RESUMO
Two-dimensional (2D) layered materials exhibit great potential for high-performance electronics, where knowledge of their thermal and phononic properties is critical toward understanding heat dissipation mechanisms, considered to be a major bottleneck for current generation nanoelectronic, optoelectronic, and quantum-scale devices. In this work, noncontact Raman spectroscopy was used to analyze thermal properties of suspended 2D WSe2 membranes to access the intrinsic properties. Here, the influence of electron-phonon interactions within the parent crystalline WSe2 membranes was deciphered through a comparative analysis of extrinsic substrate-supported WSe2, where heat dissipation mechanisms are intimately tied to the underlying substrate. Moreover, the excitonic states in WSe2 were analyzed by using temperature-dependent photoluminescence spectroscopy, where an enhancement in intensity of the localized excitons in suspended WSe2 was evident. Finally, phononic and electronic properties in suspended WSe2 were examined through nanoscale local strain engineering, where a uniaxial force was induced on the membrane using a Au-coated cantilever within an atomic force microscope. Through the fundamental analysis provided here with temperature and strain-dependent phononic and optoelectronic properties in suspended WSe2 nanosheets, the findings will inform the design of next-generation energy-efficient, high-performance devices based on WSe2 and other 2D materials, including for quantum applications.
RESUMO
Phonon dynamics is explored in mechanically exfoliated two-dimensional WSe2 using temperature-dependent and laser-power-dependent Raman and photoluminescence (PL) spectroscopy. From this analysis, phonon lifetime in the Raman active modes and phonon concentration, as correlated to the energy parameter E 0, were calculated as a function of the laser power, P, and substrate temperature, T. For monolayer WSe2, from the power dependence it was determined that the phonon lifetime for the in-plane vibrational mode was twice that of the out-of-plane vibrational mode for P in the range from 0.308 mW up to 3.35 mW. On the other hand, the corresponding relationship for the temperature analysis showed that the phonon lifetime for the in-plane vibrational mode lies within 1.42× to 1.90× that of the out-of-plane vibrational mode over T = 79 K up to 523 K. To provide energy from external stimuli, as T and P were increased, peak broadening in the PL spectra of the A-exciton was observed. From this, a phonon concentration was tabulated using the Urbach formulism, which increased with increasing T and P; consequently, the phonon lifetime was found to decrease. Although phonon lifetime decreased with increasing temperature for all thicknesses, the decay rate in the phonon lifetime in the monolayer (1L) material was found to be 2× lower compared to the bulk. We invoke a harmonic oscillator model to explain the damping mechanism in WSe2. From this it was determined that the damping coefficient increases with the number of layers. The work reported here sheds fundamental insights into the evolution of phonon dynamics in WSe2 and should help pave the way for designing high-performance electronic, optoelectronic and thermoelectric devices in the future.
