Accurate knowledge of absorption coefficient of a sample is a prerequisite for measuring the third order optical nonlinearity of materials, which could become a serious limitation for unknown samples. We introduce a new method, which measures both the absorption coefficient and the third order optical nonlinearity of materials with high sensitivity in a single experimental setup. We use a dual-beam pump-probe experiment under different conditions to achieve this goal. We also demonstrate a counterintuitive coupling of the non-interacting probe-beam with the pump-beam in pump-probe z-scan experiment.
We introduce a new regime of cascaded quadratic nonlinearities which result in a continuous red shift of the optical pump, analogous to a Raman shifting process rather than self-phase modulation. This is particularly relevant to terahertz generation, where a continuous red shift of the pump can resolve current issues such as dispersion management and laser-induced damage. We show that in the absence of absorption or dispersion, the presented Raman shifting method will result in optical-to-terahertz energy conversion efficiencies that approach $100\%$ which is not possible with conventional cas…
In this paper, we demonstrate NiCo$_2$O$_4$ (NCO) as an efficient new nonlinear optical material with straightforward potential applications in optical limiting devices. We obtain nonlinear absorption coefficient ($β$) and nonlinear refractive index ($n_2$) in parallel by performing Z-scan technique, in both open and closed aperture configurations, respectively. To understand the mechanism responsible for third order optical nonlinearity in NCO, we excited the sample with contrasting laser pulse durations, 7 ns and 120 fs, at two different off-resonant wavelengths. For ns excitation, nonlinear…
Electrically Tunable Optical Nonlinearities in Graphene-Covered SiN Waveguides Characterized by Four-Wave Mixing
我们提出了一个退化的四波混频实验氮化硅（SiN）波导覆盖栅石墨烯。我们观察到强烈的依赖性信号泵浦失谐和费米能量，即光学非线性被证明是电可调的。在带间吸收边（$2|E_F|\approx \hbarω$）附近，测量对应于石墨烯非线性薄层电导率$|σ_s^{(3)}|\approx4.3\cdot 10^{-19}$ A m $^2$ V $^{-3}$的波导非线性参数$\approx$ 6400 m $^{-1}$ W $^{-1}$的峰值。
We developed a frequency-domain model describing optical frequency-comb generation in optical resonators with second- and third-order nonlinearities. Compared with time-domain models, our model in principle allows one to express the cavity dispersion accurately, avoiding the dispersion being truncated beyond a certain order. Moreover, the frequency-domain model can readily include frequency dependence of system parameters, such as the linear absorption and the cavity coupling ratio. To demonstrate the validity of our model, we numerically simulated quadratic combs in a singly resonant second-h…
Femtosecond spectroscopy is an important tool for tracking rapid photoinduced processes in a variety of materials. To spatially map the processes in a sample would substantially expand the capabilities of the method. This is, however, difficult to achieve due to the necessity to use low-noise detection and to maintain feasible data acquisition time. Here we demonstrate realization of an imaging pump-probe setup, featuring sub-100 fs temporal resolution, by a straightforward modification of a standard pump-probe technique, using a randomly structured probe beam. The structured beam, made by a d…
Recording of transient absorption microscopy images requires fast detection of minute optical density changes, which is typically achieved with high-repetition-rate laser sources and lock-in detection. Here, we present a highly flexible and cost-efficient detection scheme based on a conventional photodiode and an USB oscilloscope with MHz bandwidth, that deviates from the commonly used lock-in scheme and achieves benchmark sensitivity. Our scheme combines shot-to-shot evaluation of pump-probe and probe-only measurements, a home-built photodetector circuit optimized for low pulse energies apply…
Up to date, quantum electrodynamics (QED) is the most precisely tested quantum field theory. Nevertheless, particularly in the high-intensity regime it predicts various phenomena that so far have not directly been accessible in all-optical experiments, such as photon-photon scattering phenomena induced by quantum vacuum fluctuations. Here, we focus on all-optical signatures of quantum vacuum effects accessible in the high-intensity regime of electromagnetic fields. We present an experimental setup giving rise to signal photons distinguishable from the background. This configuration is based on…
Pristine, undoped graphene has a constant absorption of 2.3 % across the visible to near-infrared (VIS-NIR) region of the electromagnetic spectrum. Under certain conditions, such as nanostructuring and intense gating, graphene can interact more robustly with VIS-NIR light and exhibit a large nonlinear optical response. Here, we explore the optical properties of graphene/LaAlO$_3$/SrTiO$_3$ nanostructures, where nanojunctions formed at the LaAlO$_3$/SrTiO$_3$ interface enable large (~10$^8$ V/m) electric fields to be applied to graphene over a scale of ~10 nm. Upon illumination with ultrafast V…
We propose a scheme in which an arbitrary incidence can be made perfectly reflected/transmitted if a phase setup is adjusted under a specific condition. We analyze the intracavity field variation as well as the output field with changing closed-loop phase of atomic system and relative phase of input probe beams. And we obtain the condition for perfect transmitter or reflector. By adjusting two phase setups, the medium absorption and light interference can be controlled so that photon escape from cavity can be modulated, thus the intensity switching based on phase control can be realized. Then …
Absorption spectroscopy studies the absorption of electromagnetic wave in a material sample under test. The interacting electromagnetic wave can be propagating in free space or in a waveguide. The waveguide-based absorption spectroscopy method has several advantages compared to the free space setup. The effect of the waveguide cross section on the interaction between the waveguide mode and the sample can be expressed by a factor, called interaction factor. In this article, a new formulation for the interaction factor is derived. It is shown that this factor is inversely proportional to the ene…
