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1. Direct determination of mode-projected electron-phonon coupling in the time domain

   https://doi.org/10.1126/science.aaw1662  

   Na, M. X. ; Mills, A. K. ; Boschini, F. ; Michiardi, M. ; Nosarzewski, B. ; Day, R. P. ; Razzoli, E. ; Sheyerman, A. ; Schneider, M. ; Levy, G. ; et al ( December 2019 , Science)

   Ultrafast spectroscopies have become an important tool for elucidating the microscopic description and dynamical properties of quantum materials. In particular, by tracking the dynamics of nonthermal electrons, a material’s dominant scattering processes can be revealed. Here, we present a method for extracting the electron-phonon coupling strength in the time domain, using time- and angle-resolved photoemission spectroscopy (TR-ARPES). This method is demonstrated in graphite, where we investigate the dynamics of photoinjected electrons at the$\overline{\mathrm{K}}$point, detecting quantized energy-loss processes that correspond to the emission of strongly coupled optical phonons. We show that the observed characteristic time scale for spectral weight transfer mediated by phonon-scattering processes allows for the direct quantitative extraction of electron-phonon matrix elements for specific modes.

    

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2. Exciton-polariton dynamics of the single site-controlled quantum dot-nanocavity in the coexisting strong-weak coupling regime

   https://doi.org/10.1088/1367-2630/acc26c  

   Huang, Jiahui ; Liu, Wei ; Sarihan, Murat Can ; Cheng, Xiang ; Miranda, Alessio ; Dwir, Benjamin ; Rudra, Alok ; Kapon, Eli ; Wong, Chee Wei ( March 2023 , New Journal of Physics)

   Deterministic positioning single site-controlled high symmetric InGaAs quantum dots (QDs) in (111)B-oriented GaAs photonic crystal cavities with nanometer-scale accuracy provides an idea component for building integrated quantum photonic circuits. However, it has been a long-standing challenge of improving cavityQ-factors in such systems. Here, by optimizing the trade-off between the cavity loss and QD spectral quality, we demonstrate our site-controlled QD-nanocavity system operating in the intermediate coupling regime mediated by phonon scattering, with the dynamic coexistence of strong and weak coupling. The cavity-exciton detuning-dependent micro-photoluminescence spectrum reveals concurrence of a trend of exciton-polariton mode avoided crossing, as a signature of Rabi doublet of the strongly coupled system. Meanwhile, a trend of keeping constant or slight blue shift of coupled exciton–cavity mode(CM) energy across zero-detuning is ascribed to the formation of collective states mediated by phonon-assisted coupling, and their rare partial out-of-synchronization linewidth-narrowing is linked to their coexisting strong-weak coupling regime. We further reveal the pump power-dependent anti-bunching photon statistical dynamics of this coexisting strong-weak coupled system and the optical features of strongly confined exciton-polaritons, and dark-exciton-like states. These observations demonstrate the potential capabilities of site-controlled QD-cavity systems as deterministic quantum nodes for on-chip quantum information processing and provide guidelines for future device optimization for achieving the strong coupling regime.

    

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3. Ab initio methods for polariton chemistry

   https://doi.org/10.1063/5.0167243  

   Foley, Jonathan J. ; McTague, Jonathan F. ; DePrince, A. Eugene ( December 2023 , Chemical Physics Reviews)

   Polariton chemistry exploits the strong interaction between quantized excitations in molecules and quantized photon states in optical cavities to affect chemical reactivity. Molecular polaritons have been experimentally realized by the coupling of electronic, vibrational, and rovibrational transitions to photon modes, which has spurred a tremendous theoretical effort to model and explain how polariton formation can influence chemistry. This tutorial review focuses on computational approaches for the electronic strong coupling problem through the combination of familiar techniques from ab initio electronic structure theory and cavity quantum electrodynamics, toward the goal of supplying predictive theories for polariton chemistry. Our aim is to emphasize the relevant theoretical details with enough clarity for newcomers to the field to follow, and to present simple and practical code examples to catalyze further development work.

    

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4. Influence of Mode Structure on the Generation of Phononic Frequency Combs

   Zhen Qi, Curtis R. ( March 2020 , ArXivorg)

   The mechanical analog of optical frequency combs, phononic frequency combs, has recently been demonstrated in mechanical resonators and has been attributed to coupling between multiple phonon modes. This paper investigates the influence of mode structure on comb generation using a model of two nonlinearly coupled phonon modes. The model predicts that there is only one region within the amplitude-frequency space where combs exist, and this region is a subset of the Arnold tongue that describes a 2:1 autoparametric resonance between the two modes. In addition, the location and shape of the comb region are analytically defined by the resonance frequencies, quality factors, mode coupling strength, and detuning of the driving force frequency from the mechanical resonances, providing clear conditions for comb generation. These results enable comb structure engineering for applications in areas as broad as sensing, communications, and quantum information science. 

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5. Ab initio nonadiabatic molecular dynamics of charge carriers in metal halide perovskites

   https://doi.org/10.1039/d1nr01990b  

   Li, Wei ; She, Yalan ; Vasenko, Andrey S. ; Prezhdo, Oleg V. ( June 2021 , Nanoscale)

   Photoinduced nonequilibrium processes in nanoscale materials play key roles in photovoltaic and photocatalytic applications. This review summarizes recent theoretical investigations of excited state dynamics in metal halide perovskites (MHPs), carried out using a state-of-the-art methodology combining nonadiabatic molecular dynamics with real-time time-dependent density functional theory. The simulations allow one to study evolution of charge carriers at the ab initio level and in the time-domain, in direct connection with time-resolved spectroscopy experiments. Eliminating the need for the common approximations, such as harmonic phonons, a choice of the reaction coordinate, weak electron–phonon coupling, a particular kinetic mechanism, and perturbative calculation of rate constants, we model full-dimensional quantum dynamics of electrons coupled to semiclassical vibrations. We study realistic aspects of material composition and structure and their influence on various nonequilibrium processes, including nonradiative trapping and relaxation of charge carriers, hot carrier cooling and luminescence, Auger-type charge–charge scattering, multiple excitons generation and recombination, charge and energy transfer between donor and acceptor materials, and charge recombination inside individual materials and across donor/acceptor interfaces. These phenomena are illustrated with representative materials and interfaces. Focus is placed on response to external perturbations, formation of point defects and their passivation, mixed stoichiometries, dopants, grain boundaries, and interfaces of MHPs with charge transport layers, and quantum confinement. In addition to bulk materials, perovskite quantum dots and 2D perovskites with different layer and spacer cation structures, edge passivation, and dielectric screening are discussed. The atomistic insights into excited state dynamics under realistic conditions provide the fundamental understanding needed for design of advanced solar energy and optoelectronic devices. 

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