None
Not Applicable
1. Field of the Invention
This invention relates to optical microscopy. More particularly, it relates to far-field resonance fluorescence localization microscopy.
2. Description of the Related Art Including Information Disclosed Under 37 CFR 1.97 and 1.98
The resolution limit of traditional far-field optical microscopy is about half the wavelength of the light [see, e.g., E. Abbe, Arch. Mikr. Anat. 9, 413 (1873) and L. Rayleigh, Philos. Mag. 47, 81 (1874)]. To achieve better resolution, one must switch to shorter wavelengths (e.g., electron microscopy) which is usually invasive to the system [see, e.g., A. Diaspro (ed), Nanoscopy and Multidimensional Optical Fluorescence Microscopy (CRC Press, Boca Raton, 2010)]. Near-field scanning microscopy can obtain optical imaging with sub-diffraction resolution [see, e.g., G. Binnig, C. F. Quate, and C. Gerber, Phys. Rev. Lett. 56, 930 (1986) and C. Hettich et al., Science 298, 385 (2002)], but due to the surface bound nature it is limited in application. Two-photon fluorescence microscopy first was developed to achieve a higher resolution than classical one-photon fluorescence microscopy in the far field [see, e.g., W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990) and J. H. Strickler and W. W. Webb, Proc. SPIE 1398, 107 (1991)]. Stimulated emission depletion (STED) and the related concept of ground-state depletion microscopy are then developed to overcome the far-field diffraction limit in fluorescence microscopy [see, e.g., S. W. Hell and J. Wichmann, Opt. Lett. 19, 780 (1994) and S. W. Hell and M. Kroug, Appl. Phys. B 60, 495 (1995)]. Space-dependent dark states are also proposed to achieve subwavelength resolution [see, e.g., G. S. Agarwal and K. T. Kapale, J. Phys. B 39, 3437 (2006) and S. Bretschneider, C. Eggeling, and S. W. Hell, Phys. Rev. Lett. 98, 218103 (2007)]. However, realization of these schemes is based on point-by-point scanning and is time consuming. Coherent Rabi oscillations may also be employed to break the diffraction limit [see, e.g., Z. Liao, M. Al-Amri, and M. S. Zubairy, Phys. Rev. Lett. 105, 183601 (2010) and C. Shin et al., J. Lumin. 130, 1635 (2010)], but the effect of dipole-dipole interaction has not been well discussed. Another method based on resonance fluorescence is able to measure the separation of two interacting atoms with subwavelength resolution [see, e.g., J-T Chang, J. Evers, M. O. Scully, and M. S. Zubairy, Phys. Rev. A 73, 031803(R) (2006) and Q. Sun, M. Al-Amri, M. O. Scully, and M. S. Zubairy, Phys. Rev. A 83, 063818 (2011)].
A question remains whether the locations of multiple atoms can be determined with sub-wavelength resolution even when dipole-dipole interaction is involved.
An evaluation of the resonance fluorescence spectrum of a number of two-level atoms driven by a gradient coherent laser field shows that the positions of atoms can be determined from the spectrum even when the atoms locate within the sub-wavelength range and the dipole-dipole interaction is significant. This far-field resonance fluorescence localization microscopy method does not require point-by-point scanning and is therefore more time-efficient. The present invention also includes a method to extract the position information in an extended region without requiring additional peak laser power. One particular embodiment of the invention is a method that permits 2D imaging.
The present invention utilizes collective resonance fluorescence to provide the spatial information of a multi-atom system. With this system, far-field resonance fluorescence localization microscopy (RFLM) can be performed with sub-wavelength resolution.
