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A Sceptic
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Some questions
A Sceptic   8/9/2013 10:52:43 AM
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"Instead it uses a metal-insulator transition that occurs throughout the metal-oxide crystal structure and that is dependent on electron correlation."

1. Comment: If this is the case there would be no need to set a current compliance during the switching cycles.

2. Comment: If this is the case both the ON- and OFF-state conductances must scale with the device area.

nonvolatile
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Re: Some questions
nonvolatile   8/9/2013 2:08:30 PM
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Dear Sceptic,

Thank you for your questions, but they seem more expressions of belief than healthy scepticism. In any case, I accept the challenge:

Answer to you question 1 - If that was the case there would be no need to set a current compliance during the switching cycle. In posing this quetion in reaction to the article's claim of Metal-insulator transition based in ELECTRON CORRELATIONS, you put forwar (embedded in your opinion) that you seem to know a lot about Electron Correlations and Mott transitions. 

ANSWER> You must be confusing electron-electron correlations, such as in a metal, where multual repulsion causes a "fermi Hole" between electrons, with what is also called electron correlation due to the Coulombic Potential called the Hubbard U in the literature. In that case, and it is the case here, it is the occupancy of the 3d8 shell that creates a change in the oxidation number of the Nickel and a gap is opened. That is the insulating phase and it is well known that Nickel Oxide should be a metal, by Bloch-Wilson band theory, and yet is an insulator in its's normal state. When, pressure or a lot of electron injection at the nanoscale, we have the complete screening of the gap (which technically is between 2p(oxygen) and 3d(L)9, where L=ligand). To achieve this, some of the TMOs filamentary proposals may actually be doing the same thing, either inside the filament or near the surface where many oxidation numbers occur for the TMO. Now, WHEN THE GAP CLOSES, AND THE UPPER EMPTY CONDUCTION-BAND LIKE NARROW 3d9 BAND AND THE LOWER FILLED BAND TOUCH, WE HAVE THE DEFINITION OF A METAL, i.e. BAND OVERLAP AND METALLIC CONDUCTION OCCURS. SO, TELL ME NOW HOW DOES YOU COMMENT SCORE THAT "IF THIS IS SO THERE WOULD BE NO NEED FOR COMPLIENCE" - IT IS NOT EVEN WRONG, TO QUOTE LINUS PAULING. SORRY, DUST OFF YOUR COPY OF KITTEL.

Answer to question 2 - "If this is the case the ON and OFF current should scale with device area" - this almost looks like a fair opinion, after all V=IR. But, try to understand that V=IR assumes a "Drude" conductance, meaning that this is a classical electron gas device with Rigid density of states of which the the conductivity is proportional to (and also the electron density). But, even if you go to a more semi-classical model of conductivity, like Sommerfeld's, this is not possible to be used in this case, as the conductivity for ON and OFF change because the density of states is not rigid and can be controlloed by two steps - on in the material itself, that is have only +2 and +1 and +3 so that the disproportionation reaction of the nickel is reversible - from metal to Inulator and vice-versa. And the second step is in the Device Physics itself, something that I will leave out for now because you were so certain of your opinions that I think you must do some homework in this part of the explanation. In any case, When you have the ON current, you have a dead short with a mesoscopic ballistic current - this in the filament world was confused with a connect/disconnect model of these filaments. It is not a wrong model, it is only the worng preparation of the material: if you create filaments it is because the many body phase is simply not there - that is you are stuck with many traps that create Ni(0) metallic traps and lots of oxygen vacancies that lead to Ni(+4) which all together show bad OFF state retention and scattering in the Vset and Vreset programming voltages. SO, let's now focus on your Scalling rules for both conductances: When the Mott Insulator is in the insulating state, look carefully at your IV curves and you will see what? A diode like IV - does this scale as a conductance? when that IV curve is actually from tunneling? What is a Tunneling Conductance (homework for you again)?  And  now, when it is in the metal side, we can consider this an ohmic current with a simple free electron model, and YES, YOU ARE RIght, it should scale as 1/Area. But, in the large area data, this is like controlling and measuring the diference in resistance between aluminum and copper - you can only see that if thickness/Area ratio is small and sigma (from J=sigmaE) would be dramatically difference. In advanced CMOS, length (thickness) shows a difference, but not in these large area devices that we made public to the EETIMES. Now, because the inner active area is doped differently from the two contact buffer layers of very conductive non-switchable NiO:CO, we have now 2 degrees of freedom to "fix" the resistance (and the high ON current) - Doping for scattering and thickness adjustments. Doping for scatering can be optmized not to influence the "Doping with a Ligand to compensate thte coordination sphere" (Homework: Coordination sphere? what is that? - that is what has been grossely overlooked by my filament colleagues).

Now, it seems that I still did not answer your question 2 - but I did have to set the stage and reboot some of your background, because a sense a swiss cheese span of condensed matter physics. THE ANSWER: With an IV for the OFF state depending on Square root of Voltage, a sign of the image charge and the other conductance being such that the current is ohmic (plus the large area in a metal phase), how in God's solid state do you come up with a ridiculous scaling theory? Sorry, I am not really a mean person, I just do not appreciate uneducated scepticism passing as an educated and welcome scepticism in good science.

