Direct observation of signal evolution of slow and fast light in media with saturated and reverse saturated absorption

Recently, many researchers had reported their work about sub- and superluminal propagation. And several experiments had demonstrated the signal evolution of slow and fast light. In this letter, the authors described a simple experiment for the tracing of the light signal in saturated absorption (SA) and reverse saturated absorption (RSA) media, firstly. We had, directly, observed the evolution of slow and fast signals with different waveforms that traveled in a ruby crystal and C₆₀. Through tracking the signal when slow light (v _g ≪ c) and fast light (v _g<0) was observed in a ruby crystal and C₆₀, we concluded that asymmetrical absorption on the periodical signal could account for the generation of slow and fast light in SA and RSA media.     

Interaction of a high-power laser beam with low-density porous media

We have experimentally investigated the processes of laser light absorption and energy transfer in porous targets made of “agar-agar” (C₁₄H₁₈O₇) with an average density of 1–4 mg/cm³ illuminated by the focused beam of a neodymium laser with an intensity of 10¹⁴ W/cm² within a pulse of duration 2.5 ns. Many important scientific and technical problems, e.g., inertial-confinement thermonuclear fusion, the creation of lasers in the x-ray regime, and the modeling of astrophysical phenomena under laboratory conditions, can be successfully addressed by using low-density porous media as components of such targets. In our experiments with porous targets of variable density and thickness we used optical and x-ray diagnostic methods, which ensured that our measurements were made with high temporal and spatial resolution. We show that a region forms within the porous target consisting of a dense high-temperature plasma which effectively absorbs the laser radiation. Energy is transferred from the absorption region to the surrounding layer of porous material at up to 2×10⁷ cm/s. Experimental data are in good agreement with the predictions of our theoretical model, which takes into account the specific features of absorption of laser radiation in a porous material and is based on representing the energy transfer within the material as a hydrothermal wave. Zh. éksp. Teor. Fiz. 111, 903–918 (March 1997)     

Transient optical absorption of hole polarons in ADP (NH4H2PO4) and KDP (KH2PO4) crystals

A study of transient optical absorption of the ADP (NH₄H₂PO₄) and KDP (KH₂PO₄) nonlinear crystals in the visible and UV spectral regions is reported. Measurements made by absorption optical spectroscopy with nanosecond-time resolution established that the transient optical absorption (TOA) of these crystals originates from optical transitions in the hole A and B radicals and the optical-density relaxation kinetics is rate-controlled by interdefect tunneling recombination, which involves these hole centers and the electronic H⁰ centers representing neutral hydrogen atoms. At 290 K, hole polarons and the H⁰ centers undergo thermally stimulated migration, which is not accompanied by carrier ejection into the conduction or valence band. The slow components of the TOA kinetics with characteristic times from a few tens of milliseconds to a few seconds can be assigned to diffusion-controlled annihilation of hydrogen vacancies associated with impurity or structural defects.     

S1 singlet excited-state absorption of DODCI

1 excited-state absorption cross-section spectrum of DODCI in ethylene glycol is determined in the wavelength range from 500 nm to 750 nm. The S₁ state is populated by amplified femtosecond dye laser pulses (wavelength 592 nm) and the S₁-state absorption and emission behaviour is probed with a femtosecond light continuum. A general analysis procedure is developed to extract absolute excited-state absorption cross-sections from the measured transmissions. For DODCI in ethylene glycol the wavelength regions of saturable absorption (mode-locking application), reverse saturable absorption (optical limiter application), and effective stimulated emission (laser application) are determined. Received: 25 July 1996     

A saturable absorber, coherent population oscillations, and slow light

The paper presents a critical analysis of publications on one of the methods of creating so-called slow light (light with an anomalously low group velocity) arising due to a high steepness of the refractive index dispersion curve. The method employs, for this purpose, the effect of coherent population oscillations accompanied by burning of a narrow spectral hole in the homogeneously broadened absorption spectrum. The interpretation of the experimental data in the studies under consideration is based on the analysis of the response of a nonlinear medium to a low-frequency intensity modulation of the propagating light beam. We show that all the observations of these papers can be easily interpreted in the framework of the simplest model of a saturable absorber and have nothing to do with the hole burning effect or group velocity reduction.     

