Nonthermal melting and density wave instability coupled to the lattice in La${}_4$Ni${}_3$O${}_{10}$

Abstract

The recent discovery of high-temperature superconductivity in pressurized nickelates has renewed interest in the broken-symmetry states of their ambient-pressure parent phases, where a density-wave (DW) order emerges and competes with superconductivity, but its microscopic origin remains unresolved. Using ultrafast optical spectroscopy, we track quasiparticle relaxation dynamics across the DW transition at $T_{\mathrm{DW}}\approx$ 136 K in trilayer nickelate {\LNO} single crystals, revealing the opening of an energy gap of $\sim$52 meV. Multiple coherent phonons, including $A_g$ modes near 3.88, 5.28, and 2.09 THz, display pronounced mode-selective anomalies across the transition, indicating that the DW is strongly coupled to lattice degrees of freedom and suggesting an important role of electron-phonon coupling. At higher excitation densities, the DW is nonthermally suppressed, producing a temperature-fluence phase diagram that parallels pressure-tuned behavior. These results establish the DW in {\LNO} as a lattice-entangled instability involving multiple phonon modes, and highlight ultrafast optical excitation as a nonequilibrium tuning parameter for suppressing density-wave order in nickelates.

6 pages, 4 figures