Browsing by Subject "Polarons"

Now showing 1 - 5 of 5

Open Access
Electronic structure of conducting organic polymers: insights from time-dependent density functional theory
(John Wiley & Sons Ltd., 2014) Salzner, U.
Conducting organic polymers (COPs) became an active field of research after it was discovered how thin films rather than insoluble infusible powders can be produced. The combination of the properties of plastics with those of semiconductors opened the research field of organic electronics. COPs share many electronic properties with inorganic semiconductors, but there are also major differences, e.g., the nature of the charge carriers and the amount of the exciton binding energy. Theoretical analysis has been used to interpret experimental observations early on. The polaron model that was developed from one-electron theories is still the most widely used concept. In the 1990s, time-dependent density functional theory (TDDFT) became available for routine calculations. Using TDDFT, electronic states of long oligomers can be calculated. Now UV spectra of neutral and oxidized or reduced species can be compared with in situ UV spectra recorded during doping. Likewise states of cations can be used to model photoelectron spectra. Analysis of states has resolved several puzzles which cannot be understood with the polaron model, e.g., the origin of the dual absorption band of green polymers and the origin of a 'vestigial neutral band' upon doping of long oligomers. DFT calculations also established that defect localization is not crucial for spectral changes observed during doping and that there are no bound bipolarons in COPs.
Open Access
Existence of a metallic phase in a 1D Holstein-Hubbard model at half filling
(Elsevier B.V., 2007) Krishna, P. M.; Chatterjee, A.
The one-dimensional half-filled Holstein-Hubbard model is studied using a series of canonical transformations including phonon coherence effect that partly depends on the electron density and is partly independent and also incorporating the on-site and the nearest-neighbour phonon correlations and the exact Bethe-ansatz solution of Lieb and Wu. It is shown that choosing a better variational phonon state makes the polarons more mobile and widens the intermediate metallic region at the charge-density-wave-spin-density-wave crossover recently predicted by Takada and Chatterjee. The presence of this metallic phase is indeed a favourable situation from the point of view of high temperature superconductivity.
Open Access
Hartree-Fock approximation of bipolaron state in quantum dots and wires
(Springer, 2010) Senger, R. T.; Kozal, B.; Chatterjee, A.; Erçelebi, A.
The bipolaronic ground state of two electrons in a spherical quantum dot or a quantum wire with parabolic boundaries is studied in the strong electron-phonon coupling regime. We introduce a variational wave function that can conveniently conform to represent alternative ground state configurations of the two electrons, namely, the bipolaronic bound state, the state of two individual polarons, and two nearby interacting polarons confined by the external potential. In the bipolaron state the electrons are found to be separated by a finite distance about a polaron size. We present the formation and stability criteria of bipolaronic phase in confined media. It is shown that the quantum dot confinement extends the domain of stability of the bipolaronic bound state of two electrons as compared to the bulk geometry, whereas the quantum wire geometry aggravates the formation of stable bipolarons.
Open Access
On the stability of Fröhlich bipolarons in spherical quantum dots
(Institute of Physics, 2002) Senger, R. T.; Erçelebi, A.
In the strong-electron-phonon-coupling regime, we retrieve the stability criterion for bipolaron formation in a spherical quantum dot. The model that we use consists of a pair of electrons immersed in a reservoir of bulk LO phonons and confined within an isotropic parabolic potential box. In this particular quasi-zero-dimensional geometry, where the electrons do not have any free spatial direction to expand indefinitely, a plausible approach would be to treat the electrons either to form a bipolaronic bound state or enter a state of two close, but individual polarons inside the same dot. The confined two-polaron model adopted here involves the polaron-polaron separation introduced as an adjustable parameter to be determined variationally. It is found that the fundamental effect of imposing such a variational flexibility is to modify the phase diagram to a considerable extent and to sustain the bipolaron phase in a broader domain of stability.
Open Access
Polaronic effects in a gaussian quantum dot
(Elsevier, 2008) Yanar, S.; Sevim, A.; Boyacioglu, B.; Saglam, M.; Mukhopadhyaya, S.; Chatterjee, A.
The problem of an electron interacting with longitudinal-optical (LO) phonons is investigated in an N-dimensional quantum dot with symmetric Gaussian confinement in all directions using the Rayleigh-Schrödinger perturbation theory, a variant of the canonical transformation method of Lee-Low-Pines, and the sophisticated apparatus of the Feynman-Haken path-integral technique for the entire range of the coupling parameters and the results for N = 2 and N = 3 are obtained as special cases. It is shown that the polaronic effects are quite significant for small dots with deep confining potential well and the parabolic potential is only a poor approximation of the Gaussian confinement. The Feynman-Haken path-integral technique in general gives a good upper bound to the ground state energy for all values of the system parameters and therefore is used as a benchmark for comparison between different methods. It is shown that the perturbation theory yields for the ground state polaron self-energy a simple closed-form analytic expression containing only Gamma functions and in the weak-coupling regime it provides the lowest energy because of an efficient partitioning of the Gaussian potential and the subsequent use of a mean-field kind of treatment. The polarization potential, the polaron radius and the number of virtual phonons in the polaron cloud are obtained using the Lee-Low-Pines-Huybrechts method and their variations with respect to different parameters of the system are discussed.