Coherent Nonlinear Optical Response for High-Intensity Excitation

Abstract

Calculation of the coherent nonlinear response of a system is essential to correctly interpret results from advanced techniques such as two-dimensional coherent spectroscopy (2DCS). Usually, even for the simplest systems, such calculations are either performed for low-intensity excitations where perturbative methods are valid and/or by assuming a simplified pulse envelope, such as a $\delta$-function in time. Here, we use the phase-cycling method for exact calculation of the nonlinear response without making the aforementioned approximations even for high-intensity excitation. We compare the simulation results to several experimental observations to prove the validity of these calculations. The saturation of the photon-echo signal from excitons in a semiconductor quantum well sample is measured. The excitation-intensity dependent measurement shows nonlinear contributions up to twelfth order. Intensity-dependent simulations reproduce this effect without explicitly considering higher-order interactions. Additionally, we present simulation results that replicate previously-reported experiments with high-intensity excitation of semiconductor quantum dots. By accurately reproducing a variety of phenomena such as higher-order contributions, switching of coherent signal, and changes in photon-echo transients, we prove the efficacy of the phase-cycling method to calculate the coherent nonlinear signal for high-intensity excitation. This method would be particularly useful for systems with multiple, well-separated peaks and/or large inhomogeneity.

References in corpus (20)

• Multidimensional Coherent Photocurrent Spectroscopy of a Semiconductor Nanostructure
• A Versatile Ultra-Stable Platform for Optical Multidimensional Fourier-Transform Spectroscopy
• Coherent Electronic Coupling in Atomically Thin MoSe2
• Coherent control of a V-type three-level system in a single quantum dot
• Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with 2D spectroscopy
• Multi-Wave Coherent Control of a Solid State Single Emitter
• Controlling Coherent Quantum Dot Interactions
• Ultrafast Photo-Induced Charge Transfer Unveiled by Two-Dimensional Electronic Spectroscopy
• Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots
• Oriented polaritons in strongly-coupled asymmetric double quantum well microcavities
• Quantum Dynamics of Attractive and Repulsive Polarons in a Doped MoSe${}_2$ Monolayer
• Hidden Silicon-Vacancy Centers in Diamond
• Photon echo transients from an inhomogeneous ensemble of semiconductor quantum dots
• Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach
• Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor
• Calculating non-linear response functions for multi-dimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion
• Automatic Feynman diagram generation for nonlinear optical spectroscopies
• Two-dimensional spectroscopy beyond the perturbative limit: the influence of finite pulses and detection modes
• Many-body interaction in semiconductors probed with 2D Fourier spectroscopy
• Exciton-exciton Interactions -- A Quantitative Comparison Between Complimentary Phenomenological Models

Cited by in corpus (2)

• Excitation-pulse intensity mediated control of coherent nonlinear optical response of a V-type system
• Quantitative Lineshape Analysis for Arbitrary Inhomogeneity in Two-Dimensional Coherent Spectroscopy