Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Nonlinear Optics

Experiment-theory comparison and verification of metastable electronic state description of nonlinear optical response in atoms and molecules

Anand Bahl, Jared K. Wahlstrand, Howard M. Milchberg, Miroslav Kolesik

Published Jan 1, 2017• 0 citations
Publisher

Abstract

We present first of a kind, quantitative comparison between SSSI measurements of transient nonlinear polarization and plasma generation, and the metastable electronic state description of the optical response in atoms and molecules.
DOI
10.1364/nlo.2017.nth1a.2

Related papers

Exactly Solvable Light-Matter Interaction Models for Studying Filamentation Dynamics

Jeffrey M. Brown

This dissertation demonstrates the usefulness of exactly solvable quantum models in the investigation of light-matter interaction phenomena associated with the propagation of ultrashort laser pulses through gaseous media. This work fits into the larger research effort towards remedying the weaker portions of the standard set of medium modeling equations commonly used in simulations. The ultimate goal is to provide a self-consistent quantum mechanical description that can integrate Maxwell and Schrödinger systems and provide a means to realistically simulate nonlinear optical experiments on relevant scales. The study of exactly solvable models begins with one of the simplest quantum systems available, one with a 1D Dirac-delta function potential plus interaction with the light field. This model contains, in the simplest form, the most important "ingredients" that control optical filamentation, i.e. discrete and continuum electronic states. The importance of both states is emphasized in the optical intensity regime in which filaments form, where both kinds of electronic states simultaneously play a role and may not even be distinguishable. For this model atom, an analytical solution for the time-dependent light-induced atomic response from an arbitrary excitation waveform is obtained. Although this system is well-known and has been studied for decades, this result is probably the most practically useful and general one obtained thus far. Numerical implementation details of the result are also given as the task is far from trivial. Given an efficient implementation, the model is used in light-matter interaction simulations and from these it is apparent that even this toy model can qualitatively reproduce many of the nonlinear phenomena seen in experiments. Not only does this model capture the basic physics of optical filamentation, but it is also well-suited for high harmonic generation simulations. Next, a theoretical framework for using Stark resonant states (or metastable states) to represent the medium's polarization response is presented. Researchers have recognized long ago the utility of Gamow resonant states as a description of various decay processes. Even though a bound electron experiences a similar decay-like process as it transitions into the continuum upon ionization, it was unclear whether field-induced Stark resonant states carry physically relevant information. It is found that they do, and in particular it is possible to use them to capture a medium's polarization response. To this end, two quantum systems with potentials represented by a 1D Dirac-delta function and a 1D square well are solved, and all the necessary quantities for their use as medium models are presented. From these results it is possible to conjecture some general properties that hold for all resonance systems, including systems that reside in higher than one dimensional space. Finally, as a practical application of this theory, the Metastable Electronic State Approach (MESA) is presented as a quantum-based replacement for the standard medium modeling equations.

•Jan 1, 2016•0 citations

Nonlinear spectroscopy of excited atoms, molecular gases, and plasmas

S. M. Gladkov, Nikolai I Koroteev, M. V. Rychev +2 more

IzSSR•Jun 1, 1986•0 citations

Advances in response time of strong-field ionization of atoms

Jiayin Che, Chao Chen, Weiyan Li +2 more

The response time of the electron to light in photoemission is difficult to define and measure. The tunneling ionization of atoms and molecules in a strong laser field is a type of strong field-induced photoelectric effect. In this process, the electron response time will change the time of high-order harmonic generation (HHG), which will have a fundamental influence on the reconstruction of electron attosecond dynamics through HHG. We propose a simple theory to resolve the response time problem in strong field atomic tunneling ionization. The response time corresponds to the strong interaction time of three bodies i.e. Coulomb, electron and laser field, which can be determined at the quantum-classical boundary. The observable directly obtained through response time can quantitatively reproduce a series of attoclock experimental curves and provide consistent explanations for these experimental phenomena. This work introduces the main conclusions of response time theory and summarizes in detail the research progress of this theory. Firstly, this theory can be applied to the orthogonal two-color laser field to quantitatively explain the main characteristic structures of photoelectron momentum distribution (PMD). Besides, with this response time theory, the scaling law of the observable in attoclock experiment can be obtained. The proposal of scaling law is expected to provide a systematical theoretical guide for better understanding the applicability or feasibility of the attoclock under different conditions. In addition, based on the atomic response time theory, we further consider the property of multi-center Coulomb potential of molecular and develop a response time theory suitable for molecular system. Subsequently, we further apply the response time theory to polar molecules, by utilizing the asymmetry of PMD closely related to response time to recognize the permanent dipole (PD) effect within the laser sub-cycle. In the end, we discuss the prospects for research on response time. Firstly, it is envisioned to further apply response time theory to weak light and single photon transition to detect the response time of related processes. Besides, considering the significant influence of response time on the property of time-domain of HHG electron trajectories, the recombination (re-scattering) effect based on the current strong field tunneling ionization response time theory can be further investigated, thus extending this theory to describing HHG and above threshold ionization (ATI) processes. Furthermore, designing the “re-scattering electron trajectories” reconstruction scheme based on the electron trajectories with response time correction will provide important suggestions for HHG spectroscopic experiments. Finally, considering the asymmetric ionization caused by the PD effect of polar molecules, if the net ionization yield of adjacent sub-cycles is used as the current indicator, polar molecules can be used as a “micro diode” to study a type of attosecond response switching device. Polar molecular diodes emit electrons through tunneling ionization in laser field. According to the response time theory, tunneling occurs almost instantaneously, and response time needs considering only at the tunneling exit. Based on this, by searching for suitable materials (such as two-dimensional materials), it is possible to design a type of semi-classical diode (which can utilize tunneling) with femtosecond or even sub-femtosecond response time. The response time theory can provide a convenient theoretical tool for designing of such tunneling diodes.

