Is there a way to work with files outside /nix in nixops?

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You need to set them up when switching to the configuration.
I just add a service similar to this when I have to do something like this. As you can see I also generate a keyfile and populate it with random data.

  systemd.services.roundcube-install = {
    serviceConfig.Type = "oneshot";
    wantedBy = [ "multi-user.target" ];
    script = ''
      mkdir -p /var/lib/roundcube/temp /var/lib/roundcube/logs
      chown -Rc roundcube:root /var/lib/roundcube
      chmod -c 700 /var/lib/roundcube
      if [ ! -s "/var/lib/roundcube/des_key" ]; then
        ${pkgs.coreutils}/bin/dd if=/dev/urandom bs=32 count=1 2>/dev/null | ${pkgs.coreutils}/bin/base64 > "/var/lib/roundcube/des_key"
        chown -c roundcube:root "/var/lib/roundcube/des_key"
        chmod -c 400 "/var/lib/roundcube/des_key"
      fi
      if [ -s "/var/lib/roundcube/roundcube.sqlite" ]; then
        # Just go ahead and remove the sessions on a boot
        ${pkgs.sqlite}/bin/sqlite3 "/var/lib/roundcube/roundcube.sqlite" "DELETE FROM session;"
      fi
    '';
  };