Semi-crystalline polymers such as polyethylene (PE) and polypropylene (PP) show complicated morphologies composed of a mixture of crystalline and amorphous phases. The diversity in the structure with a wide range of length scales is responsible for the durability or high toughness of semi-crystalline polymers [1,2].When a high-density polyethylene (HDPE) specimen is uniaxially drawn, the elastic deformation is followed by double yield points referred to as the first and the second yields. During such dual plastic deformations, large-scale transformation of the semi-crystalline morphology takes place, and collapse of the spherulite structures, necking of the sample specimens, and rearrangement of the lamellar crystals and the polymer chains have been observed [1][2][3][4][5][6]. Although various models, such as the lamellar local-melting and recrystallization model [4,7], and the lamellar cluster model [3,[8][9][10], have been proposed for the deformation mechanism, such complicated changes in the hierarchical structures of semicrystalline polymers are still controversial.Spectroscopic techniques have been applied for the orientational behavior of PE during elongation [11][12][13][14][15][16][17]. The infrared (IR) spectroscopy has been applied intensively, and it has been established that the molecular chains in the crystalline and amorphous phases orientate toward the draw direction [11][12][13][14]. It has also been demonstrated that the orientation proceeds rapidly after the first yield, and gradually in the neck-propagation and the strain-hardening regions.However, the IR spectroscopy gives one orientation parameter 〈P 2 〉 which corresponds to the averaged orientation. For PE, the vibrations of the side chains, such as CH 2 twisting and wagging, are IR-active, and the skeletal vibrations of the C-C bonds are IR-inactive, then the load sharing on the polymer chains could not be directly observed with the IR spectroscopy.Raman spectroscopy has several advantages to investigate the deformation behavior of polymeric materials [18][19][20][21][22][23][24]: it is applicable to opaque and thick samples, and molecular environments can be separately detected for both the crystalline and the amorphous phases. Raman scattering is an optical technique that provides a complementary approach to IR absorption when transparent and very thin (typically <100 µm thickness) films are required. In addition, it is advantageous to use Raman spectroscopy because the vibrations of the skeletal C-C bonds in main chains are directly observed [20,25]. Because the C-C stretching vibration is strongly Raman active, microenvironments of the polymer chains are probed by the spectral shifts [26,27]. Polarized Raman spectroscopy gives not only a measure of the average orientation, which is obtained by the usual spectroscopies such as birefringence and IR dichrom, but also the orientation distribution function (ODF, N(θ)) [28][29][30]. In the yielding region where the neck of the specimen is formed, complicated deformation mechanism is expect...