Size effect on the SHG properties of Cu-doped CdI2 nanocrystals

Because the optically induced second harmonic generation (SHG) is prevented by symmetry in a centrosymmetric material, one needs to form noncentrosymmetric processes in order to observe the SHG. However, one of the efficient ways to enhance the noncentrosymmetricity of a material is to dope it with an appropriate impurity and amount. We grow Cu-doped CdI₂ layered nanocrystal structures from the mixture of CdI₂ and CuI using the standard Bridgman-Stockbarger method and investigate the nano-confined effects by studying the second-order optical effect via the measurements of SHG. The second-order susceptibility for the nanocrystals is calculated and the values at liquid helium temperature range from 0.38 to 0.83 pm V⁻¹ for the thicknesses of 10-0.8 nm respectively. The size dependence demonstrates the nano-sized quantum-confined effect with a clear increase in the SHG with decreasing the thickness of the nanocrystal or crystal temperature. Since the local electron-phonon anharmonicity is described by third-order rank tensors in disordered systems, the SHG is very similar to that one introduced for the third-order optical susceptibility. It has been confirmed by observing the large photoluminescent yield of the pure crystals. The Raman scattering spectra taken for thin nanocrystals confirm the phonon modes originating from interlayer phonons crucially responsible for the observed effects. The obtained results show that the Cu-doped CdI₂ layered nanocrystals are promising materials for applications in optoelectronic nano-devices.     

Study on the second-harmonic-generation of GdCa4O(BO3)3 crystals along various phase-matching directions

In this paper, the theoretical calculations of d_eff of GdCa₄O(BO₃)₃ (GdCOB) along various phase-matching (PM) directions are reported. It is shown that the maximum d_eff is out of the main planes and the d_eff in the range of (0<θ≤90, 90<φ≤180) are larger than that in the range of (0<θ≤90, 0≤φ≤90). The PM direction along (θ=66.8, φ=132.6) for GdCOB crystal has the largest d_eff. Second-harmonic-generation (SHG) experiments were performed on GdCOB crystal along various PM directions. The results show that in GdCOB crystal, the intracavity SHG conversion efficiency is 27.6% along the PM direction (θ=66.8, φ=132.6) which is larger than that along PM directions in XY and XZ main planes, which are in good agreement with the theoretical calculations. The continuous-wave (cw) green laser output power is 1.22 W when LD pump power is 10 W in the Nd:YVO₄/GdCOB laser.     

Manifestation of hexagonal-like structure in the second-order nonlinear effects in the GaN nanocrystallites

Contribution of the hexagonal-like structural components to the photoinduced second harmonic generation (SHG) in GaN large-sized nanocrystallites (with sizes about the 10–30 nm) incorporated into the polyvinylalcohol photopolymer matrices is revealed. The SHG measurements were done using pulsed Nd:YAG laser beam (λ=1.06 μm; pulse duration τ=15–50 ps, laser power about 30 MW) as a fundamental ones and a picosecond nitrogen pulsed laser (P=10 MW; λ=0.377 μm; pulse time duration τ=10–25 ps) as a photoinducing one. We have found that with increasing pumping power density the SHG output signal increases and achieves its maximum value for the power density about 2.6 GW/cm² per pulse. The maximal output photoinduced SHG signal was achieved for parallel directions of the pumping and fundamental beam polarizations. The maximal values of the second-order nonlinear susceptibilities were equal to about 1.09 pm/V. We have observed an increase of the output SHG below 30 K and for pump-probe delaying time about 18 ps. Substantial contribution to the SHG of wurtzite-like (hexagonal) structural fragments is shown.     

IR-induced nonlinear optics in Ge-doped Bi12TiO20 large-sized nanocrystallites

Photoinduced non-linear optical effects in large-sized (up to 25 nm) nanocrystallites (NC) of Ge-doped Bi₁₂TiO₂₀ (BTO:Ge) incorporated within olygoether photopolymer matrix have been studied. Photoinduced second harmonic generation (PISHG) was measured. Nd:YAG pulsed laser (λ=1.06 μm) was used as a source of photoinducing light. As a fundamental light source for the SHG and two-photon absorption, Er:LiYF₄ laser (λ=2.065 μm) was used. We have found that with increasing IR pump power density, the output doubled frequency SHG signal (λ=1.03 μm) increases and achieves its maximum value at the pump power density about 0.45 GW/cm² and NC size about 12 nm.The values of second-order optical susceptibilities were almost 20% larger than for the pure BTO NC single crystals. With decreasing temperature below 60 K, the SHG signal increases achieving maximal value at LHeT.     

