annealing at higher temperatures makes them behave like optical limiters. Such flexibility in controlling the optical nonlinearity in these materials makes them potential candidates for photonic applications.     

Low power continuous wave laser induced optical nonlinearities in saffron (<Emphasis Type="Italic">Crocus Sativus</Emphasis> L.)

We report on the low power CW laser induced nonlinear optical responses of Saffron (stigmata of Crocus Savitus L.) ethanol and methanol extracts. The optical nonlinearities were investigated by performing Z-scan measurements at 470 and 535 nm wavelengths. At both wavelengths the material has a strong nonlinear refraction, mainly of thermal origin. However, only at 470 nm wavelength the material exhibit pronounced saturable nonlinear absorption. Long-term (70 days) stability measurements indicated that the nonlinearities in the Saffron extracts are due to their nonvolatile components. This study shows that there is great potential for Saffron extracts to be used in nonlinear photonic applications.     

碳纳米管/二硒化钼有机玻璃的非线性吸收、非线性散射和光限幅特性

MoSe₂的禁带宽度较窄（1.1–1.5 eV）,且具有可调谐的激子光电效应,这样使其在光致发光、光电晶体管、太阳能电池和光学非线性等方面具有潜在的应用价值.然而,纯的MoSe₂的光生电子空穴复合率较高,限制了其在某些光学领域中的应用.通过设计MoSe₂的复合材料,可以降低材料的光生电子空穴复合率,从而扩展其应用领域.首先,通过热溶剂法合成CNT/MoSe₂复合材料;然后,通过浇铸法将其分散在甲基丙烯酸甲酯（MMA）中制备成有机玻璃,其中MMA会聚合成聚甲基丙烯酸甲酯（PMMA）,并利用改进的Z-扫描技术首次对CNT/MoSe₂/PMMA有机玻璃的非线性吸收、非线性散射和光限幅特性进行了研究.研究表明,随着输入能量的变化,通过调节输入能量,CNT/MoSe₂/PMMA有机玻璃表现出饱和吸收（SA）和从SA到反饱和吸收的转变.结合材料特性及应用条件要求,可以得到CNT/MoSe₂/PMMA有机玻璃在光学设备,如光学限制器和锁模/调Q激光器等方向具有较好的应用前景.     

Thermally induced nonlinear optical response and optical power limiting of acid blue 40 dye

We report the investigations of thermally induced third-order nonlinear optical and optical limiting characterizations for various concentrations of acid blue 40 dye in N,N-Dimethyl Formamide, studied by employing z-scan technique under cw He–Ne laser irradiation at 633 nm wavelength. The samples exhibited nonlinear absorption and nonlinear refraction under the experimental conditions. For lower concentration, the samples display both saturable absorption (SA) and reverse saturable absorption (RSA); whereas with increase in concentration, RSA behaviour prevails. The estimated values of the effective coefficients of nonlinear absorption β_eff, nonlinear refraction n₂ and third-order nonlinear susceptibility χ⁽³⁾ were found to be of the order of 10^?2 cm/W, 10^?4 esu and 10^?6 esu respectively. Multiple diffraction rings were observed when the samples were exposed to laser beam due to refractive index change and thermal lensing. The effect of concentration and the laser intensity on the self-diffraction ring patterns was studied experimentally. The acid blue 40 dye also exhibited strong optical limiting properties under cw excitation and reverse saturable absorption is found to be the dominant nonlinear optical process leading to the observed nonlinear behaviour.     

Emerging 2D Semiconducting Materials: Tin Diselenide for Ultrafast Photonics

SnSe₂, a novel 2D semiconducting material with good photoelectric properties and tunable bandgaps structure, has been widely studied in high-performance photodetectors and superconductivity applications, etc. Herein, another excellent property, nonlinear optical absorption, is applied to ultrafast photonics. The measured nonlinear optical absorption curve of SnSe₂ with modulation depth of 5.52% is obtained. Q-switching and mode-locking in Er-doped fiber lasers based on SnSe₂ is reported. A Q-switched fiber laser can be obtained with a 0.5-m-long gain fiber and a 50:50 optical coupler. With 0.75-m-long active fiber and a 40:60 optical coupler, mode locking can be obtained. Furthermore, a third-order bound-state soliton pulse with a pulse duration of 882 fs can be achieved. The experimental results show that SnSe₂ is an excellent optical saturable absorber for the applications of ultrafast photonics.     