A Sceptic
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Re: Some questions
A Sceptic   8/10/2013 6:34:39 AM
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Dear Nonvolatile,

your model considers a non-local switching effect, i.e., no lateral confinement as in the case of filamentary switching effects. I simply wonder why you have to set a current compliance while switching from the OFF- to the ON-state. Does the overall current density become so high under the switching conditions that it would be critical for the whole MIM cell?

nonvolatile
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Re: Some questions
nonvolatile   8/10/2013 7:17:33 AM
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Dear Sceptic, The transition from insulating to metal is caused by two steps; 1, barrier lowering with classic MIM behavior dominated by image potential. The turn on shape in a linear scale should be well designed, in the second step, the bulk conduction takes over as the core potentials are severely screened, we have now a metal. So why you would not have compliance. The trick here is to keep a handle on relationship between Ion and I compliance. And as you know, current density is not a function of area or thickness, current is, in the plot of current density versus field, conductivity is the only variable that depends on materials properties. Misty versus field, conductivity is p which depends on doping and DOS. You are correct on the value of keeping the MIM under control here. I do not want to review too much here. This is when we leave chemistry and enter device physics, a real messy and confusing picture emerges if you do not have a handle on the switching mechanism, which we found and for now it is proprietary.

nonvolatile
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Re: Some questions
nonvolatile   8/10/2013 7:17:33 AM
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Dear Sceptic, The transition from insulating to metal is caused by two steps; 1, barrier lowering with classic MIM behavior dominated by image potential. The turn on shape in a linear scale should be well designed, in the second step, the bulk conduction takes over as the core potentials are severely screened, we have now a metal. So why you would not have compliance. The trick here is to keep a handle on relationship between Ion and I compliance. And as you know, current density is not a function of area or thickness, current is, in the plot of current density versus field, conductivity is the only variable that depends on materials properties. Misty versus field, conductivity is p which depends on doping and DOS. You are correct on the value of keeping the MIM under control here. I do not want to review too much here. This is when we leave chemistry and enter device physics, a real messy and confusing picture emerges if you do not have a handle on the switching mechanism, which we found and for now it is proprietary.

nonvolatile
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Re: Some questions
nonvolatile   8/10/2013 9:57:22 AM
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I do not remember answering this question, but it is a good one. The. Answer is no the current density is not so high to compromise the MIM device. But, you still need compliance. Not as much though

goafrit
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Re: Some questions
goafrit   8/9/2013 2:36:01 PM
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>> but he declined to provide further information for publication at this time

As my boss used to say "the best ideas are never in conferences and papers. See the patent office for them"

nonvolatile
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Re: Some questions
nonvolatile   8/9/2013 3:19:14 PM
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Goafrit, your old boss would be proud. We worked For 6 years on this and patents are issued in the US and all over the world. Now, academics. There is A lot of science here and it is a tough road ahead. Everyone Runs to publish half baked things. It is time to work first and publish later. Academia as many have called for change, should no longer be business neutral. We need the jobs here...

resistion
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VO2
resistion   8/9/2013 7:15:47 PM
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In VO2 device, the self-heating above transition temperature caused turn-on. What is the temperature effect here? Interestingly, the VO2 device was filamentary, i.e. thermal runaway of localized current would require compliance.

nonvolatile
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Re: VO2
nonvolatile   8/9/2013 9:45:58 PM
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Dear CEO, As you know, VOx is very temperature dependent. In fact there is a famous Korean patent for a current limiting device presumed Ed use in a device that become more resistive as the cell phone battery gets warmer. The stoichiometry of VOx makes the phase transition to be second order and very sensitive to thermal runway. It is not possible to generalize all stoichiometries and just exactly is the metal- insulator transition, Mott, or even Anderson ~ Mott, a combination of defects, specially oxygen vacancies. I will risk to say that de trapping electrons from these vacancies may together with a high current in the metal phase creates the thermal runway you talk about in VOx. But in our case we damped the oxygen vacancy content by forming stable complexes that tie up Nickel metal clusters and at the same time fixing the ohmic oxidation number with the CO complex. Since the ohmic side starts at zero voltage and very small currents, thermal runaway initiated by the current can be ruled up, for I ^2 R is very small and can be made extremely small, for example, below 100 microamps of ON current in a 100 micron square device. With R from 100 Ohms to 2000, in these particular doped samples, and a very linear and temperature independent switching fro - 269 to 150 C ,continuously switching, where can you find this thermal runway?you surely do not expect filament formation at 4 degrees kelvin? So I recommend that you unplug a little from carrying over your thermo interpretation and review the many variations of VOx and brush up on the special area of quantum phase transitions which are temperature independent and happen even at 0 K. We only went down to 4k, and it kept on running. We are trying to go to 0.4 K looking for fermi liquid behavior.....there is a lot involved in this. Rich literature. Filaments are optional and are parasitics rather than the operating principle, that is, if start with a corrected coordination sphere. Remember the Co and ammonia experiments in basic chemistry? Since ammonia is a ligand, variations in colors show how coordination chemistry change the bands and you have all those pretty colors. Google this, it's elementary but will clearly show you that these localized electrons even in an aquas solution have different band gaps due to 3d orbitals interactions. All I did is apply coordination chemistry to solid state TMOs. By the way, platinum complexes use coordination chemistry the same way in chemo therapy.

Ron Neale
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CeRAM edge effects
Ron Neale   8/10/2013 5:08:13 AM
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Volatile-While I can for the moment accept your claim that you can create buffer layers to screen the central layer, third layer of your (20nm-20nm-20nm)thick structure, what happens at the edges of the device in the lateral direction. If you have a "pore" like structure then I am at loss to understand why the surface states will not lock the material in one of its resistance states. If the material in the as born state is insulating that might be OK, if not then as you shrink the device to sub-20nm dimensions the edge will create a filament like structure of the active area and the resistance will become edge leakage dominated. I guess in analogy it could be a probem like the ratio of area/volume that the PCM promoters ignored. Would be interested in your observations.

On the subject of VOx as somebody who has made many of those in pore structures as potential matrix isolating devices the the low transition temperature was the practical problem not thermal runaway in the conducting state. Those devices with micron dimensions, had resistance that scaled with the inverse of area.

