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The physical properties of La$_4$Ni$_3$O$_{10}$ with a 2D-likeRuddlesden-Popper-type crystal structure are extraordinarily dependent ontemperature and chemical substitution. By introducing Al$^{3+}$ atoms ($x$)randomly at the Ni-sites, the average oxidation state for the twonon-equivalent Ni-cations is tuned and adopt values below the average of +2.67in La$_4$Ni$_3$O$_{10}$. La$_4$Ni$_{3-x}$Al$_x$O$_{10}$ is a solid solution for$x=0.00$ to 1.00, and are prepared by the citric acid method. The samples adopta slightly distorted monoclinic structure (P21/a), evidenced by peak broadeningof the (117) reflection. We report on a remarkable effect on the electronicproperties induced by tiny amounts of homogeneously distributed Al-cations,with clear correspondence between resistivity, magnetization, diffraction, andDFT data. DFT shows that electronically there is no significant differencebetween the non-equivalent Ni atoms and no tendency towards anyNi$^{3+}$/Ni$^{2+}$ charge ordering. The electron doping via Al-substitutionhas a profound effect on electric and magnetic properties. The resistivitychanges from metallic to semiconducting with increasing band-gap at higherAl-levels, consistent with results from DFT. The metal-to-metal transitionreported for La$_4$Ni$_3$O$_{10}$, which is often interpreted as a chargedensity wave, is maintained until $x = 0.15$ Al-level. However, the temperaturecharacteristics of the resistivity change already at very low Al-levels (below0.03). A coupling of the metal-to-metal transition to the lattice is evidencedby an anomaly in the unit cell dimensions. No long-range magnetic order isdetected by powder neutron diffraction. The introduction of the non-magneticAl$^{3+}$ changes the Ni$^{3+}$/Ni$^{2+}$ ratio and is likely to blockdouble-exchange pathways by means of -Ni-O-Al-O-Ni- fragments into the networkof corner shared octahedra with the emergence of possible short-range order inferromagnetic like islands.

Electron doping of the layered nickelate La$_4$Ni$_3$O$_{10}$ by aluminum substitution: A combined experimental and DFT study