Coherent Biexciton Transport in the Presence of Exciton-Exciton Annihilation in Molecular Aggregates

• URL: http://arxiv.org/abs/2603.04483v1
• Date: Wed, 04 Mar 2026 18:49:47 GMT
• Title: Coherent Biexciton Transport in the Presence of Exciton-Exciton Annihilation in Molecular Aggregates
• Abstract summary: Incoherent initial conditions lead to strongly non-exponential relaxation and time-dependent diffusion.<n>Coherent-to-incoherent crossover and the diffusive spreading of the exciton density are sensitive to internal conversion processes.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We present a theoretical framework for biexciton dynamics in molecular aggregates that explicitly treats populations and coherences across excitation manifolds within a reduced density-matrix formalism. By extending kinetic descriptions beyond the weak-coupling limit, the approach captures the influence of exciton delocalization and exciton-exciton annihilation while remaining computationally tractable within a Markovian description of environmental relaxation. Using this framework, we investigate how the spatial profile and momentum composition of the initial biexciton state govern fluorescence decay and transport. Incoherent initial conditions lead to strongly non-exponential relaxation and time-dependent diffusion driven by nonlinear population kinetics. In contrast, coherently prepared biexciton states exhibit pronounced early-time coherent transport, whose character depends sensitively on whether the initial state is prepared as a standing-wave or traveling-wave superposition of single-exciton modes. Despite nearly identical emission dynamics for J and H aggregate, biexciton transport properties differ markedly due to band structure-dependent interference effect. Our results demonstrate that biexciton dynamics remains strongly influenced by initial-state coherence and momentum composition. Besides initial-state preparation, the coherent-to-incoherent crossover and the diffusive spreading of the exciton density are sensitive to internal conversion processes such as exciton fusion and the decay to the first excited state. The present work establishes initial-state preparation as a key control parameter for many-exciton transport in excitonic systems and provides a general framework for interpreting nonlinear optical experiments beyond population-based descriptions.

