Browse
Submit Data
Databases
API
Help

Dataset Information

28 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Theory for polariton-assisted remote energy transfer.

ABSTRACT: Strong-coupling between light and matter produces hybridized states (polaritons) whose delocalization and electromagnetic character allow for novel modifications in spectroscopy and chemical reactivity of molecular systems. Recent experiments have demonstrated remarkable distance-independent long-range energy transfer between molecules strongly coupled to optical microcavity modes. To shed light on the mechanism of this phenomenon, we present the first comprehensive theory of polariton-assisted remote energy transfer (PARET) based on strong-coupling of donor and/or acceptor chromophores to surface plasmons. Application of our theory demonstrates that PARET up to a micron is indeed possible. In particular, we report two regimes for PARET: in one case, strong-coupling to a single type of chromophore leads to transfer mediated largely by surface plasmons while in the other case, strong-coupling to both types of chromophores creates energy transfer pathways mediated by vibrational relaxation. Importantly, we highlight conditions under which coherence enhances or deteriorates these processes. For instance, while exclusive strong-coupling to donors can enhance transfer to acceptors, the reverse turns out not to be true. However, strong-coupling to acceptors can shift energy levels in a way that transfer from acceptors to donors can occur, thus yielding a chromophore role-reversal or "carnival effect". This theoretical study demonstrates the potential for confined electromagnetic fields to control and mediate PARET, thus opening doors to the design of remote mesoscale interactions between molecular systems.

SUBMITTER: Du M

PROVIDER: S-EPMC6115621 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Ultralong-Range Polariton-Assisted Energy Transfer in Organic Microcavities.

Project description:Non-radiative energy transfer between spatially-separated molecules in a microcavity can occur when an excitonic state on both molecules are strongly-coupled to the same optical mode, forming so-called "hybrid" polaritons. Such energy transfer has previously been explored when thin-films of different molecules are relatively closely spaced (≈100 nm). In this manuscript, we explore strong-coupled microcavities in which thin-films of two J-aggregated molecular dyes were separated by a spacer layer having a thickness of up to 2 μm. Here, strong light-matter coupling and hybridisation between the excitonic transition is identified using white-light reflectivity and photoluminescence emission. We use steady-state spectroscopy to demonstrate polariton-mediated energy transfer between such coupled states over "mesoscopic distances", with this process being enhanced compared to non-cavity control structures.

| S-EPMC8361947 | biostudies-literature

Cascaded exciton energy transfer in a monolayer semiconductor lateral heterostructure assisted by surface plasmon polariton.

Project description:Atomically thin lateral heterostructures based on transition metal dichalcogenides have recently been demonstrated. In monolayer transition metal dichalcogenides, exciton energy transfer is typically limited to a short range (~1??m), and additional losses may be incurred at the interfacial regions of a lateral heterostructure. To overcome these challenges, here we experimentally implement a planar metal-oxide-semiconductor structure by placing a WS2/MoS2 monolayer heterostructure on top of an Al2O3-capped Ag single-crystalline plate. We find that the exciton energy transfer range can be extended to tens of microns in the hybrid structure mediated by an exciton-surface plasmon polariton-exciton conversion mechanism, allowing cascaded exciton energy transfer from one transition metal dichalcogenides region supporting high-energy exciton resonance to a different transition metal dichalcogenides region in the lateral heterostructure with low-energy exciton resonance. The realized planar hybrid structure combines two-dimensional light-emitting materials with planar plasmonic waveguides and offers great potential for developing integrated photonic and plasmonic devices.Exciton energy transfer in monolayer transition metal dichalcogenides is limited to short distances. Here, Shi et al. fabricate a planar metal-oxide-semiconductor structure and show that exciton energy transfer can be extended to tens of microns, mediated by an exciton-surface-plasmon-polariton-exciton conversion mechanism.

| S-EPMC5484701 | biostudies-literature

Polariton-assisted excitation energy channeling in organic heterojunctions.

