1

Predicted properties in an unknown comes with an error. Therefore we should

have:
QR = Q̂ + s(x? ) (1)
where Q is the charge the superscript R means that is the real value, Q̂ is the pre-
dicted value ans s(x? ) is the error on the unknown position x? . The error is given
by the square root of the MSE (Mean Squared Error):
√
s(x? ) = MS E (2)
where   2 
 1 − rT R−1 r 
MS E = s(x? )2 = σ2 1 − rT R−1 r + (3)
 
 1T R−1 1 
Derivative of the property (using the notation in Mills and Popelier (JCTC
2014)) can be calculated as:
∂QT ∂Q̂ ∂s
Ω
= Ω+ Ω (4)
∂αi ∂αi ∂αi
Derivative of Q̂ is described in the paper, we derive derivative of s which can be
written as:
Nf
∂s X ∂s ∂ fk
= (5)
∂αiΩ
k=1
∂ fk ∂αΩ
i

the only unknown term is ∂∂sfk . Derivative of s with respect the features can be
written as:
 
rT R−1 r ∂rT
 !
∂s  ∂rT ∂r T −1 ∂r 
= −σ 
2 
R r+r R
−1 T −1
+ 2 T −1 R r+r R
−1

∂ fk ∂ fk ∂ fk 1 R 1 ∂ fk ∂ fk 

  T −1   !
 r R r  ∂rT ∂r
= −σ2 2 T −1 + 1 R−1 r + rT R−1

(6)
∂ fk ∂ fk 

1 R 1
Force can be written as:
    
X  ∂ Q̂A + sA  ∂T AB ∂ Q̂B + sB 
FiΩ =
  

Ω
T AB Q̂B + sB + Q̂A + sA Ω
(Q̂B + sB ) + (Q̂A + sA )T AB Ω

AB
 ∂α i ∂α i ∂α i

(7)
which results in:
   
∂ Q̂A + sA ∂ Q̂B + sB
A ∂T AB
   
T AB Q̂ + s + Q̂ + s
B B A
(Q̂ + s ) + (Q̂ + s )T AB
B B A A
∂αΩ
i ∂αΩ
i ∂αΩ
i
   
∂ Q̂A   ∂ sA  
= T AB Q̂B + sB + Ω AB
T Q̂B + sB
∂αΩi ∂α i
   
  ∂T AB ∂ Q̂B ∂ sB
+ Q̂A + sA (Q̂B + sB ) + (Q̂A + sA )T AB + (Q̂A + sA )T AB (8)
∂αΩi ∂α Ω
i ∂αΩi