Charge transfer salts of Tetracyanoquinodimethane (TCNQ) were\ud synthesised and their electrical and magnetic properties were\ud investigated. These salts show unusual electrical and magnetic\ud behaviour in contrast to conventional organic compounds. These\ud salts have crystal structures which in general consist of TCNQ\ud radical ions stacked in chains, isolated from each other by the\ud diamagnetic cations. They are thus regarded as "one-dimensional"\ud electrical and magnetic systems. The ESR spectra of these salts are\ud attributed to triplet excitons showing that the spin-spin and electronelectron\ud correlation effects are important. In the ESR spectra\ud (Chapter III) of some TCNQ salts dipolar splitting is observed\ud confirming the spin-spin interaction. These triplet excitons are\ud regarded as bound electron-hole pairs. The experimentally determined\ud dipolar splitting tensors are presented in Chapter III and the intensity\ud data in Chapter IV. A large number of fine structure lines are\ud observed in the ESR spectra of Pyridinium-TCNQ and 4-Aminopyridinium-TCNQ\ud apart from regular triplet exciton lines (Chapter III). These lines\ud are attributed to the trapping of excitons on an extended formula\ud finit (TCNQ2 )n. In Chapter IV the temperature dependent magnetic\ud susceptibilities are discussed in terms of Heisenberg antiferromagnetism\ud and Pauli paramagnetism. In Chapter V temperature\ud dependent behaviour of electrical conductivity is discussed in terms\ud of an exciton band model, the lattice structure of the salts and\ud one-dimensional lattice consisting of defects giving rise to high and\ud low conducting segments. Low temperature electrical and magnetic\ud phases are discussed (Chapters IV and VII) in terms of a band and\ud hopping mechanisms.In Chapter VI self consistent field calculations are made with\ud reference to the tight binding one electron band theory using\ud simplified Roothaan equations considering CNDO approximations.\ud Theoretical results are related to experimental band gaps, spinspin\ud interactions and charge alteration
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