High-quality crystals without inversion symmetry are the conventional platform to achieve optical frequency conversion via three wave-mixing. In bulk crystals, efficient wave-mixing relies on phase-matching configurations, while at the micro- and nano-scale it requires resonant mechanisms that enhance the nonlinear light-matter interaction. These strategies commonly result in wavelength-specific performances and narrowband applications. Disordered photonic materials, made up of a random assembly of optical nonlinear crystals, enable a broadband tunability in the random quasi-phase-matching (RQPM) regime and do not require high-quality materials. Here, we combine resonances and disorder by implementing RQPM in Mie-resonant spheres of a few microns realized by the bottom-up assembly of barium titanate nano-crystals. The measured second harmonic generation (SHG) reveals a combination of broadband and resonant wave mixing, in which Mie resonances drive and enhance the SHG, while the disorder keeps the phase-matching conditions relaxed. This new phase-matching regime can be described by a random walk in the SHG complex plane whose step lengths depend on the local field enhancement within the micro-sphere. Our nano-crystals assemblies provide new opportunities for tailored phase-matching at the micro-scale, beyond the coherence length of the bulk crystal. They can be adapted to achieve frequency conversion from the near-ultraviolet to the infrared ranges, they are low-cost and scalable to large surface areas.
Light trapping in planar ultrathin-film solar cells is limited due to a small number of optical modes available in the thin-film slab. A nanostructured thin-film design could surpass this limit by providing broadband increase in the local density of states in a subwavelength volume and maintaining efficient coupling of light. Here we report a broadband metasurface design, enabling efficient and broadband absorption enhancement by direct coupling of incoming light to resonant modes of subwavelength-scale Mie nanoresonators defined in the thin-film active layer. Absorption was investigated both …
Mie-lithography: void-resonance-assisted femtosecond laser printing for deep-ultraviolet to near-infrared nano dispersion devices
State Key Laboratory of Precision Measurement Technology and Instruments, Department of Precision Instrument, Tsinghua University（精密测试技术与仪器国家重点实验室，精密仪器系，清华大学）；MIIT Key Laboratory of Complex-field Intelligent Exploration, School of Optics and Photonics, Beijing Institute of Technology（工业和信息化部复杂场智能探测重点实验室，光学与光子学院，北京理工大学）
Metadevices based on dielectric nanostructured surfaces with both electric and magnetic Mie-type resonances have resulted in the best efficiency to date for functional flat optics with only one disadvantage: a narrow operational bandwidth. Here we experimentally demonstrate broadband transparent all-dielectric metasurfaces for highly efficient polarization manipulation. We utilize the generalized Huygens principle, with a superposition of the scattering contributions from several electric and magnetic multipolar modes of the constituent meta-atoms, to achieve destructive interference in reflec…
Meta-optics based on optically-resonant dielectric nanostructures is a rapidly developing research field with many potential applications. Halide perovskite metasurfaces emerged recently as a novel platform for meta-optics, and they offer unique opportunities for control of light in optoelectronic devices. Here we employ the generalized Kerker conditions to overlap electric and magnetic Mie resonances in each meta-atom of MAPbBr3 perovskite metasurface and demonstrate broadband suppression of reflection down to 4%. We reveal also that metasurface nanostructuring is also beneficial for the enha…
Future quantum information networks operated on telecom channels require qubit transfer between different wavelengths while preserving quantum coherence and entanglement. Qubit transfer is a nonlinear optical process, but currently the types of atoms used for quantum information processing and storage are limited by the narrow bandwidth of up-conversion available. Here we present the first experimental demonstration of broadband and high-efficiency quasi-phase matching second harmonic generation (SHG) in a chip-scale periodically poled lithium niobate thin film. We achieve large bandwidth of u…
We propose an efficient broadband frequency generation technique for two collinear optical parametric processes $ω_3=ω_1+ω_2$ and $ω_4=ω_1-ω_2$. It exploits chirped quasi-phase-matched gratings, which in the undepleted pump approximation regime perform population transfer that is analogous to adiabatic population transfer in a three-state ``vee'' quantum system. The energy of the input fields is transferred adiabatically either into $ω_3$ or $ω_4$ field, depending on which of the two phase matchings occurs first by the local modulation period in the crystal. One can switch the output between $…
An efficient broadband sum frequency generation (SFG) technique using the two collinear optical parametric processes ω3=ω1+ω2 and ω4=ω1+ω3 is proposed. The technique uses chirped quasi-phase-matched gratings, which, in the undepleted pump approximation, make SFG analogous to adiabatic population transfer in three-state systems with crossing energies in quantum physics. If the local modulation period %for aperiodically poled quasi-phase-matching first makes the phase match occur for ω3 and then for ω4 SFG processes then the energy is converted adiabatically to the ω4 field. Efficient SFG of the…
