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Second harmonic spectroscopy to optically detect valley polarization in 2D materials

Abstract

Valley polarization (VP), an induced imbalance in the populations of a multi-valley electronic system, allows emission of second harmonic (SH) light even in centrosymmetric crystals such as graphene. Whereas in systems such as MoS2\mathrm{_2} or BN this adds to their intrinsic quadratic response, SH generation in a multi-valley inversion-symmetric crystal can provide a direct measure of valley polarization. By computing the nonlinear response and characterizing theoretically the respective SH as a function of polarization, temperature, electron density, and degree of VP, we demonstrate the possibility of disentangling and individually quantifying the intrinsic and valley contributions to the SH. A specific experimental setup is proposed to obtain direct quantitative information about the degree of VP and allow its remote mapping. This approach could prove useful for direct, contactless, real-space monitoring of valley injection and other applications of valley transport and valleytronics.Comment: Updating with published version, including typesetting corrections to eqs 3 and 4; 7 pages, 5 figure

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