• Corpus ID: 215768601

Nonlinear Response of a Quantum System to Impulsive Perturbations: A Non-Perturbative Real-Time Approach

  title={Nonlinear Response of a Quantum System to Impulsive Perturbations: A Non-Perturbative Real-Time Approach},
  author={Alberto Guandalini and Caterina Cocchi and Stefano Pittalis and Alice Ruini and Carlo Andrea Rozzi},
  journal={arXiv: Chemical Physics},
We argue that real-time propagation of quantum states as induced by instantaneous electrical impulses can be an ideal computational tool for investigating nonlinear optical properties of many-electron systems especially when, as in the case of optical limiting, the relevant nonlinearities are not restricted to wave mixing at a predefined order. We demonstrate the capabilities of this methodology through an application to a one-dimensional model system. We show that the Fourier transform of the… 
1 Citations

Figures from this paper

Understanding real-time time-dependent density-functional theory simulations of ultrafast laser-induced dynamics in organic molecules.

This work analyzes the ultrafast dynamics of three small molecules excited by a resonant laser pulse in the framework of the adiabatic local-density approximation and observes that the laser excitation affects the vibrational spectrum by enhancing the anharmonicities therein, while the coherent vibrational motion contributes to stabilizing the electronic excitation already within a few tens of femtoseconds.



Time-dependent theory of non-linear response and current fluctuations

A general non-linear response theory is derived for an arbitrary time-dependent Hamiltonian, not obeying necessarily time-reversal symmetry. This allows us to show a generalized and current

Time-dependent density functional theory for open quantum systems with unitary propagation.

We extend the Runge-Gross theorem for a very general class of open quantum systems under weak assumptions about the nature of the bath and its coupling to the system. We show that for Kohn-Sham (KS)

Nonlinear polarization evolution using time-dependent density functional theory.

A theoretical and computational approach to investigate temporal behavior of a nonlinear polarization in a perturbative regime induced by an intense and ultrashort pulsed electric field and a decomposition of temporal and spatial changes in the electron density in power series with respect to the field amplitude is proposed.

High-order optical processes in intense laser field: Towards nonperturbative nonlinear optics

We develop an approach describing nonlinear-optical processes in the strong-field domain characterized by the nonperturbative field-with-matter interaction. The polarization of an isolated atom in

Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems.

The major theoretical developments to address ultrafast light-driven processes, such as the new theoretical framework of quantum electrodynamics density-functional formalism for the description of novel light-matter hybrid states are described.

Multiscale time-dependent density functional theory for a unified description of ultrafast dynamics: Pulsed light, electron, and lattice motions in crystalline solids

We have developed a novel multiscale computational scheme to describe coupled dynamics of light electromagnetic field with electrons and atoms in crystalline solids, where first-principles molecular

Nonlinear optics from an ab initio approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors

We present an ab-initio real-time-based computational approach to study nonlinear optical properties in condensed matter systems that is especially suitable for crystalline solids and periodic

Real-time time-dependent density functional theory approach for frequency-dependent nonlinear optical response in photonic molecules.

This approach is based on an extension of an approach previously implemented for a linear response using the electronic structure program SIESTA and uses Gaussian enveloped quasimonochromatic external fields to speed the nonlinear calculations.

Development of nonperturbative nonlinear optics models including effects of high order nonlinearities and of free electron plasma: Maxwell-Schrödinger equations coupled with evolution equations for polarization effects, and the SFA-like nonlinear optics model

This paper is dedicated to the exploration of non-conventional nonlinear optics models for intense and short electromagnetic fields propagating in a gas. When an intense field interacts with a gas,

Formal Theory of Nonlinear Response

A new method is presented of calculating nonlinear responses to external perturbations, which is based on the theory of explicitly time-dependent dynamical invariant. In terms of dynamical