Optically Induced Symmetry Breaking Due to Nonequilibrium Steady State Formation in Charge Density Wave Material 1T-TiSe2.

The strongly correlated charge density wave (CDW) phase of 1T-TiSe2 is of interest to verify the claims of a chiral order parameter. Characterization of the symmetries of 1T-TiSe2 is critical to understand the origin of its intriguing properties. Here we use very low-power, continuous wave laser excitation to probe the symmetries of 1T-TiSe2 by using the circular photogalvanic effect. We observe that the ground state of the CDW phase (D3d) is achiral. However, laser excitation above a threshold intensity transforms 1T-TiSe2 into a nonequilibrium chiral phase (C3), which changes the electronic correlations in the material. The inherent sensitivity of the photogalvanic technique to structural symmetries provides evidence of the different optically driven phase of 1T-TiSe2, which allows us to assign symmetry groups to these states. Our work demonstrates that optically induced phase change can occur at extremely low optical intensities in strongly correlated materials, providing a pathway to engineer new phases using light.

Differential Wavevector Distribution of Surface-Enhanced Raman Scattering and Fluorescence in a Film-Coupled Plasmonic Nanowire Cavity.

We report on the experimental observation of differential wavevector distribution of surface-enhanced Raman scattering (SERS) and fluorescence from dye molecules confined to a gap between plasmonic silver nanowire and a thin, gold mirror. The fluorescence was mainly confined to higher values of in-plane wavevectors, whereas SERS signal was uniformly distributed along all the wavevectors. The optical energy-momentum spectra from the distal end of the nanowire revealed strong polarization dependence of this differentiation. All these observations were corroborated by full-wave three-dimensional numerical simulations, which further revealed an interesting connection between out-coupled wavevectors and parameters such as hybridized modes in the gap-plasmon cavity, and orientation and location of molecular dipoles in the geometry. Our results reveal a new prospect of discriminating electronic and vibrational transitions in resonant dye molecules using a subwavelength gap plasmonic cavity in the continuous-wave excitation limit, and can be further harnessed to engineer molecular radiative relaxation processes in momentum space.

Exchange coupling-mediated broken symmetries in Ta2NiSe5 revealed from quadrupolar circular photogalvanic effect.

In low-electron density materials, interactions can lead to highly correlated quantum states of matter. Ta2NiSe5, an excitonic insulator (EI) candidate, exists in a novel broken-symmetry phase below 327 K, characterized by robust exchange interaction and electron-lattice coupling. We study this phase of Ta2NiSe5 using the quadrupole circular photogalvanic effect (QCPGE). Light-matter interaction in Ta2NiSe5 mediated by electric quadrupole/magnetic dipole coupling produces helicity-dependent DC response even with centrosymmetry, making it particularly sensitive to certain other broken symmetries. We show that the exchange interaction in Ta2NiSe5 can lead to a triclinic structure with a broken C2 symmetry. Our results provide an incisive probe of the symmetries of the low-temperature phase of Ta2NiSe5 and add new symmetry constraints to the identification of a strongly correlated EI phase. The high sensitivity of QCPGE to subtle symmetry breaking in centrosymmetric systems will enable its use in studying other complex crystalline systems.

V-shaped active plasmonic meta-polymers.

We report the design and fabrication of V-shaped plasmonic meta-polymers on a glass substrate or silicon wafer using a surface functionalization approach. The efficacy of the assembly method is examined by analyzing the surface enhanced Raman scattering by an individual V-shaped antenna experimentally and using computational simulations to determine the polarization dependence of local electromagnetic field enhancement.