IP Library Granted Patent US 12699033
Granted Patent B2
US 12699033 · App. 18/690,593 · Granted Aug 4, 2026

Light scattering detectors and methods for the same

Inventors: Sébastien Rouzeau (Publier, FR); David Thomas Gillespie (Pearland, TX)
Assignee: TOSOH BIOSCIENCE LLC
G01N15/0211G01N15/14G01N21/51G01N2015/1493G01N2021/4704
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Quick Facts
Patent No.
US 12699033
App. No.
18/690,593
Granted
Aug 4, 2026
Kind
B2
Abstract

Methods for determining an assumption-free radius of gyration of particles in solution using a light scattering detector are disclosed. The method may include determining a first weighting factor based on a first form factor. The method may also include determining a second weighting factor based on a second form factor. The method may further include determining a first form factor contribution for the first form factor based on the first weighting factor and the second weighting factor. The method may also include determining a second form factor contribution for the second form factor based on the first weighting factor and the second weighting factor. The method may also include determining the assumption-free radius of gyration from the first and second form factor contributions.

Claims (767)

1 . A method performed by a computer system for determining an assumption-free radius of gyration (Rg) of particles in solution using a light scattering detector, the method comprising:

obtaining, by the computer system, light scattering intensities of the particles in the solution from the light scattering detector, wherein the light scattering intensities comprise a first scattering intensity (I θ1 ), a second scattering intensity (I θ2 ), and a third scattering intensity (I θ3 ) of the particles in the solution at a first angle, a second angle, and a third angle, respectively, wherein the first angle, the second angle, and the third angle are determined relative to a beam of light of the light scattering detector;

determining, by the computer system, a first weighting factor (FW 1 ) based on a first form factor (FF 1 ) and the light scattering intensities, wherein determining the first weighting factor FW 1 ) comprises:

determining a ratio of observed light scattering of the particles at the first angle to observed light scattering of the particles at the third angle (R′ θ1/θ3 ) based on the first scattering intensity (I θ1 ) and the third scattering intensity (I θ3 );

determining a ratio of observed light scattering of the particles at the second angle to observed light scattering of the particles at the third angle (R′ θ2/θ3 ) based on the second scattering intensity (I θ2 ), and the third scattering intensity (I θ3 );

determining a ratio of calculated light scattering at the first angle to calculated light scattering at the third angle

(

R

θ

1

θ

3

Calculated

FF

1

)

 based on the first form factor (FF 1 ), the first angle, and the third angle;

determining a ratio of calculated light scattering at the second angle to the calculated light scattering at the third angle

(

R

θ

2

θ

3

Calculated

FF

1

)

 based on the first form factor (FF 1 ), the second angle, and the third angle;

determining a best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

1

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

1

)

 based on the first form factor (FF 1 ); and

determining, by the computer system, the first weight factor (FW 1 ) based on the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

1

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

1

)

;

determining, by the computer system, a second weighting factor (FW 2 ) based on a second form factor (FF 2 ) and the light scattering intensities, wherein determining the second weighting factor (FW 2 ) comprises:

determining a ratio of calculated light scattering at the first angle to calculated light scattering at the third angle

(

R

θ

1

θ

3

Calculated

FF

2

)

 based on the second form factor (FF 2 ), the first angle, and the third angle;

determining a ratio of calculated light scattering of the second angle to calculated light scattering at the third angle

(

R

θ

2

θ

3

Calculated

FF

2

)

 based on the second form factor (FF 2 ), the second angle, and the third angle;

determining a best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

2

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

2

)

 based on the second form factor (FF 2 ); and

determining, by the computer system, the second weight factor (FW 2 ) based on the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

2

)

and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

2

)

;

determining, by the computer system, a first form factor contribution (FC 1 ) for the first form factor (FF 1 ) based on the first weighting factor (FW 1 ) and the second weighting factor (FW 2 ), wherein the first form factor contribution (FC 1 ) is determined according to Equation (1):

FC

1

=

FW

1

FW

x

,

(

1

)

wherein ΣFW x is the sum of each of the weighting factors;

determining, by the computer system, a second form factor contribution (FC 2 ) for the second form factor (FF 2 ) based on the first weighting factor (FW 1 ) and the second weighting factor (FW 2 ), wherein the second form factor contribution (FC 2 ) is determined according to Equation (2):

FC

2

=

FW

2

FW

x

;

(

2

)

determining, by the computer system, the assumption-free radius of gyration (Rg) of the particles based on the first and second form factor contributions (FC 1 , FC 2 ); and

normalizing the light scattering detector based on the assumption-free radius of gyration (Rg).

