AUTOMATED TOMOGRAPHY FIELD ION MICROSCOPE

Description

[0001] The present invention relates to a method for imaging a material at the atomic scale and a field effect ion microscope.

[0002] The field ion microscope is an instrument invented in the 1950s. This instrument offers good performance for observing structural defects in materials, but it remains little used. Its main drawback is the difficulty in controlling optimal imaging parameters during the acquisition of thousands of images of a material. This makes it difficult to effectively identify objects of interest during analysis. Variations in image quality, in particular, prevent correct extraction and reconstruction of three-dimensional information.

[0003] Traditionally, the material to be analyzed is prepared in the form of a thin needle with a small radius of curvature (less than 200 nm) and placed in a vacuum chamber. A gas, called the image gas, is introduced into the vacuum chamber and the ambient pressure of this gas, in the chamber, is low (less than 0.1 Pa). A strong DC potential (e.g. 20 kV) is applied to the tip of the needle, which has the effect of creating an intense electric field (greater than 20 V / nm) at the tip of the needle and ionizing the image gas above the surface atoms of the tip. The ions formed are then torn off the surface of the tip by the strong electric field, and their point of impact, for example on a screen, is detected. Since the distribution of the electric field is known, the trajectory of the torn off ions and their starting point can be deduced, which allows the atomic surface of the tip to be reconstructed.

[0004] To obtain a usable, sub-nanometer-scale resolved image of the surface atoms imaged by the gas, the DC potential can be varied. The potential that achieves this optimal image is called the "best image potential." This potential depends on both the nature of the image gas used and the tip's radius of curvature.

[0005] It is also possible to study the internal atomic structure of the material constituting the tip. To do this, in addition to the direct current potential, a pulse potential is applied to the tip. This has the effect of eroding the tip end, meaning that atoms on the tip surface will detach or evaporate from the tip. The potential that allows this evaporation is called the "evaporation potential."

[0006] The image gas therefore continues to ionize on the surface of the eroded tip, which makes it possible to reconstruct the internal atomic structure of the material constituting the tip.

[0007] However, tip erosion has the effect of changing the tip's radius of curvature. Therefore, the quality of surface atom images degrades over time. In addition, depending on the applied pulse potential value, either too few atoms evaporate, in which case, analyzing the internal structure of the material may be very time-consuming; or a large number of atoms evaporate from the tip, in which case it is difficult to know whether only one atomic plane has evaporated or whether several planes have evaporated. The article by Vurpillot et al., entitled "True atomic-scale imaging in three dimensions: a review of the rebirth of field-ion microscopy" and published in Microsc. Microanal. in 2017, proposes applying a constant DC potential of 7 kV to have a continuous evaporation electric field on the tip surface at the beginning of the analysis. The erosion of the tip is then continuous and occurs at a speed of 0.5 nm / s.The three-dimensional reconstruction of the material structure is done by tracking each atom on all images acquired from the tip during erosion. However, not all atoms are visible on images with the same resolution, since the applied potential is not always the best image potential, but a potential with an uncontrolled value, which makes it difficult to track some atoms.

[0008] The invention aims to remedy the aforementioned drawbacks of the prior art, more particularly it aims to propose a method for imaging a material at the atomic scale by means of a field effect ion microscope making it possible to obtain images of the same quality for each atom throughout the duration of the erosion of the tip.

[0009] An object of the invention is therefore a method for imaging a material at the atomic scale by means of a field effect ion microscope comprising a vacuum chamber configured to accommodate the material prepared in the form of a tip and an image gas, and an ion detector, characterized in that it comprises the application of a continuous electric potential and a pulsed electric potential, the maximum value of the pulse of which is noted V imp , so that the tip erodes for a potential value equal to V DC +V imp ; the acquisition, by the detector between at least two pulses of the pulsed potential, of series of at least two ion images of the impacts of the ions detached from the tip on the detector;the calculation of a characteristic quantity of an evolution of the erosion of the tip from the series of acquired ion images and the adjustment between each series of images of the values ​​of V DC and V imp so that the characteristic quantity of the evolution remains constant or included in a target interval and the ratio V DC / V imp remains constant.;

[0010] According to embodiments of the invention: the image gas is a gas having a pressure less than 0.1 Pa; the image gas is chosen from neon, helium, hydrogen, argon or a mixture comprising at least one of these gases; and the characteristic quantity of the evolution of the erosion is chosen from: a tip erosion speed, a tip atom evaporation rate or a number of atoms evaporated from the tip.