 

 

nonvolatile
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Re: CeRAM edge effects
nonvolatile   8/10/2013 6:49:46 AM
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Ron, Central to your question is the comment "if you have a pore structure". But, we do not have a pore structure, quite the opposite. Films Are dense and stoichiometric. Take a look at the XRD data : ours are exactly the reference bulk data. The XRD of sputtered devices is all over the place. Also bad edge effects due to a born on ohmic state actually goes the other direction as the area reduction increases the resistance, wanting to make the insulating state. It then takes counter doping to bring in the born ON condition. If you do not start there the born off state would require some higher voltage and certainly some form of filament is there. So, the adjustment is to start born on and cycle from there to the off state. I guess that because you do not have this corrective doping and they start with sputtered the oxidized devices, the devices of the filament people will always need Electroforming. That is what would really create edge leakage.it is sure not the case with born on . We can as just the resistance by doping every layer and achieve born on without stuck bits. This is the beauty here: once the current Density is reasonable, adjusted by the doping , the surface to volume ratio becomes manageable and we follow the R vs. square root of Voltage curve that is design to scale everything correctly. All events of switching occur above the insulating baseline which when scale without doping is a disaster and Electroforming is need. I have no problem with your VO experience. As I mentioned before it is an extremely temperature dependent material.

Ron Neale
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Re: CeRAM edge effects
Ron Neale   8/10/2013 8:29:37 AM
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Nonvolatile:-Thanks, but I still have a problem, if you do not have a pore structure as the means of defining the device, for the moment let take that out of the discussion and any influences the surface states of its dielectric might have. Consider an orthogonal array of CeRAMs where your three layers are formed as a single large area on a flat surface. The lower electrode in a narrow channel in the flat surface and the orthogonal electrode on the upper surface of the three layers. Now after all the doping and annealing you describe you creat a device that is stoichometric, doped and conducting in the on state. Now when I switch to the insulating state there is a region at the edge of the device where the material in the conducting state is in contact with the insulating material and bridging it; plus there are already many more conducting paths between electrodes!  Although you may not want to consider a "pore" as the type of structure that defines and confines your structure, the device structure options appear limited. It would appear to be either surface state effects or bridging. Unless you are using some form of masked ion implantation to achieve the control the doping as well as defining the structure, accounting for the need for annealing, i.e. a post-implant anneal.

2)I know you do not want to discuss all the details of the switching as you said in your post below. Are you able to say if there is any part of the switching  transition that displays negative resistance, I guess it would be "N" type. If so the oscillation frequency of a negative resistance oscillator constructed using your device would resolve the thermal problem and might have useful application elsewhere, especialyy if the switching time is as fast as you claimed..

nonvolatile
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Re: CeRAM edge effects
nonvolatile   8/10/2013 9:31:43 AM
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Ron, you have an interesting question. But, you are looking at the transition still as something that moves thought the device as it is a moving front of electrons depending on a classical drift velocity. As you are an expert in VO let me remind you that the Mott transition in VO was recently measured at 80 femtoseconds. So, if you think the way you seem to be going, and I am not too helpful for reasons of space more than proprietary info, you then miss a key point , specially in the insulator to metal side of the switch. So let me explain: First you should know that an insulator of this type has practically the same number of electrons as a metal.the problem is that these electrons(here 4s2 electrons from nickel ion lost to the lattice ) are far from the fermi level and thus cannot conduct. When the density of incoming electrons from the cathode form trigger the metal state, there is no gap and we clip the current. Now for your specific Ansatz, the starting of the on to off state, which in the filament theory sometimes starts at the anode, is also what happens here, but for slightly different reasons: in this case, near the anode, within a few atomic layers have gone through a quantum phase transition at a 1000 to 100000 times faster than electrons coming from the cathode. The cascading is immediate and the fermi level now is in a region of zero density of states. Thus, we depend on this lack of thermal equilibrium to switch . In the filamentary world this is called a local oxidation reaction region. But this is accounted for as a disconnect of the filament. And it is. But here, in the right phase is just the disproportionation.so, the speed of propagation of the phase transition being way faster then electron drift, causes the gap to appear faster than the speed of injected electrons and the device is instantaneously off. The negative resistance does not occur here. But it is very easy to think that it can occur if the RC time constant is long in the metal to insulating condition. It would look like a tale. This can happen if the area is really large. But RC means Maxwellian time, which may happen in the metal side as the current is starting to go a minimum as the insulator phase sets in. But this again is too slow compared to the speed of the band splitting. It maybe interesting trying to use this device in places where super fast switching is needed, but I do not know if we could get negative resistance with NiO. I do have several other materials which also use compensation doping that delivers an enormous current in a fast time. I will check that set of data to see if they have negative resistance. Just to clear the air, no ion implantation, nothing more than what I have disclosed- it is all in maintaining the coordination chemistry right.

Ron Neale
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Re: CeRAM edge effects
Ron Neale   8/10/2013 11:21:49 AM
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Nonvolatile: Thanks again you are being more than generous with your time. No  I am not an expert in VOx just got involved when trying to rescue PCM where I have a little more expertise. That is in a failed attempt to use doped VOx in a bi-directional matrix isolation device as a means of cancelling out the effects of element separation caused by current density in the PCM.  The chalc based bi-directional threshold switch was useless, irrespective of the claims by one large company for their stacked Chalc-Chalc based isolation device-memory array.

With respect to propagation of the effect, I am more in favor of a radial model, certainly works for PCM and most likely accounts for what is happening in some of the oxide ReRAMs, but not  neceassarily in all cases. I think when crystal electrodes are involved the elevated temperature failure of PCM is crystal growth, propagation in the direction of current flow. The latter  was the point I was trying to make in one of the PCM Progress  Reports Published in EETimes. It might be  a potential problem with your MIM structure.

Where am I going with the speed aspects. I have recently been exploring chalcogenide threshold switching as a posible means of constructing a thin film large area phased array antenna.  The Chalcs are much too slow and the negative resistance oscillations self FMs because of changes in the disorder which suggest things are getting warm, irrespective of what appears to be a very rapid initial switching transition. If you have other materials it might be worth thinking about that type of application for both large and small area thin film PAAs.

