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steps, they developed an integrated tworeactor system with an interreactor separator, which removes water found to inhibit some of the downstream processes. A 98% yield of butene at 99% GVL conversion was achieved at moderate pressures and temperatures in the presence of a silica-alumina catalyst. After water removal, oligomerization of the butene present in the butane-CO2 mixture with a macroporous polymeric catalyst converted 90% of the butene with 95% selectivity to liquid alkenes with eight or more carbon atoms. This approach offers the benet of producing butene fuel precursors without requiring an additional and costly hydrogenation step. Further, the process operates at elevated pressure, sufcient for conversion of CO2 to chemical products, or for sequestration without need for additional energy-intensive compression. Unlike the process of Bond et al., Lange et al. hydrogenated LA to form VA as the main product, which is then reacted with alcohols to form to a family of valerate esters suitable as gasoline- or diesel-fuel additives. This process retains all of the carbon present in LA. The initial 70% conversion of GVL has >90% selectivity for VA with 10-bar H2 at 250C. They used a platinum-silica catalyst that was bound inside a porous HZSM-5 zeolite catalyst. In a manner similar to the method reported by Bond et al., the reduction proceeds through formation of intermediate pentenoic acid isomers. Although the GVL conversion gradually drops during the reduction, the catalyst can be regenerated by periodic treatment with H2 at 400C. Under these conditions, catalyst performance and VA production were maintained for more than 1500 hours of operation. Lange et al. also report a single-step conversion of LA and ethanol into ethyl valerate using a catalytic reactive distillation system. The lower molecular weight esters (methyl, ethyl, and propyl valerate) exhibited performance suitable for use as a gasoline additive at levels of 10 and 20% (by volume). Higher esters (butyl and pentyl valerate) could be used directly as a diesel fuel or as a diesel additive. Road trials using a 15% blend of ethyl valerate in regular gasoline were carried out with 10 vehicles and a total of about 250,000 km of driving. No engine performance issues were noted, but the lower energy density of ethyl valerate resulted in an expected loss of fuel economy per volume. Thus, functionally useful biorefinery intermediates need not be structurally identical to compounds currently used in the petrochemical industry. Technology development issues must be addressed before a deeply entrenched and established biofuel (ethanol) can be replaced with promising but less recognized alternatives. Research challenges also exist: The initial LA production from sugars is still not highly efcient and has not been tested at scales necessary to ensure viability in a fuel-production scenario. Finally, the question of what to do with the formic acid produced as an unavoidable LA by-product must be addressed. A similar situation exists within the biodiesel industry, which must deal with the formation of a glycerol co-product. Formic acid can be used to reduce LA to GVL via catalytic transfer hydrogenation, but such processes have yet to be optimized (11, 12). Nonetheless, these demonstrations of a biobased chemical as an intermediate in a process compatible with petrochemical technology will spur the use of renewable biomass as a source of the next generation of biofuels, and as a replacement for traditional raw material supplies.
1. K. Weissermel, H.-J. Arpe, Industrial Organic Chemistry (Wiley-VCH, Weinheim, Germany, ed. 4, 2003). 2. M. M. Green, H. A. Wittcoff, Organic Chemistry Principles and Industrial Practice (Wiley-VCH, Weinheim, Germany, 2003). 3. J. N. Chheda, G. W. Huber, J. A. Dumesic, Angew. Chem. Int. Ed. 46, 7164 (2007). 4. E. de Jong, R. van Ree Rea, R. van Tuil, W. Elbersen, in BioreneriesIndustrial Processes and Products, B. Kamm, P. R. Gruber, M. Kamm, Eds. (Wiley-VCH, Weinheim, Germany, 2006), vol. 1, pp. 85111. 5. R. D. Perlack et al., Biomass as feedstock for a bioenergy and bioproducts industry: The technical feasibility of a billion-ton annual supply (U.S. Department of Energy, Washington DC, DOE/GO-102995-2135, 2005). 6. J. J. Bozell, Clean-Soil Air Water 36, 641 (2008). 7. J. J. Bozell, G. R. Petersen, Green Chem. 12, 539 (2010). 8. J. Q. Bond, D. M. Alonso, D. Wang, R. M. West, J. A. Dumesic, Science 327, 1110 (2010). 9. J.-P. Lange et al., Angew. Chem. Int. Ed. 49, 4479 (2010). 10. S. W. Fitzpatrick, ACS Symp. Ser. 921, 271 (2006). 11. H. Mehdi et al., Top. Catal. 48, 49 (2008). 12. H. Heeres et al., Green Chem. 11, 1247 (2009). 10.1126/science.1191662