[0011] According to one embodiment of the invention, the imaging method comprises the following steps: a) Introduction of an image gas into the vacuum chamber; b) Application of a DC electric potential to the tip so as to create an electric potential difference with respect to the walls of the vacuum chamber so that the image gas ionizes on a surface of the tip and ions thus formed by the image gas detach from the surface of the tip and migrate towards the ion detector by the effect of the potential difference; c) Acquisition, by the detector, of ion images of the impacts of the ions detached from the tip on the detector for different DC electric potential values, calculation of a first quantity characteristic of a quality of the ion images for each acquired image, selection of the ion image having a desired image quality and definition of an initialization DC potential value, noted V DC_init and of a target value of this first quantity, noted C init ,V DC_init and C init being the DC electric potential and the first quantity of the selected image; d) Application of the DC electric potential to the value V DC_init and application of a pulse electric potential, the maximum of a pulse of which is noted V imp , to the end of the tip so as to cause erosion of the tip during a pulse; e) Acquisition between at least two pulses of the pulse potential, by the detector, of ion images of the impacts of the ions detached from the eroded tip on the detector for different values ​​of the maximum of the pulse V imp , calculation of a second quantity characteristic of an evolution of the erosion of the tip for pairs of images acquired during this step for the same value of V imp , selection of the pair having the desired evolution of the erosion, definition of a target maximum value of the pulse of the pulse electric potential, called initialization pulse and noted V imp_init ,corresponding to the value of the maximum pulse of the pulsed electric potential of the selected pair and definition of a target interval around the value of the second quantity of the pair selected in step e); f) Acquisition, by the detector, by iterations and during the application of the continuous electric potential and the pulsed electric potential, of series of ion images of the impacts of the ions detached from the tip on the detector between at least two pulses of the pulsed potential, each series comprising at least two images and at each iteration, calculation of the second quantity characteristic of the evolution of the erosion of the tip of the series acquired at this iteration, then comparison of this second quantity calculated with limits of the target interval defined in step e), and adjustment of the value of the continuous electric potential applied and of the maximum of the pulse of the pulsed electric potential (V imp ) applied so that,for the next iteration, the values ​​of the second characteristic quantity of the evolution of erosion are included in the target interval and that the ratio V DC / V imp remains constant, for the first iteration, the value of the continuous potential is equal to V DC_init and the maximum of the impulse of the impulse potential is equal to V imp_init. , step f) is repeated until a stopping condition is satisfied.

[0012] According to other embodiments of the invention: the method comprises a step g) of reconstructing a three-dimensional image at the atomic scale of the material constituting the tip from the series of ion images acquired in step f); the first quantity characteristic of the quality of the ion images is chosen from: a resolution of the ion images or a contrast of the ion images; step f) comprises, during each iteration, the production of a differential image obtained by subtraction of two successive ion images from the same series; and the stopping condition is chosen from reaching a maximum potential, a manual stop by a user or even a breakage of the tip.

[0013] Another object of the invention is a field effect ion microscope for implementing the method according to the invention comprising: a vacuum chamber configured to receive a sample of a material in the form of a tip and to receive a gas; an ion detector, configured to form ion images of ion impacts and to acquire ion images of these impacts; a direct current potential generator configured to apply a direct current electric potential V DC to the tip; a pulse potential generator configured to apply a pulse electric potential whose maximum pulse value is V imp;an electronic system configured to receive and process the ion images acquired by the detector, calculate a tip erosion speed from the acquired ion images and adjust the potential values ​​V DC and V imp so that a tip erosion speed remains constant or within a target range and so that the ratio V DC / V imp remains constant and control the DC potential and pulsed potential generators.;

[0014] In another embodiment, the detector includes a camera, microchannel wafers, and a phosphor screen, the wafers being positioned facing the tip in the vacuum chamber, the screen being positioned parallel behind the wafers in the vacuum chamber, and the camera being positioned facing the screen outside the vacuum chamber.

