Pump Intensity Research Articles

Time evolution of a pumped molecular magnet—A time-resolved inelastic neutron scattering study

Introducing an experimental technique of time-resolved inelastic neutron scattering (TRINS), we explore the time-dependent effects of resonant pulsed microwaves on the molecular magnet Cr8F8Piv16. The octagonal rings of magnetic Cr3+ atoms with antiferromagnetic interactions form a singlet ground state with a weakly split triplet of excitations at 0.8 meV. A 4.6 tesla field was applied to tune the splitting between two members of the triplet excited level [Formula: see text] to resonance with 105 GHz (0.434 meV) microwaves. The time-dependent occupations of the ground state [Formula: see text], lower lying levels [Formula: see text] and [Formula: see text], and higher energy states [Formula: see text] were extracted during and after 20 s long microwave pulses incident along the (101) direction of a Cr8F8Piv16 crystal held at 1.9 K. At significantly elevated spin temperatures, we found underpopulation relative to thermal equilibrium of [Formula: see text] and spin-lattice thermalization time scales ranging from 1.6(2) s to 5.7(2) s depending on the power level. This contrasts with the relaxation time [Formula: see text]s inferred for [Formula: see text] from in situ Electron Spin Resonance measurements. By probing a broad range of excited states during intense microwave pumping, TRINS thus provides a first view of long lived excited states in a molecular antiferromagnet.

Symmetry-protected and Brillouin zone folding driven bound states in the continuum in dielectric nanorod arrays for effcient third harmonic generation

Abstract Two types of bound states in continuum (BICs), symmetry-protected and Brillouin zone folding driven, are identified in the hollow Si nanorod arrays. By modulating the direction and distance of the air holes from the center of the nanorods, it is possible to achieve either a single quasi-BIC or three quasi-BICs. The transmission spectra exhibit ultra-narrow lines, and the quasi-BICs demonstrate ultra-high Q factors. Additionally, effcient third-harmonic generation occurs at low pump intensities. The results indicate that the proposed nanostructures of two types of BICs with a flexible modulation hold great potential applications for nonlinear photonic devices.

Chiral Floquet engineering on topological fermions in chiral crystals

The interplay of chiralities in light and quantum matter provides an opportunity to design and manipulate chirality-dependent properties in quantum materials. Herein we report the chirality-dependent Floquet engineering on topological fermions with the high Chern number in chiral crystal CoSi via circularly polarized light (CPL) pumping. Intense light pumping does not compromise the gapless nature of topological fermions in CoSi, but displaces the crossing points in momentum space along the direction of light propagation. The Floquet chirality index is proposed to signify the interplay between the chiralities of topological fermion, crystal, and incident light, which determines the amplitudes and directions of light-induced momentum shifts. Regarding the time-reversal symmetry breaking induced by the CPL pumping, momentum shifts of topological fermions result in the birth of transient anomalous Hall signals in non-magnetic CoSi within an ultrafast time scale, which Mid-infrared (IR) pumping and terahertz (THz) Kerr or Faraday probe spectroscopy could experimentally detect. Our findings provide insights into exploring novel applications in optoelectronic devices by leveraging the degree of freedom of chirality in the non-equilibrium regime.

Numerical Study on the Potential Enhancement of Organic Terahertz Sources through Tilted Pulse Front Pumping

Organic crystals offer promising potential for THz generation, but face limitations in wavelength tunability and damage threshold. By applying tilted pulse‐front pumping to organic crystals an additional degree of freedom is introduced into the pumping conditions enabling a wider range of pumping wavelengths without compromising phase matching. Additionally, the lifespan of organic materials can be extended by using longer pumping wavelength and eliminate lower‐order multi‐photon absorption, allowing for higher pumping intensity without significant free‐carrier absorption, thus increasing the damage threshold. Simulations predict significant improvement for four out of six investigated crystals when tilted pulse‐front pumping is applied. By using volume phase holographic grating one can achieve pulse‐front tilt in organic crystals in collinear geometry with high diffraction efficiency. Design parameters are also presented.

