DOE OSTI · 3000746
Perspective on Many-Body Methods for Molecular Polaritonic Systems
Abstract
Recent advances in strong light–matter interactions have revealed a wealth of new physical phenomena in molecules embedded in optical cavities, including modified chemical reactivity, altered excitation spectra, and novel quantum correlations. To describe these effects from first-principles, the field of ab initio quantum electrodynamics (QED) has emerged as a compelling extension of quantum chemistry that treats electronic and photonic degrees of freedom on equal footing. In this Perspective, we review the growing landscape of many-body QED methods, including Hartree–Fock, density functional theory (QEDFT), time-dependent DFT (QED-TDDFT), configuration interaction (QED-CI), complete active space (QED-CASSCF), coupled cluster (QED-CC), quantum Monte Carlo (QED-QMC), and density matrix renormalization group (QED-DMRG), highlighting recent developments and implementations. We further explore real-time methods, gradient and Hessian formalisms, and the integration of nonadiabatic nuclear dynamics. Applications range from benchmark simulations of polaritonic chemistry to quantum simulations on emerging quantum hardware. We conclude by outlining future directions for theory development and interdisciplinary efforts at the interface of quantum chemistry, condensed matter, and quantum optics.
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Bauman, Nicholas [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)], Cunha, Leonardo A. [Flatiron Institute, New York, NY (United States)] (ORCID:0000000326712375), DePrince III, A. Eugene [Florida State Univ., Tallahassee, FL (United States)], Flick, Johannes [Flatiron Institute, New York, NY (United States); City College of New York, NY (United States)], Foley IV, Jonathan J. [Univ. of North Carolina, Charlotte, NC (United States)], Govind, Niranjan [Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States); Univ. of Washington, Seattle, WA (United States)] (ORCID:000000033625366X), Groenhof, Gerrit [Univ. of Jyvaskyla (Finland)], Hoffmann, Norah [New York Univ. (NYU), NY (United States)], Kowalski, Karol [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)] (ORCID:000000016357785X), Li, Xiaosong [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)] (ORCID:0000000173416240), Liebenthal, Marcus [Florida State Univ., Tallahassee, FL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000288070542), Maitra, Neepa T. [Rutgers Univ., Piscataway, NJ (United States)] (ORCID:0000000218408827), Manderna, Ruby [Univ. of North Carolina, Charlotte, NC (United States)], Matoušek, Mikuláš [Czech Academy of Sciences (CAS), Prague (Czech Republic); Charles Univ., Prague (Czech Republic)], Mazin, Ilia M. [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000160848992), Mejia-Rodriguez, Daniel [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000203502941), Panyala, Ajay [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)], Peng, Bo [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000242267294), Peyton, Benjamin [Michigan State Univ., East Lansing, MI (United States)], Veis, Libor [Czech Academy of Sciences (CAS), Prague (Czech Republic)] (ORCID:0000000242296335), Vu, Nam [Univ. of North Carolina, Charlotte, NC (United States)], Weidman, Jared D. [Michigan State Univ., East Lansing, MI (United States)] (ORCID:0000000242876997), Wilson, Angela K. [Michigan State Univ., East Lansing, MI (United States)] (ORCID:0000000195001628), Zarotiadis, Rhiannon A. [New York Univ. (NYU), NY (United States)], Zhang, Yu [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000189381927). 2025-10-17. Perspective on Many-Body Methods for Molecular Polaritonic Systems. https://doi.org/10.1021/acs.jctc.5c00801
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