The present invention relates generally to a ballistic exciton transistor and/or corresponding method(s) of use and manufacture. The excitonic device has industrial applications that extend to at least fast optical switching, optical communication, exciton devices, and exciton-based information processing.
The background description provided herein gives context for the present disclosure. Work of the presently named inventors, as well as aspects of the description that may not otherwise qualify as prior art at the time of filing, are neither expressly nor impliedly admitted as prior art.
The rate of miniaturization of solid-state transistors is slowing. A logical end to same is thus in sight. Moore's law, i.e., the number of transistors in a dense integrated circuit (IC) doubling about every two years, will cease to be true unless new approaches to increase transistor density continue to be discovered.
An exciton is the name for the energy packet that resides on a chromophore when it is in its excited state. When two molecules are very close to each other the energy of an excited chromophore can be transferred to a neighboring chromophore without energy loss, in contrast to the usual fluorescence resonance energy transfer (FRET) where energy loss occurs in the transfer. The packet of energy can be exchanged in a wave like manner back and forth between the two molecules. The energy packet, in this sense, acts like a quantum mechanical particle that can become delocalized or spread out over an aggregate of chromophores just like an electron can spread out its wave function over an entire molecule (molecular orbital). The Davydov splitting and the circular dichroism (CD) spectra seen in chromophore aggregates is a manifestation of this delocalization. Davydov splitting is analogous to the splitting of orbitals into bonding and antibonding orbitals when two atoms are brought close together.
When two or more chromophores are spaced sufficiently close (nanospaced), near-field interactions, such as, but not limited to, electromagnetic dipole-dipole interactions form. This can result in an increase in the coupling strength between two or more chromophores and a change in absorption of light relating to its polarization. The coupling strength between the two or more chromophore dipoles increases such that they are either weakly or strongly coupled opposed to being very weakly coupled or uncoupled. When the proximity of the chromophores is such that their orbitals overlap, in some cases this may result in an additional increase in coupling strength.
Optical systems are also becoming increasingly popular due to their high speed and high data capacity capabilities. Light has bidirectional transmission reciprocity in common dielectric materials. Breaking this reciprocity in the direction of light transmission is of great significance in classical and quantum information processing. Optical isolators, circulators, switches, and directional amplifiers are examples of non-reciprocal devices. Optical isolators are optical components which allow the transmission of light in only one direction and are typically used to prevent unwanted feedback into an optical oscillator. Optical circulators are three- or four-port optical devices designed such that light entering any of the ports exits from the next. Optical switches are devices which selectively direct optical signals from one channel to another. Optical directional amplifiers are devices which amplify an optical signal without first converting it into an electronic signal.
There exists a need in the art for a device which uses molecular dyes as networked aggregates to overcome the limitations of classical physics in achieving additional transistor densities beyond what may be achievable ultimately with traditional solid-state devices.
The following objects, features, advantages, aspects, and/or embodiments, are not exhaustive and do not limit the overall disclosure. No single embodiment need provide each and every object, feature, or advantage. Any of the objects, features, advantages, aspects, and/or embodiments disclosed herein can be integrated with one another, either in full or in part.
According to some aspects of the present disclosure, the device comprises an exciton transmission line composed of a row of chromophores (dyes). The excitons considered here are molecular excitations in which the chromophore is excited from the ground state to the lowest electronic excited state. Propagation of excitons (or their delocalization) along the line (i.e., between dyes) is mediated by an exciton exchange interaction having strength denoted by the excitonic hopping parameter J. This strength—and consequently the ability to maintain transmission along the line—is dependent on the dye orientation and proximity relative to the other dyes in the line. The gate comprises a dye whose transition dipole moment is oriented orthogonally to the transition-line dipoles along the transmission line. In that configuration an exciton is not able to transfer from the gate dye to the exciton transmission line. An exciton on the gate dye can interact with excitons on the transmission line only via a two-body exciton interaction (i.e., two dyes—the gate and its proximal dye on the transmission line—are each separately excited) having strength denoted by the parameter K (exciton-exciton interaction energy). This interaction results from changes in the charge distribution that occur when a dye molecule is excited to its lowest electronic excited state. If the gate dye is not excited, K=0 and transmission along the line occurs unimpeded. If the gate molecule is excited and K is sufficiently large, signals are backscattered as a result of the two-body interaction. As a result, the device can function as an on/off gate relative to signal propagation along the transmission line. The gate dye can be excited optically without exciting the transmission-line dyes if polarized light with a polarization parallel to the gate molecule transition dipole moment is used, because this polarization direction is orthogonal to the transition dipole moments of the transmission-line dyes. Alternatively, the gate dye can be excited optically without exciting the transmission-line dyes if the optical excitation energies of the gate dye and the transmission-line dyes are chosen so that the absorption band of the gate dye does not overlap with that of the transmission-line dyes. In this case light, regardless of polarization, will excite only the gate dye if the light wavelength lies within the absorption band of the gate dye.
According to some other aspects of the present disclosure, the ballistic exciton transistor relies on the exciton exchange interaction and the two-body exciton interaction. In the dipole approximation the exciton exchange interaction is mediated by transition dipoles (μ), whereas the two-body exciton interaction is mediated by the difference static dipoles (Δd). The direction of the transition dipole and the difference dipole need not be parallel, as they depend on the molecular structure in different ways. This allows for the possibility of orienting two chromophores (dyes a and b0) such that they can interact only via the two-body exciton interaction.
