OK, so I kept working on this. Honestly, I think typing it out helped me find the answer I was looking for. So I'm posting it here incase other's are having this issue, and/or folks find issues with my methods.
I knew that I wanted to do some form of interpolation, as I didn't want a fix adjustment to time, but a drifting one. I finally came across the linspace function, which allows me to create linerarly spaced variables of equal length between two timestamps (in my case, I chose a larger value, 5000, since I'm trying to correct for only ~90 seconds). After converting those values into datenums, I was then able to run an interpolation and convert it back in to a datetime vector.
Thanks to all that looked at this!
timeGPSdiff=datenum(linspace(timeGPSreset,timeGPSstop,5000));
timeClockdiff=datenum(linspace(timeGPSreset,timeClockstop,5000));
DTall_num=datenum(DateTime);
newDTall=datetime(interp1(timeClockdiff,timeGPSdiff,DTall_num),'ConvertFrom','datenum');
>> newDTall
newDTall =
2272×1 datetime array
28-Mar-2019 00:00:05
28-Mar-2019 01:00:05
28-Mar-2019 02:00:05
28-Mar-2019 03:00:05
28-Mar-2019 04:00:05
28-Mar-2019 05:00:05
28-Mar-2019 06:00:05
28-Mar-2019 07:00:05
28-Mar-2019 08:00:05
28-Mar-2019 09:00:05
28-Mar-2019 10:00:05
28-Mar-2019 11:00:05
28-Mar-2019 12:00:05
28-Mar-2019 13:00:05
28-Mar-2019 14:00:05
28-Mar-2019 15:00:05
28-Mar-2019 16:00:05
28-Mar-2019 17:00:05
28-Mar-2019 18:00:05
28-Mar-2019 19:00:05
28-Mar-2019 20:00:06
28-Mar-2019 21:00:06
28-Mar-2019 22:00:06
28-Mar-2019 23:00:06
29-Mar-2019 00:00:06
29-Mar-2019 01:00:06
29-Mar-2019 02:00:06
29-Mar-2019 03:00:06
...
29-Jun-2019 08:04:31
29-Jun-2019 09:04:31
29-Jun-2019 10:04:31
29-Jun-2019 11:04:32
29-Jun-2019 12:04:32
29-Jun-2019 13:04:32
29-Jun-2019 14:04:32
29-Jun-2019 15:04:32
29-Jun-2019 16:04:32
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29-Jun-2019 22:04:32
29-Jun-2019 23:04:32
30-Jun-2019 00:04:32
30-Jun-2019 01:04:32
30-Jun-2019 02:04:32
30-Jun-2019 03:04:32
30-Jun-2019 04:04:32
30-Jun-2019 05:04:32
30-Jun-2019 06:04:32
30-Jun-2019 07:04:32
30-Jun-2019 08:04:32
30-Jun-2019 09:04:32
30-Jun-2019 10:04:32
30-Jun-2019 11:04:32
30-Jun-2019 12:04:32
30-Jun-2019 13:04:32
30-Jun-2019 14:04:32
30-Jun-2019 15:04:32
:D
Best Answer