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Substitution effects of Os for Ru in {\alpha}-RuCl3 are investigated in awide composition range of 0 =< x =< 0.67 in Ru1-xOsxCl3 by X-ray and electrondiffraction, magnetic susceptibility, heat capacity, and Raman spectroscopymeasurements. Apart from the Kitaev physics with antiferromagnetic interactionsincreasing with x, a rich phase diagram is obtained, which includes anantiferromagnetic long-range order below 12 K for x =< 0.15, a dome-shapedspin-singlet dimer phase below 130 K for 0.15 =< x =< 0.40, and a magneticshort-range order for x > 0.40. A dimerization as similarly observed in{\alpha}-RuCl3 under high pressure occurs in the spin-singlet phase. It issuggested that Ru-Os pairs in the solid solutions tend to form dimers withshort bonds and trigger the first-order transition in the presence ofpseudo-threefold rotational symmetry for dimerization around a substituted Osatom only at low substitutions. This is a rare example of molecular orbitalcrystallization induced by elemental substitution in a highly disorderedsystem. The short-range order at high substitutions may be related to arandom-singlet state stabilized by bond disorder in the honeycomb net.

Dimer Crystallization Induced by Elemental Substitution in the Honeycomb Lattice of Ru1-xOsxCl3