Deep ultraviolet (DUV) and vacuum ultraviolet (VUV) lights are expected to be utilized in various fields; such as virus inactivation, [1] ozone generator, [2] and nanofabrication. [3] Especially, DUV lights in an energy range from 5.6 to 6.0 eV (207 to 222 nm) are attracting special attention because of their capability for sterilization without harm to human tissues. [4,5] Furthermore, VUV lights in an energy range above 6.2 eV (below 200 nm) can effectively produce photochemical reactions. [6,7] So far, most of commercialized DUV and VUV light sources consist of either by discharge type lamps or AlGaNbased light emitting diodes (LEDs). [8,9] However, they still have disadvantages, that is, the discharge type lamps exhibit short lifetime, high energy consumption, and large size. For AlGaN-based LEDs, their bandgap energies E g are in a range 3.4 to 6.0 eV, and they cannot produce VUV lights. [10,11] Demands are thus increasing for developing semiconductor-based light emitters in a sub-200 nm range, because of their advantages such as miniaturization, long lifetime, and low energy consumption.To develop the light emitters covering widely in DUV and VUV spectral regions, we are focusing on rocksalt-structured (RS) MgZnO alloys. RS-Mg x Zn 1Àx O alloys can vary their E g by changing x in a range from 2.45 eV of RS-ZnO to 7.8 eV of RS-MgO, [12][13][14] though the rocksalt-structure is thermally stable for x > 0.6. The E g values for the RS-Mg x Zn 1Àx O have been determined by optical transmittance measurements [14,15] to be in a range from 5.73 eV for x ¼ 0.61 to 6.53 eV for x ¼ 0.92 at 300 K. According to the first-principles calculations, [15,16] the E g values for x > 0.6 correspond to the direct Γ-Γ transition. Recently, we have succeeded in growth of atomically flat RS-MgZnO thin films on MgO substrates by the mist chemical vapor deposition (mist CVD) method. [17][18][19] The epitaxial films exhibited cathodoluminescence (CL) peaks located in a range from 5.09 eV (4.91 eV) at 6 K (300 K) for x ¼ 0.61 to 6.24 eV (6.05 eV) at 6 K (300 K) for x ¼ 0.95. [15,[17][18][19][20] The energy difference between the E g and CL peak positions is defined as the Stokes-like shift. The origin of the relatively large Stokes-like shift of 0.8-0.9 eV is a debatable issue. Possible origin was attributed to the differences in the local arrangement of Mg and Zn atoms in the Mg x Zn 1Àx O alloy by virtue of the electronic structure calculation. [15] However, Gorczyca and coworkers have recently pointed out that the clustered Zn-O-Zn configurations result in an indirect bandgap for x > 0.5 by evaluating the unfolded electronic structures for different-sized supercells. [16] Though