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Magneto-dielectric spectra of La0.95Ca0.05CoO3 covering the crossover of spinstates reveals strong coupling of its spin and dipolar degrees of freedom.Signature of spin-state transition at 30K clearly manifests in magnetization,supported by Co L_3,2-edge XAS data on the doped-specimen as consistent withits suppressed T_SST vs. ~150K for pure LaCoO3. Dispersive activation-step{\Delta}{\epsilon}'(T_{\omega})~O(10^2) and relaxation-peak{\epsilon}"(T_{\omega}) reflect the allied influence of coexistent spin-stateson the dielectric character. Dipolar relaxation in the LS regime below T_SST ispartly segmental (VFT kinetics) featuring magnetic-field tunability, whereas inthe LS/IS-spin disordered state above 30K, it is uncorrelated (Arrhenickinetics) and almost impervious to the H-field. Kinetics-switchover defines thedipolar-glass transition temperature Tg(H), below which themagneto-thermally-activated cooperative relaxations freeze-out by the VFTtemperature T_0(H). Applied H-field facilitates thermally-activated SST andaccelerates the dipolar relaxations; a critical 5T field collapsing the entirekinetics into a single Arrhenic behavior. Magneto-electricity (ME) spanningsizable thermo-spectral range registers diverse signatures here in the kinetic,spectral, and field behaviors, in contrast to the static/perturbative MEobserved close to the spin-ordering in typical multiferroics. Intrinsicmagneto-dielectricity (50%) along with vanishing magneto-loss is obtained at(27K/50kHz)_9T. Sub-linear deviant field-hysteretic split seen in{\epsilon}'(H)|_>4T suggests the emergence of robust dipoles organized intonano-clusters, realized by the internally-generated high magneto-electricfield. An elaborate {\omega}-T multi-dispersions diagram maps the rich varietyof phase/response patterns, revealing the highly-interacting magnetic andelectric moments in the system.

Magneto-thermally Activated Spin-state Transition in La0.95Ca0.05CoO3: Magnetically-tunable Dipolar Glass and Giant Magneto-electricity