No, you cannot. However, you can populate search help values dynamically in AT SELECTION-SCREEN ON VALUE-REQUEST
event:
DATA: LT_VBAK TYPE STANDARD TABLE OF VBAK.
PARAMETER P_VBELN TYPE VBELN.
AT SELECTION-SCREEN ON VALUE-REQUEST FOR P_VBELN.
CALL FUNCTION 'F4IF_INT_TABLE_VALUE_REQUEST'
EXPORTING
RETFIELD = 'VBELN'
DYNPPROG = SY-REPID
DYNPNR = SY-DYNNR
DYNPROFIELD = 'P_VBELN'
VALUE_ORG = 'S'
TABLES
VALUE_TAB = LT_VBAK
EXCEPTIONS
PARAMETER_ERROR = 1
NO_VALUES_FOUND = 2
OTHERS = 3.
IF SY-SUBRC <> 0.
MESSAGE ID SY-MSGID TYPE SY-MSGTY NUMBER SY-MSGNO
WITH SY-MSGV1 SY-MSGV2 SY-MSGV3 SY-MSGV4.
ENDIF.
where LT_VBAK
is a internal table you need to populate with values.
If your values are dependent on another selection screen parameter, use DYNP_VALUES_READ
FM to read them from screen.
Another approach is not to dynamically fill values but to create a single Search Help in DDIC and create Search Help exit which will control SHELP behavior depending on some conditions.