Ultrafast Optical Nonlinearity Research Articles

Femtosecond Third-Order Non-Linear Optical Properties of Unconstrained Green Fluorescence Protein Chromophores

We report herein results on the third-order non-linear optical (NLO) properties of four structurally unconstrained green fluorescence protein (GFP) chromophores, namely, 1, 2, 3, and 4. Using experimental techniques and theoretical calculations such as UV–visible spectroscopy, density functional theory (DFT), time-dependent density functional theory (TDDFT), and Z-scan techniques, we have investigated the linear absorption, ultrafast non-resonant third-order optical non-linearities, and the onset of optical-limiting thresholds of these benzylidenedimethylimidazolinone (BDI) dyes. The Z-scan measurements were performed at a wavelength of 800 nm with ∼70 femtosecond (fs) pulses. We have witnessed a strong reverse saturable absorption (fitted to three-photon absorption) for all of the molecules with fs pulse excitation. The valley–peak curves obtained from the closed-aperture Z-scan technique revealed the positive non-linear refractive index (self-focusing) nature of these molecules. We have evaluated the various third-order NLO coefficients (second hyperpolarizability, γ ∼10–33 esu), which were found to be larger than those of similar molecules reported in the recent literature.

Facile Synthesis of Monodispersed Titanium Nitride Quantum Dots for Harmonic Mode-Locking Generation in an Ultrafast Fiber Laser.

As a member of the transition metal nitride material family, titanium nitride (TiN) quantum dots (QDs) have attracted great attention in optical and electronic fields because of their excellent optoelectronic properties and favorable stability. Herein, TiN QDs were synthesized and served as a saturable absorber (SA) for an ultrafast fiber laser. Due to the strong nonlinear optical absorption characteristics with a modulation depth of ~33%, the typical fundamental mode-locked pulses and harmonics mode-locked pulses can be easily obtained in an ultrafast erbium-doped fiber laser with a TiN-QD SA. In addition, at the maximum pump power, harmonic mode-locked pulses with a repetition rate of ~1 GHz (164th order) and a pulse duration of ~1.45 ps are achieved. As far as we know, the repetition rate is the highest in the ultrafast fiber laser using TiN QDs as an SA. Thus, these experimental results indicate that TiN QDs can be considered a promising material, showing more potential in the category of ultrafast laser and nonlinear optics.

Spectral-temporal transient dynamics of dissipative soliton molecules in mode-locking fiber lasers

Dissipative soliton molecules that are analogous in many ways to matter molecules manifest complex evolution dynamics. Here, spectral-temporal transient internal motion dynamics of dissipative soliton molecules generated in a passively mode-locking erbium-doped fiber laser are experimentally investigated. Various categories of internal motion dynamics including attraction, creeping, dual-period breathing, and collision behaviors are revealed by employing an asynchronous time lens-based temporal magnifier together with the time stretched technique. Soliton temporal separation in those motion dynamics exhibit gradual decreasing and slightly wiggling motion. The temporal magnification factor of time lens system is substantially improved into 361. Our work makes the temporal magnifier more attractive for the applications of ultrafast measurements and nonlinear fiber optics, and benefits for fiber laser design.

Investigation of transient optical nonlinearity in pyrene-based ferrocene and its optical limiting potential for ultrafast laser absorption

The ultrafast optical nonlinearity of a pyrene-based ferrocene derivative (Py-Fc) is systematically studied via Z-scan, transient absorption spectrum (TAS), and phase object pump probe (POPP). An ultrafast broadband absorption in visible wavelength region is observed via TAS. Based on this finding, nonlinear optical absorption of the material is investigated at various wavelengths. Results indicate that different absorption mechanisms, including reverse saturable absorption and two-photon induced excited state absorption involve in the nonlinear absorption in visible spectrum. The cooperation between the two mechanisms brings strong optical limiting properties. In addition, negative nonlinear optical refraction from the excited state is observed in POPP experiment and its dynamics is discussed. These results demonstrate that the molecular Py-Fc exhibits strong optical limiting, suggesting it is a potential material for ultrafast laser protection.

