Find all positive integer $N$ such that for any infinite triangular grid with exactly $N$ black unit equilateral triangles, there exists an equilateral triangle $S$ whose sides align with grid lines such that there is exactly one black unit equilateral triangle outside of $S.$

(ltf0501)
1. **Define the Problem in Terms of \( n \)**:
   Replace \( N \) with \( n \) and call a number \( n \) *ngood* if there exists no such equilateral triangle satisfying all the given conditions and *good* otherwise.

2. **Claim**: For \( n > 3 \) and \( n \) even, \( n \) is ngood.
   - **Proof**:
     - Divide the plane into two parts via a line, say \( \ell \), which runs alongside grid lines. Assume this line to be horizontal.
     - Any unit triangle will lie on only one side of \( \ell \), either above or below.
     - Consider two black unit triangles, one with one side lying on this line \( \ell \), and the other, the reflected version along the same line \( \ell \). Call such a pair *nice* and a configuration having nice pairs only, as a *nice configuration*.

3. **Nice Configurations for Even \( n \)**:
   - Since \( n \) is even, consider nice configurations.
   - We want to show that we can't find an equilateral triangle \( \mathcal{S} \) satisfying the given properties.
   - Let \( p \) and \( q \) be the properties of lines which are \( 60^\circ \) and \( 120^\circ \) anti-clockwise rotated from \( \ell \), and let \( \mathbb{P} \) and \( \mathbb{Q} \) be their respective sets of such lines.
   - Select a line \( t \) from either \( \mathbb{P} \) or \( \mathbb{Q} \). Define *right shifting* or *left shifting* for \( t \) as moving it 1 step forward or backward respectively.
   - It suffices to show that there will always be \( >1 \) black triangle on either side of \( t \). Otherwise, we could choose a large enough triangle \( \mathcal{S} \) covering all but this alone triangle, where one side of \( \mathcal{S} \) will lie on \( t \).

4. **Shifting Algorithm**:
   - Take \( t \) from either the left side of the leftmost pair or the right side of the rightmost pair and begin shifting it right or left according to the need.
   - For \( t \) from the left side of the leftmost pair, shifting it right will always increase/decrease an even number of black triangles on either side of \( t \) due to our construction.
   - If we take 2 vertices of \( \mathcal{S} \) on \( t \) and the third one on either side of \( t \), we will always miss an even number of black triangles on one side of \( t \) and outside of \( \mathcal{S} \), forcing \( n \) to be *ngood*.
   - For \( t \) from the right side of the rightmost pair, the same argument works, forcing \( n \) to be *ngood*.

5. **Conclusion for Even \( n \)**:
   - This works for \( n \ge 4 \) (and even, obviously, due to assumption) because of the shifting algorithm.

6. **Claim**: For \( n \ge 5 \) and odd, \( n \) is ngood.
   - **Proof**:
     - Place \( \frac{n-1}{2} \) unit black triangles described earlier both above and below \( \ell \), and place 1 extra unit black triangle either above or below \( \ell \) and somewhere between those \( \frac{n-1}{2} \) unit black triangles recently chosen. Call this extra unit black triangle *special*.
     - There exists at least one nice pair on either side of this due to \( n \ge 5 \).
     - Applying the shifting algorithm, we will face no problem until we reach the special triangle from either side. Even then, we will have \( \ge 2 \) black triangles on either side, contrary to what we want, that is, one unit black triangle on one side.

7. **Conclusion for Odd \( n \)**:
   - We just need to check \( n \le 3 \).

8. **Check for Small \( n \)**:
   - For \( n = 1 \), it is trivially true.
   - For \( n = 2 \), we could choose one of the two unit black triangles, hence true.
   - For \( n = 3 \):
     - Let \( r \) be any line in any of \( \mathbb{P}, \mathbb{Q}, \mathbb{R} \). Here \( \mathbb{R} \) is the set of all horizontal lines.
     - Let \( r' \) be any other line in the same set. Call the two lines \( \{r, r'\} \), along with the space between them, a *slide* if \( r \) and \( r' \) are consecutive.
     - If all 3 unit triangles belong to different slides, the choice of \( \mathcal{S} \) is obvious.
     - If 2 of the 3 triangles are in the same slide, choose \( \mathcal{S} \) such that it contains those 2 triangles and its third vertex lies on the opposite side of the third triangle with respect to the slide containing 2 triangles.
     - If all 3 unit black triangles lie in the same slide, choose \( \mathcal{S} \) such that it covers either the first and second but not the third, or the second and third but not the first, exhausting all cases.

9. **Final Conclusion**:
   - The solution works for \( n = 1, 2, 3 \) only.

\(\blacksquare\)

The final answer is \( \boxed{ n = 1, 2, 3 } \)