Accelerated polaron formation in perovskite quantum dots monitored via picosecond infrared spectroscopy
M. Nuber, Q. Y. Tan, D. Sandner, J. Yin, R. Kienberger, C. Soci, H. Iglev
Journal of Materials Chemistry C 11 (10), 3581-3587 (2023).
The formation and nature of polarons in perovskite quantum dots (QDs) are still unclear. Due to the very limited crystal size and quantum confinement, influences on the polaron stabilization dynamics could be expected. Here, we investigate the coupling of photoexcited charges to vibrational modes in mixed cation lead halide Cs(0.2)FA(0.8)PbBr(3) QDs via picosecond mid-infrared spectroscopy in comparison to the bulk film. We find additional processes occurring in an infrared activated vibrational (IRAV) mode compared to the ground-state bleaching and screened carrier background signal. Using that mode as a proxy for the charge-molecular bond coupling, we interpret additional time constant as a polaron stabilization time. With the confinement effects present in the QDs, this time shortens from tens of picoseconds in the bulk to only a few picoseconds.
Accelerated polaron formation in perovskite quantum dots monitored via picosecond infrared spectroscopy
M. Nuber, Q. Y. Tan, D. Sandner, J. Yin, R. Kienberger, C. Soci, H. Iglev
Journal of Materials Chemistry C 7 (2023).
The formation and nature of polarons in perovskite quantum dots (QDs) are still unclear. Due to the very limited crystal size and quantum confinement, influences on the polaron stabilization dynamics could be expected. Here, we investigate the coupling of photoexcited charges to vibrational modes in mixed cation lead halide Cs(0.2)FA(0.8)PbBr(3) QDs via picosecond mid-infrared spectroscopy in comparison to the bulk film. We find additional processes occurring in an infrared activated vibrational (IRAV) mode compared to the ground-state bleaching and screened carrier background signal. Using that mode as a proxy for the charge-molecular bond coupling, we interpret additional time constant as a polaron stabilization time. With the confinement effects present in the QDs, this time shortens from tens of picoseconds in the bulk to only a few picoseconds.
Ultrafast hot-carrier relaxation in silicon monitored by phase-resolved transient absorption spectroscopy
M. Worle, A. W. Holleitner, R. Kienberger, H. Iglev
Physical Review B 104 (4), L041201 (2021).
The relaxation dynamics of hot carriers in silicon (100) is studied via a holistic approach based on phase-resolved transient absorption spectroscopy with few-cycle optical pulses. After excitation by a sub-5-fs light pulse, strong electron-electron coupling leads to an ultrafast single electron momentum relaxation time of 10 fs. The thermalization of the hot carriers is visible in the temporal evolution of the effective mass and the collision time as extracted from the Drude model. The optical effective mass decreases from 0.3m(e) to about 0.125m(e) with a time constants of 58 fs, while the collision time increases from 3 fs for the shortest timescales with a saturation at approximately 18 fs with a time constant of 150 fs. The observation shows that both Drude parameters exhibit different dependences on the carrier temperature. The presented information on the electron mass dynamics as well as the momentum-, and electron-phonon scattering times with unprecedented time resolution is important for all hot-carrier optoelectronic devices.
Toward femtosecond electronics up to 10 THz
N. Fernandez, P. Zimmermann, P. Zechmann, M. Worle, R. Kienberger, A. W. Holleitner
Conference on Ultrafast Phenomena and Nanophotonics XXIII 10916, (2019).
We numerically compute the effective diffraction index and attenuation of coplanar stripline circuits with microscale lateral dimensions on various substrates including sapphire, GaN, silica glass, and diamond grown by chemical vapor deposition. We show how to include dielectric, radiative and ohmic losses to describe the pulse propagation in the striplines to allow femtosecond on-chip electronics with frequency components up to 10 THz.