Strong Nonlinear Optical Response Research Articles

Janus Doping of Sulfur into Platinum Diselenide Ribbons.

2D platinum diselenide (PtSe2), a novel member of the transition metal dichalcogenides (TMDCs) family, possesses many excellent properties, including a layer-dependent bandgap, high carrier mobility, and broadband response, making it promise for applications in technologies like field-effect transistors and room-temperature photodetectors. Doping represents an effective method to modify the electrical properties of 2D TMDCs and to bestow upon them additional functions. However, to date, little research has been conducted on the successful doping of 2D PtSe2 for modification. In this study, sulfur (S) powder is utilized during the chemical vapor deposition growth process of 2D PtSe2 ribbons and successfully integrated into the PtSe2 lattice through substitutional doping. The Au substrate significantly decreases the substitution energy of Se atoms in the lower layer of PtSe2, resulting in the formation of the Janus PtSSe structure. S-doped PtSe2 ribbons demonstrate significant symmetry breaking and enhanced electrical properties, showcasing a strong nonlinear optical response and certain synaptic plasticity, further simulating some neuromorphological processes. This study not only demonstrates a viable method for controllable doping and modification of 2D PtSe2 but also establishes a platform for exploring the characteristics of Janus TMDCs.

Wide-Bandgap 2D SnS2-Based All-Optical Photonic Devices with Strong Nonlinear Optical Response due to Spatial Self-Phase Modulation

Wide-Bandgap 2D SnS₂-Based All-Optical Photonic Devices with Strong Nonlinear Optical Response due to Spatial Self-Phase Modulation

Strong chiroptical nonlinearity in coherently stacked boron nitride nanotubes.

Nanomaterials with a large chiroptical response and high structural stability are desirable for advanced miniaturized optical and optoelectronic applications. One-dimensional (1D) nanotubes are robust crystals with inherent and continuously tunable chiral geometries. However, their chiroptical response is typically weak and hard to control, due to the diverse structures of the coaxial tubes. Here we demonstrate that as-grown multiwalled boron nitride nanotubes (BNNTs), featuring coherent-stacking structures including near monochirality, homo-handedness and unipolarity among the component tubes, exhibit a scalable nonlinear chiroptical response. This intrinsic architecture produces a strong nonlinear optical response in individual multiwalled BNNTs, enabling second-harmonic generation (SHG) with a conversion efficiency up to 0.01% and output power at the microwatt level-both excellent figures of merit in the 1D nanomaterials family. We further show that the rich chirality of the nanotubes introduces a controllable nonlinear geometric phase, producing a chirality-dependent SHG circular dichroism with values of -0.7 to +0.7. We envision that our 1D chiral platform will enable novel functions in compact nonlinear light sources and modulators.

Strongly Interacting Photons in 2D Waveguide QED.

One-dimensional confinement in waveguide quantum electrodynamics (QED) plays a crucial role to enhance light-matter interactions and to induce a strong quantum nonlinear optical response. In two or higher-dimensional settings, this response is reduced since photons can be emitted within a larger phase space, opening the question whether strong photon-photon interaction can be still achieved. In this study, we positively answer this question for the case of a 2D square array of atoms coupled to the light confined into a two-dimensional waveguide. More specifically, we demonstrate the occurrence of long-lived two-photon repulsive and bound states with genuine 2D features. Furthermore, we observe signatures of these effects also in free-space atomic arrays in the form of weakly subradiant in-band scattering resonances. Our findings provide a paradigmatic signature of the presence of strong photon-photon interactions in 2D waveguide QED.

Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS4

AbstractImproving polarizability is an important strategy for designing high‐performance mid‐infrared (mid‐IR) nonlinear optical (NLO) materials. The substitution of equivalent or aliovalent atoms can manipulate the polarizability by adjusting the symmetry of the polyhedron. Herein, the Li+ and Cd2+ are introduced into the Cu3PS4 as the equivalent and aliovalent dopants for the Cu site. As a result, Li+ can significantly improve the bandgap (Eg) of LixCu3−xPS4 from 2.38 to 2.88 eV, leading to a higher laser‐induced damage threshold (LIDT) of 4.9 times than AgGaS2 (AGS) with a comparable second harmonic generation (SHG) response of AGS (26−45 µm). Interestingly, Cd2+ can improve the SHG response and enlarge the Eg simultaneously. As a result, Cd0.4Cu2.2PS4 has a large SHG response of 10 × AGS at 2050 nm (26−45 µm) and a LIDT of 2.6 × AGS. Theoretical calculations reveal that lattice vacancies induced by Cd2+ significantly boost polarizability compared to LixCu3−xPS4 with no vacancy, leading to a strong NLO response.

