Exciton recurrence motion in aggregate systems in the presence of quantized optical fields

Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan.
The Journal of Chemical Physics (Impact Factor: 2.95). 01/2007; 125(23):234707. DOI: 10.1063/1.2390695
Source: PubMed


The exciton dynamics of model aggregate systems, dimer, trimer, and pentamer, composed of two-state monomers is computationally investigated in the presence of three types of quantized optical fields, i.e., coherent, amplitude-squeezed, and phase-squeezed fields, in comparison with the case of classical laser fields. The constituent monomers are assumed to interact with each other by the dipole-dipole interaction, and the two-exciton model, which takes into account both the one- and two-exciton generations, is employed. As shown in previous studies, near-degenerate exciton states in the presence of a (near) resonant classical laser field create quantum superposition states and thus cause the spatial exciton recurrence motion after cutting the applied field. In contrast, continuously applied quantized optical fields turn out to induce similar exciton recurrence motions in the quiescent region between the collapse and revival behaviors of Rabi oscillation. The spatial features of exciton recurrence motions are shown to depend on the architecture of aggregates. It is also found that the coherent and amplitude-squeezed fields tend to induce longer-term exciton recurrence behavior than the phase-squeezed field. These features have a possibility for opening up a novel creation and control scheme of exciton recurrence motions in aggregate systems under the quantized optical fields.

Download full-text


Available from: Masayoshi Nakano, Dec 08, 2014
10 Reads
  • [Show abstract] [Hide abstract]
    ABSTRACT: Absorption properties of molecular trimers are studied within a model including a single monomer internal vibrational degree of freedom. Upon photoabsorption, three excited electronic states which are coupled excitonically are accessed. Band shapes resulting from different electronic coupling strengths and geometries are analyzed. It is shown that geometric information can be extracted from the band intensities. Taking data recorded for perylene bisimide aggregates as an example, the spectra for monomer, dimer, and trimer systems are compared.
    The Journal of Chemical Physics 05/2007; 126(16):164308. DOI:10.1063/1.2721540 · 2.95 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: We propose a novel dynamic exciton expression based on the quantum master equation approach using the ab initio molecular orbital (MO) singly excited configuration interaction (CI) method developed in our previous paper [M. Nakano, M. Takahata, S. Yamada, R. Kishi, T. Nitta, K. Yamaguchi, J. Chem. Phys. 120 (2004) 2359]. This expression is derived from the partition of polarization density in the configuration basis into the electron and hole contributions, and can describe both the coherent and incoherent dynamics of electron and hole density distributions, e.g., dynamic electric polarization, exciton recurrence and exciton migration.
    Chemical Physics Letters 07/2008; 460(1-3):370-374. DOI:10.1016/j.cplett.2008.05.100 · 1.90 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: The coherent exciton dynamics in molecular complexes composed of ring-shaped aggregates induced by linear- and circular-polarized laser fields has been investigated by using the quantum master equation (QME) approach. As shown in previous studies, near-degenerate states create the superposition states after irradiation of linear-polarized laser fields and thus cause the oscillatory exciton recurrence motion. In contrast, the rotatory exciton recurrence motion is found to be induced by circular-polarized laser field in a C3-symmetry complex composed of identical three ring-shaped aggregates. This exciton dynamics is predicted to originate in the superposition states between the two pairs of degenerate states, which are coherently excited by a circular-polarized laser field. The rotatory exciton recurrence motion induced by a two-mode laser field with mutually opposite circular polarizations also has been examined in the complex composed of two different-sized groups of ring-shaped aggregates. It turns out that the two-mode laser field induces mutually counter-rotatory exciton recurrence motions concurrently, which are generated separately on the two different groups of ring-shaped aggregates. These results suggest the possibility of controlling rotatory exciton recurrence motions by using the circular-polarized laser fields and ring-shaped aggregate complexes.
    The Journal of Physical Chemistry C 02/2009; 113(8):3332–3338. DOI:10.1021/jp8096555 · 4.77 Impact Factor
Show more