It is a primary object, feature, and/or advantage of the present invention to improve on or overcome the deficiencies in the art.
It is a further object, feature, and/or advantage of the present invention to provide a ballistic exciton transistor.
It is yet a further object, feature, and/or advantage of the present invention to position, orient, and configure molecules so as to selectively and optimally exchange/transfer excitons within certain regions of the ballistic exciton transistor.
It is yet a further object, feature, and/or advantage of the present invention to propagate signals through an exciton transmission line so as to produce signal gain.
The ballistic exciton transistor disclosed herein can be used in a wide variety of applications. For example, the ballistic exciton transistor can be beneficially used for optical switching and optical communication.
Methods can be practiced which facilitate use, manufacture, assembly, maintenance, and repair of the ballistic exciton transistor which accomplish some or all of the previously stated objectives.
The ballistic exciton transistor can be incorporated into exciton-based information processing devices and systems, including, but not limited to quantum information processing systems, quantum computers, optical switches, and/or other devices and systems which accomplish some or all of the previously stated objectives.
The immediately following numbered paragraphs characterize an exemplary optical switch that can be constructed employing at least some of the beneficial aspects described herein.
An optical switch comprising:
The optical switch of paragraph [0021] wherein the signal comprises light.
The optical switch of paragraph [0022] wherein the light can be modulated so as to be turned on and off.
The optical switch of paragraph [0021] wherein the exciton channel comprises a DNA origami nanotube.
The optical switch of paragraph [0024] wherein the molecules are dyes.
The optical switch of paragraph [0025] wherein the coupler comprises gold pads attached to each of the source waveguide, the gate waveguide, and the drain waveguide.
The optical switch of paragraph [0026] wherein an electric field can concentrate on said gold pads and induce electric field oscillations in the dyes.
The optical switch of paragraph [0024] wherein the DNA origami nanotube includes five duplex strands of DNA symmetrically arrayed about the exciton channel.
The optical switch of paragraph [0028] wherein the duplex strands of DNA comprise a M13 bacteriophage.
The optical switch of paragraph [0028] wherein the DNA origami nanotube comprises a three-dimensional geometrical shape formed from one long scaffold strand.
The optical switch of paragraph [0030] wherein the geometrical shape is assembled by folding said long scaffold strand in an aqueous solution consisting of a buffer containing salt.
The optical switch of paragraph [0031] wherein the solution is heated to a temperature between 60° C. and 90° C.
The optical switch of paragraph [0025] wherein the DNA origami nanotube comprises a size that is approximately identical to a diameter of said dyes.
The optical switch of paragraph [0025] wherein the dyes are attached to DNA, said dyes optionally comprising Cyanine dyes Cy5 and/or Cy5.5.
The optical switch of paragraph [0025] wherein the dyes have an asymmetric conjugated π-bond network, said dyes optionally comprising a dye selected from any one or more of the Dyomics dyes DY-550 through DY-831.
The optical switch of paragraph [0021] wherein the transition dipole comprises a strength of approximately 16 D.
The optical switch of paragraph [0021] wherein the gate dye and the proximal dye along the exciton channel cause a difference static dipole moments of a strength of approximately 16 D.
The optical switch of paragraph [0021] wherein the coupler is capable of:
(i) converting the photons into plasmons; and
(ii) converting the plasmons into the excitons.
The optical switch of paragraph [0038] wherein the optical switch is configured as a reciprocal device and a conversion according to steps (i) and (ii) is just as efficient as reciprocal conversions that include: (iii) converting the excitons to the plasmons; and (iv) the plasmons to the photons.
The optical switch of paragraph [0021] wherein the fraction is not a zero percent fraction nor a one-hundred percent fraction.
These and/or other objects, features, advantages, aspects, and/or embodiments will become apparent to those skilled in the art after reviewing the following brief and detailed descriptions of the drawings. Furthermore, the present disclosure encompasses aspects and/or embodiments not expressly disclosed but which can be understood from a reading of the present disclosure, including at least: (a) combinations of disclosed aspects and/or embodiments and/or (b) reasonable modifications not shown or described.
Several embodiments in which the present invention can be practiced are illustrated and described in detail, wherein like reference characters represent like components throughout the several views. The drawings are presented for exemplary purposes and may not be to scale unless otherwise indicated.
An artisan of ordinary skill in the art need not view, within isolated figure(s), the near infinite number of distinct permutations of features described in the following detailed description to facilitate an understanding of the present invention.
The present disclosure is not to be limited to that described herein. Mechanical, electrical, chemical, procedural, and/or other changes can be made without departing from the spirit and scope of the present invention. No features shown or described are essential to permit basic operation of the present invention unless otherwise indicated.
Referring now to
The exciton exchange interaction 104 is represented in
In one embodiment, the ballistic exciton transistor 100 can be described as including an excitonic interchange. Like road traffic interchanges, the excitonic interchange can act as a sophisticated junction or junction-like system where exchange interactions can occur. In other words, the excitonic exchange can be thought of as the means by which excitons can be exchanged and otherwise transmitted amongst molecules. For example, the excitonic exchange can comprise a first location at which a linear exciton exchange interaction can occur, said linear exciton exchange interaction being mediated by a transition dipole along the exciton transmission line; and a second location at which a two-body exciton interaction can occur, said two-body exciton being mediated by a difference static dipole along the transmission line.