[0015] Other characteristics, details and advantages of the invention will emerge from reading the description given with reference to the appended figures given by way of example and which represent, respectively: [ Fig.1 ], a diagram of the steps of the imaging method according to the invention, and [ Fig.2 ], an ion microscope allowing the method according to the invention to be implemented.

[0016] [ Fig. 1 ] represents a diagram of the steps of the imaging method according to one embodiment of the invention. The method makes it possible to analyze the internal crystalline structure of a material. This material must be prepared in the form of a tip whose apex has a radius of curvature less than 200 nm. This tip is placed in the vacuum chamber of a field effect ion microscope also comprising an ion detector.

[0017] The first step of the method (step a)) consists of introducing an image gas GI into the vacuum chamber of the microscope. This image gas GI is at low pressure in the vacuum chamber and can be chosen from neon, helium, hydrogen, argon or another gas at a pressure lower than 0.1 Pa (10 -4 < mbar).

[0018] In the second step of the process (step b)), a direct current electrical potential V DC is applied to the tip so as to create an electrical potential difference with respect to the walls of the vacuum chamber. This potential difference has the effect of causing the ionization of the image gas GI above the atoms on the surface of the tip. Still due to the effect of the potential difference, the ions thus formed by the image gas GI will detach from the surface of the tip and migrate towards the ion detector.

[0019] In step c), ion images of the impacts of ions, resulting from the ionization of the image gas GI and detached from the tip on the detector, are acquired using the ion detector for different values ​​of continuous electric potential V DC . Each atom on the surface of the tip is the source of an ion beam. In this step, a first characteristic quantity of the quality of the ion images is then calculated for each acquired image. The calculated quantity is, for example, the image resolution or the image contrast.

[0020] Then, the ion image with the desired image quality is selected and V DC_init and C init are defined. V DC_init is the DC electric potential value of the selected image and C init is the value of the first calculated quantity of the selected image. The potential value V DC_init is thus the best image potential value that allows a clear image of the atoms on the tip surface during ionization of the GI image gas and as long as the tip has not started to erode. Below this value, some areas of the tip are barely visible, because no ionization of the gas occurs, while above this value, ionization of the GI gas no longer takes place on the tip surface and the image of the tip then becomes blurred.

[0021] In the next step (step d)), the DC electric potential at the value V DC_init and an impulse electric potential are applied to the tip end, the maximum pulse value of which is denoted V imp . The maximum value of the impulse potential (at the time of the pulse) is V imp and its minimum value is 0 V. These two potentials are used to cause erosion of the tip during a pulse. The pulses are of very short duration (from 0.1 ns to 100 ns) and are reproduced at a rate of a few hertz to a few hundred kilohertz. The erosion (or evaporation of atoms) of the tip then occurs mainly at the maximum pulse V imp . Between pulses, the evaporation rate is very low, being much lower than one atom per second.In the following, we will consider that an evaporation rate expresses the number of atoms which evaporate per unit of time, while an erosion rate expresses the reduction of a characteristic dimension of the tip per unit of time.

[0022] During this step, a second characteristic quantity of the evolution of tip erosion is also calculated. For example, the tip erosion rate, the tip erosion speed, or the number of atoms evaporated can be calculated. This can be done, for example: by locally measuring the frequency of variation of light intensity, which makes it possible to obtain the evaporation speed of certain atomic planes, or more directly by counting the number of atoms imaged on each image, or by directly calculating the difference in the number of atoms present between two images of a pair of images acquired at the same value of V DC + V imp .

