1. 1 A Fast-Nonegativity-Constrained Least Squares Algorithm R. Bro, S. D. Jong J. Chemometrics,11,393-401, 1997 By : Maryam Khoshkam

2. 2 Introduction Introduction Algorithm of classical non-negative least square (nnls) Algorithm of classical non-negative least square (nnls) A numerical example A numerical example Fast nonegative least square (Fnnls) Fast nonegative least square (Fnnls) Results and discussion Results and discussion

3. 3 introduction Estimation of models subject to non-negativity constraints is of practical importance in chemistry. The time required for estimating true least squares non- negativity constrained model is typicaly many times longer than for estimating unconstrained model. Approximations procedures Unconstrained estimation+ Setting negative value to zero What is the problem of force to zero algorithm????

4. 4 1.There is no guarantee whatsoever for the quality of the model. 2.When included in multiway algorithm, it can cause the algorithm to diverge. (specially, in noisy data or difficult models) Non-negativity constrained linear least square

5. 5 NNLS NNLS will be stated using the following nomenclature: For all m Lawson, C.L. and R.J. Hanson, Solving Least-Squares Problems, Prentice- Hall, Chapter 23, p. 161, 1974. lsqnonneg command in MATLAB is based on this algorithm

6. 6 Some important aspects of the algorithm This is an active set algorithm. Thus the nnls first find the true passive and active sets, then perform the least square on corresponding columns of Z. HOW…???? First of all, it suppose that all elements of d, are in active set. R={1,2,….,M} P={} If the all elements of d are active, estimate that how the form of initial d….?????

7. 7 Initial solution vector d is feasible and set equal to a M×1 zero vector Using the vector w Then it removes the passive sets elements of d, one by one, and STEP by STEP HOW…????

8. 8 w=Z T ( x – Z d ) One necessary condition for optimally of a solution, is that the derivatives with respect to the parameters of the passive set be zero. WHY ?? How is the f ’ (d m ) if m is an active set ????

9. 9 Thus at optimal solution, we expect that: When we are being at optimal condition, w m >0. wht is the meaning of positive value for w m ?

10. 10 positive w m shows that by increasing d m to a more positive value, the change in residual is negative (f ', which is the slope is negative). It means that the residual becomes less, and more close to zero, when d m goes toward positive.

11. 11 Algorithm nnls 1.P=Ø 2.R={1,2,…,M} 3.d=0 4.w=Z T (x-Zd) loop A No Opt. sol. Of d yes P={m} & R=R-{m} S P =[(Z P ) T Z P ] -1 (Z P ) T x No d=s w=Z T (x-Zd) yes Loop C all s p >0 Loop B Build s p

12. 12 A simple numerical example loop A Max(w n )>1e-15 & R≠Ø Loop B

13. 13 Loop B No Max(w n )>1e-15 & R≠Ø Opt. sol. Of d

14. 14 Graphical representation of nonlinear least square algorithm: H 3 A ↔ H + + H 2 A - pk a1 =2.6 H 2 A - ↔ H + + HA 2- pk a2 =4.0 HA 2- ↔ H + + A 3- pk a3 =6.3 D=X +. Z (ILS) Z D X

15. 15 X (10x100) = Z (10x4) D (4x100) x 10x1 =X(:,1) Step1 d (4x1) w 0.005 x D(:,1) 1)P=[]; 2)R={1,2,3,4}

16. 16 Force to zero nnls Variation of w during nonnegative least square

17. 17 Residual matrix w w=Z T (x-Zd) = w (4×1) r (10x1) Z (10x4) T w i in each λ, is the contribution of ith species in in residual vector in each λ.

18. 18 Why it is necessary to modify the NNLS algorithm?

19. 19 PARAFAC-ALS I J K Least square

20. 20 If the size of X is 10x200x5 in a 3 component system, the size of Z is: 500x3 And so on…. Computation of Z, can be computationally costly for large arrayes Excessive memory is required to calculate X (IxJK), X (JxIK) and X (K,IJ)

21. 21 And in similar way for estimation of B and C

22. 22 Nnls can not used for this simplified version of PARAFAc, Why??

23. 23 In estimating A, and using non-negativity constraint on it, A (IxF) X (IxJK) Z = SLOW!!!!!!!  A modification…

24. 24 Fast non-negativity least square 1. Accept the cross product (xZ and Z’Z) instead of the row data w=Z T ( x – Z d )  w=Z T x – (Z T Z)d S P =[(Z P ) T Z P ] -1 (Z P ) T x  S P =[(Z T Z) P ] -1 (Z T x) 2. Set the passive and active variables, before enter to loop B d is not the zero vector in this case

25. 25 Thanks

26. 26 Ex. d=Z\xd=Z\x Force to zero RMS=103 nnlsq RMS=20

27. 27 3th element of d In unconstrained solution of d, the mth negative element is active set In constrained solution of d, the mth zero element is active set 2th and 3th elements of d What happen if the true active set is known? Thus it is not possible to realize the true active set form unconstraint least square solution.

28. 28 For example, if we know that 2th and 3th elements of d are true active sets, Then perform the simple unconstrained least square with the 1 st column of Z. (columns corresponding to passive sets. selectivity constraint !!!! NOTE!!!!! 1) 2) f(d) minimized by columns of Z corresponding to passive sets. Thus active sets which for them, d m =0, is not take a part in minimizing the residuals

29. 29 Loop C Update R and P S P =[(Z P ) T Z P ] -1 (Z P ) T x 1) 2) 3) 4) SR=0SR=0 5)