Harmison turned out for the England Lions at Worcester on Wednesday and bowled with fire and pace in returning three for 67 from 22 overs.
Among his victims was Australian opener Phillip Hughes who, at the age of 20, averages 60 in Test cricket but looked vulnerable to the short ball from Harmison.
Harmison does not expect to play in the opening test at Cardiff but hopes he has laid down a marker to be involved later in the five-match showdown with Ricky Ponting's side.
He said: "I probably would not play at Cardiff. That would be a pleasant surprise. All the talk is of playing two spinners down there.
"If the chance came, I would jump at the chance. I'd love to play. I'm desperate to play for England.
"I couldn't be disappointed about not being in the 16-man performance squad because the way England have bowled in recent Tests. I didn't fit in.
"Graham Onions and Tim Bresnan have bowled well, been the pick-out bowlers at the start of the summer, Ryan Sidebottom is fit, Jimmy Anderson and Stuart Broad are bowling well enough and Freddie (Flintoff) is back fit.
"But I want to play for England - and the day I stop wanting to play for England is the day I tell them that I've had enough.
"They've seen I want to play and can cause Australia problems. It is up to them whether they want to pick me or not."
Harmison also believes Australia are suffering from a crisis of confidence.
He said: "This is my fourth time against Australia and the one thing I picked up on the day before the game is that they are not as brash and confident as they normally are.
"I can't put my finger on it. Maybe it is to do with the side gelling together or whether they don't have the big players of recent years, and the confidence you get from that.
"But they don't seem to be the confident Australia I've known. I think there is only Ricky Ponting and Brett Lee who have played more Ashes tests than myself in the two squads.
"There are things you pick up on like body language. I've seen a little chink there. It is understandable because there are not the players in their side from bygone years.
"There is definitely something to work on for England and, if we can bat well, we have half a chance to win the Ashes back."
Australian century-maker Mike Hussey is backing Hughes to bounce back from his searching examination by Harmison and co as Australia closed on 337 for eight from 90 overs.
He said: "Phil will be fine, The thing about Phil is he plays with freedom and no fear. If he keeps a clear mind and plays his way, he will be effective. He has got to stick with what has brought him success."
Hussey is delighted to have ended his nine month drought without a century and he finished on unbeaten on 143.
He said: "It has been a long time since I scored a century and to spend so much time in the middle was important only a week before the Ashes get under way.
"I guess you do start to question whether you can still do it. It was good to get my confidence up and get a big score under my belt."
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