Rational Combination of π-Conjugated and Non-π-Conjugated Groups Achieving Strong Nonlinear Optical Response, Large Optical Anisotropy, and UV Light-Switchable Fluorescence.

Combining π-conjugated and non-π-conjugated groups is an important strategy for synthesizing new nonlinear optical (NLO) crystals. However, the second harmonic generation (SHG) response and optical anisotropy can be limited by improper spatial alignment of these functional groups in the crystal structure. In this work, it is revealed that non-π-conjugated [NH2SO3] group acts as both hydrogen bond donor and acceptor, effectively regulating the 2D planar structure formed by π-conjugated [C4N3H6] groups. The resulting organic-inorganic hybrid crystal C4N3H6SO3NH2 exhibits a strong SHG response (2.5 × KDP), large optical anisotropy (0.233@546nm), and blue-violet and green fluorescence near 360 and 520nm, respectively. This work expands the methodology for creating new NLO crystals through organic-inorganic hybridization, while also showcasing the potential of C4N3H6SO3NH2 as a multifunctional optical material.

Trithionic guanidine: A novel semi-organic short-wave ultraviolet nonlinear optical sulfate with dimeric heteroleptic tetrahedra

Sulfates are always promising short-wave ultraviolet (UV) nonlinear optical (NLO) candidates, if their birefringence could be greatly improved. Here, in terms of the insufficient birefringence, the unity of heteroleptic tetrahedral groups and triangular ones was proposed and implemented. Thus, a new semi-organic crystal, [C(NH2)3]S3O6 (G2S3O6), was obtained, which is composed of [S3O6]2− and [C(NH2)3]+ groups. It exhibits excellent optical properties with a short absorption cutoff edge of 218 nm, a strong NLO response of 1.4 × KH2PO4, and more especially, a large birefringence of 0.097@546 nm. This birefringence leap makes the G2S3O6 crystal achieve a phase-matching behavior under a 532 nm laser. Thus, the synergy of [S3O6]2− and [C(NH2)3]+ groups results in excellent optical performances. This finding opens a new horizon for exploring novel UV NLO crystals.

Emergence of threefold symmetric helical photocurrents in epitaxial low twinned Bi2Se3

We present evidence of a strong circular photon drag effect (PDE) in topological insulators (TIs) through the observation of helicity-dependent topological photocurrents with threefold rotational symmetry using THz spectroscopy in epitaxially-grown Bi2Se3 with reduced crystallographic twinning. We establish how twinned domains introduce competing nonlinear optical (NLO) responses inherent to the crystal structure that obscure geometry-sensitive optical processes through the introduction of a spurious mirror symmetry. Minimizing the twinning defect reveals strong NLO response currents whose magnitude and direction depend on the alignment of the excitation to the crystal axes and follow the threefold rotational symmetry of the crystal. Notably, photocurrents arising from helical light reverse direction for left/right circular polarizations and maintain a strong azimuthal dependence-a result uniquely attributable to the circular PDE, where the photon momentum acts as an applied in-plane field stationary in the laboratory frame. Our results demonstrate new levels of control over the magnitude and direction of photocurrents in TIs and that the study of single-domain films is crucial to reveal hidden phenomena that couple topological order and crystal symmetries.

Wide band gap selenide infrared nonlinear optical materials AIIMg6Ga6Se16 with strong SHG responses and high laser-induced damage thresholds.

Infrared (IR) nonlinear optical (NLO) materials with strong NLO response, wide band gap and high laser-induced damage threshold (LIDT) are highly expected in current laser technologies. Herein, by introducing double alkaline-earth metal (AEM) atoms, three wide band gap selenide IR NLO materials AIIMg6Ga6Se16 (AII = Ca, Sr, Ba) with excellent linear and NLO optical properties have been rationally designed and fabricated. AIIMg6Ga6Se16 (AII = Ca, Sr, Ba) are composed of unique [AIISe6] triangular prisms, [MgSe6] octahedra and [GaSe4] tetrahedra. The introduction of double AEMs effectively broadens the band gaps of selenide-based IR NLO materials. Among them, CaMg6Ga6Se16, achieving the best balance between the second-harmonic generation response (∼1.5 × AgGaS2), wide band gap (2.71 eV), high LIDT (∼9 × AgGaS2), and moderate birefringence of 0.052 @ 1064 nm, is a promising NLO candidate for high power IR laser. Theoretical calculations indicate that the NLO responses and band gaps among the three compounds are mainly determined by the NLO-active [GaSe4] units. The results enrich the chemical diversity of chalcogenides, and give some insight into the design of new functional materials based on the rare [AIISe6] prismatic units.

