Charging that Delaware officials have stopped cooperating with his investigation, Sen. Chuck Grassley has sent a pointed letter to the state’s Division of Revenue in which he outlines specific, outstanding questions about the handling of former U.S. Senate candidate Christine O’Donnell’s tax records.

“On multiple occasions, my staff has requested a copy of your records retention policy, the opportunity to speak with [officials at the state’s Division of Revenue] and other clarifications related to these matters. To date, you have failed to respond,” the letter from the Iowa Republican, sent Friday, reads in part.

In a case first reported by The Washington Times, Ms. O’Donnell — a tea party favorite who in 2010 ran unsuccessfully for Vice President Joseph R. Biden’s former U.S. Senate seat — revealed last month that her personal tax information was accessed by David Smith, an investigator with Delaware’s Division of Revenue.

Revelations about the access, gained in March 2010, spawned an inquiry by the U.S. Treasury Department and denials by Delaware officials that anything inappropriate had taken place.

Calls and emails to the Delaware Division of Revenue were not returned over the weekend.

The case has attracted the attention of Mr. Grassley and others who fear the incident shows, at best, that personal tax information is vulnerable to snooping by state governments.

At worst, as Ms. O’Donnell has said, it’s an example of using tax information to deliberately target a political candidate.

Even though the Division of Revenue concedes that the investigator examined the records in March 2010 — and maintains that it was part of a typical review and in no way improper — Ms. O’Donnell didn’t learn about the incident until January, when she received a call from an investigator with the Treasury Department.

After the access came to light, Division of Revenue Director Patrick Carter apparently met with Treasury officials to review the incident and determined that nothing inappropriate had taken place.

But Mr. Grassley is questioning how that is possible because he and his staff have been told that the state retains tax access records for only three months.

“On July 23, 2013, you reported to my staff that the Tax Data Services database utilized by Delaware only maintains an electronic audit trail of systems access for three months. This leads me to question how you were able to confirm information about systems access and its appropriateness when it occurred two years to your interaction with the Treasury Department,” the letter says.

The Division of Revenue also has said, according to Mr. Grassley, that there is no “empirical proof” that Ms. O’Donnell’s tax records weren’t examined on prior occasions, raising the prospect that her personal information was accessed on more than one occasion.

Ms. O’Donnell’s story broke just as the Treasury Department’s tax watchdog acknowledged to Mr. Grassley that at least four politicians or political donors have had their personal tax records improperly accessed since 2006, including one case in which a willful violation of federal law was identified.

But the Justice Department has declined to prosecute any of the cases. Mr. Grassley, who serves on the Senate Finance and Judiciary committees, continues to seek more answers from Justice in addition to his interactions with Treasury and the Delaware Division of Revenue.

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