Simulating the control of molecular reactions via modulated light fields: from gas phase to solution

Abstract

Simulating the control of molecular reactions via modulated light fields: from gas phase to solution. Journal of Physics B-Atomic Molecular and Optical Physics, 50(8), [082001].

Theoretical Quantum Control of Fluctuating Molecular Energy Levels in Complex Chemical Environments

“…With respect to Equation , this means that the off‐diagonal elements in the energy level matrix are zero and there is no population transfer if the laser field is switched off. This population transfer is usually captured by coupling the coordinate(s) to a dissipative bath, and it has been shown that laser pulses can be designed which are robust toward this effect . The present study treats a different aspect of environmental effect, and investigates whether laser pulses can be found which also are robust toward the fluctuations of the inhomogeneous line broadening.…”

Harnessing deep neural networks to solve inverse problems in quantum dynamics: machine-learned predictions of time-dependent optimal control fields

“…Since the main purpose of this work is to harness machine learning techniques for controlling dynamic chemical systems, we only give a brief overview of quantum optimal control and point the interested reader to several topical reviews in this area. [29][30][31][32] For chemical systems, the quantum optimal control formalism commences with the time-dependent Schrödinger equation for describing the temporal dynamics of nuclei, which, in atomic units is given by…”

Pathways to New Applications for Quantum Control

“…In this section we intend to give an illustrative description of the formalism which helps us to simulate the time evolution of molecules and their interaction with light. There are several different approaches to simulations with this goal, which have been reviewed in detail elsewhere, − and each has their own purposes and advantages. Again, we will focus on the formalism we use in our group.…”

“…After the first conceptual quantum control experiments on photoexcitation of sodium iodide, applications to chemical problems followed with selective photodissociation in the gas phase, energy flow optimization in the light-harvesting complex LH2, isomerization efficiency of dye molecules in the liquid phase or isomerization of retinal, and many others. Additionally, various theories have been developed to understand how quantum control mechanisms work and to explore the characteristics, limits, and possibilities of quantum control. − The purpose of this Account, however, is not to give a comprehensive review of either experimental or theoretical accomplishments, which has been done in several topical reviews. ,− We would rather like to look ahead and inspire the field in its search for new applications, based on a personal viewpoint and on recent findings. After introducing the theoretical formalism which we use to simulate molecular wave packets (WPs) and the application and design of light fields, we highlight a few recent key advances which connect to two possible pathways toward new applications for the field of quantum control: synthetic chemistry, which always has been a main goal to apply shaped laser pulses to but has not been possible to make broadly applicable to date (primarily because of the cost of photons), and spectroscopy, where we demonstrate with a biologically relevant example how quantum control simulations can help to explore novel experimental regimes.…”