Here,we introduce the first experimental proof of coherent oscillation and coupling of photoswitchable molecules embedded randomly in a polymeric matrix and acting cooperatively upon illumination with UV light.In part...Here,we introduce the first experimental proof of coherent oscillation and coupling of photoswitchable molecules embedded randomly in a polymeric matrix and acting cooperatively upon illumination with UV light.In particular,we demonstrate the specular reflection and Brewster phenomenon alteration of photochromic molecular dipole antennas.We successfully demonstrate the concept of Brewster wavelength,which is based on the dipolar interaction between radiating dipoles and the surrounding matrix possessing a net dipole moment,as a key tool for highly localized sensing of matrix polarity.We also introduce the concept of‘tailored molecular photonic coupling’while highlighting the role of interferences for the design of optically active media by adjusting the photonic response of the medium with the real and imaginary refractive index of photoswitchable molecules in the‘ON’state.Our results enhance our fundamental understanding of coherent dipole radiation and open a new vein of research based on glassy disordered dipolar composites that act as macroscopic antenna with cooperative action;furthermore,these results have important implications for new design rules of tailored photonics.展开更多
Broadband(1.6–18 THz) terahertz time-domain spectroscopy(THz-TDS) and time-resolved terahertz spectroscopy(TRTS) were performed on a 54 μm thick chalcogenide glass(As_(30)Se_(30)Te_(40)) sample with a two-color lase...Broadband(1.6–18 THz) terahertz time-domain spectroscopy(THz-TDS) and time-resolved terahertz spectroscopy(TRTS) were performed on a 54 μm thick chalcogenide glass(As_(30)Se_(30)Te_(40)) sample with a two-color laser-induced air plasma THz system in transmission and reflection modes, respectively. Two absorption bands at 2–3 and 5–8 THz were observed. TRTS reveals an ultrafast relaxation process of the photoinduced carrier response, well described by a rate equation model with a finite concentration of mid-bandgap trap states for self-trapped excitons.The photoinduced conductivity can be well described by the Drude–Smith conductivity model with a carrier scattering time of 12–17 fs, and we observe significant carrier localization effects. A fast refractive index change was observed 100 fs before the conductivity reached its maximum, with 2 orders of magnitude larger amplitude than expected for the optically induced THz Kerr effect, indicating that free carriers are responsible for the transient index change.展开更多
基金We gratefully acknowledge financial support from the German Research Foundation(DFG)through SFB677(C09)and partial financial support from SFB677(C01)as well as the German Academic Exchange Service(DAAD)ME thanks the Initiative and Networking Fund of the Helmholtz Association(Grant no.VH-NG-523)for providing the financial support to start his research group.
文摘Here,we introduce the first experimental proof of coherent oscillation and coupling of photoswitchable molecules embedded randomly in a polymeric matrix and acting cooperatively upon illumination with UV light.In particular,we demonstrate the specular reflection and Brewster phenomenon alteration of photochromic molecular dipole antennas.We successfully demonstrate the concept of Brewster wavelength,which is based on the dipolar interaction between radiating dipoles and the surrounding matrix possessing a net dipole moment,as a key tool for highly localized sensing of matrix polarity.We also introduce the concept of‘tailored molecular photonic coupling’while highlighting the role of interferences for the design of optically active media by adjusting the photonic response of the medium with the real and imaginary refractive index of photoswitchable molecules in the‘ON’state.Our results enhance our fundamental understanding of coherent dipole radiation and open a new vein of research based on glassy disordered dipolar composites that act as macroscopic antenna with cooperative action;furthermore,these results have important implications for new design rules of tailored photonics.
基金financial support from the Danish Research Council for Independent Research (FNU Project THz-BREW)
文摘Broadband(1.6–18 THz) terahertz time-domain spectroscopy(THz-TDS) and time-resolved terahertz spectroscopy(TRTS) were performed on a 54 μm thick chalcogenide glass(As_(30)Se_(30)Te_(40)) sample with a two-color laser-induced air plasma THz system in transmission and reflection modes, respectively. Two absorption bands at 2–3 and 5–8 THz were observed. TRTS reveals an ultrafast relaxation process of the photoinduced carrier response, well described by a rate equation model with a finite concentration of mid-bandgap trap states for self-trapped excitons.The photoinduced conductivity can be well described by the Drude–Smith conductivity model with a carrier scattering time of 12–17 fs, and we observe significant carrier localization effects. A fast refractive index change was observed 100 fs before the conductivity reached its maximum, with 2 orders of magnitude larger amplitude than expected for the optically induced THz Kerr effect, indicating that free carriers are responsible for the transient index change.
