The following works for me with blackbox_exporter 0.21.0 (maybe your first 
'expect' regexp needs to be quoted?)

modules:
  smtp_starttls:
      prober: tcp
      timeout: 5s
      tcp:
        query_response:
          - expect: "^220 ([^ ]+) ESMTP (.+)$"
            send: "EHLO prober"
          - expect: "^250-STARTTLS"
          - expect: "^250 .*$"
            send: "STARTTLS"
          - expect: "^220"
            starttls: true
          - send: "EHLO prober"
          - expect: "^250 .*$"
            send: "QUIT"

Result:

# *curl -g 
'localhost:9115/probe?module=smtp_starttls&target=aspmx.l.google.com:25&debug=true'*
Logs for the probe:
ts=2022-07-04T09:50:46.764604425Z caller=main.go:351 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Beginning probe" probe=tcp 
timeout_seconds=5
ts=2022-07-04T09:50:46.764875668Z caller=tcp.go:40 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Resolving target address" 
target=aspmx.l.google.com ip_protocol=ip6
ts=2022-07-04T09:50:46.765954096Z caller=tcp.go:40 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Resolved target address" 
target=aspmx.l.google.com ip=2a00:1450:400c:c07::1b
ts=2022-07-04T09:50:46.766011111Z caller=tcp.go:121 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Dialing TCP without TLS"
ts=2022-07-04T09:50:46.776962616Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Successfully dialed"
ts=2022-07-04T09:50:46.77708032Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Processing query response 
entry" entry_number=0
ts=2022-07-04T09:50:46.788075017Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line="220 
mx.google.com ESMTP u1-20020a056000038100b0021bbcef3a69si36572085wrf.542 - 
gsmtp"
ts=2022-07-04T09:50:46.788168204Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Regexp matched" regexp="^220 
([^ ]+) ESMTP (.+)$" line="220 mx.google.com ESMTP 
u1-20020a056000038100b0021bbcef3a69si36572085wrf.542 - gsmtp"
ts=2022-07-04T09:50:46.788223914Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Sending line" line="EHLO 
prober"
ts=2022-07-04T09:50:46.788362926Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Processing query response 
entry" entry_number=1
ts=2022-07-04T09:50:46.801755535Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" 
line="250-mx.google.com at your service, [xx:xx:xx:xx::33]"
ts=2022-07-04T09:50:46.801856147Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line="250-SIZE 
157286400"
ts=2022-07-04T09:50:46.801889927Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-8BITMIME
ts=2022-07-04T09:50:46.801922312Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-STARTTLS
ts=2022-07-04T09:50:46.801955499Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Regexp matched" 
regexp=^250-STARTTLS line=250-STARTTLS
ts=2022-07-04T09:50:46.801989646Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Processing query response 
entry" entry_number=2
ts=2022-07-04T09:50:46.802029066Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" 
line=250-ENHANCEDSTATUSCODES
ts=2022-07-04T09:50:46.802063318Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-PIPELINING
ts=2022-07-04T09:50:46.802094713Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-CHUNKING
ts=2022-07-04T09:50:46.802126198Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line="250 SMTPUTF8"
ts=2022-07-04T09:50:46.802159858Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Regexp matched" regexp="^250 
.*$" line="250 SMTPUTF8"
ts=2022-07-04T09:50:46.802191065Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Sending line" line=STARTTLS
ts=2022-07-04T09:50:46.802271697Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Processing query response 
entry" entry_number=3
ts=2022-07-04T09:50:46.812211682Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line="220 2.0.0 
Ready to start TLS"
ts=2022-07-04T09:50:46.812279339Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Regexp matched" regexp=^220 
line="220 2.0.0 Ready to start TLS"
ts=2022-07-04T09:50:46.833573801Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="TLS Handshake (client) 
succeeded."
ts=2022-07-04T09:50:46.833793385Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Processing query response 
entry" entry_number=4
ts=2022-07-04T09:50:46.833838422Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Sending line" line="EHLO 
prober"
ts=2022-07-04T09:50:46.833960852Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Processing query response 
entry" entry_number=5
ts=2022-07-04T09:50:46.84464181Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" 
line="250-mx.google.com at your service, [xx:xx:xx:xx::33]"
ts=2022-07-04T09:50:46.844771942Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line="250-SIZE 
157286400"
ts=2022-07-04T09:50:46.844839074Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-8BITMIME
ts=2022-07-04T09:50:46.844910271Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" 
line=250-ENHANCEDSTATUSCODES
ts=2022-07-04T09:50:46.844974538Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-PIPELINING
ts=2022-07-04T09:50:46.845061058Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line=250-CHUNKING
ts=2022-07-04T09:50:46.84512579Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Read line" line="250 SMTPUTF8"
ts=2022-07-04T09:50:46.845193403Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Regexp matched" regexp="^250 
.*$" line="250 SMTPUTF8"
ts=2022-07-04T09:50:46.84525809Z caller=main.go:144 module=smtp_starttls 
target=aspmx.l.google.com:25 level=debug msg="Sending line" line=QUIT
ts=2022-07-04T09:50:46.845583228Z caller=main.go:351 module=smtp_starttls 
target=aspmx.l.google.com:25 level=info msg="Probe succeeded" 
duration_seconds=0.080912196



Metrics that would have been returned:
# HELP probe_dns_lookup_time_seconds Returns the time taken for probe dns 
lookup in seconds
# TYPE probe_dns_lookup_time_seconds gauge
probe_dns_lookup_time_seconds 0.001103057
# HELP probe_duration_seconds Returns how long the probe took to complete 
in seconds
# TYPE probe_duration_seconds gauge
probe_duration_seconds 0.080912196
# HELP probe_failed_due_to_regex Indicates if probe failed due to regex
# TYPE probe_failed_due_to_regex gauge
probe_failed_due_to_regex 0
# HELP probe_ip_addr_hash Specifies the hash of IP address. It's useful to 
detect if the IP address changes.
# TYPE probe_ip_addr_hash gauge
probe_ip_addr_hash 2.766777767e+09
# HELP probe_ip_protocol Specifies whether probe ip protocol is IP4 or IP6
# TYPE probe_ip_protocol gauge
probe_ip_protocol 6
# HELP probe_ssl_earliest_cert_expiry Returns earliest SSL cert expiry date
# TYPE probe_ssl_earliest_cert_expiry gauge
probe_ssl_earliest_cert_expiry 1.661764429e+09
# HELP probe_ssl_last_chain_expiry_timestamp_seconds Returns last SSL chain 
expiry in unixtime
# TYPE probe_ssl_last_chain_expiry_timestamp_seconds gauge
probe_ssl_last_chain_expiry_timestamp_seconds 1.661764429e+09
# HELP probe_success Displays whether or not the probe was a success
# TYPE probe_success gauge
probe_success 1



Module configuration:
prober: tcp
timeout: 5s
http:
    ip_protocol_fallback: true
    follow_redirects: true
    enable_http2: true
tcp:
    ip_protocol_fallback: true
    query_response:
        - expect: ^220 ([^ ]+) ESMTP (.+)$
          send: EHLO prober
        - expect: ^250-STARTTLS
        - expect: ^250 .*$
          send: STARTTLS
        - expect: ^220
          starttls: true
        - send: EHLO prober
        - expect: ^250 .*$
          send: QUIT
icmp:
    ip_protocol_fallback: true
dns:
    ip_protocol_fallback: true
    recursion_desired: true

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