Optical frequency conversion processes in nonlinear materials are limited in wavelength by the accessible phase matching and the required high pump powers. In this letter, we report a novel broadband phase matching (PM) technique in high quality factor (Q) whispering gallery mode (WGM) resonators made of birefringent crystalline materials. This technique relies on two interacting WGMs, one with constant and the other with spatially oscillating phase velocity. Thus, phase matching occurs cyclically. The technique can be implemented with a WGM resonator with its disk plane parallel to the optic …
We show that non-Hermitian engineering can play a positive role in quantum systems. This is in contrast to the widely accepted notion that optical losses are a foe that must be eliminated or, at least, minimized. We take advantage of the interplay between nonlinear interactions and loss to show that spectral-loss engineering can relax phase-matching conditions, enabling generation of broadband pseudothermal states at new frequencies. This opens the door for utilizing the full potential of semiconductor materials that exhibit giant nonlinearities but lack the necessary ingredients for achieving…
Generating photon pairs via spontaneous parametric down-conversion (SPDC) in nonlinear crystals is important for a wide range of quantum optics experiments with spectral properties such as their bandwidths often being a crucial concern. Here, we show the generic existence of particular phase-matching conditions in quasi-phase matched KTP, MgO:LN and SLT crystals that lead to ultra-broadband, widely non-degenerate photon pairs. It is based on the existence of group-velocity matched, far apart wavelength pairs and for 2 mm long crystals results in SPDC bandwidths between 15 and 25 THz (FWHM) for…
We present a new variant of dispersion scan (d-scan) based on surface third-harmonic generation (STHG) and a ptychographic algorithm taylored for full retrieval (amplitude and phase) of broadband laser pulses. We demonstrate the technique by temporally measuring and compressing few-cycle pulses with 7 fs and 2.5 nJ from a Ti:Sapphire oscillator, using a sapphire window as the nonlinear medium. The results are in very good agreement with standard second-harmonic d-scan measurements based on a nonlinear crystal. The intrinsically broadband and phase-matching-independent nature of STHG make this …
High-index dielectric nanoparticles supporting a distinct series of Mie resonances have enabled a new class of optical antennas with unprecedented functionalities. The great wealth of multipolar responses and their delicate interplay have not only spurred practical developments but also brought new insight into fundamental physics such as the recent observation of nonradiating anapole states in the optical regime. However, how to make such a colorful resonance palette actively tunable and even switchable among different elemental multipoles is still elusive. Here, for the first time, we demons…
We propose non-phase-matched sum frequency generation (SFG) as a method for characterizing broadband multimode light. We demonstrate its advantages using high-gain parametric down conversion (PDC) as an example. By generating the sum frequency in the near-surface region of a nonlinear crystal, we increase the SFG efficiency and get rid of the modulation caused by chromatic dispersion, known as Maker fringes. The obtained results interpreted in terms of the Schmidt mode formalism reveal the sensitivity of the SFG spectrum to the number of frequency modes. Furthermore, we demonstrate efficient n…
In this paper, we present the design, fabrication and characterization of a traveling wave directional coupler modulator based on electro-optic polymer, which is able to provide both high linearity and broad bandwidth. The high linearity is realized by introducing domain-inversion technique in the two-domain directional coupler. A travelling wave electrode is designed to function with bandwidth-length product of 302GHz cm, by achieving low microwave loss, excellent impedance matching and velocity matching, as well as smooth electric field profile transformation. The 3-dB bandwidth of the devic…
We generate a 200-nm optical frequency comb at 1.5 microns by injecting two single-frequency lasers into a highly nonlinear fiber, and explore its spectral phase properties and high power to demonstrate full nonlinear conversion into its second harmonic. Combs of optical frequencies with 100-nm (~ 48 THz) bandwidths, centered at 790-800 nm and spaced by 0.8-1 nm (380-470 GHz) were produced by second harmonic and multiple sum frequency generation simply by focusing into a 2-mm long nonlinear crystal. Conventional birefringence phase matching was used in normal incidence configuration without ti…
We are reporting on terahertz generation from organic crystal BNA using a 1.15 to 1.55 um near infrared pump. We observed a very large emission spectrum extending up to 7 THz, compared to 2.5 THz from Ti:Sa pump in previous reports. The maximum optical-to-THz conversion efficiency in our experiment was 0.8% at 1 kHz repetition rate and without saturation leading to a peak electric field of 1 GV/m. Our results show pronounced phase matching privilege for intense terahertz generation using a pump in the 1.15 to 1.25 um range where high energy near infrared pump sources operate.
