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Upon laser irradiation, 2D materials experience a cascading energy transfer from electrons to optical phonons (OPs) and then to acoustic phonons (APs), resulting in a significant thermal non-equilibrium among energy carriers. This non-equilibrium presents challenges for Raman-based thermal characterization, as Raman scattering measures only OP temperature rise, while APs are the primary energy carriers. Despite recent efforts to address this issue, OP–AP thermal non-equilibrium in supported 2D materials remains poorly resolved. Here, we develop a method to distinguish the OP and AP temperature rises based on their different temporal thermal responses under laser irradiation: the OP–AP temperature difference responds almost immediately (∼a few to tens of ps), while the AP temperature rise takes longer to establish (∼tens of ns). Using energy transport-state resolved Raman, we probe the transient thermal response of Si-supported nm-thick MoS2from 20 to 100 ns. We find that the OP–AP temperature difference exceeds 120% of the AP temperature rise under ∼0.439 µm radius laser heating. The intrinsic interfacial thermal conductance of the samples, based on the true AP temperature rise, varies from 0.199 to 1.46 MW·m−2·K−1, showing an increasing trend with sample thickness.
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Distinguishing Optical and Acoustic Phonon Temperatures and Their Energy Coupling Factor under Photon Excitation in nm 2D Materials
Abstract Under photon excitation, 2D materials experience cascading energy transfer from electrons to optical phonons (OPs) and acoustic phonons (APs). Despite few modeling works, it remains a long‐history open problem to distinguish the OP and AP temperatures, not to mention characterizing their energy coupling factor (G). Here, the temperatures of longitudinal/transverse optical (LO/TO) phonons, flexural optical (ZO) phonons, and APs are distinguished by constructing steady and nanosecond (ns) interphonon branch energy transport states and simultaneously probing them using nanosecond energy transport state‐resolved Raman spectroscopy. ΔTOP −APis measured to take more than 30% of the Raman‐probed temperature rise. A breakthrough is made on measuring the intrinsic in‐plane thermal conductivity of suspended nm MoS2and MoSe2by completely excluding the interphonon cascading energy transfer effect, rewriting the Raman‐based thermal conductivity measurement of 2D materials.GOP↔APfor MoS2, MoSe2, and graphene paper (GP) are characterized. For MoS2and MoSe2,GOP↔APis in the order of 1015and 1014W m−3K−1andGZO↔APis much smaller thanGLO/TO↔AP. Under ns laser excitation,GOP↔APis significantly increased, probably due to the reduced phonon scattering time by the significantly increased hot carrier population. For GP,GLO/TO↔APis 0.549 × 1016W m−3K−1, agreeing well with the value of 0.41 × 1016W m−3K−1by first‐principles modeling.
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- Award ID(s):
- 1930866
- PAR ID:
- 10457441
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Science
- Volume:
- 7
- Issue:
- 13
- ISSN:
- 2198-3844
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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