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In the s = 1/2 antiferromagnetic spin chain material TiPO4 the formation of aspin gap takes place in a two step process with two characteristictemperatures, T*=111 K and TSP=74 K. We observe an unusual lattice dynamicsover a large temperature regime as well as evidence for an orbital instabilitypreceding the spin-Peierls transition. We relate different intrachain exchangeinteractions of the high temperature compared to the spin-Peierls phase to amodification of the orbital ordering pattern. In particular, our observation ofa high energy excitation of mixed electronic and lattice origin suggests anexotic dimerization process different from other spin-Peierls materials.

Lattice and orbital fluctuations in TiPO4