The ballistic exciton transistor 100 relies on the exciton exchange interaction 104 and the two-body exciton interaction 108. In the dipole approximation the exciton exchange interaction is mediated by transition dipoles (μ), whereas the two-body exciton interaction is mediated by the difference static dipoles (Δd). The direction of the transition dipole and the difference dipole need not be parallel, as they depend on the molecular structure in different ways. This allows for the possibility of orienting two chromophores (dyes a and b0) such that they can interact only via the two-body exciton interaction.
Squaraine dyes are an example of this in which a pair of two squaraines can be arranged such that their transition dipoles are orthogonal and, hence, do not couple (i.e., propagate an exciton), whereas the exciton-exciton interaction is mediated by a Coulombic quadrupole-quadruple interaction. The asymmetric dyes offered by Dyomics whose product numbers are in the range DY-610 through DY-780 offer examples of this. Molecule a of
The Hamiltonian
The molecule labels a and br of
The Hamiltonian operator for the system of
where ℏ is a time-dependent constant, ω is a frequency, and † is used to identify specific number operators.
Heisenberg Equations of Motion
The Heisenberg equation of motion for an operator O is
The following are equations of motion for the gate molecule a, the proximal molecule b0, and any molecule br along the transmission line 102:
and where r≠0,
Solving for the above Heisenberg equation of motion with the equations of motion for the gate molecule a, the proximal molecule b0, and any molecule br along the transmission line 102 yields:
The number operator a†a for the number of excitons on molecule a can be treated as a constant.
Exciton Transmission Lines
If there is no exciton on molecule a, then the number operator a†a can be replaced by its eigenvalue which is zero. In this case, the equation for motion with respect to br holds even at r≠0:
for all r. Due to the translation symmetry the solutions of the above equation of motion will have the Bloch form:
where k is the wave number, yielding the dispersion relation:
ωk=ωo+2ωJ cos(k).
The group velocity is defined:
Note ωJ can be positive or negative. It is positive if the molecules are aligned side by side (H configuration) or end to end (J configuration). The phase velocity vϕ=wk/k can have a different speed and sign from that of the group velocity, v9. Note also that the group velocity, v9, has the greatest magnitude when k=+π/2, for which the Bloch form can be written in the form:
where the signals carried by b(k) and b(−k) propagate in opposite directions. The transmission line signals 110, 114 propagate unimpeded along the transmission line 102.
Exciton Scattering Off of an Exciton
Where ωJ is negative, the signals carried by b(k) propagate to the left in the exciton transmission line 102 shown in
For r≠0, the result is still:
because causality signals propagating in from infinity will not be influenced by what happens at r=0 until the signals arrive at that point. For signals coming toward r=0 and which are leaving r=0, for the transmission line to the left of r=0, the result is:
for r<0 and for the transmission line 102 to the right of r=0 results in:
for r>0.
If the number of excitons at the gate molecule a is zero, variables in the previous two equations can be solved for as follows:
b
L
out(k)=bRin(k)=b(k)
and
b
R
out(k)=bLin(k)=b(−k)
If the gate molecule a is excited, then:
yielding the following by way of the br equations for r<0 and r>0 above:
(ωk−ωo−ωKa†a)b(k)=ωJ[eikbRin(k)+e−ikbRout(k)+e−ikbLout(k)+eikbLin(k)],
ωJb(k)=(ωk−ωo−ωJeik)eikbRin(k)+(ωk−ωo−ωJe−ik)e−ikbRout(k),
ωJb(k)=(ωk−ωo−ωJe−ik)e−ikbLout(k)+(ωk−ωo−ωJeik)eikbLin(k).
Note:
ωk−ωo=ωJ(eik+e−ik)
and thus collectively this yields:
[ωJ(eik+e−ik)−ωKa†a]b(k)=[eikbRin(k)+e−ikbRout(k)+e−ik+bLout(k)+eik+bLin(k)]
b(k)=bRin(k)+bRout(k),
b(k)=bLin(k)+bLout(k).
[ωJ(eik+e−ik)−ωKa†a][bRin(k)+bRout(k)]=ωJ[eikbRin(k)+e−ikbRout(k)+e−ikbLout(k)+eik+bLin(k)],
[ωJ(eik+e−ik)−ωKa†a][bLin(k)+bLout(k)]=ωJ[eikbRin(k)+e−ikbRout(k)+e−ikbLout(k)+eik+bLin(k)].
The last two equations rearranged yield:
ωJe−ikbLout(k)−(ωJeik−ωKa†a)bRout(k)=−ωJeikbLin(k)+(ωJe−ik−ωKa†a)bRin(k),
−(ωJeik−ωKa†a)bLout(k)+ωJe−ikbRout(k)=(ωJe−ik−ωKa†a)bLin(k)−ωJeikbRin(k).
This can be reduced by introducing the quantities:
F
1=−ωJeikbLin(k)+(ωJe−ik−ωKa†a)bRin(k),
F
2=(ωJe−ik−ωKa†a)bLin(k)−ωJeikbRin(k).
Further rewritten, these equations can be expressed as:
ωJe−ikbLout(k)−(ωJeik−ωKa†a)bRout(k)=F1
−(ωJeik−ωKa†a)bLout(k)+ωJe−ikbRout(k)=F2
and in Matrix form:
Solving for bLout (k) and bRout (k), this finds:
In other words:
One now has:
|ωJeik−ωKa†a|2−ωJ2=−2ωJωK cos(k)a†a+ωK2a†aa†a.
