I have a pandas dataframe with datetime index
Date
2013-02-22 00:00:00+00:00    0.280001
2013-02-25 00:00:00+00:00    0.109999
2013-02-26 00:00:00+00:00   -0.15         
        
Here's one way to do it, first grab the integer location of the index key via get_loc:
In [15]: t = pd.Timestamp("2013-02-27 00:00:00+00:00")
In [16]: df1.index.get_loc(t)
Out[16]: 3
And then you can use iloc (to get the integer location, or slice by integer location):
In [17]: loc = df1.index.get_loc(t)
In [18]: df.iloc[loc - 1]
Out[18]: 
Date    2013-02-26 00:00:00
                      -0.15
Name: 2, Dtype: object
In [19]: df1.iloc[slice(max(0, loc-3), min(loc, len(df)))]
        # the min and max feel slightly hacky (!) but needed incase it's within top or bottom 3
Out[19]:                         
Date                    
2013-02-22  0.280001
2013-02-25  0.109999
2013-02-26 -0.150000
See the indexing section of the docs.
I'm not quite sure how you set up your DataFrame, but that doesn't look like a Datetime Index to me. Here's how I got the DataFrame (with Timestamp index):
In [11]: df = pd.read_clipboard(sep='\s\s+', header=None, parse_dates=[0], names=['Date', None])
In [12]: df
Out[12]: 
                 Date          
0 2013-02-22 00:00:00  0.280001
1 2013-02-25 00:00:00  0.109999
2 2013-02-26 00:00:00 -0.150000
3 2013-02-27 00:00:00  0.130001
4 2013-02-28 00:00:00  0.139999
In [13]: df1 = df.set_index('Date')
In [14]: df1
Out[14]:                
Date                
2013-02-22  0.280001
2013-02-25  0.109999
2013-02-26 -0.150000
2013-02-27  0.130001
2013-02-28  0.139999