Enhanced Terahertz Generation From the Lithium Niobate Metasurface

The lithium niobate (LiNbO3) metasurface is an attractive platform for nonlinear frequency conversion due to its excellent nonlinearity, high damage threshold, and strong enhancement of the driving field. Here, we demonstrated the nonlinear metasurface for terahertz (THz) generation from LiNbO3on an insulator. The THz electric field from the LiNbO3metasurface of 300 nm thickness is enhanced by more than one order of magnitude compared to the unstructured sample. The enhanced terahertz electric field is very selective in the excitation wavelength due to its resonant feature and is highly anisotropic with respect to the excitation polarization. The polarization direction of the THz electric field can be controlled by rotating the optical axis of the LiNbO3metasurface. By combining the nanofabrication technology of the LiNbO3metasurface and ultrafast nonlinear optics, our work paves the way for the design of new compact terahertz photonic devices that integrate THz emitters into LiNbO3-based chips with multifaceted capabilities.

Study of ultrafast nonlinear optical response and transient dynamics of pyrene derivatives with intramolecular charge transfer characteristics

Two pyrene derivatives 1906 and 1936 with typical charge transfer characteristics were designed and synthesized to study the influence of intramolecular charge transfer (ICT) on the ultrafast nonlinear optical (NLO) absorption. Frontier molecular orbital distribution and hole-electron analysis show that compound 1906 has stronger ICT characteristics than 1936 by introducing the halogen effect. Intense ESA signals in the green region of these pyrene derivatives were observed in the transient absorption spectrum (TAS). The excited state dynamics clearly show singlet-based electronic transitions and relaxation processes. Femtosecond Z-scan experiment at 480 nm indicates the ultrafast NLO absorption performance of these pyrene derivatives can be significantly improved by enhancing the ICT characteristics. The photophysical mechanism is one-photon absorption (OPA) induced excited-state absorption (ESA). As the input intensity is 46.8 GW cm−2, the effective NLO absorption coefficient of 1906 is 7.6 × 10−13 W m−1 which is 6.3 times that of 1936. Our results indicate that these pyrene derivatives are promising potential candidates for ultrafast laser protection applications.

Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor

Searching for ideal materials with strong effective optical nonlinear responses is a long-term task enabling remarkable breakthroughs in contemporary quantum and nonlinear optics. Polaritons, hybridized light-matter quasiparticles, are an appealing candidate to realize such nonlinearities. Here, we explore a class of peculiar polaritons, named plasmon–exciton polaritons (plexcitons), in a hybrid system composed of silver nanodisk arrays and monolayer tungsten-disulfide (WS2), which shows giant room-temperature nonlinearity due to their deep-subwavelength localized nature. Specifically, comprehensive ultrafast pump–probe measurements reveal that plexciton nonlinearity is dominated by the saturation and higher-order excitation-induced dephasing interactions, rather than the well-known exchange interaction in traditional microcavity polaritons. Furthermore, we demonstrate this giant nonlinearity can be exploited to manipulate the ultrafast nonlinear absorption properties of the solid-state system. Our findings suggest that plexcitons are intrinsically strongly interacting, thereby pioneering new horizons for practical implementations such as energy-efficient ultrafast all-optical switching and information processing.

Optimal generation of delay-controlled few-cycle pulses for high harmonic generation in solids

Delay-controlled two-color, few-cycle pulses are powerful tools for ultrafast nonlinear optics. In this Letter, 35-fs, 800 nm pulses were injected into a noble-gas-filled hollow-core fiber to obtain over-octave spectra (450–1000 nm) and were divided into two parts for dispersion management by a Mach–Zehnder–type interferometer. Two few-cycle pulses with pulse widths of 9.3 and 4.5 fs were generated in the long-wavelength side and the short-wavelength side, respectively. The temporal profiles were measured as the function of the different delay between the two pulses. The shortest 3.6 fs, 0.75 mJ near-single-cycle pulses were synthesized at an optimal delay. The delay-controlled high-harmonic generation in MgO was experimentally demonstrated leading to twofold enhancement of high-order harmonic (HH) yields at 10.3 eV and the extension of HH frequency under time-delay modulation. This method provides an extensive way for manipulating delay-controlled multi-color pulses, which can be used for controlling ionization dynamics in extreme nonlinear optics. We believe that it will be a powerful tool for ultrafast science.

