Negative Refractive Index Change Research Articles

Morphology Characterization and Refractive Index Analysis of Subsurface Ultrashort‐Pulsed Laser Modifications in ZnS

A parameter study of ultrashort pulse laser‐induced modifications in the bulk of ZnS crystals is reported. Experimental results on these modifications and their dependence on the pulse energy, writing speed, and depth are presented, with an emphasis on cross‐sectional morphology and induced refractive index changes. Localized permanent material modifications have been inscribed in the bulk of the crystal using a laser with a center emission wavelength of 2.09 μm and a pulse duration of ≈4 ps. The morphology strongly depends on the laser and optical focusing parameters, in particular, on the pulse energy and processing speed, with a significant shift in depth dependence for short pulse‐to‐pulse separations. Depending on the applied pulse energy, distortions of the lateral profile of the refractive index changes appear in the form of oscillatory features in the transverse plane relative to the inducing laser beam. The true extent of the modified material is revealed by the alternating lateral profile with largest induced negative refractive index change, Δn, of −3.88 × 10−2 ± 0.18. Such parametric insight is of critical importance for the understanding and optimization of the fabrication process and for realizing compact 3D photonic devices in the bulk of materials in a reproducible manner.

Nonvolatile optical phase shift in ferroelectric hafnium zirconium oxide

A nonvolatile optical phase shifter is a critical component for enabling the fabrication of programmable photonic integrated circuits on a Si photonics platform, facilitating communication, computing, and sensing. Although ferroelectric materials such as BaTiO3 offer nonvolatile optical phase shift capabilities, their compatibility with complementary metal-oxide-semiconductor fabs is limited. Hf0.5Zr0.5O2 is an emerging ferroelectric material, which exhibits complementary metal-oxide-semiconductor compatibility. Although extensively studied for ferroelectric transistors and memories, its application to photonics remains relatively unexplored. Here, we show the optical phase shift induced by ferroelectric Hf0.5Zr0.5O2. We observed a negative change in refractive index at a 1.55 μm wavelength in a pristine device regardless of the direction of the applied electric field. The nonvolatile phase shift was only observed once in a pristine device. This non-reversible phase shift can be attributed to the spontaneous polarization within the Hf0.5Zr0.5O2 film along the external electric field.

Propagation of adjustable anomalous hollow Gaussian beams in the cascade of left-handed and right-handed media

In this paper, the propagation characteristics of adjustable anomalous hollow Gaussian beams are investigated in different cascaded systems composed of left-handed medium and right-handed medium. The propagation expressions of adjustable anomalous hollow Gaussian beams through different cascaded systems are derived, and the effects of negative refractive index and beam parameters on the propagation characteristics are analyzed in detail. It is found that when the negative refractive index changes, the position of the maximum axial intensity is different for different cascades. But the magnitude of the maximum axial intensity is not affected by the negative refractive index. The effects of negative refractive index and beam parameters on the beam width and intensity pattern evolution are also analyzed in detail. Although the propagation characteristics in this paper are obtained under certain parameters, it is very convenient to study the evolution characteristics under various conditions through the analytical formula obtained in this paper.

Quantum Dot-Induced Blue Shift of Surface Plasmon Spectroscopy.

We experimentally demonstrate the spectral blue shift of surface plasmon resonance through the resonant coupling between quantum dots (QDs) and surface plasmons, surprisingly in contrast to the conventionally observed red shift of plasmon spectroscopy. Multimode optical fibers are used for extended resonant coupling of surface plasmons with excited states of QDs adsorbed to the plasmonic metal surface. The long-lived nature of excited QDs permits QD-induced negative change in the local refractive index near the plasmonic metal surface to cause such a blue shift. The analysis utilizes the physical causality-driven optical dispersion relation, the Kramers–Kronig (KK) relation, attempting to understand the abnormal behavior of the QDs-induced index dispersion extracted from blue shift measurement. Properties of QDs’ gain spectrally resonating with plasmons can account for such blue shift, though their absorbance properties never allow the negative index change for the blue shift observed according to the KK relation. We also discuss the limited applicability of the KK relation and possible QDs gain saturation for the experiment–theory disagreement. This work may contribute to the understanding of the photophysical properties critical for plasmonic applications, such as plasmonic local index engineering required in analyte labeling QDs coupled with plasmons for biomedical imaging or assay.