And again, solving for bLout (k) and bRout(k):
The transmission T and the reflection R amplitudes can be introduced as:
When there are no excitons in molecule a, the number operator a†a can be replaced by zero and one obtains T=1 and R=0. Now:
ωJ2e−i2k−(ωJeik−ωKa†a)2=−2iωJ[ωJ sin(2k)−ωK sin(k)a†a]+2 ωJωK cos(k)a†a−ωK2a†aa†a.
The transmission amplitude can be rewritten as:
The transmission coefficient (transmission probability) can be expressed:
So if one exciton is present in molecule a, a†a can be replaced by 1 and the transmission coefficient can then be expressed as:
The behavior of this system when the excitons are at the bottom of the band can be particularly beneficial because in the case when ωJ is negative and k is near zero, a Taylor expansion of trigonometric functions in the equation above will yield:
For strong switching, the numerator would ideally be as small as possible. For example, if one were to minimize |ωJ sin(2k)−ωK sin(k)|, the Taylor expansions would become:
To make the first equation above as small as possible as k approaches 0, the linear order term can be eliminated by setting the condition:
ωK=2ωJ
and with this condition the lowest order becomes:
|T|2=k2.
Midband Performance
For a signal propagating at mid band, that is k=π/2, the condition set above should not be imposed. In this case one has:
To make the transition coefficient as small as possible, one would like to make ωK (that is K) as large as possible. If we choose such a value to satisfy ωK=2ωJ then |T|2=1/2. Hence, it may be possible to achieve a switching amplitude at room temperature of a factor of at least 2. The equation ωK=2ωJ suggests much higher switching ratios could be achieved at low temperatures.
Bound States
If the two-exciton interaction 108, K=ℏωK, is sufficiently strong and negative, exciton-exciton bound states can form between the exciton in the gate molecule a and an exciton on the transmission line 102. It is possible to determine the conditions when a bound state can form. It is noted that the existence of such bound states enables other mode of operation of the exciton transistor 100. The bound state will suppress the row of excitons 102 through the transistor 100 if there is a repulsive two-body interaction 108 between excitons on the transmission line 102. The Hamiltonian for such an interaction would have the form:
where KT is the interaction energy between two excitons residing on neighboring sites. Alternatively, if the anharmonicity parameter Δ is positive, it will be unfavorable for two excitons to occupy the same molecule and this will suppress the row of excitons 102 through the exciton transistor 100. The Hamiltonian for this interaction is given by:
In the limit Δ→∞ the excitons behave as hard-core Bosons. In this case, flow through the transistor 100 would be completely suppressed. In this limit, the Hamiltonian can be dispensed with if the molecules br are treated as satisfying Paulion commutation relations.
The bound state mode is expected to have the form:
b
r
=b
B
e
−iω
t
e
−K|r|
where molecules br need no longer satisfy the usual boson commutation relations. The equations of motion will still need to be satisfied such that:
ωK−ωo−ωKa†a=2ωJe−K
and
ωκ=ωo+2ωJ cos h(κ).
The two equations together yield:
and from this one can obtain:
Hence:
ωJ is negative at the bottom of the transmission line band when k=0. It follows that the energy at the bottom of the band in frequency units is:
ω0=ωo+2ωJ.
The condition for the existence of a bound state is
ωκ<ωo
and with this condition the equations of [0064] and [0065] yield:
and since ωJ is negative this further yields:
which is satisfied when the numerical operator a†a has an eigenvalue greater than 0. It can be concluded that when ωJ is negative and the exciton-exciton interaction is attractive (ωK is negative) there can be a bound state.
The analysis with ωJ<0 and ωK<0 can be plagued by the existence of a bound state unless a proper analysis of transmission through the exciton transistor 100 is done and one takes into account the bound state.
Suppression of Transmission by a Repulsive Interaction
When ωJ=0 so that the bottom of the band occurs at k=0 and the exciton-exciton interaction is positive ωK>0, suppression of transmission still occurs due to the repulsive interaction. For example, as shown in
Switching on-off contrast improves the larger the ratio |ωK|/|ωJ| becomes. When |ωK|=2|ωJ| this yields |T|2=1/2. The switching contrast is larger for smaller values of k, that is, when the incoming signals 110 are near the band minimum. When ωx>>2|ωJ|, the transmission coefficient becomes:
When k<<1, the transmission coefficient becomes:
For ballistic transport of excitons along a chain of chromophores (e.g., molecules br,), |ωJ| should be as large as possible to minimize decoherence due to exciton-vibron coupling. The exciton transistor described here should then become feasible provided such molecules can be found for which |ωK| is correspondingly large even when the molecular pair is configured such that the transition dipoles are orthogonal.
Constructing an Exciton Transistor
According to one embodiment, the exciton transistor 100 can be fabricated as shown in
The exciton transistor 100 can form the heart of an optical switch 300 shown in
The exciton transistor 100 comprises an exciton channel 302, pads 304, a gate 306, a source 308, and a drain 310. The gate 306, source 308, and drain 310 all represent optical waveguides which extend beyond the region shown. The source waveguide 308 carries the signal that is to be switched. The source waveguide 308, in some embodiments, comprises a steady flow of light such as that coming from a CW laser. The drain waveguide 310 carries the fraction of this light that has made it through the device: that is, the light that has been modulated or switched on or off. The gate waveguide 306 carries the light signal that performs the switching.
