Nonlinear Tunable Vibrational Response in Hexagonal Boron Nitride

TL;DR

This paper demonstrates a large, tunable nonlinear vibrational response in monolayer hexagonal boron nitride, enabled by anharmonic atomic vibrations, with potential applications in mid-infrared optoelectronics and sensing.

Contribution

It provides first-principles predictions of strong nonlinear effects and electrical tunability of vibrational modes in monolayer hBN, revealing new opportunities for mid-infrared photonics.

Findings

Large nonlinear response in monolayer hBN in mid-infrared region.

Predicted threshold field of ~40 MV/m for nonlinear effects.

Potential for electrical tuning of vibrational modes.

Abstract

Nonlinear light-matter interactions in structured materials are the source of exciting properties and enable vanguard applications in photonics. However, the magnitude of nonlinear effects is generally small, thus requiring high optical intensities for their manifestation at the nanoscale. Here, we reveal a large nonlinear response of monolayer hexagonal boron nitride (hBN) in the mid-infrared phonon-polariton region, triggered by the strongly anharmonic potential associated with atomic vibrations in this material. We present robust first-principles theory predicting a threshold light field $\sim40\,$MV/m to produce order-unity effects in Kerr nonlinearities and harmonic generation, which are made possible by a combination of the long lifetimes exhibited by optical phonons and the strongly asymmetric landscape of the configuration energy in hBN. We further foresee polariton blockade at the few-quanta level in nanometer-sized structures. In addition, by mixing static and optical fields, the strong nonlinear response of monolayer hBN gives rise to substantial frequency shifts of optical phonon modes, exceeding their spectral width for in-plane DC fields that are attainable using lateral gating technology. We therefore predict a practical scheme for electrical tunability of the vibrational modes with potential interest in mid-infrared optoelectronics. The strong nonlinear response, low damping, and robustness of hBN polaritons set the stage for the development of applications in light modulation, sensing, and metrology, while triggering the search for intense vibrational nonlinear response in other ionic materials.