For simplicity, first consider identical atoms located in a line along the x axis. Such a configuration is illustrated in
The Hamiltonian of the system and the field is:
H=H
A
+H
F
+H
AF
+H
dd, (1)
where HA=ω0Σi=1N Siz is the energy of the atoms, with ω0 being the level separation and Siz is the z component of the spin operator [see, e.g., J-T Chang, J. Evers, M. O. Scully, and M. S. Zubairy, Phys. Rev. A 73, 031803(R) (2006) and T. G. Rudolph, Z. Ficek, and B. J. Dalton, Phys. Rev. A 52, 636 (1995)]. HF=ω0a†a is the total energy of the photons, where a(a†) is the annihilation (creation) operator of the photon; HAF=(/2)Σi=1N gi(Si+a+Si−a†) is the interaction between the atoms and the field, with Si+(Si−) being the raising (lowering) operator on the ith atom, and coupling constant gi=gxi/λ and g=μ(2ω0/ε0V)1/2 (μ is the transition dipole moment between ground state and excited state); Hdd=Σi≠jΩij(Si+Sj−+Si−Sj+) is the dipole-dipole interaction energy. All transition dipole moments are polarized in the y direction and the dipole-dipole interaction energy Ωij is given by:
with 2γ=4ω03d02/(3c3) being the single-atom spontaneous decay rate, k=ω0/c (c is speed of light) and xij is the distance between atoms [see, e.g., Z. Ficek and S. Swain, Quantum Interference and Quantum Coherence: Theory and Experiment (Springer, N.Y., 2004)]. The Rabi frequency for the ith atom is given by Ωi=gi√{square root over (n)} (or μE0xi/λ) where n is the photon number.
For Ωi>>Ωij
If the dipole-dipole interaction energy is not very strong, a strong laser field may be applied such that Ωi>>Ωij. In this case, the collective resonance fluorescence spectrum of a multi-atom system may be analytically evaluated based on a dressed state picture [see, e.g., C. Cohen-Tannoudji and S. Reynaud, J. Phys. B: Atom. Molec. Phys. 10, 345 (1977) and H. S. Freedhoff, Phys. Rev. A 19, 1132 (1979)]. Let H0=HA+HF+HAF and treat Hdd as a perturbation term. The eigenvalues and eigenfunctions of H0 are given by:
where N is the number of atoms, α=1,2, . . . ,2N, |aibN-1 means that ith atom is in the excited state |a while other N−1 atoms are in the ground state |b, and χiα is a constant which can be either +1 or −1. Counting the dipole-dipole interaction term as a perturbation, the eigenenergy is shifted by
and the correction to zeroth order eigenfunction is of the order of Ωij/Ωi which can be neglected. The sublevel energy Eα,n=Eα,n0+Δα,n. The pictorial energy level for the dressed state picture is shown in
The spectrum of resonance fluorescence can be evaluated by:
where D+ and D− are the raising and lowering parts of the total atomic dipole operator [see, e.g., C. Cohen-Tannoudji and S. Reynaud, J. Phys. B: Atom. Molec. Phys. 10, 345 (1977) and H. S. Freedhoff, Phys. Rev. A 19, 1132 (1979)]. The lowering part may be written as D−=Σαβn dαβ−|β, n−1 α, n|=ΣαβDαβ−, where dαβ− is the dipole matrix element of the transition from |α, nto |β, n−1 and it is defined by dαβ−=β, n−1|Σi=1NSi−|α, nand Dαβ−=Σndαβ−|β, n−1 α, n|.
The two-time correlation function in Eq. (6) may be written as:
D+(t)D−(t+τ)=Σα≠βD+(t)Dαβ−(t+τ)+ΣαD+(t)Dαα−(t+τ) (6)
where the first term corresponds to the sideband spectrum while the second term corresponds to the central peak. According to the quantum regression theorem [see, e.g., M. O. Scully and M. S. Zubairy, Quantum Optics (Cambridge University Press, Cambrige, 1997)], the two-time correlation function D+(t)Dαβ−(t+τ)satisfies the same equation of motion as the single time average Dαβ−(t). The dynamics of Dαβ−(t)can be calculated from the master equation:
where ραβ−=α, n|ρ|β, n−1, L=Σi,j=1Nγij(Si+Sj−ρ+ρSi+Sj−−2Sj−ρSi+) is the relaxation operator with γii being the decay rate of atom i and γij being the cross damping rate. For the sidebands, one may expand (Lρ)αβ=Γαβραβ+ . . . and, from Eq. (8), one obtains:
where the non-resonance terms on the right hand side in the secular approximation have been neglected. For the central peak, as all |α, n→|α, n−1, α=1, . . . ,2N have the same transition frequency, they couple to each other and one may expand (Lρ)αα=ΣβΓαβ′ρββ+ . . . . From Eq. (8) one obtains:
According to the quantum regression theorem and Eq. (6), the spectrum is given by:
where the first term yields the central peak spectrum and the second term gives the sideband spectrum.