Mode-locked fiber laser with coexistence of m ultiple solitons and noise-like pulses

Dissipative solitons (DSs) usually play an important role in understanding the intricate phenomena in various nonlinear systems. As a special regime in the dissipative system, noise-like pulses (NLPs) can have typical characteristics of ultra-broad and smooth spectrum, high pulse energy and low temporal coherence, making them a good candidate for many applications, including supercontinuum generation, industrial micromachining and optical metrology. In this paper, a noteworthy observation concerning the dynamics on coexistence of the multiple solitons and NLPs operation in a net-normal-dispersion passively mode-locked fiber laser based on nonlinear amplifying loop mirror (NALM) is reported. In the experiment, the stable DSs can be easily obtained at a proper pump power. When appropriately increasing the pump power and changing the polarization state, the DS operation can change to the NLP regime. When the fiber laser operates in an NLP state, the single soliton bunch contains multiple pulses with different temporal spacings. And the temporal interval between the adjacent pulses is in a range of several hundred picoseconds, which decreases from left to right with time changing, indicating that there are long-distance interactions among these multiple pulses and they gradually become stronger and stronger. Besides, the pulse number of single soliton bunches on the NLP operation increases almost linearly with pump power increasing. At a maximum pump power, there are eight pulses inside the single soliton bunch. With the increase of pump power, the average output power and pulse energy of these multiple solitons in the NLP state increase. The maximum average output power and pulse energy are 12.3 mW and 1.65 nJ, respectively. In addition, the real-time dynamic evolution of these multiple solitons in the NLP state is investigated by using the time-stretch dispersive Fourier-transform method. The results show that all the pulses in NLP regime actually consist of chaotic noise waves with stochastic intensities. We believe that this paper will be of significance in studying ultrafast fiber lasers and nonlinear optics. Moreover, we hope that these findings will be helpful in understanding the physical mechanism of NLPs and paving the way for exploring other complex soliton dynamics.

Investigation of ultrafast broadband optical nonlinearity and intensity-dependent nonlinear absorption in novel hydrazone derivatives

Two novel hydrazone derivatives (BTH-1 and BTH-2) were designed and synthesized to investigate the modulation of intramolecular charge transfer (ICT) and planar π conjugation on optical nonlinearities. Femtosecond Z-scan measurements show that trithiophene-substituted BTH-2 exhibits stronger broadband (600–900 nm) reverse saturable absorption (RSA) resulting from two-photon absorption (TPA)-induced excited state absorption (ESA). Combined with quantum chemical calculations, the results indicate that the local excitation and spatial delocalization enhanced by planarized trithiophene are more conducive to promoting the nonlinear optical (NLO) response of hydrazone molecules than the ICT introduced by twisted triphenylamine. In addition, the intensity-dependent transition from saturable absorption to RSA of BTH-2 at 532 nm under multiple pulse widths (fs, ps, ns) was explored. Transient absorption spectroscopy provided information on the excited state dynamics of the compounds. This work extends NLO research on hydrazone derivatives and provides a reference for the design of hydrazone molecules with high nonlinearity. The results also suggest that BTH-2 is a promising candidate for optical limiting applications.

