Author(s): Zou, B (Zou, Bo); Wang, XA (Wang, Xiaonan); Zhou, Y (Zhou, Yu); Zhou, Y (Zhou, Yan); Wu, YY (Wu, Yanyan); Xing, TT (Xing, Tiantian); He, Y (He, Yang); Yang, JF (Yang, Jinfeng); Chen, YX (Chen, Yuxiang); Ren, P (Ren, Peng); Sun, HR (Sun, Huarui)

Source: SMALL DOI: 10.1002/smll.202206932 Early Access Date: FEB 2023

Abstract: Optical anisotropy, which is quantified by birefringence (& UDelta;n) and linear dichroism (& UDelta;k), can significantly modulate the angle-resolved polarized Raman spectroscopy (ARPRS) response of anisotropic layered materials (ALMs) by external interference. This work studies the separate modulation of birefringence on the ARPRS response and the intrinsic response by selecting transparent birefringent crystal alpha-MoO3 as an excellent platform. It is found that there are several anomalous ARPRS responses in alpha-MoO3 that cannot be reproduced by the real Raman tensor widely used in non-absorbing materials; however, they can be well explained by considering the birefringence-induced Raman selection rules. Moreover, the systematic thickness-dependent study indicates that birefringence modulates the ARPRS response to render an interference pattern; however, the amplitude of modulation is considerably lower than that by linear dichroism as occurred in black phosphorous. This weak modulation brings convenience to the crystal orientation determination of transparent ALMs. Combining the atomic vibrational pattern and bond polarizability model, the intrinsic ARPRS response of alpha-MoO3 is analyzed, giving the physical origins of the Raman anisotropy. This study employs alpha-MoO3 as an example, although it is generally applicable to all transparent birefringent ALMs.

Accession Number: WOS:000935767600001

PubMed ID: 36807515

ISSN: 1613-6810

eISSN: 1613-6829

Full Text: https://onlinelibrary.wiley.com/doi/10.1002/smll.202206932