For the zeroth order wavefunction (Eq. (4) or equivalently Eq. (21)), the transition dipole is given by:
There are three possible cases:
Case 1. β=α, dαβ−=Σi=1Nχiα/2 which contributes to the central peak ω=ω0;
Case 2. β=αp (αp is a state such that Eα0 and Eα
ωαα
From this equation, it is apparent that the positive sideband peaks can be divided into N groups: Ωp+Σk≠p±Ωpk, p=1, . . . , N. Averaging over the frequencies of each group provides the Rabi frequencies Ωp from which the positions of the atoms may be determined. The error is on the order of Ωij2/Ωi2<<1. This is the method of the present invention for optical microscopy. In an experiment, it may not be known which peak belongs to which group. However, if the gradient of laser field is changed [by an amount], the relative Rabi frequencies for different atoms change which causes the separations between different groups of spectrum shift. Because the dipole-dipole interactions do not change, the splitting between peaks belong to the same group will not change. From this phenomena, peaks belonging to different groups can be identified.
Case 3. α≠β and more than one term of Eα0 and Eβ0 have different signs, dαβ−=0 which corresponds to the forbidden transition.
The method described above is valid under the conditions: Ωi>>Ωij and |Ωi−Ωj|−2Ωij>>γ. Assuming that γ˜108 Hz and the maximum Rabi frequency is 1013 Hz, then the smallest distance that can be resolved using this method is about λ/50.
For Ωij>>Ωi
When there are two atoms in the sample whose distance is very close (e.g. rij<λ/50), the condition Ωi>>Ωij cannot be satisfied. The positions of these two atoms cannot be localized based on the method described above. However, there are ways to extract the position information of the two atoms if they are far away from other atoms (e.g., greater than λ/10). In this case a weak gradient field may be applied such that Ωi, Ωj<<Ωij. If Rabi frequency Ωi˜γ, there are only two sideband peaks located at ω0±Ωij [see, e.g., J-T Chang, J. Evers, M. O. Scully, and M. S. Zubairy, Phys. Rev. A 73, 031803(R) (2006) and T. G. Rudolph, Z. Ficek, and B. J. Dalton, Phys. Rev. A 52, 636 (1995)]. Therefore, the dipole-dipole interaction energy Ωij can be determined from the resonance fluorescence spectrum. According to Eq. (2), the distance rij between these two, close atoms can then be determined.
In one experiment, the gradient field strength was increased to a medium value (for example ˜100γ) which is still much less than dipole-dipole interaction energy. At this point, each sideband peak split into two peaks [see, id.]. For a positive sideband, it splits into two peaks:
From each equation and the relationship between Ωi and Ωj, a value for the positions ri and rj can be calculated. Because there are two equations, there may be two results. One of the results may be used as the position[s] of the two atoms or the two results may be averaged to obtained the positions of the two atoms.
Linewidth
In general, the linewidth of the emitted radiation is difficult to calculate exactly. However, the linewidth may be evaluated approximately in some cases (discussed infra). From Eq. (2), when the distance between two atoms is about λ/10, the dipole-dipole interaction energy is comparable to the linewidth of the sideband spectrum of the independent atoms. Therefore, λ/10 may be set as a threshold and the linewidth evaluated. First, when all the atoms have distances much larger than λ/10, the dipole-dipole interaction energies are much smaller than the sideband spectrum linewidth of independent atoms and the dipole-dipole interaction energies may be neglected. For independent atoms, the linewidth of the sideband spectrum is 3γ/2 [see, e.g., H. S. Freedhoff, Phys. Rev. A 19, 1132 (1979) and M. O. Scully and M. S. Zubairy, Quantum Optics (Cambridge University Press, Cambrige, 1997)], i.e., Γαβ=3γ/2 in Eq. (11). Second, when all the atoms have distances much smaller than λ/10, all dipole-dipole interaction energies Ωij are larger than 3γ/2 and the overlapped sideband spectrum splits. One can calculate (Lρ)αβ≈(N/2+1)γραβ+ . . . , from which it may be seen that Γαβ≈(N/2+1)γ. The spectrum width is about (N/2+1)γ which is similar to superradiance [see, e.g., R. H. Dicke, Phys. Rev. 93, 99 (1954)].
