When I was director I chose Lenten hymns that focused on the the return of one's attention to God. No crucifixion music until Palm/Passion Sunday. I'm no longer directing the music but still lead singing occasionally. Here's what has been planned for Ash Wednesday:

Save your People--Jim Farrell Ps. 51--Kendzia As the Deer Longs [O Waly Waly alt.] Hosea--Western Priory Agnus Dei--chant Mass XVIII, Plainsong Amazing Grace

How's that for eclectic?

I also like With the Lord--Joncas and much of the Taize stuff--lots of opportunities for ad lib harmonies and obligatos, varied instrumentation, simple, easy to learn

If you're Catholic, here's a wonderful jazz setting of the responsorial psalm after the third reading (Exodus) Let Us Sing--Fintan O'Connor, I believe. We used sax, flute, piano, drums.