We present a multi-frequency Electron Spin Resonance (ESR) study in the range of 4 GHz to 420 GHz of the quasi-one-dimensional, non-dimerized, quarter-filled Mott insulators, delta-(EDT-TTF-CONMe_2)_2X (X=AsF_6, Br). In the high temperature orthorhom
bic phase above T~190 K, the magnitude and the temperature dependence of the high temperature spin susceptibility are described by a S = 1/2 Heisenberg antiferromagnetic chain with J_AsF6=298 K and J_Br=474 K coupling constants for X=AsF_6 and Br respectively. We estimate from the temperature dependence of the line width an exchange anisotropy, J/J of ~2 * 10^{-3}. The frequency dependence of the line width and the g-shift have an unusual quadratic dependence in all crystallographic orientations that we attribute to an antisymmetric exchange (Dzyaloshinskii--Moriya) interaction.
We report the development of the frequency-modulation (FM) method for measuring electron spin resonance (ESR) absorption in the 210-420 GHz frequency range. We demonstrate that using a high-frequency ESR spectrometer without resonating microwave comp
onents enables us to overcome technical difficulties associated with the FM method due to nonlinear microwave-elements, without sacrificing spectrometer performance. FM was achieved by modulating the reference oscillator of a 13 GHz Phase Locked Dielectric Resonator Oscillator, and amplifying and frequency-multiplying the resulting millimeter-wave radiation up to 210, 315 and 420 GHz. ESR spectra were obtained in reflection mode by a lock-in detection at the fundamental modulation frequency, and also at the second and third harmonic. Sensitivity of the setup was verified by conduction electron spin resonance measurement in KC$_{60}$.
