Ab initio molecular dynamics, supported by inelastic neutron scattering and nuclear resonant inelastic x-ray scattering, showed an anomalous thermal softening of the M − 5 phonon mode in B2-ordered FeTi that could not be explained by phonon-phonon interactions or electron-phonon interactions calculated at low temperatures. A computational investigation showed that the Fermi surface undergoes a novel thermally driven electronic topological transition, in which new features of the Fermi surface arise at elevated temperatures. The thermally induced electronic topological transition causes an increased electronic screening for the atom displacements in the M − 5 phonon mode and an adiabatic electronphonon interaction with an unusual temperature dependence. DOI: 10.1103/PhysRevLett.117.076402 An electronic topological transition (ETT), first identified by Lifshitz [1], occurs when changes to a metal cause new features to appear in the topology of the Fermi surface [2]. Structural, mechanical, and electronic properties are usually altered by an ETT, which can be induced by alloying [3][4][5] or pressure [6][7][8]. Recently a novel temperature-induced ETT has been reported to alter magnetoresistivity [9]. In this Letter, we show through first-principles calculations and ancillary experiments how a thermally driven ETT drives anomalous changes in phonon dynamics.FeTi is a thermodynamically stable [10-12] nonmagnetic [13] intermetallic compound with a bcc-based B2 structure and a melting point of approximately 1600 K. FeTi is of interest for its hydrogen absorption capabilities [14][15][16] and for its mechanical properties [17,18]. It has been the subject of a large number of experimental and theoretical studies including inelastic neutron scattering [19,20] Forces and atomic configurations in the AIMD simulations were used to compute phonon energies at different temperatures with the temperature-dependent effective potential (TDEP) method [47,48], in which a model HamiltonianĤis used to sample the potential energy surface at the most probable atom positions, where p i and u i are the momentum and displacement of atom i, respectively, andΦ ij is a second-order force constant matrix. The force constants from Eq. (1) were used to obtain phonon dispersions and phonon DOS curves at temperatures from 300 to 1500 K (Fig. 1). Thermal expansion causes phonons to soften with temperature, and this was accounted for by the quasiharmonic calculations presented in the Supplemental Material [33]. The AIMD calculations were performed without thermal expansion, so Fig. 1 shows the thermal effects from pure anharmonicity and from the adiabatic EPI. These are significantly larger than the thermal softenings from quasiharmonicity reported in the Supplemental Material [33]. The nonadiabatic electron-phonon interaction (EPI) is well known from conventional superconductivity, where electrons are paired by phonons with wave vectors that span the Fermi surface [49,50]. With increasing temperature the PRL 117, 076402 (2016) P H Y S I C A L