Prediction of two-dimensional 2H-M2O3 (M = Ti and Zr) with strong linear and non-linear optical response in the infrared range

Single-layer 2H-M2O3 (M = Ti and Zr) is predicted with a strong linear optical and second-harmonic generation response in the infrared range.

The smallest triple-ring tubular gold clusters M2@Au15 with M = Mo, W: stability, electronic properties and nonlinear optical response.

The smallest triple ring tube-like gold clusters M2@Au15q with M = Mo, W and q = 1, 0, -1 are reported for the first time. Incorporation of an M2 dimer results in a remarkable modification of both atomic and electronic structures of the gold host. While the bare Au15 cluster exhibits a 3D cage shape, the doubly doped clusters M2@Au15 in all charge states are found to prefer a tubular form composed of three five-membered Au rings in an anti-prism arrangement and stabilized by an M2 unit placed inside the tube-like Au15 gold framework. The equilibrium geometry of both M2@Au15 and M2@Au15- is not much modified upon electron detachment from or attachment to their pure gold counterpart. The anion M2@Au15- with 28 itinerant electrons establishes an electron shell configuration of 1S21P61D102S21F8, in which the 1F shell splits into four different sub-levels. These stable clusters are thus not magic. Computed results on the first and second hyper-polarizability parameters of the doped clusters show a strong dependence on the charge. Overall, the neutral M2@Au15 is found to exhibit a particularly strong nonlinear optical (NLO) response. These clusters can also be extended to 1D nanowires, providing helpful guidance for the design of novel gold-based nanowires with rich optoelectronic properties.

Strong light-matter interaction and non-linear effects in organic semiconducting CuPc nanotubes: realization of all-optical diode and switching applications.

Spatial self-phase modulation based on the optical Kerr effect has gained momentum in recent years to analyse the nonlinear optical properties of 2D inorganic nanomaterials. In the present work, we investigate the strong light-matter interaction of organic semiconducting materials based on SSPM, by developing Cu-phthalocyanine (CuPc) nanotubes via a solvothermal technique. The low bandgap of CuPc facilitates the study of its nonlinear optical properties for a broad spectrum range from 671 nm to 405 nm. Intense laser light passing through the CuPc dispersion produces concentric diffraction ring patterns at the far field from which high n2 and χ(3) values, 3.667 × 10-5 cm2 W-1 and 2 × 10-3 esu, respectively, are obtained for the 405 nm laser. This strong nonlinear optical response of CuPc has been utilized to realize non-reciprocal light propagation by constructing a CuPc/SnS2 hybrid structure, which makes an effective all-optical photonic diode. In addition, the all-optical switching is presented using CuPc nanotubes based on the spatial cross-phase modulation technique. In this technique a phase change is induced in the weak signal beam modulated by the strong controlling light beam, which helps to produce all-optical logic gates and all-optical switching devices. The experimental findings of this work unravel the potentially powerful applications of CuPc nanotubes in all-optical information transmission and all-optical photonic devices.

Directly seeding epitaxial growth of tungsten oxides/tungsten diselenide mixed-dimensional heterostructures with excellent optical properties

Mixed-dimensional heterostructures have drawn significant attention due to their intriguing physical properties and potential applications in electronic and optoelectronic nanodevices. However, limited by the lattice matching, the preparation of heterostructures is experimentally difficult and the underlying growth mechanism has not been well established. Here, we report a three-step seeding epitaxial growth strategy for synthesizing mixed-dimensional heterostructures of one-dimensional microwire (MW) and two-dimensional atomic thin film. Our growth strategy has successfully realized direct epitaxial growth of WSe2 film on WOx MW and significantly improves the quality of the epitaxial WSe2 monolayer, which is evidenced by the remarkably enhanced photoluminescence (PL). More intriguingly, the as-synthesized WOx MWs exhibit a strong nonlinear optical response due to the enhancement effect of the core (WOx)-shell (WSe2) nanocavity. Our work provides a feasible route for direct growth of WOx-based mixed-dimensional heterostructures, which possess potential applications in high-performance optoelectronic devices.

Berry Curvature Dipole Induced Giant Mid-Infrared Second-Harmonic Generation in 2D Weyl Semiconductor.