Ultrafast terahertz conductivity in epitaxial graphene nanoribbons: an interplay between photoexcited and secondary hot carriers

Abstract Optical pump-terahertz probe spectroscopy has been used to investigate ultrafast photo-induced charge carrier transport in 3.4 µm wide graphene ribbons upon scaling the optical pump intensity. For low pump fluences, the deposited pump energy is rapidly redistributed through carrier–carrier scattering, producing secondary hot carriers: the picosecond THz photoconductivity then acquires a negative sign and scales linearly with an increasing pump fluence. At higher fluences, there are not enough equilibrium carriers able to accept the deposited energy, directly generated (excess) carriers start to contribute significantly to the photoconductivity with a positive sign leading to its saturation behavior. This leads to a non-monotonic variation of the carrier mobility and plasmonic resonance frequency as a function of the pump fluence and, at high fluences, to a balance between a decreasing carrier scattering time and an increasing Drude weight. In addition, a weak carrier localization observed for the polarization parallel to the ribbons at low pump fluences is progressively lifted upon increasing the pump fluence as a result of the rise of initial carrier temperature.

Bismuth telluride as a passive Q-switcher for neodymium-doped fiber laser

The scene of fiber laser has progressed very rapidly with the demonstration of various materials as saturable absorbers in a near- and mid-infrared laser cavity. However, the researchers focused on erbium-, ytterbium-, and thulium-doped fiber as a gain medium. Here, we proposed a neodymium-doped fiber laser setup to generate a Q-switched laser in a 1-μm regime. The laser utilized bismuth telluride, a topological insulator as a Q-switcher for pulse generation. With a linear absorption of approximately 5 dB at 1089 nm, this SA can generate a stable Q-switched laser in a neodymium-doped fiber laser cavity. It generates a stable Q-switched laser at 1089 nm when the pump intensity is adjusted between 167 and 190 mW. The pulsed laser owns the shortest pulse width of 6.48 μs with a maximum repetition rate of 40 kHz. The stability of the laser is promising since it has a signal-to-noise ratio of 40 dB. In the authors’ knowledge, this is the first demonstration of bismuth telluride as a saturable absorber in an all-fiberized neodymium-doped fiber laser cavity.

Dynamic phase transition region in electrically injected PT-symmetric lasers

Research on parity-time (PT) symmetry and exceptional points in non-Hermitian laser systems has been extensively conducted. However, in practical electrically injected PT-symmetric lasers, the frequency detuning and linewidth enhancement factor of the laser can influence the symmetry breaking of the system in another dimension. We find that the previous exceptional point now transforms into a dynamic phase transition region, where the states are temporally unstable, indicating the occurrence of multimode oscillation. The relative phase and field amplitude ratio in this region also exhibit many novel phenomena indicating its instability. This region can be manipulated by adjusting the coupling strength between adjacent waveguides and the pumping intensity in the loss waveguide. Experimentally, we characterize the near-field, far-field, and spectrum of several structures, and the results validate our theoretical model. This work elucidates the dynamic process and phase transition process of electrically injected PT-symmetric lasers, providing support for the practical application of PT-symmetric lasers.

Assessing the potential accuracy of a small-sized goniometer with extended dynamic range based on nuclear magnetic resonance

This paper evaluates potential accuracy characteristics of a small-sized goniometer based on nuclear magnetic resonance with an extended dynamic range. This required constructing a model of goniometer errors, estimating its accuracy based on this model, and formulating practical recommendations for the design of such a device based on the accuracy assessment. To evaluate the accuracy of a nuclear goniometer, a theoretical model was built that makes it possible to determine the optimal operating parameters of the cell gas mixture, the ranges of their permissible changes, the sensitivity of the goniometer, and the dependence of its characteristics on external and internal factors. In particular, the dependence of output signal of the device on the parameters of gas mixture and optical pumping has been determined. For a goniometer with a cell volume of 8 cm3, the optimum temperature is 130 °C, and the optimum intensity of the pumping radiation is 5 mW. The dependence of output signal on the measured angle of rotation was also established, as well as the noise and error dependence of the device on the permissible values of its parameters. Based on the model built, parameters of a goniometer with a cell volume of 8 cm3 were determined; the maximum angular sensitivity of such a goniometer with complete suppression of technical noise is δφsen=1.0 arcsec. The greatest contribution to the angle measurement error is from the instability of pumping power Ip (ΔIp/Ip=0.05) – 85 %, magnetic field B0 (ΔB0/B0=10-8) – 13 %, temperature T (ΔT/T=0,1) – 2 %. The goniometer under consideration corresponds to the medium accuracy class, δφtot≥10 arcsec. It could be used in optical manufacturing for operational control, calibration, and certification of optical products. To improve the angular accuracy of the goniometer, it is necessary to increase the stability of the laser pumping intensity