 

nonvolatile
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Re: CeRAM edge effects
nonvolatile   8/10/2013 12:39:07 PM
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No problem - I really enjoy put this out there with frank questions and learned opinions. The reasons are that may Sayers better know their stuff and knowledgeable skeptics can keep you on your toes . And finally we can perhaps challenge the pseudo science nonsense that some large companies seem so entitled to put out there disrespecting our intelligence. I completely agree with you on PCM but I cannot agree with your radial switching even for filament makers. In the electro forming step the filaments are grown surrounding grain boundaries as shown recently in the literature. In this I agree and I modeled that long time ago and measured the activation energy. But the switching is not radial growth of filaments, only electro forming . In our case we have just too much data and analysis to the contrary. In PCM the local recrystalozatiom temperature leads to a heat conductivity of about 480 C/sec and that is about equal to molten salt. There is then radial heat dissipation and you are right. In FeRAM the surface defects nuclear daim growth down very fast, so thick or old Materials like TGS or even PVF2 depend on lateral growth that cannot go faster than the speed of sound. I guess we can stay disagreeing on the mechanism until I can provide more data to match the physics. But, take a tip from the fact that (a) we can make NiO always conductive and if we have a 60 nm thick device with 100 micron squared, the resistance is 4 ohms. Now use that as buffer layer of 20 nms with a middle active switching region of 10 nms that can go to 150 mega ohms by switching, it makes radial charge transport a bit difficult. Stock to tunneling and you will stay on the right track.

resistion
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Re: CeRAM edge effects
resistion   8/10/2013 8:24:36 AM
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Thermal runaway may have been a poor terminology of the occurrence which was not destructive, the filament was a common observation. It's also possible the filament evolved into a conventional resistance, as that was also commonly observed.

resistion
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thermal stability
resistion   8/11/2013 9:24:54 AM
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In one of your papers, there was a model of the insulator state. I am not sure if that model is updated yet. It suggested self-saturating current (which I presume not correct). More seriously, it also showed that the resistance of the insulator would be dramatically decreased at an elevated temperature above 100 C. Is there an update to this in an upcoming publication?

nonvolatile
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Re: thermal stability
nonvolatile   8/11/2013 10:44:34 PM
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Dear CEO, Frankly I do not know what you are referring to. I would never promote a memory that dies at 100 Cand the data I sent to EEttimes goes to 300. Currently it is 400 C. Now the self saturating is another story. The relationship between compliance and on currenyy can saturate at low compliance values, that is also In the literature. Of filaments

Charles.Desassure
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Need more information...
Charles.Desassure   8/12/2013 12:37:57 AM
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Interesting, but I need more information.  I will wait for the next article as it relates to this topic.

nonvolatile
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Re: Need more information...
nonvolatile   8/12/2013 10:44:30 AM
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DEAR CEO,

The word "interesting" is a power word -usually used by CEO's or thesis advisors" - it really mean "What a naive person, he will know better next time" so here is the DATA.



RIGHT SIDE IS THE HRS OF A COMMON RERAM MADE WITHOUT DOPING WITH CO, THE LEFT IS CeRAM. GOT IT NOW? 

REGARDS,

CARLOS

PS. DATA TALKS, THEORY SHOUTS AND OPINIONS USUALLY...WELL, SUFFER.

krisi
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0.2V read
krisi   8/12/2013 2:12:11 PM
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0.2V read...very impressive Carlos...would you be interested in presenting this technology at CMOSET in Grenoble next year? www.cmosetr.com, best, Kris

nonvolatile
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Re: 0.2V read
nonvolatile   8/12/2013 6:38:35 PM
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Kris. Thanks for the invitation. Please send info at caraujo@aol.com

krisi
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Re: 0.2V read
krisi   8/12/2013 7:47:41 PM
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Sounds good Carlos, I have sent you the email...Kris

sframboss
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ReRAM
sframboss   8/14/2013 9:10:22 PM
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Good luck, Carlos!

Joe

nonvolatile
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Re: ReRAM
nonvolatile   8/16/2013 12:09:57 PM
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Thanks Joe. It's like FeRAM all over again, but this time we waited six years before a peep.

 

sframboss
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Re: ReRAM
sframboss   8/16/2013 12:53:49 PM
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Us too but in a different direction.  A lesson from the School of Hard Knocks!

Joe

nonvolatile
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Re: ReRAM
nonvolatile   8/17/2013 11:07:52 AM
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Joe,

Any systems for testing resistive and pick up the transition speed?

sframboss
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Re: ReRAM
sframboss   8/17/2013 12:27:53 PM
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A PUND-type architecture would probably do what you want.  Can you make individual elements or must they be tested embedded in CMOS?

Joe

nonvolatile
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Re: ReRAM
nonvolatile   8/17/2013 12:36:31 PM
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BOTH - BUT PUND in the conductive state must be done in such a way that that you do not fry the pulse generator. For materials development, we have to use the masks that are single resistors etc. In that case we have high geometry (130) and lower (30). It is necessary then to have approriate active current compliance. In the CMOS, the compliance is done with the circuit on board. 

What I was interested is to see if we can get the switching speed. In some materials, lasers had to be used due to the tens of femtoseconds regime. But, we can slow it down and see if your system could be used - however, we must also thing of feedback in the compliance, since going from metal-like to insulator is not tracktable. Any thoughts on a system with feed back so that it will not oscilate. 

sframboss
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Re: ReRAM
sframboss   8/17/2013 1:28:07 PM
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Our output stages are limited to 20mA and cannot be damaged by a short.  However, they will be slow, generating 500ns pulses off-the-shelf.  They could theoretically go to 100ns with a change in programming and some potentiometer adjustments but that is still slow for you.  The existing systems are targeted at ferroelectric devices with high impedance so current resolution is excellent above 100kohm but not in the ohm range.  That being said, an off-the-shelf system could program your elements and distinguish memory states.  With mods, we could give you more sensitivity for the conductive state if the read pulses are kept very short.  Then, with our Vision operating system already in place, you would be able to create any parameter, stress, or reliability test you wanted without our having to write custom software for you.  In particular, you could easily set up tests to run fatigue, "imprint", and retention tests of your individual memory elements over temperature and voltage conditions under automated control.  (I assume that these three classice ferroelectric reliability issues are present in your technology but just express themselves in a different manner.)