Due to its inversion-broken triple helix structure and the nature of Weyl semiconductor, 2D Tellurene (2D Te) is promising to possess a strong nonlinear optical response in the infrared region, which is rarely reported in 2D materials. Here, a giant nonlinear infrared response induced by large Berry curvature dipole (BCD) is demonstrated in the Weyl semiconductor 2D Te. Ultrahigh second-harmonic generation response is acquired from 2D Te with a large second-order nonlinear optical susceptibility (χ(2) ), which is up to 23.3 times higher than that of monolayer MoS2 in the range of 700-1500nm. Notably, distinct from other 2D nonlinear semiconductors, χ(2) of 2D Te increases extraordinarily with increasing wavelength and reaches up to 5.58nmV-1 at ≈2300nm, which is the best infrared performance among the reported 2D nonlinear materials. Large χ(2) of 2D Te also enables the high-intensity sum-frequency generation with an ultralow continuous-wave (CW) pump power. Theoretical calculations reveal that the exceptional performance is attributed to the presence of large BCD located at the Weyl points of 2D Te. These results unravel a new linkage between Weyl semiconductor and strong optical nonlinear responses, rendering 2D Te a competitive candidate for highly efficient nonlinear 2D semiconductors in the infrared region.

Impact of π-Linkers Modifications on Tuning Nonlinear Optical Amplitudes of Pyridoquinazolinone-Based Aromatic Dyes: A Rational Entry to Novel D-π-A NLO Materials

Developing efficient nonlinear optical (NLO) materials is a cutting-edge field of study. The desirability of promising NLO materials for optoelectronic applications drove us to investigate the pyridoquinazolinone-based D-π-A architectured chromophores for predicting proficient NLO compounds. Pyridoquinazolinone-based dye (WL-O) is chosen as a reference and its nine derivatives (ASH1-ASH9) are quantum chemically modeled by inserting variously reported π-linkers into the D-π-A framework. Simulations using DFT and TD-DFT provide insight into how π-linker alteration affects the NLO properties. The potential use of investigated dyes for NLO response applications is confirmed by evaluating photophysical aspects, frontier molecular orbital (FMO), natural population analysis (NPA), molecular electrostatic potential (MEP), the density of state (DOS), transition density matrix (TDM) analysis, and static, frequency-dependent NLO response properties. FMO analysis shows that all dyes’ energy gaps are lower when compared to the reference, resulting in a strong NLO response. The highest absorption wavelength of the studied dyes was found to be in the visible spectrum, as determined by UV-Vis analysis. NPA-based findings demonstrated the movement of the electrons from D to A through π-linkers resulting in the formation of a charge separation state and active NLO sensitivity of the proposed dyes. Moreover, MEP, LOL, and ELF topological investigations are performed to appraise the charge transfer inside ASH1-ASH9 and high NLO characteristics. The robust NLO response revealed the eye-catching linear polarizability(α0 ), first-hyperpolarizability (β), particularly ASH3, with the highest α0 and β0 computed to be 520.44 a.u. and 26166.79 a.u., respectively. Additionally, frequency-dependent hyperpolarizability SHG β(−2ω,ω,ω) and EOPE β(−ω,ω,0) calculations for commonly used lasers were performed at 1907.21, 532, and 1064 nm. ASH3 with terthiophene linker exhibits a striking EOPE β(−ω,ω,0) and SHG β(−2ω,ω,ω) response of 2.94 × 104 a.u. and 3.80 × 104 a.u. respectively at 1907.21 nm. This theoretical framework confirmed that the investigated dyes have fine NLO potential and are recommended for future NLO applications.

First-principles study on AgBi(CrO4)2:An effective infrared nonlinear optical compound

The investigation of nonlinear optical (NLO) materials is critically important in developing laser technologies. The AgBi(CrO4)2 which crystallizes in the tetragonal lattice with a space group of I 4¯ is a potential candidate for the infrared (IR) region due to the large birefringence (Δn = 0.18), strong NLO response than the KDP crystal and the high electro-optical coefficients are justified their good performance NLO applications. The investigation of the elastic constant of AgBi(CrO4)2 indicates the ductile nature and the large piezoelectric coefficients make this crystal has great attention as bifunctional material.

Simultaneous 3D Construction and Imaging of Plant Cells Using Plasmonic Nanoprobe-Assisted Multimodal Nonlinear Optical Microscopy.