Light trapping and radiation process from linear reciprocal photonic resonators is one of the fundamental processes in optical science and engineering. Recently, the concept of coherent virtual absorption (CVA) of light was introduced and investigated for planar and cylindrical optical structures. The key feature of CVA is that by engineering the time-dependence of the excitation waveform, one can temporarily store all the input energy into the optical structure without any leakage. Here we further explore this novel concept in integrated photonic setups made of microring resonators. By using …
In virtual-state spectroscopy, information about the energy-level structure of an arbitrary sample is retrieved by Fourier transforming sets of measured two-photon absorption probabilities of entangled photon pairs where the degree of entanglement and the delay time between the photons have been varied. This works well for simple systems but quickly becomes rather difficult when many intermediate states are involved. We propose and discuss an extension of entangled two-photon absorption spectroscopy that solves this problem by means of repeated measurements at different pump wavelengths. Speci…
One-dimensional (1D) metal-dielectric (MD) periodic structures take advantage of large refractive index contrast between metal and dielectrics to invoke extremely high nonlinear ultrafast responses of metal. These structures are also special due to their extremely high laser damage threshold. The Bragg like 1D MD structure (Ag/SiO2)4 enables strong optical field confinement with much enhanced nonlinear features as compared to simple metal or single (Ag/SiO2)1 structure. In the present work, the ultrafast nonlinear optical responses of the above structures are investigated via femtosecond broad…
All-optical modulation of light relies on exploiting intrinsic material nonlinearities. However, this optical control is rather challenging due to the weak dependence of the refractive index and absorption coefficients on the concentration of free carriers in standard semiconductors. To overcome this limitation, resonant structures with high spatial and spectral confinement are carefully designed to enhance the stored electromagnetic energy, thereby requiring lower excitation power to achieve significant nonlinear effects. Small mode-volume and high quality (Q)-factor cavities also offer an ef…
We report the existence of persistently rotating azimuthons in media with self-focusing Kerr and absorption nonlinearities. The nonlinear loss is balanced by power influx from the peripheral reservoir stored in slowly decaying tails of the azimuthons. These modes are excited by a superposition of two Bessel beams with opposite vorticities, $\pm s$, and slightly different conicities. The excited azimuthon exhibits opposite vorticity in its center to that of the input Bessel-beam superposition due to spontaneous inversion of the topological charge in the course of the azimuthon formation. Unlike…
Measurements of ultrahigh-fidelity absorption spectra can help validate quantum theory, engineer ultracold chemistry, and remotely sense atmospheres. Recent achievements in cavity-enhanced spectroscopy using either frequency-based dispersion or time-based absorption approaches have set new records for accuracy with uncertainties at the sub-per-mil level. However, laser scanning5 or susceptibility to nonlinearities limits their ultimate performance. Here we present cavity buildup dispersion spectroscopy (CBDS) in which the dispersive frequency shift of a cavity resonance is encoded in the cavit…
Our goal is to study optical signatures of quantum vacuum nonlinearities in strong macroscopic electromagnetic fields provided by high-intensity laser beams. The vacuum emission scheme is perfectly suited for this task as it naturally distinguishes between incident laser beams, described as classical electromagnetic fields driving the effect, and emitted signal photons encoding the signature of quantum vacuum nonlinearity. Using the Heisenberg-Euler effective action, our approach allows for a reliable study of photonic signatures of QED vacuum nonlinearity in the parameter regimes accessible b…
We report on a compact and spectrally intense extreme-ultraviolet (XUV) source, which is based on high-harmonic generation (HHG) driven by 395 nm pulses. In order to minimize the XUV virtual source size and to maximize the XUV flux, HHG is performed several Rayleigh lengths away from the driving laser focal plane in a high-density gas jet. As a result, a high focused XUV intensity of $5 \times 10^{13}$ W/cm$^2$ is achieved, using a beamline with a length of only two meters and a modest driving laser pulse energy of 3 mJ. The high XUV intensity is demonstrated by performing a nonlinear ionizati…
The fundamental theory of quantum electrodynamics predicts the vacuum to resemble a polarizable medium. This gives rise to effective nonlinear interactions between electromagnetic fields and light-by-light scattering phenomena. We study the collision of two optical laser pulses in a pump-probe setup using beams with circular and elliptic cross section and estimate the number of discernible signal photons induced by quantum vacuum nonlinearities. In this analysis we study strategies to optimize the quantum vacuum signal discernible from the background of the driving lasers. One of the main resu…
Snow is a highly complex medium composed of ice crystals of various shapes and sizes. Knowledge of its intrinsic optical properties such as the scattering and absorption coefficient is tantamount to radiative transfer models in climate research. The absorption coefficient, in particular, allows us to access information about light-absorbing particles contained in the snow. In contrast to snow's apparent properties like the albedo, measuring the intrinsic properties is challenging. Here, we present a simple apparatus that can measure bulk optical properties of snow using readily available compo…