 

I do not think we would see oscillation in our test circuitry during the the metal-to-insulator transition.  Mathematically, it is little different than the switching of a very square ferroelectric capacitor although the resistance range is probably several orders of magnitude higher.  (Our 20/80 PZTs change effective capacitance by a factor of 100 during switching.)

 

As for speed, it is the same situation as with ferroelectric caps:  put a memory element on a CMOS substrate to get precise pulse width control under expected operating conditions.  You could inexpensively make the control dice (not full up memories) on MOSIS and then bump down your memory elements.  This arrangement could get you probably to several nanoseconds with MOSIS specs.  That is not femtoseconds but the resulting test data cache would be huge (necessary for statistics) and robust.  We can control such a chip with our equipment so the programmability of Vision would be available immediately.

 

Please contact me directly, Carlos.  I do not know your e-mail.  Go to our web site www.ferrodevices.com and fill out a customer form.  Michelle will pass it to me. 

 

Again, good luck!

Joe

PhyandEE
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Re: ReRAM
PhyandEE   10/6/2013 10:56:17 PM
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I'm wondering how they determine whether it is a filamentary effect or not.

 

nonvolatile
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Re: ReRAM
nonvolatile   10/7/2013 7:48:17 AM
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Several ways. First, by the obvious, that is, the device is "born on", that is, it is perfectly ohmic as made - this only happens if doped by CO. Then, by degrees of doping, being always ohmic if the higher doping level is used, and down to born insulating as doping goes to zero. Optimizing doping, allows ohmic behavior as born on down to small areas. Thus, the filament idea is more of a "soft breakdown" nature when the resistance is high due to small areas. It then became a "science" as doping is not truly understood - that is, doping here is not to change the conductivity by shifting the fermi level - instead, it is a coordination number balancing - i.e., CO is a ligand that substitutes for lost oxygen and increase of uncompensated Ni. Such ligand substitution is not what the same as doping in the semiconductor sense. That is, it is not what is usually done in the so-called "Hydrogenic doping"-e.g.,as Phosphorus in Si, donating an electron to the conduction band - here, it only adjusts Ni to have Ni(+2) to be the dominant species and be the new ground state and go unimpedent to N(+1) and Ni(+3) "disproportionation reaction" responsible for the reversible Metal/Insulator transition. With formation of filaments, we have Ni(0) and Ni(+4) which impedes reversibility, unless in an area, randomly created, where the disproportionation reaction occurs and the "reconnection" of filaments leads to a "short" or "open" circuit, which becomes the operation mode of a filament based switch. Thus, an impure and stochastic systm becomes the "memory paradigm" for filamentary ReRAMs, versus a materials design technique for CeRAM. Also, the usual cross section TEM is used to detect filaments. The Metal/insulator transition is a quantum phase transition effect in most Transition Metal Oxides, but ultra thin (60 nm) devices have lots of non-stoichimetric areas, and the optimal control of oxidation number species is impossible to control in filamentary ReRAMs. Detailed transport based on "tunneling with e-e correlations" has been published in the May 31st, 2011 issue of J. Appl. Physics. More detailed work is in press.

 

PhyandEE
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Re: ReRAM
PhyandEE   10/7/2013 8:40:54 PM
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-nonvolatile- thank you for your reply.

Question 1: how you prevent oxygen in your devices? O2 could play a key role in the oxide.

Question 2: TEM observation for a filament. I have some experience on HRTEM for oxides. It is really a tough job if the filamment goes to the atomic level.

resistion
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Re: ReRAM
resistion   10/7/2013 11:36:34 PM
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Of course HRTEM is best for finding/confirming filaments. But the matrix around the filaments may also conduct with area proportionality. If it's negligible leakage level, certainly it can be said to be "filamentary."

nonvolatile
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Re: ReRAM
nonvolatile   10/8/2013 7:54:22 AM
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I am sorry but this is too speculative. It is also not confirmed by many forms of experimental results. I suggest that you read the literature on Metal/Insulator phase transitions. Explanations with "filaments" can be easily debunked.

Leakage as an evidence of extremely fine filaments, etc. is just not what is happenning physically. It can happen in the normal NiO without doping control. But, hundreds of experiment with model verification contradicts that possibility. The switching mechanism in CeRAM is due to an electron-electron interaction at the orbital level. Verification of this is solid. The same can be acting in the filamentary devices at the points of conect/disconnect areas. The filaments are continuous Ni(0) metallic phases surrounded by lots of defects with activation energy of 0.48 eV. This makes the off state very unstable with temperature. This is not the case in CeRAM. The quantum phase transition is temperature independent and has been tested from 4 degrees Kelvin to 150 degrees C. Since the interaction energy between electrons is short range coulombic, the cleaner material without too many defects is able to have in loco switching. The filamentary material, even with filaments, still requires such an interaction to exist in order to shut off conduction. It is only a matter of materials design to make the interaction the clear mechanism - such a design can only be achieved by proper charge compensation of Ni, to force it into a reversible disproportionation reaction. Without that precise doping, the switching still occurs in filamentary devices, but the control of the Vset and Vreset is really difficult and random. Thus, you see a lot of ReRAM proposals with a layer that is somewhat stoichiometric and a layer non-stoichiometric or of a different material so that charge trapping in the interface become dominant and a new thing is now controlling the storage states, but it is still very defficult to make a defective material behave the same way everytime and everywhere in the array. This has been done for 12 years without much success for product stability. Our way is better - not only it works better, it has well explained physics to propose moedl checking experiments. Thanks for your interest.

