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Surface-Confined Assemblies and Polymers de Ruiter and van der Boom



          TABLE 4. Truth Table for the Combinatorial Logic Operations of the
          Os-Based Monolayer Operating with Three Chemical Inputs and Two
          Different Starting States: Output A and Output B 32
                       chemical inputs
          entry   Cr 6þ    Co 2þ   Ir 3þ  output A a  output B b
           1       0        0       0        1          0
           2       0        0       1        0          0
           3       0        1       0        1          1
           4       0        1       1        1          1
           5       1        0       0        0          0
           6       1        0       1        0          0
           7       1        1       0        1          1
           8       1        1       1        1          1
                                                 b
          a Output A: output generated with Os 2þ  as the starting state. Output B: output
          generated with Os 3þ  as the starting state.         FIGURE 9. Relative memory increase, compared to binary memory, by
                                                               increasing the radix (N). Adapted with permission from ref 40. Copyright
                                                               2010 American Chemical Society.

                                                               technology, as the first reliable devices were bistable. Ac-
                                                               cording to Keyes, only current binary transistor technology is
                                                               feasible for computing, since transistors exhibit a large gain,
                                                               can separate inputs from outputs, and act as amplifiers,
                                                               so errors are nonaccumulative. 33  Moreover, they are self-
                                                               correcting since the input potential range is much larger than
                                                               their output range, which eliminates undesirable noise le-
                                                               vels and small variances introduced by device fabrication. 10
          FIGURE 8. (A) Combinatorial circuit operating with three chemical inputs  What is the advantage of using a different base? Informa-
                                     2þ
          (Table 3) with a static current state (1, Os ). (B) Sequential circuit generated
                                                               tion processing occurs with a certain information density
          with a dynamic current state (Os 2þ  or Os ). Adapted with permission from
                                     3þ
                                                               that is determined by the base (or radix). If the information
          ref 32. Copyright 2010 Wiley-VCH Verlag GmbH & Co. KgaA.
                                                               density is low, or the information is processed inefficiently,
          combinatorial logic circuit shown in Figure 8A. However, if
                                                               one needs simply more space to achieve a certain computa-
          Os 3þ  (logic 0) is used as the starting state, a YES gate is
                                                               tional level. In this regard, a higher-valued radix is beneficial
          generated with respect to input-two (Co 2þ ). Therefore, a logic
                                                               as it raises the information density per single logic operation.
          circuit and a gate can be mimicked with the same system, by
                                                               The most efficient radix for information processing is Euler's
          changing the oxidation state of the system at the beginning       34
                                                               number 2.718.   Since integer numbers are used, ternary
          of each entry. By doing so, all the possible combinations of
                                                               (base-3) is the most efficient. The number of digits required
          inputs and previous states (whether the starting state is Os 2þ /
                                                               to represent any given number is ∼1.6 less in ternary than
          Os 3þ ) were tested, which are required for sequential logic.
                                                               in binary, resulting in a significant increase in memory
          Interestingly, for the input string 0 0 0, the output is depen-                            d
                                                               capacity. Changing from binary memory 2 to multistate
          dent whether the starting (previous) state was Os 2þ  or Os 3þ .  d                             d
                                                               memory N leads to an exponential increase of (N/2) , where
          This reveals the sequential logic element that is present in
                                                               N is the radix and d is the amount of digits (Figure 9).
          this system, and the corresponding sequential logic circuit is
                                                                  Within the framework of molecular logic, multivalued
          depicted in Figure 8B. This circuit operates according to the
                                                               logic and data storage with molecule-based systems are
          combination of outputs A and B generated by the combina-
                                                               relatively rare. In 2006, de Silva et al. utilized the principles
          torial logic circuit and the YES gate. Although this is fundamen-
                                                               of multivalued digits for molecular computational identifica-
          tally one sequential logic circuit, it consists of two individually  35
                                                               tion (MCID).  Combinations of dyes attached to polymer
          addressable combinatorial logic scenarios. 32
                                                               beads respond to different chemical environments, enabling
                                                               multiple fluorescent states, that, when combined, operate
          V. Multistate Logic and Memory                       similarly to radio frequency identification (RFID). Ternary
          The above molecular logic gates and circuits are exclusively  logic gates were reported by Remacle and Levine who
          binary in nature. Base-2 has historically been used in silicon  showed that three coupled quantum dots can be used to
          568 ’ ACCOUNTS OF CHEMICAL RESEARCH ’ 563–573 ’ 2011 ’ Vol. 44, No. 8
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