ConfigurationManager doesn’t save settings

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I think you should call the Save method

ConfigurationManager.Save(ConfigurationSaveMode.Modified);
ConfigurationManager.RefreshSection("appSettings");

EDIT

To be able to save you have to use a configuration object returned by the OpenExeConfiguration Method

//Create the object
Configuration config = ConfigurationManager.OpenExeConfiguration(ConfigurationUserLevel.None);

//make changes
config.AppSettings.Settings["Username"].Value = txtUsername.Text;
config.AppSettings.Settings["Password"].Value = txtPassword.Text;

//save to apply changes
config.Save(ConfigurationSaveMode.Modified);
ConfigurationManager.RefreshSection("appSettings");

More references here ConfigurationManager Class

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