resistion
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Re: ReRAM
resistion   10/8/2013 8:25:02 AM
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I guess other ways are to use C-AFM or partitioned electrodes.

nonvolatile
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Re: ReRAM
nonvolatile   10/8/2013 8:45:27 AM
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Correct. Both ways would be fine. But, I do believe that you must have not only tools but also be able to create experimental scenarious that you can predict the outcome. This is important in device development, especially when the materials cannot be taken for granted, like in the case of ReRAMs. In this case, you must ask many questions, starting with the mechanism that goes into the metal/insulator transition. What turns it on and off? Is it carrier dominated, density dominated, Tunneling dominated etc. In checking all these issues you can start fine tunning the device physically and your hypothesis in a step by step way. Thus, the proper tool at the proper time is key - but most important is the asking of the proper questions. Of course this is true in science overall, but when applied to a very specific set of questions under an educated question asking system based on a physical model is key. As the questions are answered and support the physics of the device model(not just math), then a "device paradigm" comes into place, that may be completely different than other people's. In the case of ReRAM, this has happened by introducing the carbonyl ion into the materials in such a way that you can make it always conducting, for example. And, then not always conducting, but compensated enough that the transition from metal to insulator and vice versa can be controlled to a 5 nm thick region in even Aluminum or CoSi2 and other electrodes.So, it is a different beast to start with. Knowing the always conducting state had no filaments imposed, we then can build up from there and understand better. When such departures from other people's experiences occurs and you can explain it, you have something. This is our case. Many device architectures can be tested and poperties predicted with high accuracy. I had many such experiences in my professional life. Thus, it may sound old fashion but I do not see how anyone would just "go to the kitchen and cook a device" without physics. And, now I add, without chemistry and Materials Science. In closing, this is very complex device -filaments or not. In the filaments area, the insulating state is the begining. In CeRAM case, the conductive state, usually hole current is where we start. Very different starting points, but it is a cloo for the device understanding to do both types of devices (RERAM and CeRAM). 

 

PhyandEE
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Re: ReRAM
PhyandEE   10/8/2013 9:13:25 PM
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I have to say that MIT (metai-insulator-transition) is a very traditional topic, although there are many arguments, for example, the correlated electron state in a doping process. The discussion of the mechanisms in a resistive switching process involves a lot of papers, and MIT is one of them. It is interesting but also very fundamental. I heard that you are submitting your paper to a journal such as nature. They could ask you many tough questions. Anyway, congratulate to your outstanding device performance!

 

nonvolatile
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Re: ReRAM
nonvolatile   10/8/2013 9:47:52 PM
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Thank you for your congratulations. The MIT in the heavy doped devices is caused by the Anderson process, which shows that the electron localization is due to the heavy defect concentration or heavy doping. Your are correct in stating that this is a fundamental process - that there are many views. What you may be missing is that I am a professional and a professor, and  I have published in Nature and Science before. So this is not some fantasy. In the last 6 years I made sure I new the theoretical side of this by reading 7200 papers in the subject and carefully carved the device physics, which is the combination of the proper green's function and an open system in which electrons and holes can come in and out of the device. As far as priority, we published already the transport theory in the nanoscale Mott transition and got IV characteristics. Final refinement and generalization to other materials will follow. In the case of NiO, it is well known that it is a Charge Transfer Mott insulator. The question is, how does it switch  states in an thermodynamic open system like a device? What are the controlling mechanisms? And, do you have THE DATA? All this has been carefully studied by myself and my team. This is a big departure from just Breaking down NiO to make filaments. This is fixing NiO with CO to control the oxidation numbers that induce the Charge transfer MIT. Sounds like science fiction, I know, but it is a real thing and it is repeatable. The devices work well and in predictable fashion. As far as the papers coming out of this effort, I suggest that you also look at the issued patents of Symetrix. And, as far as the understanding of the theoretical side of MIT, let us see what the reviewers will say, but I appreciate your concern about "tough questions". Thank you for your interest.

PhyandEE
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Re: ReRAM
PhyandEE   10/8/2013 11:13:32 PM
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"Tough questions" only means they have found the right person. The two memristor Nature and Nature Nanotech papers by HP in 2008 are the typical cases. What would happen if theoretical physicists like Meuffels and Soni were listed as the reviewers? I don't know whether Chua was in the reviewer list. But surelly favorite comments have been given.

Your paper could be different from the HP's, becuase you are a serious physicists talking about the serious physics problems. But since you are talking about physics, then physicists will be the reviewers. As I have said, there are many arguments in MIT. One of the difficulties is to show the direct evidence. Good luck to your submission.

nonvolatile
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Re: ReRAM
nonvolatile   10/8/2013 11:23:28 PM
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The HP paper was completely non-sense. It was the best piece of pseudo science ever done by a major corporation. Thank you for separating me from that crowd. Unfortunately, or fortunately, this is how I see the filament based and Conductive bridge devices. Uterly nonsense.

Thank you for your interest. Yes, the Data will tell, and its agreement with the model. 

resistion
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Re: ReRAM
resistion   10/9/2013 7:53:04 AM
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With all due respect to your MIT model, I'd caution against completely dismissing the filamentary devices, at the very least because they are so prevalent. And can you guarantee no doping or thermal non-uniformity or defect-free device? Your model is already based on insulator phase appearing locally at one electrode. The burden is on anyone to prove they are free from defects, rather than assume so a priori.

Ron Neale
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Re: ReRAMa A Conundrum
Ron Neale   10/9/2013 6:27:49 PM
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Resistron a Conundrum in the limit can filaments switching be bulk?

If the size of the area of a filament type memory device is reduced to the point where the filament is the same diameter as the device electrode area, can that now be considered as a bulk switching effect?

If the switching depends on the collapse of the pre-switching current into a nucleating point then it might be expected that the contact area of such a device would always need to be larger than the filament. These would be devices where thermal effects play a major role in the switching event.