Modulation of naphthanthryl chalcone derivatives by push-pull electronic substituents: Ultrafast nonlinear absorption and transient dynamics

The ultrafast optical nonlinearities of two novel naphthanthryl chalcone derivatives (NAn-1 and NAn-2) with different push-pull effects were investigated and compared. Combined with femtosecond Z-scan and quantum chemical calculations, the results indicate that both compounds exhibited broadband (532–800 nm) two-photon-induced excited-state absorption, and NAn-2 exhibited wider spatial electron delocalization. The push electronic effects of the peripheral substituent increased the transition dipole moment, originating from the main nonlinear group retained stronger local excitation and ultimately enhanced the nonlinear absorption of NAn-2. Transient absorption spectroscopy revealed a transition from the locally excited to charge transfer state and showed that the dynamic processes of excited states were readily tunable via peripheral push-pull substituents. The results suggest that NAn-2 possess the potential in optical limiting applications and provide guidance for designing polycyclic aromatic hydrocarbon (PAH)-based nonlinear optical materials.

Efficient simulation of ultrafast quantum nonlinear optics with matrix product states

Ultrashort pulses propagating in nonlinear nanophotonic waveguides can simultaneously leverage both temporal and spatial field confinement, promising a route towards single-photon nonlinearities in an all-photonic platform. In this multimode quantum regime, however, faithful numerical simulations of pulse dynamics naïvely require a representation of the state in an exponentially large Hilbert space. Here, we employ a time-domain, matrix product state (MPS) representation to enable efficient simulations by exploiting the entanglement structure of the system. To extract physical insight from these simulations, we develop an algorithm to unravel the MPS quantum state into constituent temporal supermodes, enabling, e.g., access to the phase-space portraits of arbitrary pulse waveforms. As a demonstration, we perform exact numerical simulations of a Kerr soliton in the quantum regime. We observe the development of non-classical Wigner-function negativity in the solitonic mode as well as quantum corrections to the semiclassical dynamics of the pulse. A similar analysis of χ ( 2 ) simultons reveals a unique entanglement structure between the fundamental and second harmonics. Our approach is also readily compatible with quantum trajectory theory, allowing full quantum treatment of propagation loss and decoherence. We expect this work to establish the MPS technique as part of a unified engineering framework for the emerging field of broadband quantum photonics.

Recent research progress of Mamyshev oscillator for high energy and ultrashort pulse generation

The potential applications of Mamyshev oscillator in the generation of high-energy ultrashort pulses have aroused extensive research interest. This review focuses on the latest research progress of Mamyshev oscillator. Firstly, the working mechanism of Mamyshev oscillator is introduced. Then, the research results of Mamyshev oscillator in recent years are summarized according to three different wavebands of 1 μm, 1.5 μm and 2 μm. The Mamyshev oscillator can effectively improve the laser pulse energy and shorten the pulse duration, which has great advantages in industrial applications. Meanwhile, it contains abundant nonlinear effects and can be used as an excellent platform for nonlinear optical system, which stimulates the exploitation of nonlinear optics and promoting the development of ultrafast laser technology and nonlinear optics.

Strong near-infrared and ultrafast femtosecond nonlinearities of a covalently-linked triply-fused porphyrin dimer-SWCNT nanohybrid

Functional materials displaying large ultrafast third-order optical nonlinearities across a wide spectral region and broad temporal domain are required for all-optical signal processing. Particularly desirable is nonlinear optical (NLO) activity at near-infrared (NIR) wavelengths with femtosecond pulses. Herein the first triply-fused porphyrin dimer (TFP)-functionalized single-walled carbon nanotube (SWCNT) nanohybrid was successfully constructed by covalently grafting TFPs onto SWCNT. The results of Z-scan techniques demonstrate that the newly obtained TFP-SWCNT nanohybrid was found with a strong NLO performance under both nanosecond and femtosecond irradiation. In the nanosecond regime, an enhancement in optical limiting (OL) of the TFP-SWCNT nanohybrid is seen at 532 nm when compared with the performance of porphyrin monomer-functionalized SWCNT nanohybrid Por-SWCNT. Under femtosecond irradiation, the TFP-SWCNT nanohybrid exhibits a particularly strong OL effect with a giant two-photon absorption (TPA) cross section value (ca. 15,500 GM) at 800 nm pulses that mainly stems from intense TPA of TFP, in sharp contrast to the Por-SWCNT nanohybrid which exhibits only saturable absorption under identical irradiation. These results demonstrate that the newly-developed TFP-SWCNT nanohybrid is a very promising OL candidate for practical applications across wide spectral and temporal domains, and that covalently functionalizing carbon-based materials with triply-fused chromophores may be a useful approach to engineering adaptable photonic devices with broad-ranging NLO activity.