The pads 304 in
Taking the source end of the exciton channel 302 as an example, the electric field of the incoming light field can be concentrated on the gold pad 304. On the gold pad 304 this concentrated electric field can be referred to as a plasmon field. The concentrated electric field induces electric field oscillations in a row of dye molecules 406 within the exciton channel 302. In terms of the quanta of these fields, the coupler can be said to make two transformations. The first transformation is to convert a photon into a plasmon; the second transformation is to convert a plasmon into an exciton. By concentrating the electric field, the conversion of incoming photos into excitons is more efficient than if the exciton channel 302 were connected directly to the source waveguide 308. The coupler is a reciprocal device, meaning that it converts excitons into photons as efficiently as it converts photons into excitons. Hence, excitons arriving at the drain waveguide 310 of the optical switch 300 are transformed by the coupler into photons that then propagate away along the drain waveguide 310.
The exciton channel 302 can be a DNA origami nanotube 400 (
DNA origami is a DNA nanotechnology fabrication technique. One example of DNA origami is described in Rothemund, “Folding DNA to Create Nanoscale Shapes and Patterns,” Nature 2006, 440, 297-302, which is herein incorporated by reference. Rothemund illustrates in
Thereby, it is now possible to design short DNA strands, called staple strands, whose base sequences are complementary to certain regions of the scaffold strand by design. The base sequences for the staple strands are designed using the known DNA sequence of the scaffold strand and are produced by automated DNA synthesis machines. Such staple strands can be purchased commercially from foundries. One can, as an example, communicate the base sequences of the desired DNA strands to the foundry and the corresponding DNA strands are then produced by an automated DNA synthesis machine. These staple strands are designed to bind uniquely to specific regions on the scaffold strand. Examples of these are the short colored strands seen in
Other options are also available for producing large origami structures, and for the case here DNA nanotubes 400 that can serve as substrates 312 for the dyes composing the exciton channel 302. Some methods for making DNA origami scaffolds, such as the use of bacteriophage-based ssDNA production, have resulted in producing scaffolds as large as 31,274 nucleotides (nt). ssDNA 31,274 nt long has a length of 11,000 nanometers or 11 microns. Folded 5 times yields scaffolds of length 2.2 microns. This is more than sufficient to span the distance between the source and drain waveguides 308, 310 of
By these means, the long scaffold strand can be folded into a geometrical shape. This assembly occurs in an aqueous solution consisting of a buffer containing salt. The scaffold strand and the staple strands are mixed together in the solution. The scaffold strand and the staple strands diffuse in the solution and encounter each other and complementary base sequences combine (the technical term is hybridize) to spontaneously form the geometric shape. To obtain the desired shapes in high yield, the solution is heated to above the melting temperature (the temperature at which duplex DNA dissociates into single strands) and then slowly cooled to room temperature. The melting temperature depends on the length of the complementary regions of DNA but for the short staple strands employed in DNA origami, heating to a temperature somewhere in the range of 60° C. to 90° C. is sufficient.
Although the structures Rothemund produced in his initial published work were planer 2-dimensional objects, this technique can be extended to produce 3-dimensional objects. Of interest here is the formation of DNA nanotubes suitable for purposes of fabricating the ballistic exciton transistor 100 and optical switch 300 described herein that can serve as substrates on which dye molecules 406 can be arranged. In other words, DNA origami can be used to assemble DNA nanotubes, including the DNA nanotubes 400 shown in
In some embodiments, in order to produce a DNA nanotube of sufficient length, the overall structure can comprise two DNA nanotubules 400 (formed form M13 bacteriophage scaffold strands) spliced together. The two DNA origami nanotubes, individually, can be approximately 400 nanometers in length, whereas the overall structure can be approximately 800 nanometers in length.
It is worth noting
The number of parallel duplex strands making up the nanotube can be varied. In Douglas et al., a tube consisting of six such DNA strands was chosen, often referred to as a six-helix bundle. The size of the inter diameter of the tube can be varied by changing the number of duplex stands making up the bundle.
With reference to
Dyes 406 can be attached at specific points along the DNA 402. Keeping in mind that duplex DNA 402 is often a helical structure (e.g., the double helix), staple strands can be designed such that when the DNA nanotube 400 self-assembles, the attachment of the dye molecules 406 is at points on the inside of the DNA nanotube 400. The dye molecules 406 will thus be on the inside of the nanotube 400, as shown in
Software can be used to aid the design of DNA origami structures such as the nanotube 400 considered herein. One example of such software is CanDo (Computer-aided engineering for DNA origami). The design of origami structures is thus a task that can be largely automated. Examples of dyes, available commercially, that can be attached to DNA and that can serve as the dyes that constitute the exciton channel are the Cyanine dyes Cy5 and Cy5.5, but many more dye types are available and those skilled in organic chemistry can synthesis their own custom dyes that can be incorporated into DNA via covalent bonds during the synthesis of the DNA 402.