[0023] We then select the pair of ion images having a desired erosion evolution, that is to say having an erosion rate desired by the user: for example, we select the one with an erosion rate of 100 atoms per second or we select the one where 50 atoms have evaporated, etc ... It all depends on the desired precision of the analysis of the material by the user. If he wants a precise analysis of the structure of the material, the user will tend to want a slow evolution of the erosion, therefore a low speed and evaporation rate whereas if he wants a fast and not precise analysis of the material, he will accept a higher erosion speed and evaporation rate.

[0024] From the selected pair, we then define V imp_init which is the maximum value of the impulse of the impulse potential of the selected image or pair. From this value Vimp_init, we define the factor α = V imp_init / V DC_init which will be constant during analysis. We also define a target interval [int] which is an interval centered around the value of the second characteristic quantity of the evolution of the erosion of the selected image or pair. For example, if the quantity of the selected image is an evaporation rate at 100 atoms per second, we can define the target interval [int] as the interval [50 atoms / s; 150 atoms / s]. α defines the fraction of impulse electric potential for the chosen target interval.

[0025] Steps b) to e) of the method allow the process to be initialized.

[0026] The next step (step f)) is an iterative step. At each iteration, a DC electric potential and a pulsed electric potential are applied. Then, between at least two pulses of the pulsed potential and at each iteration, a series of ion images of the impacts of the ions detached from the eroded tip on the detector are acquired, then the characteristic quantity of the evolution of the erosion is calculated and compared to the limits of the target interval [int]. The value of the DC electric potential and the maximum of the pulsed electric potential are then adjusted so that the values ​​of the second characteristic quantity of the evolution of the erosion measured at the next iteration are included in the target interval [int] and so that the ratio V DC / V imp remains constant, i.e. V imp remains equal to V DC / α at the next iteration with a tolerance of a few percent, for example 5% or less, preferably 1% or less.

[0027] For example, if the second quantity is included in the interval with a tolerance of a few percent, for example 5% or less, preferably 1% or less, the values ​​of V imp and V DC from iteration n are kept for the following iteration n+1, otherwise they are modified for iteration n+1. In particular, if the calculated quantity is less than the lower limit of the target interval [int], then V DC and V imp are increased, and if it is greater than the upper limit of the target interval [int], then V DC and V imp are decreased.

[0028] For the first iteration, the value of V DC applied is V DC_init and the value of V imp is V imp_init .

[0029] Step g) is repeated when a stopping condition is met. This stopping condition can be the reaching of a maximum potential (for example when V DC reaches 15 kV), a manual stop by the user or even the rupture of the analyzed sample.

[0030] These adjustments of the values ​​of V DC and V imp between each iteration are necessary to maintain the same image quality between each series of images and constant erosion. Indeed, the radius of curvature of the tip increases as the tip erodes, so the best image potential value varies, so V DC must be modified to maintain images of the same quality and especially good quality. By modifying V DC , the total potential is modified, as well as the electric field around the tip, so V imp must also be modified to maintain the same evolution of the tip erosion, that is to say the same erosion speed or the same evaporation rate as the iterations progress.

[0031] Then the next step (step h)) is the reconstruction of a three-dimensional image I3D of the atomic structure of the material constituting the tip from the series of images acquired in the iterative step g).

[0032] Step g) may also include, during each iteration, the production of a differential image obtained by subtracting two successive images from the same series. This makes it possible in particular to calculate the number of atoms evaporated between two images.

[0033] [ Fig. 2 ] represents an ion microscope according to the invention allowing the implementation of the method according to the invention.

[0034] This field effect ion microscope M comprises a vacuum chamber CV, an ion detector Det, a DC potential generator G DC and a pulse potential generator G imp . The vacuum chamber CV is configured to receive a sample of a material prepared in the form of a tip P and to receive a gas GI. The microscope M also includes a computer system PC.

[0035] The ion detector Det is configured to form images from ion impacts generated by the tip surface and to acquire ion images of these impacts. The detector Det comprises microchannel plates G for transforming an ion impact into an electron shower and a phosphor screen E which transforms the electron shower into a light spot. The detector Det also comprises a camera C which acquires images of the spots visible on the screen E. The camera C sends these images to the computer system PC which will process them.

