An Exact Expression for Multidimensional Spectroscopy of a Spin‐Boson Hamiltonian

Liu, Albert

doi:10.1002/qute.202300399

An Exact Expression for Multidimensional Spectroscopy of a Spin‐Boson Hamiltonian

Journal Article · Mon Feb 05 00:00:00 EST 2024 · Advanced Quantum Technologies

DOI:https://doi.org/10.1002/qute.202300399· OSTI ID:2283309

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Brookhaven National Laboratory (BNL), Upton, NY (United States)

Multidimensional coherent spectroscopy is a powerful tool to characterize nonlinear optical response functions. Typically, multidimensional spectra are interpreted via a perturbative framework that straightforwardly provides intuition into the density matrix dynamics that give rise to specific spectral features. When the goal is to characterize system coupling to a thermal bath however, the perturbative formalism becomes unwieldy and yields less intuition. Here, an approach developed by Vagov et al. is extended to provide an exact expression for multidimensional spectra of a spin-boson Hamiltonian up to arbitrary order of electric field interaction. Furthermore, the utility of this expression is demonstrated by modeling polaron formation and coherent exciton-phonon coupling in quantum dots, which strongly agree with experiment.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: BNL Program Development; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 2283309

Alternate ID(s):: OSTI ID: 2290394

Report Number(s):: BNL--225240-2024-JAAM

Journal Information:: Advanced Quantum Technologies, Journal Name: Advanced Quantum Technologies Journal Issue: 3 Vol. 7; ISSN 2511-9044

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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