Project description:Exciton-polaritons are hybrid light-matter states resulting from strong exciton-photon coupling. The wave function of the polariton is a mixture of light and matter, enabling long-range energy transfer between spatially separated chromophores. Moreover, their delocalized nature, inherited from the photon component, has been predicted to enhance exciton transport. Here, we strongly couple an organic heterojunction consisting of energy/electron donor and acceptor materials to the same cavity mode. Using time-resolved spectroscopy and optoelectrical characterization, we show that the rate of exciton harvesting is enhanced with one order of magnitude and the rate of energy transfer in the system is increased two- to threefold in the strong coupling regime. Our results exemplify two means of efficiently channeling excitation energy to a heterojunction interface, where charge separation can occur. This study opens a new door to increase the overall efficiency of light harvesting systems using the tool of strong light-matter interactions.

| S-EPMC7994571 | biostudies-literature

Cavity frequency-dependent theory for vibrational polariton chemistry.

Project description:Recent experiments demonstrate the control of chemical reactivities by coupling molecules inside an optical microcavity. In contrast, transition state theory predicts no change of the reaction barrier height during this process. Here, we present a theoretical explanation of the cavity modification of the ground state reactivity in the vibrational strong coupling (VSC) regime in polariton chemistry. Our theoretical results suggest that the VSC kinetics modification is originated from the non-Markovian dynamics of the cavity radiation mode that couples to the molecule, leading to the dynamical caging effect of the reaction coordinate and the suppression of reaction rate constant for a specific range of photon frequency close to the barrier frequency. We use a simple analytical non-Markovian rate theory to describe a single molecular system coupled to a cavity mode. We demonstrate the accuracy of the rate theory by performing direct numerical calculations of the transmission coefficients with the same model of the molecule-cavity hybrid system. Our simulations and analytical theory provide a plausible explanation of the photon frequency dependent modification of the chemical reactivities in the VSC polariton chemistry.

| S-EPMC7910560 | biostudies-literature

Autologous Germline Mitochondrial Energy Transfer (AUGMENT) in Human Assisted Reproduction.

Project description:Ovarian aging is characterized by a decline in both the total number and overall quality of oocytes, the latter of which has been experimentally tied to mitochondrial dysfunction. Clinical studies in the late 1990s demonstrated that transfer of cytoplasm aspirated from eggs of young female donors into eggs of infertile women at the time of intracytoplasmic sperm injection improved pregnancy success rates. However, donor mitochondria were identified in offspring, and the United States Food and Drug Administration raised questions about delivery of foreign genetic material into human eggs at the time of fertilization. Accordingly, heterologous cytoplasmic transfer, while promising, was in effect shut down as a clinical protocol. The recent discovery of adult oogonial (oocyte-generating) stem cells in mice, and subsequently in women, has since re-opened the prospects of delivering a rich source of pristine and patient-matched germline mitochondria to boost egg health and embryonic developmental potential without the need for young donor eggs to obtain cytoplasm. Herein we overview the science behind this new protocol, which has been patented and termed autologous germline mitochondrial energy transfer, and its use to date in clinical studies for improving pregnancy success in women with a prior history of assisted reproduction failure.

| S-EPMC5545901 | biostudies-other

Long-Range and High-Efficiency Plasmon-Assisted Forster Resonance Energy Transfer.

Project description:The development of a long-range and efficient Förster resonance energy transfer (FRET) process is essential for its application in key enabling optoelectronic and sensing technologies. Via controlling the delocalization of the donor's electric field and Purcell enhancements, we experimentally demonstrate long-range and high-efficiency Förster resonance energy transfer using a plasmonic nanogap formed between a silver nanoparticle and an extended silver film. Our measurements show that the FRET range can be extended to over 200 nm while keeping the FRET efficiency over 0.38, achieving an efficiency enhancement factor of ∼108 with respect to a homogeneous environment. Reducing Purcell enhancements by removing the extended silver film increases the FRET efficiency to 0.55, at the expense of the FRET rate. We support our experimental findings with numerical calculations based on three-dimensional finite difference time-domain calculations and treat the donor and acceptor as classical dipoles. Our enhanced FRET range and efficiency structures provide a powerful strategy to develop novel optoelectronic devices and long-range FRET imaging and sensing systems.

| S-EPMC10641858 | biostudies-literature

Vibrationally Assisted Direct Intersystem Crossing between the Same Charge-Transfer States for Thermally Activated Delayed Fluorescence: Analysis by Marcus-Hush Theory Including Reorganization Energy.

