Ultrafast Optical Nonlinearity Research Articles

Femtosecond Third-Order Nonlinear Electronic Responses of 2D Metallic NbSe2

This manuscript reports on the third-order nonlinear optical responses of two-dimensional metallic NbSe2 suspended in acetonitrile (ACN). The standard Z-scan technique was employed with 190 fs optical pulses at 790 nm, a repetition rate of 750 Hz, and an intensity ranging from 30 to 300 GW/cm2. A self-focusing nonlinear refractive index (NLR), n2=+(1.8±0.1)×10−15 cm2/W, and a nonlinear absorption (NLA) coefficient, α2=+(3.5±0.2)×10−2 cm/GW, were measured, with the NLA arising from a two-photon process. Aiming to further understand the material’s electronic nonlinearities, we also employed the Optical Kerr Gate (OKG) to evaluate the material’s time response and measure the NLR coefficient in an optical intensity range different from the one used in the Z-scan. For optical pulses of 170 fs at 800 nm and a repetition rate of 76 MHz, the modulus of the NLR coefficient was measured to be n2=4.2±0.5×10−14 cm2/W for intensities up to 650 MW/cm2, with the material’s time response limited by the pulse duration. The ultrafast time response and electronic optical nonlinearities are explained based on the material’s 2D structure.

Push-Pull Carbazole-Based Dyes: Synthesis, Strong Ultrafast Nonlinear Optical Response, and Effective Photoinitiation for Multiphoton Lithography.

The present work reports on the ultrafast nonlinear optical (NLO) properties of a series of D-π-Α and D-A push-pull carbazole-based dyes and establishes a correlation between these properties and their efficiency for potential photonic and optoelectronic applications such as multiphoton lithography (MPL). The ultrafast NLO properties of the studied dyes are determined by two distinct experimental techniques, Z-scan and pump-probe optical Kerr effect (OKE), employing 246 fs laser pulses at 515 nm. The results indicate that chemical functionalization of the carbazole moiety with various strong electron-donating and/or electron-withdrawing groups, such as benzene, styrene, 4-bromostyrene, nitrobenzene, trimethyl isocyanurate, methyl, and indane-1,3-dione, can result in a controlled and significant enhancement of the NLO absorptive and refractive responses. In the context of potential applications, the efficiency of carbazole-based organic materials as photoinitiators (PIs) for MPL applications is demonstrated. The fabricated woodpile microstructure using chemically functionalized carbazole as a PI demonstrates improvements in both feature size and MPL efficiency compared to that using unfunctionalized carbazole as a PI. This is attributed to the efficient charge transfer resulting from chemical functionalization, which leads to a substantial increase (approximately 1 order of magnitude) in the values of the imaginary part of the second-order hyperpolarizability (Imγ) and the two-photon absorption cross section (σ). The achieved feature size of 280 nm is comparable to that obtained with other widely used PIs in MPL applications. Additionally, owing to the strong NLO properties of the studied functionalized carbazole, they could also be promising candidates for further applications in photonics and optoelectronics.

Watt‐Level Second‐Order Topological Charge Ultrafast Green Vortex Laser with Quasi ‐2D PEA2(CsPbBr3)n‐1PbBr4 Perovskite Films Saturable Absorber

AbstractUltrafast vortex beams have significant scientific and practical value because of their unique phase properties in both the longitudinal and transverse modes, enabling multi‐dimensional quantum control of light fields. Directly generating watt‐level ultrafast vortex beams with large angular momentum has remained a major challenge due to the limitations of mode‐locked materials and existing spatiotemporal mode‐locking generation methods. In this study, quasi‐2D PEA2(CsPbBr3)n‐1PbBr4 perovskite films are prepared by an anti‐solvent method and employed for the first time in a mode‐locked resonator operating in free space. Utilizing the angle‐based non‐collinear pumping and frequency doubling techniques, the second‐order ultrafast green vortex beams with a power of up to 1.05 W and a duration of 373 ps are generated. Experimental findings demonstrate the strong nonlinear saturable absorption properties of quasi‐2D PEA2(CsPbBr3)n‐1PbBr4 perovskite films at high power levels, highlighting their considerable potential in ultrafast laser technology and nonlinear optics.

