A “relevant clue” was reportedly found during a search of Arade Dam in Portugal, about 50km inland from the beach resort where three-year-old Madeleine McCann disappeared while on a family holiday in 2007.
Materials have now been sent for testing in Germany.
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Authorities searched two heavily wooded areas near the bank of the dam during the three-day operation, leaving behind several holes.
A “relevant clue” was found on Thursday, Portuguese newspaper Correio da Manha has reported.
The search was seen concentrated in one area of interest at the dam, the newspaper said.
Police from Portugal, Germany and the UK were involved in the search, erecting two tents beside the dam on Monday.
They cleared vegetation from the wooded areas before raking through the soil, and sent in sniffer dogs after this was done.
Bags of evidence were later seen being removed from the site.
7NEWS understands police were searching for items including Madeleine’s pyjamas, a camcorder and a gun belonging to Brueckner.
The first day of the search was concentrated on finding clothing items, Correio da Manha reported.
The possible new evidence comes after German authorities last year formally identified German man Christian Brueckner as an official suspect in the disappearance of the British girl.
German investigators believe the girl may have been killed near the dam and thrown into the water, according to Correio da Manha.
Brueckner, a convicted child abuser and drug dealer serving jail time in Germany, regularly visited the Arade Dam area around the time of Madeleine’s disappearance.
It is understood some of Brueckner’s associates may have stolen the items and left them near the dam.
The camcorder may contain video that could tie Brueckner to a number of sexual assaults and possibly Madeleine’s disappearance.
Soil samples have been taken to Germany, where they will be forensically tested.
The German prosecutor said they will announce if the samples contain anything of note as soon as this is evident.
Brueckner has denied any involvement with Madeleine’s disappearance and has not been charged with any crime related to it.
A German court last month found that German prosecutors did not have jurisdiction in relation to sexual offences he allegedly committed in Portugal between 2000 and 2017.
He was previously convicted of a rape in Portugal in 2005.
The Braunschweig state court denied responsibility for the new charges against Brueckner, due to disputed evidence about his last-known address in Germany.
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