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Research Article

Selective substitution induced anomalous phonon stiffening within quasi-one-dimensional P–P chains in SiP2

Xueting Dai1, Feng Qin1, Caiyu Qiu1, Ling Zhou1, Junwei Huang1, Fanghua Cheng1, Xiangyu Bi1, Caorong Zhang1, Zeya Li1, Ming Tang1, Shengqiang Wu2, Xiaoxu Zhao2( ), Yangfan Lu3( ), Huiyang Gou4, Hongtao Yuan1( )
National Laboratory of Solid State Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, College of Engineering and Applied Sciences, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210000, China
School of Materials Science and Engineering, Peking University, Beijing 100871, China
College of Materials Science and Engineering, National Engineering Research Center for Magnesium Alloys, Chongqing University, Chongqing 400030, China
Center for High Pressure Science and Technology Advanced Research, Beijing 100094, China
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Graphical Abstract

Based on the selective substitution of arsenic for phosphorus in quasi-one-dimensional (1D) P–P chains of SiP2, we demonstrated that the redshift of the exciton emission energy and the phonon stiffening of B31g vibration mode are strongly associated with the quasi-1D structure. Our results establish a new material platform for studying light-matter interactions of quasi-1D atomic chains in bulk crystals and for exploring potential anisotropic optoelectronic applications.

Abstract

Light-matter interactions in low-dimensional quantum-confined structures can dominate the optical properties of the materials and lead to optoelectronic applications. In anisotropic layered silicon diphosphide (SiP2) crystal, the embedded quasi-one-dimensional (1D) phosphorus–phosphorus (P–P) chains directly result in an unconventional quasi-1D excitonic state, and a special phonon mode vibrating along the P–P chains, establishing a unique 1D quantum-confined system. Alloying SiP2 with the homologous element serves as an effective way to study the properties of these excitons and phonons associated with the quasi-1D P–P chains, as well as the strong interaction between these quasiparticles. However, the experimental observation and the related optical spectral understanding of SiP2 with isoelectronic dopants remain elusive. Herein, with the photoluminescence and Raman spectroscopy measurements, we demonstrate the redshift of the confined excitonic peak and the stiffening of the phonon vibration mode B1g3 of a series of Si(P1−xAsx)2 alloys with increasing arsenic (As) compositions. This anomalous stiffening of B1g3 is attributed to the selective substitution of As atoms for P atoms within the P–P chains, which is confirmed via our scanning transmission electron microscopy investigation. Such optical spectra evolutions with selective substitution pave a new way to understand the 1D quantum confinement in semiconductors, offering opportunities to explore quasi-1D characteristics in SiP2 and the resulting photonic device application.

Keywords

SiP2quasi-one-dimensional structureRamanphotoluminescencephosphide

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Nano Research
Volume 16 Issue 1,
January 2023
Pages 1107-1114
DOI: 10.1007/s12274-022-4703-x
Cite this article:
Dai X, Qin F, Qiu C, et al. Selective substitution induced anomalous phonon stiffening within quasi-one-dimensional P–P chains in SiP2. Nano Research, 2023, 16(1): 1107-1114. https://doi.org/10.1007/s12274-022-4703-x
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Received: 21 April 2022
Revised: 09 June 2022
Accepted: 26 June 2022
Published: 26 July 2022
© Tsinghua University Press 2022
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