For the general case wherein some atoms have distances larger than λ/10 and some atoms have distances smaller than λ/10, the resonance fluorescence has the same transition frequencies but a different linewidth which is about (Neff+2)γ/2 where Neff is the average number of atoms which couple to each other and its value is between 1 and N.
In the following, the resonance fluorescence spectrum of a three-atom system is solved numerically to demonstrate how this localization microscopy works. The dressed state picture is shown in
For weak dipole-dipole interactions, according to Eq. (12) the nonzero transition dipoles are: d11±=3/2, d22±=d33±=d44±=1/2, d55±=d66±=d77±=−1/2, d88±=−3/2; d12−=d13−=d14−=d25−=d26−=d35−=d37−=d47−=d58−=d68−=d78−=1/2; d21−=d31−=d41−=d52−=d62−=d53−=d73−=d74−=d85−=d86−=d87−=−1/2. One may also calculate (Lρ)=αα=(3γ/2)ραα−(γ/2)Σα′ρα′α′ where α→α′ is allowed sideband transition. For example, if α=1, then α′=2,3,4. Thus,
From Eq. (9), one may obtain the central peak spectrum:
For the sidebands, the eigenenergy and eigenvectors of the dressed system may be numerically solved and the allowed transition frequencies calculated. In an actual experiment, the sideband peaks of the spectrum were measured. According to Eq. (13), there are three groups of allowed sideband spectrum on the positive side: ω0+Ω1±Ω12±Ω13, ω0+Ω2±Ω12±Ω23 and ω0+Ω3±Ω13±Ω23. The Rabi frequencies for each atom may be obtained by averaging over each group of the spectrum. For example, if there are three atoms and their positions are x1=0.3λ, x2=0.5λ and x3=0.7λ, the separation is λ/5. A gradient electric field is applied such that Ω(x)=100γx/λ. The resonance fluorescence spectrum is shown in
As a second example, consider that the three atoms are located at positions x1=0.45λ, x2=0.5λ and x3=0.56λ. The shortest distance is λ/20. A strong gradient electric field is applied such that Ω(x)=1500γx/λ. The resonance fluorescence spectrum is shown in
Then, the gradient laser field was slightly increased such that Ω(x)=1700γx/λ and the spectrum peaks are shown in the following table (γ):
Comparing these two tables, it is apparent that the separations between peaks in each column do not change significantly. However, the separations between peaks in different columns change significantly. From this result it can be determined that the spectrum from each column belongs to the same group. Averaging over each column of the first table one may obtain Ω1=(673.35±2.75)γ, Ω2=(751.38±2.58)γ, Ω3=(840.53±2.75)γ. The positions of the atoms may then be determined: x1=(0.449±0.002)λ, x2=(0.501±0.002)λ, and x3=(0.560±0.002)λ which also match the actual positions of the atoms quite well.
