It would probably be the other way around; I'd shoot a high contrast slide film with the aperture wide open. The image you linked to looks cross processed, which I think increases contrast as well.
You could mechanically introduce vignette by adding a home-made vignetter (like a lens hood). Just figure out your field of view and attach a black paper tube around the lens, sized to slightly obstruct your field of view. May take some trial and error but that's a way you can introduce vignette.