Linear and Nonlinear Optical Properties Of Racemic (±)2-(α-Methylbenzylamino)-5-Nitropyridine Single Crystals

Linear and nonlinear optical properties of racemic (±)2-(α-methylbenzylamino)-5-nitropyridine ((±)MBANP) single crystals have been comprehensively investigated and compared with those of the enantiomorph (–)2-(α-methylbenzylamino)-5-nitropyridine ((–)MBANP) crystals. (±)MBANP crystal exhibits very high chemical and physical stability, but relatively small nonlinear optical coefficients (d₃₁ = 6.8 pm/V, d₃₂ = 4.7 pm/V, d₃₃ = 0.84 pm/V). A comparison between the nonlinear optical coefficients of (±)MBANP and (–)MBANP demonstrates the validity of the oriented-gas model in molecular crystals that neglects all the contributions from intermolecular interaction.     

Frequency doubling of Nd:YAG- and GaAs-lasers by KNbO3: Ta crystals

Abstract

For KNb_1-xTa_xO₃ crystals the influence of the Ta-concentration on the phase-matching properties for optical second harmonic generation (SHG) was measured. For non-critical phase matched SHG of the Nd:YAG-laser (1064nm) the coefficient d₃₁ of the tensor of the nonlinear susceptibility was applied, while for the GaAs-laser (905 nm) the coefficient d₃₂ was used. For both laser wavelengths the phase-matching temperature decreases with increasing Ta-concentration. Non-critical phase-matching at room temperature can be reached with the GaAs-laser for a Ta-concentration of ≈9%. The corresponding value for the Nd:YAG-laser is ≈14%.     

Second- and third-harmonic generations for a nondilute suspension of coated particles with radial dielectric anisotropy

We derive expressions for the effective nonlinear susceptibility tensors for both the second harmonic generation (SHG) and induced third harmonic generation (THG) of nonlinear composite materials, in which nondilute coated particles with radial dielectric anisotropy are randomly embedded in the linear host. Two types of coated particles are considered. The first is that the core possesses a second order nonlinear susceptibility and the shell is linear and radially anisotropic, while the second is that the core is linear with radial anisotropy and the shell has a second order nonlinear susceptibility. We observe greatly enhanced SHG and THG susceptibilities at several surface plasmon resonant frequencies. For the second model, due to the coating material being metallic, there exists two fundamental resonant frequencies ω_c1 and ω_c2, whose difference ω_c2-ω_c1 is strongly dependent on the interfacial parameter and the radial dielectric anisotropy. Furthermore, in both systems, the adjustment of the dielectric anisotropy results in larger enhancement of both SHG and induced THG susceptibilities at surface plasmon resonant frequencies than the corresponding isotropic systems. Therefore, both the core-shell structure and the dielectric anisotropy play important roles in determining the nonlinear enhancement and the surface resonant frequencies.     

Effect of poly silicon thickness on the formation of Ni-FUSI gate by using atomic layer deposited nickel film

The effect of poly-Si thickness on silicidation of Ni film was investigated by using X-ray diffraction, auger electron spectroscopy, cross-sectional scanning transmission electron microscopy, resistivity, I–V, and C–V measurements. The poly-Si films with various thickness of 30–200 nm were deposited by LPCVD on thermally grown 50 nm thick SiO₂, followed by deposition of Ni film right after removing the native oxide. The Ni film was prepared by using atomic layer deposition with a N²-hydroxyhexafluoroisopropyl-N¹ (Bis-Ni) precursor. Rapid thermal process was then applied for a formation of fully silicide (FUSI) gate at temperature of 500 °C in N₂ ambient during 30 s. The resultant phase of Ni-silicide was strongly dependent on the thickness of poly-Si layer, continuously changing its phase from Ni-rich (Ni₃Si₂) to Si-rich (NiSi₂) with increasing the thickness of the poly-Si layer, which is believed to be responsible for the observed flat band voltage shift, ΔV_FB, in C–V curves.     

Absolute Measurement of Second-Order Nonlinear Optical Coefficient of LiNbO3 by Parametric Processes

We have redetermined the absolute values of the nonlinear optical coefficient, d₃₁, of LiNbO₃ by parametric fluorescence and, for the first time, by difference frequency generation measurements to resolve the considerable discrepancy that existed between the values determined by second-harmonic generation (SHG) and parametric fluorescence. We obtain d₃₁ = 4.8±0.5 and 4.3±0.5 pm/V at the pump wavelengths of 488 and 532 nm, respectively, in reasonable agreement with the SHG data. It appears that the previous parametric fluorescence value, d₃₁=5.8 pm/V, was overestimated.Author to whom correspondence should be addressed.     