Related papers

• Klein--Gordon Dynamics from Intrinsic Phase Periodicity [0.0]
  We show that the Klein--Gordon equation arises as the minimal local, linear, Lorentz-invariant field equation compatible with the internal phase structure.<n>Within this framework, mass acts as an intrinsic frequency scale governing wave propagation, and relativistic kinematics is fully recovered.
  arXiv  Detail & Related papers  (2026-06-24T15:07:21Z)
• Electrodynamics as a Theory of Persistent Stochastic Processes [0.0]
  A process-theoretic approach to electrodynamics based on persistent Kac-type processes is developed.<n> relativistic wave equations arise as emergent descriptions after analytic continuation of Telegrapher-type dynamics.<n>The framework is not intended to modify the successful empirical predictions of quantum electrodynamics.
  arXiv  Detail & Related papers  (2026-05-23T10:01:32Z)
• Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer [6.900133159039129]
  Exciton transport in molecular aggregates is a fundamental process governing the performance of organic optoelectronics and light-harvesting systems.<n>Recent advances in ultrafast spectroscopy have brought into focus the short-time regime, in which exciton motion remains ballistic on femtosecond-to-picosecond timescales.<n>We develop an analytical framework for short-time exciton dynamics in a one-dimensional lattice subject to both on-site energetic (diagonal) disorder and intermolecular coupling fluctuations.
  arXiv  Detail & Related papers  (2026-03-24T16:57:00Z)
• Ising-Induced Spectral Broadening Resolves the Relaxation Bottleneck in Superradiant Masers [0.0]
  We show that diagonal Ising interactions generate profound inhomogeneous broadening that exceeds the intrinsic single-particle dephasing.<n>This intense diagonal disorder suppresses resonant flip-flop exchange, effectively renormalizing the density of states available for spectral diffusion.
  arXiv  Detail & Related papers  (2026-02-04T16:31:20Z)
• Quantum optical scattering by macroscopic lossy objects: A general approach [55.2480439325792]
  We develop a general approach to describe the scattering of quantum light by a lossy macroscopic object placed in vacuum.<n>We exploit the input-output relation to connect the output state of the field to the input one.<n>We analyze the impact of the classical transmission and absorption dyadics on the transitions from ingoing to outgoing s-polariton.
  arXiv  Detail & Related papers  (2024-11-27T17:44:29Z)
• Directional superradiance in a driven ultracold atomic gas in free-space [0.0]
  We study a dense ensemble illuminated by a strong coherent drive while interacting via dipole-dipole interactions. Although the steady-state features some similarities to the reported superradiant to normal non-induced transition, we observe significant qualitative and quantitative differences. We develop a simple theoretical model that explains the scaling properties by accounting for interaction-equilibrium inhomogeneous effects and spontaneous emission.
  arXiv  Detail & Related papers  (2024-03-22T18:14:44Z)
• Dynamics of inhomogeneous spin ensembles with all-to-all interactions: breaking permutational invariance [49.1574468325115]
  We investigate the consequences of introducing non-uniform initial conditions in the dynamics of spin ensembles characterized by all-to-all interactions. We find that the dynamics of the spin ensemble now spans a more expansive effective Hilbert space.
  arXiv  Detail & Related papers  (2023-09-19T16:44:14Z)
• Reaction-diffusive dynamics of number-conserving dissipative quantum state preparation [0.0]
  We show the emergence of a diffusive regime for the particle and hole density modes at intermediate length- and time-scales. We also identify processes that limit the diffusive behavior of this mode at the longest length- and time-scales. Strikingly, we find that these processes lead to a reaction-diffusion dynamics governed by the Fisher-Kolmogorov-Petrovsky-Piskunov equation.
  arXiv  Detail & Related papers  (2023-01-12T19:11:04Z)
• Connecting steady-states of driven-dissipative photonic lattices with spontaneous collective emission phenomena [91.3755431537592]
  We use intuition to predict the formation of non-trivial photonic steady-states in one and two dimensions. We show that subradiant emitter configurations are linked to the emergence of steady-state light-localization in the driven-dissipative setting. These results shed light on the recently reported optically-defined cavities in polaritonic lattices.
  arXiv  Detail & Related papers  (2021-12-27T23:58:42Z)
• A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity [0.0]
  This perspective provides a brief introduction into the theoretical complexity of polaritonic chemistry. ab initio methods are used to tackle this complexity. Various extensions towards a refined description of cavity-modified chemistry are introduced.
  arXiv  Detail & Related papers  (2021-08-27T12:48:57Z)
• Interplay between transport and quantum coherences in free fermionic systems [58.720142291102135]
  We study the quench dynamics in free fermionic systems. In particular, we identify a function, that we dub emphtransition map, which takes the value of the stationary current as input and gives the value of correlation as output.
  arXiv  Detail & Related papers  (2021-03-24T17:47:53Z)
• On Evolution of Coherent States as Quantum Counterpart of Classical Dynamics [0.0]
  Quantum dynamics of coherent states is studied within quantum field theory. We use two complementary methods: by organizing the evolution as a Taylor series in elapsed time and by perturbative expansion in coupling within the interaction-picture formalism.
  arXiv  Detail & Related papers  (2020-11-23T06:08:29Z)
• Analog cosmological reheating in an ultracold Bose gas [58.720142291102135]
  We quantum-simulate the reheating-like dynamics of a generic cosmological single-field model in an ultracold Bose gas. Expanding spacetime as well as the background oscillating inflaton field are mimicked in the non-relativistic limit. The proposed experiment has the potential of exploring the evolution up to late times even beyond the weak coupling regime.
  arXiv  Detail & Related papers  (2020-08-05T18:00:26Z)
• Theory of waveguide-QED with moving emitters [68.8204255655161]
  We study a system composed by a waveguide and a moving quantum emitter in the single excitation subspace. We first characterize single-photon scattering off a single moving quantum emitter, showing both nonreciprocal transmission and recoil-induced reduction of the quantum emitter motional energy.
  arXiv  Detail & Related papers  (2020-03-20T12:14:10Z)

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

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.