METHOD AND SYSTEM FOR CALIBRATING A CHARGED-PARTICLE SPECTROMETER
20260088248 ยท 2026-03-26
Assignee
- Centre National De La Recherche Scientifique (Paris, FR)
- UNIVERSITE PARIS-SACLAY (Gif-Sur-Yvette, FR)
Inventors
- Luiz GALVAO TIZEI (BOURG-LA-REINE, FR)
- Yves AUAD (PARIS, FR)
- Jean-Denis BLAZIT (FORGES-LES-BAINS, FR)
- Marcel TENCE (ISSY-LES-MOULINEAUX, FR)
- Mathieu Kociak (Palaiseau, FR)
Cpc classification
H01J37/244
ELECTRICITY
International classification
Abstract
A method for calibrating a charged-particle spectrometer including generating a monochromatic incident charged-particle beam having a first energy; generating an incident laser beam having a second energy; illuminating a surface with the laser beam to generate an evanescent electromagnetic field in a region near the surface; spatially and temporally superimposing the laser beam and the incident charged-particle beam in the region to couple them via the evanescent electromagnetic field by generating a charged-particle beam as an output beam with a spectrum having distinct peaks of energies that are spectrally separated by a value equal to the second energy; measuring, by the spectrometer, all or part of the spectrum of the output beam, then determining a variation in energy of at least two of the distinct energy peaks with respect to the first energy; and determining a value of the scale factor S and a value of the offset.
Claims
1-14. (canceled)
15. A method of calibrating a spectrometer for charged particles comprising the following steps: A. generating a monochromatic incident charged particle beam having a first energy E.sub.1; B. generating an incident laser beam having a second energy E.sub.2; C. illuminating a surface of a sample with the incident laser beam to generate an evanescent electromagnetic field in a region in the vicinity of said surface; D. spatially and temporally superimposing the incident laser beam and the incident charged particle beam in said region in order to couple them via said evanescent electromagnetic field, generating a charged particle beam known as an output beam having a spectrum comprising a plurality of distinct energy peaks spectrally separated by a value equal to the second energy E.sub.2; E. measuring, using the spectrometer, all or part of the spectrum of the output beam, then determining a variation in energy E of at least two of the distinct energy peaks with respect to the first energy E.sub.1; F. determining a value of the scale factor S and a value of the offset O specific to said measurement of the spectrum of the output beam by the spectrometer from the energy variations E.
16. The method according to claim 15, wherein said variation in energy E of each of the at least two distinct energy peaks is equal to E=pE.sub.2, with p a positive or zero integer equal to a number of inter-peak intervals separating said distinct energy peak from the peak of the spectrum at the first energy E.sub.1 and wherein said variation in energy E of each of the at least two distinct energy peaks is determined in step E by the spectrometer by the following relation, referred to as the first equation:
17. The method according to claim 16, wherein it is determined that said non-linearities undergone by the charged particles are weak or zero, and, in step E, the variation in energy E of two of the distinct energy peaks, numbered by the index 1 and 2 respectively via the first equation is determined so as to obtain the following first system:
18. The method according to claim 17, wherein an integer m>1 of inter-peak intervals separating said two peaks for which the variation in energy E is determined is such that an error on the determination of the scale factor value is less than or equal to 1% of the second energy.
19. The method according to claim 16, wherein it is determined that the non-linearities undergone by said charged particles are not weak or zero and, in step E, the variation in energy E of a number N>2 of distinct energy peaks each numbered by an index i[1; M] is determined via the first equation so as to obtain the following second system:
20. The method according to claim 19, comprising a step subsequent to step F consisting in iteratively minimizing the values of the NL function by repeating steps A to F a plurality of times and modifying parameters of the path and detection of charged particles between each iteration.
21. The method according to claim 15, wherein step D further comprises a sub-step consisting in measuring a spectrum of the incident laser beam simultaneously with the generation of the output beam, the determination of the value of the scale factor S and the value of the offset O being performed from said measurement of the spectrum of the incident laser beam.
22. A system for calibrating a spectrometer for charged particles, said system comprising: a charged particle source adapted to generate a monochromatic incident charged particle beam having a first energy E.sub.1; a laser source adapted to generate an incident laser beam having a second energy E.sub.2; an optical and charged particle transport assembly adapted for: illuminating a surface of a sample with the incident laser beam to generate an evanescent electromagnetic field in a region in the vicinity of said surface: spatially and temporally superimposing the incident laser beam and the incident charged particle beam in said region in order to couple them via said evanescent electromagnetic field so as to generate a charged particle beam known as an output beam having a spectrum comprising a plurality of distinct energy peaks spectrally separated by a value equal to the second energy E.sub.2; said spectrometer being adapted to measure all or part of the spectrum of the output beam, said system further comprising a processor connected to the spectrometer and adapted for: determining a variation in energy E of at least two of the distinct energy peaks with respect to the first energy E.sub.1; determining a value of the scale factor S and a value of the offset O specific to said measurement of the spectrum of the output beam by the spectrometer from the energy variations E.