Linear and nonlinear optical properties of yttrium formate dihydrate,Y(HCOO)<Subscript>3</Subscript>·2H<Subscript>2</Subscript>O

Yttrium formate dihydrate, Y(HCOO)₃·2H₂O (point group 222), a promising new material for Raman laser frequency converters, has been reinvestigated with respect to the linear and nonlinear optical (second-harmonic generation, SHG) properties. High-precision data of refractive indices and their dispersion in the wavelength range 365–1083 nm are given, together with the three independent components of the tensor of nonlinear optical susceptibility (SHG) [d_ijk ^SHG]. A calculation of the macroscopic nonlinear optical susceptibility from the hyperpolarizabilities of the formate groups results in good agreement with the experimental values. This signals that the nonlinear optical interaction in Y(HCOO)₃·2H₂O can mainly be attributed to the formate groups. PACS 42.65.Ky; 42.70.Mp; 78.20.Ci     

Zero-reflection metal slabs: A mechanism of light tunneling in metamaterials

Thick metals are nearly opaque due to high reflectance and the huge third-order nonlinear susceptibility of metals is hardly utilized. In the present paper, zero-reflection phenomena in a thick metal (M) slab covered with one-dimensional dielectric photonic crystals (PC’s) (CD) _n are studied in heterostructures M(DC) _n and sandwiched structures (CD) _n M(DC) _n . Visible-light tunneling modes can be realized in M(DC) _n or (CD) _n M(DC) _n in which the optical epsilon-negative medium (metal) is paired with the PC, which mimics a lossless optical mu-negative medium in the gap region. The transmittance as high as 33% and 38% are observed at wavelength of 589 nm for M = Ag, with thickness d=60.2 nm in a heterostructure and d=83.1 nm in a sandwiched structure, respectively. The transmittance is more than 200 times larger than that of a single Ag layer with the same thickness in the latter case. Possible applications on metal-based nonlinearity enhancement and optical absorber are also discussed.     

Amorphous to crystalline transition in Dy-Fe thin films

The crystallization of vacuum-deposited amorphous Dy-Fe thin films was studied by transmission electron microscopy and electron diffraction. The effect of thickness, deposition rate and substrate temperature on the crystallization process have been investigated. The results show that the crystallization thicknessd _c decreases with increasing deposition rate and substrate temperature. The number density of Dy-Fe islands were found to be almost constant at (4–5)×10¹¹ cm^–2 in the thickness range 20 Å<d <50 Å. The number density decreases with increase ind _c .     

Electrical conduction in Cu/Mn multilayer films

Metallic superlattices of copper and manganese have been synthesized on glass and mica substrates by a sequential evaporation technique. The electrical resistivity and the temperature coefficient of resistance (TCR) of layered Cu/Mn has been studied for various thicknesses (d) in the range 2–6 nm by varying the number of double layers (n) from 5–35. The transition from a negative to positive TCR has been observed ford >5 nm. The thickness dependence of room temperature resistivity ( _RT) and TCR shows oscillatory behaviour.     

Nonlinear optical properties of Cu nanocluster composite fabricated by 180 keV ion implantation

Metal nanocluster composite glass prepared by 180 keV Cu ions into silica with dose of 5×10¹⁶ ions/cm² has been studied. The microstructural properties of the nanoclusters has been verified by optical absorption spectra and transmission electron microscopy (TEM). Third-order nonlinear optical properties of the nanoclusters were measured at 1064 and 532 nm excitations using Z-scan technique. The nonlinear refraction index, nonlinear absorption coefficient, and the real and imaginary parts of the third-order nonlinear susceptibility were deduced. Results of the investigation of nonlinear refraction by the off-axis Z-scan configuration were presented and the mechanisms responsible for the nonlinear response were discussed. Third-order nonlinear susceptibility χ⁽³⁾ of this kind of sample was determined to be 8.7×10⁻⁸ esu at 532 nm and 6.0×10⁻⁸ esu at 1064 nm, respectively.     

Second harmonic generation in transparent microcrystalline α-CdGa2S4-containing chalcogenide glass ceramics

Transparent glass ceramics were prepared by heat treating of the as-prepared 80GeS₂ · 10Ga₂S₃ · 10CdI₂ glass at 370 °C (T_g + 15 °C) for 72 h (labeled as GGCd10-370). The existence of α-CdGa₂S₄ crystal in GGCd10-370 glass ceramics has been testified by XRD and Raman spectroscopy. Using the typical Maker fringe technique, SHG was observed in the original transparent GGCd10-370 glass ceramics successfully, which is mainly ascribed to the α-CdGa₂S₄ nonlinear optical microcrystal. And the SH intensity is almost 0.8 times larger than that of the standard quartz reference. It can be also deduced that the thickness of crystalline layer is a little larger than the coherent length, l_c ≈ 2.7 μm.     