Fluorescence by incoherently pumped polar quantum dot placed in a low-frequency monochromatic field

Abstract We studied spectral properties of high-frequency fluorescent radiation from a two-level quantum system with broken inversion spatial symmetry, which can be implemented as a model of a one-electron two-level asymmetric polar semiconductor quantum dot whose electric dipole moment operator has permanent unequal diagonal matrix elements. The case of the excitation of this system by incoherent pumping of some sort supplemented with an additional driving monochromatic field, which frequency is much lower than the optical transition frequency of the quantum dot, was considered. An analytical expression for the fluorescence spectrum as a function of the amplitude and frequency of the monochromatic driving field, as well as of the pumping intensity, was derived. We also discussed feasible practical applications of the effects under study in the field of quantum optics and optoelectronics for the generation of high-frequency radiation, possessing stationary equidistant spectrum, and for the control of the radiative properties of such nanodevices as spasers (dipole nanolasers).

Ultrafast Charge Transfer-Induced Unusual Nonlinear Optical Response in ReSe2/ReS2 Heterostructure.

Ultrafast charge transfer in van der Waals heterostructures can effectively engineer the optical and electrical properties of two-dimensional semiconductors for designing photonic and optoelectronic devices. However, the nonlinear absorption conversion dynamics with the pump intensity and the underlying physical mechanisms in a type-II heterostructure remain largely unexplored, yet hold considerable potential for all-optical logic gates. Herein, two-dimensional ReSe2/ReS2 heterostructure is designed to realize an unusual transition from reverse saturable absorption to saturable absorption (SA) with a conversion pump intensity threshold of approximately 170 GW/cm2. Such an intriguing phenomenon is attributed to the decrease of two-photon absorption (TPA) of ReS2 and the increase of SA of ReSe2 with the pump intensity. Based on the characterization results of X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, femtosecond transient absorption spectrum, Kelvin probe force microscopy, and density functional theory calculation, a type-II charge-transfer-energy level model is proposed combined with the TPA of ReS2 and SA of ReSe2 processes. The results reveal the critical role of ultrafast interfacial charge transfer in tuning the unusual nonlinear absorption and improving the SA of ReSe2/ReS2 under different excitation wavelengths. Our finding deepens the understanding of nonlinear absorption physical mechanisms in two-dimensional heterostructure materials, which may further diversify the nonlinear optical materials and photonic devices.

Enhanced high-harmonic generation in a polarization-insensitive all-dielectric metasurface exploiting dual-Fano resonance

Nonlinear optics demands efficacious techniques for nonlinear properties engineering. Metasurfaces, as a flat technology with easy fabrication in various arrangements and without the need for phase-matching conditions, are suitable platforms for nonlinear optics. This study proposes a silicon metasurface with special geometry that provides high conversion efficiency by exploiting Fano resonances and the excitation of magnetic and toroidal dipoles. The results indicate the high efficiencies of third harmonic generation of 5.17×10−3 W−2 and fifth harmonic generation of 7.92×10−9 W−4 under 1 GW/cm2 pump intensity in the near-infrared regime. More specifically, linear and nonlinear optical responses of the structure are completely polarization-independent.

Excitation of pure quartic platicon in optical microresonators.

We analytically derive the formulas of the threshold pump intensity and the range of possible detuning for the initiation of the pure quartic platicon (PQP) in the presence of multiphoton absorption, free-carrier absorption, and free-carrier dispersion. Theoretical investigations demonstrate a feasible approach for the excitation of PQP in the normal quartic dispersion regime via the free-carrier effects in platforms such as silicon, germanium, and their derivates. Due to the time-variant nonlinear loss related to free-carrier absorption or additional nonlinear detuning induced by free-carrier plasma dispersion, PQP can be generated through turn-key or laser frequency scanning schemes in both the three- and four-photon absorption regimes. Parameter spaces associated with varying detuning and free-carrier lifetime for the different dark, oscillating, and bright PQP states are revealed in the turn-key generation case. Such solitonic pulses are more energetic than conventional quadratic solitons with the same pulse width, especially for shorter pulse operations. In the spectral domain, PQP microcombs in the mid-infrared are desired for spectroscopy. These findings will facilitate the generation and manipulation of PQP and present promising potential for Kerr microcomb related applications.