23. The system according to claim 22, wherein the incident laser beam is a continuous beam or a pulsed beam with a spectral width of less than 40 meV.
24. The system according to claim 22, comprising an additional optical spectrometer adapted to measure a spectrum of the incident laser beam simultaneously with the generation of the output beam, the processor also being connected to the additional spectrometer so that the determination of the value of the scale factor S and the value of the offset O is effected from said measurement of the spectrum of the incident laser beam.
25. The system according to claim 22, wherein the laser source and transport assembly are adapted so that the incident laser beam has an intensity greater than or equal to 10.sup.8 W/cm.sup.2 in said region.
26. The system according to claim 22, wherein the laser source and transport assembly are adapted so that the incident laser beam is polarized in a direction adapted to the geometry and the symmetry of the sample in order to locally maximize the intensity of the evanescent field in said region.
27. The system according to claim 22, wherein said transport assembly comprises an off-axis parabola adapted to focus the incident laser beam onto said surface of the sample, said parabola having an aperture through which the incident charged particle beam passes so that it co-propagates with the incident laser beam towards said region after the latter has reflected off said off-axis parabola.
28. The system according to claim 22, comprising a resonant optical cavity for the incident laser beam wherein the sample is arranged, said transport assembly and said optical cavity being further adapted so that the incident laser beam makes a plurality of reflections in the optical cavity as it passes through said region.
Description
BRIEF DESCRIPTION OF THE FIGURES
[0046] Further features, details and advantages of the invention will become apparent upon reading the description made with reference to the appended drawings given by way of example and which show, respectively:
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[0057] In the figures, unless otherwise indicated, elements are not to scale.
DETAILED DESCRIPTION
[0058]
[0059]
[0060] In a step A of the method of the invention, the charged particle source SP generates an incident charged particle beam FP. The source SP is adapted so that the beam FP is monochromatic and has a first energy E.sub.1. Monochromatic here means that the beam FP has the first energy E.sub.1 <0.1%
[0061] In a step B, the laser source SL generates an incident laser beam FL with a second energy E.sub.2=.sub.2, where .sub.2 is the center frequency of the incident laser beam. According to one embodiment, the laser source SL delivers a pulsed beam. Alternatively, in another embodiment, the laser source SL delivers a continuous beam. As will be explained later, the pulse durationvia spectral widthhas a direct influence on the accuracy of scale factor S and offset O determination.
[0062] The sources SL and SP are configured so that the beams FL and FP are directed towards the transport assembly SO.
[0063] In a step C, the transport assembly SO directs the incident laser beam FL so that it illuminates a surface SF of the sample Ech so as to generate an evanescent electromagnetic field EV in a region R close to the surface SF.
[0064] For illustrative purposes only,
[0065] The sample of the invention can take any form known to a person skilled in the art enabling the generation of the evanescent field EV by laser illumination. By way of non-limiting example, the sample is a metal surface, a metal nanotube, a metal nanowire, a nanosphere, an optical fiber, a ring-fiber cavity, a waveguide or, more generally, an optical cavity.
[0066] In a step D, the transport assembly SO spatially and temporally superimposes the incident laser beam FL and the incident charged particle beam FP in the region R. This superposition enables coupling between the beams FL and FP via the evanescent field EV. This coupling consists in the absorption or emission, by the charged particles, of photons from the laser beam FL and enables the generation of a charged particle beam (called the output beam FS) presenting a spectrum comprising a plurality of distinct energy peaks separated spectrally by a value equal to the second energy E.sub.2.
[0067] This coupling mechanism is known to those skilled in the art and is described for photon/electron interaction in Barwick, B., Flannigan, D. J., & Zewail, A. H. (2009). Photon-induced near-field electron microscopy. Nature, 462 (7275), 902-906. This phenomenon is a non-linear mechanism in which a charged particle of the beam FP of initial energy E.sub.1 absorbs or emits n1 photons so as to gain or lose an energy equal to a multiple of the energy E.sub.2 of a photon in the laser beam FL. After this interaction, the energy of the charged particle is therefore E.sub.1=E.sub.1nE.sub.2 with E.sub.1 the energy of the charged particle in the output beam FS.
[0068] As a result of this photon/charged particle interaction, the output beam FS therefore has an energy spectrum comprising a plurality of distinct energy peaks at energies E.sub.1=E.sub.1nE.sub.2 (n1) and at an energy E.sub.1 (the so-called ZLP peak). In the following, for ease of notation, the output beam FS will be said to have an energy spectrum comprising a plurality of distinct energy peaks at energies E.sub.1=E.sub.1pE.sub.2 (p integer greater than or equal to 0).