Project description:Thermally activated delayed fluorescence (TADF) has recently become an extensively investigated phenomenon due to its high potential for application in organic optoelectronics. Currently, there is still lack of a model describing correctly basic photophysical parameters of organic TADF emitters. This article presents such a photophysical model describing the rates of intersystem crossing (ISC), reverse ISC (rISC), and radiative deactivation in various media and emphasizing key importance of molecular vibrations on the example of a popular TADF dye 9,10-dihydro-9,9-dimethyl-10-(4-(4,6-diphenyl-1,3,5-triazin-2-yl)phenyl)-acridine (DMAC-TRZ). The presented experimental and theoretical investigations prove that ISC and rISC can occur efficiently between the singlet and triplet states of the same charge-transfer nature (1CT and 3CT, respectively). In emitters with the orthogonal donor and acceptor fragments, such spin-forbidden 1CT ↔ 3CT transitions are activated by molecular vibrations. Namely, the change of dihedral angle between the donor and the acceptor affords reasonable spin-orbit coupling, which together with a small energy gap and reorganization energy enable 1CT ↔ 3CT transition rates reaching 1 × 107 s-1. Evidence of direct 1CT ↔ 3CT spin-flip and negligible role of a second triplet state, widely believed as a key parameter in the design of (r)ISC materials, change significantly the current understanding of TADF mechanism. In authors' opinion, photophysics, and molecular design principles of TADF emitters should be revised considering the importance of vibrationally enhanced 1CT ↔ 3CT transitions.

| S-EPMC8028332 | biostudies-literature

Tunable single emitter-cavity coupling strength through waveguide-assisted energy quantum transfer.

Project description:The emitter-cavity strong coupling manifests crucial significance for exploiting quantum technology, especially in the scale of individual emitters. However, due to the small light-matter interaction cross-section, the single emitter-cavity strong coupling has been limited by its harsh requirement on the quality factor of the cavity and the local density of optical states. Herein, we present a strategy termed waveguide-assisted energy quantum transfer (WEQT) to improve the single emitter-cavity coupling strength by extending the interaction cross-section. Multiple ancillary emitters are optically linked by a waveguide, providing an indirect coupling channel to transfer the energy quantum between target emitter and cavity. An enhancement factor of coupling strength g̃/g>10 can be easily achieved, which dramatically release the rigorous design of cavity. As an extension of concept, we further show that the ancillae can be used as controlling bits for a photon gate, opening up new degrees of freedom in quantum manipulation.

| S-EPMC11258325 | biostudies-literature

Forster energy transfer theory as reflected in the structures of photosynthetic light-harvesting systems.

Project description:Förster’s theory of resonant energy transfer underlies a fundamental process in nature, namely the harvesting of sunlight by photosynthetic life forms. The theoretical framework developed by Förster and others describes how electronic excitation migrates in the photosynthetic apparatus of plants, algae, and bacteria from light absorbing pigments to reaction centers where light energy is utilized for the eventual conversion into chemical energy. The demand for highest possible efficiency of light harvesting appears to have shaped the evolution of photosynthetic species from bacteria to plants which, despite a great variation in architecture, display common structural themes founded on the quantum physics of energy transfer as described first by Förster. Herein, Förster’s theory of excitation transfer is summarized, including recent extensions, and the relevance of the theory to photosynthetic systems as evolved in purple bacteria, cyanobacteria, and plants is demonstrated. Förster’s energy transfer formula, as used widely today in many fields of science, is also derived.

| S-EPMC3098534 | biostudies-literature

Theory of the energy transfer efficiency and fluorescence lifetime distribution in single-molecule FRET.

Project description:In single-molecule FRET experiments with pulsed lasers, not only the colors of the photons but also the fluorescence lifetimes can be monitored. Although these quantities appear to be random, they are modulated by conformational dynamics. In order to extract information about such dynamics, we develop the theory of the joint distribution of FRET efficiencies and fluorescence lifetimes determined from bins (or bursts) of photons. Our starting point is a rigorous formal expression for the distribution of the numbers of donor and acceptor photons and donor lifetimes in a bin that treats the influence of conformational dynamics on all timescales. This formula leads to an analytic result for a two-state system interconverting on a timescale slower than the interphoton time and to an efficient simulation algorithm for multistate dynamics. The shape of the joint distribution contains more information about conformational dynamics than the FRET efficiency histogram alone. In favorable cases, the connectivity of the underlying conformational states can be determined directly by simple inspection of the projection of the joint distribution on the efficiency-lifetime plane.

| S-EPMC3356627 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data