How can I force version 5.0.1 on Note 4 to only connect to 4G LTE when available?
It seems that this answer (by Void) worked well for OP. You can setup your device to connect to &quot;4G LTE&quot; only by using the following steps:

In dialer, press *#*#4636#*#*
Go to Phone Information
Scroll down to Set preferred network type: and tap the entry below it.
Choose LTE only.
Optionally: Tap Turn off radio → Turn on radio

Or,
If you cannot access that menu using the code in dialer, then install and launch Elixir 2 → information
→ tap Telephony → Turn WiMAX (4G) on → repeat aforesaid steps 3-5.
An important note by OP

This disabled my incoming calls and they were going straight to voicemail. Not sure if this is a [New York City (high volume - stressed network)] thing or if voice just generally never goes over LTE but [I] had to switch it back.