Scissors implementation within length-gauge formulations of the frequency-dependent nonlinear optical response of semiconductors

Nastos, F.; Olejnik, B.; Schwarz, K.; Sipe, J. E.

doi:10.1103/physrevb.72.045223

Cited by 75 publications

(69 citation statements)

References 34 publications

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“…(1,2,3) we show χ (2) xyz for SiC, AlAs and GaAs with (dashed) and without (solid) the scissors correction (see Eq (44), Eq (43) and Eq (51)). A scissors correction causes a blueshift in the spectrum, as well as a redistribution of the spectral weights, resulting in an overall decreasing of the intensity, in agreement with other calculations 43,44,46,66 . In Tab.…”

Section: Resultssupporting

confidence: 74%

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Ab initiosecond-order nonlinear optics in solids: Second-harmonic generation spectroscopy from time-dependent density-functional theory

2010

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We present in detail the formulation of the ab initio theory we have developed for the calculation of the macroscopic second-order susceptibility χ (2) . We find a general expression for χ (2) valid for any fields, containing the ab initio relation between the microscopic and macroscopic formulation of the second-order responses. We consider the long wavelength limit and we develop our theory in the Time-Dependent Density-Functional Theory framework. This allows us to include straightforwardly many-body effects such as crystal local-field and excitonic effects. We compute the Second-Harmonic Generation spectra for the cubic semiconductors SiC, AlAs and GaAs and starting from the Independent-Particle Approximation for χ (2) , we include quasiparticle effects via the scissors operator, crystal local-field and excitonic effects. In particular, we consider two different types of kernels: the ALDA and the "long-range" kernel. We find good agreement with other theoretical calculations and experiments presented in literature, showing the importance of very accurate description of the many-body interactions.

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Section: Resultssupporting

confidence: 74%

“…In the second-order response the inclusion of the scissors operator is instead more complex than in the linear response as clearly pointed out by Nastos et al 66 .…”

Section: Inclusion Of the Scissors Operator In The K · P Perturbationmentioning

confidence: 64%

Ab initiosecond-order nonlinear optics in solids: Second-harmonic generation spectroscopy from time-dependent density-functional theory

2010

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“…[57] As shown in the imaginary part of the dielectric functions, we found that the optical transition along the y-axis is dominant at the band edges. The electronic band structure of β ′ -structure is plotted in Fig.…”

Section: B Linear Optical Properties and Electronic Structurementioning

confidence: 81%

Linear optical properties and electronic structures of poly(3-hexylthiophene) and poly(3-hexylselenophene) crystals from first principles

2012

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Linear optical properties of regio-regular-poly(3-hexythiophene) (rr-P3HT) and regio-regularpoly(3-hexyselenophene) (rr-P3HS) are investigated in relation to their anisotropic crystal structure by means of first-principles density functional calculations. The optical spectra are evaluated by calculating its dielectric functions, focusing on the frequency dependence of the imaginary part. The optical transition along the π-conjugation connecting backbone direction is found to be the most significant at the band edges. A group-theoretical analysis of the matrix elements is given to explain the interband transitions. The optical spectra, electronic structures and structural stabilities are calculated using the all-electron full-potential linearized augmented plane wave (FLAPW) method within the local-density approximation. We proposed several possible crystal structures of rr-P3HT, and performed structural optimizations to determine a stable structure. Comparing the total energy differences among these relaxed structures, a base-centered monoclinic structure belonging to the space group A2 is found to be the most stable structure. In the electronic structure, C and S orbitals belonging to polythiophene backbones are the biggest contributors at the valence band maximum and conduction band minimum, but there is almost no contribution from the hexyl sidechains. Lastly, the differences in electronic and optical properties between rr-P3HT and rr-P3HS are discussed. * Electronic address: tsumu@riken.jp; Present address: RIKEN, Wako, Saitama 351-0198, Japan † Jung-Hwan Song is deceased 1

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“…These integrals are to be taken over the three-dimensional k space. The k points are used for the linear analytic tetrahedron method for evaluating the three-dimensional Brillouinzone integrals [33]. Note that the Brillouin zone for the slab geometry collapses to a two-dimensional zone, with only one k point along the z axis.…”

Section: Nonlinear Susceptibility Tensormentioning

confidence: 99%

Improvedab initiocalculation of surface second-harmonic generation from Si(111)(1×1):H

et al. 2016

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We carry out an improved ab initio calculation of surface second-harmonic generation (SSHG) from the Si(111)(1×1):H surface. This calculation includes three new features in one formulation: (i) the scissors correction, (ii) the contribution of the nonlocal part of the pseudopotentials, and (iii) the inclusion of a cut function to extract the surface response, all within the independent particle approximation. We apply these improvements on the Si(111)(1×1):H surface and compare with various experimental spectra from several different sources. We also revisit the three-layer model for the SSHG yield and demonstrate that it provides more accurate results over several, more common, two-layer models. We demonstrate the importance of using properly relaxed coordinates for the theoretical calculations. We conclude that this approach to the calculation of the second-harmonic spectra is versatile and accurate within this level of approximation. This well-characterized surface offers an excellent platform for comparison with theory and allows us to offer this study as an efficient benchmark for this type of calculation.

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Scissors implementation within length-gauge formulations of the frequency-dependent nonlinear optical response of semiconductors

Cited by 75 publications

References 34 publications

Ab initiosecond-order nonlinear optics in solids: Second-harmonic generation spectroscopy from time-dependent density-functional theory

Ab initiosecond-order nonlinear optics in solids: Second-harmonic generation spectroscopy from time-dependent density-functional theory

Linear optical properties and electronic structures of poly(3-hexylthiophene) and poly(3-hexylselenophene) crystals from first principles

Improvedab initiocalculation of surface second-harmonic generation from Si(111)(1×1):H

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