Direct laser writing of depressed-cladding waveguides in extremely low expansion lithium aluminosilicate glass-ceramics

We report on direct femtosecond laser writing of depressed-cladding optical waveguides in extremely low expansion lithium aluminosilicate glass-ceramics. The waveguide cladding was formed by space-selective vitrification of nanocrystals in laser-modified regions of glass-ceramics responsible for the negative refractive index change up to 0.005. The optical properties of the laser-written waveguides were evaluated in terms of near-field and far-field intensity distribution and propagation losses at the wavelength of 1064 nm. The possibility of single-mode waveguiding with the upper limit of propagation losses 2.4 or 2.7 dB/cm for vertically or horizontally polarized light, respectively, was demonstrated. The obtained results open up new frontiers in the laser-assisted fabrication of 3D optical waveguide circuits in the media with outstanding thermal stability.

SiO2-SnO2:Er3+ planar waveguides: Highly photorefractive glass-ceramics

For different applications in laser photonics and integrated optics, photorefractive materials are surely of great interest and play an important role in miniaturization of devices and fabrication of functional photonic structures such as gratings and waveguides. In this work, high photorefractivity of sol-gel derived SiO2-SnO2:Er3+ glass-ceramic planar waveguides, with negative effective refractive index change, is demonstrated. Through the photorefractivity investigation employing the UV pulsed KrF excimer laser (λ = 248 nm), the glass-ceramic planar waveguides show fast photorefractive response after a cumulative dose of only 0.3 kJ/cm2. A higher SnO2 content in the glass-ceramics leads to a greater change of saturated effective refractive index: Δneff = - (2.60 ± 0.20) x 10-3 at 1550 nm on the TE0 mode, for the 30 mol% SnO2 planar waveguides and Δneff = - (2.00 ± 0.20) x 10-3 on the 1550 nm TE0 mode, for the 20 mol% SnO2 ones. To investigate the structural modifications involved in the photorefractivity of the SiO2-SnO2:Er3+ glass-ceramics, XRD and Raman characterizations are employed. The grating fabrication by direct UV writing on the SiO2-SnO2:Er3+ glass-ceramic planar waveguide as well as an important reduction in the employed energy is demonstrated.

Slit Beam Shaping Technique for Femtosecond Laser Inscription of Enhanced Plane-by-Plane FBGs

In this work, the development of plane-by-plane (Plb-Pl) fiber Bragg gratings (FBGs) by using a single pulse is reported. A slit oriented along the longitudinal axis of the fiber is employed for this. The purpose is to shape the beam so that the focal volume is spatially wider in the transverse direction of the fiber. In this way, it is possible to make 2-D modifications of the refractive index whose width and height depends on the slit width and the pulse energy, respectively. Through an analytical mathematical modelling, the relationship between the diameter of the Gaussian laser beam (D ) and the slit width (s = D,) is determined in order to obtain a circular cross-section. In the experimental results carried out, it can be observed that D /D, = 3 ratio cause positive and uniform refractive index changes, compared to the negative and inhomogeneous refractive index changes corresponding to point-by-point (PbP) FBGs. Likewise, Pl-b-Pl FBGs, presenting a broader modification of the core cross-section, show significantly lower losses in transmission (0.3 dB), as well as better reflectivity and FWHM. It is observed that these three parameters (losses, reflectivity and FWHM) have a monotonous tendency according to the slit width. Polarization-dependence is also evaluated.