[0069] In step E, the output beam is directed into the spectrometer SM, which measures all or part of the spectrum of the output beam FS. More precisely, the spectrometer measures an energy loss spectrum of the output beam FS. In the invention, it is essential that the measured part of the output beam FS spectrum includes at least two of the distinct energy peaks in order to be able to determine the scale factor S and the offset O (see below).
[0070]
[0071] The system further comprises a processor UT connected to the spectrometer SM and adapted to determine an energy variation E of at least two of the distinct energy peaks relative to the first energy E.sub.1. That is, the processor selects at least two peaks from the measured spectrum, each at an energy E.sub.1=E.sub.1pE.sub.2, then calculates E=E.sub.1E.sub.1=pE.sub.2. The peaks selected for calculating the energy variation E are not necessarily different from the spectrum peak at energy E.sub.1. The processor can therefore select the ZLP peak and a peak with a specific energy E.sub.1=E.sub.1nE.sub.2 (n1).
[0072] We note m the number of inter-peak intervals separating the two selected peaks, and note Em the energy separating them.
[0073] In a final step F, the processor determines the value of the scale factor S and the offset value O specific to the spectrometer SM from these energy variations E. In fact, as is well known, energy variations E are determined in step E by the spectrometer and processor via the following relationship, referred to as the first equation:
[0075] The term spectrometer matrix detector channel is used here to refer to the pixel row or sub-row (or column or sub-column, depending on detector orientation) where the distinct energy peak is detected.
[0076] The invention comprises two distinct embodiments, a first embodiment where only the value of the scale factor S and the offset value O (linear error) are determined, and a second embodiment where the value of the scale factor S and the offset value O are determined and the NL function (the non-linear error) is extrapolated (see
[0077] According to the first embodiment of the invention, the processor determines that the non-linearities experienced by the charged particles as they travel and are detected are low or zero. For example, the processor determines that the values cS+O are much higher than the values NL(c). Much higher means that the values cS+O are more than ten times the values NL(c). In the first embodiment, step E consists in determining the energy variation E of two of the distinct energy peaks, numbered by index 1 and 2, respectively, via the first equation so as to obtain the following first system (S1):
[0079] We then have a first system (S1) of two equations with two unknowns. Step F of the first embodiment then consists in solving the first equation system (S1) to determine the value of the scale factor S and the value of the offset O.
[0080] Let us consider two distinct energy peaks separated by a number of inter-peak intervals equal to m and separated by an energy E.sub.m. Let d be the number of channels separating two adjacent distinct energy peaks on the spectrometer matrix detector. Adjacent distinct energy peaks means energy peaks separated by an energy equal to E.sub.2. The two selected peaks are separated by a number of channels md on the matrix detector.
We then have:
[0081] Let E.sub.m be the precision of the energy value E.sub.m separating the two distinct energy peaks and let d.sub.m be the accuracy of determining the number of channels separating the two distinct energy peaks on the matrix detector. The accuracy E.sub.m is equal to the precision of the photon energy of the laser beam FL emitted by the source SL. This precision is the spectral width LS of the laser beam FL
[0082] In addition, we consider that precision d.sub.m is equal to the detector pixel pitch d.
[0083] The determination precision of S is then:
[0084] Defining S.sub.m=S/m, we have:
[0085] It is observed that the value of the precision on the determination of S is inversely proportional to the number of inter-peak intervals m and is equal to S.sub.m=S/m as E.sub.m=LS and as d.sub.m=d.
[0086] Two important conclusions can be drawn from these calculations: [0087] A. the method of the invention according to the first embodiment of the invention allows a determination of the value of the scale factor S and the offset value O with an error limited by the spectral width LS of the laser beam, [0088] B. in order to improve precision in determining S, it is necessary to measure peaks with a larger number of inter-peak intervals m.
[0089] The calibration method of the invention makes it possible to determine a value for the scale factor S with an accuracy S of the order of 0.01% or less of the energy E.sub.2 of the laser beam FL, even when measuring the energy variation E with two distinct energy peaks having a number of inter-peak intervals m equal to 1. For example, with commercial lasers and optical spectrometers, an accuracy of S of 30 eV for an energy E.sub.2=2 eV (that is, 620 nm wavelength) is achievable using a laser source SL with a spectral width of 10 pm. An improved precision S can be achieved by using a laser with better spectral resolution. At present, even a precision of 0.001% of the energy E.sub.2 for the scale factor S and for the offset O is already two orders of magnitude higher than the spectral resolution of state-of-the-art electronic spectrometers.
