A III–V semiconductor with a few monolayers of alkali metals (e.g., Cs) forms a negative electron affinity (NEA) surface, for which the vacuum level lies below the conduction band minimum of the base semiconductor. The photocathodes that form an NEA surface (NEA photocathodes) have various advantages, such as low emittance, a large current, high spin polarization, and ultrashort pulsed operation. The NEA-InGaN photocathode, which is sensitive to blue light, has been studied as a material for the next-generation robust photocathode. However, the proper conditions for forming NEA surfaces remain unknown. The authors consider whether the suitable process for NEA surfaces can be understood by investigating the relationship between the electron emission and the adsorption state of alkali metals. In this study, the relationship between the electron emission and the adsorption state of Cs on the p-type InGaN (0001) was analyzed by the temperature-programed desorption (TPD) method using a quadrupole mass spectrometer. From the results of the TPD measurements, it was shown that there were several adsorption states of Cs on InGaN. The quantum efficiency (QE), which indicates the ratio of emitted electrons to incident photons, increased while Cs desorption occurred. The authors divided the formation process of an NEA surface into several sections to investigate the adsorption states of Cs related to the electron emission and to discuss the reasons why the QE increased despite the desorbed Cs. From the results of the NEA activation in each section, it was shown that there were sections where the QE increased by reacting with O2 after Cs supply stopped. There is a possibility that several layers reacting with O2 and those not reacting with O2 are formed by performing NEA activation until the QE saturates. From the results of the TPD measurements in each section, it was suggested that there was a Cs peak at above 700 °C when the TPD method was carried out immediately after confirming the electron emission. Therefore, the adsorption state of Cs that formed a peak at above 700 °C had a close relation to the electron emission. It is considered that the increase of the QE in the TPD was affected by adsorbed Cs compounds that reacted with O2. Although the mechanism is not understood, it is known that the QE was increased by the reaction of Cs adsorbed compounds and O2 in previous studies. It was suspected that layers that reacted with O2 appeared from TPD and then the QE increased by reacting with O2.
Photocathodes with negative electron affinity (NEA) characteristics have various advantages, such as small energy spread, high spin polarization, and ultrashort pulsing. Nitride semiconductors, such as GaN and InGaN, are promising materials for NEA photocathodes because their lifetimes are longer than those of other materials. In order to further prolong the lifetime, it is important to better understand the deterioration of NEA characteristics. The adsorption of residual gases and back-bombardment by ionized residual gases shorten the lifetime. Among the adsorbed residual gases, H2O has a significant influence. However, the adsorption structures produced by the reaction with H2O are not comprehensively studied so far. In this study, we investigated adsorption structures that deteriorated the NEA characteristics by exposing InGaN and GaAs to an H2O environment and discussed the differences in their lifetimes. By comparing the temperature-programmed desorption curves with and without H2O exposure, the generation of CsOH was confirmed. The desorption of CsOH demonstrated different photoemission behaviors between InGaN and GaAs results. InGaN recovered its NEA characteristics, whereas GaAs did not. Considering the Cs desorption spectra, it is difficult for an NEA surface on InGaN to change chemically, whereas that for GaAs changes easily. The chemical reactivity of the NEA surface is different for InGaN and GaAs, which contributes to the duration of photoemission. We have attempted to prolong the lifetime of InGaN by recovering its NEA characteristics. We found that InGaN with NEA characteristics can be reused easily without thermal treatment at high temperatures.
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