The molecules br can also comprise other dyes, and more particularly, the chromophores of said dyes. For example, chromophores that can be used include one or more of a xanthene, fluorescein, rhodamine, oregon green, eosin, Texas red, cyanine, indocarbocyanine, oxacarbocyanine, thiacarbocyanine, merocyanine, squaraine, Seta, SeTau, Square dyes, naphthalene, dansyl, prodan, coumarin, oxadiazole, pyridyloxazole, nitrobenzoxadiazole, benzoxadiazole, anthracene, anthraquinone, DRAQ5, DRAQ7, CyTRAK Orange, pyrene, cascade blue, oxazine, Nile red, Nile blue, cresyl violet, oxazine 170, acridine, proflavin, acridine orange, acridine yellow, arylmethine, auramine, crystal violet, malachite green, tetrapyrrole, porphin, phthalocyanine, and bilirubin, and/or a combination thereof.
Methods to attach DNA 402 to gold surfaces 304 include methods by which the exciton channel 302 is connected between at least two gold pads 304. Topography can also be used to control nanotube 400 alignment.
Dipole Moments
The difference static dipole-dipole interaction, resulting from differences in the charge density of a molecule when it is in its excited state compared to when it is in its ground state, is employed. Dye 404 and the most proximal dye 406 to the gate region 306 must have difference static dipole moments.
In order to function as an exciton channel 302 that can be gated, the dye molecules 404 and 406, the latter the channel dye that is proximal to the gate region 306 must have a difference static dipole moment that is large, preferably comparable to the transition dipoles involved in exciton exchange 104. Organic dyes can have transition dipoles as high as 16 D, where D denotes the unit “debye” which is used to measure the strength of electric dipole moments. Asymmetry in the conjugated n-bond network of an organic dye molecule facilitates the position of a large difference static dipole moment that is large and hence yields exciton-exciton interactions 104 between dyes. Examples of dyes having an asymmetric conjugated n-bond network and that are commercially available for attachment to DNA are family of dyes offered by Dyomics, such as the dyes DY-550 through DY-831. This range of dyes allows the selection of dyes having optical transition frequencies close to frequencies of the light signals 110 that are to be switched. A number of organic molecules that have been theoretically calculated to have difference static dipole moments as large as 16 D are descried in Jacquemin, “Excited-state dipole and quadrupole moments: TD-DFT versus CC2,” J. Chem. Theory Comput. 2016, 12, 3993-4003, herein incorporated by reference in its entirety.
See, e.g., molecular structure 17 in Jacquemin's scheme 2 and the corresponding entries in their Table 3 where different calculational methods consistently predict large difference static dipole moments, around 16 D. The difference static dipole moments can also be referred to as “excess dipole moments.”
Beneficially, the present disclosure notes functional groups can be added to these compounds in such a way that they can be covalently attached to DNA during DNA synthesis without significantly altering the optical properties of the molecules.
The gate region 306 also contains a special dye molecule 404 (or several such dye molecules) depicted as the ellipsoid of
For typical dye molecules 406 the conjugated n-bond network is approximately linear and as a consequence the difference static dipole moment and the transition dipole tend to both be collinear with the long axis of the conjugated n-bond network. There are, however molecules for which the difference static dipoles and transition dipoles are not parallel. An example for which the two dipoles are perpendicular to each other is given by molecule 28 in scheme 2 of Jacquemin. This molecule is shown as follows:
For this molecule, the difference static dipole moment lies parallel to the horizontal axis while the transition dipole lies parallel to the vertical axis. Applicant has verified the strength of the difference static dipole moment for this molecule is approximately 8 D. Although Jacquemin did not report the value of the transition dipole moment, Applicant has calculated via time-dependent density functional theory (TD-DFT) that the molecule has a transition dipole moment of 4 D. When used as a gate molecule 404, a small transition dipole moment is not serious because the molecule 404 is not being used as part of the exciton channel 302. A difference static dipole moment of 8 D would be adequate for switching. Because the difference static dipole moment for this gate molecule 404 is perpendicular to its transition dipole moment, the gate molecule 404 can be oriented such that its transition dipole is orthogonal to the transition dipole moments of the exciton channel dipoles while its difference static dipole moment is close to parallel with that of the channel dyes, thereby giving rise to a large exciton-exciton interaction 108.
Other Non-Limiting Examples of Excitonic Devices that can Employ the Excitonic Ballistic Transistor
It is to be appreciated that exciton wires may be formed when a series of chromophores are held within the architecture so that when a first chromophore, the “input chromophore,” is excited and emits an exciton, the exciton passes, without loss of energy if sufficiently close, to a second chromophore. That chromophore may then pass the exciton to a third chromophore, and so on down a line of chromophores in a wavelike manner. The wires may be straight or branched and may be shaped to go in any direction within the architecture. The architecture may contain one or more wires. Depending on the architecture system used, the exciton wires may be formed along a single nucleotide brick, such as in using the scaffold strand of nucleotide origami, or multiple bricks may comprise the wire, such as in molecular canvases. When two or more wires are brought sufficiently close to each other such that they are nanospaced, the exciton may transfer from one wire to the other. By controlling this transfer, it is possible to build quantum circuits and gates. Some examples of said quantum circuits and gates are described in co-owned, co-pending U.S. patent application Ser. No. 17/447,839, titled ENTANGLEMENT OF EXCITONS BY ACOUSTIC GUIDING, filed Sep. 16, 2021. The originally filed contents of U.S. patent application Ser. No. 17/447,839 are hereby incorporated by reference in their entirety including without limitation, the specification, claims, and abstract, as well as any figures, tables, appendices, or drawings thereof. Quantum algorithms enable the speed-up of computation tasks such as, but not limited to, factoring and sorting. These computations may be performed by an excitonic quantum computer. The excitonic quantum computer can be made from exciton coherence wires, circuits, and gates, such as those described in co-pending, co-owned U.S. Pre-Grant Pub. No. 2019/0048036, which is herein incorporated by reference in its entirety.
