Alfio Basile has resigned as coach of Argentina, the country's football association have confirmed.
Wednesday's 1-0 defeat to Chile in Santiago left Argentina seven points behind South American leaders Paraguay in their World Cup qualifying group, while they have won only one World Cup qualifier this year, a 2-1 home triumph over Uruguay on Saturday following four consecutive draws against Ecuador, Brazil, Paraguay and Peru, to lie third in the standings.
Basile's resignation brings the curtain down on the 64-year-old's second stint in charge of the national team.
He had previously led Argentina to the 1994 World Cup in the USA before they were knocked out in the second round by Romania, prompting him to quit.
Basile took the helm once more after the 2006 World Cup following Jose Pekerman's resignation and guided Argentina to the final of the Copa America in 2007, where they lost 3-0 to arch-rivals Brazil.
Sergio Batista, who was part of the 1986 World Cup-winning side, is certain to be among the front-runners to replace Basile after coaching Argentina to gold at this summer's Olympic Games.
"I'm convinced I can coach the senior team. If it's my turn, I will take it," he said.
River Plate boss Diego Simeone and Miguel Angel Russo, coach of league leaders San Lorenzo, are other potential candidates.
Midfielder Lionel Messi had earlier expressed his deep disappointment at Argentina's performance against Chile.
"The truth is that we've done everything badly," he said.
"I know I didn't play well. We all didn't play well. We must correct a lot of things for the future."
"I know him [Batista] and I like his style of work," said Messi, who starred in Argentina's Olympic triumph. "I trust in him. It would be a good choice."
Grondona admitted Basile's decision had caught him off-guard.
"I'm surprised. Basile told me he resigned for personal reasons. I don't know which those reasons are, time will tell," he said.
"I wasn't expecting this. I guess he was feeling uncomfortable for some reason but if we look at our qualifying position, we were not too bad."
Grondona echoed Bialo's comments that the AFA had not yet begun the search for a new boss.
"We can't talk about the successor yet. It's too soon," he added.