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  1. Spectral line shapes provide a window into the local environment coupled to a quantum transition in the condensed phase. In this paper, we build upon a stochastic model to account for non-stationary background processes produced by broad-band pulsed laser stimulation, as distinguished from those for stationary phonon bath. In particular, we consider the contribution of pair-fluctuations arising from the full bosonic many-body Hamiltonian within a mean-field approximation, treating the coupling to the system as a stochastic noise term. Using the Itô transformation, we consider two limiting cases for our model, which lead to a connection between the observed spectral fluctuations and the spectral density of the environment. In the first case, we consider a Brownian environment and show that this produces spectral dynamics that relax to form dressed excitonic states and recover an Anderson–Kubo-like form for the spectral correlations. In the second case, we assume that the spectrum is Anderson–Kubo like and invert to determine the corresponding background. Using the Jensen inequality, we obtain an upper limit for the spectral density for the background. The results presented here provide the technical tools for applying the stochastic model to a broad range of problems.
    Free, publicly-accessible full text available August 7, 2023
  2. Frenkel excitons are the primary photoexcitations in organic semiconductors and are ultimately responsible for the optical properties of such materials. They are also predicted to form bound exciton pairs, termed biexcitons, which are consequential intermediates in a wide range of photophysical processes. Generally, we think of bound states as arising from an attractive interaction. However, here, we report on our recent theoretical analysis, predicting the formation of stable biexciton states in a conjugated polymer material arising from both attractive and repulsive interactions. We show that in J-aggregate systems, 2J-biexcitons can arise from repulsive dipolar interactions with energies E 2 J > 2 E J , while in H-aggregates, 2H-biexciton states with energies E 2 H < 2 E H can arise corresponding to attractive dipole exciton/exciton interactions. These predictions are corroborated by using ultrafast double-quantum coherence spectroscopy on a [poly(2,5-bis(3-hexadecylthiophene-2-yl)thieno[3,2-b]thiophene)] material that exhibits both J- and H-like excitonic behavior.
    Free, publicly-accessible full text available May 14, 2023
  3. Free, publicly-accessible full text available March 31, 2023
  4. null (Ed.)
  5. Recent theories and experiments have explored the use of entangled photons as a spectroscopic probe of physical systems. We describe here a theoretical description for entropy production in the scattering of an entangled biphoton Fock state within an optical cavity. We develop this using perturbation theory by expanding the biphoton scattering matrix in terms of single-photon terms in which we introduce the photon-photon interaction via a complex coupling constant, ξ. We show that the von Neumann entropy provides a concise measure of this interaction. We then develop a microscopic model and show that in the limit of fast fluctuations, the entanglement entropy vanishes, whereas in the limit of slow fluctuations, the entanglement entropy depends on the magnitude of the fluctuations and reaches a maximum. Our result suggests that experiments measuring biphoton entanglement give microscopic information pertaining to exciton-exciton correlations.
  6. In order for a photovoltaic cell to function, charge carriers produced by photoexcitation must fully dissociate and overcome their mutual Coulomb attraction to form free polarons. This becomes problematic in organic systems in which the low dielectric constant of the material portends a long separation distance between independent polaron pairs. In this paper, we discuss our recent efforts to correlate the role of density of states, entropy, and configurational and energetic disorder to the open-circuit voltage, V OC , of model type-II organic polymer photovoltaics. By comparing the results of a fully interacting lattice model to those predicted by a Wigner–Weisskopf type model we find that energetic disorder does play a significant role in determining the V OC ; however, mobility perpendicular to the interface plays the deciding role in the eventual fate of a charge-separated pair.