Lattice Dynamics and Contraction of Energy Bandgap in Photoexcited Semiconducting BN Nanotubes.

Lattice Dynamics and Contraction of Energy Bandgap in Photoexcited Semiconducting BN Nanotubes.

Li, Zhongwen;Xiao, Rui-Juan;Xu, Peng;Zhu, Chunhui;Sun, Shuaishuai;Zheng, Dingguo;Wang, Hong;Zhang, Ming;Tian, Huanfang;Yang, Huai-Xin;Li, Jian-Qi;
acs nano 2019
240
li2019latticeacs

Abstract

Structural dynamics and changes in electronic structures driven by photoexcited carriers are critical issues in both semiconducting and optoelectronic nanodevices. Herein, a phase diagram for the transient states and relevant dynamic processes in multi-walled BN nanotubes (BNNTs) has been extensively studied for a full reversible cycle after a fs-laser excitation in ultrafast TEMs, and the significant structural features and evolution of electronic natures have been investigated using pulsed electron diffraction and femtosecond-resolved electron energy-loss spectroscopy (EELS). It is revealed that nonthermal anisotropic alterations of the lattice apparently precede the phonon-driven thermal transients along the radial and axial directions. Ab-initio calculations support these findings and show that electrons excited from the π to π* orbitals in the BN nanotubes weaken the intralayer bonds while strengthening the interlayer bonds along the radial direction. Importantly, time-resolved EELS measurements show remarkable contraction of the energy bandgap after fs-laser excitation associated with nonthermal structural transients. This fact verifies that laser-induced bandgap renormalisation in semiconductors can essentially be correlated with both the rapid processes of excited carriers and nonthermal lattice evolution.

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10.1021/acsnano.9b05466
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