References

PHYSICS

An Atomic View of Quantum Phase Transitions

Brian DeMarco

The transformation of individual cold atoms between quantum phases has been imaged.

lthough it is evident that strong interactions between particles can lead to the formation of quantum-mechanical phases such as high-temperature superconductivity, there are many gaps in our understanding of the underlying physics. Cold atoms trapped in optical lattices have emerged as an ideal model system for understanding the creation of these phases because the strength of the particle interactions can be smoothly tuned and complicating factors
Department of Physics, University of Illinois at UrbanaChampaign, Urbana, IL 61801, USA. E-mail: bdemarco@ illinois.edu

in solids such as disorder can be controlled. Although much progress has been made, new techniques are needed if these experiments are to reveal enough detail to verify theoretical models. On page 547 of this issue, Bakr et al. (1) used their quantum gas microscope (2) to image and study the dynamics of individual atoms as they transform between different quantum phases. An artificial solid is created in optical lattice experiments by first cooling atoms trapped as a gas in ultrahigh vacuum to nanokelvin temperatures (3). The atoms are then captured in a lattice that is created by slowly turning on a combination of laser beams.

The atoms play the role of the electrons or superconducting pairs of electrons in a solid, whereas the light substitutes for the underlying ionic crystal. Different crystal geometries can be produced depending on the arrangement of the lasers. The holographic technique used by Bakr et al. to create a square lattice is especially powerful because it can, in principle, produce any two-dimensional crystal geometry. Optical lattices have been used for a broad spectrum of experiments at the forefront of atomic physics. Strontium atoms trapped in an optical lattice were used to demonstrate the most accurate clockone that loses a sec-

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PERSPECTIVES
ond every 200 million years based on neutral atoms (4). Optical lattices are also an attractive platform for quantum computing (5), in part because a lattice can provide large numbers of properly initialized quantum bits. The application that has garnered perhaps the most attention uses optical lattices to simulate physics models that we do not completely understand (6). One of these is the Hubbard model, which incorporates only two key ideas: Electrons can hop between sites by quantum tunneling, and they interact with each other only if they are on the same site. A key and surprising feature of the Hubbard model is that electrons that would be expected to be mobile can be pinned by strong electronic interactions in a quantum phase known as a Mott insulator. Two versions of this model are realized by cold-atom systems, depending on the atomic species. The FermiHubbard (FH) model is used if the atoms are fermions (7, 8). This model has been applied to materials of key technological importance, such as the high-temperature superconducting cuprates. The Bose-Hubbard (BH) model (9) is used if atoms are bosons, such as the rubidium-87 atoms used by Bakr et al. in their experiments. Variants of the BH model have been applied to granular superconductors and arrays of Josephson junctions. Despite the apparent simplicity of Hubbard models, some of their most basic features have confounded physicists. For example, it is not clear how different phases arise in the FH and disordered BH model as parameters such as the interaction energy are varied. The source of this confusion is twofold. Theoretical approaches have failed to produce a complete understanding of these models. In this situation, physicists often resort to numerical simulation to provide answers. Unfortunately, in cases such as the FH model, our most powerful supercomputers can exactly simulate the dynamics of only tens of electrons, and advances consistent with Moores Law have increased the simulation size by about one electron per decade. The advantage of replacing computation with optical-lattice simulations is that highly precise atomic physics techniques can be used to coax answers directly from nature. The equivalent of materials parameters in solids can be easily and directly controlled, for
Quantum gas microscopy. At the bottom, atoms (shown in red) in a circular Mott-insulator shell are trapped using lasers. Above this sample, a hemispherical lens that is part of a high-resolution imaging system used by Bakr et al. creates an image of this quantum state.