Study on nonlinear optical absorption properties of [(CH3)4N]2[Cu(dmit)2] by Z-scan technique

The third-order optical nonlinearities of an organo-metallic compound, [(CH₃)₄N]₂[Cu(dmit)₂] (dmit²⁻=4,5-dithiolate-1,3-dithiole-2-thione), abbreviated as MeCu, dissolved in acetone are characterized by Z-scan technique with picosecond and nanosecond laser pulses in the near-infrared region. Two-photon absorption has been found when the sample solution is irradiated by 40 ps pulse width at 1064 nm and the two-photon absorption (TPA) coefficient β_TPA is 4×10⁻¹³ m/W. While excited by 15 ns laser pulses at 1053 nm, the Z-scan spectra reveal strong reverse saturable absorption (RSA) and the nonlinear absorption coefficient β_RSA is estimated to be as high as 7.07×10⁻¹¹ m/W which is much larger than β_TPA. An explanation for this enhancement is given. All the results suggest that MeCu may be a promising candidate for the application to optical limiting in the near-infrared region.     

Stable bonds and unstable bonds in Y(Pr)-123 system

The Pr content dependence of the bond lengths of Y–Cu, Y–O, O–O, Cu–O, Ba–Cu and Ba–O in PrBa₂Cu₃O_y are analyzed and discussed in detail. The different valence bonds can be divided into two groups: stable bonds and unstable bonds. Since the bond lengths and angles between every two ions among O2, Cu2 and O3 are very stable, we conclude that the three ions form an unchangeable triangle when the Pr doping changes. The triangle is called “fixed triangle”. This “fixed triangle” can slightly rotate around the Cu2 ions. It is just this rotation that leads to the unstable bonds. As the increase of the Pr content, the bond lengths between the two Cu(2)–O planes becomes larger and larger, the Cu(2)–O planes bend towards the Ba–O plane. The bonds lengths between the Cu(2)–O and Ba–O planes vary oppositely from those of Cu(2)–O, and become shorter and shorter. These changes connected with the superconductivity are discussed.     

Magnetic order in CaMn2Sb2 studied via powder neutron diffraction

This paper reports a neutron powder diffraction study of CaMn₂Sb₂ in the temperature range of 20–300 K. Collinear long-range antiferromagnetic order of manganese ions occurs below 85 K, where a transition is observed in the dc magnetic susceptibility measured with a single crystal. Short-range magnetic order, characterized by a broad diffraction peak corresponding to a d-spacing of approximately 4 Å (2θ≈22°), is also observed above 20 K. The long-range antiferromagnetic order is indexed by the chemical unit cell, indicating a propagation vector k=(0 0 0), with a refined magnetic moment of 3.38 μ_B at 20 K. Two possible magnetic models have been identified, which differ in spin orientation for the two manganese ions with respect to the ab plane. The model with spins oriented at a 25±2° angle relative to the ab plane gives an improved fit compared to the other model in which the spins are constrained to the ab plane. Representational analysis can account for a model involving a c-axis component only by the mixing of two irreducible representations.     

The electronic structure of ordered Cu3Au(001)

The electronic structure of the (001) face of ordered Cu₃Au was studied using synchrotron radiation at BESSY, in the photon energy range 22–80 eV. The Cu 3d-derived bands in Cu₃Au look like the foldedd-bands of fcc Cu metal. Three Au 5d-derived bands were observed at 5.0, 6.1 and 7.0 eV below the Fermi level, which showed no dispersion with change in photon energy. The Cu 3d- and the Au 5d-derived bands are found to be separated in energy. We have calculated self-consistent energy bands along the (001) direction using the fully relativistic LMTO method. Comparison of these bands with those experimentally determined shows good agreement. From the calculated bands along –X the direction dependent densities of states were determined, which give a consistent account for the non-dispersive Au-bands.     

Calculation of current–voltage characteristics of a Cu (II) complex/n-Si/AuSb Schottky diode

In this study, Cu (II) complex/n-Si structure has been fabricated by forming a thin organic Cu (II) complex film on n-Si wafer. It has been seen that the structure has clearly shown the rectifying behaviour and can be evaluated as a Schottky diode. The contact parameters of the diode such as the barrier height and the ideality factor have been calculated using several methods proposed by different authors from current–voltage (I–V) characteristics of the device. The calculated barrier height and ideality factor values from different methods have shown the consistency of the approaches. The obtained ideality factor which is greater than unity refers the deviation from ideal diode characteristics. This deviation can be attributed to the native interfacial layer in the organic/inorganic interface and the high series resistance of the diode. In addition, the energy distribution of the interface state density (N_ss) in the semiconductor band gap at Cu (II) complex/n-Si interface obtained from I–V characteristics range from 2.15 × 10¹³ cm⁻² eV⁻¹ at (E_c − 0.66) eV to 5.56 × 10¹² cm⁻² eV⁻¹ at (E_c − 0.84) eV.