Ultrafast second-order nonlinear photonics—from classical physics to non-Gaussian quantum dynamics: a tutorial

Photonic integrated circuits with second-order (χ(2)) nonlinearities are rapidly scaling to remarkably low powers. At this time, state-of-the-art devices achieve saturated nonlinear interactions with thousands of photons when driven by continuous-wave lasers, and further reductions in these energy requirements enabled by the use of ultrafast pulses may soon push nonlinear optics into the realm of single-photon nonlinearities. This tutorial reviews these recent developments in ultrafast nonlinear photonics, discusses design strategies for realizing few-photon nonlinear interactions, and presents a unified treatment of ultrafast quantum nonlinear optics using a framework that smoothly interpolates from classical behaviors to the few-photon scale. These emerging platforms for quantum optics fundamentally differ from typical realizations in cavity quantum electrodynamics due to the large number of coupled optical modes. Classically, multimode behaviors have been well studied in nonlinear optics, with famous examples including soliton formation and supercontinuum generation. In contrast, multimode quantum systems exhibit a far greater variety of behaviors, and yet closed-form solutions are even sparser than their classical counterparts. In developing a framework for ultrafast quantum optics, we identify what behaviors carry over from classical to quantum devices, what intuition must be abandoned, and what new opportunities exist at the intersection of ultrafast and quantum nonlinear optics. Although this article focuses on establishing connections between the classical and quantum behaviors of devices with χ(2) nonlinearities, the frameworks developed here are general and are readily extended to the description of dynamical processes based on third-order χ(3) nonlinearities.

Mesoscopic ultrafast nonlinear optics—the emergence of multimode quantum non-Gaussian physics

Over the last few decades, nonlinear optics has become significantly more nonlinear, traversing nearly a billionfold improvement in energy efficiency, with ultrafast nonlinear nanophotonics in particular emerging as a frontier for combining both spatial and temporal engineering. At present, cutting-edge experiments in nonlinear nanophotonics place us just above the mesoscopic regime, where a few hundred photons suffice to trigger highly nonlinear dynamics. In contrast to classical or deep-quantum optics, the mesoscale is characterized by dynamical interactions between mean-field, Gaussian, and non-Gaussian quantum features, all within a close hierarchy of scales. When combined with the inherent multimode complexity of optical fields, such hybrid quantum-classical dynamics present theoretical, experimental, and engineering challenges to the contemporary framework of quantum optics. In this review, we highlight the unique physics that emerges in multimode nonlinear optics at the mesoscale and outline key principles for exploiting both classical and quantum features to engineer novel functionalities. We briefly survey the experimental landscape and draw attention to outstanding technical challenges in materials, dispersion engineering, and device design for accessing mesoscopic operation. Finally, we speculate on how these capabilities might usher in some new paradigms in quantum photonics, from quantum-augmented information processing to nonclassical-light-driven dynamics and phenomena to all-optical non-Gaussian measurement and sensing. The physics unlocked at the mesoscale present significant challenges and opportunities in theory and experiment alike, and this review is intended to serve as a guide to navigating this new frontier in ultrafast quantum nonlinear optics.

Giant excited-state absorption in resonant absorption band and intensity-depend ultrafast sign switching of nonlinear absorption in azonaphthalene compound

The ultrafast optical nonlinearity of an azonaphthalene derivative, hydroxy naphthol blue (HNB) disodium salt, is investigated using transient absorption spectra (TAS) and Z-scan technique. Reverse saturable absorption (RSA) is observed within the resonant absorption band, which is usually dominated by ground-state bleaching (GSB) and stimulated emission (SE) in most organic compounds. This observation indicates a remarkably strong excited-state absorption (ESA) in HNB. Global analysis of TAS suggests an ultrafast conversion from saturable absorption (SA) to RSA, which is assigned to the internal conversion from locally excited (LE) state to the first singlet (S1) state. Further Z-scan study verifies the above results and reveals another intensity-depend SA-RSA transition, indicating increased S1 population under strong laser irradiation. The calculated value of third-order nonlinear absorption coefficient at 650 nm, 190 fs is determined as 1.23 × 10−12 m/W. These studies demonstrate significant potential of azonaphthalene in ultrafast laser protection if further modulation of excited-state absorption can be achieved.

