Phase memory of the electronic polarization in transient nonlinear optical spectra of gallium arsenide at 2 eV

1990 ◽  
Vol 41 (11) ◽  
pp. 7549-7558 ◽  
Author(s):  
G. Böhne ◽  
T. Sure ◽  
R. G. Ulbrich ◽  
W. Schäfer
Keyword(s):  
Gallium Arsenide ◽  
Nonlinear Optical ◽  
Optical Spectra ◽  
Electronic Polarization ◽  
Phase Memory

Few-Particle Effects in Nonlinear Optical Spectra of Semiconductor Quantum Dots

1999 ◽  
Vol 571 ◽  
Author(s):  
Ulrich Hohenesteri ◽  
Fausto Rossi ◽  
Elisa Molinari
Keyword(s):  
Quantum Dots ◽  
Density Matrix ◽  
Nonlinear Optical ◽  
Coherent Control ◽  
Optical Spectra ◽  
Carrier Dynamics ◽  
Semiconductor Quantum Dots ◽  
Nonequilibrium Carrier ◽  
Optical Nonlinearities ◽  
Matrix Approach

ABSTRACTWe present a density-matrix approach for the description of nonequilibrium carrier dynamics in optically excited semiconductor quantum dots, that explicitly accounts for exciton-exciton as well as exciton-carrier interactions. Within this framework, we analyze few-particle effects in the optical spectra and provide a consistent description of additional peaks appearing at high photoexcitation density. We discuss possible applications of such optical nonlinearities in future coherent-control experiments.

The Influence of Electronic Polarization on Nonlinear Optical Spectroscopy

2021 ◽  
Author(s):  
Shao-Yu Lu ◽  
Tim J. Zuehlsdorff ◽  
Hanbo Hong ◽  
Vincent P. Aguirre ◽  
Christine M. Isborn ◽  
...  
Keyword(s):  
Optical Spectroscopy ◽  
Nonlinear Optical ◽  
Electronic Polarization ◽  
Nonlinear Optical Spectroscopy

scholarly journals Nonlinear Spectroscopy in the Condensed Phase: The Role of Duschinsky Rotations and Third Order Cumulant Contributions

2020 ◽  
Author(s):  
Tim Zuehlsdorff ◽  
Hanbo Hong ◽  
Liang Shi ◽  
Christine Isborn
Keyword(s):  
Excited State ◽  
Condensed Phase ◽  
Nonlinear Optical ◽  
Order Term ◽  
Optical Spectra ◽  
Cumulant Expansion ◽  
Third Order ◽  
The Third ◽  
Mode Mixing

First-principles modeling of nonlinear optical spectra in the condensed phase is highly challenging because both environment and vibronic interactions can play a large role in determining spectral shapes and excited state dynamics. Here, we compute two dimensional electronic spectroscopy (2DES) signals based on a cumulant expansion of the energy gap fluctuation operator, with a specific focus on analyzing mode mixing effects introduced by the Duschinsky rotation and the role of the third order term in the cumulant expansion for both model and realistic condensed phase systems. We show that for a harmonic model system, the third order cumulant correction captures effects introduced by a mismatch in curvatures of ground and excited state potential energy surfaces, as well as effects of mode mixing. We also demonstrate that 2DES signals can be accurately reconstructed from purely classical correlation functions using quantum correction factors. We then compute nonlinear optical spectra for the Nile red and Methylene blue chromophores in solution, assessing the third order cumulant contribution for realistic systems. We show that the third order cumulant correction is strongly dependent on the treatment of the solvent environment, revealing the interplay between environmental polarization and the electronic-vibrational coupling.

scholarly journals Nonlinear Spectroscopy in the Condensed Phase: The Role of Duschinsky Rotations and Third Order Cumulant Contributions

2020 ◽  
Author(s):  
Tim Zuehlsdorff ◽  
Hanbo Hong ◽  
Liang Shi ◽  
Christine Isborn
Keyword(s):  
Excited State ◽  
Condensed Phase ◽  
Nonlinear Optical ◽  
Order Term ◽  
Optical Spectra ◽  
Cumulant Expansion ◽  
Third Order ◽  
The Third ◽  
Mode Mixing

First-principles modeling of nonlinear optical spectra in the condensed phase is highly challenging because both environment and vibronic interactions can play a large role in determining spectral shapes and excited state dynamics. Here, we compute two dimensional electronic spectroscopy (2DES) signals based on a cumulant expansion of the energy gap fluctuation operator, with a specific focus on analyzing mode mixing effects introduced by the Duschinsky rotation and the role of the third order term in the cumulant expansion for both model and realistic condensed phase systems. We show that for a harmonic model system, the third order cumulant correction captures effects introduced by a mismatch in curvatures of ground and excited state potential energy surfaces, as well as effects of mode mixing. We also demonstrate that 2DES signals can be accurately reconstructed from purely classical correlation functions using quantum correction factors. We then compute nonlinear optical spectra for the Nile red and Methylene blue chromophores in solution, assessing the third order cumulant contribution for realistic systems. We show that the third order cumulant correction is strongly dependent on the treatment of the solvent environment, revealing the interplay between environmental polarization and the electronic-vibrational coupling.

Sign in / Sign up

Export Citation Format

Share Document