Exciton wires can be made by closely spacing chromophores br together as depicted in
Exciton circuits made from these exciton wires may be made to be analogous to electronic circuits but where excitons carry the signals rather than electrons in classical computing. By bringing two exciton wires sufficiently close to each other an exciton can hop from one wire to the other by transferring from one chromophore to another. By doing this carefully one can make devices that function as signal dividers such as those found in Yurke et al., “Passive Linear Nanoscale Optical and Molecular Electronics Device Synthesis from Nanoparticles, 2000, Phys. Rev. A, 81, 033814, which is herein incorporated by reference in its entirety. The division ratio depends on rates with which excitons can be transferred between chromophores in the coupling region. The transfer rate depends on the spacing between the chromophores and their orientations. This dependence on spacing and orientation enables the construction of signal dividers with, for practical purposes, any division ratio. An exciton propagating down one exciton wire will become delocalized so that one must think of the exciton as being in a superposition state where it resides on both exciton wires. This excitonic device is a basis-change gate. The function of which is analogous to that of an optical beam splitter or microwave directional coupler. A basis-change gate is one of the fundamental quantum gates.
Another quantum gate of fundamental importance is a phase-shift gate. The phase accumulated by an exciton is proportional to the distance it travels. Hence, a phase-shift gate can simply be made by engineering the wire that the exciton travels over to have the length needed to accumulate the proper amount of phase. The phase an exciton accumulates is also determined by its energy relative to the optical transition energy for the chromophore. The optical transition energy here denotes the energy difference between the chromophore's ground electronic state and its lowest excited electronic state that has an allowed optical transition. Hence, phase shifters can also be fashioned choosing the chromophores of differing optical transition energies. It is also possible to make phase shifters by terminating two ports of a signal divider with chromophores having differing optical transition energies.
Another quantum gate of fundamental importance is a controlled basis change gate. In contrast to the gates already discussed, which rely on wave interference effects, a controlled basis change gate relies on the interaction between two excitons. When two excitons reside on neighboring chromophores they feel each other's presence just like two electrons will feel each other's Coulomb repulsion when they are brought close together. The two-exciton interaction arises from static Coulomb interactions between molecules and is most strong when the molecules have an asymmetric molecular structure. Asymmetric molecules possess a permanent electric dipole which changes sign when the molecule is excited from the ground state to the excited state. The static Coulomb interaction, in this case is a dipole-dipole interaction which, when both chromophores are excited (the two-exciton case), differs in sign from the case when only one chromophore is excited (the one-exciton case). Due to the static Coulomb interactions between chromophores one exciton will accumulate extra phase in the presence of the other exciton. As a result, the presence or absence of one exciton can control how the other exciton moves through a basis change gate.
These three types of gates, the basis-change gate, the phase-shift gate, and the controlled basis-change gate, form a complete set if the phase-shift gates can be produced with a finite set of phase angles. Because the phase angles can be controlled by the exciton path length, the optical transition energies of the phase-shifter wire chromophores, or through the construction of optical phase-shifter gates out of basis-change gates with selected ports terminated, this last requirement can be met. With this finite set of gates, one can assemble exciton circuits that perform any quantum computation. A set of gates having this property is said to be capable of universal quantum computation. This is analogous to the electronic computer case where the NAND gate is a universal gate in that any Boolean function can be implemented by a circuit employing only NAND gates.
It is possible to perform universal quantum computation with just basis-change gates and phase-shift gates, but the number of parts (gates) one needs grows exponentially with the size of the problem. So, doing quantum computation this way performs as well as classical computers. By introducing controlled basis-change gates one can drastically reduce the parts count so that much fewer parts are required than for a classical computer. The controlled basis-change gate enables the entanglement of many-body (many-exciton) states so that a network of quantum gates acts as if it is performing many different computations simultaneously. This is similar to an n bit memory register. In a classical computer each memory element of the register can be in either a “zero” or a “one” state but not both simultaneously. In contrast a quantum mechanical register can be in a state that is a quantum mechanical superposition of being in the zero state and the one state. An n bit quantum memory in this sense can act as if it is holding 2n bits of information, whereas the classical computer memory only holds n bits of information. A single controlled basis-change gate accepting as inputs the contents of memory elements i and j and delivering the outputs back to memory elements i and j can update the amplitudes of all of the 2n states in the superposition of the memory register simultaneously. This is quantum parallelism.
Not all math problems are known to benefit from quantum speedup, but several classes of problems are known where quantum computers can vastly outperform classical computers. Two of the problems are factoring and database searching.
Chromophores, however, exhibit many non-ideal characteristics for quantum computing. The electronic degrees of freedom are strongly coupled to the vibrational and environmental degrees of freedom. This causes phase jitter, which causes phase error to grow with time, thus spoiling the interference effects that the quantum gates relay on. All quantum computers suffer from this problem to a greater or lesser extent. Chromophores are also difficult to arrange in the requisite configurations.