Dual-media laser system: Nitrogen vacancy diamond and red semiconductor laser.

Diamond is a potential host material for laser applications due to its exceptional thermal properties, ultrawide bandgap, and color centers, which promise gain across the visible spectrum. More recently, coherent laser methods offer improved sensitivity for magnetometry. However, diamond fabrication is difficult in comparison to other crystalline matrices, and many optical loss channels are not yet understood. Here, we demonstrate a continuous-wave laser threshold as a function of the pump intensity on nitrogen-vacancy (NV) color centers. To achieve this, we constructed a laser cavity with both an NV diamond medium and an intracavity antireflection-coated diode laser. This dual-medium approach compensates intrinsic losses of the cavity by providing a fixed additional gain below threshold of the diode laser. We observe a continuous-wave laser threshold of the laser system and linewidth narrowing with increasing green pump power on the NV centers. Our results are a major development toward coherent approaches to magnetometry.

Optimization of polarization spectroscopy signal for laser-frequency stabilization

Abstract We experimentally generate polarization spectroscopy (error) signals corresponding to the D2-line hyperfine transitions, F g = 2 → F e = 1 , 2 , 3 of 87Rb, and F g = 3 → F e = 2 , 3 , 4 of 85Rb, and show that the strongest error signals correspond to the closed hyperfine transitions (oscillator strength ∼ 0.7 ), F g = 2 → F e = 3 and F g = 3 → F e = 4 , respectively. We make the generated error signal robust to fluctuations in external parameters by finding optimum values for the vapor cell temperature and pump-probe intensities at two different beam diameters. We further employ these optimized error signals to directly (without the need for frequency/phase modulation) lock the laser frequency—reducing the rms drift/linewidth from ∼ 10 MHz to < 500 kHz, when measured over a ∼ 60 min duration. In addition, by comparing theoretically calculated and experimentally measured error signals for the pump intensities ranging from ∼ 0.1 I sat 0 − 10 I sat 0 (where, I sat 0 ∼ 1.6 mW cm−2 is the two-level saturation intensity for the Rb D2-line transitions), we discuss the applicability and limitations of existing numerical and analytical approaches based on a full multi-level rate equation model for polarization spectroscopy.

Second harmonic generation at a time-varying interface

Time-varying metamaterials rely on large and fast changes of the linear permittivity. Beyond the linear terms, however, the effect of a non-perturbative modulation of the medium on harmonic generation remains largely unexplored. In this work, we study second harmonic generation at an optically pumped time-varying interface between air and a 310 nm Indium Tin Oxide film. We observe a modulation contrast at the second harmonic wavelength up to 93% for a pump intensity of 100 GW/cm2, leading to large frequency broadening and shift. We experimentally demonstrate that a significant contribution to the enhancement comes from the temporal modulation of the second order nonlinear susceptibility. Moreover, we show the frequency-modulated spectra resulting from single and double-slit time diffraction could be exploited for enhanced optical computing and sensing, enabling broadband time-varying effects on the harmonic signal and extending the application of Epsilon-Near-Zero materials to the visible range.

Unveiling the Influence of Brightness Heterogeneity in Fluorescence Correlation Spectroscopy of Perovskite Nanocrystals.

Nanoparticles (NPs), including perovskite nanocrystals (PNCs) with single photon purity, present challenges in fluorescence correlation spectroscopy (FCS) studies due to their distinct photoluminescence (PL) behaviors. In particular, the zero-time correlation amplitude [g2(0)] and the associated diffusion timescale (τD) of their FCS curves show substantial dependency on pump intensity (IP). Optical saturation inadequately explains the origin of this FCS phenomenon in NPs, thus setting them apart from conventional dye molecules, which do not manifest such behavior. This observation is apparently attributed to either photo-brightening or optical trapping, both lead to increased NP occupancy (N) in the excitation volume, consequently reducing the g2(0) amplitude [since g2(0) α 1/N] at high IP. However, an advanced FCS study utilizing alternating laser excitation at two different intensities dismisses such possibilities. Further investigation into single-particle blinking behaviors as a function of IP reveals that the intensity dependence of g2(0) primarily arises from the brightness heterogeneity prevalent in almost all types of NPs. This report delves into the complexities of the photophysical properties of NPs and their adverse impacts on FCS studies.