Nonlinear increase, invisibility, and sign inversion of a localized fs-laser-induced refractive index change in crystals and glasses

Multiphoton absorption via ultrafast laser focusing is the only technology that allows a three-dimensional structural modification of transparent materials. However, the magnitude of the refractive index change is rather limited, preventing the technology from being a tool of choice for the manufacture of compact photonic integrated circuits. We propose to address this issue by employing a femtosecond-laser-induced electronic band-gap shift (FLIBGS), which has an exponential impact on the refractive index change for propagating wavelengths approaching the material electronic resonance, as predicted by the Kramers–Kronig relations. Supported by theoretical calculations, based on a modified Sellmeier equation, the Tauc law, and waveguide bend loss calculations, we experimentally show that several applications could take advantage of this phenomenon. First, we demonstrate waveguide bends down to a submillimeter radius, which is of great interest for higher-density integration of fs-laser-written quantum and photonic circuits. We also demonstrate that the refractive index contrast can be switched from negative to positive, allowing direct waveguide inscription in crystals. Finally, the effect of the FLIBGS can compensate for the fs-laser-induced negative refractive index change, resulting in a zero refractive index change at specific wavelengths, paving the way for new invisibility applications.

Direct Laser Written Waveguide in Tellurite Glass for Supercontinuum Generation in 2 μm Spectral Range

A depressed cladding waveguide composed of 36 parallel tracks is inscribed in high purity 70TeO2-22WO3-8Bi2O3 glass by femtosecond laser operating at 1030 nm. The Sellmeier formula for the refractive index of the investigated glass is obtained for the range of 1170–2350 nm. The module of the negative refractive index change in a track is found to increase with increasing wavelength in the range of 640–2000 nm. The waveguide shows single mode behavior in the wavelength range of 1700–2100 nm with mode field diameter (MFD) of 20 μm. The propagation loss is predominantly due to scattering in the waveguide. Spectrum broadening as large as 503 nm was demonstrated in a 14 mm long waveguide pumped by femtosecond pulses at 1950 nm. In the low input pulse energy region, the spectrum broadening is well described by generalized nonlinear Shrodinger equation (GNLSE) taking into account Kerr and the Raman nonlinearities under the assumption of constant MFD along the waveguide. Under higher energy pumping, an extra broadening was observed that is attributed to the focusing effect of Kerr lens in the waveguide mode.

Double line waveguide amplifiers written by femtosecond laser irradiation in rare-earth doped germanate glasses

We report the production of active double waveguides in Er/Yb doped GeO2-PbO glasses, by direct femtosecond laser writing. The glasses were produced using the melt-quenching technique and the active waveguides were written using 30 fs laser pulses, at 800 nm, with writing speed of 0.06 mm/s and pulse energy of 32 μJ. The photo-induced negative refractive index change was of −7.4 × 10−3. The Er/Yb doped sample showed a relative gain (signal enhancement of 7.5 dB/cm, for 105 mW of 980 nm pump power. The relative gain compensates both, the propagation losses and the absorption losses, and a positive maximum internal gain of 4.6 dB/cm can be obtained at the signal wavelength of 1550 nm. The results obtained in present work demonstrate that Er/Yb glasses are promising materials for the fabrication of integrated amplifiers, lossless components and lasers based on germanate glasses.

Femtosecond laser micromachining in ophthalmic hydrogels: spectroscopic study of materials effects

Femtosecond laser micromachining relies on tightly focused, ultrashort laser pulses to locally modify material properties through nonlinear absorption, and is finding applications in the field of vision correction. Here we study the material effects of femtosecond laser micromachining in hydrogels to understand the mechanisms of laser-induced refractive index (RI) changes. Single layer dense line patterns were inscribed successively into the middle of hydrogels using a 405 nm femtosecond laser. A maximum phase change of ∼1.2 waves could be obtained at 543 nm with only 60 mW beam intensity at the focal volume. The phase change profile, fitted to a photochemical scaling model from earlier study, indicated that the micromachining process was mainly dominated by two-photon absorption. A confocal micro-Raman system was custom-designed to quantify the structural changes in written regions, especially the local water content. Change in the local water content exhibited three distinctive stages as a function of beam intensity. Below the optical breakdown threshold, a significant increase of local water content within the written layer was observed, while all Raman signatures remained the same. We posited that the negative RI changes were likely due to the generation of free radicals, followed by water permeation in the modified volume. This increase of local water content, likely presented as free water, was further confirmed by thermogravimetric analysis. Fourier-transform infrared spectroscopy was also used to gain insights into the chemical changes in the depolymerization stage.

Femtosecond laser inscription of depressed cladding single-mode mid-infrared waveguides in sapphire.