What exciton quantum computers have in their favor is fast switching time, compact size (the components are relatively small molecules), and possible room temperature operation. Because photons are readily converted into excitons and excitons are readily converted into photons, it is noted that the above excitonic devices may find application in optical information processing, apart from quantum computing, as more compact embodiments of the currently employed optical phase shifters, signal dividers, and switches that can employ Kerr nonlinearities, which have the functionality of controlled basis-change gates. For these applications the performance requirements are less demanding than that for quantum computation.
Finally, it is to be appreciated Applicants have created compositions of non-reciprocal optical devices comprising of aggregates of chromophores either attached to a nucleotide architecture or covalently bonded having a desired conformation, such as those described in co-owned, co-pending U.S. patent application Ser. No. 17/443,285, titled MOLECULAR AGGREGATE FOR OPTICALLY-PUMPED NONRECIPROCAL EXCITON DEVICES, filed Jul. 23, 2021. The originally filed contents of U.S. patent application Ser. No. 17/443,285 are hereby incorporated by reference in their entirety, including without limitation, the specification, claims, and abstract, as well as any figures, tables, appendices, or drawings thereof.
From the foregoing, it can be seen that the present invention accomplishes at least all of the stated objectives.
The following table of reference characters and descriptors are not exhaustive, nor limiting, and include reasonable equivalents. If possible, elements identified by a reference character below and/or those elements which are near ubiquitous within the art can replace or supplement any element identified by another reference character.
Unless defined otherwise, all technical and scientific terms used above have the same meaning as commonly understood by one of ordinary skill in the art to which embodiments of the present invention pertain.
The terms “a,” “an,” and “the” include both singular and plural referents.
The term “or” is synonymous with “and/or” and means any one member or combination of members of a particular list.
The terms “invention” or “present invention” are not intended to refer to any single embodiment of the particular invention but encompass all possible embodiments as described in the specification and the claims.
The term “about” as used herein refer to slight variations in numerical quantities with respect to any quantifiable variable. Inadvertent error can occur, for example, through use of typical measuring techniques or equipment or from differences in the manufacture, source, or purity of components.
The term “substantially” refers to a great or significant extent. “Substantially” can thus refer to a plurality, majority, and/or a supermajority of said quantifiable variable, given proper context.
The term “generally” encompasses both “about” and “substantially.”
The term “configured” describes structure capable of performing a task or adopting a particular configuration. The term “configured” can be used interchangeably with other similar phrases, such as constructed, arranged, adapted, manufactured, and the like.
Terms characterizing sequential order, a position, and/or an orientation are not limiting and are only referenced according to the views presented.
In mesoscopic physics, “ballistic conduction” (ballistic transport) is an unimpeded flow (or transport) of charge carriers (usually electrons), or energy-carrying particles, over relatively long distances in a material. In general, the resistivity of a material exists because an electron, while moving inside a medium, is scattered by impurities, defects, thermal fluctuations of ions in a crystalline solid, or, generally, by any freely-moving atom/molecule composing a gas or liquid. Without scattering, electrons obey Newton's second law of motion at non-relativistic speeds. Here, the definition is extended to excitons that propagate without energy loss.
A “chromophore” is the part of a molecule responsible for its color. The chromophore is a region in the molecule where the energy difference between two separate molecular orbitals falls within the range of the visible spectrum. Visible light that hits the chromophore can thus be absorbed by exciting an electron from its ground state into an excited state. In biological molecules that serve to capture or detect light energy, the chromophore is the moiety that causes a conformational change of the molecule when hit by light.
A “J-aggregate” is a type of dye with an absorption band that shifts to a longer wavelength (bathochromic shift) of increasing sharpness (higher absorption coefficient). In “H-aggregates”, a hypsochromic shift is observed with low or no fluorescence. Bathrochromically shifted “J-bands” and hypsochromically shifted “H-bands” have been explained in terms of molecular exciton coupling theory, i.e., coupling of transition moments of the constituent dye molecules. J and H aggregates can aggregate under the influence of a solvent or additive or concentration as a result of supramolecular self-organization. J and H aggregates can alternatively be formed by templating dyes to a scaffold such as DNA to control their proximity and orientation. Thus, it is to be appreciated the present disclosure is not to be limited to solely the aggregation phenomena to a self-organizing process.
A “bathochromic shift” is often referred to as a “red shift” in photochemistry. Bathochromic shifts are a change of spectral band position in the absorption, reflectance, transmittance, or emission spectrum of a molecule to a longer wavelength (lower frequency). Hypsochromic shifts are often referred to as “blue shifts” in photochemistry. Blue shift is the phenomenon in which the frequency of an electromagnetic wave, such as light, emitted by a source moving towards the observer is shifted towards the blue side of the electromagnetic spectrum (wavelength is decreased or energy is increased).
The “scope” of the present invention is defined by the appended claims, along with the full scope of equivalents to which such claims are entitled. The scope of the invention is further qualified as including any possible modification to any of the aspects and/or embodiments disclosed herein which would result in other embodiments, combinations, subcombinations, or the like that would be obvious to those skilled in the art.
This application claims priority under 35 U.S.C. § 119 to provisional patent application U.S. Ser. No. 63/199,104, filed Dec. 7, 2020. The provisional patent application is herein incorporated by reference in its entirety, including without limitation, the specification, claims, and abstract, as well as any figures, tables, appendices, or drawings thereof.
This invention was made with government support under Grant Number US DE-SC0020089 awarded by the United States Department of Energy. The government has certain rights in the invention.
Number | Date | Country | |
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63199104 | Dec 2020 | US |