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The Orthodox think that the split with Rome is theological.
They think that Rome has lapsed into theological heresies, the first being that the Holy Spirit proceeds from the Father AND THE SON.
The Orthodox say this is false. The Holy Spirit proceeds from the Father, not the Son. The Orthodox consider this to be a fundamental theological issue concerning the very nature of the Trinity.
Of course, were Catholics to drop the "and the Son" from the Creed, a very large theological difference with Orthodoxy would be removed.

Certain Greek theologians have struggled to adopt a philosophical framework in which the Catholic concept of the Holy Spirit proceeding from the Father "and the Son" is not a serious error (because it is not to be taken literally but figuratively). However, the Orthodox laity are not persuaded by this at all. They think that the Catholics lapsed into heresy by adding the term "and the Son" to the Creed, and that this is a dramatic theological error, because the Holy Spirit does NOT, in fact, proceed from the Son at all, and it is stubborn error: heresy, to insist that he does.

I think that's a little thing, because all of that high theology is really very abstract and not very important to my own relationship with God. But the Orthodox all know this distinction, and they think it's a big thing, a great theological gulf, a Roman HERESY, even though their bishops are now trying to tamp down that word.

The next great theological gulf erupts over the authority of the Pope. The Orthodox believe that the Pope is First Among Equals, he who presides at Councils of the Church, etc. But the Pope himself is subject to the Councils of the Church. He cannot change anything that the Seven Ecumenical Councils have decided upon. To Catholics, the infallibility of the Pope, when speaking ex cathedra on matters of faith and morals, is a THEOLOGICAL matter, itself an infallible doctrine. The Orthodox consider that doctrine to be in error. Just as Peter presided over, but did not have the authority to singularly direct the outcome of the Council of Jerusalem in Acts, so to the Pope is the Senior in Dignity, First Among Equals, but in the end just a patriarch, with an equal vote in Councils of the Church and no power to bind another patriarch of the Church. To the Orthodox, this is a disciplinary matter. But to Catholics, it is a theological matter, based on the concept of the power of the keys.

For the Orthodox to be willing to reunite with the Catholic Church, the Catholic Church must remove the heretical words (in the opinion of the Orthodox) "and from the Son" which they added, without authority, to the Nicene Creed, and the Catholics must abandon the heretical (in the opinion of the Orthodox) doctrine of Papal Supremacy.
These really are theological matters, not political ones.

The original split occurred over those words "and from the Son", which was a Western use but never an Eastern one. That's really theological, and not merely political. The Pope ordered that the "filioque" be used in the East. The Patriarch of Constantinople refused. The Pope excommunicated the Patriarch for heresy, and the Patriarch excommunicated the Pope for heresy in return. The East doesn't believe in the filioque. The West does.

Now, a compromise, from the Catholic position, might be to allow the Orthodox to practice their liturgy without saying the filioque. After all, the Eastern Rites and most ancient liturgies of the Catholic Church don't use it. Pope John Paul II and the Ecumenical Patriarch jointly presided at a mass/liturgy, and they did NOT say the words "And from the Son" when the recited the Creed - there are old Catholic liturgies that predate the adoption of the filioque, and the Pope used that.

Probably the Ecumenical Patriarch would be willing to go with that difference. But the Patriarch of Moscow will not tolerate that. Why? Because the words "and from the Son" will continue to be used in the Latin Church, and those words are heretical error, just like referring to Mary as co-redemptrix is a serious heretical error, bordering on blasphemy in the minds of conservative Eastern Orthodox. Of course, Catholicism did not embrace the co-redemptrix movement, but it also did not excommunicate it or fiercely condemn it as heretical either. The East doesn't like these strange new doctrines, like the filioque, or papal supremacy.

Even if the bishops of the East get around the problem intellectually, there is still the problem of the Orthodox laity. The organization of the Orthodox Church is radically different from the organization of the Roman Catholic. The Catholic clergy and episcopacy are monarchic: priests are made by bishops, bishops are made by other bishops, and bishops can be removed by the Pope. The laity doesn't vote for bishops, and can't remove clergy.
But in the East, the laity DO have a say in who becomes their bishop, and they can remove a bishop in certain circumstances.

So, for example, Cardinal Law, the former Bishop of Boston implicated in the pedophile priest-shuffling scandal: had he been an Orthodox bishop, the laity may have removed him from his episcopacy. The Eastern Church is not exactly democratic, but the laity DO retain a power of selection and removal. Now, is this a merely DISCIPLINARY matter, or is it a fundamentally THEOLOGICAL matter, about the proper ordering of the Church?

I would say that it is a theological matter.
I would also say that the Greeks and Russians are about as willing to accept a monarchical papacy and episcopacy as Americans are to accept a King. Thus, one of the prices that Rome will have to be willing to pay to reunite with the Orthodox East will be to allow the Eastern laity to remove from office those bishops, patriarchs and priests sent by Rome, which the laity find odious.

These are two profoundly different Churches at heart, and I think that the similarity in some appearances is glossed over by wishful thinking, almost entirely on the Roman Catholic side, about reunification.

The Orthodox agree that the Church should be unified. And they think that it will be when Rome abandons the heresies into which it has lapsed and readopts the Orthodox faith that Christ founded, which it believes Rome abandoned when it added strange doctrines like the filioque and the monarchic papacy.

All my life, ever since I understood the difference, like many Catholics I have dreamt of reunification of the Church, East and West. Pope John Paul II spoke of bringing the two "lungs" of the Church back together.
He, and many Catholics, are deeply sincere in their desire for reunion.

I have never met any Orthodox who were so eager. They do agree that Christ preached unity, but they think that the Roman Catholics are really just the first Protestants, and their view of reunification with Rome on any terms other than Rome simply abandoning all of the new doctrines adopted since the Seventh (and in their view, last) Ecumenical Council would be precisely the same thing as Roman Catholics would view the prospect of reuniting with Lutheranism by adopting Lutheran theology and practices.

Roman Catholics could not consider such a thing, because they believe it would be abandoning the truth for a sham of unity. That's how the Orthodox look at the various forms of Protestantism in the West, including Roman Catholicism. Again, this is from their eyes.

The theological problems are, I think, quite large. And given the full participation of the Orthodox laity in decisions in the Orthodox Church, it is a matter of somehow convincing millions of Orthodox to embrace Rome again.

This is altogether less likely, I think, than Rome and Canterbury coming back into union.