2 . The method of claim 1 , wherein the first scattering intensity (I θ1 ), the second scattering intensity (I θ2 ), and the third scattering intensity (I θ3 ) are excess scattering intensities, and wherein the respective excess scattering intensities of each of the first, second, and third angles are normalized for quantum efficiency, gains, geometric volume, or a combination thereof.

3 . The method of claim 1 , wherein determining the best fit comprises an iterative process.

4 . The method of claim 1 , wherein determining the first weighting factor (FW 1 ) further comprises determining a radius of gyration (Rg 1 ), based on the first form factor (FF 1 ), associated with the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

1

)

and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

1

)

.

5 . The method of claim 4 , wherein the determining the radius of gyration (Rg 1 ) associated with the best fit comprises determining the radius of gyration (Rg 1 ), based on the first form factor (FF 1 ), associated with a minimum sum of squares residual (SSR 1 ) of a difference between the ratio (R′ θ1/θ3 ) and the ratio

(

R

θ

1

θ

3

Calculated

FF

1

)

and a difference between the ratio (R′ θ2/θ3 ) and the ratio

(

R

θ

2

θ

3

Calculated

FF

1

)

.

6 . The method of claim 5 , wherein determining the second weighting factor (FW 2 ) further comprises determining a radius of gyration (Rg 2 ), based on the second form factor (FF 2 ), associated with the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

2

)

and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

2

)

.

7 . The method of claim 6 , wherein the determining the radius of gyration (Rg 2 ) associated with the best fit comprises determining the radius of gyration (Rg 2 ), based on the second form factor (FF 2 ), associated with a minimum sum of squares residual (SSR 2 ) of a difference between the ratio (R′ θ1/θ3 ) and the ratio

(

R

θ

1

θ

3

Calculated

FF

2

)

and a difference between the ratio (R′ θ2/θ3 ) and the ratio

(

R

θ

2

θ

3

Calculated

FF

2

)

.

8 . The method of claim 7 , wherein the first weighting factor (FW 1 ) is based on the minimum sum of squares residual (SSR 1 ), the second weighting factor (FW 2 ) is based on the minimum sum of squares residual (SSR 2 ), or a combination thereof.

9 . The method of claim 1 , wherein one or more of the first form factor (FF 1 ), the second form factor (FF 2 ), or a combination thereof is a form factor for a homogenous rigid particle, and wherein the form factor for the homogenous rigid particle is one of: a homogenous sphere, a spherical shell, a spherical concentric shell, particles of spherical subunits, an ellipsoid of revolution, a tri-axial ellipsoid, a cube and rectangular parallelepipedon, a truncated octahedra, a faceted sphere, a lens, a cube with terraces, a cylinder, a cylinder with an elliptical cross section, a cylinder with hemi-spherical endcaps, a cylinder with half lens end caps, a toroid, an infinitely thin rod, an infinitely thin circular disk, or a fractal aggregate.

10 . The method of claim 1 , wherein one or more of the first form factor (FF 1 ), the second form factor (FF 2 ), or a combination thereof is a form factor for a polymer model, and wherein the form factor for the polymer model is one of: a spherical particle form factor, a rodlike particle form factor, a random coil particle form factor, or a combination thereof.

11 . The method of claim 1 , wherein:

the light scattering detector comprises a multi-angle light scattering detector;

the particles in solution comprise monodispersed particles;

the light scattering detector comprises a goniometer configured to observe light scattering at two or more angles;

the particles in solution comprise polydispersed particles; and/or

the assumption-free radius of gyration (Rg) of the particles is from about 5 nm to about 500 nm, from about 30 to about 250 nm, or from about 50 to about 150 nm.

12 . The method of claim 1 , wherein the first angle is about 90° relative to the beam of light of the detector, the second angle is about 170° relative to the beam of light of the detector, and the third angle is about 10° relative to the beam of light of the detector.

