Abstract Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. Here we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe3(X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highestAgmode in CrGeTe3splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 200K. These modes correspond to localized oscillations of Ge2Te6clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe3, demonstrating the generalizability of this phenomenon. Our findings demonstrate that Raman scattering effectively probes high-frequency nonlinear phonon modes, offering insight into the generation of long-lived, tunable phonon frequency combs with potential applications in ultrafast material control and phonon-based technologies.
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Influence of Mode Structure on the Generation of Phononic Frequency Combs
The mechanical analog of optical frequency combs, phononic frequency combs, has recently been demonstrated in mechanical resonators and has been attributed to coupling between multiple phonon modes. This paper investigates the influence of mode structure on comb generation using a model of two nonlinearly coupled phonon modes. The model predicts that there is only one region within the amplitude-frequency space where combs exist, and this region is a subset of the Arnold tongue that describes a 2:1 autoparametric resonance between the two modes. In addition, the location and shape of the comb region are analytically defined by the resonance frequencies, quality factors, mode coupling strength, and detuning of the driving force frequency from the mechanical resonances, providing clear conditions for comb generation. These results enable comb structure engineering for applications in areas as broad as sensing, communications, and quantum information science.
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- Award ID(s):
- 1807272
- PAR ID:
- 10147624
- Date Published:
- Journal Name:
- ArXivorg
- ISSN:
- 2331-8422
- Page Range / eLocation ID:
- arXiv:2003.10202v1
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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