Enhanced Second-Harmonic Generation in Thin-Film Lithium Niobate Circular Bragg Nanocavity.

Second-order nonlinearity gives rise to many distinctive physical phenomena, e.g., second-harmonic generation, which play an important role in fundamental science and various applications. Lithium niobate, one of the most widely used nonlinear crystals, exhibits strong second-order nonlinear effects and electro-optic properties. However, its moderate refractive index and etching sidewall angle limit its capability in confining light into nanoscales, thereby restricting its application in nanophotonics. Here, we exploit nanocavities formed by second-order circular Bragg gratings, which support resonant anapole modes, to achieve a 42 000-fold enhanced second-harmonic generation in thin-film lithium niobate. The nanocavity exhibits a record-high normalized conversion efficiency of 1.21 × 10-2 cm2/GW under the pump intensity of 1.9 MW/cm2. Besides, we also show s- and p-polarization-independent second-harmonic generation in elliptical Bragg nanocavities. This work could inspire the study of nonlinear optics at the nanoscale on thin-film lithium niobate, as well as other novel photonic platforms.

Optimized terahertz generation in BNA organic crystals with chirped Ti:sapphire laser pulses.

We report on the efficient generation of intense terahertz radiation from the organic crystal N-benzyl-2-methyl-4-nitroaniline pumped by chirped Ti:sapphire femtosecond laser pulses. The THz energy and spectrum as a function of the pump fluence and duration of the chirped laser pulses are studied systematically. For the appropriate positively chirped pump pulses, a significant boost in the THz generation efficiency by a factor of around 2.5 is achieved, and the enhancement of high-frequency components (>1 THz) shortens the THz pulse duration. Via complete characterization of THz properties and transmitted laser spectra, this nonlinear behavior is attributed to the extended effective interaction length for phase matching as a result of the self-phase modulation of the intense pump laser pulses. Numerical calculations well reproduce the experimental observation. Our results demonstrate a robust, efficient, strong-field (up to several MV/cm) THz source using the common sub-10 mJ and sub-100 fs Ti:sapphire laser systems without optical parametric amplifiers.

Microfluidics-Driven Dripping Technique for Fabricating Polymer Microspheres Doped with AgInS2/ZnS Quantum Dots.

Fluorescent microspheres are at the forefront of biosensing technologies. They can be used for a wide range of biomedical applications. They consist of organic dyes and polymers, which are relatively immune to photobleaching and other environmental factors. However, recently developed AgInS2/ZnS quantum dots are a water-soluble, low-toxicity class of semiconductor nanocrystals with enhanced stability as fluorescent materials. Here, we propose a simple way for making microspheres: a microfluidic dripping technique for acrylamide polymer spheres doped with quantum dots. Analyses of their spectra show that the emission of quantum dots, dispersed in water, is saturated with an increasing pump intensity, while quantum dots embedded into polymer microspheres exhibit a more sustained emission. Moreover, our study unveils a remarkable reduction in the luminescence lifetime of quantum dots embedded in microspheres: the mean value of the decay time for quantum dots in solutions was 91 and 3.5 ns for similar quantum dots incorporated into polymer microspheres.

Dynamically Tunable Circularly Polarized Selectivity in Plasmon-Enhanced Halide Perovskite Nanocrystal Glasses.

Ultrafast spin manipulation for optical spin-logic applications requires material systems with strong spin-selective light-matter interactions. The optical Stark effect can realize spin-selective light-matter interactions by breaking the degeneracy of spin-selective transitions with an external electric field. Halide perovskites have large exciton binding energies, which enable a room-temperature optical Stark effect. However, halide perovskites are prone to degradation when interacting with light and polar solvents, limiting further integration with nanophotonic structures. We demonstrate a hybrid material system consisting of CsPbBr3 nanocrystal glass weakly coupled to resonant plasmonic silver nanoparticles, showing ultrafast tunable spin-based polarization selectivity at room temperature. We performed circularly polarized pump-probe characterizations to investigate the optical Stark effect in this material system, which resulted in a maximum energy shift of ∼3.67 meV (detuning energy of 0.11 eV and pump intensity of 0.62 GW/cm2). We show that halide perovskite nanocrystal glasses have excellent resistance to heat and moisture, which may be favorable for integration with nanophotonic structures for further engineering polarization states, energy tuning, and coherence time.