Mid-infrared optical waveguides were inscribed in sapphire with femtosecond pulses at 515nm. We show that such pulses induce a smooth negative refractive index change allowing for the inscription of a depressed cladding waveguide by closely overlapping the corresponding type I modification traces. The resulting structure consists of a highly symmetrical, uniform, and homogeneous waveguide. The size and numerical aperture of the waveguides were tailored to achieve efficient transmission in the mid-infrared. Single mode operation at a wavelength of 2850nm and propagation loss of <0.37 dB/cm are reported for a 33mm long depressed cladding waveguide. Thermal annealing was performed, and the refractive index contrast was still preserved to 50% (i.e., Δn=∼2.5×10-3) up to 1400°C.

Pulse energy dependence of refractive index change in lithium niobium silicate glass during femtosecond laser direct writing.

Femtosecond laser-induced refractive index changes in lithium niobium silicate glass were explored at high repetition rate (300 fs, 500 kHz) by polarized light microscopy, full-wave retardation plate, quantitative birefringence microscopy, and digital holographic microscopy. We found three regimes on energy increase. The first one corresponds to isotropic negative refractive index change (for pulse energy ranging 0.4-0.8 μJ/pulse, 0.6 NA, 5μm/s, 650μm focusing depth in the glass). The second one (0.8-1.2 μJ/pulse) corresponds to birefringence with well-defined slow axis orientation. The third one (above 1.2 μJ/pulse) is related to birefringence direction fluctuation. Interestingly, these regimes are consistent with crystallization ones. In addition, an asymmetric orientational writing effect has been detected on birefringence. These topics extend the possibility of controlling refractive index change in multi-component glasses.

Femtosecond laser processing induced low loss waveguides in multicomponent glasses

We have investigated that femtosecond laser induced optical waveguides in AF32 and in Borofloat-33 glasses. Type-I positive and type-II negative refractive index change mechanisms were established in AF32 and in Borofloat-33 glass waveguides, respectively. Lowest propagation loss of 1.1 ± 0.31 dB/cm could be attained in AF32 glass, which has a typically higher index change than in Borofloat-33 glass. Resultant losses are directly correlated with densification and non-bridging oxygen hole centers, which can be authenticated by Raman and photoluminescence studies.

Optical limiting performance of a GaAs/AlAs heterostructure microcavity in the near-infrared.

A multilayer GaAs/AlAs heterostructure forming a Fabry-Perot microcavity with a narrow resonance at 1.1 μm was produced by molecular-beam epitaxy. Under nanosecond pulsed laser radiation, a blueshift of the resonant line, associated with a photo-induced negative change in refractive index in GaAs, was experimentally registered by using an optical parametric oscillator. The spectral shift was accompanied by a reduction in peak transmittance, associated with nonlinear intracavity absorption. Such a cavity can be used as an optical limiter at the resonant wavelength when both the spectral shift and the transmittance reduction contribute to the limiting effect. An exceptionally low limiting threshold of about 1 mJ/cm2 was observed in the experiment.

Chemical basis for alteration of an intraocular lens using a femtosecond laser.

The chemical basis for the alteration of the refractive properties of an intraocular lens with a femtosecond laser was investigated. Three different microscope setups have been used for the study: Laser Induced Fluorescence (LIF) microscopy, Raman microscopy and coherent anti-Stokes Raman Scattering (CARS) microscopy. Photo-induced hydrolysis of polymeric material in aqueous media produces two hydrophilic functional groups: acid group and alcohol group. The spectral signatures identify two of the hydrophilic polar molecules as N-phenyl-4-(phenylazo)-benzenamine (C18H15N3) and phenazine-1-carboxylic acid (C13H8N2O2). The change in hydrophilicity results in a negative refractive index change in the laser-treated areas.