If there are two atoms whose distance is smaller than this limit, the method described above may be used. For example, there are three atoms and their positions are x1=0.485λ, x2=0.5λ and x3=0.6λ. The distance between the first atom and the second atom is 0.015λ which is less than λ/50. From Eq. (2), one may calculate that the dipole-dipole interaction energy is 891.92γ which is very large. In this situation, a weak gradient laser field may be applied first such that the corresponding Rabi frequency is Ω(x)=1γx/λ. The resonance fluorescence spectrum may be solved numerically and the result is shown in
where Ω12=1794.84γ. Assuming that Ω1=200γx1/λ and Ω2=200γ(X1+Δx12)/λ, one may get x1=0.4816λ from Eq. (18) and x1′=0.4837λ from Eq. (19). Averaging these two results produces
Above, it was disclosed how to resolve atoms located within one wavelength. For a region larger than one wavelength, one simple method is to stretch the standing wave with larger periods to cover the entire region. This method is easy to perform, but one disadvantage is that the field intensity increases as the working region increases. If the region is too large, the field will be incredible large. Therefore, for a working region beyond several wavelengths extension, a new way may be needed. One way to extend this limitation is via the divide-and-conquer method. The scheme is shown in
The method of the present invention may also be applied to a 2D image. Such a scheme is shown in
The resonance fluorescence spectrum of a number of two-level atoms is driven by a gradient coherent laser field. In the weak dipole-dipole interaction region (separation less than λ/50), a very strong laser field may be applied such that the Rabi frequency is much larger than the dipole-dipole interaction energy. From the spectrum the positions of each atom may be determined by just a few measurements. This subwavelength microscopy scheme is entirely based on far-field technique and it does not require point-by-point scanning, which makes the method more time-efficient. When two atoms are very close to each other (less than λ/50), the position information for each atom may still be obtained with very high accuracy provided that they are not too close to other atoms. The method may be extended to an arbitrary large region without requiring more peak laser power and only a few measurements are required.
In the method of the present invention, uncertainty may be due to the linewidth of the spectrum and the calibration of the light intensity. Lower density of atoms within λ/10 provides narrower linewidth and therefore smaller uncertainty. Good calibration of the light intensity is also required in an experiment in order to extract more precise position information. There is a limitation on the number of atoms within one wavelength which is about 50 in 1D and 2500 in 2D space. Another limitation of the method is that it is still not clear how to extract the spatial information of atoms when more than two atoms are very close to each other (less than λ/50).
Eigenvalues and Eigenvectors
The eigenvalue and eigenvector for H0i are:
where Ωi=g√{square root over (ni)} and ni is the mean number of photons that interact with the ith atom. The eigenvalues of H0 are just the summation of the eigenvalues of each atom:
where α=1,2, . . . , 2N, n=Σi ni and χiα=±1. The corresponding eigenvectors are:
which is equivalent to Eq. (2).
The perturbation energy due to the dipole-dipole interaction is:
wherein the photon part has been ignored because the dipole-dipole Hamiltonian only depends on atomic operators.
Linewidth
Assume that |α→|βis an allowed transition, i.e., α=β or they differ from each other by only one term. The relaxation term for the |α→|βtransition is given by:
(Lρ)αβ=Σi,j=1Nγij(α|Si+Sj−Σ|β+α|ΣSi+Sj−|β−2α|Sj−ρSi+|β)
For i=j,
where |αiand |αhave different sign only on the ith term and |βiand |βhave different sign on the ith term. There are N−1 pairs which satisfy this condition. From (26-29), one may obtain:
in which the first equation in Eq. (28) is for α=β, while the second equation is for α≠β but only differs in one term. The last three terms in the second equation may be ignored in the secular approximation because they have a different transition frequency from ωαβ. The survival of the second term depends on the coupling of the system. If all dipole-dipole interaction energies are small and can be neglected, the second term survives because ωα
In Eq. (25), spontaneous emission terms (i≠j) have also been correlated. These terms appear only when the dipole-dipole interaction cannot be neglected. If an extreme case wherein all dipole dipole interaction cannot be neglected and no spectrum is overlapped, one has:
where . . . denote terms that have different transition frequencies from ωαβ and they can be neglected in the secular approximation. Then:
The first summation vanishes because χiα=χiβ and χjα=χjβ for i,j≠p. Because χpα=−χpβ and χjα=χjβ, the first two terms in the second summation drop out. Similarly, the first two terms of the third summation also drop out. The remaining terms in the second summation and the third summation are just opposite because
When the first order correction of the wavefunction is considered, this correlated spontaneous emission rate is nonzero. However their values are on the order of (Ωij/Ωi)2 which may be assumed to be very small.
Although particular embodiments of the present invention have been shown and described, they are not intended to limit what this patent covers. One skilled in the art will understand that various changes and modifications may be made without departing from the scope of the present invention as literally and equivalently covered by the following claims.