Optical power limiter in the femtosecond filamentation regime

We present the use of a power limiting apparatus to evaluate ultrafast optical nonlinearities of transparent liquids (water and ethanol) in the femtosecond filamentation regime. The setup has been previously employed for the same purpose, however, in a longer pulsewidth (> 20 ps) regime, which leads to an ambiguous evaluation of the critical power for self-focusing. The uncertainty originates from the existence of a threshold power for optical breakdown well below the critical power for self-focusing within this timeframe. Contrarily, using the proposed apparatus in the femtosecond regime, we observe for the first time a unique optical response, which features the underlying physics of laser filamentation. Importantly, we demonstrate a dependence of the optical transmission of the power limiter on its geometrical, imaging characteristics and the conditions under which a distinct demarcation for the critical power for self-focusing can be determined. The result is supported by numerical simulations, which indicate that the features of the observed power-dependent optical response of the power limiting setup are physically related to the spontaneous transformation of the laser pulses into nonlinear conical waves.

Investigation of the intensity dependent transition from saturable absorption to reverse saturable absorption and ultrafast negative refraction in terthiophene-based chalcone derivatives

Two novel chalcone derivatives C12 & C13 are designed and synthesized. Terthiophene group is employed to provide the planar π-conjugated system in these molecules while the molecular planarity is tuned by the different substitutions at the terminal group. The ultrafast optical nonlinearities are investigated via transient absorption spectrum and Z-scan. It is generally assumed that a large planar π-system and strong intramolecular charge transfer can enhance the optical nonlinearities in organic nonlinear optical materials. However, the molecule with larger planar molecular structure displayed weaker nonlinear absorption due to the competition between saturable absorption and reverse saturable absorption. With DFT calculation, the structure-property relation and the enhancement of π-conjugated system on nonlinear absorption and refraction are discussed. The investigations and discussions may provide a different perspective of the nonlinear absorption and refraction in these organic molecules and the results also suggest that these chalcone derivatives are potential nonlinear refraction materials for all-optical applications. • Two terthiophene-based chalcone derivatives are designed and synthesized. • The transition from SA to RSA and the negative refraction are investigated. • Both compounds are low-loss nonlinear optical refraction materials.

Third-order nonlinear optical responses of CuO nanosheets for ultrafast pulse generation

As a representative transition metal oxide, cupric oxide (CuO) has attracted a lot of interest in miscellaneous fields. In the present work, the prominent third-order nonlinear optical (NLO) features of CuO nanosheets were demonstrated via the typical Z-scan technique at 1 μm. The open-aperture (OA) Z-scan measurements at different intensities clearly showed that CuO nanosheets possessed the saturable absorption (SA), reverse saturable absorption (RSA) and optical limiting behaviors. The closed-aperture (CA) Z-scan technology was implanted to investigate the nonlinear refractive index and the third-order nonlinear susceptibility. In virtue of the strong nonlinear optical absorption properties of CuO nanosheets, a stable all-solid-state mode-locked laser with the as-prepared CuO nanosheets as saturable absorber at 1.06 μm was realized for the first time. Our work confirmed that CuO nanosheets exhibited outstanding NLO properties, which might stimulate the development in ultrafast photonics and nonlinear optics.

Ultrafast Third-Order Nonlinear Optical Response Excited by fs Laser Pulses at 1550 nm in GaN Crystals.

