Related papers: Polariton Enhanced Free Charge Carrier Generation in Donor-Acceptor Cavity Systems by a Second-Hybridization Mechanism

Polariton Enhanced Free Charge Carrier Generation in Donor-Acceptor Cavity Systems by a Second-Hybridization Mechanism

URL: http://arxiv.org/abs/2210.01278v1
Date: Mon, 3 Oct 2022 23:58:20 GMT
Title: Polariton Enhanced Free Charge Carrier Generation in Donor-Acceptor Cavity Systems by a Second-Hybridization Mechanism
Authors: Weijun Wu, Andrew E. Sifain, Courtney A. Delpo, and Gregory D. Scholes
Abstract summary: We study the quantum dynamics of a coherent donor-acceptor cavity system. We find that polaritons have the potential to connect excitonic states and charge separated states. Our work shows that polaritons can affect the charge separation mechanism and promote free charge carrier generation efficiency.
Score: 0.0
License: http://creativecommons.org/licenses/by-nc-sa/4.0/
Abstract: Cavity quantum electrodynamics has been studied as a potential approach to modify free charge carrier generation in donor-acceptor heterojunctions because of the delocalization and controllable energy level properties of hybridized light-matter states known as polaritons. However, in many experimental systems, cavity coupling decreases charge separation. Here, we theoretically study the quantum dynamics of a coherent and dissipative donor-acceptor cavity system, to investigate the dynamical mechanism and further discover the conditions under which polaritons may enhance free charge carrier generation. We use open quantum system methods based on single-pulse pumping to find that polaritons have the potential to connect excitonic states and charge separated states, further enhancing free charge generation on an ultrafast timescale of several hundred femtoseconds. The mechanism involves that polaritons with proper energy levels allow the exciton to overcome the high Coulomb barrier induced by electron-hole attraction. Moreover, we propose that a second-hybridization between a polariton state and dark states with similar energy enables the formation of the hybrid charge separated states that are optically active. These two mechanisms lead to a maximum of 50% enhancement of free charge carrier generation on a short timescale. However, our simulation reveals that on the longer timescale of picoseconds, internal conversion and cavity loss dominate and suppress free charge carrier generation, reproducing the experimental results. Thus, our work shows that polaritons can affect the charge separation mechanism and promote free charge carrier generation efficiency, but predominantly on a short timescale after photoexcitation.

Related papers

Stability and decay of subradiant patterns in a quantum gas with photon-mediated interactions [34.82692226532414]
We study subradiance in a Bose-Einstein condensate positioned at the mode crossing of two optical cavities. metastable density structures that suppress emission into one cavity mode prevent relaxation to the stationary, superradiant grating. We reproduce these dynamics by a quantum mean field model, suggesting that subradiance shares characteristics with quasi-stationary states predicted in other long-range interacting systems.
arXiv Detail & Related papers (2024-07-12T12:47:07Z)
Frequency-resolved Purcell effect for the dissipative generation of steady-state entanglement [49.1574468325115]
We report a driven-dissipative mechanism to generate stationary entangled $W$ states among strongly-interacting quantum emitters placed within a cavity. The non-harmonic energy structure of the interacting ensemble allows this transition to be resonantly selected by the cavity. Evidence of this purely dissipative mechanism should be observable in state-of-the-art cavity QED systems in the solid-state.
arXiv Detail & Related papers (2023-12-19T18:04:22Z)
Dissipative stabilization of maximal entanglement between non-identical emitters via two-photon excitation [49.1574468325115]
Two non-identical quantum emitters, when placed within a cavity and coherently excited at the two-photon resonance, can reach stationary states of nearly maximal entanglement. We show that this mechanism is merely one among a complex family of phenomena that can generate both stationary and metastable entanglement when driving the emitters at the two-photon resonance.
arXiv Detail & Related papers (2023-06-09T16:49:55Z)
Excitons guided by polaritons [0.0]
We show that an exciton on a discrete chain of sites can be guided by effective measurements induced by an ambient, non-equilibrium medium. For experimental verification, we propose a hybrid cold atom platform, carrying the exciton as electronic excitation on a chain of atoms. Despite the guiding mechanism being incoherent, the exciton pulse can be coherently transported with high fidelity.
arXiv Detail & Related papers (2023-04-28T16:10:38Z)
Unveiling the mixed nature of polaritonic transport: From enhanced diffusion to ballistic motion approaching the speed of light [0.0]
Coupling with light can enhance the diffusion coefficient of molecular excitons by six orders of magnitude. Our studies reveal intricate behavior which stems from the hybrid nature of polaritons.
arXiv Detail & Related papers (2022-05-13T14:37:31Z)
Driving Force and Nonequilibrium Vibronic Dynamics in Charge Separation of Strongly Bound Electron-Hole Pairs [59.94347858883343]
We study the dynamics of charge separation in one, two and three-dimensional donor-acceptor networks. This allows us to identify the precise conditions in which underdamped vibrational motion induces efficient long-range charge separation.
arXiv Detail & Related papers (2022-05-11T17:51:21Z)
Enhancement of Quantum Excitation Transport by Photonic Nonreciprocity [8.700048798573993]
Enhanced interaction between two two-level emitters (e.g., atoms) by nonreciprocal photonic media can be of benefit to broad areas. We show that breaking electromagnetic reciprocity makes it possible for the cooperative decay rate to exceed the spontaneous decay rate. We then show that breaking reciprocity in such a system via driving a DC current through the plasmonic material can drastically increase the probability of photon emission from one emitter to another.
arXiv Detail & Related papers (2022-04-26T17:44:52Z)
Single quantum emitters with spin ground states based on Cl bound excitons in ZnSe [55.41644538483948]
We show a new type of single photon emitter with potential electron spin qubit based on Cl impurities inSe. Results suggest single Cl impurities are suitable as single photon source with potential photonic interface.
arXiv Detail & Related papers (2022-03-11T04:29:21Z)
Entangling free electrons and optical excitations [0.0]
We propose a scheme to generate pure entanglement between designated optical excitations in a cavity and separable free-electron states. Specifically, we shape the electron wave-function profile to dramatically reduce the number of accessible cavity modes. We exemplify this concept through a theoretical description of free-electron entanglement with degenerate and nondegenerate plasmon modes in silver nanoparticles and atomic vibrations in an inorganic molecule.
arXiv Detail & Related papers (2022-02-01T17:50:03Z)
Driving chemical reactions with polariton condensates [0.0]
We study the effect of vibrational polariton condensation on the kinetics of electron transfer processes. Compared with excitation with infrared laser sources, the condensate changes the reaction yield significantly. Our results offer tantalizing opportunities to use condensates for driving chemical reactions.
arXiv Detail & Related papers (2021-06-23T04:57:35Z)
Parallel dark soliton pair in a bistable 2D exciton-polariton superfluid [47.187609203210705]
2D dark solitons are unstable and collapse into vortices due to snake instabilities. We demonstrate that a pair of dark solitons can be formed in the wake of an obstacle in a polariton flow resonantly supported by a homogeneous laser beam.
arXiv Detail & Related papers (2020-03-25T13:52:22Z)

This list is automatically generated from the titles and abstracts of the papers in this site.