VCSEL-based oxygen spectroscopy for structural analysis of pharmaceutical solids

We present a minimalistic and flexible single-beam instrumentation based on sensitive tunable diode laser absorption spectroscopy (TDLAS) and its use in structural analysis of highly scattering pharmaceutical solids. By utilising a vertical cavity surface emitting laser (VCSEL) for sensing of molecular oxygen dispersed in tablets, we address structural properties such as porosity. Experiments involve working with unknown path lengths, severe backscattering and diffuse light. These unusual experimental conditions has led to the use of the term gas in scattering media absorption spectroscopy (GASMAS). By employing fully digital wavelength modulation spectroscopy and coherent sampling, system sensitivity in ambient air experiments reaches the 10^-7 range. Oxygen absorption exhibited by our tablets, being influenced by both sample porosity and scattering, was in the range 8×10^-5 to 2×10^-3, and corresponds to 2–50 mm of path length through ambient air (L_eq). The day-to-day reproducibility was on average 1.8% (0.3 mm L_eq), being limited by mechanical positioning. This is the first time sub-millimetre sensitivity is reached in GASMAS. We also demonstrate measurements on gas transport on a 1-s time scale. By employing pulsed illumination and time-correlated single-photon counting, we reveal that GASMAS exhibits excellent correlation with time-domain photon migration. In addition, we introduce an optical measure of porosity by relating oxygen absorption to average photon time-of-flight. Finally, the simplicity, robustness and low cost of this novel TDLAS instrumentation provide industrial potential. PACS 42.62.Fi; 39.30.+w; 78.55.Mb; 42.62.Cf; 87.64.Cc     

Thermally induced nonlinear optical response and optical power limiting of acid blue 40 dye

We report the investigations of thermally induced third-order nonlinear optical and optical limiting characterizations for various concentrations of acid blue 40 dye in N,N-Dimethyl Formamide, studied by employing z-scan technique under cw He–Ne laser irradiation at 633 nm wavelength. The samples exhibited nonlinear absorption and nonlinear refraction under the experimental conditions. For lower concentration, the samples display both saturable absorption (SA) and reverse saturable absorption (RSA); whereas with increase in concentration, RSA behaviour prevails. The estimated values of the effective coefficients of nonlinear absorption β_eff, nonlinear refraction n₂ and third-order nonlinear susceptibility χ⁽³⁾ were found to be of the order of 10^?2 cm/W, 10^?4 esu and 10^?6 esu respectively. Multiple diffraction rings were observed when the samples were exposed to laser beam due to refractive index change and thermal lensing. The effect of concentration and the laser intensity on the self-diffraction ring patterns was studied experimentally. The acid blue 40 dye also exhibited strong optical limiting properties under cw excitation and reverse saturable absorption is found to be the dominant nonlinear optical process leading to the observed nonlinear behaviour.     

Use of short-wavelength synchrotron radiation to measure luminescence quantum yield and the luminescence excitation spectrum of polymers

We describe an optical diagnostics module and the instrumental and methodological features of ultrahigh vacuum experiments investigating the optical characteristics of condensed media in the short-wavelength (hv ~ 3.5–25 eV) range of the spectrum of probing synchrotron radiation. We give a brief presentation of the results of an experimental determination of the spectral dependence of the luminescence quantum yield and the luminescence excitation spectrum of ablatable polymer dielectrics on the Kurchatov synchrotron radiation source at values of the probing radiation power density (I ₀ ~ 10¹² photons/cm²∙sec) that are below threshold for extended surface vaporization and a surface temperature of the condensed targets equal to 77–300 K.     

Metastable optical absorption of relaxed electronic excitations in BeO-Zn crystals

Spectra of metastable optical absorption and its relaxation kinetics have been studied in zinc-doped BeO crystals by time-resolved pulsed absorption spectroscopy. A comparison of the observed induced optical absorption of self-trapped excitons and small-radius excitons bound to the zinc impurity suggests that their hole components have similar structures and reveals distinctive features of “forbidden” optical transitions in the electronic components. Metastable optical absorption in Zn⁺ centers has been discovered. It is shown that the small-radius excitons bound to the zinc impurity form in the hole stages of thermally stimulated tunneling recombination processes involving Zn⁺ electronic centers. It has been found that the high recombination probability of the electronic and hole centers created in BeO-Zn crystals by an electron beam may be due to the high degree of their spatial correlation. Fiz. Tverd. Tela (St. Petersburg) 41, 601–605 (April 1999)     

Detecting a true quantum pump effect

Reflectance measurements from p-type GaSb:Zn epitaxial films with different hole concentrations (10¹⁷–10¹⁸ cm^-3) have been investigated over the frequency region of 100–1000 cm^-1. A minimum broadening feature corresponding to the hole plasmon was observed in the reflectance spectra. The experimental infrared spectra were well fitted using a Lorentz-Drude dispersion model. The real part ε₁ of the dielectric function decreases with increasing hole concentration. However, the imaginary part ε₂ increases with hole concentration in the far-infrared region. This indicates that the acoustic- and optic-phonons mainly participate in the free carrier absorption processes. The hole mobility obtained from Hall-effect measurements is slightly larger than that derived from optical measurements and the average ratio of mobilities is estimated to be 1.33. Owing to overdamping effects, the upper branch of longitudinal-optical phonon plasmon (LPP) coupled modes was observed. The upper LPP⁺ frequency increases with hole concentration and it shows a transition from phonon-like to plasmon-like behavior. A theoretical analysis with solutions in the complex frequency plane describes these experimental results.     