Acta Physica Sinica•Jan 1, 2023•6 citations

Systematic errors from scalar slowing-down models in transient SERF magnetometry

Marek Kopciuch, Harini Raghavan, Morgan W. Mitchell

Reduced Bloch models of spin-exchange-relaxation-free (SERF) magnetometers commonly describe the coupled electron--nuclear spin dynamics using a single nuclear slowing-down factor. We show that this scalar description becomes inaccurate when the polarization magnitude changes appreciably. We derive an effective Bloch equation with separate longitudinal and transverse slowing-down factors, $q_\parallel(P)$ and $q_\perp(P)$, governing changes in polarization magnitude and direction. For $^{87}\mathrm{Rb}$ under representative SERF conditions and undergoing free-induction decay (FID), comparison with master-equation simulations shows that the dynamic scalar model produces a magnetic-field estimation bias of up to $4.2\%$ at high initial polarization, while fixing the slowing-down factor at a reference value increases the error to $10.1\%$. Lowering the polarization suppresses this bias but also reduces the magnetic-field information contained in the FID signal. We further show that the anisotropic response modifies noncollinear optical pumping and introduces an additional nonlinear contribution to the harmonic response under periodic driving. The resulting model retains the simplicity of a three-component Bloch description while improving the quantitative accuracy of transient and driven SERF magnetometry.

physics.atom-phCross-listedarXiv:2609.31865•Sep 29, 2026•0 citations

Polarization effects in the nonlinear ionization spectroscopy of atoms

G. A. Delone, B. A. Zon, K. B. Petrosian

MoIzN•Jan 1, 1980•0 citations

The Spectral Distribution of the Two-Photon Emission from the Metastable State of Singly Ionized Helium: Optical Collisional Excitation with Very Low Energy Metastable Positive Helium Ions.

