Contents 1. Introduction 3519 2. Origin of Residual Dipolar Couplings and Complementary Observables 3520 2.1. Residual Dipolar Couplings (RDCs) 3520 2.2. Chemical Shift Anisotropy (CSA) 3521 2.3. Pseudocontact Shifts in Paramagnetic Systems 3522 2.4. Cross-Correlated Relaxation 3522 3. Alignment of Samples 3523 3.1. Bicelles 3523 3.2. Bacteriophage 3523 3.3. Polyacrylamide Gels 3524 3.4. Other Media 3524 3.5. Practical and Theoretical Considerations 3524 4. RDC Data Acquisition 3526 4.1. One-Bond H N −N and C−H RDCs 3526 4.2. Other Protein Backbone RDCs 3528 4.3. One-Bond C−C and C−H RDCs in Protein Side-Chains 3531 4.4. Proton−Proton RDCs 3531 5. Structural Interpretation of RDCs 3532 5.1. Additional Constraints in Structure Determination and Refinement 3533 5.2. Direct Structure Determination 3533 5.3. A Tool for Structure Validation or Homology Searches 3535 5.4. Orientational Relationships between Components 3535 6. Limitations and Future Directions 3537 7. Abbreviations 3537 8. Acknowledgments 3538 9. References 3538

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