We demonstrate the application of as-grown calcium barium niobate (CBN) crystal with random-sized ferroelectric domains as a broadband frequency converter. The frequency conversion process is similar to broadband harmonic generation in commonly used strontium barium niobate (SBN) crystal, but results in higher conversion efficiency reflecting a larger effective nonlinear coefficient of the CBN crystal. We also analyzed the polarization properties of the emitted radiation and determined the ratio of d 32 and d 33 components of the second-order susceptibility tensor of the CBN crystal.Ferroelectric crystal has been exploited in a wide range of devices since its discovery in the 1920s [1]. These devices include filters for wireless communications, modulators in optical circuits, and optical frequency converters in laser technology. Most of these functions are based on 180°antiparallel ferroelectric domains and the ability to engineer these domains on the micro or submicroscale [2]. Of the many ferroelectrics, those asgrown with random-sized ferroelectric domains form a unique group. As far as application in nonlinear optics is concerned, the random domain pattern results in a spatially random modulation of the quadratic nonlinearity of the material. Thus, a pool of reciprocal lattice vectors with random orientations and random magnitudes is created to phase match nonlinear interactions over a broad spectrum of wavelengths. Such a technique is known as random quasi-phase matching (QPM) [3][4][5].A good case in point is strontium barium niobate (Sr x Ba 1−x Nb 2 O 6 , SBN) crystal, which has been commonly used for broadband second harmonic generation (SHG) [6], cascaded third harmonic generation [7,8], and even Čerenkov-type nonlinear interactions [9][10][11]. However, the phase transition temperature (Curie temperature, T c ) of the SBN crystal is low [12], which is a main drawback for laser applications. At high pump power, the crystal will undergo a transition to the paraelectric state, and consequently, the quadratic nonlinear optical effects will disappear [13]. Compared with SBN, calcium barium-niobated (Ca x Ba 1−x Nb 2 O 6 , CBN) crystal is more suitable for practical optical devices operating at higher pump powers because of its higher phase transition temperature. For example, the CBN crystal exhibits a transition temperature of about 539 K for the congruently melting composition with 28 mol. % of calcium (x 0.28, CBN-28) [14,15], but the SBN crystal shows a lower transition temperature of about 353 K for the congruently melting composition with 61 mol. % of strontium content (x 0.61, SBN-61) [16,17]. Recently, Čerenkov-type SHG has been demonstrated in the CBN-28 crystal, which can be used as a nonlinear prism [18][19][20].In this Letter, we show that the CBN crystal is superior over the traditional SBN crystal in terms of the frequency mixing process, which leads to a higher conversion efficiency. We demonstrate experimentally that the broadband SHG process in the CBN crystal is three to four times higher ...