Carmine J. Artura

•Jan 1, 1969•0 citations
This dissertation demonstrates the usefulness of exactly solvable quantum models in the investigation of light-matter interaction phenomena associated with the propagation of ultrashort laser pulses through gaseous media. This work fits into the larger research effort towards remedying the weaker portions of the standard set of medium modeling equations commonly used in simulations. The ultimate goal is to provide a self-consistent quantum mechanical description that can integrate Maxwell and Schrödinger systems and provide a means to realistically simulate nonlinear optical experiments on relevant scales. The study of exactly solvable models begins with one of the simplest quantum systems available, one with a 1D Dirac-delta function potential plus interaction with the light field. This model contains, in the simplest form, the most important "ingredients" that control optical filamentation, i.e. discrete and continuum electronic states. The importance of both states is emphasized in the optical intensity regime in which filaments form, where both kinds of electronic states simultaneously play a role and may not even be distinguishable. For this model atom, an analytical solution for the time-dependent light-induced atomic response from an arbitrary excitation waveform is obtained. Although this system is well-known and has been studied for decades, this result is probably the most practically useful and general one obtained thus far. Numerical implementation details of the result are also given as the task is far from trivial. Given an efficient implementation, the model is used in light-matter interaction simulations and from these it is apparent that even this toy model can qualitatively reproduce many of the nonlinear phenomena seen in experiments. Not only does this model capture the basic physics of optical filamentation, but it is also well-suited for high harmonic generation simulations. Next, a theoretical framework for using Stark resonant states (or metastable states) to represent the medium's polarization response is presented. Researchers have recognized long ago the utility of Gamow resonant states as a description of various decay processes. Even though a bound electron experiences a similar decay-like process as it transitions into the continuum upon ionization, it was unclear whether field-induced Stark resonant states carry physically relevant information. It is found that they do, and in particular it is possible to use them to capture a medium's polarization response. To this end, two quantum systems with potentials represented by a 1D Dirac-delta function and a 1D square well are solved, and all the necessary quantities for their use as medium models are presented. From these results it is possible to conjecture some general properties that hold for all resonance systems, including systems that reside in higher than one dimensional space. Finally, as a practical application of this theory, the Metastable Electronic State Approach (MESA) is presented as a quantum-based replacement for the standard medium modeling equations.
The response time of the electron to light in photoemission is difficult to define and measure. The tunneling ionization of atoms and molecules in a strong laser field is a type of strong field-induced photoelectric effect. In this process, the electron response time will change the time of high-order harmonic generation (HHG), which will have a fundamental influence on the reconstruction of electron attosecond dynamics through HHG. We propose a simple theory to resolve the response time problem in strong field atomic tunneling ionization. The response time corresponds to the strong interaction time of three bodies i.e. Coulomb, electron and laser field, which can be determined at the quantum-classical boundary. The observable directly obtained through response time can quantitatively reproduce a series of attoclock experimental curves and provide consistent explanations for these experimental phenomena. This work introduces the main conclusions of response time theory and summarizes in detail the research progress of this theory. Firstly, this theory can be applied to the orthogonal two-color laser field to quantitatively explain the main characteristic structures of photoelectron momentum distribution (PMD). Besides, with this response time theory, the scaling law of the observable in attoclock experiment can be obtained. The proposal of scaling law is expected to provide a systematical theoretical guide for better understanding the applicability or feasibility of the attoclock under different conditions. In addition, based on the atomic response time theory, we further consider the property of multi-center Coulomb potential of molecular and develop a response time theory suitable for molecular system. Subsequently, we further apply the response time theory to polar molecules, by utilizing the asymmetry of PMD closely related to response time to recognize the permanent dipole (PD) effect within the laser sub-cycle. In the end, we discuss the prospects for research on response time. Firstly, it is envisioned to further apply response time theory to weak light and single photon transition to detect the response time of related processes. Besides, considering the significant influence of response time on the property of time-domain of HHG electron trajectories, the recombination (re-scattering) effect based on the current strong field tunneling ionization response time theory can be further investigated, thus extending this theory to describing HHG and above threshold ionization (ATI) processes. Furthermore, designing the “re-scattering electron trajectories” reconstruction scheme based on the electron trajectories with response time correction will provide important suggestions for HHG spectroscopic experiments. Finally, considering the asymmetric ionization caused by the PD effect of polar molecules, if the net ionization yield of adjacent sub-cycles is used as the current indicator, polar molecules can be used as a “micro diode” to study a type of attosecond response switching device. Polar molecular diodes emit electrons through tunneling ionization in laser field. According to the response time theory, tunneling occurs almost instantaneously, and response time needs considering only at the tunneling exit. Based on this, by searching for suitable materials (such as two-dimensional materials), it is possible to design a type of semi-classical diode (which can utilize tunneling) with femtosecond or even sub-femtosecond response time. The response time theory can provide a convenient theoretical tool for designing of such tunneling diodes.
Reduced Bloch models of spin-exchange-relaxation-free (SERF) magnetometers commonly describe the coupled electron--nuclear spin dynamics using a single nuclear slowing-down factor. We show that this scalar description becomes inaccurate when the polarization magnitude changes appreciably. We derive an effective Bloch equation with separate longitudinal and transverse slowing-down factors, q∥(P)q_\parallel(P)q∥​(P) and q⊥(P)q_\perp(P)q⊥​(P), governing changes in polarization magnitude and direction. For 87Rb^{87}\mathrm{Rb}87Rb under representative SERF conditions and undergoing free-induction decay (FID), comparison with master-equation simulations shows that the dynamic scalar model produces a magnetic-field estimation bias of up to 4.2%4.2\%4.2% at high initial polarization, while fixing the slowing-down factor at a reference value increases the error to 10.1%10.1\%10.1%. Lowering the polarization suppresses this bias but also reduces the magnetic-field information contained in the FID signal. We further show that the anisotropic response modifies noncollinear optical pumping and introduces an additional nonlinear contribution to the harmonic response under periodic driving. The resulting model retains the simplicity of a three-component Bloch description while improving the quantitative accuracy of transient and driven SERF magnetometry.