Computation of Second Harmonic Generation for Crystalline Urea and KDP. An ab Initio Approach through the Coupled Perturbed Hartree–Fock/Kohn–Sham Scheme

The static and dynamic electronic (hyper)polarizabilities of the equilibrium conformations of 2,2′-bithiophene (anti-gauche and syn-gauche) were computed in the gas phase. The calculations were carried out using Hartree-Fock (HF), Møller-Plesset second-order perturbation theory (MP2), and density functional theory methods. The properties were evaluated for the second harmonic generation (SHG), and electrooptical Pockels effect (EOPE) nonlinear optical processes at the typical λ=1064 nm of the Nd:YAG laser. The anti-gauche form characterized by the S–C2–C2′–S dihedral angle of 137° (MP2/6-311G**) is the global minimum on the potential energy surface, whereas the syn-gauche rotamer (S–C2–C2′–S = 48°, MP2/6-311G**) lies ca. 0.5 kcal/mol above the anti-gauche form. The structural properties of the gauche structures are rather similar to each other. The MP2 electron correlation effects are dramatic for the first-order hyperpolarizabilities of the 2,2′-bithiophenes, decreasing the HF values by ca. a factor of three. When passing from the anti-gauche to the syn-gauche conformer, the static and frequency-dependent first-order hyperpolarizabilities increase by ca. a factor of two. Differently, the electronic polarizabilities and second-order hyperpolarizabilities of these rotamers are rather close to each other. The syn-gauche structure could be discriminated from the anti-gauche one through its much more intense SHG and EOPE signals.

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Ab initio Theory of Second Harmonic Generation from Semiconductor Surfaces and Interfaces

phys stat sol (a) ◽

10.1002/1521-396x(200112)188:4<1267::aid-pssa1267>3.0.co;2-2 ◽

2001 ◽

Vol 188 (4) ◽

pp. 1267-1280 ◽

Cited By ~ 8

Author(s):

V.I. Gavrilenko

Keyword(s):

Second Harmonic Generation ◽

Ab Initio ◽

Harmonic Generation ◽

Second Harmonic ◽

Semiconductor Surfaces ◽

Surfaces And Interfaces ◽

Ab Initio Theory

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THE INVESTIGATION OF SECOND-ORDER NONLINEAR OPTICAL PROPERTIES OF P-NITROPHENYLAZOANILINE: SECOND HARMONIC GENERATION AND AB INITIO COMPUTATIONS

Journal of Theoretical and Computational Chemistry ◽

10.1142/s0219633612500149 ◽

2012 ◽

Vol 11 (01) ◽

pp. 209-221 ◽

Cited By ~ 8

Author(s):

ASLI KARAKAŞ ◽

ZİYA ERDEM KOÇ ◽

MICHAELA FRIDRICHOVÁ ◽

PETR NĚMEC ◽

JAN KROUPA

Keyword(s):

Second Harmonic Generation ◽

Harmonic Generation ◽

Density Functional ◽

Nonlinear Optical ◽

Second Harmonic ◽

Second Order ◽

Photon Absorption ◽

Nlo Properties ◽

Hartree Fock ◽

H Nmr

p-nitrophenylazoaniline (1) belongs to the family of compounds with conjugated bonds and delocalized π-electrons, structurally similar to the well known push-pull compound Disperse Red 1 (DR1).1 Due to the assembly of the molecule, nonlinear optical (NLO) properties are expectable and can be more or less accurately predicted. To estimate the potential for second-order NLO properties, the electric dipole moment (μ), dispersion-free dipole polarizabilities (α) and first hyperpolarizabilities (β) have been determined by density functional theory (DFT) quantum chemical calculations at B3LYP/ 6-311 + G(d, p) level. According to the computation results, the synthesized compound exhibits non-zero β values and it might have second-order NLO behavior. Title compound has been synthesized and characterized by FT-IR, 1H-NMR and UV-Vis spectroscopies. The maximum one-photon absorption (OPA) wavelengths were estimated to be shorter than 450 nm by quantum mechanical computations using the configuration interaction (CI) method. The same result was achieved by UV-Vis spectra measurements, whereas the compound exhibited good optical transparency to the visible light. Quantitative measurements of second harmonic generation (SHG) at 800 nm and 1064 nm have been performed. The relative efficiency comparable with that of KDP (kalium diphosphate) has been observed with the exciting wavelength of 1064 nm, while the other wavelength led to strong absorption of produced light by the sample. In the following more detailed study on frequency-dependent first hyperpolarizabilities using time-dependent Hartree–Fock (TDHF) method have been computed at the wavelengths used in SHG measurements.

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AB-Initio Calculations Of Second Order Optical Response Functions In Wurtzite GAN and ALN, And Their Short Period Superlattices

MRS Proceedings ◽

10.1557/proc-482-857 ◽

1997 ◽

Vol 482 ◽

Author(s):

Sergey N. Rashkeev ◽

Walter R. L. Lambrecht ◽

B. Segall

Keyword(s):

Band Structure ◽

Second Harmonic Generation ◽

Ab Initio Calculations ◽

Ab Initio ◽

Harmonic Generation ◽

First Principles ◽

Second Harmonic ◽

Response Functions ◽

Short Period ◽

Short Period Superlattices

AbstractSecond harmonic generation coefficients were calculated from first-principles for wurtzite GaN, AlN and the (0001) superlattices (SL) (GaN)n,(AlN)n for n = 2, 4. The effects of the LDA gap underestimate are discussed. The SLs are found to have a strongly reduced static SHG response. The frequency dependent SHG coefficients are found to be sensitive to the SL band structure and to differ significantly form a superposition of the bulk components, indicating a strong intermixing of the bands.

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Ab initio study of the enantio-selective magnetic-field-induced second harmonic generation in chiral molecules

Physical Chemistry Chemical Physics ◽

10.1039/c5cp07127e ◽

2016 ◽

Vol 18 (3) ◽

pp. 1846-1858 ◽

Cited By ~ 1

Author(s):

Antonio Rizzo ◽

G. L. J. A. Rikken ◽

R. Mathevet

Keyword(s):

Magnetic Field ◽

Magnetic Fields ◽

Second Harmonic Generation ◽

Ab Initio ◽

Harmonic Generation ◽

Second Harmonic ◽

Experimental Setup ◽

Ab Initio Study ◽

Chiral Molecules ◽

Static Magnetic Fields

Magnetic field induced SHG in chiral molecules is studied computationally. An experimental setup, exploiting intense static magnetic fields, is proposed.

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