Mid-infrared metamaterial based on perforated SiC membrane: engineering optical response using surface phonon polaritons

We theoretically and experimentally study electromagnetic properties of a novel mid-infrared metamaterial: optically thin silicon carbide (SiC) membrane perforated by an array of sub-wavelength holes. Giant absorption and transmission is found using Fourier transformed infrared (FTIR) microscopy and explained by introducing a frequency-dependent effective permittivity ε_eff(ω) of the perforated film. The value of ε_eff(ω) is determined by the excitation of two distinct types of hole resonances: delocalized slow surface polaritons (SSPs) whose frequencies are largely determined by the array period, and a localized surface polariton (LSP) corresponding to the resonance of an isolated hole. Only SSPs are shown to modify ε_eff(ω) strongly enough to cause giant transmission and absorption. Because of the sub-wavelength period of the hole array, anomalous optical properties can be directly traced to surface polaritons, and their interpretation is not obscured by diffractive effects. Giant absorbance of this metamaterial can be utilized in designing highly efficient thermal radiation sources. PACS 41.20.Cv; 42.70.Qs; 71.45.Gm     

Structure and NLO property relationship in a novel chalcone co-crystal

Single crystals of a chalcone co-crystal (C₁₈H₁₉NO₄/C₁₇H₁₆NO₃Br; 0.972/0.028) have been grown by slow evaporation from solution. The powder second harmonic generation (SHG) efficiency of this chalcone co-crystal is 7 times that of urea. The dependence of second harmonic (SH) intensity on particle size revealed the existence of phase matching direction in this crystal. The large SHG efficiency observed is mainly due to the unidirectional alignment of molecular dipoles, in which the dipole moment of each molecule adds to establish a net polarization. The weak N–H⋅⋅⋅O hydrogen-bond interactions help to stabilize the noncentrosymmetric crystal packing and also contribute partly to the SHG. The better thermal stability, transparency and high laser damage resistance (>1.5 GW cm⁻² at 532 nm, 8 ns) of this chalcone co-crystal indicate that it is a promising material for frequency doubling of diode lasers down to 470 nm. This molecule also shows a third-order NLO response and good optical limiting property of 8 ns laser pulses at 532 nm. The mechanism for optical limiting in this chalcone was attributed to two-photon induced excited state absorption that leads to reverse saturable absorption. The structure–property relationship in this chalcone and related compounds is discussed based on the experimental results and semiempherical hyperpolarizability calculations.     

Soliton-induced supercontinuum generation in liquid-filled photonic crystal fibre

We aim to study the nonlinear optical phenomena with ultra-broadband radiation in photonic crystal fibre (PCF). While PCFs with cores made from different glasses are well studied in previous works, in this paper, it is planned to investigate the dynamics of nonlinear processes of supercontinuum generation (SCG) in liquid-filled PCF (LCPCF) to understand the physical phenomena of femtosecond pulse propagation, particularly, the temporal and spectral changes of the pulse propagating through specific PCFs. Since the CS₂-filled LCPCF has complex nonlinear phenomena, we intend to analyse the role of saturable nonlinear response and slow nonlinear response on SCG in detail. For the physical explanation, soliton fission and modulational instability techniques will be implemented to investigate the impact of slow nonlinear response and saturable nonlinear response respectively, in SCG process.     

