Revealing the Presence of Potential Crossings in Diatomics Induced by Quantum Cavity Radiation

Triana, Johan F.; Sanz-Vicario, José Luis

doi:10.1103/physrevlett.122.063603

Cited by 49 publications

(50 citation statements)

References 20 publications

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“…Another problem where a collaboration between theory and experiments can be fruitful is strong coupling in the gas phase. Detailed theoretical predictions about spontaneous generation of infrared light with diatomic molecules under conditions of electronic strong coupling [184,185] represent a challenge for experimental verification, as achieving the strong coupling regime with gas-phase cavities is comparably difficult, although in principle possible.…”

Section: Discussionmentioning

confidence: 99%

Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

260

248

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This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared cavities. Using a microscopic quantum electrodynamics formulation, we discuss the competition between the collective cooperative dipolar response of a molecular ensemble and local dynamical processes that molecules typically undergo, including chemical reactions. We highlight some of the observable consequences of this competition between local and collective effects in linear transmission spectroscopy, including the formal equivalence between quantum mechanical theory and the classical transfer matrix method, under specific conditions of molecular density and indistinguishability. We also overview recent experimental and theoretical developments on strong and ultrastrong coupling with electronic and vibrational transitions, with a special focus on cavity-modified chemistry and infrared spectroscopy under vibrational strong coupling. We finally suggest several opportunities for further studies that may lead to novel applications in chemical and electromagnetic sensing, energy conversion, optoelectronics, quantum control and quantum technology.

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Section: Discussionmentioning

confidence: 99%

Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

260

248

View full text Add to dashboard Cite

show abstract

“…Although many observations can be described by problemadopted quantum-optical models [21][22][23][24][25][26][27][28], ab initio methods are necessary for a detailed and unbiased understanding of the effects [17,29,30]. To this aim, some electronic structure methods have already been extended to include the photons explicitly [30][31][32][33][34][35][36][37][38][39] with quantum-electrodynamical density functional theory (QEDFT) being one of the most prominent approaches [29,[40][41][42][43]. While being formally exact, QEDFT relies on development of accurate and robust approximate functionals, which is especially challenging in case of significant correlation effects [44] and strong matter-cavity couplings [45].…”

Section: Introductionmentioning

confidence: 99%

Polaritonic coupled-cluster theory

Mordovina

Bungey

Appel

et al. 2020

Phys. Rev. Research

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We develop coupled-cluster theory for systems of electrons strongly coupled to photons, providing a promising theoretical tool in polaritonic chemistry with a perspective of application to all types of fermion-boson coupled systems. We show benchmark results for model molecular Hamiltonians coupled to cavity photons. By comparing to full configuration interaction results for various ground-state properties and optical spectra, we demonstrate that our method captures all key features present in the exact reference, including Rabi splittings and multiphoton processes. Furthermore, a path on how to incorporate our bosonic extension of coupled-cluster theory into existing quantum chemistry programs is given.

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“…In particular, real-time imaging of molecular dynamics can be achieved in experiments with a pump-probe setup with femtosecond resolution combined with the measurement of photoelectron spectra [31]. While similar approaches could in principle provide a dynamical picture of molecules under strong light-matter coupling [35][36][37], common molecular observables (such as dissociation or ionization yields or photoelectron spectra) are difficult to access in typical experimental setups, with molecules embedded in a solid-state matrix and confined within nanoscale cavities [4][5][6].…”

Section: Introductionmentioning

confidence: 99%

Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses

et al. 2020

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Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a wavepacket in the molecule. A subsequent probe pulse can then dissociates or ionizes the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. In this work, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light-matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light-matter) potentials in the strong light-matter coupling regime as well as bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a new route towards ultrafast molecular spectroscopy with plasmonic nanocavities. :1907.12607v1 [cond-mat.mes-hall] arXiv

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Revealing the Presence of Potential Crossings in Diatomics Induced by Quantum Cavity Radiation

Cited by 49 publications

References 20 publications

Molecular polaritons for controlling chemistry with quantum optics

Molecular polaritons for controlling chemistry with quantum optics

Polaritonic coupled-cluster theory

Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses

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