通过飞秒泵浦探测技术研究PbS纳米颗粒的激发态瞬态动力学过程

利用飞秒泵浦探测技术研究了PbS半导体纳米颗粒复合的SiO₂溶胶凝胶薄膜的瞬态动力学过程。通过改变激发探测波长和激发光强度,研究引起PbS半导体纳米颗粒的非线性吸收的两种机制。当激发探测波长选在激子吸收峰附近(620nm)时,由于激子的饱和吸收引起的光致漂白,当激发波长选在激子能态的低能侧(753,800nm),同时观察到激子的饱和吸收和双激子效应引起的光致吸收。研究了激子的饱和吸收和双激子效应引起的激发态吸收随激发态电子-空穴对浓度的变化关系,表明双激子效应与载流子浓度有很大关系。在高激发强度下,双激子效应引起的诱导吸收远远大于激子跃迁引起的光致漂白,双激子效应在非线性吸收中起着决定性作用。     

Modulation of the second-harmonic generation in MoS_2 by graphene covering

Nonlinear optical frequency mixing,which describes new frequencies generation by exciting nonlinear materials with intense light field,has drawn vast interests in the field of photonic devices,material characterization,and optical imaging.Investigating and manipulating the nonlinear optical response of target materials lead us to reveal hidden physics and develop applications in optical devices.Here,we report the realization of facile manipulation of nonlinear optical responses in the example system of MoS₂ monolayer by van der Waals interfacial engineering.We found that,the interfacing of monolayer graphene will weaken the exciton oscillator strength in MoS₂ monolayer and correspondingly suppress the second harmonic generation(SHG)intensity to 30%under band-gap resonance excitation.While with off-resonance excitation,the SHG intensity would enhance up to 130%,which is conjectured to be induced by the interlayer excitation between MoS₂ and graphene.Our investigation provides an effective method for controlling nonlinear optical properties of two-dimensional materials and therefore facilitates their future applications in optoelectronic and photonic devices.     

Wavelength dependence of nonlinear absorption in a bis-phthalocyanine studied using the Z-scan technique

The wavelength dependence of the nonlinear absorption of a bis-phthalocyanine, Nd(Pc)₂, dissolved in dimethyl formamide was studied in the rising part of the Q-band using the open aperture Z-scan technique, to determine the wavelength region over which the nonlinear absorption changes from reverse saturable absorption to saturable absorption. It was found that the sample could be used as a reverse saturable absorber, and hence as an optical limiter, up to a wavelength of about 604 nm. The imaginary part of the third order susceptibility was also calculated for these wavelengths. Resonant enhancement of the imaginary part of the third order susceptibility was clearly observed. Received: 26 April 2002 / Revised version: 30 June 2002 / Published online: 20 December 2002 RID="*" ID="*"Corresponding author. Fax: +91-484/576-714, E-mail: kpu@cusat.ac.in RID="**" ID="**"Present address: Optical Sciences Center, University of Arizona, Tucson, USA     

Studies on third-order nonlinear optical properties and reverse saturable absorption in polythiophene/poly (methylmethacrylate) composites

We report here the studies on third-order nonlinear optical properties of two novel polythiophene composite films investigated using the Z-scan technique. The measurements were carried out using a Q-switched, frequency doubled Nd:YAG laser producing 7 nanosecond laser pulses at 532 nm. Z-scan results reveal that the composite films exhibit self-defocusing nonlinearity. The real and imaginary parts of the third-order nonlinear optical susceptibility were of the order 10⁻¹² esu. The effective excited-state absorption cross section was found to be larger than the ground state absorption cross section, indicating that the operating nonlinear mechanism is reverse saturable absorption (RSA). The polythiophene composite films also exhibit good optical power limiting of the nanosecond laser pulses. The nonlinear optical parameters are found to increase on increasing the strength of the electron-donor group, indicating the dependence of χ ⁽³⁾ on the electron-donor/acceptor units of polythiophenes.