example, by tuning the intensity of the lattice lasers. Rather than developing techniques to grow new samples, as in experiments on solids, these adjustments can be made once every experimental cycle (time scales of minutes). Bakr et al. imaged individual atoms transforming from a superuid into a Mottinsulator phase as the ratio of interaction to tunneling energy was increased (see the gure). Similar studies of this phase transition in an optical lattice probed on the most microscopic scale have also been reported by Sherson et al. (10). This transformation corresponds to a Mott insulatorsuperconductor transition in an electronic system; the bosonic Rb atom acts like a superconducting electron pair. In the cold-atom Mott-insulator phase, a xed number of atoms occupy each lattice site at zero temperature; at any nite temperature the atom number somewhat uctuates. Fortuitously, unintended ripples present in the atom trap used by Bakr et al. revealed that nearly one-dimensional Mott-insulator islands can be prepared with unexpected, ultrahigh delity even at nite temperatures. Additional cooling likely occurs when this state ejects thermal excitations into neighboring superuid or thermal regions. Bakr et al. were also able to measure how fast a Mott insulator formed at the single-site level by varying the time over which they increased the lattice laser intensity. Atom-number uctuations in Mott-insulating sites were suppressed in only a few milliseconds. These measurements provide important new information for ongoing research into equilibrium in lattice experiments (11). The experiments by Bakr et al. build on previous work demonstrating optical (12)

1. W. S. Bakr et al., Science 329, 547 (2010). 2. W. S. Bakr, J. I. Gillen, A. Peng, S. Flling, M. Greiner, Nature 462, 74 (2009). 3. I. Bloch, Nat. Phys. 1, 23 (2005). 4. A. D. Ludlow et al., Science 319, 1805 (2008). 5. C. Monroe, Nature 416, 238 (2002). 6. M. Lewenstein et al., Adv. Phys. 56, 243 (2007). 7. U. Schneider et al., Science 322, 1520 (2008). 8. R. Jrdens, N. Strohmaier, K. Gnter, H. Moritz, T. Esslinger, Nature 455, 204 (2008). 9. M. Greiner, O. Mandel, T. Esslinger, T. W. Hnsch, I. Bloch, Nature 415, 39 (2002). 10. J. F. Sherson et al., http://arxiv.org/abs/1006.3799 (2010). 11. C.-L. Hung, X. Zhang, N. Gemelke, C. Chin, Phys. Rev. Lett. 104, 160403 (2010). 12. K. D. Nelson, X. Li, D. S. Weiss, Nat. Phys. 3, 556 (2007). 13. P. Wrtz, T. Gericke, A. Vogler, F. Etzold, H. Ott, Appl. Phys. B 98, 641 (2010). 14. I. Bloch, Science 319, 1202 (2008). 15. T. Paiva, R. Scalettar, M. Randeria, N. Trivedi, Phys. Rev. Lett. 104, 066406 (2010). 16. J.-S. Bernier et al., Phys. Rev. A 79, 061601 (2009). 10.1126/science.1193401

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CREDIT: FIGURE COURTESY OF MARKUS GREINER/HARVARD UNIVERSITY, DEPARTMENT OF PHYSICS

and electron (13) imaging of individual optical lattice sites. However, their result provides an atomic view in the strongly correlated regime, in which many-particle statessuch as the Mott insulatorexist that cannot be understood qualitatively using a single-particle theory. This microscopic view of strongly correlated states may be instrumental in achieving a grand challenge for fermion lattice experiments (14), that is, cooling the system to low enough temperatures to observe any potential d-wave superuid phase. Such a result would conrm that the FH model is sufcient to explain high-temperature superconductivity. The rst step en route to this goal is to cool below the temperature for antiferromagnetic ordering, which so far has been out of reach of experiments (15). Microscopy at the single site level will be an important tool for developing and diagnosing new cooling methods. Furthermore, by combining microscopy with holographic potentials, Bakr et al. have the means to accomplish entropy segregation through atom-trap engineering (16), which may be a viable approach to achieve these exotic quantum states.

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