Dual scatterers preserve the helicity of an incident field, whereas antidual scatterers flip it completely. In this setting of linear electromagnetic scattering theory, we provide a completely general proof on the non-existence of passive antidual scatterers. However, we show that scatterers fulfilling the refractive index matching condition flip the helicity of the fields very efficiently without being in contradiction with the law of energy conservation. Moreover, we find that this condition is paired with the impedance matching condition in several contexts of electromagnetism and, in parti…
Unidirectional wave propagation in nonreciprocal structures enables exciting opportunities to control and enhance wave-matter interactions in extreme ways. Within this context, here we investigate the possibility of using terminated unidirectional plasmonic waveguides to enhance typically weak nonlinear effects by orders of magnitude. We theoretically demonstrate remarkable levels of electric field enhancement and confinement (field hot-spots) when the unidirectional waveguiding structure is terminated with a suitable boundary that fully stops the one-way mode. Such a large field enhancement, …
Chi-3 micro resonators have enabled compact and portable frequency comb generation, but require sophisticated dispersion control. Here we demonstrate an alternative approach using a chi-2 sheet cavity, where the dispersion requirement is relaxed by cavity phase matching. 21.2 THz broadband comb generation is achieved with uniform line spacing of 133.0 GHz, despite a relatively large dispersion of 275.4 fs^2/mm around 1064nm. With 22.6 % high slope efficiency and 14.9 kW peak power handling, this chi-2 comb can be further stabilized for navigation, telecommunication, astronomy, and spectroscopy…
We study the theory of linearly chirped biphoton wave-packets produced in two basic quasi-phase-matching configurations: chirped photonic-like crystals and aperiodically poled crystals. The novelty is that these structures are considered as definite assembles of nonlinear layers that leads to detailed description of spontaneous parametric down-conversion (SPDC) processes through the discrete Gauss sums. We demonstrate that biphoton spectra for chirped photonic crystals involving a small number of layers consist from definite well-resolved spectral lines. We also discuss the forming of broadban…
Phase-matched nonlinear processes exhibit a tradeoff between the conversion efficiency and the acceptance bandwidth. Adiabatic nonlinear processes, in which the phase mismatch varies slowly along the interaction length, enable us to overcome this tradeoff, allowing an efficient frequency conversion with broad spectral and thermal bandwidths. Until now, the variation in the phase mismatch condition was mainly based on quasi-phase matching in ferroelectric crystals. However, this solution is limited to low power sources. Here, instead, we study the adiabatic second harmonic in birefringently pha…
Energy of propagating electromagnetic waves can be fully absorbed in a thin lossy layer, but only in a narrow frequency band, as follows from the causality principle. On the other hand, it appears that there are no fundamental limitations on broadband matching of thin absorbing layers. However, known thin absorbers produce significant reflections outside of the resonant absorption band. In this paper we explore possibilities to realize a thin absorbing layer which produces no reflected waves in a very wide frequency range, while the transmission coefficient has a narrow peak of full absorption…
When a laser pump beam of sufficient intensity is incident on a Raman-active medium such as hydrogen gas, a strong Stokes signal, red-shifted by the Raman transition frequency Ω$_R$, is generated. This is accompanied by the creation of a "coherence wave" of synchronized molecular oscillations with wavevector Δβ determined by the optical dispersion. Within its lifetime, this coherence wave can be used to shift by Ω$_R$ the frequency of a third "mixing" signal, provided phase-matching is satisfied, i.e., Δβ is matched. Conventionally this can be arranged using non-collinear beams or higher-order…