However, in a device where conducting precursors determine the location of the filament (i.e. devices that normally require forming) the location of the filament would be positioned stochastically.

In those devices where defects allow some form of true bulk switching effect in a region close to the surface of one electrode with the defects or metal precipitates acting as a series resistor carrying most of the current through the bulk which have been alluded to here in the comments. Is a type which might be considered filament for large area and might claim to be bulk with scaling but as the electrode area is reduced will only work if the required defect path is certain to be present.

Would a multi-filament device where the set current would determine the number of filaments that come into play (weakest first) be considered a filament device or when the total area is involved a pseudo bulk switching device?

 

 

eavedrop44
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Re: ReRAM
eavedrop44   4/21/2014 4:26:33 AM
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nonvolatile
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Re: ReRAM
nonvolatile   10/9/2013 12:58:57 AM
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The paper by Meuffels and Soni, does debunk the HP model with an electrochemical argument. Actually in two lines we can show that the HP model is not a physical model. There is no way to show a Mott transition with a classical argument though. The paper lacks on that. Now the original Memristor concept is a naive mathematical explanation of a circuit element. It lacks physical understanding of the meaning of conductance In an ultra thin TMO film. The original paper also had no intrinsic long term retention. It was a phase difference misinterpreted as memory. Although paper by Meufffel and Sony correctly addresses the gross aspects of the HP model, it fails in explaining how such a device would work if TiO was more stoichiometric as in other RRAM devices with filaments. The evidence is strong of MIT in such devices. Where HP went wrong is that the two fluid model was modeling a bad device and not what a true Memristor, If such a thing is allowed to exist, should not be based on a circuit element, but instead on a model of TMO conductivity based on quantum mechanics. Conductivity without scattering has to start at least with Lubo"s formula. Then at mesoscopic scale and non rigid density of states, the current has to be calculated completely different from a simple Drude"s model! Not Boltzmann Transport either. The TiO layers were 30 nm thick. Ballistic transport with e-e interactions and e-oxygen vacancy interaction should have been used. None of these approaches were used. I was amazed that a drift-diffusion two fluid model was used. Vacancy flow had only the effect to trap or de trap electrons and if they moved they had no way to flow as electrons into the electrodes. So what was understood as an MIT with crazy hydrodynamic explanations was nothing but charge trapping with some movement of defects aided by the tunneling current. A simple test of retention over temperature for different pulse width would show low activation energy of the off state and low memory effect with high temperature. I can even guess that the activation energy would be in the order of 0.35 eV, typical of titanates oxygen vacancies de trapping. Very naive pele did that work. Poor Hynix, I wonder if they will ever make a device, I do want to leave it here for the record that if the Titanate is balanced as we did with NiO, it does work as a CeRAM. We have beautiful data on that. In fact we made a 10 nm thick titanate active region and it works just fine. We will present both NiO and TiO data in our papers. ,

PhyandEE
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Re: ReRAM
PhyandEE   10/9/2013 10:54:09 PM
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Nonvolatile said my HRTEM comment on the filament observation is rather speculative, Resistion said Nonvolatile is priori in his NiO devices, and Ron Neal said it is like a Conundrum.

It is interesting. I have collected a bunch of papers on this topic. In the reports, filament size ranges from microns to nano, and to atomic scale. HRTEM and CAFM are the two facilities frequently used. There are also some theoretical modeling works.

No matter what, as Nonvolatile has said, DATA talks, I think we should see the data first. The outstanding device performance as described is a good news to the resistive switching study. I have to mention that although it is difficult to observe the filaments through HRTEM, it does not mean that filament should or should not work. For this reason, I think the work by nonvolatile has good chance to be accepted. It is not the kind of works by HP.

nonvolatile
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Re: ReRAM
nonvolatile   10/9/2013 11:58:01 PM
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It is not possible to look at this matter with the eyes of an indepemdemt electron description. That is, without the ability to show that the change in oxidation number is the result of electron localization, which causes the repulsive coulombic force responsible for the charge gap, one can go around circles. The disproportionation reaction is responsible for the charge gap. It is completely not dependent on position of the Ni ion, so that, after the defects such as oxygen vacancies are compensated by trapped electrons, it is totally possible to have a local MIT which would complete the filament or break it. This can be easily be missed measured as a redox reaction, if you are just checking the oxidation number -like EELS. So, it is not an easy thing to be 100% sure. Other approaches in the electrical measuremnt must be taken. One example is to measure the capacitance of the insulating state as a function of frequency. You can immediately see that the low frequency CV plot is hysterectic due to interfacial polarization and this causes the Vset and Vreset  divergence. This also show that the many oxydation states on the surface of a non compensated NiO is to blame. On the other hand, the compensated NiO is a smooth CV plot without hysteresis. 

I am not at liberty tight now to disclose a few other things. This will come out in due time. But, as we all know, the conductivity is always proportional to DOS. If you use the independent electron approximation (typical of metals and semiconductor), you can never show the f=non-rigid DOS afforded by TMOs. Only if you let DOS=0 and DOS= finite, that you can show the teo states - insulating and metal. Thus, it does not matter if you have filaments or not to have these two states. Somewhere in the filament model, where the filament is broken, an oxidation number-disproportionation -reaction will contribute to the closing and opening of the filament. Thus, as Ron says, this is a conundrum, until you get to reliability. Then, when you see your off state unstable with temperature and your Vset/Vreset variations, you would ask, How cab I control this? well, with the right device physics. Which then requires the stable material to satrt with. Off coarse we do not erradicated all defects, but enough to have a better device and one that we do not have to breakdown the oxide and have these filaments inside the material as the only means of switching. Thus, let us say that we have "quantum scale" filaments....still, how do the close and open? with a in-loco disproportionation. So, why not make the bulk all like that to start with. 