Ultrafast laser-induced refractive index changes in Ge_15As_15S_70 chalcogenide glass

Understanding and controlling laser-induced refractive index modifications in bulk chalcogenide glasses is important for a range of photonics applications targeting the mid-infrared spectral region. We focus here on material engineering aspects and pulse spatio-temporal design characteristics that are able to induce and maintain positive refractive index changes in laser-irradiated Sulfur-based chalcogenide glass, mandatory for 3D photonic design. Specifically we study the photoinscription process of a Ge-doped Sulfur-based chalcogenide glass, Ge15As15S70, irradiated by focused ultrafast near-infrared laser pulses where Ge doping plays a determinant role in generating high-contrast positive index changes. By means of aposteriori and real-time in situ observations we show that positive refractive index changes (type I) are the result of a restructuring of the glass matrix and a photo-induced contraction process initiated by two-photon electronic excitation leading to bond softening, molecular mobility, structural changes and rearrangements. Oppositely, negative refractive index changes (type II) could be associated with two different processes: photo-expansion at higher intensities and hydrodynamic evolution initiated by plasma generation and laser heating, with thermomechanical relaxation and stress unload. Alongside the role of Ge in setting various degrees of the matrix connectivity, the structural arrangement developed under different thermal history schemes for glass preparation is equally important as it defines to which extent further structural flexibility is possible. Thus we indicate the role of glass matrix metastability in generated high-contrast refractive index changes and we show that a higher degree of relaxation is an impediment for contrasted positive index changes, while these are developing in unrelaxed glasses, where several degrees of structural flexibility exist. Alongside dynamic time-resolved imaging experiments probing the development and relaxation of excitation, we also show, via static Raman analysis of the modified regions, that significant structural changes are induced by laser irradiation and we discuss the potential processes involved.

Chloride photo-thermo-refractive glasses

The known photo-thermo-refractive (PTR) glass is a photosensitive multi-component silicate glass containing fluorine and bromine and doped with cerium, antimony, and silver. The UV irradiation and subsequent heat treatment of this glass result in the crystalline phase precipitation and negative refractive index change up to 1000 ppm in the UV-irradiated area. This effect is used for holographic recording the volume Bragg’s gratings. In the present research, we developed and studied the new class of chlorine-containing PTR glasses in which the UV irradiation and subsequent heat treatment cause the precipitation of silver nanoparticles with a shell consisting of mixed silver and sodium chlorides. The growth of the shell on the silver nanoparticle was shown to lead to a local positive refractive index change in the UV-irradiated area against the unirradiated one up to 1500 ppm.

Excitation and relaxation dynamics in ultrafast laser irradiated optical glasses

We discuss the dynamics of ultrashort pulsed laser excitation in bulk optical silica-based glasses (fused silica and borosilicate BK7) well-above the permanent modification threshold. We indicate subsequent structural and thermomechanical energy relaxation paths that translate into positive and negative refractive index changes, compression and rarefaction zones. If fast electronic decay occurs at low excitation levels in fused silica via self-trapping of excitons, for carrier densities in the vicinity of the critical value at the incident wavelength, persistent long-living absorptive states indicate the achievement of low viscosity matter states manifesting pressure relaxation, rarefaction, void opening and compaction in the neighboring domains. An intermediate ps-long excited carrier dynamics is observed for BK7 in the range corresponding to structural expansion and rarefaction. The amount of excitation and the strength of the subsequent hydrodynamic evolution is critically dependent on the pulse time envelope, indicative of potential optimization schemes.

Large increase in refractive index inside silica glass after the movement of voids caused by femtosecond laser pulses

When a transparent material is irradiated by focused femtosecond laser pulses, various types of structural modification can occur inside the material. Recently, it has been reported that asymmetric structures, which are composed of two regions with positive and negative refractive index changes (Δn), can be inscribed by irradiation of multiple femtosecond laser pulses at high (∼MHz) repetition rates. Interestingly, the amount of positive Δn in this type of modification is larger than those in conventional structural modifications by one order of magnitude. However, the mechanisms underlying such modifications are still unclear. In this paper, we describe that similar asymmetric structures can be inscribed by using femtosecond laser pulses at a low repetition rate. Then, we examine the formation and spectroscopic characteristics of the asymmetric structures. The observation of the processed areas reveals that the asymmetric structures are formed after the movement of voids. Furthermore, micro-Raman spectroscopy suggests a large increase of three-membered ring structures in the region with positive Δn, which may account for the large Δn.