[0090] According to a preferred embodiment of the invention, the incident laser beam is a continuous beam or a pulsed beam with a spectral width of less than 40 meV. Thus, by adapting the detection of the spectrometer SM, it is possible to determine the value of the scale factor S with an accuracy S less than or equal to 0.01% of the energy E.sub.2.
[0091] In one embodiment, the laser source SL is a femtosecond laser with a spectral width of LS=40 meV and the matrix detector of the spectrometer SM has 1000 channels and a dispersion of 20 meV/channel. By measuring the energy variation E with two distinct energy peaks with a number of inter-peak intervals m equal to 5, the value of the scale factor S is determined with an accuracy of
or an accuracy S equal to 0.01% of the energy E.sub.2.
[0092] More generally, according to a preferred embodiment of the invention, for a fixed spectral width LS, the spectrometer SM is adapted so that the number of inter-peak intervals m separating the two peaks for which the energy variation E is determined is such that S is less than or equal to 1% of the second energy E.sub.2, preferentially less than 0.01% of the second energy E.sub.2.
[0093] It has been shown that the probability of the photon/charged particle interaction giving rise to the distinct energy peaks is proportional to the strength of the evanescent field EV (F. Javier Garcia de Abajo et al., Nano Letters, 10, 1859 (2010)). In addition, in a known manner, the detection sensitivity of the spectrometer SM is limited by the background noise generated by a number of factors. Thus, according to a preferred embodiment of the invention, the laser source SL and the transport assembly SO are adapted so that the incident laser beam has an intensity greater than or equal to 10.sup.8 W/cm.sup.2 in the region R. This intensity makes it possible to generate an evanescent field EV with an intensity sufficiently high for the rate of photon/charged particle interaction to be sufficiently high to generate a plurality of energy peaks in the output beam FS sufficiently intense to enable their detection by the spectrometer SM. Increasing the intensity of the incident laser beam in the R region will therefore enable the detection of a greater number of distinct peaks in the spectrum of the output beam, thus improving the accuracy of the scaling factor determination S and offset 0 by selecting a number of inter-peak intervals m in step E.
[0094] In the embodiment shown in
[0095] Although this arrangement is preferred, it is understood that other transport devices for the beams FL and FP may be used by those skilled in the art to form the transport assembly SO. Thus, according to another embodiment, the transport assembly SO comprises one or more mirrors and/or one or more lenses and/or a fiber coupling.
[0096] In order to more easily control the temporal superposition of the beams FL and FP, according to one embodiment of the invention, the system 1 comprises a delay line arranged in the optical path of the laser beam FL.
[0097] Preferentially, the laser source and transport assembly are adapted so that the incident laser beam is polarized in a direction substantially adapted to the geometry and symmetry of the sample, in order to locally maximize the evanescent field EV intensity in the region R. For example, when the sample is a nanotube or nanowire, polarization in a direction substantially parallel to the longitudinal axis of the nanotube or nanowire maximizes the intensity of the evanescent field EV in the region R.
[0098]
[0099]
[0100] Preferentially, the cavity CO is a micrometric cavity to improve the compactness of the system 1. Even more preferentially, the transport assembly SO comprises an optical fiber adapted to couple the beam FL to the cavity CO.
[0101]
With c.sub.i the channel of the matrix detector where the distinct energy peak of index i is detected and with pi the number of photons absorbed/emitted by the charged particles of the peak of index i.
[0102] In the second embodiment, step F involves solving the second equation system (S2) to determine the values of NL(c.sub.i), i[1; N] and the value of the scale factor S and the offset value O. In addition, step F comprises a second sub-step consisting in extrapolating the NL function from the N values NL(c.sub.i), i [1; N] to characterize the non-linearities undergone by the charged particles during their path and detection. Following step F, and given a number N of distinct peaks of sufficiently high energies detected, the method of the invention enables characterization of the non-linearities undergone by the charged particles as they travel through the system 1.
[0103] Preferentially, the method of the second embodiment of the invention comprises a step subsequent to step F consisting in iteratively minimizing the values of the NL function by repeating steps A to F a plurality of times and modifying parameters of the path and detection of charged particles between each iteration. In this way, the method minimizes the non-linear effects experienced by charged particles in the system 1.
[0104] For example, these parameters could be the alignment of the optical components of the system 1.
[0105] Alternatively, minimization of the NL function values is performed using the processor UT by implementing the following sub-steps: [0106] A. generating a correction table for the pixel energy values of the matrix detector of the spectrometer SM; [0107] B. correcting a subsequent measurement of the spectrum of a charged particle beam by the spectrometer SM using the correction table, so as to obtain energy measurements that are not or only slightly modified by non-linear effects.