Photoinduced light absorption by C60 films in the 0.08–4.0-eV spectral range

Spectra of photoinduced light absorption in C₆₀ films at high and low excitations in the temperature range between 15 and 300 K have been measured. In addition to the well-known explanation of photoinduced absorption in terms of optical transitions in the system of photogenerated singlet excitons, triplet excitons, and polarons, changes in the absorption spectrum of the fullerite ground state must be considered. We suggest taking into account the effect of crystal field in explaining the features of the photoinduced absorption spectrum. A feature similar to the inverted luminescence spectrum and ascribed to optical excitation of singlet excitons, which is partially allowed owing to intermolecular interaction, has been detected in spectrum of photoinduced absorption. Zh. éksp. Teor. Fiz. 112, 246–256 (July 1997)     

NO分子b4Σ--a4Πi(4,0)带的吸收光谱

通过对NO与He流动混合气体放电, 产生了激发态的NO(a⁴Π_ii) 分子. 利用光外差-浓度调制吸收光谱技术测量了NO分子在12530-12850 cm^-1波段内的吸收光谱, 并标识出b⁴Σ^--a⁴Π_i(4,0)带在该波段内的324条光谱跃迁谱线. 采用标准⁴Σ^--⁴Π_i哈密顿量模型, 通过非线性最小二乘法拟合其中267条谱线, 拟合残差(0.0071 cm^-1) 接近实验系统测量误差(0.007 cm^-1). 获得的主要分子常数与文献提供的常数符合, 并且拟合得到了精细结构分子常数.     

Recombination kinetics in nonlinear defective LiB3O5 crystals

A study of recombination kinetics in LiB₃O₅ (LBO) crystals by time-resolved luminescence and absorption spectroscopy is reported. An investigation of the kinetics of transient optical absorption (TOA) and luminescence under ns-scale electron-beam excitation performed within a broad temperature range of 77–500 K and a 1.2–5-eV spectral interval has established that the specific features in the recombination kinetics observed in LBO involve electronic, B²⁺, and hole, O⁻, trapping centers. The TOA and luminescence kinetics, as well as their temperature dependence, are interpreted by a model of competing hole centers. Relations connecting the kinetics parameters and the temperature dependence to the parameters of the main LBO point defects are presented. Fiz. Tverd. Tela (St. Petersburg) 40, 2008–2014 (November 1998)     

Optical Nonlinearity of Emerging ZrS2 and HfS2 Semiconductors

Compatible with existing processing technology, chemical vapor deposition method is used to synthesize ZrS₂ and HfS₂ films a a large scale. The nonlinear optical properties are characterized by Z-scan measurement with femtosecond pulses at 800 nm. The results show that saturable absorption happens in ZrS₂ owing to the larger ground state absorption than the excited state absorption, while reverse saturable absorption appears in HfS₂ due to the two-photon absorption. The figure of merit values of ZrS₂ (≈4.30 ± 0.12 × 10⁻¹⁵ esu cm) and HfS₂ (≈6.0 ± 1.4 × 10⁻¹⁵ esu cm) are much larger than those of MoS₂ and graphene in ultrafast nonlinear optical performance at the wavelength of 800 nm.     

The third order nonlinear optical characteristics of amorphous vanadium oxide thin film

We studied the nonlinear absorptive characteristics (saturation intensity threshold and effective nonlinear absorption coefficients) and nonlinear refraction in a 50-nm-thick VO _x thin amorphous film prepared by pulsed DC magnetron reactive sputtering. The absorptive and refractive nonlinearities were investigated by pump–probe and Z-scan techniques. The closed-aperture Z-scan results reveal self-defocussing characteristics of the amorphous VO _x thin film for both nanosecond and picosecond pulse durations. Experimental results show that a phase transition does not occur in the range of intensities used for the experiments and the investigated sample can be treated as an amorphous semiconductor structure. The open-aperture Z-scan curves with nanosecond pulses exhibit saturable absorption for all input intensities. On the other hand, the open-aperture Z-scan curves with picosecond pulses exhibit nonlinear absorption/saturable absorption for low/high input intensities, respectively. Saturation intensity thresholds were found to be 15.3 MW/cm² for 4-ns pulse duration and 586 MW/cm² for 65-ps pulse duration.     

Short-living defects and recombination processes in Li6Gd(BO3)3 crystals

Results of a study of transient optical absorption (TOA) and luminescence of lithium-gadolinium orthoborate Li₆Gd(BO₃)₃ (LGBO) in the visible and ultraviolet spectral regions are presented. As revealed by absorption optical spectroscopy with nanosecond time resolution, the LGBO TOA derives from optical transitions in hole centers, with the optical density relaxation kinetics being mediated by interdefect tunneling recombination involving these centers and neutral lithium atoms acting as electronic Li⁰ centers. At 290 K, the Li⁰ centers are involved in thermally stimulated migration, which is not accompanied by carrier transfer to the conduction or valence band. The slow TOA decay kinetics components, with characteristic times ranging from a few milliseconds to seconds, have been assigned to diffusion-limited annihilation of lithium interstitials with vacancies. The mechanisms responsible for the creation and relaxation of short-living Frenkel defect pairs in the LGBO cation sublattice have been analyzed.