Nonlinear THz Control of the Lead Halide Perovskite Lattice

Frenzel, Maximilian; Cherasse, Marie; Urban, Joanna; Wang, Feifan; Xiang, Bo; Nest, Leona; Huber, L.; Perfetti, L.; Wolf, Martin; Kampfrath, Tobias; Zhu, Xia; F., Maehrlein, Sebatian

doi:10.48550/arxiv.2301.03508

Cited by 1 publication

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“…Figure 2B shows the TKE data recorded at several temperatures for both 2DHPs. To minimize the potential misinterpretation of Kerr effect signals due to the temporal walk-off between the pump and probe pulses within the anisotropic media (38,39), we selected samples with the same thickness (i.e., ~100 μm). For the n = 2 sample at room temperature (green curve), only nonoscillatory signals are observed after the initial electronic response induced by the THz pulse.…”

Section: Resultsmentioning

confidence: 99%

“…Second, the initial response shows a bipolar character (40,41), signaled by the two lobes with opposite signs that do not follow the incident THz waveform. Although differences in the lineshape of the TKE signals may be explained by the nonlinear dispersion effects (31,38,39), a notable difference in the n = 1 system lies in the immediate appearance of a long-lived sinusoidal modulation following the initial electronic response in the n = 1 system. The oscillation frequency of 1.8 THz (see Fig.…”

Section: Resultsmentioning

confidence: 99%

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Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite

Zhang

Liu

et al. 2023

Sci. Adv.

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Layered hybrid perovskites exhibit emergent physical properties and exceptional functional performances, but the coexistence of lattice order and structural disorder severely hinders our understanding of these materials. One unsolved problem regards how the lattice dynamics are affected by the dimensional engineering of the inorganic frameworks and their interaction with the molecular moieties. Here, we address this question by using a combination of spontaneous Raman scattering, terahertz spectroscopy, and molecular dynamics simulations. This approach reveals the structural dynamics in and out of equilibrium and provides unexpected observables that differentiate single- and double-layered perovskites. While no distinct vibrational coherence is observed in double-layered perovskites, an off-resonant terahertz pulse can drive a long-lived coherent phonon mode in the single-layered system. This difference highlights the dramatic change in the lattice environment as the dimension is reduced, and the findings pave the way for ultrafast structural engineering and high-speed optical modulators based on layered perovskites.

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Section: Resultsmentioning

confidence: 99%