Nanophotonics with Plasmonic Nanorod Metamaterials

AbstractTaking advantage of their unique and tuneable electromagnetic properties, plasmonic metamaterials constitute a versatile platform for a variety of applications ranging from high‐resolution imaging, sensing and spontaneous emission engineering to ultrafast nonlinear optics and light polarization control. Here, recent advances in the design and applications of plasmonic metamaterials based on aligned metallic nanorod assemblies are reviewed, and the fast‐developing trends in their exploitation in nanophotonics are outlined. The fabrication of the nanorod‐based metamaterials is introduced and their linear and nonlinear optical properties are presented from both microscopic and phenomenological considerations. Multiscale structuring allowing precise engineering of the electromagnetic modes supported by the nanorod metamaterials, as well as nonlocal spatial dispersion effects and their impact on nanophotonic performance are discussed. To illustrate the developing field of practical applications of these metamaterials, some of their main application domains in sensing, photochemistry and nonlinear optics are overviewed and novel designs of anisotropic metamaterials directly derived from the nanorod architecture are introduced.

Ultrafast Dynamics, Optical Nonlinearities, and Chemical Sensing Application of Free-Standing Porous Silicon-Based Optical Microcavities.

The present work demonstrates the ultrafast carrier dynamics and third-order nonlinear optical properties of electrochemically fabricated free-standing porous silicon (FS-PSi)-based optical microcavities via femtosecond transient absorption spectroscopy (TAS) and single-beam Z-scan techniques, respectively. The TAS (pump: 400 nm, probe: 430-780 nm, ∼70 fs, 1 kHz) decay dynamics are dominated by the photoinduced absorption (PIA, lifetime range: 4.7-156 ps) as well as photoinduced bleaching (PIB, 4.3-324 ps) for the cavity mode (λc) and the band edges. A fascinating switching behavior from the PIB (-ve) to the PIA (+ve) has been observed in the cavity mode, which shows the potential in ultrafast switching applications. The third-order optical nonlinearities revealed an enhanced two-photon absorption coefficient (β) in the order of 10-10 mW-1 along with the nonlinear refractive index (n2) in the range of 10-17 m2 W-1. Furthermore, a real-time sensing application of such FS-PSi microcavities has been demonstrated for detecting organic solvents by simultaneously monitoring the kinetics in reflection and transmission mode.

Pulse buildup dynamics in a self-starting Mamyshev oscillator.

The Mamyshev oscillator (MO) can generate high-performance pulses. However, due to their non-resonant cavities, they usually are not self-starting, and there is almost no effort to reveal the pulse buildup dynamics of the MO. This paper investigates the dynamic of single pulse (SP) and multi-pulse formation in a self-starting MO. It indicated that both SP self-starting and multi-pulse self-starting can be obtained by adjusting the oscillator parameters. More importantly, increasing pump power could only result in bound state pulses (BSPs) if SP self-starting was formed. With the increase of the pump power, the pulse number in BSPs would increase. However, multiple pulses could not be formed only by increasing the pump power, and the BSPs obtained here underwent SP generated from noise, amplified, and then bounded, which is different from conventional passive mode-locked fiber lasers (CPMLFLs). On the other hand, if multiple pulses were self-initiated, BSPs, pulse bunch, and harmonic mode-locked pulses (HMLPs) could be obtained by adjusting the polarization state and pump power in the cavity. Furthermore, once any of the above states are formed, if the oscillator polarization state and filter interval are unchanged, only increasing the pump power from zero, the original state can still be obtained, which is consistent with the characteristics of the CPMLFLs. These findings will provide new insights into the pulse dynamics of self-starting MO, which will be significant for studying ultrafast laser technology and nonlinear optics.

Violet phosphorene as a saturable absorber for controllable soliton molecule generation in a mode-locked fiber laser

Controllable soliton molecules were generated in a Er-doped mode-locked fiber laser with a few-layered violet phosphorene saturable absorber.

Revealing the pulse dynamics in a Mamyshev oscillator: from seed signal to oscillator pulse.

The Mamyshev oscillator (MO) is a promising platform to generate high-peak-power pulse with environmentally stable operation. However, rare efforts have been dedicated to unveil the dynamics from seed signal to oscillator pulse, particularly for the multi-pulse operation. Herein, we investigate the buildup dynamics of the oscillator pulse from the seed signal in a fiber MO. It is revealed that the gain competition among the successively injected seed pulses leads to higher pump power that is required to ignite the MO, hence resulting in the higher optical gain that supports buildup of multiple oscillator pulses. The multiple oscillator pulses are identified to be evolved from the multiple seed pulses. Moreover, the dispersive Fourier transform (DFT) technique is used to reveals the real-time spectral dynamics during the starting process. As a proof-of-concept demonstration, a highly intensity-modulated pulse bunch was employed as the seed signal to reduce the gain competition effect and avoid the multi-pulse starting operation. The experimental results are verified by numerical simulations. These findings would give new insights into the pulse dynamics in MO, which will be meaningful to the communities interested in ultrafast laser technologies and nonlinear optics.

