Resonance-type thickness dependence of optical second harmonic generation in thin-films of the topological insulator Bi2Se3

Abstract

Optical second harmonic generation (SHG) has been measured for the first time in reflection from the nanometer-thick films (6 to 40 nm) of the topological insulator Bi2Se3 using 1.51 eV (820 nm) Ti:Sapphire laser photons and revealed a strong dependence of the integral SHG intensity on the film thickness. The integral SHG intensity was determined by area integration of the SHG rotational anisotropy patterns measured for different input-output light polarization geometries. A ~100-fold enhancement of the integral SHG intensity with decreasing film thickness has been suggested to result from the DC-electric-field-induced SHG (EFISHG) effects. Two sources of dynamically created DC electric field were proposed: (i) the capacitor-type DC electric field that gradually increases with decreasing film thickness from 40 to 6 nm due to a dynamical imbalance of photoexcited long-lived carriers between the opposite-surface Dirac surface states and (ii) an DC electric field associated with a nonlinearly excited Dirac plasmon, which is responsible for the resonant enhancement of the integral SHG intensity for the 10 nm thick film with a Lorentz-shaped resonance of ~1.6 nm full width at half maximum. Additionally to the general SHG enhancement trends with decreasing film thickness, a relative decrease of the out-of-plane contribution with respect to the in-plane contribution was observed. Using a theoretical treatment of the measured SHG rotational anisotropy patterns, this effect has been suggested to result from the joint contributions of the linear and quadratic DC electric field effects to the EFISHG response.

References in corpus (9)

• Discovery (theoretical prediction and experimental observation) of a large-gap topological-insulator class with spin-polarized single-Dirac-cone on the surface
• Dielectric function, screening, and plasmons in 2D graphene
• Phase transition between the quantum spin Hall and insulator phases in 3D: emergence of a topological gapless phase
• Bulk Fermi surface coexistence with Dirac surface state in Bi${}_2$Se${}_3$: a comparison of photoemission and Shubnikov-de Haas measurements
• Ultrafast Optical Excitation of a Persistent Surface-State Population in the Topological Insulator Bi2Se3
• Surface State Transport and Ambipolar Electric Field Effect in Bi2Se3 Nanodevices
• Nonlinear optical probe of tunable surface electrons on a topological insulator
• Effect of carrier recombination on ultrafast carrier dynamics in thin films of the topological insulator Bi2Se3
• Thickness tunable quantum interference between surface phonon and Dirac plasmon states in thin-films of the topological insulator Bi2Se3

Cited by in corpus (2)

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