13 . The method of claim 1 , further comprising:

determining a third weighting factor (FW 3 ) based on a third form factor (FF 3 );

determining a third form factor contribution (FC 3 ) for the third form factor (FF 3 ) based on the all the weighting factors (FW i ); and

determining the assumption-free radius of gyration (Rg) from the first, second, and third form factor contributions (FC 1 , FC 2 , FC 3 ).

14 . The method of claim 1 , wherein the method does not comprise one or more of:

determining a molecular weight of the particles in solution prior to determining the assumption-free radius of gyration (Rg); and

fitting a Zimm, Berry, Debye, or Guinier plot to a polynomial function.

15 . The method of claim 1 , further comprising implementing a rejection criteria to determine a corrected assumption-free radius of gyration, wherein the rejection criteria is based on one of: a respective minimum sum of squares residual, respective a minimum sum of squares squared, or respective a minimum sum of squares absolute for each of the form factors.

16 . A method for determining a molecular weight of the particles in solution of claim 1 , the method comprising determining the molecular weight of the particles in solution based on the assumption-free radius of gyration (Rg).

17 . A method performed by a computer system for determining one or more properties of composite particles in solution, the method comprising:

obtaining, by the computer system, light scattering intensities of the particles in the solution from the light scattering detector, wherein the light scattering intensities comprise a first scattering intensity (I θ1 ), a second scattering intensity (I θ2 ), and a third scattering intensity (I θ3 ) of the particles in the solution at a first angle, a second angle, and a third angle, respectively, wherein the first angle, the second angle, and the third angle are determined relative to a beam of light of the light scattering detector;

determining, by the computer system, a first weighting factor (FW 1 ) based on a first form factor (FF 1 ) and the light scattering intensities, wherein determining the first weighting factor (FW 1 ) comprises:

determining a ratio of observed light scattering of the particles at the first angle to observed light scattering of the particles at the third angle (R′ θ1/θ2 ) based on the first scattering intensity (I θ1 ) and the third scattering intensity (I θ3 );

determining a ratio of observed light scattering of the particles at the second angle to observed light scattering of the particles at the third angle (R′ θ2/θ3 ) based on the second scattering intensity (I θ2 ), and the third scattering intensity (I θ3 ); and

determining a ratio of calculated light scattering at the first angle to calculated light scattering at the third angle

(

R

θ

1

θ

3

Calculated

FF

1

)

,

 based on the first form factor (FF 1 ), the first angle, and the third angle;

determining, by the computer system, a second weighting factor (FW 2 ) based on a second form factor (FF 2 ) and the light scattering intensities, wherein determining the second weighting factor (FW 2 ) comprises:

determining a ratio of calculated light scattering at the first angle to calculated light scattering at the third angle

(

R

θ

1

θ

3

Calculated

FF

2

)

 based on the second form factor (FF 2 ), the first angle, and the third angle;

determining a ratio of calculated light scattering of the second angle to calculated light scattering at the third angle

(

R

θ

2

θ

3

Calculated

FF

2

)

 based on the second form factor (FF 2 ), the second angle, and the third angle;

determining a best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

2

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

2

)

 based on the second form factor (FF 2 );

determining the second weight factor (FW 2 ) based on the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ

1

θ

3

Calculated

FF

2

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ

2

θ

3

Calculated

FF

2

)

;

determining, by the computer system, a first form factor contribution (FC 1 ) for the first form factor (FF 1 ) based on the first weighting factor (FW 1 ) and the second weighting factor (FW 2 ), wherein the first form factor contribution (FC 1 ) is determined according to Equation (1):

FC

1

=

FW

1

FW

x

,

(

1

)

wherein ΣFW x is the sum of each of the weighting factors;

determining, by the computer system, a second form factor contribution (FC 2 ) for the second form factor (FF 2 ) based on the first weighting factor (FW 1 ) and the second weighting factor (FW 2 ), wherein the second form factor contribution (FC 2 ) is determined according to Equation (2):

FC

2

=

FW

2

FW

x

;

(

2

)

determining, by the computer system, the one or more properties of the composite particles based on the first form factor contribution (FC 1 ) and the second form factor contribution (FC 2 ); and

generating an output, on a display, a readout, a report, or a disk storage of the computer system, based on the one or more properties of the composite particles.