Broadband dual-comb spectroscopy has attracted increasing interests due to its unique advantages in high spectral resolution, fast detection, and so on. Although the dual-comb technique is relatively mature in the infrared wavelengths, it is, currently, not commercially capable of practical applications in the terahertz regime due to the lack of high performance broadband terahertz dual-comb sources. In the terahertz frequency range, the electrically pumped quantum cascade laser (QCL) is a suitable candidate for the dual-comb operation. However, free running terahertz QCL dual-comb sources nor…
Ultra-fast laser pulses have made possible the study of extreme nonlinear processes. Many of these experiments however require a full characterization of the electric field, which typically requires a separate parametric optical process. As the central wavelength range of new sources continues to increase so too does the need for nonlinear crystals suited for characterizing these differing wavelengths. Here we report on the use of polycrystalline Zinc Selenide as a universal nonlinear crystal in the frequency resolved optical gating characterization technique from the near to long-wavelength i…
Epsilon-near-zero (ENZ) metamaterial with the relative permittivity approaching zero has been a hot research subject in the past decades. The wave in the ENZ region has infinite phase velocity ($v=1/\sqrt{\varepsilonμ}$), whereas it cannot efficiently travel into the other devices or air due to the impedance mismatch or near-zero group velocity. In this paper, we demonstrate that the tunable index-near-zero (INZ) modes with vanishing wavenumbers ($k=0$) and nonzero group velocities ($v_\mathrm{g} \neq 0$) can be achieved in nonreciprocal magneto-optical systems. This kind of INZ modes has been…
Supercontinuum generation in integrated photonic waveguides is a versatile source of broadband light, and the generated spectrum is largely determined by the phase-matching conditions. Here we show that quasi-phase-matching via periodic modulations of the waveguide structure provides a useful mechanism to control the evolution of ultrafast pulses and the supercontinuum spectrum. We experimentally demonstrate quasi-phase-matched supercontinuum to the TE20 and TE00 waveguide modes, which enhances the intensity of the SCG in specific spectral regions by as much as 20 dB. We utilize higher-order q…
Extreme-ultraviolet (XUV) sources including high-harmonic generation, free-electron lasers, soft x-ray lasers and laser-driven plasmas are widely used for applications ranging from femtochemistry and attosecond science to coherent diffractive imaging and EUV lithography. The bandwidth of the XUV light emitted by these sources reflects the XUV generation process used. While light from soft-x-ray lasers and XUV FELs typically has a relatively narrow bandwidth, plasma sources and HHG sources driven by few-cycle laser pulses emit broadband XUV pulses. Since these characteristic properties of a giv…
We propose a novel optical parametric amplification scheme which combines quasi-phase-matching with a composite pulse approach that involves crystal segments of specific lengths. The presented scheme highly increases the robustness of the frequency conversion against variations of the nonlinear coupling and of the pump, idler or signal wavelengths and has therefore the potential to enhance high amplification and broadband operation. Simulations examples applied to LiNbO_3 are given.
The resonance band in hollow-core photonic crystal fiber (HC-PCF), while leading to high-loss region in the fiber transmission spectrum, has been successfully used for generating phase-matched dispersive wave (DW). Here, we report that the spectral width of the resonance-induced DW can be largely broadened due to plasma-driven blueshifting soliton. In the experiment, we observed that in a short length of Ar-filled single-ring HC-PCF the soliton self-compression and photoionization effects caused a strong spectral blueshift of the pump pulse, changing the phase-matching condition of the DW emis…
Broadband Chromatic Dispersion of Thermo-refractive Coefficients and its Impact in Silicon Nitride Nonlinear Photonics
Joint Quantum Institute, NIST/University of Maryland（联合量子研究所，美国国家标准与技术研究院/马里兰大学）；Microsystems and Nanotechnology Division, National Institute of Standards and Technology（微系统与纳米技术部，美国国家标准与技术研究院）
