You know, I think Jack Kotz had some inorganic computational exercises that he developed using CAChe. CAChe was the first computational package that we incorporated into our classes at Hope College (oh, so long ago). It would be wonderful to get a hold of those and perhaps adapt them for DFT calculations. Everything Jack did, he did with care, thoroughness, and good insight, so I know they would make great starting points. Let's look into this!

For example:

Here's a link to an inorganic lab they use (or "used," the link suggest it's from 2004) at SUNY Binghamton that is adapted from Microscale Inorganic Chemistry, by Z. Szafran, R. M. Pike, and M. M. Singh, John Wiley: New York, 1991 AND from Jack Kotz (SUNY Oneonta).

http://chemistry.binghamton.edu/chem445/dmso/dmso.htm

It has an interesting computational component that could be adapted.

(It makes more sense if you read my posts from bottom to top, in chronological order.)

Once I remembered CAChe, I found a number of useful resources. These are not the "tested experiments" you're looking for, but they're great starting points for developing new exercises. Even though the computational approach might not be what you want, the pedagogy has been thought through (how the problem is posed, what questions are asked). So it saves a little of reinventing the wheel.

Crispin Wong and James Currie of Pacific University edited a really good volume on teaching with CAChe. It is available for free download at http://www.fqs.pl/chemistry/cache/teaching

It has a chapter with a significant number of inorganic exercises. Here's the Table of Contents for that chapter (Scott, it has an exercise on MO's of diatomics):

Part 4: Inorganic Chemistry
Experiment 10 Polarities of Small Molecules
Experiment 11 Structures of Molecules Which Exceed the Octet Rule
Experiment 12 Comparison of Gas Phase Acidities of Binary Hydrogen Compounds
Experiment 13 Crystal Lattices and Close Packing Sites
Experiment 14 Identification and Execution of Symmetry Operations
Experiment 15 The Relationship Between Infrared Spectra and Molecular Geometry
Experiment 16 Molecular Orbitals of Simple Molecules
Experiment 17 Molecular Orbitals of Diatomic Molecules of Second Period Elements
Experiment 18 Molecular Orbitals of Octahedral Transition Metal Complexes
Experiment 19 Relative Ligand Field Strengths
Experiment 20 Stereoselectivity of Chiral Chelating Ligands in Metal Complexes

Karen Brewer also developed some nice CAChe tutorials. http://www.chem.vt.edu/chem-dept/brewer/CAChe/cache.html

By the way, CAChe is now part of Fujitsu's Chemical and Materials Science Group and is called SciGress Explorer. http://www.fqs.pl/chemistry/cache

****I am imagining our first big communal VIPEr publication. Everyone can take one of these experiments to adapt, post their result on VIPEr and then we can write a zillion-author J Chem Ed paper explaining it all!

We have used PC Spartan in our department for many years, especially in the organic chemistry curriculum.  I teach the fall semester of general chemistry (structure and bonding), and have developed simple Spartan activities for exploring atomic orbitals and molecular structure and polarity.  

In my second year inorganic course, I use Spartan extensively for molecular orbitals of diatomics and I usually try and build in one or more exercises for polyatomics.  Last year, I was at the ACS meeting in Salt Lake City at the conclusion of our MO unit, and so I assigned a lengthy "in-class" Spartan activity for students to complete in my absence.  For all of these activities, I calculate the models in advance and students examine the surfaces and the calculated energy levels.

I have used Spartan less in Advanced Inorganic, although I would like to try some more independent projects with students based on some of the learning objects posted on VIPEr.

I would be more than happy to share the materials I have.

Our department moved from Spartan to Gaussian a few years ago. Prior to the transition, I used Spartan with my sophomore inorganic students to model very basic homonuclear diatomic models. Our organic chemists also used it in some of their course work.

When we were using Spartan, I found the books published by Wavefunction to contain many good activities & nuggets around which activities could be developed. You can find the books on their website: http://www.wavefun.com/products/books/books.html.

I posted the Spartan activity that I asked students to complete while I was away at the ACS conference last spring.  This is for my 200-level sophomore inorganic course "on steroids" (meaning I do a fair amount of MO theory in this course).

Exploring Molecular Orbitals With Spartan

Included with this activity is a "How To" sheet that I provide for students on viewing models in Spartan and that we have already used once before in class prior to this assignment.