Catalonia has a strong independence movement and plans to hold a vote on independence regardless, leading to several recent attempts by the national government to stop the vote.
The regional leader considered the Generalitat is a victim of a coordinated aggression to prevent "the Catalonian people from freely demonstrating its opinion on October 1". The Spanish government also ordered the national post office not to distribute any material linked to the referendum, and private courier companies have been raided. It gave no details on the number of agents involved.
Security operations in Catalonia, an affluent region with a population of 7.5 million, sparked fierce backlash from pro-independence protesters who turned out in their thousands along Barcelona's main thoroughfare Gran Vía where police were raiding the regional government ministry of economy.
Catalan President Carles Puigdemont accused the Spanish government on Wednesday of a de-facto suspension of the region's self-governance with its actions to impede the Catalonia independence referendum.
Asked whether the vote could prove as divisive as the Brexit referendum has in the United Kingdom, the Catalan government source replied: "Democracy doesn't divide; it's the absence of democracy that divides people..."
After a series of rulings from the Constitutional Court decreed the vote illegal, Prime Minister Mariano Rajoy is imposing financial curbs on the regional administration and has promised tougher sanctions still if officials refuse to back down.
Puigdemont says the police operations are unlawful and are aimed at preventing Catalans from voting on October 1.
Finance minister Cristobal Montoro signed an order late on Tuesday that limits new credit and requires central authorities' supervision for every payment of non-essential services in Catalonia, the ministry said.
The reasons for Mr Jove's arrest were not immediately clear, but Spain's central government had warned that officials who help stage the referendum could face criminal charges.
Catalonia represents a fifth of Spain's 1.1-trillion-euro economy.
As news of the arrests emerged, protesters began to gather outside the ministry of economic affairs, and by mid-morning the crowd had swelled to more than 2,000, blocking Gran Via, one of Barcelona's principal thoroughfares.
He said the question of legality was "an internal issue for the Spanish and Catalan people", but added that democracy meant "to respect the will of the people". Both officials declined to be identified by name, following internal protocol.
Catalonia's pro-separatist government challenged the measure in Spain's Supreme Court but a court spokeswoman told AFP it was "in force" and would not be suspended while judges rule on its legality.