Nonlinear optical response of noble metals determined from first-principles electronic structures and wave functions: Calculation of transition matrix elements

We develop a theory describing the effects of many-particle Coulomb correlations on the coherent ultrafast nonlinear optical response of semiconductors and metals. Our approach is based on a mapping of the nonlinear optical response of the "bare" system onto the linear response of a "dressed" system. The latter is characterized by effective time-dependent optical transition matrix elements, electron/hole dispersions, and interaction potentials, which in undoped semiconductors are determined by the single-exciton and two-exciton Green functions in the absence of optical fields. This mapping is achieved by eliminating the optically-induced charge fluctuations from the Hamiltonian using a Van Vleck canonical transformation. It takes into account all many-body contributions up to a given order in the optical fields as well as important Coulomb-induced quantum dynamics to all orders in the optical field. Our approach allows us to distinguish between optical nonlinearities of different origins and provides a physically-intuitive interpretation of their manifestations in ultrafast coherent nonlinear optical spectroscopy.

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The linear and nonlinear optical response of CsGeX3 (X=Cl, Br, and I): The finite field and first-principles investigation

Optik ◽

10.1016/j.ijleo.2018.10.159 ◽

2019 ◽

Vol 179 ◽

pp. 89-98 ◽

Cited By ~ 2

Author(s):

Qiaoqiao Zhang ◽

Hahaer Mushahali ◽

Haiming Duan ◽

Ming-Hsien Lee ◽

Qun Jing

Keyword(s):

Finite Field ◽

First Principles ◽

Nonlinear Optical ◽

Optical Response ◽

Nonlinear Optical Response ◽

Linear And Nonlinear

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ON A SELECTION RULE FOR ELECTRIC TRANSITIONS IN AXIALLY-SYMMETRIC NUCLEI

International Journal of Modern Physics E ◽

10.1142/s0218301310015102 ◽

2010 ◽

Vol 19 (04) ◽

pp. 685-691 ◽

Cited By ~ 1

Author(s):

A. DOBROWOLSKI ◽

A. GÓŹDŹ ◽

J. DUDEK

Keyword(s):

Transition Matrix ◽

Selection Rule ◽

Wave Functions ◽

Matrix Elements ◽

Axially Symmetric ◽

Many Body ◽

Absolute Value ◽

Angular Momenta ◽

Abrupt Changes ◽

Transition Matrix Elements

We consider many-body E-l transition matrix-elements between two nuclear states of different axially-symmetric deformations characterised by two different (mutually non-orthogonal) sets of single-particle wave-functions. Yet, when varying the deformations of the initial, final, or both these states one notices abrupt changes in the form of vanishing and possibly reappearance of the transition matrix elements calculated between the corresponding Slater determinants. The mechanism is explained in terms of the conservation of the |m| quantum number (absolute value of the projection of individual-nucleonic angular-momenta); consequences for the more general calculations of this type also without axial symmetry are discussed.

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Diamondoids in nanotechnology: First-principles simulation of electronic structure and nonlinear optical response in adamantane

2007 International Semiconductor Device Research Symposium ◽

10.1109/isdrs.2007.4422407 ◽

2007 ◽

Author(s):

Thomas F. George ◽

Guoping Zhang ◽

G. Ali Mansoori ◽

Lahsen Assoufid

Keyword(s):

Electronic Structure ◽

First Principles ◽

Nonlinear Optical ◽

Optical Response ◽

Nonlinear Optical Response

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Theoretical study on thiophene-based double helicenes with intrinsic large second-order nonlinear optical response

RSC Advances ◽

10.1039/c6ra18421a ◽

2016 ◽

Vol 6 (88) ◽

pp. 84705-84711 ◽

Cited By ~ 2

Author(s):

Yanling Si ◽

Xinyu Zhao ◽

Ziyi Su ◽

Guochun Yang

Keyword(s):

Electronic Structures ◽

Nonlinear Optical ◽

Theoretical Study ◽

Optical Response ◽

Second Order ◽

Nonlinear Optical Response ◽

High Transparency ◽

Nlo Response ◽

Nlo Materials

In view of the intrinsic non-centrosymmetric electronic structures, high transparency, and the large second-order NLO response values, the studied thiophene-based double helicenes are expected to be excellent second-order NLO materials.

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