Honestly, we can dope the device to the tipping point that we have a soft electroforming like behavior - sort of born-off. One could interpret that such a device has Nanofilaments. Thus, after a slightly higher voltage than the norma set voltage, the device works just fine. But, if you go a litlle more in doping, it is no longer the case and you have a born-on device. So, the ability to go from always conductive down to just insulating enough to need a little push, is for me a clear demonstration that we have a point. Doping can eliminate the need for filaments. Thus, I am  not so worried about this. It may even be possible that the filaments are doped grain boundaries. Still, doping with CO passivates the device and yields control.

resistion
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Re: ReRAM
resistion   10/7/2013 9:51:51 AM
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Check how current changes with area.

PhyandEE
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Re: ReRAM
PhyandEE   10/7/2013 7:57:46 PM
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I have to disagree that it is not a good method after reading more papers on this topic, although some guys are using this in their papers. For example, firstly making a device 200 microns for the electrode, then 100, 50 etc.

A simple question is where is the filament? If you don't know it, changing area does not make sense. I also have many other concerns.

 

PhyandEE
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Re: ReRAM
PhyandEE   10/7/2013 8:24:18 PM
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One recent paper talks that multiple nano-filaments can even co-exist in the same thin film.

Another concern is that how they get the resistance value. I also have several other more concerns. The area dependent method is really too simple.

 

resistion
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Re: ReRAM
resistion   10/7/2013 11:19:56 PM
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As long as the proportionality with area is violated, it is filamentary, i.e. localized at some points. Almost certainly at multiple locations. The single filament is an idealization, the current density would be unphysical.

resistion
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Re: ReRAM
resistion   10/7/2013 11:27:35 PM
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Maybe should clarify, check resistance vs. area. A filamentary case is virtually area-independent. The resistance would depend on the writing current. Alternatively, the writing current would depend on area.

resistion
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nickel vacancies
resistion   10/10/2013 3:36:06 AM
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I just recalled some papers mentioning nickel vacancies in NiO, maybe CO doping eliminates O vacancies but adds Ni vacancies?

nonvolatile
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Re: nickel vacancies
nonvolatile   10/15/2013 7:47:15 AM
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Thank you for your question. We can see that when the CO level, introduced in the oxide by wet chemistry (i.e., already in solution in the Ni precursor, for Ni(CO)4 is extremely poisonous and not added to the precursor as such-please, anyone trying this DO NOT use Ni(CO)4, it kills), the resulting material is always in a metal-like state. This is very much thickness dependent. Thus, it is not clear if vcancies has anything to do with the metal phase, as a vacancy would be completely screened by the surrounding electrons in the Drude regime. Now, in the less conductive case, it is then possible to have a reversible Mott transition due to the disproportionation reaction of Ni(+2) to Ni(+1) + Ni(+3). The CO doping technology is able to make the disproportionation reaction to be the dominant reaction, which is specifically the charge species that can be reversed without the need of filaments. Because disproportionation reactions are simultaneous oxidation/reduction type of reactions, it can be easily confused with a redox reaction. Redox reactions can occur in severely damaged materials, but they are not very reproduceable. Well then, the CO can be electron donor via a pi bond, and an acceptor in the sigma bond. The other two defect reactions in NiO are Ni(+2) + Vox(+2) --> Ni(+4) + Vox(0){two trapped electrons} and Ni(+2) + 2 e(-) -->Ni(0). The first reaction with oxygen vacancies creates a peak of Ni(+4) in the XRD spectrum. And the metal Ni(0) also shows up in XRD. Both peaks disappear with CO doping, but they are dominant in non-doped materials. Thus, it seems that the pi bond is dominant. It is a possible that in the filamentary versions of NiO, All species occur and we have a situation that the insulating phase dominates at the small areas (the area dependence is very strong, for other reasons). Thus, when the soft breakdown occurs, the filament is strongly Ni(0) and surrounding it, there are many Vox's. Where the filament is disconected - this is seen mostly around the anode - we believe that the "CeRAM effect" (i.e. - a disproportionation/Mott transition) may be occuring to bridge the metal-like filament to the electrodes and create the metal like state of the ReRAM. Extending this to other transition metal oxides, has been achieved by our group.

Thus, I hope that this gives you the general idea. The problem of all ReRAM is the Roff state being unstable with temperature and dispersed in the cummulative probability of good bits. Thus, so far, the dispersion of the off states, specially after many write pulses makes the "freak bits" population too high for commercialization. The other two areas are the high on current and the Vset/Vreset dispersion -specially the Vset dispersion. All these things are extremelly reduced in the CeRAM approach.

As we make a 3 layer structure with Heavy doping/10 nm of low doping/heavy doping, we completely screen the active middle region from the electrodes and be electrode agnostic (CoSi, SiNi, Al..), we have cleaned up the material to have only the right species, lowered Schottky effect, and we are "born on", that is, it is already ohmic as built. The details of this will be coming as we make our next press release - probably late November. (When I said 2 months, it was mid september, so we are delayed a little) - what is holding us back? - everything, including many activities such as ALD and difficulties in nanoscale areas. But, it is going. Thanks for your interest.

 

PhyandEE
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Re: nickel vacancies
PhyandEE   10/16/2013 11:46:49 PM
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What is the resistance switching ratio? Is it uni-polar or bi-polar switching?

nonvolatile
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Re: nickel vacancies
nonvolatile   10/17/2013 4:38:01 AM
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The ratio is adjustable by doping, but a good number is 10,000 to 1. It is important to have a good Ron that is not to low, as this and Imaxon need to be well controlled. A lower than 100 microamp Imaxon is prefered. Doping for higher Ron, can be easly acomplished by "elemental"doping and does not disturb the the CO doping that heals the coordination sphere of Ni. This is another important aspect - after CO doping, the material is clean, and then one can dope for scateering in the on state independently of anything. It is this bulk control, which cannot be achieved very easily if filaments are just being connected/disconnected in some microscopic area, that makes the coordination control doping so elegant. Thank you for your question.



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