{"title":"Quantum electrodynamics formulation of multidimensional spectroscopy.","authors":"Frank Schlawin","doi":"10.1063/5.0267953","DOIUrl":null,"url":null,"abstract":"<p><p>We present a description of multidimensional spectroscopy, where all the light pulses are treated quantum-mechanically and the signal is expressed as a quantum dynamical map of the broadband light fields. Focusing in particular on the rephasing contribution to two-dimensional spectroscopy, we demonstrate how the semiclassical description emerges naturally as a limiting case of the quantum description. Our work establishes a formalism to apply quantum information methods to the optimization of multidimensional spectroscopy and address, e.g., fundamental resolution limits from a quantum metrological perspective.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"162 17","pages":""},"PeriodicalIF":3.1000,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1063/5.0267953","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
We present a description of multidimensional spectroscopy, where all the light pulses are treated quantum-mechanically and the signal is expressed as a quantum dynamical map of the broadband light fields. Focusing in particular on the rephasing contribution to two-dimensional spectroscopy, we demonstrate how the semiclassical description emerges naturally as a limiting case of the quantum description. Our work establishes a formalism to apply quantum information methods to the optimization of multidimensional spectroscopy and address, e.g., fundamental resolution limits from a quantum metrological perspective.
期刊介绍:
The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance.
Topical coverage includes:
Theoretical Methods and Algorithms
Advanced Experimental Techniques
Atoms, Molecules, and Clusters
Liquids, Glasses, and Crystals
Surfaces, Interfaces, and Materials
Polymers and Soft Matter
Biological Molecules and Networks.