[0036] The microchannel plates G are placed facing the tip P in the vacuum chamber CV and the screen E is placed parallel behind the plates G in the vacuum chamber CV. The camera C is placed facing the screen E outside the vacuum chamber CV.

[0037] If you do not want to place camera C in front of screen E, for reasons of space for example, it is possible to offset it in relation to the screen and use a mirror between the two.

[0038] The DC potential generator G DC is configured to apply a DC electric potential V DC to the tip P. This generator G DC is controlled by the PC computer system.

[0039] The pulse potential generator G imp is configured to apply a pulse electric potential V imp to the tip of the tip P.

[0040] The generators G imp and G DC can be two separate generators, as shown in the figure. It is also possible to have a single generator capable of delivering a pulsed electric potential whose maximum value (at the time of the pulse) is V DC +V irnp and whose minimum value is V DC .

[0041] The PC computer system is configured to receive and process the ion images acquired by the detector Det, in particular by the camera C. It is also configured to calculate a characteristic quantity of the quality of the acquired ion images, such as for example the resolution or the contrast of the image. It is configured to calculate a characteristic quantity of the evolution of the erosion, it can thus calculate the erosion speed of the tip and / or the evaporation rate of the tip and / or the number of evaporated atoms. It is also configured to calculate the adjustment of the DC potential (V DC ) and maximum pulse of the pulse potential (V imp ) values ​​and to control the DC potential (G DC ) and pulse potential (G imp ) generators.

[0042] According to another embodiment of the invention, the PC computer system is also configured to reconstruct a three-dimensional image I3D of the structure of the material constituting the tip from the different ion images acquired by the detector Det.

[0043] According to another embodiment of the invention, the PC computer system is configured to produce a differential image resulting from the subtraction of two ion images.

[0044] According to another embodiment of the invention, the PC computer system is configured to apply a light spot detection algorithm to the ion images and / or to a differential image.

[0045] According to another embodiment, the ion detector D comprises micro-channel plates and a spatial localization system for the electron shower of the resistive anode or delay line type.

[0046] In another embodiment, the ion detector Det comprises a charge-coupled device (CCD) or a complementary metal-oxide semiconductor (CMOS) sensor placed directly in front of the tip. In this case, the detector may also comprise an amplifier.

Claims

1. A method for imaging an atomic-scale material by means of a field ion microscope (M) comprising a vacuum chamber (CV) configured to accommodate the prepared material in the form of a tip (P) and an image gas (GI), and an ion detector (Det), characterized in that it comprises the application of a direct-current electrical potential (VDC) and of a pulsed electrical potential, the maximum value of the pulse of which is denoted Vimp, so that the tip erodes for a potential value equal to VDC+Vimp; acquisition by the detector, between at least two pulses of the pulsed potential, of series of at least two ion images of the impacts of ions detached from the tip on the detector; calculation of a quantity characteristic of an evolution of the erosion of the tip from the series of ion images acquired and adjustment between each series of images of the values of VDC and Vimp so that the quantity characteristic of the trend remains constant or within a target range and the ratio VDC / Vimp remains constant.

2. The imaging method according to claim 1, wherein the image gas is a gas having a pressure of less than 0.1 Pa.

3. The imaging method according to one of claims 1 to 2, wherein the image gas is chosen from neon, helium, hydrogen, argon or a mixture comprising at least one of these gases.

4. The imaging method according to one of claims 1 to 3, wherein the quantity characteristic of the erosion trend is selected from: a tip erosion rate, a tip atom evaporation rate, or a number of evaporated tip atoms.

