Kipczak Łucja, Karmakar Arka, Grzeszczyk Magdalena, Janiszewska Róża, Woźniak Tomasz, Chen Zhaolong, Pawłowski Jan, Watanabe Kenji, Taniguchi Takashi, Babiński Adam, Koperski Maciej, Molas Maciej R
Faculty of Physics, Institute of Experimental Physics, University of Warsaw, 02-093, Warsaw, Poland.
Institute for Functional Intelligent Materials, National University of Singapore, Singapore, 117544, Singapore.
Sci Rep. 2024 Mar 29;14(1):7484. doi: 10.1038/s41598-024-57622-w.
We investigate the vibrational and magnetic properties of thin layers of chromium tribromide (CrBr) with a thickness ranging from three to twenty layers (3-20 L) revealed by the Raman scattering (RS) technique. Systematic dependence of the RS process efficiency on the energy of the laser excitation is explored for four different excitation energies: 1.96 eV, 2.21 eV, 2.41 eV, and 3.06 eV. Our characterization demonstrates that for 12 L CrBr, 3.06 eV excitation could be considered resonant with interband electronic transitions due to the enhanced intensity of the Raman-active scattering resonances and the qualitative change in the Raman spectra. Polarization-resolved RS measurements for 12 L CrBr and first-principles calculations allow us to identify five observable phonon modes characterized by distinct symmetries, classified as the A and E modes. The evolution of phonon modes with temperature for a 16 L CrBr encapsulated in hexagonal boron nitride flakes demonstrates alterations of phonon energies and/or linewidths of resonances indicative of a transition between the paramagnetic and ferromagnetic state at Curie temperature ( K). The exploration of the effects of thickness on the phonon energies demonstrated small variations pronounces exclusively for the thinnest layers in the vicinity of 3-5 L. We propose that this observation can be due to the strong localization in the real space of interband electronic excitations, limiting the effects of confinement for resonantly excited Raman modes to atomically thin layers.
我们利用拉曼散射(RS)技术研究了三溴化铬(CrBr)薄层(厚度范围为3至20层,即3 - 20L)的振动和磁特性。针对四种不同的激发能量:1.96 eV、2.21 eV、2.41 eV和3.06 eV,探索了RS过程效率对激光激发能量的系统依赖性。我们的表征表明,对于12L的CrBr,由于拉曼活性散射共振强度增强以及拉曼光谱的定性变化,3.06 eV激发可被视为与带间电子跃迁共振。对12L CrBr进行的偏振分辨RS测量和第一性原理计算使我们能够识别出五种具有不同对称性的可观测声子模式,归类为A和E模式。封装在六方氮化硼薄片中的16L CrBr的声子模式随温度的演变表明,在居里温度( K)下,声子能量和/或共振线宽发生了变化,这表明顺磁态和铁磁态之间发生了转变。对声子能量的厚度效应的探索表明,仅在3 - 5L附近的最薄层中出现了微小的变化。我们认为,这一观察结果可能是由于带间电子激发在实空间中的强烈局域化,将共振激发拉曼模式的限制效应限制在了原子级薄的层中。