chili
Synopsis

Simulation of slow-motional cw EPR spectra

chili(Sys,Exp)
spec = chili(...)
[B,spec] = chili(...)
... = chili(Sys,Exp,Opt)

See also the tutorial on how to use chili.

Description

chili computes cw EPR spectra of systems with one unpaired electron and one or more nuclei in the slow-motional regime.

Up to three input arguments are accepted:

If no input argument is given, a short help summary is shown (same as when typing help chili).

Up to two output arguments are returned:

If no output argument is given, chili plots the spectrum.

Sys is a structure containing the parameters of the spin system. Only S=1/2 systems are supported. Used parameters are g, gpa, Nucs, A, Apa. See the documentation on spin system structures for details. The nuclear quadrupole interaction is not included in the computation.

In addition, Sys collects values for dynamic parameters of the spin system. The following parameters are possible:

tcorr Rotational correlation time for isotropic rotational diffusion, in seconds. If tcorr is set, Diff is ignored.
For isotropic rotational motion, the correlation time tcorr and the diffusion rate Diff are related by tcorr = 1/(6*Diff).
For anisotropic rotational diffusion, use Diff or logDiff.
logtcorr Base-10 logarithm of the correlation time, offering an alternative way to input the correlation time. If given, tcorr is ignored.
Use this instead of tcorr for least-squares fitting with esfit.
Diff Rotational diffusion rates (principal values of the rotational diffusion tensor), in second-1.
  • One number: isotopic diffusion tensor
  • two numbers: input [Dxy Dzz] gives axial tensor [Dxy Dxy Dzz]
  • three numbers: rhombic tensor [Dxy Dxy Dzz]
Diff is ignored if tcorr is given.
logDiff Base-10 logarithm of Diff. If given, Diff is ignored.
Use this instead of Diff for least-squares fitting with esfit.
Diffpa 3-element vector
Euler angles describing the orientation of the rotational diffusion tensor in the molecular frame.
lw 1- or 2-element array of FWHM linewidths (all in mT).
  • 1 element: GaussianFWHM.
  • 2 elements: [GaussianFWHM LorentzianFWHM].
lambda An array of coefficients for the orienting potential, with up to five elements

  [lambda20 lambda22 lambda40 lambda42 lambda44],

corresponding to the five coefficients λ2,0, λ2,2, λ4,0, λ4,2, and λ4,4 (sometimes, the symbols c or ε are used instead in the literature).
If you give less than five numbers, the omitted ones are assumed to be zero. See the literature for details, esp. Earle/Budil 2006.
The frame of the ordering potential is collinear with that of the diffusion tensor.

Exchange Heisenberg spin exchange frequency, in Hz.

Exp contains the following experimental parameters.

mwFreqSpectrometer frequency in GHz
nPointsNumber of points along field axis (default 1024)
CenterSweep2-element vector [center sweep] with center field center and full field sweep range sweep, both in mT. If both CenterSweep and Range are not specified, the magnetic field range is automatically determined to cover the full spectral range.
Range2-element vector [minField maxField] with lower and upper limit of field scan range in mT. Range is only used if CenterSweep is not given. If both CenterSweep and Range are not specified, the magnetic field range is automatically determined to cover the full spectral range.
HarmonicDetection harmonic (0, 1 or 2), default is 1.
MOMD 1 or 0, depending on whether the MOMD model should be used.

If MOMD=1, spectra for a number of orientations are computed and added up. This is only needed if an orienting potential is present. The number of orientations is taken from Opt.nKnots.

If MOMD=0, or if MOMD is not given, only one single orientation is computed. The orientation is given by Exp.psi.

psi angle between magnetic field and director axis, in radians.

If given, it specifies the angle between the external magnetic field and the director axis (ie the principal axis of the orienting potential). This angle is often called the "director tilt".

If not given, zero is assumed.

If the MOMD model is used, psi is neglected.

Opt, the options structure, collects all settings relating to the algorithm used and the behaviour of the function. The following fields are available:

Verbosity 0 (default), 1
Determines how much information chili prints to the screen. If Opt.Verbosity=0, is is completely silent. 1 prints details about the progress of the computation.
LLKM 4-element vector [evenLmax oddLmax Kmax Mmax]
Specifies the basis size by giving the maximum values for, in that order, even L, odd L, M and K. M and K must be less than or equal to the maximum value of L.
If this field is not specified, chili sets the basis size automatically. This is adequate for most, but not all, cases.
nKnots Number of orientations used in a MOMD simulation (see Exp.MOMD). Default is 5. Increase this value if the orienting potential coefficients Sys.lambda are large.
Example

The cw EPR spectrum of a slow tumbling nitroxide radical can be simulated with the following lines.

Sys = struct('g',[2.008 2.0061 2.0027],'Nucs','14N','A',[16 16 86]);
Sys.tcorr = 1e-9;  % 1 ns
Exp = struct('mwFreq',9.5);
chili(Sys,Exp);
Algorithm

chili solves the Stochastic Liouville equation (SLE) in the eigenframe of the diffusion tensor and in an eigenbasis of the diffusion operator. The eigenfunctions are normalized Wigner rotation functions DLK,M(Ω) with -L≤K,M≤L. The number of basis functions is determined by maximum values of even L, odd L, K and M. The larger these values, the larger the basis and the more accurate the spectrum.

chili computes EPR line positions to first order. For the diffusion, both secular and nonsecular terms are included.

If the spin system contains more than one nucleus, only the first nucleus is included in the full SLE simulation. The effect of all the others is added by post-convolution: The isotropic stick spectrum due to all other nuclei is simulated and the used to convole the SLE-simulated spectrum of the first nucleus.

For full details of the algorithm see

See also

esfit, fastmotion, garlic