The boson peak in deeply cooled water confined in nanopores is studied to examine the liquid-liquid transition (LLT). Below ∼180 K, the boson peaks at pressures P higher than ∼3.5 kbar are evidently distinct from those at low pressures by higher mean frequencies and lower heights. Moreover, the higher-P boson peaks can be rescaled to a master curve while the lower-P boson peaks can be rescaled to a different one. These phenomena agree with the existence of two liquid phases with different densities and local structures and the associated LLT in the measured (P, T) region. In addition, the P dependence of the librational band also agrees with the above conclusion. DOI: 10.1103/PhysRevLett.115.235701 PACS numbers: 64.70.Ja, 25.40.Fq, 63.50.-x Water is a continuing source of fascination to scientists because of its abnormal behavior at low temperatures T. Upon cooling, its thermodynamic properties, such as density, isobaric heat capacity, and isobaric thermal expansivity, deviate from those of simple liquids significantly [1][2][3][4]. In addition, glassy water, also called amorphous ice, exhibits polyamorphism. Experiments show that two kinds of amorphous ice, low-density amorphous ice (LDA) and high-density amorphous ice (HDA), exist at very low temperatures [5][6][7]. These two phases can transform to each other through a first-order-like transition [7,8]. To account for these mysterious phenomena, a "liquid-liquid critical point (LLCP)" scenario, which assumes a first-order low-density liquid (LDL) to high-density liquid (HDL) phase transition in the deeply cooled region of liquid water, has been proposed [9]. Therefore, experimental tests on the existence of the LDL and the HDL and the associated liquid-liquid transition (LLT) are important for understanding water. Nevertheless, such measurements are practically difficult due to the rapid crystallization of bulk water below the homogeneous nucleation temperature (235 K at 1 atm). To overcome this barrier and enter the deeply cooled region of water, different systems, including aqueous solutions [10][11][12][13][14], microsized water droplets [15], and confined water systems [16][17][18][19], have been prepared and studied. Particularly, when confined in a nanoporous silica matrix, MCM-41, with a 15-Å pore diameter, water can be kept in the liquid state at least down to 130 K [20,21]. Thus, the MCM-41-confined water system provides a chance to explore the hypothetical LLT.Recently, we observed a likely LLT in heavy water confined in MCM-41 by a density measurement. The associated phase diagram is shown in Fig. 1(a) [22]. However, the relevant measurements on the dynamic properties are still lacking. In fact, various dynamic properties, including the structural relaxation [10,16], the stretching vibration [10,11], the mean square displacement [23], etc., have been measured to study the phase behaviors of aqueous solutions or confined water. Examinations of FIG. 1 (color online). (a) Phase diagram of deeply cooled confined heavy water [22]. The inset shows th...