Nonlinear optical (NLO) imaging has emerged as a promising plant cell imaging technique due to its large optical penetration, inherent 3D spatial resolution, and reduced photodamage; exogenous nanoprobes are usually needed for nonsignal target cell analysis. Here, we report in vivo, simultaneous 3D labeling and imaging of potato cell structures using plasmonic nanoprobe-assisted multimodal NLO microscopy. Experimental results show that the complete cell structure can be imaged via the combination of second-harmonic generation (SHG) and two-photon luminescence (TPL) when noble metal silver or gold ions are added. In contrast, without the noble metal ion solution, no NLO signals from the cell wall were acquired. The mechanism can be attributed to noble metal nanoprobes with strong nonlinear optical responses formed along the cell walls via a femtosecond laser scan. During the SHG-TPL imaging process, noble metal ions that crossed the cell wall were rapidly reduced to plasmonic nanoparticles with the fs laser and selectively anchored onto both sides of the cell wall, thereby leading to simultaneous 3D labeling and imaging of the potato cells. Compared with the traditional labeling technique that needs in vitro nanoprobe fabrication and cell labeling, our approach allows for one-step, in vivo labeling of plant cells, thus providing a rapid, cost-effective method for cellular structure construction and imaging.

Glancing angle deposition of helical manganese oxide nanostructures on the glass substrate and study the optical nonlinearity by Z-scan technique

Helical manganese oxide nanostructures have been deposited on glass substrate by glancing angle deposition along with electron-beam evaporation technique. X-ray diffraction analysis, FESEM images, and FTIR spectroscopy confirmed the successful growth of the nanostructured thin film. The surface morphology and roughness of the deposited helical manganese oxide thin film were considered using the 2-D and 3-D AFM images. The optical constants along axes a, b, and c have been calculated from the effective medium approximation of Bruggeman. The refractive indices were found to be equal for helical manganese oxide nanostructures along a- and b-axes and greater than the refractive index along c-axis at λ < 600 nm; while these results are reversed for wavelengths greater than 600 nm. The same variations were observed for the extinction coefficients. The Z-scan measurements under continuous-wave (CW) laser irradiation at 532 nm showed a positive sign for both the nonlinear absorption coefficient and nonlinear refractive index of nanostructured helical manganese oxide demonstrating the attendance of induced absorption process and self-defocusing phenomena, respectively. We computed a 3rd-order nonlinear optical susceptibility, χ(3), equal to 0.042 esu that suggests the glancing angle deposited helical manganese oxide nanostructures with a strong nonlinear optical response can be a good candidate to develop nanophotonic devices.

Graphdiyne-Based All-Solid-State Passively Q-Switched Tm:YAP Laser at 2 μm.

All-solid-state Tm lasers have a wider wavelength range and higher output power compared to other types of lasers. In this work, we demonstrate an all-solid-state, high repetition, Tm:YAP laser Q-switched by a graphdiyne (GDY) saturable absorber. The high-quality optical nonlinear material GDY, synthesized by a cross-coupling method, exhibits a strong nonlinear optical response. The application of GDY as a saturable absorber in the passively Q-switched (PQS) Tm:YAP of an all-solid-state laser has been realized with the shortest pulse duration of ~785 ns and repetition frequency of ~199.6 kHz at a central wavelength of 1985.8 nm. This represents the shortest pulse duration and the highest repetition frequency achieved from GDY in a solid-state Tm laser to date. Our work demonstrates the remarkable nonlinear optical properties of GDY, which holds promising potential in the field of optoelectronics.

Low-loss skimming waveguides with controllable mode leakage for on-chip saturable absorbers

Abstract Emerging 3D photonic circuits would greatly benefit from the ability to integrate skimming waveguides with low loss and controllable inscription depth into photonic circuits. These waveguides allow for the interaction of guiding light directly with external modulation signals and enable programmable photonic circuits. Here, we report the fabrication of a novel photonic-lattice-like skimming waveguide (PLLSW) using femtosecond laser writing. Our method enables fine control of cross-sectional symmetry and writing depth of waveguides, achieving a minimum depth of 1 μm and a low insertion loss of 1 dB. Based on the PLLSW, we demonstrate on-chip light modulation by designing an evanescent-field-type saturable absorber through the coupling of a carbon nanotube film with the PLLSW, which exhibits saturation intensity from 20 to 200 MW/cm2 through the balanced twin-detector measurement. The strong nonlinear optical response of the PLLSW-based saturable absorber is further exploited to drive a Q-switched pulse laser at 1550 nm based on a fiber laser cavity. Our work demonstrates an effective method to integrate nonlinear optical materials into a glass chip for all-optical switching based on 3D waveguides, which holds great potential for the construction of large-scale programmable photonic circuits in the future.