18 . The method of claim 17 , wherein the one or more properties comprise structural features, substructures, or combinations thereof, and/or wherein the composite particles in solution comprise branched particles.

19 . A non-transitory computer-readable medium storing instructions that, when executed by one or more processors of a computing system, cause the computing system to perform operations for determining an assumption-free radius of gyration (Rg) of particles in solution using a light scattering detector, the operations comprising:

obtaining, by the computing system, light scattering intensities of the particles in the solution from the light scattering detector, wherein the light scattering intensities comprise a first scattering intensity (I θ1 ), a second scattering intensity (I θ2 ), and a third scattering intensity (I θ3 ) of the particles in the solution at a first angle, a second angle, and a third angle, respectively, wherein the first angle, the second angle, and the third angle are determined relative to a beam of light of the light scattering detector;

determining, by the computing system, a first weighting factor (FW 1 ) based on a first form factor (FF 1 ) and the light scattering intensities, wherein determining the first weighting factor (FW 1 ) comprises:

determining a ratio of observed light scattering of the particles at the first angle to observed light scattering of the particles at the third angle (R′ θ1/θ3 ) based on the first scattering intensity (I θ1 ) and the third scattering intensity (I θ3 );

determining a ratio of observed light scattering of the particles at the second angle to observed light scattering of the particles at the third angle (R′ θ2/θ3 ) based on the second scattering intensity (I θ2 ), and the third scattering intensity (I θ3 );

determining a ratio of calculated light scattering at the first angle to calculated light scattering at the third angle

(

R

θ1

θ3

Calculated

FF

1

)

 based on the first form factor (FF 1 ), the first angle, and the third angle;

determining a ratio of calculated light scattering at the second angle to the calculated light scattering at the third angle

(

R

θ2

θ3

Calculated

FF

1

)

 based on the first form factor (FF 1 ), the second angle, and the third angle;

determining a best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ1

θ3

Calculated

FF

1

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ2

θ3

Calculated

FF

1

)

 based on the first form factor (FF 1 ); and

determining, by the computing system, the first weight factor (FW 1 ) based on the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ1

θ3

Calculated

FF

1

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ2

θ3

Calculated

FF

1

)

;

determining, by the computing system, a second weighting factor (FW 2 ) based on a second form factor (FF 2 ) and the light scattering intensities, wherein determining the second weighting factor (FW 2 ) comprises:

determining a ratio of calculated light scattering at the first angle to calculated light scattering at the third angle

(

R

θ1

θ3

Calculated

FF

2

)

 based on the second form factor (FF 2 ), the first angle, and the third angle;

determining a ratio of calculated light scattering of the second angle to calculated light scattering at the third angle

(

R

θ2

θ3

Calculated

FF

2

)

 based on the form factor (FF 2 ), the second angle, and the third angle;

determining a best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ1

θ3

Calculated

FF

2

)

 and the ratio (R′ θ2/θ3 ) to the ratio

(

R

θ2

θ3

Calculated

FF

2

)

 based on the second form factor (FF 2 ); and

determining, by the computing system, the second weight factor (FW 2 ) based on the best fit of the ratio (R′ θ1/θ3 ) to the ratio

(

R

θ1

θ3

Calculated

FF

2

)

 and the ratio (R′ θ2/θ2 ) to the ratio

(

R

θ2

θ3

Calculated

FF

2

)

determining, by the computing system, a first form factor contribution (FC 1 ) for the first form factor (FF 1 ) based on the first weighting factor (FW 1 ) and the second weighting factor (FW 2 ), wherein the first form factor contribution (FC 1 ) is determined according to Equation (1):

FC

1

=

FW

1

FW

x

,

(

1

)

wherein μFW x is the sum of each of the weighting factors;

determining, by the computing system, a second form factor contribution (FC 2 ) for the second form factor (FF 2 ) based on the first weighting factor (FW 1 ) and the second weighting factor

FC

2

=

FW

2

FW

x

;

(

2

)

determining, by the computing system, the assumption-free radius of gyration (Rg) of the particles based on the first and second form factor contributions (FC 1 , FC 2 ); and

normalizing the light scattering detector based on the assumption-free radius of gyration (Rg).