The ultrafast third-order optical nonlinearity of c-plane GaN crystal, excited by ultrashort (fs) high-repetition-rate laser pulses at 1550 nm, wavelength important for optical communications, is investigated for the first time by optical third-harmonic generation in non-phase-matching conditions. As the thermo-optic effect that can arise in the sample by cumulative thermal effects induced by high-repetition-rate laser pulses cannot be responsible for the third-harmonic generation, the ultrafast nonlinear optical effect of solely electronic origin is the only one involved in this process. The third-order nonlinear optical susceptibility of GaN crystal responsible for the third-harmonic generation process, an important indicative parameter for the potential use of this material in ultrafast photonic functionalities, is determined.

All‐Optical Modulation with Dielectric Nanoantennas: Multiresonant Control and Ultrafast Spatial Inhomogeneities

The transient optical response of multiresonant all‐dielectric nanoantennas via a combination of broadband ultrafast reflectivity experiments and nonlinear optics nanoscale modeling is studied. Ultrafast all‐optical control of the reflectivity is demonstrated in variably sized nanoantennas over four distinct Mie resonances (including Fano‐like resonances), spanning a broad spectral range, from the red to the near‐infrared. A spatially inhomogeneous dynamical model, which accounts for diffusion of the photogenerated carriers inside the semiconductor, is introduced and exploited to isolate the physical phenomena leading to the overall transient response, namely, Drude plasma formation and Pauli blocking following band filling and thermo‐optical effect. The results pave the way to the development of multiwavelength all‐optically reconfigurable filters for next‐generation ultrafast add/drop multiplexing.

Ultrafast Nonlinear Optical and Structure-Property Relationship Studies of Pyridine-Based Anthracene Chalcones Using Z-Scan, Degenerate Four-Wave Mixing, and Computational Approaches.

The structural, thermal, linear, and femtosecond third-order nonlinear optical (NLO) properties of two pyridine-based anthracene chalcones, (2E)-1-(anthracen-9-yl)-3-(pyridin-2-yl)prop-2-en-1-one (2PANC) and (2E)-1-(anthracen-9-yl)-3-(pyridin-3-yl)prop-2-en-1-one (3PANC), were investigated. These two chalcones were synthesized following the Claisen-Schmidt condensation method. Optically transparent single crystals were achieved using a slow evaporation solution growth technique. The presence of functional groups in these molecules was established by Fourier transform infrared and NMR spectroscopic data. The detailed solid-state structure of both chalcones was determined from the single-crystal X-ray diffraction data. Both crystals crystallized in the centrosymmetric triclinic space group P1̅ with the nuance of unit cell parameters. The crystals (labeled as 2PANC and 3PANC) have been found to be transparent optically [in the entire visible spectral region] and were found to be thermally stable up to 169 and 194 °C, respectively. The intermolecular interactions were investigated using the Hirshfeld surface analysis, and the band structures (highest occupied molecular orbital-lowest unoccupied molecular orbital, excited-state energies, global chemical reactivity descriptors, and molecular electrostatic potentials) were studied using density functional theory (DFT) techniques. The ultrafast third-order NLO properties were investigated using (a) Z-scan and (b) degenerate four-wave mixing (DFWM) techniques using ∼50 fs pulses at 800 nm (1 kHz, ∼4 mJ) from a Ti:sapphire laser amplifier. Two-photon-assisted reverse saturable absorption, self-focusing nonlinear refraction, optical limiting, and optical switching behaviors were witnessed from the Z-scan data. 3PANC demonstrated a stronger two-photon absorption coefficient, while 2PANC depicted a stronger nonlinear refractive index among the two. The time-resolved DFWM data demonstrated that the decay times of 2PANC and 3PANC were ∼162 and ∼180 fs, respectively. The second hyperpolarizability (γ) values determined by DFT, Z-scan, and DFWM were found to be in good correlation (with a magnitude of ∼10-34 esu). The ultrafast third-order NLO response, significant NLO properties, and thermal stability of these chalcones brands them as potential candidates for optical power limiting and switching applications.