Highly nonlinear optic nucleic acid thin-solid film to generate short pulse laser

Using aqueous precursors, we report successfully fabricating thin-solid films of two nucleic acids, ribonucleic acid (RNA) and deoxyribonucleic acid (DNA). We investigated the potential of these films deposited on a fiber optic platform as all-fiber integrated saturable absorbers (SAs) for ultrafast nonlinear optics. RNA-SA performances were comparable to those of DNA-SA in terms of its nonlinear transmission, modulation depth, and saturation intensity. Upon insertion of these devices into an Erbium-doped fiber ring-laser cavity, both RNA and DNA SAs enabled efficient passive Q-switching operation. RNA-SA application further facilitated robust mode-locking and generated a transform-limited soliton pulse, exhibiting a pulse duration of 633 femtoseconds. A detailed analysis of these pulsed laser characteristics compared RNA and DNA fiber optic SAs with other nonlinear optic materials. The findings of this research establish the feasibility of utilizing RNA as a saturable absorber in ultrafast laser systems with an equal or higher potential as DNA, which presents novel possibilities for the nonlinear photonic applications of nucleic acid thin solid films.

Conversion from Q-switched to bright-dark soliton pair mode-locked operation in an InSb based erbium-doped fiber laser

In this experiment, stable Q-switched pulses and bright-dark soliton pairs were realized in an InSb based erbium-doped fiber laser. Firstly, when the pump power was between 70 and 115 mW, a stable passive Q-switched operation with a central wavelength of 1565.38 nm was achieved, and the signal-to-noise ratio (SNR) was about 37 dB. As the pump power increased, the repetition frequency of the Q-switched pulse can be increased from 4.0145 to 10.623 kHz. When the pump power was increased to the range of 185 to 450 mW, stable bright-dark soliton pairs mode-locked operation was realized, and the two peaks of the spectrum were located at 1568.67 and 1569.34 nm, respectively. The pulse repetition rate was 3.419 MHz, and the SNR was about 59 dB. This research will broaden the application of InSb in ultrafast optics and nonlinear optics.

Polarization-dependent ultrafast optical nonlinearities of N,N-dimethylformamide at 400 nm

Polarization-dependent ultrafast optical nonlinearities of N,N-dimethylformamide at 400 nm

Interfacial modification of GO-FePt hybrid film leads to giant ultrafast optical nonlinearity

Excellent optical nonlinearity is highly promising for the development of multifunctional ultrafast photonics techniques and integrated optoelectronic devices. However, existing numerous optical materials commonly suffer from several challenges, such as bad functional integration, slow response speed, and weak optical nonlinearity thus severely hindering their extensive applications. Here, we first engineer new scalable graphene oxide (GO)-FePt films by chemistry induced self-assembly and then demonstrate the enhanced ultrafast optical nonlinearity by resorting to their interfacial modifications. It is found that the FePt magnetic nanoparticles (NPs) are easily assembled on the surface of the GO by exchanging the surface ligands of the former with evaporated solvent, leading to good water solubility and super-paramagnetism. The femtosecond Z-scan test results show that both the nonlinear saturation absorption and optical Kerr refraction of the pure GO are subjected to reversion once the FePt NPs are introduced. More importantly, we can greatly enhance the ultrafast nonlinear optics response of as-prepared GO-FePt hybrid film by promoting the concentration of magnetic NPs. In addition, the associated optical nonlinearity can be further boosted with femtosecond vectorial beams excitation instead of the linearly polarized one. In principle, the enhanced optical nonlinearity may arise from direct metal-to-semiconductor interfacial charge transfer transition (DICTT) related to the difference in work function and Fermi level together with complicated interaction between the vectorial light fields and the hybrid films. The GO-based magnetic hybrid films with giant ultrafast optical nonlinearity have potential wide-ranging applications in integrated optoelectronics, ultrafast nanophotonics, opto-magnetic storage, and beyond.