5. The imaging method according to one of claims 1 to 4 comprising the following steps: a) Introduction of an image gas (GI) into the vacuum chamber; b) Application of a direct electrical potential (VDC) to the tip so as to create an electrical potential difference with respect to the walls of the vacuum chamber, so that the image gas ionizes on a surface of the tip and ions thus formed by the image gas detach from the surface of the tip and migrate to the ion detector as a result of the potential difference; c) Acquisition, by the detector, of ion images of the impacts of ions detached from the tip on the detector for different values of direct-current electrical potential (VDC), calculation of a first quantity characteristic of a quality of the ion images for each image acquired, selecting the ion image with the desired image quality and defining an initialization DC potential value, denoted VDV_init, and a target value for this first quantity, denoted Cinit, where VDV_init et Cinit are the direct-current electrical potential and the first quantity of the selected image; d) Application of the direct-current electrical potential at the value VDC_init and application of a pulsed electrical potential, the maximum of a pulse of which is denoted Vimp, to the end of the tip so as to cause erosion of the tip during a pulse; e) Acquisition by the detector, between at least two pulses of the pulsed potential, of ion images of the impacts of ions detached from the eroded tip on the detector for different values of the maximum of the pulse Vimp, calculation of a second quantity characteristic of an erosion trend of the tip for pairs of images acquired during this step for the same value of Vimp, selection of the pair having the desired erosion trend, definition of a target maximum value of the pulse electric potential, called initialization pulse and denoted Vimp_init, corresponding to the value of the maximum pulsed electric potential of the selected pair and definition of said target interval ([int]) around the value of the second quantity of the pair selected in step e); f) Acquisition, by the detector, in iterations and during the application of the direct-current electric potential and of the pulsed electric potential, of series of ion images of the impacts of the ions detached from the tip on the detector between at least two pulses of the pulsed potential, each series comprising at least two images and at each iteration, calculation of the second quantity characteristic of the erosion trend of the tip of the series acquired at this iteration, then comparison of this calculated second quantity with bounds of the target interval ([int]) defined in step e), and adjusting the value of the direct-current electrical potential (VDC) applied and the maximum of the pulse of the pulsed electrical potential (Vimp) applied in such a way that, for the next iteration, the values of the second quantity characteristic of the erosion trend lie within the target interval and the ratio VDC / Vimp remains constant, for the first iteration, the value of the direct-current potential is equal to VDC_init and the maximum of the pulse of the pulsed potential is equal to Vimp_init. step f) is repeated until a stop condition is satisfied.

6. The imaging method according to claim 5 comprising a step g) of reconstructing an atomic-scale three-dimensional image (13D) of the tip material from the series of ion images acquired in step f).

7. The imaging method according to one of claims 5 to 6, wherein the first quantity characteristic of the quality of the ion images is chosen from: a resolution of the ion images or a contrast of the ion images.

8. The imaging method according to one of claims 5 to 7, wherein step f) comprises, during each iteration, the production of a differential image obtained by subtracting two successive ion images from the same series.

9. The imaging method according to one of claims 5 to 8 wherein the stop condition is selected from a maximum potential being reached, a manual stop by a user, or the tip breaking.

10. A field ion microscope for carrying out the method according to one of the preceding claims, comprising: - a vacuum chamber (CV) configured to receive a sample of a material in the form of a tip (P) and to receive a gas (GI); - an ion detector (Det), configured to form ion images of ion impacts and to acquire ion images of these impacts; - a direct-current potential generator (GDC) configured to apply a direct-current electrical potential VDC to the tip; - a pulsed potential generator (Gimp) configured to apply a pulsed electrical potential whose maximum pulse value is Vimp; - an electronic system (PC) configured to receive and process ion images acquired by the detector, to calculate a tip erosion rate from the acquired ion images, and to adjust the VDC and Vimp potential values so that a tip erosion rate remains constant or within a target range and the VDC / Vimp ratio remains constant, and to control the direct-current and pulsed potential generators.

11. The microscope according to claim 10, wherein the detector comprises a camera (C), microchannel plates (G) and a phosphor screen (E), the plates being positioned facing the tip in the vacuum chamber, the screen being positioned parallel behind the plates in the vacuum chamber and the camera being positioned facing the screen outside the vacuum chamber.