The Lagrangian structure, the Euler equation, and second Newton’s law of ultrafast nonlinear optics

With a notable exception of space–time variable swap, pulse evolution equations of ultrafast optics are mathematically similar to the equations of quantum mechanics and beam dynamics. The Lagrangian structure of these equations is, however, much less intuitive. Here, we show that such a structure can be identified via a path-integral analysis of the pulse evolution equation, offering useful insights into the Lagrangian underpinning of ultrafast nonlinear optics. The Euler–Lagrange equation applied to the optical analog of the Lagrange function leads to a second-order differential equation that parallels in its structure second Newton’s law. Stationary-phase space–time paths found by solving such an equation reveal the hidden inner workings behind a vast class of field-waveform transformations in ultrafast optics, including the buildup of nonlinear phase, modulation instabilities, and soliton breather dynamics.

Highly stable femtosecond pulse generation enabled by the indium tin oxide nanocrystals

The ultrafast third-order optical nonlinearity of indium tin oxide nanocrystals (ITO NCs) and their application in femtosecond laser generation have been investigated experimentally. The ITO NCs exhibit a large modulation depth of ∼25%, nonlinear refractive behavior with self-focusing, ultrafast carrier recovery time of ∼300 fs, and high damage threshold of ∼1.16 TW cm−2, and the stable femtosecond Er-doped fiber laser can be delivered with a signal-to-noise ratio over 80 dB modulated by the ITO NCs successfully. The experimental results indicate that the ITO NCs can be excellent ultrafast nonlinear optical materials for developing highly stable photonic and optoelectronic devices.

Ultrafast optical nonlinearity in natural van der Waals heterostructure nanosheets of franckeite

Franckeite, a natural van der Waals heterostructure with excellent physicochemical characteristics, has shown great potential for high-performance optoelectronic device. Here, the few-layer franckeite nanosheets have been prepared by liquid phase-exfoliation method successfully, and the nonlinear optical absorption and carrier dynamics behaviors of the nanosheets have been studied experimentally. The franckeite nanosheets show wavelength- and intensity-dependent nonlinear absorption characteristics, and exhibit ultrafast carrier dynamic process. The ultrafast optical nonlinearity in franckeite nanosheets has been further validated via an Er3+-doped fiber laser to deliver stable femtosecond pulse. The experimental results reveal that franckeite heterostructure nanosheets can be an ideal candidate in the design and manufacture of ultrafast nonlinear optoelectronic devices.

High-contrast optical bistability using a subwavelength epsilon-near-zero material.

Optical bistability opens up a promising avenue toward various optical nonlinear functions analogous to their electrical counterparts, such as switches, logic gates, and memory. Free-space bistable devices have unique advantages in large-scale integration. However, most proposed free-space schemes for optical bistability have limitations in one or more aspects of low contrast ratio, compromised compatibility, slow switching speed, and bulk size. Epsilon-near-zero (ENZ) materials have recently shown an ultrafast and giant optical nonlinearity within a subwavelength scale, potentially overcoming these obstacles. Using large-mobility indium-doped cadmium oxide (CdO) as the ENZ material, we numerically demonstrate two efficient schemes for high-contrast optical bistability within a deep subwavelength size based on the ENZ mode and the Berreman mode. The ENZ wavelength can be optically tuned with a typical time scale of sub-picoseconds, giving rise to a switchable bistability between the near-zero state and the high-reflection state. Our work contributes to the advances on compact and ultrafast all-optical signal processing.

MoxTa(1-x)Se2 as saturable absorber for ultrafast photonics

Two-dimension ternary transition metal dichalcogenides have drawn great interests from both the fields of nanotechnology and materials science, due to their extraordinary physical performance, and great potential applications in nanodevice. Here, the applications of MoxTa(1-x)Se2 nanosheets in ultrafast photonics are discussed. The MoxTa(1-x)Se2 nanosheets are prepared by liquid phase exfoliation method. A MoxTa(1-x)Se2-based saturable absorber is fabricated by depositing these nanosheets onto the side surface of d-shaped fiber, which is inserted into a Er-doped fiber laser cavity. By adjusting polarization state and pump power, both harmonic mode-locking and large energy mode-locking operations are realized, respectively. In the former state, a 56th harmonic mode-locking is obtained, which corresponds to a repetition rate of 312.5 MHz. For the later state, the maximum average output power of 12.24 mW and single pulse energy of 2.19 nJ are obtained when the pump power is 500mW. The results demonstrate that MoxTa(1-x)Se2 can be widely used in ultrafast photonics and nonlinear optics.